Review
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Laser Fabrication of Bioinspired Gradient Surfaces
for Wettability Applications
Junrui Wu, Kai Yin,* Si Xiao, Zhipeng Wu, Zhuo Zhu, Ji-An Duan, and Jun He
Inspired by nature, gradient surfaces have attracted broad research interest
because of their potential in microfluidics, fog/water collection, and water
electrolysis. Among the various techniques for preparing gradient surfaces,
laser processing is substrate-independent, facile and efficient, pattern-
diverse, which can be used to prepare diverse gradient surfaces. Here, recent
advances in the laser fabrication of gradient surfaces for wettability applica-
tions are summarized. The preparation principles of gradient surfaces and
advantages of laser processing are introduced. Various laser fabrication strat-
egies and wettability applications of gradient surfaces including wettability
gradients and geometric gradients are discussed. Challenges and future per-
spectives for the laser fabrication of gradient surfaces are finally presented.
1. Introduction
Millions of years of natural selection and evolution have given
rise to biological surfaces with multifunctional gradients to
meet the challenges of harsh living environments.[1–9] A species
of beetle in the Namib Desert possesses a wettability gradient
enabling it to capture water from air.[10] This wettability gra-
dient arises from a series of hydrophobic/hydrophilic patterns
on its back. In another example, the gradient wedge corner
of peristome surfaces plays an essential role for directional
droplet transport.[11] Besides, Cacti and spider webs can achieve
directional water collection and transport from air, where the
main driving force results from the combination of wettability
gradients and geometric gradients.[12,13] Learning from nature
has proven to be effective for developing functional mate-
rials.[14–19] Wettability gradients and geometric gradients can be
applied in microfluidic devices, fog/water collection, and water
electrolysis, all of which may help alleviate water shortages
and associated engineering problems. Preparing functional
J. Wu, Prof. K. Yin, Prof. S. Xiao, Z. Wu, Z. Zhu, Prof. J. He
Hunan Key Laboratory of Super Microstructure and Ultrafast Process
School of Physics and Electronics
Central South University
Changsha 410083, P. R. China
E-mail: kaiyin@csu.edu.cn
Prof. K. Yin, Prof. J.-A. Duan
The State Key Laboratory of High Performance and Complex
Manufacturing
Central South University
Changsha 410083, P. R. China
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/admi.202001610.
DOI: 10.1002/admi.202001610
Adv. Mater. Interfaces 2021, 8, 2001610 2001610  (1 of 23)
materials with gradients inspired by bio-
logical surfaces has therefore attracted
much interest.
Strategies for preparing gradient sur-
faces include vapor-phase diffusion,
gradual immersion, electrochemical
oxidation, and photolithography that
have broadly adopted.[20–26] However,
their material constraints, tedious and
time-consuming processes, and their
single-pattern limit their widespread use.
Developing a substrate-independent, facile
and efficient, pattern-diverse method for
preparing gradient surfaces would aid fun-
damental science and practical application.
Among various techniques, laser pro-
cessing has recently emerged as a powerful tool in integrated-
optics and biomimetic micro–nanodevices. This technology can
be used to precisely control the preparation of micro/nanoscale
structures on various substrates such as metals, glass, ceramics,
and polymers.[27–33] Besides, the high energy density of lasers
allows the machining process to be completed quickly and effi-
ciently. Combining laser machining with computer-aided con-
trol allows laser ablation parameters to be precisely controlled,
including the processing position, scanning speed, scanning
interval, and scanning track. Laser processing can therefore be
used to produce flexible and diverse patterns in complex work-
pieces. And laser micro/nano fabrication has been applied to
regulate surface wettability.[34–43] Therefore, laser processing
has great potential for developing samples with different wet-
tability and geometries on various materials.
This review discusses laser fabrication of bioinspired gra-
dient surfaces for wettability applications, whose overview is
shown in Figure  1. The related backgrounds including gra-
dient surfaces in natural creatures, the theoretical basis of wet-
tability, and the distinct characteristics of laser processing are
introduced. Gradient surfaces can be classified into wettability
gradients and geometric gradients, and they are discussed in
terms of various laser fabrication approaches and wettability
applications. It is worth mentioning the definition of wettability
gradient and geometric gradient in this review. Wettability gra-
dient is defined as a surface with no obvious geometric change
in the shape, and there is a difference of contact angles on the
macro level resulting from the roughness gradient on the micro
level. Geometric gradient is defined as a surface possessing sig-
nificant geometric changes in the shape, but not much differ-
ence in the roughness of the entire surface at the microscopic
level. Specially, a wettability gradient surface generates a water
driving force as a result of its varying surface roughness. Wetta-
bility gradient surfaces can be applied in water droplet control,
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Figure 1.  An overview of bioinspired gradient surfaces fabricated by laser for wettability applications, including wettability gradients and geometric
gradients. Images of desert beetle and spider: Reproduced with permission.[10] Copyright 2013, Wiley-VCH GmbH.

fog/water collection, and spilled oil crossflow collection. A geo-
metric gradient structure generates a Laplacian pressure differ-
ence by exploiting its asymmetric shape. Geometric structures
can be applied in directional self-transport in microfluidics,
fog/water collection, and water electrolysis. Finally, the outlook
for laser fabricated gradient surfaces is discussed.
2. Background
2.1. Nature Creatures with Gradient Surfaces
Organisms with fascinating structures and optimized func-
tions are common in nature, which can aid them adapt to harsh
environments. The desert beetle has a tailor-made covering for
water collection in dry conditions (Figure 2a), which is an array
of hydrophilic non-waxy bumps distributed on a hydrophobic
wax-coated background.[10] Flattened hemispheres with diame-
ters of ≈10 µm constitute the microstructure of the hydrophobic
region and they are arranged in a regular hexagonal array. The
surface wettability gradient results in droplets moving from the
hydrophobic region to hydrophilic region, allowing the beetle to
collect water in arid environments.
The peristome surface of Nepenthes alata can realize contin-
uous, directional water transport from the inner to outer side
(Figure 2b), which has a two-order hierarchical arrangement.[11]
Along the second-order microgrooves, arched microcavities
are regularly tilted upward with the vault pointing outward.
The vertical section of the peristome shows that the arc-shaped
microcavities are closed, and the enclosed surface has sharp
edges to form wedge corners. The opening angle of the wedge
corners decreases with height, which renders a gradient force
for directional droplet transport.
The cactus has an integrated multifunctional system that
allows water capture from air.[12] The spine of the cactus com-
prises three different structural features: the tip with oriented
barbs, the middle with gradient grooves, and the base with
belt-structured trichomes (Figure 2c). The spine and barbs have

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Figure 2.  Photographs and microstructures of organisms with gradient surfaces. a) The bumpy back of the desert beetle has a wettability gradient with
alternating hydrophobic, wax-coated regions and hydrophilic, non-waxy regions. Reproduced with permission.[10] Copyright 2013, Wiley-VCH Verlag.
b) The peristome surface possesses a wedge corner gradient that provides a driving force for directional droplet transport. Reproduced with permission.[11]
Copyright 2017, Wiley-VCH Verlag. c) The cactus utilizes geometric gradients and wettability gradients which collectively impart efficient fog collection
capability. Reproduced with permission.[12] Copyright 2012, Springer Nature. d) Wet-rebuilt spider silk has geometric and wettability gradients, which act
together to achieve directional collection of water droplets around the spindle-knots. Reproduced with permission.[13] Copyright 2012, Wiley-VCH Verlag.

conical shaped gradients, which can drive water toward the
larger radius side. The apex angle of the conical shape in the
spine and barb are 12.3 ± 1.6° (2α) and 19.5 ± 3.3° (2β), respec-
tively. The grooves have a width gradient along the spine, with
an average width of ≈6.8 mm near the wide base and ≈4.3 mm
near the narrow tip. The sparse microgrooves in the base have a
lower roughness than the tip, which form a wettability gradient
that facilitates water droplets moving toward the base. As the
droplet approaches the base, it is absorbed by the capillarity of
the hydrophilic belt-structured trichomes immediately. These
distinct structural features of the cactus are all conducive to the
directional transport of water from the tip to the base, especially
the wettability gradient and geometric gradient of the spine.
Spider silk with fiber structure can also realize directional
water transport and collection.[13] Wet-rebuilt spider silk is com-
posed of alternating 21.0 ± 2.7 µm spindle-knots and 5.9 ± 1.2 µm
joints, that have a periodicity of 89.3  ± 13.5  µm (Figure  2d).
Magnified images show that the spindle-knots possess a rough
topography with highly random nanofibrils, while the joints are
relatively smooth with aligned nanofibrils. A spindle has a curved
gradient that is composed of two conical shapes with apex angles
of ≈19° (2γ). The spindle-knot is more hydrophilic and the joint
is less hydrophilic that forms a wettability gradient. The wet-
tability gradient generated by the anisotropic surface structure
and the geometric gradient generated by the conical shape col-
lectively drive water droplets from the joints to the spindle-knots.
2.2. Wettability Theory
As one of the most important properties of solid substrates,
surface wettability is determined by surface free energy and

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Figure 3.  Wetting behaviors of droplets on various solid surfaces. a–c) Contact angles with different wetting states: Young’s model, Wenzel model,
and Cassie model. d) Sliding angle of a droplet on the tilted substrate. e) A wettability gradient force generated by the surface roughness difference.
f) Schematic of Laplace pressure function. g) The Laplace pressure difference produced by the wedge shape gradient. h) The Laplace pressure differ-
ence arising from the conical shape gradient. i) Diagram of contact angle hysteresis.

micro/nano roughness.[44–52] Wettability can be evaluated by r (γ SV − γ SL )

measuring the contact angle (CA) and sliding angle (SA) of
a small liquid droplet on the target substrate. CA refers to
the angle (θ) between the tangent of the air/liquid surface
and the liquid/solid interface at the three-phase contact line
when a droplet drops on a surface.[53] In order to explain CA
in different states, three classical models were produced,
namely Young mode (θY), Wenzel model (θW) and Cassie
model (θC).
The wettability of a droplet on ideal smooth surface is com-
monly described by Young wetting model (Figure  3a), and the
equilibrium CA can be calculated by Young’s equation[54]
γ SV − γ SL
cosθ Y = (1)
γ LV
cosθ W = = r cosθ Y (2)
γ LV
where r is the roughness factor defined as the ratio of the actual
contact area to projected area.
In the Cassie state, the liquid is repelled by the microstruc-
tural valleys of the rough substrate and is hard to penetrate into
the valleys. Therefore, the liquid droplet can just sit on the top
microstructures with air trapped in (Figure  3c). In contrast to
Wenzel state, the adhesion between the liquid and substrate is
ultralow for the Cassie state. Cassie proposed a new model to
describe a small droplet on such a solid/air heterogeneous sub-
strate, and the specific CA was given as follows[58]
cosθC = f cos θY + f − 1 (3)

where the γSV, γSL, and γLV represent the interfacial tensions of
solid–vapor, solid–liquid, and liquid–vapor interfaces.
The Young’s equation only applies to ideal smooth sub-
strates, while the surface of substrates usually has different
roughness in most cases. And the surface roughness of the
material has an important effect on wettability. To illustrate
wettability with different roughness, two classical wettability
models were proposed: Wentzel state and Cassie state.[55–58]
In the Wenzel state, the liquid can wet the microstructure
of the rough surface and fill the microstructural valleys. The
adhesion between the liquid and the matrix is relatively high
(Figure 3b). Besides, Wenzel pointed out the actual surface area
of the droplet is larger than the apparent surface area, so he
modified Young’s equation by the following[56,57]
where f is the area fraction of the surface in contact with the
liquid.
CA is used to reflect the static aspect of the surface wetta-
bility while SA is used to reflect the dynamic behavior of micro-
droplets on the substrate. As the substrate tilts gradually until
the droplet is just enough to roll away, this tilt angle is referred
to as SA (Figure  3d). The value of SA reflects the degree of
adhesion between the solid substrate and droplet, which is pos-
itively correlated with adhesion force.[59–61]
A stationary droplet on a uniform solid surface is generally
subjected to a balanced external force. However, a wettability
gradient force (Fchem) will be generated when the roughness
gradient exists on the surface (Figure 3e), which is described by
the following[62–64]

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B
Fchem = ∫γ (cosθ m − cosθ l ) dl (4)
A
where γ is the surface tension, θl and θm are the con-
tact angles of the less wettable and the more wettable side
of droplet, dl is the integral variable along the direction of
motion from A to B, respectively. From Equation (4), it can be
deduced that when a droplet is placed on wettability gradient
surface, the droplet will move from the less wettable region
to the more wettable region under the action of wettability
gradient force.
For all types of droplets, a Laplace pressure (ΔP) will be
generated by a curved liquid surface pointing to the curvature
center (Figure 3f), which can be calculated as[65–67]
2γ
∆P = (5)
R cessing. The monochromatism of a laser ensures that the
where R is the curvature radius of the circle. From the Equa-
tion  (5), it can be inferred that a smaller radius of curvature
can produce a larger force. On a geometric gradient surface, the
Laplace pressure difference becomes the main driving force for
an asymmetric droplet.
When the droplet is released at the minor side of a wedge
shape (Figure 3g), the droplet is pressed by the margins of the
trapezoid resulting in a minor rear curvature radius (R1) and
a large front curvature radius (R2). According to Equation  (5),
the Laplace Pressure difference (ΔPtrapezoid) produced by the two
opposite sides can be described as[68]
1 1
∆Ptrapezoid  γ  −  (6)
 R1 R 2 
Driven by the ΔPtrapezoid, the droplet on the trapezoid plat-
form can achieve spontaneous and directional transport from
the minor side to the large side.
The wedge-shaped surface provides a width gradient along
the longitudinal direction, while the cone structure provides a
radius gradient by varying the length (Figure  3h). Due to the
asymmetry of the conical geometry, there is also a Laplace pres-
sure difference on two opposite sides of the droplet, which can
be calculated as[69,70]
RL
2γ
∆Pcone  − ∫ (R + R )
2
sin α dz (7)
Rs 0
where R is the local radius, R0 is the drop radius, α is the half-
apex angle of the cone, and dz is the integrating variable along
the diameter of the cone. The Laplace pressure on the high
curvature site (small radiusRS) is larger than that on the low-
curvature site (large radiusRL). This difference of Laplace pres-
sure can drive droplet move from the small radius to the large
radius along the cone.
In most cases, the movement of droplet is subject to contact
angle hysteresis resistance due to the surface inhomogeneity
(Figure  3i). This force comes from the difference between the
advancing contact angle (θa) and receding contact angle (θr) of
the droplet, which can be expressed as[71,72]
Fres  π r0γ (cos θ r − cos θ a ) (8)
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where r0 is the contact radius. As a matter of fact, smaller hys-
teresis resistance contributes to the directional movement of
droplet.
2.3. Laser Processing
Laser sources have some advantages over traditional light
sources, including high brightness, high directivity, high
monochromatism, and high spatiotemporal coherence.[73–75]
A focused high-brightness laser beam can produce tempera-
tures of tens of thousands of degrees near the focal point,
making it possible to process almost any material. The high
directivity of a laser enables it to effectively transmit a long
distance and ensures that the final laser spot has a high-
power density, both of which are important in laser pro-
high-power beam can be accurately focused to a focal point.
The high spatial coherence allows laser to be focused on a
small point, produce photochemical reactions, and remove
material by breaking chemical bonds. These characteris-
tics have greatly promoted the use of lasers in processing
applications.
Laser processing has strong potential in integrated-optics
and micro–nanodevices for the following advantages.[76–79] 1) It
is contactless and has no direct impact, so there is no mechan-
ical deformation of the sample. Laser machining allows for a
high degree of freedom in processing environment and does
not require highly clean conditions. 2) It can be used to pro-
cess a wide variety of materials such as metals, glass, ceramics,
and polymers. And it is especially advantageous in processing
materials with high hardness, high brittleness, or high melting
point. 3) It has high production efficiency and quality because
the high energy density of laser allows machining to be com-
pleted quickly and efficiently. This can also maximize the pro-
cessing quality with minimal thermal deformation. 4) It has
high processing precision because laser spots can be focused
extremely small through an optical lens. 5) It is often combined
with numerical (computer-aided) control systems because
laser beam can be easily guided, focused, and transformed.
This allows precise control of laser ablation parameters, such
as processing position, scanning speed, scanning interval, and
scanning track. Therefore, laser processing can produce flexible
and diverse patterns in complex workpieces, including carving
inside a structure, punching microholes in integrated circuits,
and carving of silicon wafers.
A laser processing system generally comprises a laser source,
light path, and motion-stage system. Two typical laser pro-
cessing systems are shown in Figure 4. The sample is mounted
on a 3D motion stage to control the geometric shape and spatial
location. An electromechanical shutter in the optical path con-
trols the exposure of the laser beam. Optical lens is commonly
used to help the laser beam focus on the sample. The laser
scanning route is usually programmed into the computer-aided
control system to guide the entire fabrication. And the scan-
ning path is generally controlled by one of the following two
ways. The first uses a galvanometer to transform the laser scan-
ning path, while the 3D platform remains stationary after the
initial position is focused (Figure  4a).[80] The second involves
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Figure 4.  Two typical laser processing systems and various exquisite patterns prepared by laser micro–nano fabrication. a) Moving laser beam with
stationary sample in laser processing. Reproduced with permission.[80] Copyright 2018, Elsevier. b) Moving sample with stationary laser beam in laser
processing. Reproduced with permission.[81] Copyright 2017, Royal Society of Chemistry. c) A 3D “micro-bull” sculptures prepared by two-photon
absorption. Reproduced with permission.[94] Copyright 2010, Elsevier. d) A dual-3D femtosecond laser processing technique to manufacture intelligent
microflowers. Reproduced with permission.[95] Copyright 2019, American Chemical Society. e) The self-assembled metal nanogap structures fabricated
by 3D laser printing. Reproduced with permission.[96] Copyright 2020, Wiley-VCH Verlag. f) 3D femtosecond laser printing to manufacture capillary-
induced chiral self-assembly. Reproduced with permission.[97] Copyright 2020, Wiley-VCH Verlag.

controlling the scanning path by back and forth movement of
the 3D platform while the laser is stationary (Figure 4b).[81]
Laser processing can produce various precise and detailed
patterns, which has been widely applied to various samples
with wide applications, such as surface-enhanced Raman scat-
tering substrates, power generators, supercapacitors, sensors,
and actuators.[82–91] Line-by-line scanning and point-by-point
ablation can both be realized by adjusting the scanning speed.
Line-by-line scanning is widely used to produce separate micro-
grooves or homogeneous large-area coarse surfaces. Point-by-
point ablation can be used for drilling to prepare microporous
arrays.[92,93] Conventional laser systems are generally used for
processing 2D patterns, whose laser are divided into x-axis
deflection and y-axis deflection. After certain processing, the
laser can be used to draw the required 2D pattern. Figure 4a,b
show two traditional laser systems, and there are also other
laser processing systems. With the development of laser, two-
photon absorption has been proved to be an effective tool for
processing 3D micro–nano exquisite structures. The intelligent
zoom system in 3D laser processing has one extra set of lenses
compared with the 2D system. These extra lenses can dynami-
cally adjust the focal length of the laser beam in the z-axis
deflection. For example, Sun et  al. created a 3D “micro-bull”
sculpture on resin materials by a two-photon absorption system
(Figure 4c).[94] These 10 m-long, 7 m-high bulls were very small
animal models, about the size of a red blood cell. Zhang et al.
designed a dual-3D femtosecond laser processing technique,
which could form arbitrary and flexible 3D microactuators and
realize the intelligentization of ordinary photopolymer mate-
rials (Figure  4d).[95] Based on this strategy, they designed and
manufactured intelligent microflowers with the total feature
size of ≈30  µm. Under the stimulation of a certain solvent,
microflowers can switch back and forth between “flowering”
and “budding” morphologies. 3D printing technology is a rapid
prototyping technology, which circumvents traditional molding
methods and greatly shortens the product design and produc-
tion cycle. Laser printing based on two-photon polymerization
has advantages of simple integration, maskless processing, and
suitability for non-planar substrates, which makes it useful for
preparing 3D micro–nano structures. For example, Lao et  al.
fabricated the self-assembled metal nanogap structures with
supercritical drying-switchable capillary-force self-assembly
by 3D laser printing (Figure  4e).[96] To demonstrate the flex-
ibility of the 3D-printed nanogap structures, more complex

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“NANOGAP” and “Taiji” patterns with 4-pillars were also
formed. Hu et  al. utilized the flexibility of femtosecond laser
printing to control the geometry and spatial topology of micro-
pillars synergistically, thus generating capillar-induced chiral
self-assembly (Figure  4f).[97] They prepared diverse mesoscale
hierarchical assemblies with different handedness.
In summary, laser processing can be used to form surface
micro–nano structures and produce various geometric patterns.
It has therefore attracted much interest for preparing gradient
surfaces. Next, we discuss the laser fabrication of bioinspired
gradient surfaces and their wettability applications, in terms of
wettability gradients and geometric gradients.
3. Wettability Gradients
3.1. Laser Fabrication of Wettability Gradient Surfaces
Inspired by the unique structural features of desert beetles, var-
ious methods combining laser processing have been developed
to fabricate wettability gradient surfaces. It is worth mentioning
that wettability is governed by the surface chemical composi-
tion and surface micro/nanostructures, so the preparation of
wettability gradient surface can be achieved by regulating these
two factors.
Song et  al. prepared a hybrid wettability gradient Cu
mesh sample containing hydrophobic and superhydro-
phobic regions (Figure  5a).[98] By spinning a mixed liquor
of the polydimethylsiloxane (PDMS) and graphene (G), the
PDMS/G coating uniformly adhered to the Cu mesh. Fol-
lowed by laser etching, this PDMS/G film presented super-
hydrophobicity with a water contact angle (WCA) of 153° due
to the pyrolysis and solidification. Then treating the hybrid
sample with ultrasonic vibration, some area of the copper
mesh was naked exhibiting hydrophobicity with a WCA of
92°. Thus, a kind of hybrid wetting surfaces was successfully
designed by the combination of laser etching and ultrasonic
vibration.
In Figure  5b, repeated patterns with gradient wettability
were successfully created on the PDMS substrate via laser

Figure 5.  Various methods to prepare wettability gradient surfaces. a) A wettability gradient surface with hydrophobic and superhydrophobic regions
prepared by laser etching and ultrasonic vibration. Reproduced with permission.[98] Copyright 2018, Royal Society of Chemistry. b) Repeated patterns
with wettability gradient were created on the PDMS substrate by laser engraving with varied GS. Reproduced with permission.[99] Copyright 2019, Royal
Society of Chemistry. c) A wettability gradient surface on NiTi alloy fabricated via ultrashort pulse laser etching approach followed by coating stearic
acid. Reproduced with permission.[100] Copyright 2020, Elsevier BV. d) Microgroove surfaces with wettability gradients prepared by laser processing,
vacuum storage, and partial soaking in H2O2 solution. Reproduced with permission.[103] Copyright 2019, Elsevier Inc.

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engraving with spatially varied laser dose, where the laser
dose could be controlled by changing the value of gray scale
(GS).[99] The unmodified substrate was uniformly superhydro-
phobic, while the surface wettability of modified substrates
decreased with GS. In detail, the substrate with GS = 10%
represented the more hydrophobic edge with WCA of 152.5 ±
2.8°, the substrate with GS = 14% represented the center pat-
tern with WCA of 137.2  ± 1.8°, and the substrate with GS =
18% represented the more hydrophilic edge with WCA of
125.7  ± 3.4°. It is confirmed that laser irradiation with dif-
ferent GS can produce surface patterns with gradient wetta-
bility, and the gradient is distributed along the long side of the
rectangle.
Zhang et al. fabricated a laser-induced wettability gradient
surface on nickel–titanium (NiTi) alloy by manipulating the
pore distances (Figure  5c).[100] By using ultra-short pulse
laser etching, three micro-sized porous structures with dif-
ferent pore distances (190, 110, and 30  µm) were created on
the surface of NiTi alloy. Then the sample was immersed
into ethanol solution of stearic acid at room temperature.
After immersion, taken out and dried in an oven, there is
the generation of a wettability gradient on the sample. The
four regions of gradient-NiTi were respectively named as
NiTi, LP1, LP2, and LP3, whose contact angles were corre-
spondingly 94  ± 3°, 111  ± 2°, 133  ± 2°, 155  ± 2°. The differ-
ence in contact angles indicated the successful formation of
wettability gradient surface, which was prepared via ultra-
short pulse laser etching approach followed by coating stearic
acid. Yin et  al. fabricated a gradient-wettability mesh with
nanoripple structures, which was prepared by femtosecond
laser direct writing on assembled meshes with different
pores (≈230, ≈90, ≈50, and ≈10 µm).[101]  Ta  et  al. fabricated
a wettability gradient surface machined by direct nano-
second laser texturing on a brass surface with a tilted angle
of α = 1.3°.[102] Because the sample was inclined during pro-
cessing, the different laser-ablated morphologies lead to the
wettability gradient.
Three steps for nanosecond (ns) laser treated wetta-
bility gradients surfaces with microgrooves are shown in
Figure  5d.[103] Firstly, ns laser micromachining technology
was used to prepare periodic microgrooves on a copper sur-
face, and the laser treated sample was superhydrophilic.
Then the sample was stored in a container with a mechanical
pump to create a vacuum environment by evacuating the
air. When the sample was stored in such an environment
for 3 h, it became superhydrophobic with CA of 158.4 ± 5.0°
due to the adsorption of organic compounds. Finally, part
of the sample was soaked in H2O2 solution in a beaker, so
the prepared samples could be divided into three areas after
5  min of soaking. The fully soaked left part possessed high
hydrophilicity (θleft), arising from the removal of adsorbed
organic compounds and the increase of the surface oxide.
The middle part was hydrophilic (θmiddle) affected by the
rising H2O2 solution level. While the right part retained its
superhydrophobicity (θright) because it was unaffected by the
soaking process. At this time, the microgroove surfaces with
different wettability (θleft  < θmiddle  < θright) were successfully
prepared by laser processing, vacuum storage and partial
soaking in H2O2 solution.
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3.2. Applications of Wettability Gradients
3.2.1. Control Behaviors of Droplets
Under the action of the wettability gradient, the droplet can
move from the less wettable area to the more wettable area.
Therefore, wettability gradient surfaces can be prepared to con-
trol droplet behaviors, which provide a solid technical basis for
microfluidic channel devices. Qi et  al. prepared repeated pat-
terns with wettability gradient by laser irradiation, which could
be successfully applied in long-distance droplet translocation
and droplet mixing.[99] The detailed wettability gradient and
preparation diagram of the repeated pattern are already pre-
sented in Figure 5b. The droplets on this surface moved toward
the more hydrophobic part of the same pattern and across
the pattern boundary, then to the next more hydrophilic part
of the pattern through mechanical agitation. When the vibra-
tion amplitude (A0) and vibration frequency (f) were appro-
priate (A0  = 4  mm, f  = 10  Hz), the droplet could transport for
a long distance of 16  mm in 400  ms along the 1D trajectory
(Figure 6a). Besides, the long-distance movement along prede-
termined 2D trajectory was also demonstrated. The 2D trajec-
tory consisted of a linear cascade of four repeated wettability
gradient patterns, with the head and tail joining each other to
form a square shape. With a vibration of ≈9 Hz along the lon-
gitudinal direction of the first cascade, the droplet moved from
corner 1 to corner 2. Subsequently, the droplet moved along the
direction of the wettability gradient to corner 3, corner 4, and
ultimately returned back to corner 1. Mixing of two droplets is
a basic skill of open microfluidic channel and is widely used
in biochemical analysis. In their study, two sets of wettability
gradient patterns were arranged for droplet mixing, where their
more hydrophobic edges met in the central region (Figure 6b).
When two droplets stained with different colors were released
at the two distal ends, both droplets moved toward the center
region and encountered each other within ≈300 ms.
In addition to control the droplet at room temperature, the
droplet behaviors at high temperature can also be controlled.
When a liquid is dropped on a hot surface, it does not moisten
the hot surface but merely forms a vapor layer on top of it. This
phenomenon is known as the Leidenfrost effect.[104–107] On this
basis, Chen et  al. fabricated micropillared surfaces with wetta-
bility gradient by sputter coating and laser etching, and the sur-
face was heated on the thermostatic heater.[108] The green arrow
in Figure  6c indicated the direction of enhanced wettability
from 37°to 82°, which was measured at room temperature by
goniometer. When the maximum droop of the water droplet is
greater than the height of pillars, the droplet touches the bottom
of the cavity between the two columns, that is, the droplet is in
Wenzel state. From Equation  (2), the contact angle increases
with the roughness of the surface. The top view of surface mor-
phology shows that the roughness of the larger superficial area
of micropillars (LSAM) is greater than that of the smaller super-
ficial area of micropillars (SSAM). Therefore, the contact angle
at LSAM is greater than that SSAM, which is consistent with the
increasement of wettability gradient. It was observed that the
Leidenfrost droplet on this sample tended to self-propel from
SSAM to LSAM on the hot gradient surface. This phenomenon
was caused by the surface structure and the escaping vapor flow.
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Figure 6.  Wettability gradient surfaces for applications in controlling behaviors of droplets. a) Long-distance droplet movement along a linear 1D
pattern and a predetermined 2D trajectory. b) Droplet mixing by moving two droplets toward the central region. a,b) Reproduced with permission.[99]
Copyright 2019, Royal Society of Chemistry. c) Sequential photographs showing the self-transport of Leidenfrost droplets from the smaller superfi-
cial area of micropillars to the larger superficial area of micropillars. Reproduced with permission.[108] Copyright 2018, Elsevier. d) Sequential optical
photographs for rapid water flow movement by Sur.1p. Reproduced with permission.[103] Copyright 2019, Elsevier Inc.

Long et  al. fabricated surfaces with microgrooves and nonu-
niform wettability for rapid water flow movement,[103] where the
specific preparation steps were already shown in Figure  5d. To
simplify the descriptions, the laser-processed surface with uni-
form wettability was denoted as Sur.0. And the laser-processed
surface stored in a vacuum environment for 1 h and then partially
soaked in the hydrogen peroxide (H2O2) solution was denoted as
Sur.1p. In their experiments, water flow could be accelerated by
Sur.1p with wettability gradient compared to the normal Sur.0
surface with uniform wettability, and the average flow velocity
increased from 28.1 to 47.6 mm s−1 (Figure 6d). In other words,
the as-prepared wettability gradient surface accelerated the
droplet transport speed successfully. This phenomenon is con-
sistent with the wettability gradient theory introduced above. On
the Sur.1p sample, θleft < θmiddle < θright, it can be deduced that a
droplet can spontaneously move from the right part to the left
part according Equation (4). Therefore, water flow could be accel-
erated by Sur.1p compared to the normal Sur.0 surface.
3.2.2. Fog/Water Collection
Fog/water harvesting is a potential way to alleviate global water
shortages, especially being meaningful to the desert and arid
regions.[109–111] Therefore, the preparation of materials with
fog/water collection capacity has received increasing interests.
Enlightened by the fog harvesting of the Namib desert beetle,
some hybrid surfaces with wettability gradient have emerged
to meet the need for water collection. Song et  al. prepared a
hybrid wetting sample with hydrophobic and superhydrophobic
regions by laser etching and ultrasonic vibration in Figure  5a.
In order to quantitatively characterize the as-prepared sam-
ples, the fog collection rates (FCR) of the original Cu mesh, the
hybrid wetting and superhydrophilic Cu mesh samples were
compared by the self-made fog collection device (Figure 7a).[98]
It was observed that the FCR of as-prepared hybrid wetting
sample was about 5.4 g cm−2 h−1, which was significantly higher
than the original Cu mesh and the superhydrophilic samples.
These samples have different fog collection processes with
the increase of time due to their different wettability. On the
original sample, the fog flow condensed to tiny water droplets
and gradually coalesced after contacting the original Cu Mesh.
Then the large droplets of condensation adhered to the original
sample before falling off. In contrast, fog flow passed through
the hybrid wetting sample and condensed to tiny droplets in a
short time. Under the action of surface wettability gradient, tiny
droplets on the superhydrophobic region were propelled to the
hydrophobic region and then merged into larger water droplets

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Figure 7.  Hybrid surfaces with wettability gradients for applications in fog/water collection. a) Fog collection comparisons between a hybrid superhy-
drophobic–hydrophobic wetting sample and other surfaces by the homemade fog-harvesting system. Reproduced with permission.[98] Copyright 2018,
Royal Society of Chemistry. b) Water collection comparisons of a hybrid superhydrophobic–hydrophilic surface and other samples by the homemade
water-harvesting system. Reproduced with permission.[112] Copyright 2017, Royal Society of Chemistry.

before falling off. On the superhydrophilic sample, fog flow
contacted the Cu mesh surface and formed tiny water droplets.
As time went on, the diffusing droplets connected to each other
forming a water film and spread out over the surface. From the
water collection processes, it could be observed that the water
droplets on the original and superhydrophilic samples had
higher viscous forces to the surface, which made their FCR
lower than the hybrid wetting sample.
Yin et  al. prepared a hybrid superhydrophobic–hydrophilic
surface by depositing polytetrafluoroethylene (PTFE) nanoparti-
cles on the assembly of copper mesh and copper sheet through
femtosecond laser.[112] They built a homemade fog collection
system to compare the water collection rate (WCR) of different
samples, including pristine hydrophobic copper mesh, pristine
hydrophilic copper sheet, as-treated superhydrophobic copper
mesh, pristine hydrophobic–hydrophilic copper mesh-sheet,
and as-prepared superhydrophobic–hydrophilic hybrid sample
(Figure  7b). The WCR of the first four samples were similar,
much lower than the WCR of as-treated hybrid sample with
an WCR of about 203  mg cm−2 h−1. In order to compare the
water collecting behaviors of the pristine hydrophobic–hydro-
philic mesh and the as-prepared hybrid sample more clearly,
dynamic optical images were exhibited to reveal the water col-
lecting processes. Similar to the above Song’s study, water drop-
lets attached to the pristine sample due to the high adhesion at
the liquid–solid interface. While the as-prepared hybrid sample
had a wettability gradient with superhydrophobic–hydrophilic
and low adhesion, the droplets could merge into large drop-
lets within a short time. When the growing weight of droplets
was large enough to overcome the resistance force, the droplets
departed from the surface. In other words, the wettability gra-
dients enabled the hybrid sample to have a structure similar to
the back of beetle, which greatly improved the water harvesting
efficiency.
3.2.3. Spilled Oil Crossflow Collection
The frequent occurrence of oil spill not only seriously dam-
ages marine ecosystem, but also causes a huge loss of energy
resources.[112–114] Traditional methods of cleaning spilled oil,
such as absorbers, chemical dispersion and skimmers, suffer
from low efficiency. In nature, fish gills can collect small food
from parallel flow of suspension liquid and drain water away
effectively. Inspired by fish gills, a gradient-wettability mesh
with nanoripple structures was fabricated by femtosecond
laser direct writing technology, which could be used for spilled
oil crossflow collection.[101] Figure  8a is a schematic diagram
of a system that can quantitatively describe the oil collection
efficiency, which consists of two moving platforms, an oil con-
tainer, the gradient-wettability mesh and a water cylinder. The
gradient mesh was placed at an inclination of 30° with small
pores at the top and large pores at the bottom, and its 2D direc-
tion and speed could be adjusted by two moving platforms.

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Figure 8.  Wettability gradient surface for applications in spilled oil crossflow collection. a) Schematic diagram of the system for spilled oil crossflow
collection. b) Oil collection rates of the gradient-wettability mesh for various oils. c) Comparisons of oil collection rates between the wettability gradient
mesh and the mesh with different pore sizes (≈90 and ≈50 µm). d,e) Schematic illustration of the oil and water behaviors on the laser-treated mesh
with single pore size (≈50 µm) and gradient-wettability mesh. d,e) Reproduced with permission.[101] Copyright 2018, Elsevier.
Water and oil were poured into the tank to simulate the oil
spill, and the oil layer was set to be 3  mm thick. Because of
the different oil and water wettability of the sample, water was
gradually filtered through the larger pores at the bottom. While
the oil was not filtered and transported from the bottom to top,
eventually collected by the container. The oil collection rate
(OCR) was calculated by R = V/(W × t), where V is the volume
of collected oil, W is the mesh width, and t is the collection
time.
The collection rate for different oil types decreased slightly
as the collection time increased. However, the OCR was still
greater than 58 L m−1 min−1 after 30 min, indicating that the
as-prepared sample possessed good oil collection performance
regardless of oil types (Figure  8b). In addition, they compared
the oil collection rate of the wettability gradient mesh with
the normal mesh with different pore sizes (≈90 and ≈50  µm).
It was observed that the OCR of gradient sample was signifi-
cantly higher than that of normal samples, exhibiting excellent
performance of spilled oil crossflow collection (Figure  8c).
Figures  8d,e shows the possible mechanism of spilled oil col-
lection in the laser-treated mesh with single pore size (≈50 µm)
and the gradient-wettability mesh. For the laser-treated mesh
with single pore, water continuously and uniformly penetrates
through the mesh. Meanwhile, the water and oil are both trans-
ported upward along the mesh. Eventually, the container col-
lects a mixture of oil and a small amount of water (Figure 8d).
For the gradient-wettability mesh, water penetrates through
the mesh with larger pores with high flux and is trapped in the
smaller pores. But the oil is repelled by the sample and con-
tinuously collected by mesh in the smaller pores, eventually
flowing into the container (Figure 8e).
In this section, we introduce the efficient and rapid prepara-
tion of various wettability gradient surfaces by different laser
processing methods. The related applications of wettability gra-
dient surfaces for controlling droplet behavior, fog/water col-
lection, and spilled oil crossflow collection are also introduced.
And Table  1 summarizes different processing parameters for
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the fabrication of wettability gradient surfaces and their various
related applications.
4. Geometric Gradients
4.1. Laser Fabrication of Different Geometric Gradient Surfaces
4.1.1. Wedge Shape Gradients
The surface of a wedge shape gradient has a narrower tip and a
wider end, and the chemical composition of the surface is uni-
form. Another important feature is that the gradient width of
the wedge surface increases gradually along the axis direction,
and wedge-shaped gradients surfaces usually contain some
areas hydrophilic to the liquid. On the one hand, laser pro-
cessing can adjust the wettability of the surface by altering the
micro/nano structures and chemical elements. On the other
hand, lasers can also be adopted to cut materials into different
geometric shapes or scan different paths. Based on the above
characteristics of laser, laser processing techniques reveal great
advantages in producing wedge shape gradients.
One way is to cut the sample into the anticipated wedge
shape by laser, then modify the wettability into hydrophilic to
liquid by chemical modification. In Figure 9a, a trapezoidal gra-
dient slippery surface was successfully prepared by the method
of CO2-laser cutting, superhydrophobic modification, and fluo-
rine infusion.[115] First, a hydrophobic polymethyl methacrylate
(PMMA) was cut into the desired wedge gradient morphology
under the assistance of the controllable CO2-laser device. Then,
the wedge surface became superhydrophobic with WCA of
152 ± 2° by painting the superhydrophobic solution on its sur-
face. Finally, the roughness of the surface was greatly reduced
by introducing the Fluorinert liquid on the surface. The WCA
on the slippery surface decreased to 118  ± 3°, indicating the
as-prepared sample was hydrophobic in air. When it was
immersed in an aqueous environment, the slippery surface
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Table 1.  Laser processing of wettability gradient surfaces and their applications.

Laser source Parameters (wavelength/repetition Main material Wettability gradient Mechanism Application Ref.
rate/duration/intensity)
Universal Laser Systems 5000 Hz, 25 W PDMS Hydrophobic–hydrophilic Laser scanning Droplet translocation [99]
and droplet mixing
– – Silicon wafer Hydrophilic–more hydrophilic Laser etching Self-motion of Leiden- [108]
frost droplet
Nanosecond fiber laser 1064 nm, 40 kHz, 100 ns, 430 µJ Copper Hydrophilic–superhydrophobic Laser scanning Fast water flow [103]
A ultra-short pulse laser 20 Hz, 6 W NiTi alloy Hydrophobic–more hydrophobic Laser etching Low water resistance [100]
Laser at a special power 20 kHz, 200 ns, 30 W Cu, PDMS/G Superhydrophobic and Laser etching Fog collection [98]
hydrophobic
Femtosecond laser 1030 nm, 75 kHz, 250 fs, 6 W Copper mesh, copper Superhydrophobic–hydrophilic Laser scanning Fog collection [112]
sheet
Femtosecond laser 1030 nm, 75 kHz, 250 fs, 6 W Stainless steel meshes Olephilic–more olephilic Laser scanning Spilled oil crossflow [101]
collection
Nanosecond pulsed 1064 nm, 25 kHz, 220 ns, 0.252 mJ Brass sheets Hydrophilic–more hydrophilic Laser scanning Multi-sensitivity [102]
fibre laser chemical sensors

became aerophilic with bubble contact angle (BCA) of 63 ± 2°.
In other words, a trapezoidal gradient slippery surface was suc-
cessfully fabricated by laser cutting and chemical modification.
Another method is to cut the sample into a wedge and change
the wettability of the surface into hydrophilic both by laser. For
example, the rectangular PTFE sheet was cut into a trapezoid
by femtosecond laser, then the trapezoidal platform was line
by line scanned by femtosecond laser to alter the wettability
(Figure 9b).[116] The original PTFE had a smooth surface, and its
wettability was hydrophilic in air with WCA of 76 ± 1° (θorig) and
hydrophobic in water with BCA of 95 ± 1°. When the trapezoid
sample was laser-treated, the surface became rough with many
cavities and protrusions distributed. And its wettability changed
into superhydrophobic in air with WCA of ≈159° (θlaser) and

Figure 9.  Various methods to prepare wedge shape gradient surfaces. a) The fabrication of a trapezoidal gradient slippery surface by laser cutting,
superhydrophobic modification, and fluorine infusion. Reproduced with permission.[115] Copyright 2018, American Chemical Society. b) The preparation
procedures of the trapezoidal platform with micro/nano hierarchical structures by femtosecond laser cutting and scanning. Reproduced with permis-
sion.[116] Copyright 2019, Elsevier. c) The fabrication of the dual-rails wedge gradient system via one-step femtosecond laser ablation. Reproduced with
permission.[117] Copyright 2020, American Institute of Physics.

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underwater superhydrophilic with BCA of ≈0°. The differences
of WCA can be explained by Cassie model, where f is connected
with the proportion of protrusion and surface roughness. For
laser treated PTFE, 0 < f < 1. So we can derive that cos θlaser <
cos θorig according Equation  (3), which means θlaser  > θorig. A
trapezoidal platform with micro/nano hierarchical structures
was fabricated by femtosecond laser cutting and scanning.
In addition to cutting the substrate into a trapezoid-shape
gradient, the dual rails wedge gradient can also be prepared
by one-step laser ablation.[117] The interior of the dual rail can
be considered as a trapezoid, where the detailed preparations
are shown in Figure 9c. A hollow dual rail pattern was formed
by direct femtosecond laser scanning on stainless-steel sheet.
The hollow stainless-steel sheet and PDMS substrate were com-
bined by physically sticking, which was then vertically crossed
scanned by femtosecond laser irradiation to enhance the sur-
face roughness. The wettability of the dual rails was superhy-
drophobic being beneficial to the underwater bubble adhesion.
However, the rest portion of the substrate was superhydrophilic
to reduce the bubble adhesion. Therefore, a system of super-
hydrophobic narrowing dual rails was constructed by one-step
femtosecond laser ablation.
4.1.2. Conical Shape Gradients
Geometric gradients can not only be generated from wedge-
shaped surface, but also can be generated from conical surface.
However, these two gradient structures are produced in dif-
ferent ways. The wedge surface provides a gradient width along
the longitudinal while the cone structure provides a radius
gradient by varying the length. There is a Laplace differential
pressure on the conical structure due to the asymmetry between
the front and rear ends. A two-step femtosecond laser direct
writing technique can enormously improve the processing effi-
ciency of cone (Figure  10a).[118] Specifically, PTFE was cut into
conical shape by the modified sharpener, and then the surface
was directly scanned by two-step femtosecond laser forming a
hierarchical microstructure. There were many coral-like micro-
structures with the size of several micrometers randomly dis-
tributed on the laser treated PTFE conical gradient surface.
Therefore, a macroscopic conical structure was formed via two-
step femtosecond laser direct writing. Natural pine needles are
conical in shape and have a gradient in height, opposing flat
and curved surfaces. These unique features contribute to the
water transport on pine needles, which inspires Feng et  al. to
prepare pine needle-inspired asymmetric surfaces (PNAS) by
3D printing (Figure  10b).[119] PNAS were made of tilted (≈70°)
and flat-curved conical pillars with a height gradient ≈20°,
which were dispersed on a square array with interpillar dis-
tance of s = 300 µm. They also fabricated tilted flat-curved pil-
lars without gradient in height for comparison. By 3D printing,
neat conical arrays with different height gradients could be
quickly prepared.
Apart from the macroscopic conical gradient structure, many
miniature conical gradients are incorporated into the design
of sample due to their enhanced effect on wetting. Microcones
can generally be obtained by laser drilling, which can be car-
ried out before or after chemical modification. In the work of
Chen et  al., a flexible PDMS membrane was first obtained by
spin-coating and curing.[120] Then the PDMS membrane was
processed into micropore-arrayed pattern through a subsequent

Figure 10.  Various methods to prepare conical shape gradients. a) The preparation of macroscopic conical structure by two-step femtosecond laser
direct writing. Reproduced with permission.[118] Copyright 2018, American Institute of Physics. b) Pine needle-inspired asymmetric surfaces fabricated
by 3D printing. Reproduced with permission.[119] Copyright 2020, American Association for the Advancement of Science. c) The fabrication of the
micropore-arrayed PDMS by spin-coating, curing, and subsequent laser drilling. Reproduced with permission.[120] Copyright 2019, Wiley-VCH GmbH.
d) Fabrication procedures and wettability of the polyester/nitrocellulose textile with asymmetric conical micropores via CO2 laser drilling, plasma
modification. Reproduced with permission.[121] Copyright 2019, Wiley-VCH GmbH.

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laser drilling process (Figure  10c). Since the essence of the
laser was a Gaussian beam, the upper and lower surfaces were
induced into different morphologies. This morphological differ-
ence resulted from the different roughness and wettability on
both sides, whose WCA are 95  ± 3° (upper), 147  ± 5° (lower),
respectively. The cross-sectional view of the micropore-arrayed
PDMS indicated that the micropores are all conical shapes. In
Figure  10d, the unmodified polyester/nitrocellulose (PE/NC)
textile with conical micropores was first fabricated by CO2
laser drilling, and then the drilled textile was modified with
plasma.[121] SEM images of a single micropore indicate that it
was a conical shape with asymmetric morphology. In the air,
the PE layer showed hydrophobicity with WCA of 80.0  ± 1.6°,
and the NC layer showed superhydrophilicity with WCA of ≈0°.
The schematic diagram visually displayed the structure and
characteristics of the as-prepared PE/NC textiles with asym-
metric microcones. In another study, Ren et at. also prepared
the hydrophilic/hydrophobic heterogeneous membrane with
conical micropores drilling and scanning both by laser.[122]
4.1.3. Wedge-Shaped Combination Gradients
For a single wedge and conical gradient, their size makes it dif-
ficult for them to achieve large-scale applications. In order to
improve this problem, the formation of wedge-shaped combi-
nation gradient combing laser has become the research focus.
Similar to the preparation of other geometric structures, the
laser processing can be used to produce micro–nano struc-
tures at any stage of the experiment. For instance, Wang et al.
fabricated the tree-shaped hierarchical cones by chemical
modification and laser scanning.[123] This design could not take
full advantage of the entire surface with only multilevel tree-
shaped hierarchical cones. The existing tracks restrict each
other, which limits their overall sizes and flexible designs.
In order to effectively utilize most areas of the substrate, Liu
et  al. prepared a superhydrophilic–superhydrophobic vena-
tion network (Figure  11a).[124] The aluminum (Al) sheet was
first irradiated by femtosecond laser to create micro–nano
dual-scale hierarchical structures. Regular micropillars with
dense nanoparticles were distributed on its surface after first
laser irradiation. Then the samples were modified by the 1H,
1H, 2H, 2H-perfluorodecyltrimethoxysilane alcohol solution,
which made it superhydrophobic. Finally, the modified sample
was irradiated by a selective nanosecond laser to scan venation
network patterns. The network patterns were superhydrophilic
due to the removal of the 1H, 1H, 2H, 2H-perfluorodecyltri-
methoxysilane modification layer. After the nanosecond laser
irradiation, dense nanovillus replaced almost all the existing
nanoparticles. By this time, the venation network surfaces
with ultra-contrasting wettability were prepared by twice laser
treatment.
Hou et  al. proposed a facile and reliable method to fabri-
cate superhydrophilic triangular array on copper substrates
(Figure  11b).[125] By wet-etching process and silane treatment,
the superhydrophobic copper surfaces were first created. Then
superhydrophilic triangular array was selectively inscribed by
laser-engraving. The patterns in the array were all isosceles tri-
angles, where the tip of the lower triangle connected to the base
of the upper triangle in the vertical direction. A thin layer of
knife-like nanostructures covered on the superhydrophobic sur-
face with WCA of ≈168°. After laser treating, the nanostructures

Figure 11.  Various methods to prepare wedge-shaped combination gradients. a) Fabrication processes of the superhydrophilic–superhydrophobic
venation network based on twice irradiation of ultra-fast lasers. Reproduced with permission.[124] Copyright 2019, Royal Society of Chemistry. b) The
fabrication processes of triangular array on the superhydrophobic substrates by laser ablation. Reproduced with permission.[125] Copyright 2020, Wiley-
VCH GmbH. c) Fabrication processes of cactus kirigami with triangle-shaped combination gradients via laser cutting and hydrophobic modification.
Reproduced with permission.[130] Copyright 2020, Royal Society of Chemistry. d) Preparations for a serial wedge-shaped wettability pattern by a universal
method composed of electrochemical etching and laser etching. Reproduced with permission.[131] Copyright 2019, Royal Society of Chemistry.

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and the coating material were removed, leaving the superhydro-
philic triangular pattern with rough microtextures. As a result,
the triangular-shaped array on the superhydrophobic substrates
were successfully fabricated by laser ablation.
In addition to traditional metallic materials, the common
low-cost paper can also be used to prepare wedge-shaped
combination gradients. The traditional art of kirigami creates
some interesting geometric structures by cutting and folding
paper, inspiring many designs in the field of advanced mate-
rials.[126–129] Enlightened by cactus spines and kirigami, a
cactus kirigami with fog collecting spines was designed that
simplifies the 3D complicated structure into 2D hollow plate
(Figure  11c).[130] The fabrication processes of cactus kirigami
included the laser cutting filter paper by a CO2 laser marker,
and hydrophobic modification by soaking the laser-cutting
sample into the melting paraffin. The laser-cutting paper spine
with triangle-shape possessed superhydrophilicity due to its
porous structure of cellulose microfibers. Paraffin wax has pure
chemical composition and durable hydrophobicity, which has
been widely used in commercial products including disposable
cup and stencil paper. So the spine became hydrophobic with
WCA of 102.2  ± 0.8° after simple wax modification, and the
surface became smooth compared to the ablated paper. That is,
the cactus kirigami with triangle-shaped combination gradients
could be fabricated by laser cutting and wax modification.
The traditional geometric gradient structures are gener-
ally not large enough, which constitutes the barrier to their
practical applications. This problem could be figured out by
a serial wedge-shaped wettability pattern, which consists of a
front triangle and several rear trapezoids connected end to
end.[131] In this pattern, the terminal size has no relationship
with the length of the whole pattern meaning the length is not
limited, where the detailed fabrication processes are shown in
Figure  11d. First, superhydrophilic Al plate with micrometer-
scale rough structures were obtained by electrochemical etching
the Al in sodium chloride solution (NaCl). Then the superhy-
drophilic sample was immersed in fluoroalkyl silane (FAS)
solution, which deposited the FAS layer on the rough structures
to make it superhydrophobic. Finally, the serial wedge-shaped
gradient was formed by laser scanning, and the wettability of
the wedge tracks transformed from superhydrophobic into
superhydrophilic. Therefore, a serial wedge-shaped wettability
pattern with exterior superhydrophilic and interior superhy-
drophobic was prepared by chemical modification and laser
scanning. The superhydrophobic region (WCA = 159.0  ± 2.3°)
consisted of rectangular plateaus and step-like structures with
sizes of ≈1–5 µm. The superhydrophilic region (WCA ≈ 0°) had
rough micropores and protrusions, which were composed of
particles with sizes of 100 nm to 4 µm.
4.2. Applications of Geometric Gradient Surfaces
4.2.1. Directional Self-Transport
The directional and continuous transportation of microfluid
without energy input has aroused extensive interest,[132–139]
which advances excellent performances in microfluid move-
ment, microfluid collection, and water splitting. So far, most
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studies have demonstrated that geometric gradient surfaces
can achieve directional self-transport in different environments,
such as underwater bubbles, underoil water droplets, and water
droplets in air. Ma et  al. facilely prepared superaerophilic tra-
pezia-shape PE surface, which was capable of spontaneously
and directionally self-transporting the underwater bubbles
from the minor side to the large side of the trapezoid.[136] The
superaerophilic trapezoidal PTFE platform that prepared by
femtosecond laser in the work of Yin et al. displays the similar
behaviors of underwater bubbles.[116] The microhole-arrayed
PDMS with conical-shapes of Chen et  al. could speed up the
unidirectional self-transport of underwater bubble.[120]
In fact, the directional self-transport in oil environment
is more difficult than that in water environment due to the
viscous oil tends to stick to objects. In order to realize self-
transport in oil, a superhydrophilic trapezoidal stainless-steel
platform was fabricated to realize the directional self-transport
of underoil water droplets (Figure 12a).[140] Affected by the geo-
metric gradient, this structure could transport underoil water
droplets spontaneously and directionally from the minor side to
the large side of the trapezoidal platform.
On the horizontally-oriented trapezoidal platform surface,
the three forces that determine the movement of water are the
geometry-gradient force (Fshape), the hysteresis resistance force
(Fres), and the drag force of oil (FD). The resulting total force (F)
can be deduced as
F = Fshape + Fres + FD (9)
1 1
From Equation  (6), Fshape  γ  −  . When water was
 R1 R 2 
released on the under-oil sample, R1 < R2, which renders Fshape
as the driving force. Because the laser treated surface is under-
oil superhydrophilic, both θr and θa can be taken as 0°, which
produce Fres close to zero according Equation (8). The resistant
force FD hinders the motion of water, and can be expressed
as FD  ≈ CDρν2A, where CD and ρ are the drag coefficient and
density of oil, respectively; ν and A are the transport velocity
and cross-sectional area of the water, respectively. The resistant
force FD is smaller than Fshape, so water can accomplish move-
ment from the minor side to the large side under the driving
force.
The trapezoid semi-apex angle, the tilt angle of the trap-
ezoid platform, and the volume of water play a crucial role in
determining the transport speed of water droplets. The trans-
port speed of the drop is inversely proportional to the trapezoid
semi-apex angle and proportional to the tilt angle of the trap-
ezoid and the volume of the drop. These phenomena are con-
sistent with theory. From Equation  (6), the R1 and R2 have an
important influence on the Laplace pressure difference. When
the semi-apex angle decreases or the volume of water increases,
the difference between R1 and R2 increases resulting from the
increasement of the Laplace pressure. The transport speed
decreases with the trapezoid tilt angle can be well explained by
the force analysis of water droplet on the oblique trapezoid sur-
face. The gravity component along the slope impedes the water
uphill movement from the minor side to the large side. When
the trapezoid tilt angle increases, the gravity component of the
water increases and thus decreases the transport speed.
© 2021 Wiley-VCH GmbH
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Figure 12.  Different geometric gradient surfaces for directional self-transport. a) The superhydrophilic trapezoidal stainless-steel platform is capable
of transporting the underwater bubble from the minor side to the large side. Reproduced with permission.[140] Copyright 2020, Royal Society of Chem-
istry. b) Water droplet directional self-propulsion without mass loss or mixing on the superhydrophobic microtracks. Reproduced with permission.[141]
Copyright 2020, American Chemical Society. c) The long-distance delivery of underwater bubbles was realized by a serial wedge-shaped wettability
pattern. Reproduced with permission.[131] Copyright 2019, Royal Society of Chemistry. d) Spontaneous and unidirectional transportation the wide end
to narrow end of the superhydrophobic narrowing dual rails. Reproduced with permission.[117] Copyright 2020, American Institute of Physics. e) The
dynamic transport processes of bubble on the laser-treated cone at 0° and 90°. Reproduced with permission.[118] Copyright 2018, American Institute of
Physics. f) Droplet transports on the PNAS with height gradient and tilted flat-curved pillars without height gradient. Reproduced with permission.[119]
Copyright 2020, American Association for the Advancement of Science.

During the aforementioned directional transport processes,
a certain amount of fluid mass is lost or mixed with the sur-
face. That is, instead of spreading the deposited mass, a frac-
tion of fluid mass reaches the final end of the hydrophilic
region. Stamatopoulos et  al. prepared a superhydrophobic
wedge track-based topography by laser micromachining and
chemical etching followed by surface hydrophobization. This
design could achieve water droplet directional self-propulsion
without mass loss or mixing on the superhydrophobic micro-
tracks (Figure  12b).[141] Its propulsion force derived from the
Laplacian pressure of trapezoidal structure between the adja-
cent superhydrophilic grooves. However, the abovementioned
structures cannot realize long distance directional self-trans-
port which greatly restricts their practical application. A serial
wedge-shaped wettability pattern designed in Figure  11d could
be applied to realize long-distance underwater bubbles.[131] The
bubbles released at the beginning could easily cross 10 junc-
tions and travel up to 80 mm (Figure 12c).
Directional self-transport can be realized not only by trape-
zoidal structure, but also by other geometric gradient structure,
such as dual rails system and conical structure. The superhy-
drophobic narrowing dual rails system designed in Figure  9c
could spontaneously and unidirectionally transport underwater
bubbles from the wide end to narrow end (Figure  12d).[117]
The superaerophilic PTFE cone fabricated in Figure  10a was
placed horizontally (0°) to minimize the effect of buoyancy and
enhance the influence of geometric gradient on bubble behav-
iors (Figure  12e).[118] When the bubble contacted the cone, the
bubble was captured effectively and transported toward the
large side with velocity of 8.8  cm s−1. As the cone was placed
at 90°, the transport velocity increased to 18.5  cm s−1. These
phenomena indicate that the conical structure can realize direc-
tional self-transport of underwater bubbles. In the work of Feng
et al., tip-induced flipping of droplets occurred on conical PNAS
with height gradient, whose transport direction was toward pos-
itive +x.[119] On tilted flat-curved pillars without height gradient,

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droplets not only could get ejected in the +x direction as they
coalesce, but also could turn back in the −x direction due to int-
erpillar coalescence (Figure 12f). The synergistic effects of cur-
vature and height gradients enabled the directional transport
of droplets on conical PNAS with height gradient. The above
transport phenomena all do not require external forces, whose
motion forces are derived from the Laplace pressure difference
generated by their own geometric structures.
4.2.2. Fog/Water Collection
The fog/water collection can be realized by wettability gradients,
but such collection cannot be transported and collected along the
specified tracks. In contrast, the precise and directional fog/water
acquisition can be realized by geometric gradient structures.
For example, Liu et  al. fabricated superhydrophilic/superhydro-
phobic patterned surfaces to achieve high fog collection efficiency
(Figure  13a).[142] Superhydrophobic surfaces were prepared by
laser etching and low surface energy modification, and superhy-
drophilic fan-shaped patterned surface were formed by secondary
laser etching. The upper part was composed of a parallel wedge
pattern, which could accelerate the transport efficiency of droplet.
Finally, the droplet merged directionally in the lower triangular
region and increases gradually until the droplet rolls down. This
fog collection phenomenon could be observed on various sam-
ples, including Al, Cu, steel, and Ti plates. Wang et al. fabricated
a tree-shaped hierarchical cone pattern, which could drive drop-
lets move toward the larger cones directionally and collect water
precisely and continuously at the target location.[123] Liu et  al.
prepared the venation network utilizing ultra-fast lasers, whose
large area were devoted to collecting the condensed water toward
the target location.[124] And the hydrophilic/hydrophobic hetero-
geneous membrane with conical micropore arrays fabricated by
Ren et al. could also be adopted to harvest water. This heteroge-
neous membrane possessed a large enhancement of WCR than
the normal superhydrophilic membranes.[122] The superhy-
drophilic triangular patterns in the work of Hou et  al. can fast
condensate droplet nucleation, directional delivery, and efficient
departure, which can be used for dew harvesting.[125]
Apart from these traditional metallic materials, the common
low-cost paper designed in Figure  11c can simplify the cactus-
inspired fog collection spines from 3D cone to 2D triangle.[130]
It was noted that the arrangement of the spines will influ-
ence fog collecting, so two distinct cactus kirigami structures
including symmetric and alternative arrangements were com-
pared (Figure 13b). Under the forces of geometric gradient, all
arrays of spines could carry droplets from the tip to the root.

Figure 13.  Different geometric gradient surfaces for fog/water collection. a) Fan-shaped patterned surface for fog collection on different metal sur-
faces. Reproduced with permission.[142] Copyright 2020, American Chemical Society. b) The fog harvesting performances of two distinct structures of
cactus kirigami, including symmetric and alternative arrangements. Reproduced with permission.[130] Copyright 2020, Royal Society of Chemistry. c) An
improved self-propelled miniboat composed of a superhydrophilic wedge-shaped pattern, a superhydrophobic background and a superhydrophobic
miniboat was assembled for long-distance movement. Reproduced with permission.[144] Copyright 2020, Wiley-VCH Verlag.

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However, the critical volume of droplet sliding on the spines
with symmetric arrangement was larger than that of the spines
with alternative arrangement. Therefore, the spines with alter-
native arrangement were selected for water harvesting because
suspended droplets on spines should be discharged facilely
and stored quickly to reduce possible water loss. By setting
appropriate parameters, the water harvesting rate of the low-
cost paper substrates could be up to ≈4000  mg cm−2 h−1. This
implied that ordinary paper could be designed to cactus kiri-
gami structures, which was satisfied with the scalable and
affordable fog collection in practical applications. The hard-
ness of glass is relatively high, and the superwettability of glass
treated by laser is relatively less studied. So, Zhang et  al. uti-
lized laser ablation and fluoroalkylsilane modification to pre-
pare wedge-shaped patterns on glass, which could be a prom-
ising candidate for water harvesting.[143] It is worth noting that
the above substrates for fog/water harvesting are all equipped
with geometric gradient, which supplies the Laplace driving
force for water transport and collection.
The geometric gradient structures can not only be used for
fog collection merely, but also can reuse the collected water
to drive other objects. Song et  al. discovered a green method
for miniboat self-propelling based on the Laplacian pressure
of water droplets (Figure  13c).[144] When water droplets were
put on the inclined superhydrophilic pore on the superhydro-
phobic triangular miniboat, water passed through the pore
and formed a jellyfish-like jet. This jet could propel a mini-
boat spontaneously and directionally without extra energy. But
the miniboat could not move long distances continuously due
to the short propelling time of water. In order to tackle this
problem, an improved self-propelled miniboat composed of a
superhydrophilic wedge-shaped pattern, a superhydrophobic
background and a superhydrophobic miniboat was assembled.
Water could be absorbed by the root-like part and then trans-
ported to the trunk, eventually moving to the end of the pattern.
When the collected water accumulated to a certain volume, it
passed through the superhydrophilic hole to propel the long-
distance movement of miniboat.
4.2.3. Water Electrolysis
Water electrolytic as a highly promising method of hydrogen
and oxygen production has attracted much attention.[145–147] Tra-
ditional methods of water electrolysis suffer from high cost and
poor stability, and the application of geometric gradient struc-
ture greatly simplifies the configuration. For example, Long et al.
designed a facile water-splitting device with functions of bubble
generation, transport, and pure collection (Figure  14a).[148] The
core components of the device were two electrodes and two
trapezoidal gradient arrays with the superhydrophobic surface
facing up. The installation of the two arrays was complemen-
tary and compact, which contributed to improve the electrolytic
efficiency. Time sequences of images exhibited the process of
water electrolysis, where bubbles mainly generated below the
trapezoidal gradient and passed through the foam channel.
Then the bubbles on the upper surface moved to the root of the
respective trapezoidal gradient and finally were collected by the
two-receiving flask. The gas collection of H2 and O2 increased
in a step-like manner, indicating that bubble transport existed
in the process of water electrolysis. The volume ratio of H2 and
O2 fluctuated at the beginning while subsequently stabilized at
a ratio of 2:1, which verified that this device could accurately
and effectively realize water electrolysis.

Figure 14.  Different geometric gradient surfaces for water electrolysis. a) The designed device with two multi-electrode arrays for water electrol-
ysis. Reproduced with permission.[148] Copyright 2020, Wiley-VCH GmbH. b) The star-shaped slippery electrode for water electrolysis under high pressure
(≈0.65 MPa). Reproduced with permission.[115] Copyright 2018, American Chemical Society.

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The above device can realize water electrolysis under
normal temperature and pressure, but it is still difficult
to realize water electrolysis under high-pressure environ-
ment. To work out this problem, a star slippery electrode
with conductive copper wire covering the edge was prepared
(Figure  14b).[115] The copper electrode was connected to the
negative electrode of the battery by a copper wire. When
voltage was applied at high pressure (≈0.65  MPa), a large
number of hydrogen microbubbles generated on the copper
electrode. As the hydrogen bubbles grew and came into con-
tact with the slippery surface, they were captured and trans-
ported to the center. With continuous capture and transport,
the generated H2 bubbles eventually released into the gas con-
tainer under the effect of buoyancy. Therefore, the as-prepared
star slippery electrode achieved continuous water electrolysis
and efficient collection of H2, demonstrating potential func-
tions in high-pressure environments. In the aforementioned
water electrolysis device, the existence of geometric structure
makes the gas generated by water decomposition effectively
collected, and the two gases of hydrogen and oxygen do not
interfere with each other.
In this section, we introduce different laser processing
methods for various geometric gradient surfaces, including
wedge shape gradients, conical shape gradients, and wedge-
shaped combination gradients. The related applications of
geometric gradient surfaces can be applied in directional self-
transport of microfluidics, fog/water collection, and water
electrolysis. And Table  2 summarizes different processing

Table 2.  Laser processing of geometric gradient surfaces and their applications.

Laser source Parameters(wavelength/repeti- Main material Geometrical shape Mechanism Application Ref.
tion rate/duration/intensity)
CO2-laser device 30 W PE sheet Trapezoid Laser cutting Directional self-transport of under- [136]
water bubble
Femtosecond laser 1030 nm, 75 kHz, 250 fs, 10 W PTFE Trapezoid Laser cutting and Directional self-transport of under- [116]
scanning water bubble
Femtosecond laser 800 nm, 1 kHz, 104 fs, 350 mw PDMS Microcone Laser etching and laser Unidirectional self-transport of under- [120]
drilling water bubble
Femtosecond laser 1030 nm, 75 kHz, 250 fs Stainless steel Trapezoid Laser cutting and Directional self-transport of underoil [140]
scanning water
Ultra-short pulsed laser 515 nm, 1 MHz, 800 fs, 2 W Copper Trapezoidal microtracks Laser scanning Directional self-transport of water [141]
A fiber laser marking 1064 nm, 20 kHz, 20 W Aluminium plate A serial wedge-shaped Laser scanning Long-distance directional [131]
system pattern self-transport
Femtosecond laser – Steel sheet Dual-rails Laser cutting and Directional self-transport of under- [117]
scanning water bubble
Femtosecond laser 1030 nm, 75 kHz, 250 fs, 6 W PTFE Cone Laser scanning Directional self-transport of under- [118]
water bubble
Microstereolithography- – ZnO Cone – Directional self-transport of water [119]
based 3D printing
A laser machine 20 kHz, 100 ns Al, Cu, Steel, Ti Fan-shaped pattern Laser scanning Fog collection [142]
A commercial fiber 1.06 µm, 8 W Copper foil Triangular-shaped Laser scanning Dew collection [125]
laser-engraving system pattern
Laser direct writing 405 nm, 500 kHz, 2000 ns, Ti film Tree-shaped hierarchical Laser scanning Water collection [123]
system-1500 56.6 J cm−2 cones
Femtosecond laser and 1030 nm, 800 fs; 532 nm, 12 ns Aluminum alloy Venation network Laser scanning Water collection [124]
nanosecond laser
Femtosecond laser 800 nm, 1 kHz, 104 fs Aluminum foil Microcone Laser etching and laser Fog collection [122]
drilling
CO2 laser – Filter paper Cactus kirigami Laser cutting and Fog collection [130]
scanning
Fiber laser system 1064 ± 5 nm, 20 kHz, 100 ns, Glass Wedge-shaped patterns Laser scanning Fog collection [143]
318.5 J cm−2
– 1064 nm, 20 kHz, 100 ns Al plate Wedge-shaped pattern Laser etching and laser Self-propelling miniboat [144]
drilling
A laser device – Nickel foam Triangles Laser cutting Water electrolysis [148]
CO2-laser device 27 W PMMA Trapezoid and a star Laser cutting Water electrolysis under high-pressure [115]
slippery electrode
CO2 Laser 40 W PE/NC Microcone Laser drilling Moisture and thermal management [121]
membrane

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parameters for the fabrication of geometric gradient surfaces
and their various related applications.
5. Conclusion and Outlook
This review summarizes the recent research on the laser fab-
rication of bioinspired gradient surfaces for wettability appli-
cations. Background including gradient surfaces in natural
creatures, the theoretical basis of wettability, and distinct fea-
tures of laser processing was introduced. Laser processing can
be used to process diverse patterns on various substrates with
a facile and efficient manner, so is effective for preparing bioin-
spired gradient surfaces. Laser fabricated gradient surfaces can
be divided into wettability gradients and geometric gradients,
whose respective fabrication approaches and wettability applica-
tions were presented. Laser-processed wettability gradients are
derived from differences in roughness, and can be applied in
controlling droplet behavior, fog/water collection, and spilled
oil crossflow collection. Laser-ablated geometric gradients are
derived from the geometric configuration, and can be applied
in directional self-transport in microfluidics, fog/water collec-
tion, and water electrolysis.
The past few years have witnessed the development of
micro–nanotechnology, and lots of functional materials have
been studied.[149–163] Despite advances in laser-treated gradient
functional surfaces, challenges, and opportunities remain.
Reported studies are limited to a very small amount of living
organisms with gradient structures, such as desert beetles, peri-
stome, cacti, spiders, and pine needles. More species with gra-
dient organisms undoubtedly remain to be discovered, which
will provide further insight and inspiration. The gradient sur-
faces discussed in this review comprise wettability gradients
and geometric gradients, while other unknown gradients and
mixed gradients remain to be explored. On the microscopic
scale, the interaction between droplets and gradient surfaces
may produce further interesting phenomena. Reported gra-
dient surfaces also typically suffer from poor chemical stability
or low performance in poor environments. It is necessary to
improve the stability, durability, and long-distance transporta-
tion capacity of laser treated samples. This may be addressed by
doping with composite materials such as inorganic nanoparti-
cles and graphene. Finally, current applications of gradient sur-
faces mainly concentrate on behavior control and collection in
microfluidics. The scope should be scaled up to include applica-
tions such as drug delivery and aerosol filtration.
Laser processing has an important role in preparing gradient
surfaces on various materials. The rapid development in laser
technology may further produce gradient surfaces with high
stability, durability, and arbitrary shapes. And the development
of 3D laser printing technology will also give new vitality in the
preparation and application of gradient surfaces. Therefore,
laser fabrication of bioinspired gradient surfaces should be
expected to lead to broad future innovations.
Acknowledgements
This research was supported by National Natural Science Foundation
of China (Grant No. 52075557, 51805553), Natural Science Foundation
Adv. Mater. Interfaces 2021, 8, 2001610 2001610  (20 of 23)
www.advmatinterfaces.de
of Hunan Province (Grant No. 2018JJ3666), the Project of State Key
Laboratory of High Performance Complex Manufacturing, Central South
University (Grant No. ZZYJKT2019-12).
Conflict of Interest
The authors declare no conflict of interest.
Keywords
bioinspired, geometric gradients, laser processing, wettability
applications, wettability gradients
Received: September 11, 2020
Revised: November 22, 2020
Published online: January 18, 2021
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Junrui Wu is currently a graduate student in the School of Physics and Electronics, Central South
University. She was awarded a national scholarship in 2020, and she will receive her master’s
degree in 2021. Her research mainly focuses on the influence of femtosecond laser micro–nano
fabrication on wettability and its application in wettability.

Kai Yin received his Ph.D. in Mechanical Engineering in 2016 from Central South University
(CSU), and being a visiting Ph.D. student from 2014 to 2015 at the University of Rochester, USA.
In 2017, he became an assistant professor of CSU. In 2018, he became an associate professor of
CSU. His research interests include laser micro–nano machining, superwetting interface design,
and functional device manufacturing and application.

Adv. Mater. Interfaces 2021, 8, 2001610 2001610  (23 of 23) © 2021 Wiley-VCH GmbH