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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,

Hai Zhu,

2,3

Rizhao Ma,

and Qing-Hua Xu

2,3,

State Key Laboratory of Luminescent Materials and Devices (SKLLMD), South China University of Technology,

Guangzhou 510640, China

Department of Chemistry, National University of Singapore, 117543, Singapore

NUSNNI-NanoCore, National University of Singapore, 117576, Singapore

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

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

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