Optics & Laser Technology 135 (2021) 106687

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Optics and Laser Technology

journal homepage: www.elsevier.com/locate/optlastec

Review

Femtosecond laser-based processing methods and their applications in

optical device manufacturing: A review
Xiaoduo Wang a, b, Haibo Yu a, b, *, Peiwen Li a, b, c, Yuzhao Zhang a, b, d, Yangdong Wen a, b, d,
Ye Qiu a, b, d, Zhu Liu a, b, YunPeng Li a, e, Lianqing Liu a, b, *
a
State Key Laboratory of Robotics, Shenyang Institute of Automation, Chinese Academy of Science, Shenyang 110016, China
b
Institutes for Robotics and Intelligent Manufacturing, Chinese Academy of Sciences, Shenyang 110016, China
c
Northeastern University, Shenyang 110016, China
d
University of Chinese Academy of Sciences, Beijing 100049, China
e
Criminal Investigation Police University of China, Shenyang 110016, China

A R T I C L E I N F O A B S T R A C T

Keywords: The unique advantages of surface and volume processing enabled by femtosecond laser fabrication makes it one
Femtosecond laser processing of the most powerful tools for manufacturing optical and photonic devices based on complex three-dimensional
Parallel processing structures with diverse functions. In this review, we focus on the recent advancements of femtosecond laser
Microlens array
fabrication technologies and their versatile applications in different fields (e.g., nanotechnology, soft robotics,
Micro/nano grating
Photon crystal
optics, and optoelectronics). Herein, the characteristics and development of laser direct writing, spatial light
Optical fiber modulator-based fabrication and interference-based approaches are reviewed. Furthermore, typical applications
and approaches related to the manufacturing of cutting-edge optical devices including microlens arrays, micro/
nano gratings, photonic crystals, and optical fibers are summarized. Finally, the current challenges and emerging
trends of this technology are discussed.

1. Introduction
The rapid developments in optics, nanophotonics, optoelectronics,
biomedical engineering, and bionics have imposed higher requirements
for the fabrication of micro/nanodevices. Lithographic technologies
(such as those based on ultraviolet curing, e-beam, and X-ray), injection
molding, and nanoimprinting have been successfully adopted for
patterning small structures that show excellent performance. However,
these methods suffer from complicated three-dimensional (3D) fabri­
cation processes, inability to integrate several components within a
given material, and restrictions in surface design [1,2]. The femtosecond
laser technique, as a new manufacturing tool, provides the advantages of
high precision, flexibility, mask-free processing, and the ability to pro­
cess a wide range of materials. It can facilitate flexible and efficient 3D
fabrication with sub-micrometer feature sizes, which can meet the re­
quirements of specific applications better, and thus furthers the ongoing
trends of functionalization, miniaturization, and integration.
The invention of femtosecond laser has changed tiny structure and
ultra-fast physical processes appear, and it provides precise instruments
for basic research and practical application in the fields of physics,
chemistry, biology, and medical engineering [3–5]. The ultrashort pulse
duration and ultrahigh peak power (1012 to 1015 W/cm2) of a femto­
second laser provide unprecedented extreme physical conditions for
scientific experimental research, such as high temporal resolution, high
electric and magnetic field intensity, high pressure, and high tempera­
ture[6–9]. Owing to these characteristics, femtosecond lasers are mainly
applied in two fields: time-resolved spectroscopy based on the femto­
second time scale and micromachining of materials based on the high
laser power density. Since the peak power of a femtosecond laser reaches
1020 W/cm2, the intensity of the generated electromagnetic field ex­
ceeds the Coulomb field intensity of the electrons around the atomic
nucleus, and so it can inject energy into the highly spatially selected
regions of the material in a shorter duration than lattice thermal diffu­
sion can (10-12 s scale); this opens up related research fields such as
controlled nuclear fusion, laser plasma physics, and laser micro/nano
processing. During the micro-modification of materials, the electrons
surrounding the nuclei of atoms can be stripped off by the highly
concentrated energy of the femtosecond laser [10]. Moreover, highly
spatially selective microstructure modification is realized owing to the
nonlinear effects of the femtosecond laser, including multi-photon

* Corresponding authors.
E-mail addresses: yuhaibo@sia.cn (H. Yu), lqliu@sia.cn (L. Liu).

https://doi.org/10.1016/j.optlastec.2020.106687
Received 2 July 2020; Received in revised form 29 September 2020; Accepted 12 October 2020
Available online 14 November 2020
0030-3992/© 2020 Elsevier Ltd. All rights reserved.
X. Wang et al.
absorption and multi-photon ionization, which endow the materials
with unique optical functions. Recently, an increasing number of studies
have focused on the micromachining of microlens arrays, photonic
crystals, optical waveguides, and gratings, which have significantly
promoted the development and application of micro-/nano-optical
systems, micro-optical sensors, and other devices.
This review is focused on the latest advancements of femtosecond
laser micromachining that particularly emphasizes the optics of the
systems and the applications on optical devices. The paper is organized
as follows. Section 2 introduces the principles of different femtosecond
laser processing processes on different kinds of materials. Section 3
illustrated the optical technologies to improve the femtosecond laser
processing efficiency, resolution and dimension. The latest advancement
of the smart material fabrication and the spatiotemporal focusing
technology are introduced in detail. Section 4 reviews the various op­
tical devices processed by femtosecond laser and the corresponding
applications, including microlens arrays, micro/nano gratings, photonic
crystals and optical fibers. The advantages and disadvantages of various
approaches are analyzed, as well as the challenges. Finally, the pre­
vailing challenges and future prospects are given in section 5.
2. Physical mechanisms for femtosecond laser processing
To efficiently implement laser-based processing for the construction
of structures with desired resolutions, it is necessary to understand the
fundamental physical mechanisms of femtosecond laser-material in­
teractions [11]. For the femtosecond laser ablation of materials, a
thermal damage model that focuses on thermal damage caused by im­
purities and defects in samples has been studied comprehensively [12].
According to this model, the threshold limit of the thermally induced
damage of a material is proportional to the square root of the pulse
width, and is influenced by the intrinsic parameters of the material such
as its melting point, thermal expansion coefficient, thermal conductivity
coefficient, and tensile strength. The two-temperature model proposed
by Anisimov et al. is widely used to discuss the various phenomena of
metal ablation by a femtosecond laser [13,14]. Gamaly et al. claimed
that the ablation mechanisms for metals and dielectric materials are the
same when the intensity of the femtosecond laser is greater than or equal
to 1014 W/cm2; they also theoretically deduced and experimentally
verified the ablation threshold value and ablation velocity formula of
the metal and dielectric material [15,16]. The interaction between a
femtosecond laser and a transparent dielectric material is explained by
the avalanche model. A complex secondary process of high-temperature
and high-pressure plasma at the tightly focused laser point would induce
a phase or structural modification of the material [17]. Jia et al.
calculated the avalanche rate and photoionization rate based on the
fluster-double model and Keldysh theory, respectively [18]. Qiu et al.
classified the micro/nano-structures induced in transparent materials
into four types based on optical coloration, refractive index modifica­
tion, micro-hole creation, and micro-crack creation [19]. Two-photon
absorption is a kind of third-order nonlinear optical process that oc­
curs between the medium and light field of a femtosecond laser through
the absorption of photon energy. The two-photon polymerization(TPP)
occurs when the photoinitiator-activated free radical induces monomers
in the resin or hydrogel to polymerize, and the monomers or high con­
centration oligomers cross-linked to form a cured “point”. Owing to the
nonlinear absorption of energy during the interaction with a transparent
material, the spatial position of two-photon polymerization is selective
in bulk material and the fabrication resolution depends on the laser
energy, exposure duration, and concentration of the free radical [20].
Despite various models and explanations of femtosecond laser-
material interaction, most only reveal partial dynamics to rationalize
specific experimental phenomena. Direct visualization of the dynamics
evolution of the femtosecond laser-material interaction process [21] is
of fundamental importance for establishing a complete theoretical basis
for fine-scale and multifunctional femtosecond laser micromachining
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Optics and Laser Technology 135 (2021) 106687
and is worthy of more attentions.
3. Femtosecond laser fabrication systems and methods
Femtosecond laser micromachining can be classified into two types:
(i) femtosecond laser direct writing and (ii) femtosecond laser parallel
micro/nano processing. The basic concepts, characteristics, and impor­
tant optical components of the two types are described in detail in [22].
Since the lateral resolution of micromachining is inversely proportional
to the numerical aperture of the objective lens, achievable resolution
increases with an increase in the numerical aperture. However, the
trade-off between working distance and resolution should be taken into
consideration in specific applications. For instance, for surface pro­
cessing, an oil-immersed objective lens with a large numerical aperture
can be adopted to improve resolution, while for 3D machining carried
out inside a thick sample (such as optical waveguides and microfluidic
channels) where long working distances are required, it is reasonable to
employee an objective lens with a numerical aperture of ~0.5 [22].
Meanwhile, the cross-section of the focused spot of the femtosecond
laser is usually ellipsoidal with a large aspect ratio, leading to lower
axial resolution and making it difficult to meet the circular section re­
quirements in applications. Placing a slit oriented parallel to the scan­
ning direction before the objective lens can greatly reduce the aspect
ratio of the hollow microchannel [23,24]. However, the efficiency with
which the femtosecond laser energy is utilized is low and the orientation
of the slit should be adjusted along with the scanning direction. He et al.
controlled the cross-section of microfluidic channels by the temporal
focusing of the femtosecond laser pulse [25]. The simultaneous spatial
and temporal focusing of femtosecond pulses is realized by spatially
separating the spectral components of femtosecond laser pulses in space
before the pulses enter the objective lens and then overlapping at the
spatial focal point focus of the objective lens. The shortest pulse duration
is confined to the spatial focus, facilitating a symmetric spherical light
intensity distribution and improved axial resolution. At the same time,
this approach can be used to achieve large-scale femtosecond laser
micromachining with high resolution. In contrast, it is necessary to
improve the aspect ratio of hollow microchannel for some potential
application in microfluidics. By combining temporally shaped [22] laser
pulse and spatially shaped femtosecond laser Bessel beam pulse, Lu et al.
enhanced the etching depth of the microchannel by a factor of 13, which
realized the high-throughput fabrication of an ultra-high-aspect-ratio
hollow microchannel [26]. The underlying transient dynamics of the
spatio-temporal shaped femsecond laser pulses in nanoscale structuring
are described in [27,28].
3.1. Femtosecond laser fabrication through direct writing
The fabrication of two-dimensional (2D) and 3D microstructures by
femtosecond laser direct writing are usually realized in two ways, either
through the movement of the 3D transform stage or through a galva­
nometer combined with the transform stage. The former approach is
applicable to array machining and applications where high precision is
not strictly required [29,30]. Efficiency can be improved through the
line scanning of the Bessel Beam [31]. However, it is still very slow to
achieve rapid and flexible micromachining of complex microstructures
at a large scale.
Owning to highly developed high power, high repetition frequency,
and miniaturized femtosecond laser, scanning galvanometers and piezos
are adopted to achieve high throughput and high resolution micro­
machining both axially and laterally, which is beneficial for the
commercialization of femtosecond laser micromachining. Through the
two-photon polymerization technique, it is simple to construct complex
mesoscale 3D microstructures with nanoscale precision; for instances,
entire hollow devices [32] and spiral phase plates [33]. The maximum
achievable height is 8 mm with a commercial femtosecond laser TPP
system, while the lateral and axial resolutions are 100 and 200 nm,
X. Wang et al.
respectively. Femtosecond laser ablation and modification on extensive
materials have been achieved to form various porous network micro­
structures [34], hierarchical structures [35], nanogrooves, nanoholes
[36], and 3D resonant optical cavities [37,38], which are widely used in
applications such as hydrophilic and hydrophobic treatments, optical
communication and sensors and biomedicine. However, high-resolution
processing is always limited to oil-working conditions, making it un­
suitable for biomaterials (e.g., cells and tissues). Recently, a spatial
resolution of less than 20 nm in an atmospheric environment was ach­
ieved through a far-field-induced near-field breakdown nanowriting
approach, opening a new avenue for the industrial micromachining of
nanopatterns with femtosecond laser [36].
Moreover, femtosecond laser direct writing is becoming an appealing
tool for the construction of large-scale multi-functional smart materials
with 3D gradient densities that can be widely employed in the pro­
cessing of four-dimensional (4D) smart sensors, actuators and soft ro­
bots. Hydrogels are soft materials with high biocompatibility and
deformability, and widely used in biomedicines, soft sensors and soft
robotics [39] . By programming the scanning path, step length, and
exposure dosage at each printing voxel in a poly(ethylene glycol) dia­
crylate (PEGDA) hydrogel, Sun et al. tailored the 3D gradient cross­
linking density [40] and flexibly controlled both the 3D morphology and
3D interconnected network of microstructures to fabricate 3D micro­
actuators (Fig. 1a) [41]. Similarly, Duan et al. modulated the cross­
linking density, stiffness, and the degree of deformation of smart stimuli-
responsive hydrogels by adjusting the femtosecond laser pulse dosage to
construct 4D reconfigurable micromachines (Fig. 1b). A series of micro
claw-like actuators and LEGO-like programmable micromechanical de­
vices were also fabricated [42-44]. These studies showed the great po­
tential of femtosecond laser smart processing in the development of 4D
smart microrobots.
3.2. Parallel processing systems and methods
To make the fabrication of complex microstructures more efficient
Fig. 1. Design principle and femtosecond laser fabrication of smart materials with a three-dimensional gradient density. (a1) Schematic illustration of dual-3D
femtosecond laser nanofabrication technology that permits reversible deformation. (a2) Design and processing of smart microflower by dual-3D nanofabrication
technology. Copyright © 2019, American Chemical Society. (b1) Schematic illustration of 4D femtosecond laser fabrication of reconfigurable compound micro­
machines. (b2) Design of smart microcrawler actuator by crosslinking densities modulation. Copyright © 1969, Elsevier.
3
Optics and Laser Technology 135 (2021) 106687
and flexible, various methods have been developed, including multi-
focus parallel processing through optical modulation and diffraction,
structured light, photolithography based on a digital micromirror
deviced (DMD), and a liquid crystal spatial light modulator (LC-SLM).
Among them, methods based on DMD and SLM can dynamically
modulate the graphics of processing to meet the needs of most appli­
cations, and are widely used. Meanwhile, cross-scale high throughput
processing with submicron resolution can be achieved through a
spatiotemporal synchronization focusing approach.
3.2.1. Femtosecond laser processing based on DMD
The light sheet can ben modulated into arbitrary 2D patterns through
a DMD, enabling high throughput processing of large-scale microstruc­
tural arrays. It is worth noting that the light sheet irradiant on the DMD
should be shaped into a spatially homogenized flat-headed beam
[45,46]. Meanwhile, owing to the high coherence of femtosecond lasers,
micromirror arrays on DMD also works as a diffraction grating. In ap­
plications where super-resolution is not required, an objective lens with
moderate magnification could be selected to obtain a larger field of view
and patterned area. Owning to the unique advantages of DMD, femto­
second laser processing based on DMD is of high-throughput, high-
contrast, rapid-response, and easy-to-use. In terms of patterning pro­
cessing, single-pulse fabrication of the complex microstructure arrays
has been demonstrated [45]. The fabrication efficiency of this method is
improved significantly while the feature size is maintained at the
wavelength-scale [46]. Moreover, the combination of DMD and digital
holography technology can realize the flexible modulation of light
amplitude and phase, enabling the printing of various complex 3D
structures with high resolution in an efficient manner [47,48]. Recently,
a novel DMD-based spatiotemporal synchronously focusing addictive
manufacturing approach was proposed (Fig. 2a1). This approach en­
ables the realization of high-throughput parallel machining of arbi­
trarily complex 3D structures with super-resolution. Compared with
existing TPP technologies, the printing speed is 1,000 times higher, and
the axial resolution could be 175 nm [49], as shown in Fig. 2 (a2).
X. Wang et al. Optics and Laser Technology 135 (2021) 106687

Fig. 2. Parallel processing systems: optical systems, principle and experimental results. (a1), (b1) Illustrations of optical systems and principles for parallel pro­
cessing systems based on digital micromirror devices (DMD) and liquid crystal spatial light modulator (LC-SLM). (a2) Printing results of various complex three-
dimensional (3D) structures with sub-micrometer resolution using the system of a1. Copyright © 2019, The American Association for the Advancement of Sci­
ence. (b2) Various 3D microcages fabricated with the dynamic holographic processing technique using the system of b1. Copyright © 2019 American Chemical
Society. (c1) Optical system and principle for spatiotemporal synchronization focusing technology based on dual-grating. Copyright © 2018 WILEY-VCH Verlag
GmbH & Co. KGaA, Weinheim. (c2) Large-scale 3D hand model with an embedded microfluidic channel fabricated with the spatiotemporal synchronization focusing
technology shown in c1. Copyright © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

However, the diffraction of the incident laser on the DMD leads to a
significant loss of energy, necessitating the power of the femtosecond
laser to be significantly high. For instance, when the incident angle of a
femtosecond laser with a wavelength of 800 nm on the DMD surface is
57◦ , and the blazing angle is 33◦ , the energy of the blazed beam at order
m = 5 is 75% of the incident laser beam. Moreover, owing to the
reflection of the laser from the DMD surface and the energy loss due to
the gaps between the micromirrors, the energy of the laser irradiating
the sample is less than 44% [46].
3.2.2. Femtosecond laser processing based on LC-SLM
Instead of the amplitude modulation by DMD, LC-SLM modulates the
phase of the light field by varying the distribution of liquid crystals, and
the utilization rate of the light energy by an LC-SLM is higher. The
combination of LC-SLM with femtosecond laser was first proposed by
researchers from Tokushima University [50]. As a flexible micro-
patterning approach, SLM-based femtosecond laser processing has
attracted immense attention in recent years. Both the holographic al­
gorithm [51] and fabrication approaches [52–54] have been improved
to achieve the desired patterned beam in order to improve the accuracy,
efficiency and resolution of the LC-SLM based femtosecond laser pro­
cessing. Structured laser micromachining provides a rapid and flexible
solution for building special microstructures. Taking advantage of the
regular intensity distribution and the diversification of controllable
parameters, a Matthew beam is generated by the phase SLM to fabri­
cated complex microcages [55], as shown in Fig. 2(b1) and (b2). Taking
advantage of the non-diffracting high-quality beam, Bessel beams with
various kinds of shapes [56] were modulated to fabricate high aspect
ratio microtubes [57], hollow microhelical structures [58], and chiral
rotating microstructures [59].
DMD and LC-SLM based femtosecond laser processing can realize the
graphic fabrication of arbitary structures with high speed and flexibility.
However, the challenge for both approaches is that it is difficult to
achieve high precision and large size simultaneously in TPP applica­
tions. This is because TPP usually occurs in the bulk volume of a sample,
the square of the axial size of the focal spot is inversely proportional to
the numerical aperture, while the working distance of the objective lens
with a high numerical aperture is usually short. The spatiotemporal
synchronization focusing technology proposed by Cheng et al. can
realize the shortest laser pulse width and the highest laser intensity at
the focus of the objective lens synchronously, thus effectively improves
the resolution of large-scale 3D microstructures (Fig. 2c1) [60,61].
Through this method, a 3D transparent hand of 3 × 2.7 × 1.1 cm3
containing a complete microchannel vascular system was fabricated
(Fig. 2c2) with micro-resolution [62]. Overall, the efficiency, volume,
resolution, and flexibility of femtosecond laser fabrication have been
improved to allow for commercial applications.
3.3. Femtosecond laser micromachining via interference
Micromachining of periodic structure with a femtosecond laser has
shown great potential in fields such as bionic robots, photonic crystals,
and high-density information storage. Owing to excellent coherence
throughout the pulse duration, femtosecond laser interference provides
sufficient energy density for micromachining [63]. Consequently, large-
scale periodic micro/nano structures can be etched or induced directly
on the surface of hard materials or within transparent materials. The
period, morphology, and dimension of the structures can be tuned by
adjusting the laser energy, angle of incidence, number of interference
beams, focal length of the focusing lens, exposure time, laser wave­
length, and other parameters. Generally, splitting lenses and gratings are
used to generate the interference beams. To make the system simple,

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X. Wang et al. Optics and Laser Technology 135 (2021) 106687

stable, and applicable, coaxial interference of a vortex beam and plane
wave was proposed to produce 3D spiral optical fields, and chiral mi­
crostructures were realized in an isotropic material, as shown in Fig. 3
(a1), (a2), and (a3) [59]. For efficient and flexible surface patterning, a
Michelson interferometer-based femtosecond laser spatiotemporal
interference approach was proposed, and by controlling the phase-
difference with an SLM, a custom-designed gray-scale patterning on a
bulk material could be achieved with a single laser pulse (Fig. 3b1, b2,
and b3) [64]. Direct femtosecond laser interference patterning has been
adopted in nanoparticles size distribution tailoring [65], multi-
functional metal surface modification [63], and among others. While
fine adjustment of the optical system is required to achieve multi-beam
interference with a beam splitter, the multi-beam interference can be
realized more simply by grating, and the size of the interference area
generated by diffraction is similar to the size of the incident light
[66,67]. The advantages of femtosecond laser interference, such as
single-step processing, high efficiency, and controllable period, make it
an invaluable tool for building periodic functional micro/nano-
structures, which could be widely applied in information storage,
biomedical engineering, and metamaterials.
4. Applications in optical devices fabrication
4.1. Microlens arrays
Owing to the advantages of small volume, low cost, and distinctive
optical performance, microlens arrays have been playing an irreplace­
able role in fields of light modulation [68,69], optical sensors, and
integration of optical systems [70]. Microlens fabrication approaches
based on a femtosecond laser can be categorized into three main
branches: subtractive fabrication, additive fabrication, and laser-
induced modification.
To achieve the subtractive fabrication of microlens arrays on hard
materials with a femtosecond laser, additional auxiliary techniques are
required to produce microlenses with smooth surfaces and high imaging
performance, as shown in Fig. 4(a). Assisted by subsequent wet etching
(such as HF solution) and dry etching (such as induction coupling
plasma [71]), femtosecond laser ablation can process large-scale
concave microlens arrays [72], lens-on-lens arrays [73], and plano-
convex cylindrical microlens arrays [74] on plane surfaces, as well as
3D-light-modification-based concave microlens arrays on concave sur­
faces [75]. The additive fabrication of microlens arrays is mainly real­
ized through the TPP of the femtosecond laser. Recently, biomimetic
protein-based microlenses fabricated by TPP have exhibited dynami­
cally tunable focal distance when stimulated by external stimuli [76],
unique stretchability, good biocompatibility and biodegradability [77],
as shown in Fig. 4(b). The surface roughness of microlenses fabricated
by dry-etching-assisted femtosecond laser processing can be approxi­
mately 1.5 nm, which offers the potential for application to integrated
optical systems where high imaging performance is required [78]. The
fabrication of microlens arrays on soft substrates requires the combi­
nation of femtosecond laser micromachining, wet/dry etching, and
nano-imprinting [79]. For instance, through the combination of single-
pulse femtosecond laser wet etching and thermal embossing, large-scale
dragonfly-eye-inspired artificial compound eyes with sophisticated im­
aging capability have been constructed [80]. The subtractive and ad­
ditive fabrication approaches are efficiency, flexible, and applicable to
most materials while the fabrication processes are complex. The laser-
induced modification approaches for microlens fabrication are neither
additive nor subtractive, and they offer a cost-effective solution for mass

Fig. 3. Micromachining of femtosecond laser interference via various interference approaches. (a1), (b1), Optical systems for interference via coaxial beams split by
a spatial light modulator (SLM) and Michelson interferometer split by a splitting lens, respectively. (a2), (b2) Simulation of the interference of the two beams
corresponding to (a1) and (b1). (a3) Scanning electron microscopy (SEM) images of the microscale letters of ‘L’ (left) and ‘R’ (right) arranged with left- and right-
handed microstructures fabricated using system in (a1) Copyright © 2017, Springer Nature. (b3) SEM images of the crosslinked micro/nanopatterns. Copyright ©
2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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X. Wang et al. Optics and Laser Technology 135 (2021) 106687

Fig. 4. Microlens arrays fabricated using different approaches. (a) Subtractive fabrication of microlens arrays: illustration of an optical system and the fabrication
process (left, Copyright © 2015 Optical Society of America), an artificial compound eye consisting of a microlens array (middle, Copyright © 2016 WILEY-VCH
Verlag GmbH & Co. KGaA, Weinheim) and the imaging performance of a compound microlens array (right, Copyright © 2018 Optical Society of America). (b)
Biomimetic protein microlenses fabricated by two-photon polymerization with the optical system for two-photon polymerization of protein (left), soft stretchable
microscale phase-type lens fabricated by femtosecond laser (middle), and protein-based microlens with a tunable focal distance (right). Copyright © 2014 WILEY-
VCH Verlag GmbH & Co. KGaA, Weinheim. Copyright © 2014, Springer Nature. (c), (d) Microlens arrays fabricated by a route that is neither additive nor subtractive.
(c) Schematic fabrication of polymeric microlens arrays by direct laser printing (left) and the printed microlenses with different sizes (right). Copyright © 2016
American Chemical Society. (d) Schematic of fabrication of quasi-three-dimensional (3D) microlens array by laser induced dot deformation (left), and experimental
results for a convex-concave microlens array (right). Copyright © 2016, Springer Nature.

manufacturing. For example, tailored polymeric microlenses with
tunable geometry and size can be printed by the femtosecond laser-
induced forward transfer method illustrated in Fig. 4(c). Benefiting
from the surface tension of the microdrops, the root-mean-square error
values of the microlens surface could be λ⁄27 (on a polydimethylsiloxane
substrate) [81]. Furthermore, based on the laser-induced thermal
deformation of simple 2D patterns, complex quasi-3D surface structures
were fabricated and kaleidoscopic imaging patterns have been realized
(Fig. 4d) [82]. While most mcirolens arrays are fabricated by various
surface manufacturing methods, completely enclosed cavity [83],
concave, and convex [84] microball lens arrays embedded in trans­
parent bulk polymer have been realized through high repetition
femtosecond laser direct writing, which enabled super-wide angle im­
aging and is convenient for aligning with other optical devices beyond
submillimeter scale. The surface roughness of microlens arrays made by
laser-induced modification is much higher than those fabricated by
subtractive and additive approaches. However, the accessible shapes of
the mcirolens are limited.
Microlens arrays are widely used in parallel micromachining, optical
imaging, and illumination. To meet the high optical performances and
functionality of instruments such as endoscopes, illumination systems,
and miniature robots, ultracompact multi-lens objective lens arrays
were manufactured by femtosecond laser multiphoton lithography [85].
For optical beam shaping, double-sided microlens arrays with double-
axial hyperboloids and rotational displacement exhibit high homoge­
nization performance [86,87]. Owing to their excellent properties, (i.e.,
large field of view, high optical performance, small volume, tunable
focus lengths, and ease of integration with other systems), microlens
arrays have shown great potential in numerous applications, including
in flexible and stretchable photonics and optics, impact and multi-
functional lab-on-chips, intelligent robots, and biomedical devices.
4.2. Micro/nano gratings
An attractive application of femtosecond laser-based micro/nano-
processing is the processing of gratings. Several novel methods have
been proposed recently, including femtosecond laser direct writing,
direct laser interference patterning, laser induced periodic surface
structures (LIPSS), etc. With direct laser writing, the femtosecond laser
phase mask technique and fusion splicing technique were adopted in the
processing of phase-shifted fiber gratings [88,89]. Using the femto­
second laser overexposure technique, highly reflective negative-index
gratings [90] and highly birefringent fiber Bragg gratings [91] were
inscribed by a femtosecond laser. Moreover, shrinkable silver diffraction
gratings were fabricated by femtosecond laser-induced photoreduction
of silver ions inside PEGDA hydrogel [92]. It is flexible to fabricated
gratings of various dimensions and shapes using high resolution
femtosecond laser direct laser writing, however, the efficieny is low.
Direct laser interference patterning and LIPSS [93] are simple and
widely used approaches for the formation of micro and nanoscale
gratings on the surface with high efficiency. Through the interference
femtosecond laser stamping approach, microgratings with a period of 5
μm on a 100 nm thin film was achieved [94]. The gratings inscribed
through interference are of high quality while the resolution is relatively

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X. Wang et al.
low (~1 μm). LIPSS provides a mask-free, high resolution processing
procedure for micro/nano grating fabrication. To date, multiple works
on LIPSS formation have been conducted on various materials, including
metals [95-97]. The morphology of the periodic ripples can be improved
both through optimization of processing parameters [98] and sample
treatment [99]. The combination of femtosecond laser and chemical
etching can improve uniformity of micro/nano grating further, for
instance, cylindrically focused nonablative femtosecond laser process­
ing assisted by subsequently chemical etching can achieve extremely
long-range uniform gratings with high throughput and controllable
morphology [100]. Through the all-femtosecond-laser processing tech­
nology, 2D period Cu-Ag nanogratings inscribed inside 3D glass micro­
fluidic channel was realized and utilized as surface-enhanced Raman
spectroscopy (SERS) substrate [97]. Moreover, homogeneous nano­
gratings formed by the spontaneous self-organization process have been
realized for a wide range of materials [101,102]. The periods of the
nanogratings can be tens of nanometers. To meet the requirements of
various applications, more and more micro-nano gratings need to be
processed with two or more microprocessing techniques. The capability
of precisely controlling the dispersion and steering properties of optical
beams means that the micro/nano gratings have been applied in
numerous fields, for instance, optical sensors [97,103], optical com­
munications [104], and bionic robots [105]. The materials, processing
methods, lateral and axial structure resolutions, and applications of
several periodic structures processed by femtosecond laser are listed in
Table 1.
4.3. Photonic crystals
The special 3D dielectric structure of photonic crystals can generate a
band gap to prevent the propagation of electromagnetic waves of spe­
cific frequencies. This unique function equals the optical analogue of
semiconductor crystals, enabling the realization of integrated photonics,
and elevating the application potential of photonic crystals in wave­
guides [106], communications [107], lasers [108], and exciting mo­
lecular chemical reactions [109]. Femtosecond lasers have been applied
for photonic crystal processing owing to its excellent properties such as
high precision, high efficiency, 3D processing capability, and non-
polluting nature. In recent decades, intensive research efforts have
focused on the photonic crystal fabrication by femtosecond lasers. The
photonic bandgaps of photonic crystals produced by femtosecond laser
multiphoton polymerization has been extended from mid-infrared to
visible light [110,111]. To meet the requirement of synchronization of
the phases of interacting waves in applications such as ultrafast signal
processing, and terahertz technology, 3D spatial nonlinearity modula­
tion by a 3D nonlinear photonic crystal is needed. Recently, the fabri­
cation of a 3D lithium niobate nonlinear photonic crystal through
femtosecond laser selective erasing was experimentally demonstrated
Table 1
Periodic structures processed by femtosecond laser.
7
Optics and Laser Technology 135 (2021) 106687
[112], and nonlinear beam shaping was realized via nonlinear holog­
raphy using a femtosecond laser, which improved the fabrication effi­
ciency by two orders of magnitude compared with that achieved by the
traditional 2D technology [113]. In addition, 3D photonic crystals with
nonlinear phase matching along any direction were fabricated by
femtosecond laser domain inversion [114]. All-optical poling of ferro­
electric barium calcium titanate 3D photonic crystal was achieved for
domain reversal inside a crystal with non-standard crystallographic
orientation. The ferroelectric barium calcium titanated 3D nonlinear
photonic crystal was used to demonstrate the nonlinear wavefront
shaping capability [115] (Fig. 5). The 3D nonlinear photonic crystal can
offer all spatial degrees of freedom of phase mismatch compensation
during nonlinear wavefront shaping, which offers potential for the op­
tical modulation of light beams. In terms of application, based on the
color-changing laser-induced periodic surface structure [116], strain
sensor [117], protein hydrogel-based selective detector, and uranyl ion
monitoring [118] have been realized. The photonic crystal makes real­
ization of the all-optical and micro-nano integration of information
processing technology possible, and its combinations with nanotech­
nology, quantum dot, fiber and dirac cone offer the potential to revo­
lutionize information technology. However, the fabrication of 3D
photonic crystal with bandgaps available for visible light, the intro­
duction of specific defect at optional location, the fabrication of high
efficiency photon conduction materials, and the load of current and
voltage on photonic crystal remain a challenge.
4.4. Optical fibers
Owing to the small diameter of the optical fiber and the transparency
of the material, the processing technology used on fibers must be precise
and reliable. Unlike traditional processing approaches, such as chemical
vapor deposition (CVD), plasma chemical vapor deposition (PCVD), and
vapor axial deposition (VAD), femtosecond laser direct writing can
achieve high efficiency, zero pollution, and 3D precision machining that
enables control over shape and dimension of a component, which could
greatly improve the performance of optical fibers. Hence, femtosecond
laser direct writing has become an important approach for optical fiber
processing, and the innovation and application of special optical fibers.
For instance, femtosecond laser processing was applied to achieve
flexible and reliable inscriptions on a fiber core and clad to realize
versatile optical elements and optical fiber sensors [119]. Donko et al.
utilized femtosecond laser direct writing micro-processing technology to
fabricate a multi-core fiber for multiplexing [120]. The flexibility of the
femtosecond laser has enabled the novel photonic integration of several
kinds of optical devices on surfaces and in the bulk volume of flat optical
fibers [121]. Lab-on-fiber means the integration of multifunctional
micro/nano materials and devices within a single optical fiber. Owning
to the advantages of miniaturization, biocompatibility, robustness, and
X. Wang et al. Optics and Laser Technology 135 (2021) 106687

Fig. 5. Schematics of multilayer nonlinear spatial modulation by ferroelectric barium calcium titanated 3D nonlinear photonic crystal. (a)-(c) 3D position of
multilayer structures, including fork structures, linear grating and circular grating; (d)-(f) the 3D visualization of the 3D nonlinear photonic crystals obtained by
nonlinear Čerenkov microscopy. Copyright © 2019, Springer Nature.

flexibility, lab-on-fiber has shown great potential for applications to
multifunctional sensing and actuating [122,123]. Through femtosecond
laser direct writing, both dielectric and metallic nanostructures can be
fabricated on the fiber tip [122]. Ultracompact multi-lens objectives
with high optical performance that could be applied in miniature optical
instruments can be manufactured at the end of an optical imaging fiber
(Fig. 6a) [85]. In term of lab-in-fiber, 3D optical circuits and micro­
fluidic systems have been integrated in a single-mode fiber by femto­
second laser direct writing (Fig. 6b) assisted by selective chemical
etching [124]. In this multi-components fiber sensor, 3D waveguides, X-
couplers, Bragg gratings, mciroholes, mirrors, optofluidic components
and microfluidic structures were processed within a single mode fiber.
The surface roughness of the elements could be 10 nm in bulk fused
silica [125], paving a novel way for 3D lab-in-fiber development. The
combination of femtosecond laser and optical fiber offers a unique
approach to on-surface and sub-surface fabrication of optical devices
and microfluidic devices, allowing for integration onto an optical plat­
form, furthermore, various materials with diverse physical, chemical,
mechanical, and biological properties can be integrated onto an optical
fiber. Thus, the fabrication and application of optical fiber is promising.
5. Summary and outlook
The absorption of a femtosecond laser by a material is nonlinear and

Fig. 6. Lab-on-fiber and lab-in-fiber devices enabled by femtosecond laser fabrication. (a) Processing of a lab-on-fiber multi-lens at the top of the optical fiber.
Copyright © 2016, Springer Nature. (b) Schematic of lab-in-fibers based on the femtosecond laser writing. Copyright © 2014, Royal Society of Chemistry.

8
X. Wang et al.
material-independent, which enables it to be an invaluable tool for
fabricating complex 3D structures in compound substrates with
nanometer-scale precision. Spatial and temporal beam shaping tech­
nologies, combined with parallel processing technologies, can address
the challenge of resolution, productivity and materials, while modern
laser technology is developing fast. The 3D microfabrication of 3D/4D
smart actuators and microrobots by smart materials is a successful
emerging application. The one-step integration of optical devices with
other components through femtosecond laser processing is attractive for
novel devices, and for applciations, such as 3D microfluidic [97],
optofludic, electrofluidic and electrooptic devices [126–128]. Active
photonic integration on silicon substrate and the load of current and
voltage on the integrated devices are prospective issues impeding
practical applications of femtosecond laser processing. Furthermore, the
fabrication of scalable metamaterials with multiscale dimensions
ranging from tens of nanometers to centimeters by femtosecond laser-
based additive manufacture [129] is another successful emerging
application. Although the applications of micro/nano structures built by
femtosecond laser have been explored, related studies have not been
systematic. To unravel the great potential of femtosecond laser pro­
cessing in the fields of machinery, electronics, biosensors and drives,
physics, and chemistry, further exploration and research are needed; for
instance, comprehensive models and methodologicals improvements,
along with improvements to corresponding measurement systems, are
needed [11,130,131].
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgements
This work was supported by the National Natural Science Foundation
of China [grant numbers 61727811, 61973298, 61803366 and
61821005], the External Cooperation Program of Chinese Academy of
Sciences [grant number 173321KYSB20170015], the Interdisciplinary
Innovation Team of Chinese Academy of Sciences [grant number JCTD-
2019-09], Liaoning Revitalization Talents Program [grant number
XLYC1807006], the Youth Innovation Promotion Association of the
Chinese Academy of Sciences [grant number Y201943] and the
Fundamental Research Funds for the Central Universities [grant number
D2017020].
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