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超短脉冲激光烧蚀石墨产生的喷射物的时间分辨发射光谱研究

冯培培 吴寒 张楠

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超短脉冲激光烧蚀石墨产生的喷射物的时间分辨发射光谱研究

冯培培, 吴寒, 张楠

Study of the time-resolved emission spectra of the ejected plume generated by ultrashort laser ablation of graphite

Feng Pei-Pei, Wu Han, Zhang Nan
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  • 本文使用不同激光能流(18 J/cm2–115 J/cm2)和脉冲宽度(50 fs–4 ps)的超短脉冲激光在真空中(4×10-4 Pa)烧蚀高定向热解石墨. 通过测量烧蚀喷射物的时间分辨发射光谱研究喷射物的超快时间演化. 在喷射物发射光谱中, 观察到了C2基团的天鹅带光谱系统, 416 nm附近C15基团的由电子能级1Σu+ 和1Σg+之间的振动跃迁产生的光谱峰以及连续谱. 50 fs, 115 J/cm2的脉冲激光烧蚀产生的喷射物的连续谱的强度衰减分为快速下降和慢速下降两个阶段(以20 ns时间延迟为分界). 这表明连续谱是由两种不同的组分贡献的. 快速下降阶段, 连续谱主要由碳等离子体通过韧致辐射产生; 慢速下降阶段, 连续谱主要由烧蚀后期产生的大颗粒碳簇的热辐射贡献. 实验结果还揭示了激光能流的提高, 会明显增加喷射物中碳等离子体和激发态C2的含量, 但对质量稍大的C15的影响较小; 此外, 50 fs脉冲激光烧蚀产生的连续谱的存在时间会随着激光能流的减小而增大, 这说明低能流更有利于在烧蚀后期产生碳簇. 脉宽主要影响喷射物连续谱的时间演化. 4 ps脉冲激光烧蚀产生的连续谱的整个时间演化过程明显慢于50 fs脉冲产生的连续谱.
    In this paper ultrashort laser pulses with different fluences (18 J/cm2-115 J/cm2) and pulse widths (50 fs-4 ps) are employed to ablate highly oriented pyrolytic graphite in vacuum (4×10-4 Pa). By recording the time-resolved emission spectra of the ablated plume, the ultrafast time evolution of the ablation process is investigated. The Swan bands of C2 radicals, the spectral band near 416 nm which may be assigned to the electronic transition from 1Σu+ to X1Σg+ of C15 clusters, and the emission continuum ranging from 370-700 nm are observed. From the recorded time-resolved emission spectra of the ablated plume, it is seen that at larger time delays only the emission continuum is observed. The decay process of the emission continuum of the plume generated by 50 fs, 115 J/cm2 laser pulses can be divided into a fast decreasing stage (before 20 ns time delay) and a slow decreasing stage (after 20 ns time delay), indicating that the emission continuum may come from two different compositions. During the fast decreasing process, the bremsstrahlung of the ablation-generated carbon plasma contributes to the major part of the continuum; while during the slow decreasing process, the thermal radiation of carbon clusters generated at a later stage of ablation mainly contributes to the continuum. In addition, the existence time of the continuum generated by 50 fs laser pulses increases with the decrease of laser fluence, indicating that laser pulses with lower fluences can generate more carbon clusters at later stages of ablation. It is also found that for the 50 fs pulses, when the laser fluence increases at the early stage of ablation, the quantities of carbon plasma and excited C2 radicals in the plume increase significantly, but the quantity of excited C15 radicals with larger mass only increases slightly. Therefore the laser fluence has a great impact on the concentrations of different compositions in the ejected plume, implying that different material removal mechanisms exist for ablation induced by laser pulses with different laser fluences. Finally, pulse width plays an important role in the time evolution manner of the emission continuum. As the laser pulse width increases, the two-stage decay process of the emission continuum gradually changes into one-stage process, indicating that the existence time intervals of carbon plasma and carbon clusters overlap each other for longer laser pulse width. And the whole evolution process of the emission continuum induced by 4 ps laser pulses is much slower than that induced by 50 fs laser pulses. Longer laser pulse width also causes the decrease of the spectral intensity of C2 radicals, and thus higher laser intensity favors the generation of excited C2 radicals.
      通信作者: 张楠, zhangn@nankai.edu.cn
    • 基金项目: 国家自然科学基金(批准号: 61137001, 11274185, 11004111)和中南大学高性能复杂制造国家重点实验室开放研究基金(项目编号: Kfkt2013-08)资助的课题.
      Corresponding author: Zhang Nan, zhangn@nankai.edu.cn
    • Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 61137001, 11274185, 11004111), and the Open Research Fund of Key Laboratory of High Performance Complex Manufacturing, Central South University, China (Grant No. Kfkt2013-08).
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    Qian L, Wang Y, Liu L, Fan S 2011 Acta Phys. Sin. 60 028801 (in Chinese) [潜力, 王昱权, 刘亮, 范守善 2011 物理学报 60 028801]

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    Yan A, Lau B W, Weissman B S, Kulaots I, Yang N Y C, Kane A B, Hurt R 2006 Adv. Mater. 18 2373

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    Cappelli E, Orlando S, Morandi V, Servidori M, Scilletta C 2007 J. Phys. 59 616

    [13]

    Jin Z, Zhao L, Peng H, Zhou C, Zhang B, Chen B, Chen Y, Li M 2005 Acta Phys. Sin. 54 4294 (in Chinese) [金曾孙, 赵立新, 彭鸿雁, 周传胜, 张冰, 陈宝玲, 陈玉强, 李敏君 2005 物理学报 54 4294]

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    Orden A V, Saykally R J 1998 Chem. Rev. 98 2313

    [15]

    Al-Shboul K F, Harilal S S, Hassanein A 2013 J. Appl. Phys. 113 163305

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    Amoruso S, Ausanio G, Vitiello M, Wang X 2005 Appl. Phys. A 81 981

    [17]

    Fuge G M, Ashfold M N R, Henley S J 2006 J. Appl. Phys. 99 014309

    [18]

    Park H S, Nam S H, Park S M 2005 J. Appl. Phys. 97 113103

    [19]

    Vidal F, Johnston T W, Laville S, Barthelemy O, Chaker M, Le Drogoff B, Margot J, Sabsabi, M 2001 Phys. Rev. Lett. 86 2573

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    Tanabashi A, Hirao T, Amano T, Bernath P F 2007 Astrophys J. Suppl. Ser. 169 472

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    Maier J P 1997 Chem. Soc. Rev. 26 21

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    Naulin B C, Costes M, Dorthe G 1988 Chem. Phys. Lett. 143 496

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    Zhang N, Wang W, Zhu X, Liu J, Xu K, Huang P, Zhao J, Li R, Wang M 2011 Opt. Express 19 8870

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    Paltauf G, Dyer P E 2003 Chem. Rev. 103 487

  • [1]

    Peng N, Huo Y, Zhou K, Jia X, Pan J, Sun Z, Jia T 2013 Acta Phys. Sin. 62 094201 (in Chinese) [彭娜娜, 霍燕燕, 周侃, 贾鑫, 潘佳, 孙真荣, 贾天卿 2013 物理学报 62 094201]

    [2]

    Hu A, Rybachuk M, Lu Q B, Duley W W 2007 Appl. Phys. Lett. 91 131906

    [3]

    Lorazo P, Lewis L J, Meunier M 2006 Phys. Rev. B 73 134108

    [4]

    Wu H, Zhang N, Zhu X 2014 Appl. Surf. Sci. 317 167

    [5]

    Feng P, Zhang N, Wu H, Zhu X 2015 Opt. Lett. 40 17

    [6]

    Wu Z, Zhu X, Zhang N 2011 J. Appl. Phys. 109 053113

    [7]

    Loir A S, Garrelie F, Donnet C, Belin M, Forest B, Rogemond F, Laporte P 2004 Thin Solid Films 453-454 531

    [8]

    Qian L, Wang Y, Liu L, Fan S 2011 Acta Phys. Sin. 60 028801 (in Chinese) [潜力, 王昱权, 刘亮, 范守善 2011 物理学报 60 028801]

    [9]

    Yoo E J, Okata T, Akita T, Kohyama M, Nakamura J, Honma I 2009 Nano Lett. 9 2255

    [10]

    Yan A, Lau B W, Weissman B S, Kulaots I, Yang N Y C, Kane A B, Hurt R 2006 Adv. Mater. 18 2373

    [11]

    Puretzky A A, Schittenhelm H, Fan X, Lance M J, Allard Jr. L F, Geohegan D B 2002 Phys. Rev. B 65 245425

    [12]

    Cappelli E, Orlando S, Morandi V, Servidori M, Scilletta C 2007 J. Phys. 59 616

    [13]

    Jin Z, Zhao L, Peng H, Zhou C, Zhang B, Chen B, Chen Y, Li M 2005 Acta Phys. Sin. 54 4294 (in Chinese) [金曾孙, 赵立新, 彭鸿雁, 周传胜, 张冰, 陈宝玲, 陈玉强, 李敏君 2005 物理学报 54 4294]

    [14]

    Orden A V, Saykally R J 1998 Chem. Rev. 98 2313

    [15]

    Al-Shboul K F, Harilal S S, Hassanein A 2013 J. Appl. Phys. 113 163305

    [16]

    Amoruso S, Ausanio G, Vitiello M, Wang X 2005 Appl. Phys. A 81 981

    [17]

    Fuge G M, Ashfold M N R, Henley S J 2006 J. Appl. Phys. 99 014309

    [18]

    Park H S, Nam S H, Park S M 2005 J. Appl. Phys. 97 113103

    [19]

    Vidal F, Johnston T W, Laville S, Barthelemy O, Chaker M, Le Drogoff B, Margot J, Sabsabi, M 2001 Phys. Rev. Lett. 86 2573

    [20]

    Tanabashi A, Hirao T, Amano T, Bernath P F 2007 Astrophys J. Suppl. Ser. 169 472

    [21]

    Maier J P 1997 Chem. Soc. Rev. 26 21

    [22]

    Naulin B C, Costes M, Dorthe G 1988 Chem. Phys. Lett. 143 496

    [23]

    Zhang N, Wang W, Zhu X, Liu J, Xu K, Huang P, Zhao J, Li R, Wang M 2011 Opt. Express 19 8870

    [24]

    Paltauf G, Dyer P E 2003 Chem. Rev. 103 487

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出版历程
  • 收稿日期:  2015-05-03
  • 修回日期:  2015-07-07
  • 刊出日期:  2015-11-05

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