搜索

x

留言板

尊敬的读者、作者、审稿人, 关于本刊的投稿、审稿、编辑和出版的任何问题, 您可以本页添加留言。我们将尽快给您答复。谢谢您的支持!

姓名
邮箱
手机号码
标题
留言内容
验证码

苝四甲酸二酐薄膜电子结构的同步辐射共振光电子能谱研究

李智浩 曹亮 郭玉献

引用本文:
Citation:

苝四甲酸二酐薄膜电子结构的同步辐射共振光电子能谱研究

李智浩, 曹亮, 郭玉献

Electronic structure of a 3, 4, 9, 10-perylene-tetracarboxylic-dianhydride thin film revealed by synchrotron-based resonant photoemission spectroscopy

Li Zhi-Hao, Cao Liang, Guo Yu-Xian
PDF
导出引用
  • 利用基于同步辐射的近边X射线吸收精细结构谱(NEXAFS)和共振光电子谱(RPES)研究了苝四甲酸二酐分子(PTCDA)薄膜的电子结构.碳K边NEXAFS谱中能量小于290 eV的四个峰对应于PTCDA分子不同化学环境碳原子1s电子到未占据分子轨道的共振跃迁.RPES谱中观察到共振光电子发射和共振俄歇电子发射导致的共振峰结构,以及二次谐波激发的碳1s信号.根据电子动能对入射光能量的依赖性分别对三类峰结构进行了归属.同时,发现PTCDA分子轨道共振光电子峰的强度具有光子能量依赖性.这种能量选择性共振增强效应是由于PTCDA分子轨道空间分布差异导致的.共振俄歇峰主要源于高结合能(4.1 eV)分子轨道能级电子参与的退激发过程.明确RPES实验谱图中各个峰结构的起源有助于准确利用基于RPES的芯能级空穴时钟谱技术定量估算有机分子/电极异质界面处电子从分子未占据轨道到电极导带的超快转移时间.
    The electronic structure of a 3,4,9,10-perylene-tetracarboxylic-dianhydride (PTCDA) thin film is investigated in situ using synchrotron-based near edge X-ray absorption fine structure (NEXAFS) spectroscopy and resonant photoemission spectroscopy (RPES).The NEXAFS spectroscopy can monitor the electronic transitions from core level to unoccupied states.The C K-edge NEXAFS spectrum of the PTCDA thin film shows four distinct absorption peaks below 290 eV,which are attributed to the transitions from 1s core level of C-atoms in different chemical environments (perylene core C-atoms vs anhydride C-atoms) into lowest unoccupied molecular orbitals (LUMOs) with * symmetry. The RPES spectra are collected in the valence band region by sweeping photon energy across the C 1s * absorption edge.Three typical features of the C 1s signals excited by second-order harmonic X-ray,resonant photoemission and resonant Auger features are observed in RPES spectra,and are identified,relying on the development of kinetic energy of the emitted photoelectrons upon the change of incident photons energy.It is found that the C 1s signals excited by second-order harmonic X-ray are present at high kinetic energy side of spectrum.The kinetic energy of this feature shows photon energy dependence,that is,this feature shifts to higher kinetic energy by photon energy increasing twice.Resonant Auger peaks in RPES spectra are located on the low kinetic energy side with constant kinetic energy regardless the change of photon energy.The resonant Auger may originate from deeper molecular orbitals with binding energy large than 4.1 eV,suggesting that the resonant Auger decay process involved in deeper molecular orbitals occurs on a time scale comparable to C 1s core hole lifetime of 6 femtoseconds.Resonant enhancement of highest occupied molecular orbitals (HOMOs) derived valence band features or HOMO-1 and HOMO-2 derived resonant photoemission features in our case are lying between the C 1s signals and the resonant Auger signals.The Kinetic energy increases as the photon energy sweeps across the absorption edge,whereas their binding energy remains constant.In addition, the enhancements of two resonances show photon energy dependence that enhancement of HOMO-1 related resonance dominates over HOMO-2 related resonance at energies corresponding to perylene core C 1s to LUMOs transitions, whereas HOMO-2 related resonance becomes dominant at transitions from anhydride C 1s to LUMOs.This behavior can be related to the wavefunction character and symmetry of the frontier molecular orbitals.Clarifying each resonant feature in RPES spectra and their origin will pave the way for accurately determining the ultrafast charge transfer time at organic/electrode interfaces using synchrotron-based core hole clock technique implementation of RPES.
      通信作者: 曹亮, lcao@hmfl.ac.cn;guo_yuxian@163.com ; 郭玉献, lcao@hmfl.ac.cn;guo_yuxian@163.com
    • 基金项目: 国家自然科学基金(批准号:11574317,21503233)、安徽省自然科学基金(批准号:1608085MA07)和安徽高校自然科学研究项目(批准号:KJ2016A143)资助的课题.
      Corresponding author: Cao Liang, lcao@hmfl.ac.cn;guo_yuxian@163.com ; Guo Yu-Xian, lcao@hmfl.ac.cn;guo_yuxian@163.com
    • Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 11574317, 21503233), Anhui Provincial Natural Science Foundation, China (Grant No.1608085MA07), and the Natural Science Foundation from the Education Bureau of Anhui Province, China (Grant No.KJ2016A143).
    [1]

    Tang M L, Bao Z N 2011 Chem. Mater. 23 446

    [2]

    Mei J G, Diao Y, Appleton A L, Fang L, Bao Z N 2013 J. Am. Chem. Soc. 135 6724

    [3]

    Torsi L, Magliulo M, Manoli K, Palazzo G 2013 Chem. Soc. Rev. 42 8612

    [4]

    Reineke S, Thomschke M, Lssem B, Leo K 2013 Rev. Mod. Phys. 85 1245

    [5]

    Hains A W, Liang Z Q, Woodhouse M A, Gregg B A 2010 Chem. Rev. 110 6689

    [6]

    Zhao J B, Li Y K, Yang G F, Jiang K, Lin H R, Ade H, Ma W, Yan H 2016 Nat. Energy 1 15027

    [7]

    Ostroverkhova O 2016 Chem. Rev. 116 13279

    [8]

    Hu Z H, Zhong Z M, Chen Y W, Sun C, Huang F, Peng J B, Wang J, Cao Y 2016 Adv. Funct. Mater. 26 129

    [9]

    Pan X, Ju H X, Feng X F, Fan Q T, Wang C H, Yang Y W, Zhu J F 2015 Acta Phys. Sin. 64 077304 (in Chinese) [潘宵, 鞠焕鑫, 冯雪飞, 范其瑭, 王嘉兴, 杨耀文, 朱俊发 2015 物理学报 64 077304]

    [10]

    Cao L, Wang Y Z, Zhong J Q, Han Y Y, Zhang W H, Yu X J, Xu F Q, Qi D C, Wee A T S 2014 J. Phys. Chem. C 118 4160

    [11]

    Brhwiler P A, Karis O, Mrtensson N 2002 Rev. Mod. Phys. 74 703

    [12]

    Zharnikov M 2015 J. Electron. Spectrosc. Relat. Phenom. 200 160

    [13]

    Cao L, Gao X Y, Wee A T S, Qi D C 2014 Adv. Mater. 26 7880

    [14]

    Forrest S R 2003 J. Phys. Condens. Matter 15 S2599

    [15]

    Tautz F S 2007 Prog. Surf. Sci. 82 47

    [16]

    Guo Y L, Yu G, Liu Y Q 2010 Adv. Mater. 22 4427

    [17]

    Ou G P, Song Z, Wu Y Y, Chen X Q, Zhang F J 2006 Chin. Phys. B 15 1296

    [18]

    Cao L, Zhang W H, Chen T X, Han Y Y, Xu G Q, Zhu J F, Yan W S, Xu Y, Wang F 2010 Acta Phys. Sin. 59 1681 (in Chinese) [曹亮, 张文华, 陈铁锌, 韩玉岩, 徐法强, 朱俊发, 闫文盛, 许杨, 王峰 2010 物理学报 59 1681]

    [19]

    Han Y Y, Cao L, Xu F Q, Chen T X, Zheng Z Y, Wan L, Liu L Y 2012 Acta Phys. Sin. 61 078103 (in Chinese) [韩玉岩, 曹亮, 徐法强, 陈铁锌, 郑志远, 万力, 刘凌云 2012 物理学报 61 078103]

    [20]

    Coville M, Thomas T D 1991 Phys. Rev. A 43 6053

    [21]

    Cao L, Wang Y Z, Zhong J Q, Han Y Y, Zhang W H, Yu X J, Xu F Q, Qi D C, Wee A T S 2011 J. Phys. Chem. C 115 24880

    [22]

    Cao L, Wang Y Z, Chen T X, Zhang W H, Yu X J, Ibrahim K, Wang J O, Qian H J, Xu F Q, Qi D C 2011 J. Chem. Phys. 135 174701

    [23]

    Taborski J, Vterlein P, Dietz H, Zimmermann U, Umbach E 1995 J. Electron. Spectrosc. Relat. Phenom. 75 129

    [24]

    Kikuma J, Tonner B P 1996 J. Electron. Spectrosc. Relat. Phenom. 82 41

    [25]

    Kera S, Setoyama H, Onoue M, Okudaira K K, Harada Y, Ueno N 2001 Phys. Rev. B 63 115204

    [26]

    Zahn D R T, Gavrila G N, Gorgoi M 2006 Chem. Phys. 325 99

  • [1]

    Tang M L, Bao Z N 2011 Chem. Mater. 23 446

    [2]

    Mei J G, Diao Y, Appleton A L, Fang L, Bao Z N 2013 J. Am. Chem. Soc. 135 6724

    [3]

    Torsi L, Magliulo M, Manoli K, Palazzo G 2013 Chem. Soc. Rev. 42 8612

    [4]

    Reineke S, Thomschke M, Lssem B, Leo K 2013 Rev. Mod. Phys. 85 1245

    [5]

    Hains A W, Liang Z Q, Woodhouse M A, Gregg B A 2010 Chem. Rev. 110 6689

    [6]

    Zhao J B, Li Y K, Yang G F, Jiang K, Lin H R, Ade H, Ma W, Yan H 2016 Nat. Energy 1 15027

    [7]

    Ostroverkhova O 2016 Chem. Rev. 116 13279

    [8]

    Hu Z H, Zhong Z M, Chen Y W, Sun C, Huang F, Peng J B, Wang J, Cao Y 2016 Adv. Funct. Mater. 26 129

    [9]

    Pan X, Ju H X, Feng X F, Fan Q T, Wang C H, Yang Y W, Zhu J F 2015 Acta Phys. Sin. 64 077304 (in Chinese) [潘宵, 鞠焕鑫, 冯雪飞, 范其瑭, 王嘉兴, 杨耀文, 朱俊发 2015 物理学报 64 077304]

    [10]

    Cao L, Wang Y Z, Zhong J Q, Han Y Y, Zhang W H, Yu X J, Xu F Q, Qi D C, Wee A T S 2014 J. Phys. Chem. C 118 4160

    [11]

    Brhwiler P A, Karis O, Mrtensson N 2002 Rev. Mod. Phys. 74 703

    [12]

    Zharnikov M 2015 J. Electron. Spectrosc. Relat. Phenom. 200 160

    [13]

    Cao L, Gao X Y, Wee A T S, Qi D C 2014 Adv. Mater. 26 7880

    [14]

    Forrest S R 2003 J. Phys. Condens. Matter 15 S2599

    [15]

    Tautz F S 2007 Prog. Surf. Sci. 82 47

    [16]

    Guo Y L, Yu G, Liu Y Q 2010 Adv. Mater. 22 4427

    [17]

    Ou G P, Song Z, Wu Y Y, Chen X Q, Zhang F J 2006 Chin. Phys. B 15 1296

    [18]

    Cao L, Zhang W H, Chen T X, Han Y Y, Xu G Q, Zhu J F, Yan W S, Xu Y, Wang F 2010 Acta Phys. Sin. 59 1681 (in Chinese) [曹亮, 张文华, 陈铁锌, 韩玉岩, 徐法强, 朱俊发, 闫文盛, 许杨, 王峰 2010 物理学报 59 1681]

    [19]

    Han Y Y, Cao L, Xu F Q, Chen T X, Zheng Z Y, Wan L, Liu L Y 2012 Acta Phys. Sin. 61 078103 (in Chinese) [韩玉岩, 曹亮, 徐法强, 陈铁锌, 郑志远, 万力, 刘凌云 2012 物理学报 61 078103]

    [20]

    Coville M, Thomas T D 1991 Phys. Rev. A 43 6053

    [21]

    Cao L, Wang Y Z, Zhong J Q, Han Y Y, Zhang W H, Yu X J, Xu F Q, Qi D C, Wee A T S 2011 J. Phys. Chem. C 115 24880

    [22]

    Cao L, Wang Y Z, Chen T X, Zhang W H, Yu X J, Ibrahim K, Wang J O, Qian H J, Xu F Q, Qi D C 2011 J. Chem. Phys. 135 174701

    [23]

    Taborski J, Vterlein P, Dietz H, Zimmermann U, Umbach E 1995 J. Electron. Spectrosc. Relat. Phenom. 75 129

    [24]

    Kikuma J, Tonner B P 1996 J. Electron. Spectrosc. Relat. Phenom. 82 41

    [25]

    Kera S, Setoyama H, Onoue M, Okudaira K K, Harada Y, Ueno N 2001 Phys. Rev. B 63 115204

    [26]

    Zahn D R T, Gavrila G N, Gorgoi M 2006 Chem. Phys. 325 99

  • [1] 陶聪, 王敬民, 牛美玲, 朱琳, 彭其明, 王建浦. 非磁性发光材料的磁场效应: 从有机半导体到卤化物钙钛矿. 物理学报, 2022, 71(6): 068502. doi: 10.7498/aps.71.20211872
    [2] 黄超, 刘凌云, 方军, 张文华, 王凯, 高品, 徐法强. 强磁场对酞菁铁薄膜分子取向及形貌的影响. 物理学报, 2016, 65(15): 156101. doi: 10.7498/aps.65.156101
    [3] 潘宵, 鞠焕鑫, 冯雪飞, 范其瑭, 王嘉兴, 杨耀文, 朱俊发. F8BT薄膜表面形貌及与Al形成界面的电子结构和反应. 物理学报, 2015, 64(7): 077304. doi: 10.7498/aps.64.077304
    [4] 曹宁通, 张雷, 吕路, 谢海鹏, 黄寒, 牛冬梅, 高永立. 酞菁铜与MoS2(0001)范德瓦耳斯异质结研究. 物理学报, 2014, 63(16): 167903. doi: 10.7498/aps.63.167903
    [5] 刘瑞兰, 王徐亮, 唐超. 基于粒子群算法的有机半导体NPB传输特性辨识. 物理学报, 2014, 63(2): 028105. doi: 10.7498/aps.63.028105
    [6] 蔡春锋, 张兵坡, 黎瑞锋, 徐天宁, 毕岗, 吴惠桢, 张文华, 朱俊发. 利用同步辐射光电子能谱技术测量ZnO/PbTe异质结的能带带阶. 物理学报, 2014, 63(16): 167301. doi: 10.7498/aps.63.167301
    [7] 蹇磊, 谭英雄, 李权, 赵可清. 吐昔烯衍生物分子的电荷传输性质. 物理学报, 2013, 62(18): 183101. doi: 10.7498/aps.62.183101
    [8] 万力, 曹亮, 张文华, 韩玉岩, 陈铁锌, 刘凌云, 郭盼盼, 冯金勇, 徐法强. FePc与TiO2(110)及C60界面电子结构研究. 物理学报, 2012, 61(18): 186801. doi: 10.7498/aps.61.186801
    [9] 张旺, 徐法强, 王国栋, 张文华, 李宗木, 王立武, 陈铁锌. Fe/ZnO (0001)体系界面相互作用中薄膜厚度效应的光电子能谱研究. 物理学报, 2011, 60(1): 017104. doi: 10.7498/aps.60.017104
    [10] 曹亮, 张文华, 陈铁锌, 韩玉岩, 徐法强, 朱俊发, 闫文盛, 许杨, 王峰. 苝四甲酸二酐在Au(111)表面的取向生长及电子结构研究. 物理学报, 2010, 59(3): 1681-1688. doi: 10.7498/aps.59.1681
    [11] 汪润生, 孟卫民, 彭应全, 马朝柱, 李荣华, 谢宏伟, 王颖, 赵明, 袁建挺. 有机半导体的物理掺杂理论. 物理学报, 2009, 58(11): 7897-7903. doi: 10.7498/aps.58.7897
    [12] 李训栓, 彭应全, 杨青森, 刑宏伟, 路飞平. 有机半导体异质界面电荷传输解析模型研究. 物理学报, 2007, 56(9): 5441-5445. doi: 10.7498/aps.56.5441
    [13] 任俊峰, 张玉滨, 解士杰. 铁磁/有机半导体/铁磁系统的电流自旋极化性质研究. 物理学报, 2007, 56(8): 4785-4790. doi: 10.7498/aps.56.4785
    [14] 王国栋, 张 旺, 张文华, 李宗木, 徐法强. Fe/ZnO(0001)界面的同步辐射光电子能谱研究. 物理学报, 2007, 56(6): 3468-3472. doi: 10.7498/aps.56.3468
    [15] 何少龙, 李宏年, 王晓雄, 李海洋, I. Kurash, 钱海杰, 苏 润, M. I. Abbas, 钟 俊, 洪才浩. Yb2.75C60同步辐射光电子能谱. 物理学报, 2005, 54(3): 1400-1405. doi: 10.7498/aps.54.1400
    [16] 李宏年. Rb掺杂C60单晶的相衍变和电子态. 物理学报, 2004, 53(1): 248-253. doi: 10.7498/aps.53.248
    [17] 苑进社, 陈光德, 齐鸣, 李爱珍, 徐卓. 分子束外延GaN薄膜的X射线光电子能谱和俄歇电子能谱研究. 物理学报, 2001, 50(12): 2429-2433. doi: 10.7498/aps.50.2429
    [18] 吕 明, 徐少辉, 张松涛, 何 钧, 熊祖洪, 邓振波, 丁训民. 基于多孔硅分布Bragg反射镜的有机微腔的光学性质. 物理学报, 2000, 49(10): 2083-2088. doi: 10.7498/aps.49.2083
    [19] 施一生, 赵特秀, 刘洪图, 王晓平. Pd/W/Si(111)双层膜界面X射线光电子能谱与俄歇电子能谱研究. 物理学报, 1992, 41(11): 1849-1855. doi: 10.7498/aps.41.1849
    [20] 钟战天, 王大文, 廖显伯, 范越, 李承芳, 牟善明. Au/a-Si:H界面X射线光电子能谱和俄歇电子能谱研究. 物理学报, 1991, 40(2): 275-280. doi: 10.7498/aps.40.275
计量
  • 文章访问数:  5460
  • PDF下载量:  181
  • 被引次数: 0
出版历程
  • 收稿日期:  2017-05-31
  • 修回日期:  2017-08-23
  • 刊出日期:  2017-11-05

/

返回文章
返回