FISH Aquavit 2015
FISH Aquavit 2015
This discussion paper is/has been under review for the journal Atmospheric Chemistry FISH review
and Physics (ACP). Please refer to the corresponding final paper in ACP if available.
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J. Meyer et al.
Discussion Paper
Two decades of water vapor
Title Page
measurements with the FISH Abstract Introduction
fluorescence hygrometer: a review Conclusions References
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J. Meyer1,* , C. Rolf1 , C. Schiller1,† , S. Rohs1,2 , N. Spelten1 , A. Afchine1 ,
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M. Zöger3 , N. Sitnikov4 , T. D. Thornberry5,6 , A. W. Rollins5,6 , Z. Bozóki7,8 ,
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7,8 9,10 9,10 9 11 J I
D. Tátrai , V. Ebert , B. Kühnreich , P. Mackrodt , O. Möhler ,
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H. Saathoff , K. H. Rosenlof , and M. Krämer J I
1
Institut für Energie und Klimaforschung 7, Forschungszentrum Jülich, 52425 Jülich, Germany Back Close
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Institut für Energie und Klimaforschung 8, Forschungszentrum Jülich, 52425 Jülich, Germany
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Deutsches Zentrum für Luft und Raumfahrt, FX, 82234 Oberpfaffenhofen, Germany
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Central Aerological Observatory, Dolgoprudny, Russia
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NOAA ESRL Chemical Sciences Division, Boulder, USA
Discussion Paper
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Cooperative Institute for Research in Environmental Sciences, University of Colorado Interactive Discussion
Boulder, Boulder, CO, USA
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Department of Optics and Quantum Electronics, University of Szeged, Szeged, Hungary
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MTA-SZTE Research Group on Photoacoustic Spectroscopy, Szeged, Hungary
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Physikalisch-Technische Bundesanstalt (PTB), 38116 Braunschweig, Germany
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Reaktive Strömungen und Messtechnik, Technische Universität Darmstadt, 64287
Darmstadt, Germany
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Institute for Meteorology and Climate Research (IMK-AAF), Karlsruhe Institute of
Technology, 76344 Eggenstein-Leopoldshafen, Germany 15, 7735–7782, 2015
*
now at: Institute of Energy and Environmental Technology (IUTA), 47229 Duisburg, Germany
†
deceased FISH review
Received: 17 December 2014 – Accepted: 2 February 2015 – Published: 12 March 2015
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J. Meyer et al.
Discussion Paper
Correspondence to: C. Rolf (c.rolf@fz-juelich.de)
Published by Copernicus Publications on behalf of the European Geosciences Union.
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Abstract Introduction
Conclusions References
Tables Figures
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Interactive Discussion
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Abstract
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The Fast In-situ Stratospheric Hygrometer (FISH) is an airborne Lyman-α photofrag-
ment fluorescence hygrometer for accurate and precise measurement of total water 15, 7735–7782, 2015
mixing ratios (WMR) (gas phase + evaporated ice) in the upper troposphere and lower
5 stratosphere (UT/LS) since almost two decades. Here, we present a comprehensive FISH review
review of the measurement technique, calibration procedure, accuracy and reliability
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of FISH. A crucial part for the FISH measurement quality is the regular calibration to J. Meyer et al.
Discussion Paper
a water vapor reference, namely the commercial frostpoint hygrometer DP30. In the
frame of this work this frostpoint hygrometer is compared to German and British trace-
Title Page
10 able metrological water standards and its accuracy is found to be 2–4 %. Overall, in
the range from 4–1000 ppmv, the total accuracy of FISH was found to be 6–8 % as Abstract Introduction
stated also in previous publications. For lower mixing ratios down to 1 ppmv, the uncer-
Conclusions References
tainty reaches a lower limit of 0.3 ppmv. For specific, non-atmospheric conditions, as
set in experiments at the AIDA chamber – namely mixing ratios below 10 and above Tables Figures
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15 100 ppmv in combination with high and low pressure conditions – the need to apply a
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modified FISH calibration evaluation has been identified. The new evaluation improves J I
the agreement of FISH with other hygrometers to ±10 % accuracy in the respective
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mixing ratio ranges. Further, a quality check procedure for high total water measure-
ments in cirrus clouds at high pressures (400–500 hPa) is introduced. The performance Back Close
20 of FISH in the field is assessed by reviewing intercomparisons of FISH water vapor
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data with other in-situ and remote sensing hygrometers over the last two decades. We
find that the agreement of FISH with the other hygrometers has improved over that time
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span from overall up to ±30 % or more to about ±5–20 % @ < 10 ppmv and to ±0–15 %
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@ > 10 ppmv. Interactive Discussion
25 As presented here, the robust and continuous calibration and operation procedures
of the FISH instrument over the last two decades, establish the position of FISH as one
of the core instruments for in-situ observations of water vapor in the UT/LS.
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1 Introduction
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Water vapor in the upper troposphere and lower stratosphere (UT/LS) plays an impor-
tant role in the climate of the Earth. It is a basic component in ozone photochemical 15, 7735–7782, 2015
processes in the lower stratosphere (Vogel et al., 2011) and its concentration also af-
5 fects the formation of clouds (Pruppacher et al., 1997). Water vapor’s direct role as FISH review
a greenhouse gas and its indirect role in cloud formation processes have significant
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impacts on the radiation budget of the Earth (Solomon et al., 2010; Forster et al., 2002; J. Meyer et al.
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Smith et al., 2001; Wang et. al., 1976). For example, isentropic transport of moist air
from the upper tropical troposphere to the lower stratosphere (LS) affects the radia-
Title Page
10 tive budget in two ways. Directly it produces an increase of water vapor in the dry LS
and indirectly it impacts thin cirrus formation near the tropopause (Dessler et al., 2009; Abstract Introduction
Spang et al., 2014).
Conclusions References
Accurate measurements of water in the UT/LS are required to understand the un-
derlying exchange, dehydration, and transport processes (Ploeger et al., 2006) and Tables Figures
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15 to provide input data for atmospheric and climate models (e.g. Solomon et al., 2010;
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Riese et al., 2012). One prominent example is the discussion Peter et al. (2006) in- J I
spired about observed massive supersaturations in the atmosphere, which seemed to
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contradict the understanding of the microphysics of ice formation. As a result, new,
so far unknown microphysical processes were sought and intensive reviews of mea- Back Close
20 surement uncertainties were initiated. As a side note, this “supersaturation puzzle” was
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further investigated based on FISH-measurements as reported by Krämer et al. (2009).
They applied a quality check procedure to in-cloud supersaturation measurements and
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could explain all valid supersaturations by established microphysics.
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Due to the difficulties measuring water vapor in the UT/LS region, global or long term Interactive Discussion
25 observations of stratospheric water vapor are rare (Hurst et al., 2011; Rosenlof et al.,
2001). Consequently, Rosenlof et al. (2001) and Kley et al. (2000) combined water
vapor measurements from different instruments to derive long-term changes of strato-
spheric water. They identified systematic differences between individual hygrometers
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on the order of 20 %, which was partially accounted for by the relative trend analysis
of that study. However, for many other applications, such as radiation calculations and ACPD
cloud formation studies, the absolute accuracy of the water measurement is essential.
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Since the first comprehensive comparison of hygrometers specifically designed to
5 measure in the UT/LS region (Kley et al., 2000, see Sect. 5.1), larger systematic dis-
crepancies between hygrometers have been reported. At mixing ratios below 10 ppmv, FISH review
and particularly below 5 ppmv, differences may be on the order of several tens of per-
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J. Meyer et al.
cents (Fahey et al., 2014; Weinstock et al., 2009) and thus exceeded the combined
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uncertainties stated for the individual hygrometers. As a result of this dilemma, lab-
10 oratory and aircraft based intercomparisons were organized between 2007 to 2013
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(see e.g. Fahey et al., 2014; Rollins et al., 2014) and the measurement quality of the
individual hygrometers was reassessed. Abstract Introduction
This study presents the results of an extensive review process for the Fast In-situ
Conclusions References
Stratospheric Hygrometer (FISH), which was developed at the Forschungszentrum
15 Jülich. FISH has been used for atmospheric measurements of water vapor in the UT/LS Tables Figures
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region for more than two decades. The current version of the instrument is an update
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of the instrument described in Zöger et al. (1999). It was redesigned to run in an au- J I
tomatic mode. FISH has been integrated on a variety of different platforms, including
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balloons, a number of different aircraft (Geophysika, Learjet, Falcon, HALO, WB-57)
20 and laboratory facilities (AIDA). Over the years, FISH has participated in a number of Back Close
field campaigns in the tropics, mid latitudes and the polar region (a subset is given
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in Table 1 of Schiller et al., 2008). A map of all 348 FISH aircraft flights is shown in
Fig. 1. From these flights, a unique set of UT/LS water vapor data is compiled. FISH
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measurements have been used in both high-precision process studies and climatolog-
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25 ical studies with respect to water vapor transport (e.g. Kunz et al., 2008) or cirrus ice Interactive Discussion
water content (Schiller et al., 2008; Krämer et al., 2009; Luebke et al., 2013). Thus,
after more than two decades of operation and more than 100 publications including
FISH measurements, a comprehensive review of the measurement principle, calibra-
tion procedure and data evaluation of water vapor data from the FISH instrument was
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performed and is presented in the following sections of this paper. Additionally, the con-
sistency of the FISH measurements with other in-situ and remote sensing hygrometers ACPD
is reported.
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5 J. Meyer et al.
(1999), was developed for fast and precise airborne and balloon-borne measurements
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of low water vapor concentrations in the lower stratosphere. Over the years, FISH was
also applied for airborne measurements in the upper troposphere with higher water Title Page
vapor concentrations.
Abstract Introduction
10 FISH is a ’closed path hygrometer’, i.e. the instrument is mounted inside of the re-
spective platform and the sample air must be supplied via a tube. On an aircraft, this Conclusions References
tube is in most cases connected to a forward facing the inlet supplying a free flow
Tables Figures
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through the measuring cell driven by the pressure difference between the inlet and gas
outlet. An advantage of this system is that the flow rate is high enough to reduce the
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15 effect of significant contamination of the water signal by outgassing of water molecules
from the walls of the inlet system and the closed cell (see Sect. 3.2). During cloud J I
penetrations, ice particles that also enter the inlet, which is heated, sublimate and thus
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a signal of ice water content is added to the gas phase water (see Sect. 4.4 or Schiller
et al., 2008). Full Screen / Esc
20 The measurement principle used by FISH is based on photofragment fluorescence
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(a sketch of the FISH design is displayed in Fig. 2): water molecules are split into Printer-friendly Version
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a excited OH molecule and a single H atom by Lyman-α radiation (121.6 nm). The
Interactive Discussion
excited OH molecules emit radiation in the 285–330 nm range when relaxing to the
ground state. This emitted radiation is detected by a photomultiplier tube (PMT). The
25 number of detected fluorescence photons Ng is proportional to the water vapor mixing
ratio (WVMR) with a calibration factor ck . This calibration factor is determined prior to
each experiment in the laboratory (see Sect. 3).
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FISH consists of a vacuum-tight measuring cell, the Lyman-α radiation lamp, the
PMT in photon-counting mode and detectors to monitor the Lyman-α intensity I0 and ACPD
the lamp intensity reduced by water vapor absorption (UVA) in the cell (see Fig. 2).
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The Lyman-α radiation lamp operates with a constant flow of argon and hydrogen
5 (mixing ratio 99/1) and maintains a constant emission by RF-excited discharge (details
in Zöger et al., 1999). FISH review
As the lamp is not monochromatic, the number of lamp background counts also
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J. Meyer et al.
have to be taken into account. Therefore a swiveling mirror is implemented between
Discussion Paper
the lamp and the measuring cell. During one measuring cycle the mirror is placed in
10 three different positions to determine the total fluorescence rate Ng (mirror position 1),
Title Page
the background rate Nu (mirror position 3) and the lamp intensity I0 (mirror position 2).
I0 has to be recorded because the Lyman-α intensity depends on the pressure in Abstract Introduction
the cell due to a changing number of absorbing oxygen molecules and higher atmo-
Conclusions References
spheric H2 O concentrations in the light path. This recording avoids any influence of
15 lamp intensity changes, e.g. by aging of the MgF2 -window which is placed between the Tables Figures
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Lyman-α source and the measuring cell, on the water vapor measurement. The water
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vapor mixing ratio can now directly be determined using the so called FISH equation: J I
Ng − fu · Nu J I
µ = ck · (1)
I0 · Kf Back Close
where fu is a second calibration constant accounting for transmission loss by the mirror Full Screen / Esc
20 during the background measurements (see Sect. 3). The pressure dependent Kf factor
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consider non-radiative transitions of the excited OH into the ground state (for details see Printer-friendly Version
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Zöger et al., 1999). Since FISH measures mixing ratios, this factor is close to 1 at high Interactive Discussion
pressures (∼1000 hPa) and less than 1 at lower pressures (e.g. 0.975 at 100 hPa).
The characteristics of FISH that guarantee a highly accurate measurement of the
25 WVMR µ are (i) the regular recording of I0 and Nu and (ii) frequent calibration with
an automated calibration bench to determine ck and fu , which is described in the next
section.
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3 FISH calibration procedure – an update
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The core of the FISH data evaluation is the calibration of the fluorescence signal. Thus,
FISH is regularly connected to a calibration bench to determine the calibration coeffi- 15, 7735–7782, 2015
cients ck and fu needed to calculate the WVMR (µ) via Eq. (1) (see Sect. 2). The
5 Jülich calibration bench consists of three parts (Fig. 3): a humidifier, a mixing unit to FISH review
mix dry and humid air and a reference water vapor instrument. The current reference
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water vapor instrument is a commercially available MBW Dew Point instrument (model J. Meyer et al.
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K-1806/DP30-SHSX-III, MBW Elektronik AG, Switzerland, www.mbw.ch), in the fol-
lowing denoted as DP30. The previous reference instrument, a General Eastern type
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10 1311DRX frost point hygrometer, was replaced in 2001. Another version of the MBW
frostpoint hygrometer portfolio, the MBW 373 LX, is currently under evaluation for use Abstract Introduction
as a reference. Inside the DP30, the thickness of a frost layer on a mirror is optically
Conclusions References
monitored and held constant by a heating and cooling system. The temperature of the
mirror is measured and hence the water vapor content can be determined by means Tables Figures
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15 of the water vapor saturation pressure formula. The accuracy of the DP30 is ±0.1 C
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frostpoint and the instrument can measure equilibrium temperatures between −75 and J I
+20 ◦ C at a constant pressure of 2 bar. Today, two DP30 instruments are in use in
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the Jülich laboratories in order to detect potential drifts of individual instruments. The
accuracy of the reference instruments will be discussed in Sect. 4.1. Back Close
20 Via the mixing unit, different humidity levels can be generated during a calibration
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cycle. Standard calibrations cover humidity levels between 1 and several 100 ppmv
relevant for the UT/LS. In addition, the pressure within the FISH measuring cell can be
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adjusted independently to account for variable conditions.
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Interactive Discussion
3.1 FISH calibration
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ter a maximum of two flights, ideally after each flight. Since in the field the supply with
dry air is often limited, the calibrations are performed at low flow rates of about 5 stan- ACPD
dard liter per minute (slm) to minimize the amount of dry air per calibration. Deviations
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of the FISH WVMR caused by the low flow rate can be accounted for (discussed later
5 in Sect. 3.2), but do not occur during flight conditions where the typical flow rates at
altitudes between 500 and 80 hPa range from 30 to 10 slm. With a cell volume of 0.3 L, FISH review
the exchange time for air in the cell is 0.3 to 0.15 s, respectively.
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Figure 4 displays a FISH calibration run, both in linear scaling to highlight the high
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WVMR range, and in logarithmic scaling to visualize the lower WVMR. The blue line
10 shows the DP30 signal illustrating the six chosen WVMR steps, while the black line
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represents the cell pressure variations. The red line denotes the FISH signal, using
coefficients ck = 0.00209 and fu = 3.47 derived from this particular calibration run. The Abstract Introduction
calibrations factors are determined by rearranging Eq. (1) to:
Conclusions References
1 Nu Ng Tables Figures
+ · fu =
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, (2)
ck I0 · µDP30 I0 · µDP30
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15 and then applying a linear fit where the y intercept (first term) is the inverse of ck and
fu is the slope of the line. J I
The WVMR of FISH and DP30 show a very good agreement for most of the cali- Back Close
bration conditions, except for the lowest and highest mixing ratios steps. Here, a de-
pendence of the WVMR on the cell pressure can be seen (see Fig. 4), which is not Full Screen / Esc
20 considered in the linear FISH calibration (Eq. 1), and thus points to some deviations
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from the idealized measurement principle described above. Printer-friendly Version
Discussion Paper
In the low humidity range, the measured water content decreases for the highest Interactive Discussion
pressure levels, while for the high humidity range the pressure behavior is reversed, i.e.
the measured water vapor amount increases with increasing pressure in the FISH mea-
25 suring cell. This effect also becomes obvious during experiments at the AIDA cham-
ber, where experiments under atmospherically atypical conditions (low WVMR/high
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pressure, high WVMR/low pressure) were performed, e.g. during the AquaVIT-1 and
AquaVIT-2 campaigns in 2007 and 2013 (see Sect. 5.2). ACPD
3.2 Extended FISH calibration evaluation 15, 7735–7782, 2015
For low humidities and low flow rates, the relative contribution of additional water FISH review
5 sources in the FISH system may become important. Although leakages are carefully
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avoided in the FISH measuring system, outgassing of small amounts of water from J. Meyer et al.
surfaces inside the FISH flow system cannot be completely suppressed under such
Discussion Paper
conditions. This effect becomes increasingly important the lower the flow rate through
the cell is and the smaller the amount of water vapor in the sample flow. As outgassing Title Page
10 is mainly controlled by the water vapor partial pressure difference between the gas flow Abstract Introduction
and the adsorbed water on the wall surface, the water content added from the walls de-
creases with increasing cell pressure P (see Fig. 4b) up to the equilibrium pressure Peq. Conclusions References
where the partial pressure difference vanish. Tables Figures
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One way to minimize the effect of outgassing on low water vapor contents is to keep
Discussion Paper
15 the air flow through the FISH measuring cell above 10 slm, which is always the case J I
for airborne FISH measurements in the inlet forward mode (see Sect. 2). For lower flow
rates, as used for laboratory experiments, the effect can be accounted for including an J I
additional calibration factor Xw and a pressure and flow dependent term to Eq. (1) as Back Close
follows:
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Ng − fu · Nu (Peq. − P ) · I0
20 µ = ck · − ck · X w · (3)
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I0 flow Printer-friendly Version
Discussion Paper
Applying this modification to the FISH equation results in a constant fu factor of 1.1 to Interactive Discussion
1.2 for different calibration runs, which is close to the theoretical value of 1.15. When
using Eq. (2) to calculate fu , it ranges between 1.2–4, since the slope is very sensitive
to variations in low humidity steps (high Nu /(I0 · µDP30 ) values).
25 Figure 5 (top panel) shows the effect of Eq. (1) (red curve) vs. Eq. (3) (green curve)
on the calculated WVMR for the same calibration as shown in Fig. 4. It can be clearly
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seen that using Eq. (3) results in a better agreement between FISH and DP30 (blue
curve). ACPD
For high humidities, the response time of the detector system limits the functional-
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ity of FISH. In general, the intensity of the generated fluorescence radiation increases
5 with increasing water vapor content. Thus the time between subsequent counts de-
tected by the photomultiplier PMT becomes shorter with a higher amount of water FISH review
vapor molecules in the air. As the PMT sensor and the electronics needs a certain time
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to process the signal produced by one fluorescence photon, additional photons will not
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be processed and thus not counted in this so called dead time. The dead time of the
10 PMT sensor system and the processing electronics was experimentally determined to
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be DT = 370 ns.
The PMT count rate, Ng , is higher at lower pressures due to less absorption of the Abstract Introduction
Lyman-α by oxygen. The loss of counts due to the detector dead time is thus much
Conclusions References
more pronounced at lower pressures in the FISH measuring cell under high humidity
15 conditions (atypical for the atmosphere). As the water vapor content measured dur- Tables Figures
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ing operation on aircraft as well as the atmospheric pressure in the UT/LS are usually
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low, this effect on the airborne FISH measurements is negligible. For laboratory ex- J I
periments, however, the impact of the detector dead time on the measured count rate
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Ng,meas , can be corrected by assuming a Poisson process for incoming photons:
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Ng,meas
20 Ng,true = . (4) Full Screen / Esc
1 − Ng,meas · DT
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Figure 5 (bottom panel) displays the highest WVMR level from the same calibration Printer-friendly Version
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run as in Fig. 4 except that using Eqs. (3) and (4) instead of Eq. (1). As expected, the Interactive Discussion
modified FISH calibration evaluation (green line) levels out the dependence of WVMR
on the cell pressure and therefore decreases the FISH uncertainty for high WVMR and
25 low cell pressure considerably. The calibration factor ck changes very little due to the
detector dead time correction (ck = 0.00194 compared to ck = 0.00209), whereas fu
is shifted from 3.47 down to 1.22, which is close to the theoretical value of 1.15. This
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calibration run demonstrates an extreme example of the outgassing effect, usually the
variations of fu are smaller. ACPD
We checked all FISH datasets susceptible to changes when applying the modified
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FISH calibration evaluation. For atmospheric WVMR and pressure ranges, FISH data
5 remain unchanged. Only during measurements at the AIDA chamber (see Sect. 5.2,
Fig. 11) where experiments with high WVMR at low pressures and low WVMR at high FISH review
pressures were performed, does the modified calibration equation become important.
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4 Data quality of FISH measurements – a survey
Title Page
During a measurement period, a crucial factor for accurate water vapor measurements
Abstract Introduction
10 with FISH, besides correct determination of the calibration coefficients, is the stability
of the lamp and detector in between calibrations. Also, the calibration reference DP30 Conclusions References
is crucial to the quality of the FISH water vapor measurements. Thus, a comprehensive
Tables Figures
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check of the DP30 accuracy and precision (Sect. 4.1), the reproducibility of the FISH
calibration (Sect. 4.2) as well as the resulting FISH measurement uncertainty is
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J I
15 given here. In Sect. 4.4 a new quality check procedure for high WMR in cirrus at
high pressures (400–500 hPa), unfavorable conditions for the Lyman-α technique, is J I
presented.
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The accuracy and precision of the DP30 is reviewed by three independent tests. Firstly,
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20
the Jülich DP30 instruments are sent to the manufacturer from time to time to be re- Interactive Discussion
calibrated against another reference frostpoint hygrometer. This reference instrument is
traceable to a British primary standard at the National Physical Laboratory (NPL). The
result of one such comparison, performed in August 2007, is shown in Fig. 6a (purple
25 squares). For frostpoint temperatures between −60 and −40 ◦ C, the differences were
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negligible, i.e. below ±0.1 ◦ C. But, for the lowest temperature measurement at −77.8 ◦ C
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the deviation between the DP30 and the reference instrument was −2.97 ◦ C which ACPD
corresponds to a difference of about 60 % in water vapor mixing ratio. However, the
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validity of this data point is questionable as such a deviation could not be reproduced
5 by any other procedure thus the data point is be ignored in the further discussion.
A second check was performed by connecting both DP30 instruments to the Jülich FISH review
calibration bench and by operating them in parallel at different frostpoints. Fig. 6a (light
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blue dots and blue triangles) displays the comparisons carried out on 12 Septem-
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ber 2007 and on 7. November 2007, respectively. For both measurements the sec-
◦
10 ond DP30 shows the tendency to measure about 0.1–0.4 C lower frostpoint temper-
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atures than the DP30 that was sent to MBW. No major variability could be observed.
As a consequence, the first DP30 is used for standard calibrations, and the frostpoint Abstract Introduction
temperatures of the second DP30 are corrected for this constant offset. Conclusions References
For the third test, a permeation source was provided by the Physikalisch
Technische Bundesanstalt (PTB), the German institute for metrology. This Tables Figures
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coulometric standard (http://www.ptb.de/cms/fachabteilungen/abt3/fb-32/ag-321/ J I
sicherung-und-rueckfuehrung-von-gasfeuchtemessungen.html). The principle of the J I
secondary standard is based on permeation of water through a solid material due to
20 concentration differences. The permeability is influenced by the size and thickness of Back Close
the membrane as well as the surrounding temperature and pressure. In this case the Full Screen / Esc
membrane was a PTFE tube embedded in a water filled metal cylinder which then was
placed in a water bath. Thus for each experiment the temperature was held constant
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while the flow through the tube was varied to adjust the water vapor mixing ratio. The
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25 water vapor mixing ratio is calculated using Eq. (5). The coefficients a, b, c and d Interactive Discussion
were determined via a calibration to the PTB primary standards.
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Dry synthetic air is further dried by a Hydrosorb cartridge (molecular sieve, drying the
air to less than 20 ppbv) and then sent to the permeation source. After passing through ACPD
the permeation source, the air, now having a well defined water vapor mixing ratio, is
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delivered to the DP30 for calibration. A crucial parameter to calculate the source WVMR
5 is the flow through the permeation source which is set by a mass flow controller. This
flow controller was calibrated against a soap film flowmeter and found to depend on FISH review
the pressure at its inputn (pre-pressure).
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Fig. 6b (black triangles, measurement condition with pressure between 2–2.5 bar)
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displays the deviation in water vapor mixing ratio of the DP30 measurement to the
10 permeation source for different humidity levels. This deviation lies between −2 and
Title Page
+2 %. The light and dark gray squares show how much the WVMR is affected if the pre-
pressure is varied by a few tens of bar without considering the pressure-dependence of Abstract Introduction
the flow. This depict the lower and upper uncertainty of the permeation source. Thus,
Conclusions References
we estimate the uncertainty in WVMR to about 4 % for this calibration setup due to the
15 pressure dependence of the flow. Tables Figures
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For converting frostpoint temperatures measured by the DP30 into the correspond-
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ing WVMR, the equation to convert frostpoint temperature into saturation pressure by J I
Sonntag et al. (1994) and the equation to convert saturation pressure into water va-
J I
por mixing ratio (Wallace et. al., 1976) are applied by default. A detailed discussion
20 about different equilibrium approximations including a complex numerical solution for Back Close
the thermodynamic equilibrium situation can be found in Murphy and Koop (2005). In
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Fig. 6b these different approximations all describing the equilibrium saturation pressure
are plotted (stars) for one water vapor mixing ratio. A difference of about 3 % between
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the extreme estimates is apparent, with the Sonntag approximation used for the DP30
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25 falling into a range of 1 % width where most of the estimates and especially the param- Interactive Discussion
eterization according to Murphy and Koop (2005) are centered. The conversion of the
DP30 WVMR via the Sonntag equation therefore results in a maximum error of 1 %.
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Figure 6c shows the combined results of all three methods. Summarizing the uncer-
tainties, the previously estimated DP30 accuracy of 2–4 % is well reproduced with the ACPD
comparison to the permeation source and all other tests described above.
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4.2 Reproducibility of FISH calibration
FISH review
5 Calibrations are normally performed after each flight or in regular intervals of a few
|
days in order to detect potential drifts of the instrument sensitivity. Major changes of J. Meyer et al.
the calibration factors occur only when modifications e.g. replacement of a detector,
Discussion Paper
the MgF2 window or the mirror have been performed. For aircraft experiments, the
calibration factors show only a very weak trend, which may be caused by dirtying of Title Page
10 the cell and optical components. For clean chamber experiments as AquaVIT-1 and Abstract Introduction
2, the calibration factors do not show an obvious trend (see Fig. 7). Thus, frequent
calibrations, e.g. as during AquaVIT-1, can be used to test the reproducibility of the Conclusions References
calibration and to increase their statistical significance. The SD of ck from the mean Tables Figures
|
commonly is ±1.5 %, and that of fu is ±2 %. Older measurements before AquaVIT-1 in
Discussion Paper
15 2007 have a larger uncertainty of fu around ±20 % due to neglecting the outgassing J I
effect described in Sect. 3. These numbers can be used as a measure of the reliability
of the calibration coefficients determination, not including the systematic uncertainties J I
of the reference instrument (Sect. 4.1). Including the extended calibration procedure Back Close
described in the previous section does not significantly influence the stability of the
20 calibration constants during a measurement period (not shown here). Full Screen / Esc
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4.3 FISH uncertainty Printer-friendly Version
Discussion Paper
Interactive Discussion
Assuming high flow aircraft conditions, the uncertainty of the WVMR is determined by
propagation of the uncertainties in ck and fu in Eq. (1):
fu · Nu
dµ/µ = dck /ck + · dfu /fu (6)
Ng − fu · Nu
7749
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The measurement uncertainties of the count rates (Ng and Nu ) as well as the intensity
I0 are relatively small and, compared to the uncertainties in the calibration factors, neg- ACPD
ligible. The uncertainty in fu mainly impacts the low WVMR range when Ng becomes
15, 7735–7782, 2015
the same order of magnitude as Nu . As an example, for a WVMR of 1.2 ppmv (the low-
5 est WVMR we ever measured in the atmosphere; Schiller et al., 2009) typical values
of Ng and Nu are 2500 and 500, respectively. With fu = 1.2 an uncertainty dfu /fu = 2 % FISH review
results in an additional uncertainty of the WVMR of 1 % (second addend in Eq. 6). As
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J. Meyer et al.
described above, FISH data prior to 2007, and especially 2001, should be considered
Discussion Paper
with a higher uncertainty of the low WVMR of 5 % in the light of our current procedures.
10 For higher WVMR, the second addend becomes negligible and dµ/µ is determined
Title Page
primarily by the uncertainty of ck .
To determine the overall measurement uncertainty, we have to add the different con- Abstract Introduction
tributions from Sects. 4.1 to 4.3. For typical operational conditions, the combined total
Conclusions References
accuracy is 6–8 % (6–10 % before 2007 and 2001), mostly dependent on the stabil-
15 ity of the continuous calibrations during the measurement campaign. This value was Tables Figures
|
already reported by Zöger et al. (1999), but here we provide new evidence based on
Discussion Paper
more accurate reference instruments and calibration procedure. In particular for low J I
WVMR, we further have to consider the noise or detection limit which is on the order of
J I
0.15–0.40 ppmv depending on instrument performance. Thus:
Back Close
20 uncertainty = accuracy + detection limit (7)
Full Screen / Esc
In summary, for mixing ratios of 1–4 ppmv, an absolute uncertainty of 0.3 ppmv is
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a good first-order approximation for our measurements in the lower stratosphere, or Printer-friendly Version
Discussion Paper
30 to 8 % in relative terms over this range. From 4–1000 ppmv, an accuracy of 6–8 % Interactive Discussion
is usually achieved. Around 1000 ppmv, further non-linear effects determine the up-
25 per limit of the dynamical measurement range of FISH (see also next section). Due
to increasing pressure or water vapor content, the measuring cell becomes optically
thick, i.e. the Lyman-α radiation is stronger absorbed by molecular oxygen and wa-
ter vapor and therefore is no longer sufficient to illuminate the measurement volume.
7750
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Discussion Paper
Thus, FISH is not operated at pressures above 500 hPa. For specific operation condi-
tions e.g. chamber experiments, we have to apply the flow, pressure and water vapor ACPD
content dependent correction described previously (see Sect. 3).
15, 7735–7782, 2015
4.4 Quality check procedure for high WVMRs
FISH review
5 FISH measures total water (gas phase + evaporated ice) by means of a forward looking
|
inlet (see Sect. 2). In thick cirrus clouds at lower UT altitudes, i.e. at higher pressures J. Meyer et al.
(above 400 hPa) and temperatures (above 220 K), high total WMR close to or more than
Discussion Paper
1000 ppmv can occur. Such conditions are unfavorable for the Lyman-α fluorescence
technique since they lead to an increase of the optical thickness in the measuring cell Title Page
10 and reveal the upper detection limit of FISH (see Sect. 4.2). Thus, these high H2 Otot in Abstract Introduction
thick cirrus have to be carefully checked and rejected if the measurement is found to
be not valid. Conclusions References
The extended high WVMR evaluation and the development of a rejection algorithm Tables Figures
|
for invalid measurements is described in the following. From the calibrations, a relation
Discussion Paper
15 for the fluorescence count rate Ng , depending on pressure and the normalized inversed J I
I0 (max(I0 )/I0 = I0∗ ) can be derived. Figure 8a shows the relation for one calibration. The
WVMRs (blue dots), different combinations of I0∗ and Ng , increases along the lines of J I
∗
specific pressure levels (black lines). The reason for using I0 is to clearly distinct the Back Close
high WVMR at different pressure levels. From the calculated it function (black lines),
∗ Full Screen / Esc
20 depending only on I0 and pressure, corresponding Ng along one pressure level can
be calculated. Thus, it is possible to derive a theoretical count rate (Ng,calc ) from the I0
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intensity measurement and the corresponding cell pressure for measurement flights. Printer-friendly Version
Discussion Paper
When the measuring cell becomes optically thick due to high pressure and/or high Interactive Discussion
WVMR, the measured Ng no longer fits the measured lamp intensity I0 .
25 Figure 8b shows the time series of a flight during the ML-Cirrus campaign. If the
measured count rate Ng (green) deviates more than 30 % from Ng,calc (black), we de-
fine a mismatch of I0 and Ng and reject the data point (H2 O out, red). The first increase
of WVMR, caused by a cirrus cloud at 12:55:05 to 12:55:20 UTC, looks correct if con-
7751
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Discussion Paper
sidering only the WVMR. However, Ng and the WVMR are already too low for the
detected I0 . That means the measurement cell has started to become optically thick ACPD
and the corresponding WVMRs have to be rejected. The second cloud in Fig. 8b at
15, 7735–7782, 2015
12:55:40 to 12:55:50 UTC, caused an enhanced optical thickness of the cell (very low
5 Ng compared to I0 ), which resulted in decreased instead of increased WVMR. Thus,
these values are also rejected. However, the enhanced values to the right of this cloud FISH review
correspond to a thinner cirrus which can be detected with FISH.
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J. Meyer et al.
From the extended high WVMR evaluation it follows that the upper detection limit of
Discussion Paper
FISH is not clearly defined. A first estimate for the upper detection limit is 1000 ppmv.
10 For thick cirrus at pressures below 300 hPa the WVMRs no data has to be rejected.
Title Page
However, at pressures above 300 hPa the amount of rejected data increases with pres-
sure; this varies with the type of observed cirrus. This behavior was first observed Abstract Introduction
during MACPEX in 2011, where very dense and thick cirrus were observed. However,
Conclusions References
the cirrus measurements in previous campaigns, published in Schiller et al. (2008) and
15 Krämer et al. (2009), were observed either at higher altitudes (lower pressures) or with Tables Figures
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distinct lower total WMRs and are therefore not considered to be invalid measurements.
Discussion Paper
J I
Back Close
High accuracy and measurement stability in a laboratory environment does not neces-
sarily imply the same performance in the field. Especially for in-situ water vapor mea- Full Screen / Esc
20 surements on board of aircraft and balloons, operation and sampling conditions poten-
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tially influence the measurements. One way to cross-check the in-flight performance Printer-friendly Version
Discussion Paper
is to compare the FISH measurements to other spatially and temporally collocated in-
Interactive Discussion
situ or satellite-based water vapor measurements. Since water vapor measurements
are valuable for a wide variety of research in the UT/LS region, other hygrometers
25 were often operated in parallel to FISH, which provided opportunities for instrument
intercomparisons (see Table 1). In addition, FISH participated in a number of projects
where flight patterns and aircraft instrumentation were specifically designed to allow in-
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Discussion Paper
strument intercomparisons and instrument performance tests. FISH also participated in
systematic tests of the instrumentation in the laboratory such as the AIDA cloud cham- ACPD
ber, where various measurement conditions including clouds can be simulated (Fahey
15, 7735–7782, 2015
et al., 2014). Note that such comparisons are not absolute proof for the high accu-
5 racy of FISH but nevertheless strengthen the confidence in the FISH performance. An
overview of all campaigns allowing comparisons of FISH to other hygrometers is given FISH review
in Table 1 and a list of all instruments compared with FISH can be found in Table 2.
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J. Meyer et al.
Discussion Paper
5.1 In-flight performance and aircraft intercomparisons
During multiple FISH research flights, a number of possibilities arose to compare the Title Page
10 FISH performance to other hygrometers measuring UT/LS water vapor (see Tables 1– Abstract Introduction
3). This set of comparisons includes flights where other in-situ hygrometers were flown
spatially and temporally coincident with FISH but not on the same platform. Such a set Conclusions References
of comparisons dating back to the early FISH operation period before 2000 is men- Tables Figures
|
tioned in Kley et al. (2000) where it was found that the FISH measurements, the frost-
Discussion Paper
15 point hygrometer LMD and the capacitive sensor MOZAIC agreed within 10 % in rel- J I
ative humidity (RH). FISH water vapor measurements during THESEO and SOLVE 1
also matched with those of the high precision Harvard Lyman-α hygrometer HWV, the J I
Jet Propulsion Laboratory (JPL) laser hygrometer JLH and the frostpoint hygrometer Back Close
NOAA-CMDL within 1 ppmv, although a systematic low offset with respect to JLH and
20 a systematic high offset with respect to NOAA-CMDL was observed. Full Screen / Esc
The most extensive dataset for in-situ comparison however, was obtained on board
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the high-altitude aircraft Geophysica, where both the FISH total water instrument and Printer-friendly Version
Discussion Paper
the FLASH Lyman-α hygrometer (Sitnikov et al., 2007) flew. The relative difference Interactive Discussion
of the two instruments is of specific interest as the combination of FISH and FLASH
25 measurements is used to derive the ice water content IWC (Schiller et al., 2008) and
relative humidity inside and outside of clouds (Krämer et al., 2009). Thus, a review
1
note here that all abbreviations of campaigns and instruments are listed in Tables 1 and 2.
7753
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of all flights in clear sky conditions, indicated by relative humidities lower than 80 %, is
summarized in Fig. 9 (see also Tables 1–3). The graph shows the percentage difference ACPD
in clear sky water vapor content in dependence on the flight pressure level. The colors
15, 7735–7782, 2015
indicate the frequency of occurrence of the deviations for the entire data set. Although
5 FISH and FLASH differ by up to 100 % in extreme cases, values smaller than 30 % are
most frequent. There seems to be no systematic offset between the two instruments. FISH review
A slight trend of FISH measuring slightly higher values in high pressure areas might be
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J. Meyer et al.
due to imperfect rejection of cloudy airmasses. Otherwise, no correlation of the relative
Discussion Paper
difference between the two instruments to other atmospheric variables (such as relative
10 humidity or temperature) were found.
Title Page
Beyond research flights, the MACPEX campaign with the NASA WB-57 research air-
craft (Rollins et al., 2014) provided an opportunity for an intensive in-situ hygrometer in- Abstract Introduction
tercomparison. Within the combined instrument uncertainties, FISH measured slightly
Conclusions References
drier water vapor content (≈ 10–20 % or ≈ 0.6 ppmv below 10 ppmv) in comparison to
15 most of the other instruments including HWV and the NOAA Chemical Ionization Mass Tables Figures
|
Spectrometer (CIMS) with in-flight calibration (Rollins et al., 2014). The slight dry bias
Discussion Paper
of FISH with respect to HWV and CIMS during MACPEX was consistently observed, J I
even when applying the newly developed FISH calibration scheme described in detail
J I
in Sect. 3.2. However, both frostpoint hygrometers (FPH and CFH) operated on a bal-
20 loon during MACPEX agreed quite well with the FISH (≈ 1 % or ≈ 0.05 ppmv at the Back Close
4 ppmv level) (Rollins et al., 2014). The reason for the difference between the frostpoint
Full Screen / Esc
based instruments (FPH, CFH and also FISH) and the other instruments aboard the
WB-57 (e.g. CIMS, HWV, DLH) remains unclear.
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Printer-friendly Version
On board the new German research aircraft HALO, FISH was operated in 2012 side
Discussion Paper
25 by side with the new hygrometer HAI (Buchholz, 2014) during the combined campaigns Interactive Discussion
TACTS (Engel et al., 2013) and ESMVal (Schlager et al., 2014). In the lower range
from 4 ppmv down to 1.6 ppmv HAI reveals a fairly good mean relative deviation (MRD)
between −14.9 and −5.9 % during a flight in the antarctic vortex (for details see Rolf
et al., 2015).
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Another systematic in-situ hygrometer intercomparison was embedded in the Air-
toss campaign, which took place in 2013 on-board of a Learjet. The intercomparison ACPD
was part of the Eufar DENCHAR project (Smit et al., 2014). This project is dedicated
15, 7735–7782, 2015
to the development, testing and comparison of new, compact instruments measuring
5 WVMR above 10 ppmv. In the top panel of Fig. 10 we show a comparison between
FISH and the photoacoustic instrument WASUL (red dots, details in Tátrai et al., 2014). FISH review
A generally good agreement of about −13.3 % for WMVR up to 1000 ppmv was found
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J. Meyer et al.
for WASUL. During the ML-Cirrus mission with the HALO aircraft the TDL hygrometer
Discussion Paper
SHARC measured gas-phase MR parallel to the total water measurements of FISH. In
10 the bottom panel of Fig. 10 SHARC and FISH measurements outside of clouds from
Title Page
one flight (13 April 2014) are shown and reveal a very good agreement (MRD) of below
−3.7 % ranging from 10 to 600 ppmv. Abstract Introduction
In general, the in-situ aircraft intercomparisons are within their combined instrument
Conclusions References
uncertainties.
Tables Figures
|
15 5.2 Laboratory intercomparisons
Discussion Paper
J I
Starting in 2007, FISH participated in two laboratory intercomparison experiments:
AquaVIT-1 (Fahey et al., 2014) and AquaVIT-2. In this context, the instruments were J I
systematically tested under simulated natural operation conditions, but also extreme Back Close
environmental and water vapor settings were addressed. HWV, FLASH, APicT, WA-
20 SUL, CFH (a modification of the NOAA FPH) and JLH were part of AquaVIT-1, while Full Screen / Esc
APicT, HAI, WASUL and the NOAA-TDL participated in AquaVIT-2 (more information
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on the instruments is given in Tables 1–2). Printer-friendly Version
Discussion Paper
In comparison to the systematic and non-systematic airborne intercomparisons Interactive Discussion
shown in the previous section, the deviations of water vapor observed by the instru-
25 ments HWV, FLASH, APicT, CFH and JLH to FISH were generally smaller during the
AquaVIT-1 static intercomparison periods (see Table 3). For the laboratory experiments
in the 10 to 150 ppmv range, Fahey et al. (2014) report variations in measured water
vapor content of about ±10 % around a mean value which was derived from the core
7755
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Discussion Paper
subset of the participating instruments due to the lack of an appropriate reference in-
strument. Thus, the deviations between FISH and the other hygrometers mostly fell ACPD
within the combined instrument uncertainties for that water vapor range. Fahey et al.
15, 7735–7782, 2015
(2014) also found a “fair” agreement of ±20 % for water vapor contents between 1 to
5 10 ppmv, slightly larger than the combined uncertainties of the instruments. However,
below 1 ppmv H2 O, the percentage difference of measured water vapor detected by FISH review
the different instruments increased (Fahey et al., 2014). The value of these sub 1 ppmv
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J. Meyer et al.
AIDA measurements is of questionable value when considering the atmospheric mea-
Discussion Paper
surements, since mixing ratios this low at the high pressures used in AIDA never occur
10 in the atmosphere, and as such is outside the design parameters of the in situ instru-
Title Page
mentation.
As an example of the systematic intercomparison experiments during AquaVIT-1, Abstract Introduction
Fig. 11 shows two time series of water vapor measurements made with the instruments
Conclusions References
listed above. FISH measurements are displayed twice, first using the standard calibra-
15 tion Eq. (1), and second applying the extended calibration Eqs. (3) and (4) described Tables Figures
|
in Sect. 3.2.
Discussion Paper
The upper panel in Fig. 11 shows a time series for mixing ratios up to 150 ppmv, J I
where the largest discrepancies occur at the highest mixing ratios and low chamber
J I
pressure. Here, the extended calibration equations increases FISH (light purple) by
20 about 6 % (dark purple) and shifts it closer to the AIDA hygrometer APicT. This hygrom- Back Close
eter, though not used as an absolute standard during AquaVIT-1, provided data closest
Full Screen / Esc
to the mean of all core instruments for almost all water vapor ranges (Fahey et al.,
2014). Thus, the relative differences of FISH to the other hygrometers for high mixing
|
Printer-friendly Version
ratios becomes similar as for other AquaVIT-1 water vapor ranges, i.e. 1–10 ppmv.
Discussion Paper
25 For the mixing ratio range below 1 ppmv, the bottom panel of Fig. 11 shows how Interactive Discussion
the FISH data are corrected for outgassing, again shifting FISH by 10–15 % and thus
closer to APicT. Hence, part of the FISH data points in the AquaVIT experiment shown
in Fahey et al. (2014), in particular those for the lowest mixing ratios below 1 ppmv and
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Discussion Paper
those at highest mixing ratios are revised, leading to an agreements of about 10 % with
the other hygrometers, which is consistent with those obtained in the 1–20 ppmv range. ACPD
The extended calibration evaluation scheme is also applied to the FISH data col-
15, 7735–7782, 2015
lected during AquaVIT-2 in 2013. Here, the mean relative deviation (MRD) between
5 FISH, the reference instrument APicT and the NOAA-TDL is between −2.4 to 0.7 %
in the range of 7 up to 20 ppmv and even better between −0.9 to 1.6 % in the upper FISH review
range from 20 to 600 ppmv (see Fig. 12 and Table 3). Altogether, the generally better
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J. Meyer et al.
agreement of FISH during laboratory intercomparisons using the extended calibration
Discussion Paper
evaluation scheme is demonstrated from Figs. 11 and 12.
Title Page
10 5.3 Satellite intercomparisons: FISH – Aura MLS
Abstract Introduction
Water vapor in the UT/LS region is not only measured by in-situ instrumentation on
board of aircraft and balloons but is also monitored by satellite based instruments. In Conclusions References
the past, whenever possible, FISH measurements were readily taken to validate these Tables Figures
|
satellite based hygrometers (Thomason et al., 1994; Kanzawa et al., 2002; Offermann
Discussion Paper
15 et al., 2002; Lumpe et al., 2006; Kiemle et al., 2008; Müller et al., 2008; Milz et al., J I
2009; Wetzel et al., 2013).
Figure 13 exemplarily demonstrates the comparison of the Microwave Limb Sounder J I
(MLS) (Lambert et al., 2007; Read et al., 2007) installed on the NASA Aura satellite Back Close
with respect to the FISH instrument. For the comparison, all MLS measurements within
20 12 h, 5◦ latitude, and 2◦ longitude from a FISH vertical profile flight location during the Full Screen / Esc
Troccinox, Amma, Scout, Reconcile and MACPEX (see Table 1) were considered. Be-
|
cause of for the MLS averaging kernel, the analysis is limited to the lower stratosphere, Printer-friendly Version
Discussion Paper
at the standard MLS level of 82 hPa and all FISH vertical flight profiles in that region. Interactive Discussion
For each campaign, a mean value and a SD of the difference is calculated from all com-
25 parable FISH–MLS profiles (see Fig. 13). Differences are between ±2 ppmv for the low
water vapor contents in the stratosphere (typically smaller than 10 ppmv). The mean
differences FISH-MLS for the different campaigns range from −0.2 and −0.5 ppmv –
with MLS having slightly higher values – and are therefore smaller than 10 % at the
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Discussion Paper
4 ppmv stratospheric level. An exception is the Reconcile campaign, where MLS has
a larger deviation with moister values of about 0.7 ppmv compared to FISH. This slightly ACPD
higher values observed for flights taking place at higher latitudes during the Reconcile
15, 7735–7782, 2015
campaign appear to be a MLS retrieval artifact (S. Davis, personal communication,
5 2014). Similar deviations of −0.2 to 0.7 ppmv are found for all campaigns by using the
100 hPa MLS level instead of the 82 hPa level. Overall, Fig. 13 impressively demon- FISH review
strates the excellent agreement between FISH and MLS water vapor measurements
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J. Meyer et al.
on a long-term basis between 2005 and 2011.
Discussion Paper
6 Summary Title Page
Abstract Introduction
10 Since 1996, the Lyman-α fluorescence hygrometer FISH has been deployed on bal-
loons and multiple aircraft platforms, as well as at the AIDA chamber during numer- Conclusions References
ous campaigns. After this long time of operation and using on the large database we
Tables Figures
|
compiled, we have now reassessed the calibration, measurement, and data evaluation
procedures for FISH as well as its performance on aircraft and in the laboratory.
Discussion Paper
J I
15 First, the calibration reference frost point mirror instrument (DP30) was compared to
two different traceable standards (PTB and NPL) confirming a maximum uncertainty J I
of ±4 % for the water mixing ratio. Second, we introduced a modified calibration eval-
Back Close
uation which now also accounts for high WVMRs together with low pressures and low
WVMRs together with high pressures (AIDA chamber conditions), which are typically Full Screen / Esc
20 not encountered by FISH during atmospheric sorties. With the modified calibration eval-
|
uation, the agreement of FISH with the other hygrometers improved for these special Printer-friendly Version
Discussion Paper
conditions from ±20 % @ < 10 ppmv and 10 % @ > 100 ppmv reported by Fahey et al.
Interactive Discussion
(2014) to ±10 % and < 10 %, respectively. Furthermore, a quality check procedure has
been developed that accounts for invalid total water measurements that can occur in
25 thick cirrus clouds at high pressures of about 400–500 hPa.
During the last two decades, FISH had many opportunities to compare with other
in-situ hygrometers, especially since some campaigns were partly dedicated to assess
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the performance of airborne hygrometers, like the MACPEX campaign with the WB-
57 in 2011 (Rollins et al., 2014), Airtoss in 2013 on-board of a Learjet and the AIDA ACPD
intercomparisons AquaVIT-1 in 2007 (Fahey et al., 2014) as well as AquaVIT-2 in 2013.
15, 7735–7782, 2015
An encouraging result of all the intercomparisons is that the agreement between the
5 hygrometers has improved over the years from overall up to ±30 % or more to about
±5–20 % @ < 10 ppmv and to ±0–15 % @ > 10 ppmv. FISH review
In addition to the in-situ intercomparisons, FISH was also compared to the remote
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J. Meyer et al.
sensing instrument MLS on-board the Aura satellite during five airborne campaigns
Discussion Paper
between 2005 and 2011. The agreement between both instruments was found to be
10 better than 10 % at the 4 ppmv level, which can also be seen as a validation of the
Title Page
satellite instrument.
Summing up, the intense review of the FISH calibration technique and its validation Abstract Introduction
against traceable reference water standards as well as laboratory, in-flight and remote
Conclusions References
sensing instrumentation overall increased our confidence in the FISH ability to precisely
15 and reliably measure water vapor in the UT/LS region of the atmosphere. Tables Figures
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Discussion Paper
J I
Dedication to Dr. Cornelius Schiller
J I
This work is dedicated to our highly appreciated and valued colleague and mentor Dr.
Back Close
Cornelius Schiller. Without him, this work, and especially the instrumentation described
here, would not have reached its high level of quality. He devoted all his efforts towards Full Screen / Esc
20 improving the FISH (see Fig. 1) instrument making it one of the leading instruments
|
for measuring low water vapor contents in the stratosphere. His efforts contributed to Printer-friendly Version
Discussion Paper
develop a better understanding of the transport mechanisms and changes of water
Interactive Discussion
vapor in the UT/LS. With his death, we lost not only a treasured colleague and friend,
but a also mentor and a paragon in the instrumental community.
25 Acknowledgements. We are grateful for the support of the technical staff at the AIDA facility
and especially that of Tomasz Chudy, Georg Scheurig and Steffen Vogt during the AQUAVIT
campaigns. Special thanks also to MBW Elektronik AG, Switzerland, who always carefully
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serviced our reference frostpoint hygrometers DP30 and who included regular comparisons of
the instruments to a traceable reference water standard into the routine. Finally, we thank all ACPD
the coordinators of the different field and intercomparison campaigns.
15, 7735–7782, 2015
5 The article processing charges for this open-access publication have been covered
by a Research Centre of the Helmholtz Association.
FISH review
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J. Meyer et al.
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Smith, J. B., Spelten, N., Troy, R. F., Vömel, H., Wagner, S., and Wienhold, F. G.: The
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Helten, M., Smit, H. G. J., Sträter, W., Kley, D., Nedelec, P., Zöger, M., and Busen, R.: Assessing
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30 Schwartz, M. J., Snyder, W. V., Stek, P. C., Su, H., Takacs, L. L., Thurstans, R. P., Vomel, H.,
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25 Hydration and dehydration at the tropical tropopause, Atmos. Chem. Phys., 9, 9647–9660,
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15 lyás, G., and Szabó, G.: Dual-channel photoacoustic hygrometer for airborne measurements: Conclusions References
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20 Chem. Phys., 10, 2159–2173, doi:10.5194/acp-10-2159-2010, 2010. 7757
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Voigt, C., Hall, B., and Fahey, D. W.: Measurement of low-ppm mixing ratios of water vapor in
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25 Thornberry, T. D., Rollins, A. W., Gao, R. S., Watts, L. A., Ciciora, S. J., McLaughlin, R. J.,
Voigt, C., Hall, B., and Fahey, D. W.: Measurement of low-ppm mixing ratios of water vapor in
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the upper troposphere and lower stratosphere using chemical ionization mass spectrometry,
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Vogel, B., Feck, T., and Grooß, J.-U.: Impact of stratospheric water vapor enhancements
30 caused by CH4 and H2O increase on polar ozone loss, J. Geophys. Res., 116, D05301,
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measurements by the cryogenic frost point hygrometer: instrumental details and observa- ACPD
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MAN-MADE pertubations of trace gases, Science, 194, 685–690, 1976. 7738 FISH review
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Siegel, P. H., Cofield, R. E., Filipiak, M. J., Flower, D. A., Holden, J. R., Lau, G. K. K.,
Discussion Paper
10 Livesey, N. J., Manney, G. L., Pumphrey, H. C., Santee, M. L., Wu, D. L., Cuddy, D. T.,
Lay, R. R., Loo, M. S., Perun, V. S., Schwartz, M. J., Stek, P. C., Thurstans, R. P.,
Boyles, M. A., Chandra, K. M., Chavez, M. C., Chen, G. S., Chudasama, B. V., Dodge, R., Title Page
Fuller, R. A., Girard, M. A., Jiang, J. H., Jiang, Y. B., Knosp, B. W., LaBelle, R. C., Lam, J. C.,
Abstract Introduction
Lee, K. A., Miller, D., Oswald, J. E., Patel, N. C., Pukala, D. M., Quintero, O., Scaff, D. M.,
15 Van Snyder, W., Tope, M. C., Wagner, P. A., and Walch, M. J.: The Earth Observing System Conclusions References
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1075–1092, 2006. 7768 Tables Figures
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20 Validation of the Harvard Lyman-α in situ water vapor instrument: implications for the
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Fix, A., Iarlori, M., Kleinert, A., Lengel, A., Milz, M., Mona, L., Müller, S. C., Ovarlez, J., Pap- Full Screen / Esc
25 palardo, G., Piccolo, C., Raspollini, P., Renard, J.-B., Rizi, V., Rohs, S., Schiller, C., Stiller, G.,
Weber, M., and Zhang, G.: Validation of MIPAS-ENVISAT H2 O operational data collected
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between July 2002 and March 2004, Atmos. Chem. Phys., 13, 5791–5811, doi:10.5194/acp-
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13-5791-2013, 2013. 7757 Interactive Discussion
Zöger, M., Afchine, A., Eicke, N., Gerhards, M.-T., Klein, E., McKenna, D. S., Mörschel, U.,
30 Schmidt, U., Tan, V., Tuitjer, F., Woyke, T., and Schiller, C.: Fast in situ stratospheric hygrom-
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Table 1. List of all campaigns where FISH performance is compared to other instruments (list
of instruments see Table 2). ACPD
Campaign Location Flight Dates Instrument Intercomparison
15, 7735–7782, 2015
◦
APE-THESEO 1999 Seychelles, 5 S, Midlatitude 0219, 0304, 0306, 0309 FLASH
THESEO / SOLVE 2000 Kiruna 68◦ N, Arctic 0127 HWV, JPH, NOAA-CMDL
◦
FISH review
Envisat 2002 Forli 44 N, Midlatitude 0713, 0718, 0722, 1008, 1014,1017, FLASH
1022, 1024, 1028
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Euplex 2003 Kiruna 68◦ N, Arctic 0115, 0119, 0123, 0126, 0206, 0208, FLASH
Discussion Paper
0209, 0211
◦
Envisat 2003 Kiruna 68 N, Arctic 0228, 0302, 0308, 0312, 0316 FLASH
◦
Troccinox 2005 Aracatuba, 21 S, Tropics 0127, 0201, 0204, 0208, 0212, 0215, FLASH, AURA-MLS Title Page
0217
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◦
Cirrus-III 2006 Hohn, 54 N, Midlatitude 1124, 1128, 1129 MOZAIC sensor
Discussion Paper
AquaVIT-1 2007 Karlsruhe, 49◦ N cf. Fahey et al. (2014) APicT, CFH, FLASH, HWV, JLH and
other (cf. Fahey et al., 2014) J I
◦
Reconcile 2010 Kiruna 68 N, Arctic 0117, 0122, 0124, 0125, 0128, 0130, FLASH
0202, 0302, 0302 J I
MACPEX 2011 Houston, 29◦ S, Midlatitude cf. Rollins et al. (2014) CIMS, HWV, DLH, CFH and other (cf.
Rollins et al., 2014) Back Close
◦
TACTS/ESMVal 2012 Oberpfaffenhofen, 48 N, Midlatitude 0913 HAI (cf. Rolf et al., 2015)
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Airtoss 2013 (DENCHAR) Hohn, 54◦ N, Midlatitude 0507, 0508, 0829, 0830, 0903, 0904, WASUL, IHD, WVSS2
0905
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AquaVIT-2 2013 Karlsruhe, 49◦ N 0415, 0416, 0417, 0418, 0419 APicT, HWV, NOAA-TDL, WASUL, Printer-friendly Version
CFH, HAI, WVSS2
Discussion Paper
ML-Cirrus 2014 Oberpfaffenhofen, 48◦ N, Midlatitude 0326, 0327, 0329, 0401, 0403, SHARC Interactive Discussion
0404_1, 0404_2, 0407, 0411, 0413
APE-THESEO: Airborne Platform for Earth observation – THird European Stratospheric Experiment on Ozone; SOLVE: SAGE III Ozone Loss and Validation
Experiment; Envisat: Envisat validation campaign; Euplex: EUropean Polar stratospheric cloud and Lee-wave EXperiment; Troccinox: Tropical Convection,
Cirrus, and Nitrogen Oxides Experiment; Marschals: Marschals validation campaign; Scout-O3: Stratospheric-Climate links with emphasis On the Upper
Troposphere and lower stratosphere; Amma: African Monsoon Multidisciplinary Analyses; Cirrus-III: Cirrus 3 campaign; AquaVIT-1: Aqua Validation and
Instrument Tests 1; Reconcile: Reconciliation of essential process parameters for an enhanced predictability of arctic stratospheric ozone loss and its climate
interactions; MACPEX: Mid-latitude Airborne Cirrus Properties Experiment; TACTS/ESMVal: Transport And Composition in the UTLS/Earth System Model
Validation; Airtoss (DENCHAR): Development and Evaluation of Novel Compact Hygrometer for Airborne Research; AquaVIT-2: Aqua Validation and Instrument
Tests 2; ML-Cirrus: Midlatitude Cirrus.
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ACPD
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FISH review
Table 2. List of instruments compared with FISH.
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Discussion Paper
Acronym Instrument technique Platform Reference
1 APicT open path dTDLAS (1.4 µm) AIDA Fahey et al. (2014)
2 CFH frostpoint Balloon, AIDA Vömel et al. (2007) Title Page
3 CIMS chemical ionization mass spectrometer WB-57 Thornberry et al. (2013a)
4 DLH open path TDLAS (1.4 µm, 2f detection) WB-57 Diskin et al. (2002)
Abstract Introduction
5 FLASH Lyman-α Geophysica, AIDA Sitnikov et al. (2007)
6 FPH frostpoint Ballon Hurst et al. (2011)
7 HAI open & closed path dTDLAS (1.4 and 2.6 µm) HALO, AIDA Buchholz (2014) Conclusions References
8 HWV Lyman-α WB-57, AIDA Weinstock et al. (2009)
9 JLH open path TDLAS (1.4 µm, 2f detection) WB-57, AIDA May (1998) Tables Figures
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10 LMD-CNRS frostpoint Ballon, Falcon Ovarlez (1991)
11 MLS microwave limb sounder, satellite EOS Aura Waters et. al. (2006)
Discussion Paper
12 MOZAIC sensor capacitive sensor Falcon, Learjet Helten et al. (1998); Neis et al. (2014)
J I
13 NOAA-CMDL frostpoint Balloon, ER-2 Mastenbrook (1980)
14 NOAA-TDL closed path TDLAS (2.6 µm, 2f detection) Global Hawk, AIDA Thornberry et al. (2013b)
15 SHARC closed path dTDLAS (1.4 µm) HALO – J I
16 WASUL photoacoustic Learjet, AIDA Tátrai et al. (2014)
1: AIDA PCI in-cloud TDL, KIT, Germany; 2: Cryogenic Frostpoint Hygrometer (a modification of the NOAA FPH), NOAA, USA; 3: Chemical Ionization Mass Back Close
Spectrometer, NOAA, USA; 4: Diode Laser Hygrometer, JPL, USA; 5: Fluorescent airborne stratospheric hygrometer, CAO, Russia; 6: Frost Point Hygrometer of the
National Oceanic and Atmospheric Administration, NOAA, USA; 7: Hygrometer for Atmospheric Investigations, PTB/FZJ, Germany; 8: Harvard Water Vapor, Harvard,
USA; 9: Jet Propulsion Laboratory Laser Hygrometer, JPL, USA; 10: Laboratoire de Météorologie Dynamique (LMD) of the Centre National De Recherche Full Screen / Esc
Scientifique, France; 11: Microwave Limb Sounder, JPL, NASA, USA; 12: Measurements of OZone, water vapour, carbon monoxide and nitrogen oxides by in-service
AIrbus airCraft, FZJ, Germany; 13: Climate Monitoring and Diagnostics Laboratory of the National Oceanic and Atmospheric Administration, NOAA, USA; 14: National
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Oceanic and Atmospheric Administration – Tunable Diode Laser; 15: Sophisticated Hygrometer for Atmospheric Research, DLR, Germany; 16: WASUL-Hygro,
Hilase, Hungary. Printer-friendly Version
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Table 3. List of all FISH in-situ comparisons (list of instruments see Table 2).
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Year Instrument Range (ppmv) Agreement (%) Campaign Platform
low high low high Title Page
a
1995 MOZAIC 100–500 10 in RH – Falcon
b Abstract Introduction
1999–2010 FLASH 1–1000 5 30 several Geophysica
2000 HWV, JPH, NOAA-CMDL <10 20 SOLVEc DC-8 and ER-2
2003 MOZAIC 10–600 5 in RH CIRRUS-3d Learjet
Conclusions References
2007 HWV, FLASH, APicT, CFH, JLH <10 10–150 20 (10h ) <10 AquaVIT-1e AIDA
MACPEXf Tables Figures
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2011 CIMS, HWV, DLH <10 10–150 10–20 <7 WB-57
2012 HAI 1.6–4 −14.9–−5.9 TACTS/ESMValg HALO
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2013 WASUL 10–1000 −13.3 Airtoss Learjet
2013 APicT, NOAA-TDL 7–20 20–600 −2.4–0.7 −0.9–1.6 AquaVIT-2 AIDA J I
2014 SHARC 10–1000 −3.7 ML-Cirrus HALO
a
see Helten et al. (1998),
J I
b
see Krämer et al. (2009),
c
see Kley et al. (2000), Back Close
d
see Neis et al. (2014),
e
see Fahey et al. (2014),
f
g
see Rollins et al. (2014), Full Screen / Esc
see Rolf et al. (2015),
h
new extended calibration evaluation
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Title Page
Abstract Introduction
Conclusions References
Tables Figures
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J I
J I
Back Close
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Figure 1. FISH (Fast In-situ Stratospheric Hygrometer) map of 348 aircraft flights. The “fish
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cloud” is in memory of our colleague Cornelius Schiller – see also dedication at the end of the Interactive Discussion
paper.
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Inlet
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Title Page
Outlet Measuring Cell
Abstract Introduction
3
Lyman- α
Conclusions References
2 121.6 nm
Source
H
Tables Figures
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OH
1 *
H2O
*
UVA
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J I
Mirror Detector
MgF2 J I
Detector
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Figure 2. Conceptual diagram illustrating the principal mechanical and optical components of
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the FISH. The size of the cell is 0.3 L in total.
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Reference Hygrometer
MBW K-1806 / DP30
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DEW POINT CONTROL INSTRUMENT
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Mixing Unit
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MFC1
Title Page
Mixed
MFC3 Hygrometer
air Abstract Introduction
FISH
MFC2 Saturated (or other)
Dry Air Air Conclusions References
Pressure
Reducer Tables Figures
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Pressure
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Valve J I
J I
Pump
Back Close
Dry Air
Humidifier
Full Screen / Esc
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Figure 3. This diagram illustrates the principal set-up of the Jülich calibration bench. The col-
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ored path (green, dark and light blue) indicate the air flow through the system. Green and dark Interactive Discussion
blue represent the flow of dry and water saturated air respectively. The user-defined, stable
humidity level generated by mixing the dry and saturated air is colored in light blue.
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Title Page
0 1000
10:00:00 12:00:00 14:00:00 16:00:00 Abstract Introduction
20.05.08 20.05.08 20.05.08 20.05.08
Time (UTC) Conclusions References
b) 1000 10
Tables Figures
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FISH
DP30
FISH:Cell pressure
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100
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100
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10
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10:00:00 12:00:00 14:00:00 16:00:00
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20.05.08 20.05.08 20.05.08 20.05.08
Time (UTC) Interactive Discussion
Figure 4. FISH and DP30 WVMR time series measured with the Jülich calibration bench with
a flow rate of 5 slm: (a) linear scale; (b) logarithmic scale.
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1.5
Abstract Introduction
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10:30 10:40 10:50 11:00 11:10 11:20 11:30 11:40 11:50
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10
460 Tables Figures
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Cell pressure (hPa)
440 J I
H2O (ppmv)
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420 100
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400 FISH with DT/Cont.
FISH wo. DT/Cont. Full Screen / Esc
DP30
380 FISH:Cell pressure
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15:05 15:10 15:15 15:20 15:25 15:30 15:35 15:40 15:45 15:50
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Time (UTC) Interactive Discussion
Figure 5. Lowest and highest level of the same calibration shown in Fig. 4, but calculated with
the modified calibrations equations (green line). For more detail see text.
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a)
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b)
Title Page
Abstract Introduction
Conclusions References
Tables Figures
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c)
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J I
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Figure 6. Reference Hygrometer calibration: (a) difference of the measured frostpoints be- Printer-friendly Version
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tween the first Jülich DP30 frostpoint hygrometer and a MBW reference frostpoint hygrometer
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calibrated to a NPL standard (purple squares) or the second Jülich DP30 (dark blue triangles
and light blue dots); (b) relative deviation of the DP30 WVMR measurement to the WVMR given
by the permeation source (PTB, traceable to primary standard) for different pre-pressure lev-
els and comparison of different saturation equilibrium approximations applied to the measured
frostpoints (stars); (c) combination of the measurements of (a) and (b).
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1.8
0.0044 mean ck: 0.00416 ± 0.00005 (1.3 %)
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mean fu: 1.19 ± 0.01 (1.1 %) 1.7
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0.0043 1.6
Title Page
1.5
0.0042 Abstract Introduction
FISH: ck
FISH: fu
1.4 Conclusions References
0.0041
1.3 Tables Figures
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0.0040 1.2 J I
1.1 J I
0.0039
1.0 Back Close
08.10. 15.10. 22.10. 29.10. 05.11.
day of AquaVIT 2007 campaign Full Screen / Esc
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Figure 7. Time series for the calibration constants ck and fu during AquaVIT-1 campaign eval- Printer-friendly Version
uated with the enhanced calibration scheme.
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Title Page
Abstract Introduction
b) Ng
Ng calc
Conclusions References
H2O
H2O out
Tables Figures
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10 4 10 5
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H2O (ppmv)
J I
10 3 10 4 J I
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time (UTC)
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∗
Figure 8. Quality check procedure for high WVMRs: (a) correlation between I0 and Ng (cal-
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ibration data, blue dots) with pressure dependent fit function (black lines); (b) time series of
calculated count rate (Ng,calc , black dots), measured count rate (Ng , green dots), water vapor
(blue dots), and rejected water vapor (H2 O out, red dots) during one flight of ML-Cirrus.
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frequency
of occurance
(%) FISH review
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40
35
pressure (hPa)
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250 J I
5
300 0
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Figure 9. Relative difference between FISH and FLASH water vapor content outside of clouds Printer-friendly Version
for all coincident flights between 1999 and 2012 in dependence on pressure (51 563 data
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points = 14.3 flight hours). Clear sky conditions are defined by relative humidities lower than Interactive Discussion
80 %.
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Abstract Introduction
Conclusions References
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Figure 10. Scatterplot of FISH–WVMR vs.: WASUL (red) during Airtoss/DENCHAR 2013 (top
panel) and SHARC during ML-Cirrus 2014 (bottom panel). The mean relative deviation (MRD)
with SD to FISH is given for each individual instrument.
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Abstract Introduction
Conclusions References
Tables Figures
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Figure 11. Time series of water vapor measurements at the AIDA chamber in Karlsruhe during
the AquaVIT campaign in 2007.
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Figure 12. Scatterplot of WVMR during: AquaVIT-2 (19.04.2012); top: WVMR 20–1000 ppmv;
bottom: zoom for WVMR 7–20 ppmv. Mean relative deviation (MRD) to FISH is given for each
individual instrument.
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FISH-MLS, 82 hPa
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Troccinox -0.295 (0.904)
Scout -0.474 (0.830)
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2 AMMA -0.208 (0.711)
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Reconcile -0.772 (0.304)
FISH-MLS WVMR (ppmv)
Abstract Introduction
0 Conclusions References
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AMMA
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2 Reconcile J I
Scout Back Close
3
2004 2005 2006 2007 2008 2009 2010 2011 2012
Year Full Screen / Esc
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Figure 13. Comparison of FISH with MLS (Microwave Limb Sounder on the Aura satellite) for Printer-friendly Version
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different aircraft campaigns. Mean deviation with respective SD for each campaign is given in
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the upper right.
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