Review Article Vol. 3, No.

4 / April 2016 / Optica 414

Dual-comb spectroscopy
IAN CODDINGTON,1,* NATHAN NEWBURY,1,2 AND WILLIAM SWANN1
1
National Institute of Standards and Technology, 325 Broadway, Boulder, Colorado 80305, USA
2
e-mail: nathan.newbury@nist.gov
*Corresponding author: ian.coddington@nist.gov

Received 26 January 2016; revised 15 March 2016; accepted 16 March 2016 (Doc. ID 258273); published 14 April 2016

Dual-comb spectroscopy is an emerging new spectroscopic tool that exploits the frequency resolution, frequency
accuracy, broad bandwidth, and brightness of frequency combs for ultrahigh-resolution, high-sensitivity broadband
spectroscopy. By using two coherent frequency combs, dual-comb spectroscopy allows a sample’s spectral response to
be measured on a comb tooth-by-tooth basis rapidly and without the size constraints or instrument response lim-
itations of conventional spectrometers. This review describes dual-comb spectroscopy and summarizes the current
state of the art. As frequency comb technology progresses, dual-comb spectroscopy will continue to mature and could
surpass conventional broadband spectroscopy for a wide range of laboratory and field applications.
OCIS codes: (300.0300) Spectroscopy; (300.6360) Spectroscopy, laser; (280.0280) Remote sensing and sensors; (300.6495)
Spectroscopy, terahertz.

http://dx.doi.org/10.1364/OPTICA.3.000414

1. INTRODUCTION optical or rf reference [62,63]. Laser frequency combs have had

Dual-comb spectroscopy (DCS) combines many of the strengths a significant impact on diverse fields and, ever since their inven-
of conventional broadband spectroscopy and tunable laser spec- tion, have been considered an attractive source for spectroscopy
troscopy into a single platform [1–59]. As with conventional [64,65]. However, the challenge of using frequency combs for
Fourier-transform infrared (FTIR) spectrometers, broad swaths broadband spectroscopy was clear from very early on. To exploit
of the optical spectrum can be interrogated, and with the use the frequency accuracy and spectral resolution provided by the
of only a single photodetector. As with laser spectrometers, the frequency comb structure, one needs to spectrally resolve each
frequency resolution and accuracy is set by the laser rather than individual comb tooth. Comb light could be coupled into con-
the instrument, and the bright single spatial mode output enables ventional spectrometers. However, since the comb tooth spacing
long interrogation paths for high sensitivity. Since the first is finer than the resolution of nearly all spectrometers, the comb
demonstrations [2–4,60], interest in DCS has spawned a large then simply acts as a very bright, collimated light source; its as-
number of proof-of-concept experiments [1–59]. DCS quickly sociated frequency resolution and accuracy are lost. To fully capi-
evolved to provide comb-tooth-resolved spectra [6,9], ultimately talize on the underlying comb structure, several high-resolution
providing a high signal-to-noise ratio (SNR) over broad optical dispersive spectrometer and Fourier transform spectrometer tech-
bandwidths in the near-IR [24,25,50]. From its inception, re- niques have been developed for resolving individual comb teeth,
searchers have explored DCS at longer wavelengths, where including virtually imaged phase array (VIPA) spectrometers
spectroscopic signatures are strong [2–7]. Experiments have high- [66–68], comb-cavity Vernier spectrometers [69,70], and high-
lighted its compatibility with enhancement cavities [14,43], resolution FTIR spectrometers [71–75]. While VIPA and FTIR
multipass cells [25,50,51], gas-filled fibers [56], and turbulent techniques have seen compelling demonstrations, to date the
open-air paths [3,21,36,53]. DCS has been applied to ultrabroad- most widely pursued form of direct comb spectroscopy is DCS,
band near-IR spectroscopy [50], to near-field microscopy for which dispenses with the dispersive spectrometer altogether. This
subwavelength spatial resolution [5,8], to precision metrology of same technique appears in the literature as multiheterodyne spec-
molecular line centers [22,29,50], to a spectral lidar [21,31], and troscopy, linear optical sampling, coherent Fourier-transform
to greenhouse gas monitoring [36,51,53]. Recently, it has been ex- spectroscopy (FTS), and terahertz (THz) asynchronous optical
tended to nonlinear spectroscopy for stimulated Raman scattering, sampling (ASOPS), but the IR/visible community has largely set-
comb-based coherent anti-Stokes Raman spectroscopy (CARS) tled on the moniker “dual-comb spectroscopy,” which we use
[27,32], and two-photon spectroscopy [40,61]. As DCS continues here. This review focuses primarily on DCS in the IR region of
to mature, this list of applications will continue to expand. the spectrum, although we draw connections to DCS in the THz
Underlying DCS is the frequency comb laser emitting an array region. (The THz domain has been discussed in several excellent
of narrow, phase-coherent spectral lines, or “teeth.” Perfectly spaced reviews [7,49].) As mentioned earlier, DCS has a number of ad-
in frequency, these teeth can all be simultaneously stabilized to an vantages over conventional spectrometers in the basic performance
 Review Article Vol. 3, No. 4 / April 2016 / Optica 415

metrics of frequency resolution, accuracy, acquisition speed, and axis. DCS in the near-IR can indeed yield the latter and support
SNR, as well as in the potential for a compact system, since its measurements, for example, of line centers [29,50] or of gas
performance is not fundamentally limited by the instrument concentrations [36,53]. In the mid/far-IR, DCS is generally still
optical path length as in grating or FTIR spectrometers. limited to proof-of-concept demonstrations, with the exception of
The DCS concept is illustrated in Fig. 1(a). Two combs with methane concentration and line center measurements [22,51].
slightly different repetition rates are interfered on a photodiode However, as mid- and far-IR combs continue to evolve, so too
generating an rf comb composed of distinguishable heterodyne will their DCS spectra.
beats between pairs of optical comb teeth. This rf comb is easily The review is organized as follows. Section 2 provides a brief
accessible with rf electronics and contains the relevant spectral summary of DCS in the absence of phase noise, with an emphasis
information in the optical comb spectra. To perform spectros- on the basic scaling laws. Actual laboratory DCS must contend
copy, a sample is introduced into one or both optical beam paths. with the finite linewidths and drift of the combs, and Section 3
The sample’s response is encoded on the comb light; this response categorizes DCS demonstrations by frequency comb coherence.
is then recovered through heterodyne detection. The exact infor- Section 4 summarizes existing DCS demonstrations across differ-
mation recovered will vary depending on the system architecture, ent spectral regions. Section 5 is a more complete discussion of
as shown in Fig. 1(b). In the first configuration, one comb is SNR limitations and summarizes demonstrations that have
transmitted through the sample and then interfered with the pushed these limits. In particular, it discusses coherent averaging,
second “local oscillator” comb. This asymmetric approach is which will serve a critical role in applications of DCS. Section 6
analogous to the “dispersive” FTIR technique, and the full phase concludes by summarizing current progress and future challenges.
and amplitude response of the sample is measured [76]. In the Although we focus here on DCS applied to linear spectroscopy
second, symmetric approach, both combs are transmitted through as a broadband coherent system, the same basic technique has
the sample. This approach is analogous to the typical FTIR been applied to closely related applications. The ability to simulta-
configuration and measures only the sample’s absorption, but neously record loss and dispersion has made dual-comb approaches
is more robust to turbulent measurement paths. In either case, attractive for characterizing telecom components, fiber gratings,
the variations in the comb spectrum must be effectively normal- and microresonators [78–80]. A modified dual-comb system can
ized out so that only the sample’s response is measured. monitor active sources such as static and fast-swept cw waveforms
To date, DCS has outpaced other comb spectroscopy tech- [81–84], arbitrary optical waveforms [57,85,86], and even pulsed
niques, as well as swept laser spectroscopy, in terms of spectral or incoherent sources [87,88]. All these techniques have the same
coverage, though it is unlikely to ever match the full spectral underlying dual-comb/single-receiver architecture and serve to
coverage possible with conventional FTIR. Figure 2 shows an highlight the versatility of this approach, which is ultimately no
overview of the spectral coverage of DCS demonstrations. These more than a simple extension of standard heterodyne laser inter-
DCS experiments span a wide range in terms of realized resolu- ferometry to frequency comb sources.
tion, accuracy, SNR, control of systematics, etc. This range
reflects the fact that the unique advantages of DCS do come with 2. DUAL-COMB SPECTROSCOPY: THE IDEAL
experimental challenges, and the quality of the DCS spectra CASE
largely mirrors the technological sophistication of the frequency
combs in the given spectral region. For example, the acquisition A. DCS in the Time and Frequency Domains
of a semiquantitative spectrum with free-running combs is sig- In the frequency domain, the DCS output is simply an rf comb
nificantly simpler than the acquisition of a high-SNR, high- [see Figs. 3(a) and 3(b)]. The intensity and phase of the detected
resolution absorbance spectrum with a fully calibrated frequency rf comb teeth are proportional to the product of the electric fields

Fig. 1. (a) Simple DCS concept. Two combs with repetition rates f r and f r ! Δf r are mixed and detected by a single photoreceiver. As a result of the
comb structure, each pair of optical teeth yields an rf heterodyne signal at a unique rf frequency. These rf frequencies form an rf comb of spacing Δf r . The
rf teeth can be tightly packed such that >105 comb teeth can be observed simultaneously. For much of the original DCS work, f r was typically
∼100 MHz and Δf r was 100 Hz to 1 kHz, but these values can vary considerably across different frequency comb sources. (b) For spectroscopy,
either one or both combs are passed through the sample. The resulting absorption (or phase shifts) on the comb teeth is encoded onto the corresponding
amplitude (or phase) of the measured rf comb teeth.
 Review Article Vol. 3, No. 4 / April 2016 / Optica 416

Fig. 2. Spectral coverage of dual-comb spectroscopy demonstrations (top band) and underlying frequency comb technologies (bottom band). The span
covers over 14 octaves across the THz, IR, and optical. DCS has also been proposed in the extreme UV [77]. Section 4 discusses some of these different
demonstrations. PCA, photoconductive antenna; OPO, optical parametric oscillator; DFG, difference frequency generation; QCL, quantum cascade
laser; SHG, second-harmonic generation; HHG, high-harmonic generation.

of the two optical comb teeth. DCS effectively maps the optical response of the sample, which can be viewed equally well in either
spectrum of width, Δν, to an rf spectrum of width, Δν∕m, the time or frequency domain [20].
where m " f r ∕Δf r . Here, f r is the comb repetition frequency
and Δf r is the repetition frequency difference between the B. Acquisition Speed
two combs. Compression factors m of 30,000–1,000,000 are The minimum time to resolve the rf comb teeth, and therefore
common, and several hundred thousand comb teeth, spanning acquire a single spectrum, is simply 1∕Δf r. Therefore, with
tens to hundreds of THz, can be mapped into a 100 MHz rf band Eq. (1) there is a direct trade-off between optical bandwidth
and digitized. From inspection of Fig. 3, it is clear that the one- and acquisition speed. Nevertheless, at 100 MHz comb tooth
to-one mapping from the optical to rf domain is only maintained spacing, a single spectrum having over a million spectral elements
if the optical spectral bandwidth satisfies can be acquired in milliseconds; narrower spectra can be acquired
proportionally faster. However, this speed advantage is offset by
mf r f 2r the low SNR per single spectral acquisition. In practice, multiple
Δν ≤ " ; (1)
2 2Δf r spectra must be co-added, and the minimum acquisition time is
instead set by the required SNR. Still, the rapid single-shot
which can be doubled for in-phase/quadrature detection.
acquisition is important for measurement in turbulent environ-
Figures 3(c) and 3(d) provide the complementary time-domain
ments, since the turbulence-induced noise is “frozen” out over
picture of DCS. In this picture the two combs sample each other,
a single interferogram [36,89]. Moreover, the development of
with very fine effective time shifts between each consecutive pair
mid-IR [16,22,28,33,35,41,48,51,58] and far-IR [2,3,5,37,
of pulses given by
38,52] DCS and long interaction path lengths through optical
Δf r 1 cavities [14,43], multipass cells [25,43,51], and open paths [36]
ΔT " ≈ ; (2) may relax the need for a high SNR somewhat by providing
f r #f r ! Δf r $ mf r
enhanced absorption signals. Furthermore, note that this speed
which is in the picosecond to femtosecond range. One can see increases with the square of the comb tooth spacing. Emerging
the analogy to linear optical sampling or a sampling oscilloscope; microresonator combs [90], electro-optic modulator (EOM)
the sampling gate given by the femtosecond pulses of one comb combs [43,54–57], and quantum cascade laser (QCL) combs
asynchronously samples the repetitive pulse train from the other [37,38,90] have repetition rates in excess of 10 GHz; with these
comb, allowing observation of a downsampled version of that one can consider recording complete spectra in time scales below
comb. The resulting time-domain signal is also viewed as an 1 μs. The spectral spacing is relatively coarse, but such devices
“interferogram” that is highly analogous to FTIRs. The effective could allow studies of fast dynamic processes such as chemical
sampling time step per point of ΔT imposes a Nyquist condition reactions or rapid measurements of the broad absorption features
that is the same as Eq. (1). The time-domain picture also of liquids or solids [91,92].
highlights the importance of detector linearity, since an accurate Note that the discussion above assumes an entire interfero-
spectrum requires a linear detector response from the strong gram is digitized. Instead, only a limited region of the interfero-
centerburst to the weaker tails visible in Fig. 3(d). Note that gram about the centerburst can be digitized, corresponding to
the Fourier transform of a series of interferograms yields the rf an apodized interferogram in the language of conventional FTS.
spectrum of the frequency-domain picture in Fig. 3(b). This apodization nominally shortens the acquisition time of a
To obtain the sample response, we must use one of the con- particular single spectrum, but of course the acquisition rate of
figurations shown in Fig. 1(b) and normalize by the unperturbed consecutive spectra is still Δf r . Moreover, the frequency comb
(i.e., sample-free) dual-comb spectrum. The result is the linear structure is lost, since the Fourier transform of the apodized
 Review Article Vol. 3, No. 4 / April 2016 / Optica 417

pffiffiffiffiffiffiffiffiffiffiffiffi
[20]. In the ideal shot-noise limit, the SNR ≈ τncomb ∕M ,
where τ is the acquisition time and ncomb is the number of de-
tected comb photons per second. However, the actual SNR
per spectral element will depend on the dominant noise source,
which is discussed in detail
pffiffiffi in Section 5. Nevertheless, the basic
scaling law of SNR ≈ τ∕M is retained and illustrates the trade-
off in SNR versus bandwidth, since Δν " M f r . It also illustrates
the importance of a long coherent averaging time, or equivalently
a long effective mutual coherence time between combs, which sets
the maximum possible τ. Finally, this scaling
pffiffiffi drives the choice of a
useful figure of merit of SNR ≈ M ∕ τ, used in Section 5 to
compare the SNR across different acquired DCS spectra.

3. DUAL-COMB SPECTROSCOPY WITH

IMPERFECT COMBS
The ideal picture of the previous section assumed ideal frequency
combs composed of narrow (delta-function-like) comb teeth at
well-defined frequencies. Actual frequency combs can approach
this ideal performance, but it is experimentally challenging.
DCS “doubles” that challenge by requiring two such combs with
high mutual coherence. In practice, DCS has been demonstrated
over a wide range of frequency comb performance. Coarsely, DCS
demonstrations can be broken into three categories: free-running
combs, mutually coherent combs, and fully referenced combs, as
listed in Fig. 4 and summarized below. Clearly, the experimental
challenges increase in moving from free-running combs to fully
referenced combs, but so too does the performance in terms
of improved spectral resolution, frequency accuracy, and SNR
(through increased coherent averaging times).
Figure 4(a) depicts the case of free-running combs, where the
relative optical linewidth between the combs is greater than Δf r .
Fig. 3. (a) Two frequency combs (red and blue) are mixed to produce
(b) the rf comb. Solid gray lines indicate filter functions applied in the rf In that case, there can be varying degrees of overlap or blending
and optical to avoid aliasing effects. (c) The equivalent time-domain pic- with the corresponding rf comb, resulting in a much lower fre-
ture showing the pulse-to-pulse walk-off between the two comb pulse quency resolution. Nevertheless, demonstrations with free-
trains. (d) The photoreceiver voltage output corresponds to the product running combs have been important as basic proof-of-principle
of the two comb pulses, integrated over the receiver bandwidth. This experiments, for example, the first demonstration of DCS by
output can be viewed in laboratory time, where the samples are at time Keilmann and coworkers [2,3], cavity-enhanced DCS [14], and
intervals of 1∕f r , or in effective time, where the samples are at time in- many demonstrations with novel comb sources in the mid-IR and
tervals of ΔT (as with FTIR interferograms). In both time scales k is the far-IR [16,28,33,35,37,38,41,48,51,93].
sample number. The large “centerburst” corresponds to the simultaneous Figure 4(b) depicts the case of high mutual coherence, where
arrival of the two pulses. Also visible in the “tail” to the right is a weak
the relative linewidth between the combs is well below Δf r. The
ringing containing absorption information of the sample gas.
mutual coherence can be enforced through active feedback to the
combs and/or signal processing, as discussed later, or through
comb designs where the coherence is at least partially inherent
interferogram yields a spectrum that is smoothed across comb [43,54,55,57,94–97]. In this case the individual comb teeth
teeth. This spectral smoothing does lead to an improved SNR are spectrally resolved, and therefore each comb tooth pair pro-
per (coarser) spectral point at the cost of lower spectral resolution. vides a single independent spectral sample. Since the fundamental
The SNR for the detection of a given molecular species remains resolution is set by the comb tooth linewidth, which can be sev-
unchanged, since it will be independent of the spectral smooth- eral orders of magnitude smaller that the spectral point spacing,
ing [20]. there is minimal cross talk between adjacent spectral elements,
i.e., no instrument line shape. This sets DCS apart from conven-
C. Signal-to-Noise Ratio
tional broadband spectrometers, where instrument line shapes are
One strength of DCS is that only a single detector is needed to always present and will distort the recorded spectra in ways that
record millions of spectral points. However, there is a “multi- can shift over time. Moreover, at typical comb repetition frequen-
plexed” penalty associated with the use of a single detector. cies the spectral point spacings are 50–200 MHz, matching
Essentially, for M spectral elements (i.e., comb teeth),pone
ffiffiffiffiffi might the highest resolution FTIRs, traditionally the gold standard of
expect the SNR per spectral element to scale as 1∕ M as one high-resolution broadband spectroscopy. Finally, this point spac-
spreads a fixed laser power over M spectral elements. However, ing is not the actual resolution limit; if needed, the comb can be
the use of a p single
ffiffiffiffiffi detector leads to an additional multiplexed scanned for higher point density up to a resolution limit set by
penalty of 1∕ M , leading to the overall SNR scaling with 1∕M the absolute comb tooth linewidths (typically a few kilohertz to
 Review Article Vol. 3, No. 4 / April 2016 / Optica 418

Fig. 4. Three different categories of DCS demonstrations. (a) Free-running combs can yield dual-comb spectra, but with low resolution, low frequency
accuracy, and low SNR, since only limited signal averaging is possible; (b) mutually coherent combs can yield comb-tooth-resolved spectra that can be
averaged for high SNR; and (c) fully referenced combs yield spectra with simultaneous high resolution, absolute frequency accuracy, and high SNR. Text
boxes indicate some general rules of thumb for frequency combs based on mode-locked lasers.

megahertz) [22,39,59]. There is an important second conse- are still developing. For this reason, most demonstrations using
quence to high mutual coherence, namely, it allows for longer highly coherent [i.e., Fig. 4(b)] or fully stabilized combs [i.e.,
acquisition times, τ, and therefore higher SNR, as discussed in Fig. 4(c)] have taken place in the near-IR (or THz), and they
Section 2.C and later in Section 5. are discussed first below.
Finally, Fig. 4(c) depicts the “ideal” case, where the two
mutually coherent combs are referenced back to an absolute A. Near-IR DCS with Fiber-based Frequency Combs
frequency standard. This is easiest to achieve for combs based Figure 5 provides an example of a DCS spectrum acquired in the
in difference frequency generation (DFG) or with THz combs, near-IR using the dispersive configuration and fiber-laser-based
where the carrier-envelope offset frequency, f ceo , is identically zero frequency combs with 100 MHz repetition rates [15]. The high
[5–7,11,18,23,39,45–47,49]. In other cases, f ceo is not zero; SNR and flat baseline are due to long-term coherent averaging,
stabilizing f ceo still allows the comb teeth to reach kilohertz time-multiplexed signal and reference measurements, and sequen-
accuracies, so that tooth-resolved DCS spectra exceed the accuracy tial acquisition over subbands to avoid detector nonlinearity.
of conventional broadband spectrometers by many orders of mag- The quality of this early data was facilitated in part by the rel-
nitude [9,19,22,25,36,53]. Absolute referencing also removes atively advanced nature of the near-IR optical componentry.
common-mode frequency drifts of the two combs that would Indeed, to date the majority of DCS demonstrations have been
otherwise broaden the instrument line shape over long averaging performed in the ∼1550 nm telecommunication band, where
times, potentially washing out spectral features of interest. there are relatively inexpensive and robust erbium fiber frequency
Molecular line centers retrieved with fully stabilized DCS have combs, fiber-optic components, and high-bandwidth, sensitive
frequency accuracies superior to high-resolution FTIRs, and trace- photoreceivers [9,10,17,19,24,25,29,34,36,42,44,50,53]. For
ability to the underlying frequency reference. However, spectral example, the near-IR saw the first demonstration of tooth-
distortions can limit line center retrievals to about a part per thou- resolved DCS spectra, which was achieved by use of active
sand of the linewidth. [22,29]. phase/timing correction of the two combs [9] and also included
absolute frequency stabilization. This work was followed closely
by the first demonstration of a digital phase/timing correction
4. DUAL-COMB SPECTROSCOPY that essentially imposes mutual phase coherence via signal
DEMONSTRATIONS IN DIFFERENT SPECTRAL processing and achieves tooth-resolved spectra [10]. References
REGIONS [42,44] developed an analog adaptive sampling approach that also
In this section, we review DCS demonstrations by spectral cover- leads to tooth-resolved spectra and is more accessible to many
age, following the summary presented in Fig. 2. As emphasized in laboratories.
Fig. 2, the first requirement for DCS is the existence of a fre- Section 5.C discusses these important methods of extending
quency comb in the desired spectral range. While near-IR comb the mutual coherence in more detail.
technology is becoming more robust [98–101], combs in the Near-IR DCS demonstrations have also shown that DCS is
mid-IR [16,22,28,33,35,41,48,51,58] and far-IR [2,3,37,38] compatible with nonlinear spectral broadening. Operating in
 Review Article Vol. 3, No. 4 / April 2016 / Optica 419

Fig. 5. Signature of the full rotational band from the C-H overtone of HCN gas as measured in the dispersive dual-comb spectrometer configuration
[19]. (a) The phase and amplitude signature at 100 MHz point spacing has a signal-to-noise ratio per point of ∼4000 with respect to unity transmission;
(b) expanded view showing the spectral sampling points; (c) joint time–frequency domain signature from the short-time Fourier transform of the data that
clearly shows the free-induction decay signals in the “P” and “R” branches as vertical stripes. The overall decay results from Doppler and collisional
dephasing.

the erbium or ytterbium gain windows provides access to only a phase/timing approach was extended to enable coherent co-
small set of molecules. Fortunately, the spectrum of a comb can be adding of interferograms on an FPGA, effectively allowing
broadened in nonlinear fibers. With spectral broadening, Zolot infinitely long averaging times without incurring dead time.
et al. demonstrated tooth-resolved DCS over 43 THz, allowing Alternatively, Refs. [17,24] further refined the digital phase/timing
interrogation of atmospheric trace molecules such as methane, correction approach to allowing for similarly limitless continuous
carbon dioxide, and water [25]. Okubo et al. have shown real-time coherent averaging on a field programmable gate array
that DCS is possible over an even broader spectrum covering (FPGA) and yielding spectral SNRs exceeding all other techniques
140 THz or almost the entire 1–2 μm supercontinuum span to date.
of Er fiber frequency combs [50].
Near-IR DCS is also one of the few regions, other than the B. Near-IR DCS with EOM-based Frequency Combs
THz, where the technology has ventured beyond instrument Near-IR dual-comb systems can also be based on “electro-optic
demonstrations. It has been used for accurate measurement of modulator” frequency combs generated by strong modulation
molecular line centers [29,50] and, most recently, greenhouse of a cw laser. In fact, as early as 2001 a dual-comb system based
gas monitoring over outdoor air paths [36,53], in both cases pro- on EOM combs was used in a high-speed optical coherent tomog-
viding performance beyond what is possible with conventional raphy demonstration [60]. EOM-based dual-comb systems have
broadband spectrometers. the advantage of a flexible repetition rate that can exceed 10 GHz,
These systems all make use of erbium fiber frequency combs. high-power comb teeth, and intrinsic mutual coherence between
DCS based on ytterbium fiber frequency combs centered at 1 μm combs, since the two combs are generated from the same cw laser
is less common but has been used for a very early demonstration and rf time base [43,54,55,57], but their operation is thus far
of cavity-enhanced DCS [14]. Further toward the visible spec- restricted to relatively narrow spectra comprising ∼50–100 teeth
trum, DCS based on doubled erbium fiber frequency combs at over tens of gigahertz and to the telecom band where efficient
760–780 has been used for Rb and O2 spectroscopy [30,40], modulators are commercially available. As such, they are well
while DCS based on doubled ytterbium fiber frequency combs matched to rapid, sensitive spectroscopy across single near-IR
at 520 nm has been used for iodine spectroscopy [26]. molecular lines, and EOM-based DCS has been demonstrated
Finally, the near-IR also saw the first demonstrations of in the detection of the complex (phase and amplitude) spectrum
long-term averaging, using techniques discussed in Section 5.D. of CO2 [43] and HCN [54,55]. Through external spectral
With these modified schemes, DCS can truly have SNRs com- broadening in nonlinear fiber, EOM-based DCS has been dem-
parable to FTIR or grating spectrometers. In Ref. [19], the active onstrated at up to ∼300 GHz instantaneous bandwidth [56].
 Review Article Vol. 3, No. 4 / April 2016 / Optica 420

With future mid-IR modulators, it should be possible to extend demonstrated in narrowband mid-IR DCS near 3.4 μm for the
this technique beyond the near-IR. Finally, note that there is accurate line center measurements of methane [22]. In that case,
no absolute frequency accuracy, unless the cw laser frequency is the Er fiber comb was shifted to the mid-IR via DFG with a cw
measured, and any frequency noise on that cw laser will limit the 1 μm laser in periodically poled lithium niobate. Higher-power,
ultimate resolution. broader-bandwidth (and f ceo -free) combs are generated by DFG
with the reamplified 1 μm light generated by supercontinuum
C. Related Near-IR Systems generation from the Er fiber comb [51,58]. Reference [51] dem-
It is also worth noting that there is a range of emerging techniques onstrated rapid, sensitive methane detection with such a system
that bear a strong resemblance to the dual-comb approach both over 3.17–3.44 μm. Through additional external spectral broad-
in concept and in underlying technology. In most cases it is too ening, future DFG-based systems have the potential to cover the
soon to know where these offshoots will lead, but they offer an full mid-IR (3–5 μm).
interesting trade-off space to explore. DFG-based combs can also permit DCS further into the IR.
One of the simplest variations of DCS and FTIR is the use of a As mentioned above, the first DCS demonstrations were based on
single frequency comb coupled with an unbalanced interfero- a Ti:sapphire comb whose output was shifted to the 9–12 μm
meter [102–105]. Sometimes referred to as optical scanning by region through DFG in Ga:Se [2]. This system has been applied
cavity tuning (OSCAT), this technique works by continuously to the rapid detection of ammonia over a 44 m outdoor path [3]
scanning the repetition rate of the comb [106]. This sweeping and to scanning near-field optical microscopy [5]. Furthermore,
repetition rate, combined with the significant differential time the Ti:sapphire laser can be replaced with an all-fiber system
delay in the unbalanced interferometer (often ∼1 μs), gives two allowing even greater tunable spectral coverage from 4 to 17 μm
pulse trains with a continuously varying relative timing that can with 21 THz of instantaneous bandwidth [110]. Future develop-
be interfered to create an interferogram similar to DCS, though ments in optically patterned gallium arsenide could make for
typically with lower spectral resolution. In a related approach, an even more efficient generation, high-power DFG combs in the
acousto-optic tunable filter in one arm of the interferometer can far-IR [111].
allow for a rapidly changing differential delay even with a static Mid-IR combs can also be generated directly by OPOs at high
comb, although the maximum path delay and spectral resolution power and with broad tuning ranges [28,33,35,41,48,68,72,
are restricted [107] 112,113]. DCS presents the daunting challenge of operating
A second interesting system is known as dual-etalon cavity two coherent OPOs. However, there has been a series of single
ringdown spectroscopy (with the memorable acronym OPOs designs for DCS where two mode-locked lasers at
DEFCOM) [108]. Two high-finesse etalons are excited with a slightly different repetition rates pump a single OPO cavity
single common optical pulse. As both etalons ring down, they [28,33,35,41,48]. Nonlinear interaction of the pulses in the OPO
emit two trains of pulses that can be interfered to mimic DCS. cavity can be minimized by counterpropagating the two pump
This technique inherently combines the strengths of cavity ring- lasers in the OPO cavity [41,48]. With this approach, OPO-
down spectroscopy and Fourier transform techniques. However, based DCS has been demonstrated in spectroscopy of methane
to date, DEFCOM has been demonstrated only with limited and acetylene over 3.1–3.4 μm [35,41,48]. Finally, the use of
bandwidths. degenerate OPOs offers the possibility of extremely broadband
Finally, there are a number of systems that seek to dispense DCS across the mid-IR [112,114].
with the requirement of two mode-locked lasers by generating Interesting new dual-comb Raman techniques also offer access
dual combs with offset repetition frequencies from a single laser to the 7–50 μm range [27,32]. This technique combines the
system [94–97]. In the near-IR, the recent work of Ref. [97] ex- advantages of CARS with the resolution/accuracy of combs to
hibits very-high-quality dual-comb spectra using this approach. probe the far-IR molecular spectrum. As discussed in Ref. [32],
this approach has the potential for high-speed broadband CARS
D. Mid-IR and Far-IR DCS and can be applied to spectro-imaging of complex samples.
While DCS does have applications in the near-IR and visible Finally, mid-IR comb light can also be generated directly from
regions, the principle spectral region of interest for molecular mode-locked lasers. Proof-of-principle DCS experiments have
spectroscopy is at wavelengths greater than 3 μm, where mole- been conducted at 2.4 μm with two Cr2! :ZnSe femtosecond
cules exhibit much stronger absorption cross sections. This is also lasers, and several groups are actively pursuing mid-IR mode-
the principle area in which DCS lags behind FTIR, the primary locked fiber lasers [115,116]. Further into the IR, QCLs provide
workhorse for analytical spectroscopy. Indeed for all its advan- interesting possibilities, since they can provide a path toward a
tages, DCS will never usurp FTIR for many applications until it chip-scale, electrically pumped system for DCS [52]. Preliminary
has much broader spectral coverage into the mid-IR (3–5 μm) and demonstrations of DCS using QCL-frequency combs have been
far-IR (6–13 μm). As illustrated in Fig. 2, frequency combs reported at 7–8.5 μm with over 64 comb teeth at 15 GHz sep-
continue to expand into these spectral regions, and there have aration in the molecular fingerprint far-IR region [37,38,52].
been a number of interesting DCS demonstrations including With improvements in spectral coverage, these QCL DCS
the pioneering work of Keilmann and coworkers [2,3]. systems could eventually provide a compact, high-speed far-IR
Mid- and far-IR frequency combs can be generated based on spectrometer.
DFG from near-IR sources or directly from mid-IR/far-IR mode-
locked lasers, optical parametric oscillators (OPOs), microresona- E. THz DCS
tors, or QCLs [109]. An advantage of using DFG-based DCS is At longer wavelengths one enters the THz region, which is also
that the coherence of the underlying near-IR comb sources can very attractive for spectroscopy. DCS demonstrations in the THz
be directly translated into the mid-IR. This high coherence was are as prevalent as in the near-IR and have an earlier inception [4]
 Review Article Vol. 3, No. 4 / April 2016 / Optica 421

as well as several excellent reviews [7,49]. In the THz, DCS is In general, the shot-noise-limited SNR of Section 2 does not
effectively equivalent to THz time-domain spectroscopy or apply, as the comb power is either too low, so that the photore-
ASOPS [4,6–8,11,13,18,39,45–47,49], and commercial systems ceiver’s noise equivalent power (NEP) dominates, or too high, so
are available [117]. THz systems often use either Ti:sapphire or that it must be attenuated to avoid photoreceiver saturation. The
fiber-based combs to drive photoconductive antennas that emit former case might be encountered in the far-IR, where the comb
broadband THz combs. As with DFG, this process cancels the powers might be lower and NEP higher than in the near-IR. In
carrier-envelope offset frequency, and the long wavelengths make that case, the SNR is
the system more tolerant of timing jitter. THz DCS has been pffiffiffiffiffiffiffiffiffiffi
1 P 1 P 2 pffiffiffi
demonstrated with absolute frequency accuracy, high SNR SNR NEP ∝ τ;
through longer integration times, and comb-tooth-resolved spec- M NEP
tra [6,11,23,45–47,49]. where P 1 and P 2 are the powers of the two combs at the detector
In the THz region, Doppler broadening is correspondingly and τ is the averaging time. Clearly, the route to a higher SNR is
smaller than in the near-IR, and for a sufficiently dilute gas higher comb power and lower NEP. Since the NEP can be a func-
the molecular absorption features can be narrower than the tion of the photoreceiver bandwidth, one can possibly realize
comb spacing. Interleaving of comb spectra can fill these gaps lower NEP by compressing the rf comb into bandwidths well be-
[22,39,59], and coherent processing is required to account for low f r ∕2, provided the comb linewidths are sufficiently narrow.
time-domain features that can extend across multiple interfero- On the other hand, many near-IR or visible comb sources can
grams [39]. generate hundreds of milliwatts of optical power, which can easily
drive a photoreceiver into nonlinearity or full saturation if not
attenuated. In this case, the SNR is effectively limited by the
5. DUAL-COMB SPECTROSCOPY: SNR dynamic range of the photoreceiver, D (as in FTIR):
The previous section categorized DCS demonstrations in terms of D pffiffiffiffiffiffiffi
spectral region. However, as noted, many DCS experiments out- SNR DynRange ∝ τf r :
M
side of the near-IR and THz have been limited to proof-of-
concept spectra with low SNR. In order for future experiments Note that the actual noise floor might be shot-noise limited, but
to exploit the full frequency resolution and accuracy afforded by since the dynamic range sets the maximum comb power, we refer
DCS, a high-SNR spectrum is critical. Otherwise, the strong to this case as dynamic-range limited. Dynamic ranges vary, but a
spectral noise will mask the fine detail present in molecular commercial 100 MHz InGaAs amplified photoreceiver might
spectra. This section summarizes the approaches for achieving have a limited D of ∼500 (given by the ratio of the maximum
high-SNR DCS spectra. peak power to the NEP integrated over a bandwidth of f r ).
Section 5.A summarizes the limitations to the SNR Clearly, the route to higher SNR here is increased dynamic range.
pffiffiffi in DCS.
Section 5.B defines the figure of merit, SNR ≈ M ∕ τ, discussed One solution is to simply push deeper toward saturation. The first
in Section 3.C and summarizes the figure of merit achieved in effect at the onset of saturation is the mixing of adjacent rf comb
recent DCS experiments. Of course, this figure of merit is most lines, leading to slight distortions (∼1 MHz) of the measured ab-
sensible if the DCS data are acquired for at least 1 s, the normal- sorption line centers [22,29,50], with distortions in the integrated
ized acquisition time. Section 5.C discusses the methods for DCS line strength appearing at yet higher powers. For many applica-
data acquisition over seconds. Finally, Section 5.D discusses two tions, such line center shifts are inconsequential, and many DCS
methods that allow for long-term coherent averaging spanning demonstrations have operated at least partially into this nonlinear
minutes, hours, or even days. regime. If this dynamic range is set by the rf amplification of the
To understand the importance of coherent averaging, consider strong centerburst (rather than intrinsic nonlinearity in the pho-
apffiffiDCS spectrometer with a figure of merit of SNR ≈ M ∕ todetection), the peak signal intensity can be reduced by strongly
ffi
τ " 106 Hz1∕2 . It then requires 10,000 s of averaging to reach chirping one of the two frequency combs [17]. In the near-IR
an SNR per spectral point of 1000 over 100,000 spectral points. below ∼1.8 μm, there has been considerable recent progress in
This long-time acquisition over 10,000 s is possible but requires the development of high-dynamic-range InGaAs detectors to sup-
the techniques discussed in Section 5.D. port microwave photonics [118]. Finally, one could spectrally dis-
Note that in this section we focus on spectral SNR, defined as perse subbands of the spectrum onto multiple photoreceivers to
the standard deviation of a normalized transmission spectrum. improve the SNR [20] at the cost of experimental complexity.
This spectral SNR is independent of path length and allows This analysis ignores the multiplicative noise from differential
use across platforms with widely varying paths and purposes. phase noise between the combs. This noise will clearly be most
prevalent for free-running combs [e.g., Fig. 4(a)]. However, even
A. Practical Limitations to the SNR for mutually coherent combs with linewidths below Δf r, there is
Broadband time-domain noise will lead to “broadband” spectral still a residual phase noise pedestal on any given rf tooth. Phase
noise, corresponding to uncorrelated point-to-point fluctuations noise at Fourier frequencies below Δf r will contribute to slow
across the measured spectral points (comb teeth). The resulting baseline variations [20] and should be removed though interfero-
SNR has been analyzed in detail in Ref. [20]. Note that this SNR gram phase correction (see Section 5.D). Phase noise at Fourier
of a single spectral point differs from the SNR for the detection of frequencies above Δf r will affect neighboring rf comb teeth,
a molecular species. The latter would be integrated over the full limiting the SNR. The full impact of this higher frequency multi-
absorption spectrum and could be higher or lower depending on plicative noise has not yet been rigorously examined, but active
the molecule’s summed line strength and, of course, on the total real-time phase correction as in Ref. [24] will suppress its effects
effective path length. (again, see Section 5.D).
 Review Article Vol. 3, No. 4 / April 2016 / Optica 422

Finally, the goal is to measure the sample’s response, not the comb tooth spacing f r ) and to 1 s acquisition times. With the
comb spectrum. Therefore the comb spectrum must be normal- exception of Refs. [51,56], which used 250–300 MHz comb
ized out. This normalization is common to any spectroscopic sys- tooth spacing, all experiments used approximately 100 MHz
tem, but here it is exacerbated by the strongly varying comb comb tooth spacing. (A higher repetition rate shifts the points
spectra. While a DCS spectrum can cover 100 THz [50], the to wider optical bandwidths for the same nominal figure of merit).
broadband comb spectrum will generally have significant struc- As shown in Fig. 6, most demonstrations so far have a figure
ture showing up to 20 dB of intensity variations (which is not of merit in the range of 106 –107 . Also, Fig. 6 emphasizes the
captured in Fig. 2), regardless of the wavelength band. Regions significant advantage of digital phase/timing correction, which,
of the spectrum may be unusable for spectroscopy due to low combined with a high dynamic range detector, yields a record
power, while other regions may have strong variations over short figure of merit [24] of ∼2 × 108 Hz1∕2 . Finally, when operating
wavelength spans that are difficult to remove from the final sam- at the highest possible figure of merit, one must be wary of in-
ple spectrum, particularly for broad absorbers. To date, most creased nonlinearities that can degrade the instrument line shape
DCS experiments have interrogated small molecules in the gas (by mixing the response across rf comb teeth) and lead to system-
phase. Because the resulting absorption linewidths are narrower atic distortions of the spectrum.
than the comb variations, a piecewise linear baseline fit can suffice
C. DCS with Mutual Coherence Time of Seconds
to remove these background variations [36], as in conventional
FTIR. Additionally, experiments have explored normalization us- As discussed above, the SNR improves with the square root of the
ing a second reference channel, sequential measurements with averaging time, but only up to the mutual coherence time of
and without the sample, and even time-interleaved interferograms the two combs, which sets the linewidth of the rf comb teeth.
[15,51]. The best option will depend strongly on the comb spec- For THz combs or EOM-based frequency combs, this mutual
trum, the optical configuration (e.g., presence of etalons), and the coherence can be established with relatively minimal active
spectral signature of the sample (broad or narrow absorbers). control. In the IR, mutual coherence is much harder to enforce
However, as with conventional spectrometers, a “flat” baseline because of the higher carrier frequency and broader optical band-
at the parts-per-thousand level is challenging. widths.
Three different approaches have been taken in IR DCS to
B. Figure of Merit for SNR force mutual coherence times on the order of seconds: active
As shown in the previous section, in the shot-noise limit, phase/timing feedback, digital phase/timing correction, and ana-
dynamic-range limit, or detector-noise limit, the SNR scales as log adaptive sampling. In all three cases, the two combs are each
pffi
τ
. For this reason, we identify a useful figure of merit for compared to a pair of common references, for example, to two cw
M
DCS as SNR × M at τ " 1 s, which also connects the SNR with lasers separated by a few THz [9,17,42]. (Alternatively, Ref. [50]
the measured optical bandwidth, Δν " M f r [20]. It can be chal- used fully self-referenced combs compared against a single cavity-
lenging to extract values for the SNR and bandwidth from the stabilized cw laser.) The comparison generates two pairs of error
literature because of variations in whether the peak or average signals that reflect the fluctuations in the two combs. In the
SNR is given and in the definition of optical bandwidth. approach of active phase/timing feedback, these error signals
Nevertheless, Fig. 6 reviews the state of the art for DCS in terms are input to a phase-locked loop that actively stabilizes both fre-
of this figure of merit for a few different demonstrations. All SNRs quency combs via high-bandwidth actuators to achieve subhertz
are scaled to the unapodized value (i.e., resolution equal to the residual linewidths and a known, stable repetition frequency
[9,19,22,25,36,50,53]. In the approach of digital phase/timing
correction, these error signals are digitized along with the inter-
ferograms. Signal processing then removes both carrier phase
noise and relative timing noise by resampling the interferograms
[10,17,24,30,31]. In the approach of analog adaptive sampling,
these error signals are input to a set of analog electronics that
corrects for any relative carrier phase noise and adjusts the digi-
tizer sampling clock to match the difference in repetition rates
[26,42,44].
Both the digital phase/timing correction and the analog adap-
tive sampling do require low-bandwidth active feedback so that
the detected error signals and interferograms remain within useful
frequency windows, but they avoid the experimental challenges
associated with high-bandwidth active feedback. Analog adaptive
sampling can be implemented with readily available rf electronics,
Fig. 6. Spectral SNR versus bandwidth for DCS demonstrations in but digital phase/timing correction is more powerful, since it can
the near-IR (NIR; yellow triangles) and mid-IR (MIR; red triangles).
take advantage of modern FPGAs and is readily extended to long-
In the near-IR, data points include only experiments that enforced mu-
tual coherence through either active phase/timing feedback [25], digital term coherent averaging, discussed next.
phase/timing correction [24], or analog adaptive sampling [42]. The solid D. Coherent Averaging: DCS Acquisition over Hours
triangles indicate that coherent averaging was implemented. Approximate
and Days
regions of operation for FTIR and tunable laser spectroscopy (TLS) are
added in blue. The number of spectral elements M is the bandwidth∕f r , When acquiring DCS data over times greater than a few seconds,
where f r is ∼100 MHz for most demonstrations shown here. two problems arise: data overload and interferogram dephasing.
 Review Article Vol. 3, No. 4 / April 2016 / Optica 423

The solution is to implement real-time coherent averaging, as de- coherence at short times with a high effective bandwidth, imple-
scribed below. Coherent averaging (the analog of co-adding inter- ments a real-time interferogram-based phase correction at update
ferograms in FTIR) has been demonstrated both using active times of 1∕Δf r , and finally implements real-time co-adding for
phase/timing feedback combined with post processing and using deep averaging.
real-time digital phase/timing correction implemented on an In the THz, the same need for coherent averaging arises. Here,
FPGA [19,22,24,25,36,39,43,47,50]. The former has allowed mutual coherence is easier to establish because of the longer wave-
for DCS across an open-air path that ran continuously for three lengths, and because it can be sufficient to stabilize the repetition
days [36]. The latter has enabled real-time, continuous coherent rate [6,7,11,12,39,45–47,49]. For THz signals, a Doppler lim-
averaging for 24 h with record levels of SNRs on both short time- ited absorption feature can be less than the comb spacing, but
scales (see Fig. 6) and long timescales, reaching an SNR of the coherent co-added interferogram preserves the resolution of
316,000 at 100 MHz point spacing [24]. the system to observe this fine structure [46].
To understand the problem of data overload, the direct 16-bit
digitization of both signal and reference interferograms at f r ∼
100 MHz generates 3 Gbits/s of data, presenting a significant 6. CONCLUSION
storage and processing challenge. The solution is to align the Frequency combs are an ideal source for broadband spectroscopy,
two frequency combs such that the interferograms will be iden- as they provide high frequency resolution, broad spectral cover-
tical and comprise an integer number of samples. (This condition age, and a high-brightness collimated beam. DCS fully exploits
is met if the repetition rates of both combs and the difference of these frequency comb properties to measure a sample’s complex
their f ceo frequencies are all integer multiples of Δf r ). In the case response on a comb tooth-by-tooth basis with only a single photo-
of active phase/timing feedback, this condition is accomplished detector. The most extensive demonstrations so far have been
via careful choice of the rf offsets in the four phase-locked loops conducted in the near-IR, where experiments have demonstrated
that control the combs. In the case of digital phase/timing cor- the full benefits of DCS of bandwidth, resolution, SNR, and ac-
rection, this condition is easily met by adjusting the interferogram curacy. While proof-of-principle experiments continue, near-IR
phase and resampling it essentially at will. In either case, sequen- DCS has also evolved to the point where it can be used as a tool
tial interferograms are then co-added point by point on an FPGA to support practical spectral measurements.
over a period up to 1 s, providing a factor of 100–1000 reduction Farther into the IR, DCS is still under development, as mid-IR
in data load [19,24]. Since the final coherently averaged interfero- combs have yet to match their near-IR counterparts in terms of a
gram is only 1∕Δf r in length in lab time or 1∕f r in effective time robust, affordable system that can provide high stability, coher-
(see Fig. 3), there may be a misconception that the spectral res- ence, and suitably wide spectral bandwidths. Nevertheless, there
olution is limited by this time window. This is not the case, as the has been much progress in this region, and DCS remains one of
coherently averaged interferogram is actually measured over a to- the primary motivations driving mid- and far-IR comb develop-
tal acquisition time t acq , and its Fourier transform is mathemati- ment. With continued development, one can speculate that in the
cally equivalent to streaming the entire time data to memory, future DCS will become a lithe, agile spectroscopic tool that could
Fourier transforming the time sequence, and then selecting only replace traditional FTIR in many applications both in the labo-
the power at multiples of Δf r . The resolution of each spectral ratory and in the field, enabling much greater resolution and sen-
point is then the larger of the comb tooth linewidth or the inverse sitivity in a much more compact system.
acquisition time.
After a second at most, the interferograms will drift out of Funding. Defense Sciences Office, DARPA (DSO);
phase because of phase/timing drifts between the two combs Advanced Research Projects Agency - Energy (ARPA-E); National
due to path length variations in the spectrometer that are not Institute of Standards and Technology (NIST).
detected in the comparison with the common reference lasers.
The solution is to apply a phase correction to the interferograms, Acknowledgment. We thank Adam Fleisher and Brian
as is traditionally done in FTIR [76] either in postprocessing Washburn for helpful discussions.
software [19] or as part of the real-time digital signal processing
[24]. In this approach, the phase at the center of each consecutive,
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