Li et al.

Light: Science & Applications (2023)12:164 Official journal of the CIOMP 2047-7538
https://doi.org/10.1038/s41377-023-01178-3 www.nature.com/lsa

ARTICLE Open Access

Nanoscale multi-beam lithography of photonic

crystals with ultrafast laser
Jiaqun Li 1
, Jianfeng Yan 1
, Lan Jiang2 ✉, Jiachen Yu1, Heng Guo1 and Liangti Qu3

Abstract
Photonic crystals are utilized in many noteworthy applications like optical communications, light flow control, and
quantum optics. Photonic crystal with nanoscale structure is important for the manipulation of light propagation in
visible and near-infrared range. Herein, we propose a novel multi beam lithography method to fabricate photonic
crystal with nanoscale structure without cracking. Using multi-beam ultrafast laser processing and etching, parallel
channels with subwavelength gap are obtained in yttrium aluminum garnet crystal. Combining optical simulation
based on Debye diffraction, we experimentally show the gap width of parallel channels can be controlled at nanoscale
by changing phase holograms. With the superimposed phase hologram designing, functional structures of
complicated channel arrays distribution can be created in crystal. Optical gratings of different periods are fabricated,
which can diffract incident light in particular ways. This approach can efficiently manufacture nanostructures with
controllable gap, and offer an alternative to the fabrication of complex photonic crystal for integrated photonics
applications.
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Introduction modulators, and resonators8–10. Photonic crystal struc-

Manipulation of light propagation is an interesting field tures in these optical devices are characterized as one-
in optics and optoelectronics1,2. As one of basic compo- dimensional (1D), two-dimensional (2D), and three-
nents of integrated photonics, photonic crystals play an dimensional (3D) according to lattice arrangements. Dif-
important part in the transmission and regulation of ferent from the 1D and 2D cases, the fabrication of 3D
light3–5. Photonic crystals are a kind of structure con- structure is rather difficult because the refractive index
sisting of a periodic array of uniform dielectric “atoms”. should be varied at three spatial directions11,12.
The uniform dielectric “atoms” can be air-filled holes, Laser lithography is one of potential techniques for 3D
channels, dielectric rods, and other structures which have structure fabrication in crystals. It is known that ultrafast
different refractive index with original materials. Due to laser is a versatile tool used for marking, cutting, pat-
the periodical arrangement of different refractive index terning, and structuring. Due to the ultrahigh intensity,
structures, photonic crystals behave a considerable ultrafast laser can overcome bandgap of crystals and
manipulation ability for light and photonics since its realize direct micromachining13. The ultrashort pulse
discovery6,7. Due to unique optical properties of photonic duration also makes ultrafast laser lithography a non-
crystals, photonics devices can be constructed including thermal processing method, which can be used in many
light emitting devices, optical receivers, switchers, applications like aerospace, energy14, and optoelec-
tronics15. Recently, femtosecond laser is employed to
fabricate photonic crystals because of its processing ability
Correspondence: Lan Jiang (jianglan@bit.edu.cn)
1
State Key Laboratory of Tribology in Advanced Equipment, Department of for micro-nanostructures16,17, especially three-
Mechanical Engineering, Tsinghua University, Beijing 100084, China
2
dimensional fabrication in transparent materials18. Fem-
School of Mechanical Engineering, Beijing Institute of Technology, Beijing
tosecond laser can induce physical and chemical changes
100081, China
Full list of author information is available at the end of the article in focus region due to well confinement of energy, which
These authors contributed equally: Jiaqun Li, Jianfeng Yan

© The Author(s) 2023

Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction
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Li et al. Light: Science & Applications (2023)12:164 Page 2 of 12

originated from the ultrafast properties19–21. Ultralow- The laser-affected region overlapping will induce sec-
loss geometric phase optical elements like prism, lens, and ondary processing, which limits the reduction of structure
vector beam convertors can be fabricated through a new size. Besides, the accuracy and stability of mechanical
type of laser modification inside silica glass22. After laser movement will influence fabricated structures. Multiple
processing, post-treatment like chemical etching23 and scanning requires accurate control over relative motion
annealing24 can help to form hollow structures in laser- between laser and crystals.
affected areas. Based on laser-induced structural changes, To improve the capacity of conventional single-beam
many photonic crystal structures can be fabricated in processing method, parallel laser processing techniques,
transparent dielectrics such as glass, sapphire, and such as microlens array fabrication (MLA) and laser
Lithium niobite25–27. A micro-structured optical wave- interference lithography (LIL), have been developed. MLA
guides was fabricated in a single-crystal by femtosecond lithography enables the rapid fabrication of large-scale
laser inscribing and acid etching, which can realize mid- micro/nano pattern arrays on substrate surfaces39,40.
infrared waveguiding with a low loss28. However, a single micro lens array can only produce a
The size and spacing of structure in photonic crystals specific multi-focus array. Micro lens arrays with varying
can greatly affect the performance of light manipulation29. morphologies and distributions must be fabricated for
To realize the control of light propagation, it is required different micro-nanostructures processing demand.
that the structure of photonic crystal is comparable to its Besides, it is required to design each micro lens if the focus
working wavelength. For photonic crystals with a bandgap of multi-beam field have a special distribution. LIL tech-
at microwave range, the characteristic size needs to be nique generates interference patterns of two incident laser
controlled at centimeters scale. A negative refraction beams and prints patterns onto materials to directly form
phenomenon of microwaves can be found in a metallic micro/nanostructure arrays41,42. While LIL offers the
photonic crystal, which is consisted with centimeters advantage of easily switching micro/nanomachining pat-
rods30. For Terahertz (THz) wave and midinfrared wave terns, it is generally limited to the fabrication of planar
range, photonic crystal structure should be micrometers. structures. Therefore, a processing method with 3D
An integrated platform was fabricated based on photonic manufacturing capability and easy adjustment is necessary.
crystal waveguides of micrometers lattice constant, which In this work, a multi-beam laser lithography strategy based
can be used in terahertz communications31. Studies have on beam shaping is proposed to realize customizable
shown the fabrication of photonic crystal with nanoscale three-dimensional nanostructure fabrication in crystals.
structure is important to realize visible and NIR light Here, we show parallel channels with nanoscale gaps can
manipulation32,33. be realized in yttrium aluminum garnet (YAG) crystal by
In femtosecond laser processing, the realization of tightly focusing of multi-beam femtosecond laser. The
nanoscale structure was mainly restricted by optical dif- multi-beam laser direct writing process is performed by
fraction limit. Recently, some works have reported the spatial light shaping with an optical phase hologram
fabrication of nanostructures at tens of nanometers by applied on a spatial light modulator (SLM). Laser-modified
laser direct writing lithography34. Nanogrooves with a region is etched to obtain hollow channel structures after
minimum feature size down to 30 nm can be formed direct writing. The distance between parallel channels can
directly on silicon surface with pulsed nanosecond laser be varied from hundreds of nanometers to several micros
irradiation35. Straight large-area nanoscale laser-induced by changing the SLM phase holograms distribution.
periodic surface structures was fabricated with two fem- Meanwhile, the laser fabrication efficiency is also pro-
tosecond laser beams36. These methods are still limited to moted due to the multi-beam parallel processing, which is
planar and non-transparent materials. The structure can demonstrated through 4-channels and 8-channels fabri-
only be fabricated on the sample surface. It is necessary to cation. Complicated channel arrays can be produced with
propose a more suitable method for the processing of multi-beams distribution control. This is achieved by
three-dimensional nanostructure inside crystals. To pro- superimposed phase hologram design. Based on the multi-
cess three-dimensional structures in transparent dielec- beam lithography method, optical devices like diffraction
trics, it is known that femtosecond laser-induced gratings are created in crystals. The diffraction test of
structure can break diffraction limit by tight focusing, fabricated gratings is consistent with theoretically analyzed
multiphoton effect, and other nonlinear processes37,38. results. This method allows precise and efficient fabrica-
These methods use conventional single-beam direct tion for nanoscale structure in photonic crystals.
writing and require multiple scanning. Thus, the laser
spot overlapping and movement accuracy are imperative Results
to be considered in femtosecond laser direct writing. In Multi-beam laser direct writing method
conventional single-beam processing, multiple scanning The principle and experiment detail of multi-beam laser
method is employed to fabricate complicated structures. direct writing was summarized and displayed in Fig. 1.
Li et al. Light: Science & Applications (2023)12:164 Page 3 of 12

a b (x) c
0 0.5d d

R 2
… … r2
0  0 0  2R
0
3R
Original light field

2R SLM
nR 2 R 2 2R 2 3R 2 4R 2
(x)
(x) Oil-immersed
 0.5d d N.A.=1.42
2  Phase hologram
x R1
0 R2 r
R3
0
 R4
2 –
x1 xn x1 +1 d xn +1 d Rn
R1 R2 R3 R4
2 2 Plane projection light field

d e xi

Ei (r,)

I Et (,)
r
ing

yi
nn

R x
ca
rs
se


La

z  E(x,y,z)
O L z
x P y F
y

Fig. 1 Schematic illustration of multi-beam processing in YAG crystal with SLM-based femtosecond laser system. a SLM holograms used to
generate a simple multi-beam light field. b Description of hologram phase for complicated light field. c Multi-beam light field shaping with
superimposed phase hologram. d Diagram of multi-beam scanning strategy. e Diagram of Debye diffraction integral, P represents the pupil,
L represents the objective lens, and F represents the focusing region

As shown in Fig. 1a, a Dammann grating phase was used to strategy. The laser energy of each beam is controlled
generate simple multi-beam light field. Adjusting the turn- higher than modification threshold of YAG crystal but
ing point of binary phase, the spacing and numbers of multi- lower than its ablation threshold. Thus, the laser scanning
beam focus can be controlled. Figure 1b presents the original process only induce structural change rather than mate-
and optimized Fresnel phase used to reorganize the multi- rial removal or ripple formation. After laser inscribing, all
beam focus spatial distribution. Combining Dammann the processed area was etched with acid to form channels.
grating phase and Fresnel phase, we apply the superimposed Our experiments utilized the transverse writing scheme
phase hologram onto SLM as Fig. 1c describes. A compli- which can abandon the constraints of the lens working
cated multi-beam light field consisted of 8-focus spots in x-z distance, despite asymmetric focus spot. Due to the non-
plane can be obtained. As Fig. 1d displays, a multi-channel circle laser focus spot, the cross-section of channels is not
array can be modified by using multi-beam scanning a standard circle. Figure 2 displays the etching result after
method in a transparent crystal sample. After laser scanning, traditional single beam and proposed multi-beam laser
the modification areas were etched by acid from hollow irradiation. A tightly focused light field was utilized to
channels which is detailed described in Method. To theo- form modified line tracks with a 20 μm s−1 scanning
retically analyze the multi-beam light field, Debye diffraction speed. Figure 2a shows the light field simulation and
integration was employed to calculate optical intensity dis- etched single channel after unshaped single beam laser
tribution in a tightly focused condition as Fig. 1e shows. processing. A single straight channel with about 1μm
width can be seen. The measured channel width is a little
Parallel channels fabrication with controllable nanoscale larger than the simulated diameter XAC. Figure 2b pre-
gap sents the etched double channels processed with a two-
The crystal is modified with conventional single beam beam light field. Channel 1 and Chanel 2 can be seen from
scanning method and our proposed multi-beam scanning top view of optical microscope, and quite distinct with
Li et al. Light: Science & Applications (2023)12:164 Page 4 of 12

a i
3.6
B b 1.8
E
ii i ii B
3.0 1.5

Intensity (a.u.)
Intensity (a.u.)
2.0 1.0

1.0 A C 0.5 C D
A F
0 0
A B C
0 –1.5 –1.0 –0.5 0 0.5 1.0 1.5 A BC DE F 0 –1.5 –1.0 –0.5 0 0.5 1.0 1.5
X (μm) X (μm)

iii iv iii iv

Gap
Channel 1

261 nm

Channel Channel 2

2 μm 2 μm 2 μm 2 μm

c
1 2 3 4 5 6 7 8 2π

Number of stripes

0
Channels and gaps

3 μm

d e
3.5 1.5 Gap width 1.6
Gap width 0.45
3.0 Channel width Channel width
1.4
1.4
Channel width (μm)

Channel width (μm)

2.5
Gap width (μm)

Gap width (μm)

1.3 0.40
2.0 1.2
1.2
1.5 0.35
1.1
1.0
1.0
Nanoscale gap 1.0
0.30
0.5 0.8
0.9
0
0.0 E = 1.6 mW K=4
0.8 0.25 0.6
2 4 6 8 10 12 14 16 0.05 0.10 0.15 0.20 0.25 0.30
Number of stripes Energy (mW)

Fig. 2 Demonstration of double-channel processing. a i) Simulated intensity distribution of single beam in x–y plane; ii) Intensity profile of single
beam; iii) top view optical micrography of conventional single beam processing result; iv side view optical micrography of conventional single beam
processing result. b i) Simulated intensity distribution of double beams in x–y plane; ii Intensity profile of double beams; iii) top view optical
micrography of double beams processing result; iv) side view optical micrography of double beams processing result. c SLM phase holograms and
experimental results for different stripe numbers K. d Measured gap and channel width against different stripe numbers K. e Measured gap and
channel width against different pulse energy

each other. The width of channel was measured ~0.7 μm. there is no apparent difference between two channels and
A narrow gap down to 261 nm width can be seen clearly their surrounding areas. Thus, we can infer the multi-
both in top view and side view image. The simulation beam parallel scanning strategy help to get uniform sub-
provides an estimate of gap width XCD, which is about wavelength photonic crystals structures without second-
200 nm. The calculation is almost equal to the experiment ary processing or mechanical fluctuations which displayed
result. The difference between simulated and experi- in Fig. S3.
mentally measured results is mainly due to that the energy Applying optical holograms on spatial light modulator
at CD points is lower than the modification threshold of allows to fabricate multi channels with a high freedom. By
crystal, resulting in the width of the actual etched area is changing the stripe numbers of binary phase mask holo-
smaller than the simulated value. It can be found that gram, the distance between two-beam focus spots can be
Li et al. Light: Science & Applications (2023)12:164 Page 5 of 12

adjusted. In Fig. 2c, we can see the gap width has a positive studied. Figure 3a displays Raman spectrum of unmodi-
correlation with stripe numbers of grating phases. When fied region and laser-modified tracks in crystals. There is
the stripe numbers increase from 2 to 16, the distance no apparent difference between laser-modified tracks
between two channel increases gradually. Figure 2d shows a (blue and red lines) and unmodified region (black lines) in
more detailed analysis for the gap width and channel size. most area. An intensity increment of the 403 cm−1 T2g
When the stripe numbers K are <8, the size of gap remains Raman mode can be found, which represents the increase
at nanoscale. With stripe numbers increasing, gap size of aluminum ion in octahedral site. In Fig. 3b, the Raman
behaves a linearly increasing relationship. Meanwhile, it can mode of laser-modified tracks behaves a slight blue shift
be observed that only K = 2 and K = 4 can obtain a channel (i.e., from 403.5 cm−1 to 404.1 cm−1) and FWHM
with width less than 1 μm. When the stripe numbers are 6, broaden (i.e., from 6.5 cm−1 to 9 cm−1 at 263 cm−1). The
the channel width has an abrupt promotion. The pulse two changes of Raman spectrum may imply the presence
energy during laser writing can also influence the gap and of lattice defects such as partial damage and bond broken
channel width. Figure 2e gives the result of processed in laser-processed crystal due to crystal transformation as
nanostructures with pulse energy varied from 50 to 300 nJ. previous research has reported in similar crystals43. The
The gap width has a negative relationship with pulse energy higher chemical reactivity caused by defects is the reason
when the channel width behaves positive. for the chemical etching rate difference between laser-
For larger size up to several micros, the relationship modified tracks and untreated region44,45. It can also be
between gap width and stripe numbers was summarized seen that the Raman spectrum of single-beam and 8-beam
in Fig. S4. There is an interesting phenomenon that the processed area tracks are almost the same.
gap width increases and the cross-section length decrea- X-ray photoelectron spectroscopy (XPS) was used to
ses when the number of interference stripes increases. It is characterize the chemical state of crystal components.
believed that the phenomenon can be explained by XPS intensity of Al2p spectrum in 8-beam processed
Fraunhofer diffraction theory and can be predicted with region and unmodified region are shown in Fig. 3c. The Al
Debye diffraction integral simulation. When the stripe ion spectrum of unmodified crystal can be divided into
numbers increase from 18 to 72, the distance between two contributions, the octahedral site (AlVI) and tetra-
adjacent channels increases from 6 to 18 μm. The hedral site (AlIV), located at respectively 74.27 eV and
experiment results taken from top view and side view are 73.78 eV. The relative ratio of peak area is 2:3, consistent
well consistent with optical simulation. Changing the with the unit cell of garnet structure. After laser inscrib-
phase value of hologram on SLM can adjust the relative ing, the peak area of AlVI was found to have an increase
size of two focus as Fig. S5 displayed. Based on channel when the peak area of AlIV suffered a decline. It can be
size and gap width control, a costumed binary mask attributed to the transformation of Al ions from tetra-
hologram can be designed, allowing the fabrication of hedral site to octahedral site, which is similar in the
microchannel arrays with arbitrary size and gap width. Raman spectrum results. The XPS intensity of 8-beam
To expand the efficiency and flexibility of multi-beam laser-modified region is almost the same as traditional
direct writing method, other Dammann grating phase single-beam written results. It means multi-beam pro-
holograms are designed to generate desired light field dis- cessed regions have no difference in structures or com-
tribution for more channels. Fig. S6 shows 2,4,8-beam light ponents with single beam fabricated one. Based on Raman
field simulation and processed results, respectively. Designed and XPS analysis, the uniformity (the interval of processed
Dammann grating phase holograms and corresponding light channels remains invariable) and stability of multi-beam
field simulation were presented. Applying the grating phase, direct writing method can be seen, which means the
two, four, and eight parallel tracks can be processed with approach can offer possibilities for efficient fabrication of
multi-beam direct writing. We show the laser-modified channel arrays with a determinant size.
tracks behave different refractive index compared to
untreated area, which can be seen as a darker region. After Complicated structure fabrication using superimposed
phosphoric acid treating, the dark region was etched to form SLM phase
hollow channels. From side and top view of optical image, Aiming to generate the more complicated light field, a
the cross-section of etched channels both shows a uniform superimposed SLM hologram was used. As Fig. 4a shows,
distribution. By using the N-beam light field, the efficiency a simple binary Dammann grating phase can be applied to
of laser scanning process was raised by N-1 times. get two-beam focus spots split along x-y plane. An opti-
mized blazed Fresnel phase can be calculated to generate
Discussion a spot away from the original focus plane along the pro-
Structure analysis of modified crystals pagating direction. When the two phase was combined,
In order to further validate the capabilities of proposed two focus spots deviated from the original position can be
method, structure changes of laser-modified areas are obtained in x-z plane. In Fig. 4b, we proposed a SLM-
Li et al. Light: Science & Applications (2023)12:164 Page 6 of 12

a b
8-Foci modified tracks (8-foci) Laser modified track
Eg T2g A1g
Laser modified tracks Unmodified region
Unmodified region
Peak 404.1 cm–1

Normalized intensity (a.u.)

Normalized intensity (a.u.)

FWHM=9.0 cm–1

Peak 403.5 cm–1

FWHM=6.5 cm–1

200 400 600 800 250 300 350 400 450

Raman shift (cm–1) Raman shift (cm–1)

c Unmodified YAG crystals Laser treated crystals, single beam Laser treated crystals, 8 beams

Al (2p) Al (2p) Al (2p)

Al (IV) Al (IV) Al (IV)
Al (VI) Al (VI) Al (VI)
Intensity (a.u.)

Intensity (a.u.)
Intensity (a.u.)

Al (Tetrahedral) Al (Tetrahedral)
Al (Tetrahedral)

Al (Octahedral)
Al (Octahedral)
Al (Octahedral)

77 76 75 74 73 72 78 77 76 75 74 73 72 71 78 77 76 75 74 73 72 71
Binding energy (eV) Binding energy (eV) Binding energy (eV)

Fig. 3 Structure characterization of multi-beam direct writing results. a Raman intensity spectrums of laser processed area and unmodified
region. b Enlargement of Raman intensity spectrums for wavenumbers from 230 cm−1 to 460 cm−1. c XPS intensity of multi-beam processed area
and unmodified region

split-use approach to generate aimed laser intensity dis- was found barely affected. For more channel array fabri-
tribution. The SLM was divided into several strip areas cation, the number of sub-SLMs should be expanded to
which can be used as sub-SLMs to apply different phase produce desired plane intensity distribution. It is worth
holograms. The strip width d1 and d2 can be adjusted to noting that other SLM-split-use approach can also be
balance the multi-beam focus intensity. used to generate superimposed light field as Fig. S8 pre-
In this experiment, Phase-A applied to SLM1 is a sents. In this case, each angle of sub-SLMs need to be
Dammann grating phase that can generate four-beam designed specially.
focus spots at focusing plane of objective lens. Phase-B As shown in Fig. 5, multi-channel arrays with different
applied to SLM2 is a superimposed phase combining a spatial distribution are processed. A parallelogram-
Dammann grating phase and a blazed Fresnel phase that distributed channels array is displayed in Fig. 5a. The
can generate two spots away from the focal plane. The surface morphology is experimentally captured. The
simulated optical intensity distribution of x-z plane for incident light can be coupled to the fabricated structure
each phase was shown in bottom right insert image. The from a corner (bottom left) and the output from another
ratio between d2 and d1 was set as 3:4. The final super- corner (top right) can be observed if the parameters are
imposed SLM hologram was shown in Fig. 4c. Debye specially designed. Figure 5b shows a rhombus-like
diffraction integration was done to simulate the optical channel array with a central unmodified area. The cen-
intensity of x-z plane. A combination of 4 beams in the tral area is surrounded by processed tracks and can serve
central part and 2 beams offset the focus plane can be as a cladding waveguide. Other waveguiding structures
seen. The intensity of S1 and S2 at x-y plane were also can also be fabricated with the multi-beam direct writing
calculated. Although each sub-SLM only diffracts part of method. A 2 × 4 spatial beam splitter structure is pre-
the incident laser, the focus result of each phase hologram sented in Fig. 5c. The incident light passing through the
Li et al. Light: Science & Applications (2023)12:164 Page 7 of 12

a Phase 1 Phase 2 Superimposed b

2π

d2
+ =
d1
0
1
Phase-A
⏐Exy⏐2
+ =
y

O x

⏐Exz⏐2
+ =
z 0
O x SLM 1 SLM 2 Phase-B

S2

S1
z

O x
Superimposed SLM phase X-Z plane intensity S2 intensity S1 intensity

Fig. 4 Schematic illustration of superimposed SLM holograms for complicated multi-beam generation. a Phase holograms and simulated
intensity for Dammann grating phase, Fresnel phase, and superimposed phase. b Diagram of SLM-split-use approach and phase holograms applied
to sub-SLMs. c Final composed SLM phase hologram and simulated optical intensity

binding waveguide structure can be divided into a 2 × 4 diffraction equation, the diffraction angle can be calcu-
light arrays of almost the same intensity. In Fig. 5d, a bulk lated almost coincide with the experimental results.
light divider based on evanescent coupling can be pre- Subwavelength grating can induce light response in a
pared by multi-beam scanning with varied channel spa- particular way which is different from traditional gratings.
cing. When the length of each channel satisfies the For a visible or near-infrared light luminescence source,
evanescent wave coupling condition, the incident light the characteristic size of subwavelength grating needs to
from a single input can be divided into two output beams be hundreds of nanometers. By applying multi-beam light
(~1:1 energy ratio). field with nanoscale beams interval, it can be seen a
subwavelength grating structure is obtained as Fig. 6c
Fabrication of diffraction gratings displayed. The insert image iii shows only 0th and -1st
The multi-beam processing approach provides poten- order diffraction green light can be observed after passing
tials of fabrication for a variety of photonic crystals ele- through the grating structure. The relative intensity of 0th
ments. Figure 6a shows a diffraction grating processed by and -1st order light is mainly dependent on the size of
8-beam light field. A multicolor distribution on the fab- grating structure channel elements and incident wave-
ricated crystal can be observed under a white light illu- length. Simulation of channel size influence based on nneff
mination. The fabricated grating consists of channels with was presented in Fig. 6d.
3.5 μm gap spacing as can be seen in insert image ii. Other optical elements like waveguide and beam splitter
Theoretically, the grating structure allows to diffract can also be fabricated using the multi-beam parallel
incident green light into 13 diffraction orders from -6th to processing method. A photonic crystals micro-structured
6th. Due to the weak intensity of higher diffraction orders, optical waveguide was shown in Fig. S10a schematically.
only -4th to 4th orders can be photographed in image iii. Hexagon distribution of hollow channels with size of
Varying the incident angle of illumination light, the dif- 1.2 × 0.6 μm2 can be seen and the central area with a
fraction angle of each diffraction order changes, which is diameter of 3 μm can be used to guide incident light. Fig.
recorded by a CCD camera in Fig. 6b. According to the S10b shows the simulation of intensity mode profile for
Li et al. Light: Science & Applications (2023)12:164 Page 8 of 12

L y 10 μm
x
D2 D1

10 μm
z y
x

c Out
z = +20 z=0 z = –20

L2

L1 20 μm
z y
x

z y 20 μm
x

Fig. 5 Design and fabrication of different complicated structures in crystals. a Plane and 3D schematics, optical microscope image for the
parallelogram-distributed structures. b Plane and 3D schematics, optical microscope image for the rhombus-like structures. c Plane and 3D
schematics, optical microscope image for a 2 × 4 beam splitter. d Plane and 3D schematics, optical microscope image for a light divider element

the waveguide under 800 nm light luminescence. The through phase distribution control. To process compli-
distribution of the mode electric field component and cated channel arrays, Blazed Fresnel phase was utilized to
power flow density with 800 nm light luminescence was reorganize the spatial distribution of multi-beam focus.
calculated in Fig. S10c. Combining the SLM-spilt use approach, superimposed
In summary, a multi-beam direct writing method fol- phase hologram was designed to fabricated complicated
lowed by etching is reported to realize nanoscale structure channel array structure with multi-layers. Based on the
lithography in crystals. The structure consisted of multi- method, optical gratings of nanoscale gaps were processed
channel arrays with subwavelength gaps. The laser direct which can diffract incident light in a particular way. The
writing process was performed by spatial light shaping with flexible control of nanogap between parallel channels
a SLM phase hologram. Dammann grating phase was used makes the approach an alternative to weave complex
to generate multi-beam light field which can modify the photonic crystals with subwavelength structure. The
area to be etched. Parallel channels with subwavelength potentials of multi-beam processing method may open
gap of 261 nm are created in YAG crystal. Gap width can possible ways to fabricate nanostructure for applications in
be varied by changing the interval between multi-beams optical communication and light manipulation.
Li et al. Light: Science & Applications (2023)12:164 Page 9 of 12

a c
i ii i ii

200 μm 10 μm 200 μm 4 μm

iii iii

–4th –3rd –2nd –1st 0th 1st 2nd 3rd 4th 0th –1st

b d
Theoretical 1
0° Experimental 0th order

Diffaraction efficiency
30° –30°

i 45°

60° i 30° –60°

–1st order
0.1
i 15°

i 0°
90° 0th –90° 1300 1400 1500 1600 1700
Channel height (nm)

Fig. 6 Demonstration and characterizations of processed optical gratings. a Gratings with a period of 3.5 μm. i) Grating image under white light
illumination. ii) Optical microscope image of fabricated long-period gratings structures. iii) Diffraction pattern with green light illumination. b Analysis
and test of fabricated gratings with illumination from different incident angles. c Grating structure with a subwavelength period of about 600 nm. i)
Grating image under white light illumination. ii) Optical microscope image of fabricated subwavelength gratings structures. iii) Diffraction pattern
with green light illumination. d Theoretical analysis of diffraction efficiency

Materials and methods annealing algorithm or global gradient method. In the

Phase holograms design second half period, the phase step coordinates can be
The multi-beam light field was generated by applying described by adding a π phase to the first half, as shown
holograms on a 1920 × 1080 pixels liquid-crystal spatial in equation (2). When a two-beam light field distribu-
light modulator (LC-SLM). To obtain a simple multi- tion is needed, the number of dividing lines N is 2.
beam laser beam, a binary Dammann grating phase was Calculated phase step coordinate x1 is 0.5 if we set the
applied to the liquid-crystal screen of SLM. The grating period d as 1. When a four-beam light field distribution
phase consists of two kinds of phase values (0 and π). The is needed, the number of dividing lines N should be 4.
variation of the multi-beam light field is achieved by The phase step coordinates x1, x2 are calculated as
changing the position of the phase value turning point. 0.22057 and 0.44563.
The position and the number of binary phase pattern To realize more complicated structure lithography in
dividing lines are designed specifically to realize control of crystals, a light intensity distribution at x-z plane or y-z
multi-beam distribution. On one-dimensional condition, plane is required. It is known that the position of light
when a single period of an even type Dammann grating is focus will have an offset along the propagation direction
irradiated by monochromatic light, the relative amplitude with a Fresnel phase. Fresnel phase is consisted with a
of each diffraction order can be described by series of concentric circles. The function of Fresnel phase
can be written as
n P
N=2
 
AðnÞ ¼ 1ð1Þ
πn ð1Þk expð2πnxk Þ π π r
k¼1 φFresnel ¼ þ  signum mod 40  20
φðxk þ d=2Þ ¼ φðxk Þ þ π 2 2 8 ´ 106

where n is the diffraction order, d is the period of where r is the location variable in polar coordinate.
Dammann grating, N is the number of phase pattern When a Fresnel phase was superimposed to the original
dividing lines in the first half period. Dammann grating phase, a planar light intensity dis-
In above equations, xk is the coordinate of the phase tribution in x-z plane was obtained. It can be found that
step, which can be solved numerically by simulated two focus spots split along the propagating direction.
Li et al. Light: Science & Applications (2023)12:164 Page 10 of 12

By optimizing the Fresnel phase distribution, the beam In above equation, Etx, Ety, Etz are three orthogonal
focus spot can only move away or approach along a single components of transmitted light passing through the
direction. The function of optimized blazed Fresnel phase objective lens in a cartesian coordinate system, when Eix,
used in the experiment is Eiy, Eiz are three orthogonal components of the
incident light.
 qffiffiffiffiffiffiffiffiffiffiffiffiffiffi 
2π Considering the focusing system satisfied Abbe’s sine
φBlazedFresnel ¼ ð f 2 þ r2  f Þ condition, the final electric field intensity can be described
λ 2π
as a function of wave vector k.
Z αZ 2π
Eðx; y; zÞ ¼ PðθÞE t ðθ; ϕÞ exp½iðk z z  k x x  k y yÞ sin θdϕdθ
Experimental setup 0 0

A SLM-based laser direct writing system is used in

The wave vector k is defined as kxex+kyey+kzez, where
experiment. The ultrafast laser source was an amplified
kx = −kcosϕsinθ, ky = −ksinϕsinθ, kz = kcosθ. If we let
Ti: sapphire femtosecond laser system, with a central
ξ = −cosϕsinθ/λ and η = −sinϕsinθ/λ, the above equation
wavelength of 800 nm, pulse duration of 35 fs and repe-
can be written as
tition rate of 1 kHz. A liquid-crystal spatial light mod-
ZZ
ulator was used to shape the laser intensity distribution by
Eðx; y; zÞ ¼ PðθÞE t ðθ; ϕÞ= cos θ ´ expðik z zÞ exp½i2πðξx þ ηyÞdξdη
applying phase holograms. A 4 f system consisted of two
convex lenses was utilized to eliminate the diffraction
which means the electric field intensity in the focusing
effect before laser focusing. The focus length of two
region is Fourier transformation of the transmitted field
convex lens is 400 mm. The shaped laser was tightly
intensity passing through the objective lens.
focused with an oil-immersed microscope objective. The
numerical aperture (NA) of objective lens was 1.42 and In this paper, light field simulation is based on above
the working distance was 0.15 mm. two equations. The phase and polarization information
are coupled into the incident laser distribution with a
Debye diffraction integration vector expression of light field. Three orthogonal com-
The light field distribution was simulated with vectorial ponents Ex, Ey, Ez at the focusing region can be obtained,
Debye diffraction theory for tightly focused condition. separately. The final optical intensity is the sum of the
According to the Richards-Wolf vectorial diffraction square of three components.
integration method, the electric field intensity of a certain
location in focusing region can be described as Laser lithography
A 10 × 5 × 0.5 mm3 YAG crystal with crystal orienta-
R α R 2π tion <111> was used in the experiment. The focused
Eðx; y; zÞ ¼ A 0 0PðθÞE t ðθ; ϕÞ expðikz cos θÞ sin θ ´
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi laser spot was controlled about 100 μm beneath the
expfik x2 þ y2 sin θ cos θ½arctanðy=xÞ  ϕgdϕdθ
surface. The refractive index of YAG crystal is 1.82 and
the refractive index of silicone oil we used is 1.42.
A is a constant determined by focus length and wave- Considering the refractive index difference between
length, P(θ) is apodization function, and wavenumber k is YAG crystal and silicone oil, the depth of laser focus
defined as 2π/λ. θ is refraction angle of objective obtained spot can be calculated as 100 × 1.82/1.42 = 128 μm. In
by formula sinθ = rNA/(Rnt), where R is beam radius at the experiment, the line scanning process was per-
the incident pupil, NA is the numerical aperture of formed in a plane perpendicular to the laser propaga-
objective, and nt is the refractive index of focusing med- tion direction. Fig. S1 displays the relationship between
ium. r and ϕ is the polar coordinates at the incident plane. processed tracks and pulse density, which is determined
x, y, z is the cartesian coordinates in the focusing region. by line scanning speed. To get a consecutive and uni-
Et (θ, ϕ) describes the transmitted field of incident light form modified area, the scanning speeds of laser were
passing though the objective lens, which can be calculated set as 20 μm s−1.
with the incident light field intensity Ei (r, ϕ). In the actual The laser scanning process is performed in liquid
calculation, the transmitted intensity Et (θ, ϕ) can be environment. The interface between oil and crystal may
described by cause fluctuations of laser light field and discontinuity
2 3 2 32 3
E tx 1 þ ðcos θ  1Þcos2 ϕ ðcos θ  1Þ cos ϕ sin ϕ  sin θ cos ϕ E ix
6 7 pffiffiffiffiffiffiffiffiffiffi6 76 7
4 E ty 5 ¼ cos θ4 ðcos θ  1Þ cos ϕ sin ϕ 1 þ ðcos θ  1Þsin2 ϕ  sin θ sin ϕ 54 E iy 5
E tz sin θ cos ϕ sin θ sin ϕ cos θ E iz
Li et al. Light: Science & Applications (2023)12:164 Page 11 of 12

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