Ultrafast dynamics of high-contrast nano-grating formation on gold film
induced by temporally shaped femtosecond laser
Guangqing Du, Feng Chen
⇑
, Qing Yang, Yan Ou, Yanmin Wu, Yu Lu, Hao Bian, Xun Hou
State Key Laboratory for Manufacturing Systems Engineering & Key Laboratory of Photonics Technology for Information, School of Electronics & Information Engineering, Xi’an
Jiaotong University, 710049, China
article info
Article history:
Received 6 December 2013
In final form 18 February 2014
Available online 25 February 2014
abstract
We theoretically investigated the ultrafast dynamics of high-contrast nano-grating formation on gold
film surface with respect to non-equilibrium thermal excitation processes. It is proposed that the high-
contrast nano-grating can be desirably achieved by optimizing the non-equilibrium thermal dynamics
processes. The grating contrast can be largely promoted by 64% with adjusting thermal dynamics via tai-
loring temporally shaped femtosecond laser. The results are attributed to the competitive energy transfer
routes between electrons thermal diffusion and electron–phonon relaxation processes during grating for-
mation, which can be w ell manipulated by temporally shaped femtosecond laser. The study provides for
strategy for production of high-quality periodic surface structures with sharp grating profiles.
Ó 2014 Elsevier B.V. All rights reserved.
1. Introduction
Laser induced periodic nanostructures, especially the nano-
gratings have been widely studied because of their potential inter-
ests for both scientific and practical aspects [1–4]. The high-quality
nano-grating would be extremely beneficial for promoting perfor-
mance of periodic structured devices, such as surface plasmons
sensors, polarizing beam splitter, solar cells and mechanical fric-
tion devices, etc. Generally, the nano-grating formation is widely
accepted as the interference between incident laser with scattering
surface wave, which may originate from surface roughness, surface
electron excitation, surface instability [5–8]. Unfortunately, laser
patterned grating usually presents poor appearance with low-
contrast and quasi-periodicity due to thermal recast effect during
grating formation process. Recently, the temporally shaped femto-
second laser, namely, multi-pulse sequence with variable temporal
separation have found potential advantages in patterning of micro-
structures and periodic nano-grating, such as high ablation effi-
ciency and less thermal recast effect [9–13]. It becomes possible
to manipulate grating contrast via tailoring the temporally shaped
femtosecond laser. When temporally shaped femtosecond laser
interactions with metallic materials, the non-equilibrium thermal
relaxation dynamics, which are closely related to pulse-to-pulse
relevance can be mainly responsible for regulating ablation fea-
tures [14,15]. It is demonstrated that the interplay between the
electron thermal diffusion and electron–phonon coupling
processes can definitely influence the grating contrast [16–18].
However, it is currently challenging to control the processes of
interplay between electron thermal diffusion and electron–phonon
coupling for a given target for optimizing the grating features for a
wide range of applications.
In this Letter, we present the dynamics of grating contrast tun-
ing on gold via manipulating the temporally shaped femtosecond
laser. For femtosecond laser ablation, the target can be removed
during the non-equilibrium electron–phonon relaxation period in
the ablation regime. As a result, the condition of simulations is lim-
ited to the non-equilibrium processes within several picoseconds
in the early stage of grating formation. The thermal relaxation
mechanism in the early stage of grating formation is proposed
for exploring grating contrast modulation dynamics. It is revealing
that the interplay of competitive energy transfer routes between
the electrons thermal diffusion and the electron–phonon relaxa-
tion processes can be optimized via temporally shaping the femto-
second laser pulses for generation of high contrast grating. In this
Letter, we focus on the ultrafast thermal relaxation dynamics in
the early stage of grating formation for analysis of the grating-con-
trast features. The interference between surface plasmon polari-
tions and the wide-spectrum femtosecond pulse are taken as the
nano-grating formation mechanism. The generation of surface
wave like the surface plasmon polaritons can physically originate
from surface roughness of gold film. The interference patterns for
regulating grating profiles are equalized as the periodically modu-
lated laser source. As the ultrashort laser pulses irradiation of gold
film, the target can be excited out of equilibrium dramatically [19].
Namely, the electrons and phonons can be treated as respective
http://dx.doi.org/10.1016/j.cplett.2014.02.035
0009-2614/Ó 2014 Elsevier B.V. All rights reserved.
⇑
Corresponding author.
E-mail address: chenfeng@mail.xjtu.edu.cn (F. Chen).
Chemical Physics Letters 597 (2014) 153–157
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Chemical Physics Letters
journal homepage: www.elsevier.com/locate/cplett