Appl. Phys.
A (2016) 122:834
DOI 10.1007/s00339-016-0361-8
Femtosecond laser-induced periodic surface structural formation
on sapphire with nanolayered gold coating
Kai Yin1,2 Cong Wang2 Jian Duan2 Chunlei Guo1
Received: 7 February 2016 / Accepted: 10 August 2016 / Published online: 19 August 2016
 Springer-Verlag Berlin Heidelberg 2016
Abstract Sapphire has a potential as a new generation of
electronics display. However, direct processing of sapphire
surface by visible or near-IR laser light is challenging since
sapphire is transparent to these wavelengths. In this study,
we investigate the formation of femtosecond laser-induced
periodic surface structures (LIPSSs) on sapphire coated
with nanolayered gold film. We found a reduced threshold
by about 25 % in generating uniform LIPSSs on sapphire
due to the nanolayered gold film. Different thickness of
nanolayered gold films are studied, and it is shown that the
change in thickness does not significantly affect the
threshold reduction. It is believed that the diffusion of hot
electrons in the gold films increases interfacial carrier
density and electronphonon coupling that results in a
reduced threshold and more uniform periodic surface
structure generation.
1 Introduction
The formation of femtosecond laser-induced periodic sur-
face structures (LIPSSs) has gained significant attention in
recent years, mainly due to wide range of potential appli-
cations in superhydrophobic [1, 2], solar cells [35], heat
dissipation devices [6, 7], and surface-enhanced Raman
scattering [8]. The period, orientation, morphology, and
& Chunlei Guo
guo@optics.rochester.edu
1 optics, and substrate for semiconductor devices [28]. For
The Institute of Optics, University of Rochester, Rochester,
NY 14627, USA
2 fluence threshold.
The State Key Laboratory of High Performance and Complex
Manufacturing, Central South University, Changsha 410083,
China
composition of LIPSSs depend on both the laser and
material properties, such as pulse number [9], laser fluence
[10, 11], polarization [1214], laser wavelength [15, 16],
repetition rate [17], and focusing position [18]. Further-
more, the formation mechanisms of LIPSSs, including
excitation of surface plasmon polaritons (SPPs) [1921],
effect of grating-assisted surface plasmon laser coupling
[22], self-organization [23], and second harmonic genera-
tion [24], have been proposed.
Despite the extensive amount of studies on LIPSSs, the
mechanism and various features of LIPSSs formation still
require further studies. Among various features, only lim-
ited studies have been conducted regarding the threshold of
LIPSSs generation. Deng et al. [25] studied the temperature
dependence of laser-induced nanostructures for multiple
linearly polarized femtosecond laser pulse irradiation of
silicon in air. Jiang et al. [26] investigated the phenomenon
of strong dependence of the anisotropic formation of
periodic ripples on crystal orientation; they concluded that
it is much easier to form ripple structures when the
polarization direction is aligned with the lattice axis. Wang
et al. studied the pulse energy threshold of surface nano/
micromorphology modifications by irradiating different
materials surfaces in air and in water. They found that the
laser pulse energy thresholds required for the permanent
modification in water are lower than those in air [27].
Sapphire is a useful material for its extreme hardness, high
transparent, and stable dielectric constant. Such properties
make sapphire an important candidate in many applica-
tions, such as space and military optical systems, sensor
some of those applications, it is important to reduce the
In this study, we experimentally demonstrate the
nanoscale gold film-assisted femtosecond laser fabrication
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834 Page 2 of 5
technology. By depositing a layer of gold film of *12 nm,
we can achieve a significant threshold reduction and more
uniform periodic surface structures on sapphire. In addi-
tion, the thickness of nanolayered Au film has little depend
on threshold of LIPSSs generation, which is an interesting
phenomenon first reported here. We believe that diffusion
of hot electrons on the Au film increases interfacial carrier
density and electronphonon coupling that results in a
reduced threshold and more uniform periodic surface
structure generation.
2 Experimental
Figure 1 shows the schematic diagrams of the fabrication
procedures, which comprise four steps. Polished sapphire
samples were deposited by a layer of gold film with a
thickness of *12 nm by a thin film deposition system
(Kurt J. Lesker, Inc), which is accurately controlling the
thickness of depositing lay. Then, an amplified Ti:sapphire
laser system is used that generates 66-fs pulses of about
1.1 mJ/pulse at a 1-kHz repetition rate with a central
wavelength of 800 nm. The beam was focused onto the
sample [29]. We performed multipulse ablation experi-
ments, where the sample was irradiated with bursts of 20
laser pulses. To select 20 pulses, an electromechanical
Fig. 1 Schematic diagrams of
the fabrication procedures
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K. Yin et al.
shutter was used. A half-wave plate and a linear polarizer
were used to control the laser fluence incident on the
sample surface. After laser ablation, the samples were
cleaned by the lens tissue and rinsed for 10 min with
acetone, alcohol, and deionized water in an ultrasonic bath
cleaner in order to remove the depositing gold films and
scraps from the ablation process, respectively. Finally, the
chemical composition in the ablation regions was exam-
ined by an energy-dispersive X-ray spectroscopy, which
showed that there is no Au or other elements deposited on
the surface after ablation and cleaning. Also, the irradiated
regions were characterized by a scanning electron micro-
scope (SEM) and an atomic force microscope (AFM).
3 Results and discussion
In this experiment, the laser beam was focused on one spot
with 20 pulses. The fluence was varied from low to high.
The left panel of Fig. 2 shows the optical microscope
images of the structure on sapphire and Au-coated sapphire
(Au-sapphire) induced by different laser fluence. The flu-
ence of (a1) and (b1) on the far right side is 1.58 J/cm2,
from right to left, the pulse fluence was increased by
0.13 J/cm2, and the total irradiation condition of the two
cases are the same. It is shown that the structures irradiated
Femtosecond laser-induced periodic surface structural formation on sapphire with nanolayered Page 3 of 5 834

Fig. 2 Optical and SEM images of the structures on sapphire and Au-sapphire induced by different laser fluences. Note the different scaling of
the images

on sapphire are less visible than on Au-sapphire, more

detailed of those are shown in the right panel of the Fig. 2.
The right panel of Fig. 2 shows the SEM images evolution
of generating LIPSSs after irradiation on sapphire and Au-
sapphire. In Fig. 2a1a3 are irradiated on sapphire, while
b1b3 are irradiated on Au-sapphire. In Fig. 2a1, b1, as the
laser fluence is 1.58 J/cm2, it is found that there is nothing
on sapphire which means that the fluence is lower than the
threshold of LIPSSs generation. While, original LIPSSs are
fabricated on the Au-sapphire. As the fluence increased,
there are some nanocracks emerging on the sapphire at the
fluence 1.97 J/cm2. At the meantime, the LIPSSs are well
formed on the Au-sapphire, according to Fig. 2a2, b2. As
the fluence up to 2.11 J/cm2, the LIPSSs is formed on the
sapphire, but the morphologies of LIPSSs is not clearly
visible. There are some broken LIPSSs and nanocracks in
it. In contrast, it is found that well-defined LIPSSs are
fabricated on the Au-sapphire.
In order to gain deeper insight into the information
about the spatial characteristics on sapphire and Au-sap-
phire after laser irradiation, the high-magnification SEM Fig. 3 SEM images and AFM profiles of the surface morphology
images and AFM profiles are observed at 2.24 J/cm2, fabricated on sapphire and Au-sapphire at 2.24 J/cm2, respectively
which present a stable surface structure. As shown in LIPSSs. Those defects distribute nearly half of the whole
Fig. 3a, some of the LIPSSs are interrupted, which shows LIPSSs covered area. In Fig. 3b, for comparison, well-
some holes or bifurcations that break the continuity of defined and clear LIPSSs are found on Au-sapphire, and

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there is no branch or defect in it. Figure 3c shows the AFM
profiles of LIPSSs on sapphire and Au-sapphire. We can
clear see that the LIPSSs on sapphire fluctuate widely,
which is mainly due to the existence of branch and broken
structures. At the same time, the LIPSSs on Au-sapphire
have a much more uniform structure with clear peaks and
valleys.
Figure 4 shows the fluence dependence of the LIPSSs
period for both sapphire and Au-sapphire, respectively. The
fluence of generating well-defined LIPSSs on sapphire is
between 2.11 and 2.37 J/cm2 with a period of 210355 nm,
which means that there is no LIPSSs emerging under the
fluence of 2.11 J/cm2, while the LIPSSs start to break
above the fluence of 2.37 J/cm2. For comparison, it has a
much lower fluence for fabricating LIPSSs on the Au-
sapphire. At a fluence range of 1.582.37 J/cm2, the well-
defined LIPSSs can be generated, and the fluence of the
LIPSSs appearance is decreased by 25 %. This means that
we can fabricate LIPSSs on samples of a lower and a wider
range fluence, which can be contributed to improve the
efficiency and stability for fabricating.
We also vary the thickness and more detailed laser
fluence to further investigate in Au film-assisted fem-
tosecond laser fabricating LIPSSs. The effects of Au films
thickness on threshold of the LIPSSs generation are shown
in Fig. 5, where the error bar indicates the obtainable
threshold of LIPSSs generation range in our experiments
for a certain thickness of Au film. It is found that the
threshold is reduced significantly with a very thin gold
film; the thickness is around 4 nm. As the thickness
increasing, the threshold maintains nearly a constant. This
means that the threshold of LIPSSs generation does not
significant depend on the thickness of coating film, and we
can achieve a threshold-reduced LIPSSs by depositing
several nanometers layered gold film.
Fig. 4 LIPSSs periods on sapphire and Au-sapphire in dependence
on the laser fluence
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K. Yin et al.
Fig. 5 Threshold of the LIPSSs generation at different nanolayered
thickness
The possible mechanisms of nanolayered gold films
assisted femtosecond laser fabrication of threshold-reduced
uniform periodic surface structure is discussed as followed.
The formation of LIPSSs is widely explained by the
interference between the incident laser and surface plas-
mons [1921]. During the process of femtosecond laser
fabricating, the Au film is heated up, electrons are highly
energetic and a significant diffusion occurs. Hot electrons
diffused forwards to the interface between Au film and
sapphire, this will increases the interfacial carrier density
and enhances the interfacial electronphonon coupling, it
has been demonstrated by Feng et al. [30], Li et al. [31].
The higher interfacial carrier density and enhanced inter-
facial electronphonon coupling in the Au-sapphire can
lead to the surface plasmons enhanced. Meanwhile, more
energy will uniformly deposited on the sapphire surface
due to the high thermal conductivity of gold film, higher
temperature of the sapphire surface will play an important
role for the formation and evolution of the LIPSSs; it will
also enhance the surface plasmons. Aforementioned effects
result in the decrease in threshold during fabricating uni-
form periodic surface structure on the sapphire.
4 Conclusions
In conclusion, the nanolayered gold film-assisted fem-
tosecond laser fabricate surface pattern is demonstrated.
The experimental results show a significant reduction of
fabricating threshold and more uniform periodic surface
structure on the sapphire, which opens up a new path for
high-efficiency surface processing. The threshold of
LIPSSs generation does not significantly depend on the
thickness of the deposited nanolayered film, which means
that we achieve a threshold-reduced LIPSSs by depositing
Femtosecond laser-induced periodic surface structural formation on sapphire with nanolayered
several nanometers layered gold film. The physical
responsible for the threshold-reduced LIPSSs formation is
attributed to the diffusion of hot electrons on the Au film
increases interfacial carrier density and electronphonon
coupling, which lead to the surface plasmons enhanced,
results in fabricating threshold-reduced uniform periodic
surface structure on the sapphire.
Acknowledgments This research is supported by the U.S. Army
Research Office, NYSERDA, Bill & Melinda Gates Foundation,
China Scholarship Council, the National Basic Research Program of
China (973 Program; Grant No. 2011CB013000), and National Nat-
ural Science Foundation of China (NSFC; Grant Nos. 91123035,
91323301 and 51335011).
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