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Lifetime modulation of graphene oxide film by laser direct writing for the fabrication of micropatterns

Qiao Zhi-Xing Qin Cheng-Bing He Wen-Jun Gong Ya-Ni Xiao Lian-Tuan Zhang Guo-Feng Chen Rui-Yun Gao Yan Jia Suo-Tang

Lifetime modulation of graphene oxide film by laser direct writing for the fabrication of micropatterns

Qiao Zhi-Xing, Qin Cheng-Bing, He Wen-Jun, Gong Ya-Ni, Xiao Lian-Tuan, Zhang Guo-Feng, Chen Rui-Yun, Gao Yan, Jia Suo-Tang,
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  • The strong, broad and tunable fluorescence emission of graphene oxide (GO) has shown the exciting optical applications in many areas, such as fluorescence imaging in living cell, high sensitive detection of heavy metal ions, and the fabrication of optoelectronic devices. However, the intrinsic heterogeneous fluorescence intensity resulting from the variability in the power density of excitation laser and the non-uniform thickness of GO film, hinders its further applications in the micropatterning, information storage and display technology, which requires homogeneous fluorescence emission. In contrast to the fluorescence intensity, the fluorescence lifetime of GO is determined by the intrinsic nature of chromophores, rather than the film thickness or excitation power density. Here we report that the fluorescence lifetime is homogeneous for GO film, which eliminates the anisotropic optical properties of GO film. By reducing the GO film through the irradiation from a 405 nm continuous-wave laser at a certain power density on a home-built scanning confocal microscope, we find that the lifetime can be precisely modulated by controlling the duration of laser irradiation. It is determined that the lifetime gradually decreases with the increase of duration. As reported in the previous researches, the GO fluorescence originates from the graphene-like confined sp2 clusters and sp3 domains consisting of oxygen-containing functional groups, where the lifetime of sp3 domain is about 1.4 ns, and that of sp2 domain is 0.14 ns. During the photoreduction, the long-lived sp3 domains will decrease or convert into short-lived sp2 domains, resulting in the decrease of lifetime. Hence, by controlling the reduction degree or the ratio of the two domains, the lifetime of GO film can be determined. More importantly, the lifetime distributions of the reduction areas are very narrow, leading to a relatively homogenous background. The precise manipulation of lifetime can be used to fabricate micropatterns with high contrast. Combining with laser direct writing with features of maskless, facile processing ability and high spatial resolution, many versatile micropatterns, such as quick response code, barcode, graphic, alphabet, and numbers can be readily created based on the modulation of fluorescence lifetime. By using three optimized durations of laser irradiation, three distributions with narrow widths are obtained. Based on this processing, the micropatterns with three colors are determined, which indicates that the multimode optical recording can be created on the GO film based on the modulation of fluorescence lifetime. Furthermore, the multilayer micropatterns are also created. The robust and versatile micropatterns with film-thickness and excitation-power-independent features show their promising applications in electronics, photonics, display technology and information storage.
      Corresponding author: Qin Cheng-Bing, chbqin@sxu.edu.cn;xlt@sxu.edu.cn ; Jia Suo-Tang, chbqin@sxu.edu.cn;xlt@sxu.edu.cn
    • Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. U1510133, 61527824, 11374196, 61675119, 11434007, 1504216, 61605104), the Program for Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China (Grant No. IRT13076), and the 1331KSC.
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    [3]

    Stoller M D, Park S, Zhu Y, An J, Ruoff R S 2008 Nano Lett. 8 3498

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    Eda G, Fanchini G, Chhowalla M 2008 Nat. Nanotech. 3 270

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    Eda G, Chhowalla M 2010 Adv. Mater. 22 2392

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    Furio A, Landi G, Altavilla C, Sofia D, Iannace S, Sorrentino A, Neitzert H C 2017 Nanotechnology 28 054003

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    Marquez C, Rodriguez N, Ruiz R, Gamiz F 2016 RSC Adv. 6 46231

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    Sun X, Liu Z, Welsher K, Robinson J T, Goodwin A, Zaric S, Dai H 2008 Nano Res. 1 203

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    Huang J, Gao X, Jia J, Kim J K, Li Z 2014 Anal. Chem. 86 3209

    [22]

    Wang X, Tian H, Mohammad M A, Li C, Wu C, Yang Y, Ren T L 2015 Nat. Commun. 6 7767

    [23]

    Sokolov D A, Morozov Y V, McDonald M P, Vietmeyer F, Hodak J H, Kuno M 2014 Nano Lett. 14 3172

    [24]

    Tongay S, Suh J, Ataca C, Fan W, Luce A, Kang J S, Liu J, Ko C, Raghunathanan R, Zhou J, Ogletree F, Li J, Grossman J C, Wu J 2013 Sci. Rep. 3 2657

    [25]

    He W, Qin C, Qiao Z, Zhang G, Xiao L, Jia S 2016 Carbon 109 264

    [26]

    Li B, Zhang G F, Jing M Y, Chen R Y, Qin C B, Gao Y, Xiao L T, Jia S T 2016 Acta Phys. Sin. 65 218201 (in Chinese) [李斌, 张国峰, 景明勇, 陈瑞云, 秦成兵, 高岩, 肖连团, 贾锁堂 2016 物理学报 65 218201]

    [27]

    Gao Y, Qiao Z X, Qin C B, Chen R Y, Zhang G F, Xiao L T, Jia S T 2015 Sci. Sin.-Phys. Mech. Astron. 45 024201 (in Chinese) [高岩, 乔志星, 秦成兵, 陈瑞云, 张国峰, 肖连团, 贾锁堂 2015 中国科学:物理学力学天文学 45 024201]

    [28]

    Liu Z B, Zhao X, Zhang X L, Yan X Q, Wu Y P, Chen Y S, Tian J G 2011 J. Chem. Phys. Lett. 2 1972

    [29]

    Zhang X F, Shao X N, Liu S P 2012 J. Phys. Chem. A 116 7308

  • [1]

    Lee C, Wei X, Kysar J W, Hone J 2008 Science 321 385

    [2]

    Bolotin K I, Sikes K J, Jiang Z, Klima M, Fudenberg G, Hone J, Kim P, Stormer H L 2008 Solid State Commun. 146 351

    [3]

    Stoller M D, Park S, Zhu Y, An J, Ruoff R S 2008 Nano Lett. 8 3498

    [4]

    Bonaccorso F, Sun Z, Hasan T, Ferrari A C 2010 Nat. Photon. 4 611

    [5]

    Bao Q, Zhang H, Wang B, Ni Z, Lim C H Y X, Wang Y, Tang D Y, Loh K P 2011 Nat. Photon. 5 411

    [6]

    Novoselov K S, Fal'ko V I, Colombo L, Gellert P R, Schwab M G, Kim K 2012 Nature 490 192

    [7]

    Wang W R, Zhou Y X, Li T, Wang Y L, Xie X M 2012 Acta Phys. Sin. 61 038702 (in Chinese) [王文荣, 周玉修, 李铁, 王跃林, 谢晓明 2012 物理学报 61 038702]

    [8]

    Senyuk B, Behabtu N, Martinez A, Lee T, Tsentalovich D E, Ceriotti G, Tour J M, Pasquali M, Smalyukh I I 2015 Nat. Commun. 6 7157

    [9]

    Zhang Y, Guo L, Wei S, He Y, Xia H, Chen Q, Sun H B, Xiao F S 2010 Nano Today 5 15

    [10]

    Kymakis E, Petridis C, Anthopoulos T D, Stratakis E 2014 IEEE J. Sel. Top. Quantum Electron. 20 10

    [11]

    Eda G, Fanchini G, Chhowalla M 2008 Nat. Nanotech. 3 270

    [12]

    Eda G, Chhowalla M 2010 Adv. Mater. 22 2392

    [13]

    Furio A, Landi G, Altavilla C, Sofia D, Iannace S, Sorrentino A, Neitzert H C 2017 Nanotechnology 28 054003

    [14]

    Marquez C, Rodriguez N, Ruiz R, Gamiz F 2016 RSC Adv. 6 46231

    [15]

    Fatt Teoh H, Tao Y, Soon Tok E, Wei Ho G, Haur Sow C 2012 J. Appl. Phys. 112 064309

    [16]

    Wei Z, Wang D, Kim S, Kim S Y, Hu Y, Yakes M K, Laracuente A R, Dai Z, Marder S R, Berger C, King W P, de Heer W A, Sheehan P E, Riedo E 2010 Science 328 1373

    [17]

    He Y, Zhu L, Liu Y, Ma J N, Han D D, Jiang H B, Han B, Ding H, Zhang Y L 2016 IEEE Photon. Technol. Lett. 28 1996

    [18]

    Chien C T, Li S S, Lai W J, Yeh Y C, Chen H A, Chen I S, Chen L C, Chen K H, Nemoto T, Isoda S, Chen M, Fujita T, Eda G, Yamaguchi H, Chhowalla M, Chen C W 2012 Angew. Chem. 51 6662

    [19]

    Loh K P, Bao Q, Eda G, Chhowalla M 2010 Nat. Chem. 2 1015

    [20]

    Sun X, Liu Z, Welsher K, Robinson J T, Goodwin A, Zaric S, Dai H 2008 Nano Res. 1 203

    [21]

    Huang J, Gao X, Jia J, Kim J K, Li Z 2014 Anal. Chem. 86 3209

    [22]

    Wang X, Tian H, Mohammad M A, Li C, Wu C, Yang Y, Ren T L 2015 Nat. Commun. 6 7767

    [23]

    Sokolov D A, Morozov Y V, McDonald M P, Vietmeyer F, Hodak J H, Kuno M 2014 Nano Lett. 14 3172

    [24]

    Tongay S, Suh J, Ataca C, Fan W, Luce A, Kang J S, Liu J, Ko C, Raghunathanan R, Zhou J, Ogletree F, Li J, Grossman J C, Wu J 2013 Sci. Rep. 3 2657

    [25]

    He W, Qin C, Qiao Z, Zhang G, Xiao L, Jia S 2016 Carbon 109 264

    [26]

    Li B, Zhang G F, Jing M Y, Chen R Y, Qin C B, Gao Y, Xiao L T, Jia S T 2016 Acta Phys. Sin. 65 218201 (in Chinese) [李斌, 张国峰, 景明勇, 陈瑞云, 秦成兵, 高岩, 肖连团, 贾锁堂 2016 物理学报 65 218201]

    [27]

    Gao Y, Qiao Z X, Qin C B, Chen R Y, Zhang G F, Xiao L T, Jia S T 2015 Sci. Sin.-Phys. Mech. Astron. 45 024201 (in Chinese) [高岩, 乔志星, 秦成兵, 陈瑞云, 张国峰, 肖连团, 贾锁堂 2015 中国科学:物理学力学天文学 45 024201]

    [28]

    Liu Z B, Zhao X, Zhang X L, Yan X Q, Wu Y P, Chen Y S, Tian J G 2011 J. Chem. Phys. Lett. 2 1972

    [29]

    Zhang X F, Shao X N, Liu S P 2012 J. Phys. Chem. A 116 7308

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  • Received Date:  29 October 2017
  • Accepted Date:  03 January 2018
  • Published Online:  20 March 2018

Lifetime modulation of graphene oxide film by laser direct writing for the fabrication of micropatterns

    Corresponding author: Qin Cheng-Bing, chbqin@sxu.edu.cn;xlt@sxu.edu.cn
    Corresponding author: Jia Suo-Tang, chbqin@sxu.edu.cn;xlt@sxu.edu.cn
  • 1. State Key Laboratory of Quantum Optics and Quantum Optics Devices, Institute of Laser Spectroscopy, Shanxi University, Taiyuan 030006, China;
  • 2. Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan 030006, China
Fund Project:  Project supported by the National Natural Science Foundation of China (Grant Nos. U1510133, 61527824, 11374196, 61675119, 11434007, 1504216, 61605104), the Program for Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China (Grant No. IRT13076), and the 1331KSC.

Abstract: The strong, broad and tunable fluorescence emission of graphene oxide (GO) has shown the exciting optical applications in many areas, such as fluorescence imaging in living cell, high sensitive detection of heavy metal ions, and the fabrication of optoelectronic devices. However, the intrinsic heterogeneous fluorescence intensity resulting from the variability in the power density of excitation laser and the non-uniform thickness of GO film, hinders its further applications in the micropatterning, information storage and display technology, which requires homogeneous fluorescence emission. In contrast to the fluorescence intensity, the fluorescence lifetime of GO is determined by the intrinsic nature of chromophores, rather than the film thickness or excitation power density. Here we report that the fluorescence lifetime is homogeneous for GO film, which eliminates the anisotropic optical properties of GO film. By reducing the GO film through the irradiation from a 405 nm continuous-wave laser at a certain power density on a home-built scanning confocal microscope, we find that the lifetime can be precisely modulated by controlling the duration of laser irradiation. It is determined that the lifetime gradually decreases with the increase of duration. As reported in the previous researches, the GO fluorescence originates from the graphene-like confined sp2 clusters and sp3 domains consisting of oxygen-containing functional groups, where the lifetime of sp3 domain is about 1.4 ns, and that of sp2 domain is 0.14 ns. During the photoreduction, the long-lived sp3 domains will decrease or convert into short-lived sp2 domains, resulting in the decrease of lifetime. Hence, by controlling the reduction degree or the ratio of the two domains, the lifetime of GO film can be determined. More importantly, the lifetime distributions of the reduction areas are very narrow, leading to a relatively homogenous background. The precise manipulation of lifetime can be used to fabricate micropatterns with high contrast. Combining with laser direct writing with features of maskless, facile processing ability and high spatial resolution, many versatile micropatterns, such as quick response code, barcode, graphic, alphabet, and numbers can be readily created based on the modulation of fluorescence lifetime. By using three optimized durations of laser irradiation, three distributions with narrow widths are obtained. Based on this processing, the micropatterns with three colors are determined, which indicates that the multimode optical recording can be created on the GO film based on the modulation of fluorescence lifetime. Furthermore, the multilayer micropatterns are also created. The robust and versatile micropatterns with film-thickness and excitation-power-independent features show their promising applications in electronics, photonics, display technology and information storage.

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