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We report a simple solution-processed method for the fabrication of low-cost, flexible optical limiting materials based on graphene oxide (GO) impregnated polyvinyl alcohol (PVA) sheets. Such GO–PVA composite sheets display highly efficient broadband optical limiting activities for femtosecond laser pulses at 400, 800, and 1400 nm with very low limiting thresholds. Femtosecond pump–probe measurement results revealed that nonlinear absorption played an important role for the observed optical limi
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Flexible, robust and highly efficient broadband nonlinear
optical materials based on graphene oxide
impregnated polymer sheets
Xiao-Fang Jiang,
1,2,3,4
Lakshminarayana Polavarapu,
2
Hai Zhu,
2,3
Rizhao Ma,
2
and Qing-Hua Xu
2,3,
*
1
State Key Laboratory of Luminescent Materials and Devices (SKLLMD), South China University of Technology,
Guangzhou 510640, China
2
Department of Chemistry, National University of Singapore, 117543, Singapore
3
NUSNNI-NanoCore, National University of Singapore, 117576, Singapore
4
e-mail: msxfjiang@scut.edu.cn
*Corresponding author: chmxqh@nus.edu.sg
Received January 8, 2015; revised March 8, 2015; accepted March 11, 2015;
posted March 13, 2015 (Doc. ID 232097); published April 22, 2015
We report a simple solution-processed method for the fabrication of low-cost, flexible optical limiting materials
based on graphene oxide (GO) impregnated polyvinyl alcohol (PVA) sheets. Such GO–PVA composite sheets dis-
play highly efficient broadband optical limiting activities for femtosecond laser pulses at 400, 800, and 1400 nm
with very low limiting thresholds. Femtosecond pump–probe measurement results revealed that nonlinear ab-
sorption played an important role for the observed optical limiting activities. High flexibility and efficient optical
limiting activities of these materials allow these composite sheets to be attached to nonplanar optical sensors in
order to protect them from light-induced damage. © 2015 Chinese Laser Press
OCIS codes: (310.6860) Thin films, optical properties; (160.4330) Nonlinear optical materials; (190.7110)
Ultrafast nonlinear optics; (300.6500) Spectroscopy, time-resolved.
http://dx.doi.org/10.1364/PRJ.3.000A87
1. INTRODUCTION
Nonlinear optical materials (optical limiters and saturable
absorbers) play a significant role in the field of optics owing
to their unprecedented ability to modulate lasers pulses. Over
the past decades, significant research efforts have been de-
voted to the development of broadband optical limiting mate-
rials and related devices. Good optical limiting materials
generally exhibit high transmittance at low input intensities
but can attenuate intense laser pulses. Such materials are im-
portant for protecting human eyes and sensitive detectors
from damage by high-intensity light beams. Effective optical
limiting behaviors have been observed in various nanomate-
rials such as carbon nanotubes (CNTs) [
1,2], fullerenes [3],
quantum dots [
4], and noble metal nanoparticles [5,6]. It was
recently found that suspensions of two-dimensional material
such as graphene [
7,8], hydrogen exfoliated graphene [9],
graphene oxide (GO) [
10,11], and their composites with other
materials [
12–17] exhibited broadband optical limiting proper-
ties. In 2011, Lim et al. [
15] reported a giant broadband non-
linear optical response for nanosecond laser pulses on
functionalized GO nanostructure dispersion. Very recently,
Liaros et al. also demonstrated broadband near infrared opti-
cal power limiting behaviors of few layered GO dispersed in
different organic solvents under nanosecond laser pulses [
18].
Nonlinear scattering and nonlinear absorption are two pos-
sible mechanisms responsible for optical limiting behaviors
[
3,6,10,19]. Most of the reported optical limiting studies were
performed on nanomaterials dispersed in different solvents, in
which solvent microbubbles-induced nonlinear scattering at
higher intensities played an important role [
1,3,5]. Thin film
materials are more convenient to use but generally display
strong saturable absorption [
8,20]. For example, although
suspensions of metal nanoparticles [
5,6], graphene, and
graphene–polymer composites [
20–23] showed strong broad-
band optical limiting activities, their thin films generally exhib-
ited strong saturable absorption behavior [
8,20,24–27]. One
major challenge is fabrication of stable and flexible thin film-
based optical limiting devices for practical applications.
Flexible and low-cost materials that exhibit high broadband
nonlinear absorption are ideal choices. Previously, we have
demonstrated that spin-coated GO thin films on glass or plas-
tic substrates exhibited tunable broadband optical limiting
response for femtosecond laser pulses, and the nonlinear op-
tical response of GO could be tuned from nonlinear absorp-
tion to saturable absorption by partial reduction of GO [
28].
However, these spin-coated GO films have a few drawbacks.
First, GO tends to be reduced into reduced GO easily under
normal light in the long run. Secondly, a significant amount of
GO solution was wasted in the spin-coating process. Thirdly,
the interaction of GO with glass or plastic surface is not very
strong, which may result in the detachment of GO from the
surface. Herein, we demonstrated a simple method for fabri-
cation of flexible nonlinear optical films by impregnating GO
into polyvinyl alcohol (PVA) polymer sheets using a solution-
processing method. The prepared GO–PVA composite sheets
have been characterized by ultraviolet–visible–near-infrared
(UV–Vis–NIR) transmittance, Raman spectroscopy, and
atomic force microscopy (AFM). Broadband optical limiting
properties of as-prepared flexible GO–PVA sheets made of
different GO/PVA weight ratios have been investigated by
Jiang et al. Vol. 3, No. 3 / June 2015 / Photon. Res. A87
2327-9125/15/030A87-05 © 2015 Chinese Laser Press
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