Coverage dependence of the level alignment for methanol on TiO2(110)

被引:12
|
作者
Migani, Annapaola [1 ,2 ]
Mowbray, Duncan J. [3 ,4 ,5 ]
机构
[1] ICN2 Inst Catala Nanociencia, E-08193 Barcelona, Spain
[2] CSIC, E-08193 Barcelona, Spain
[3] Univ Pais Vasco UPV EHU, Nanobio Spect Grp, E-20018 San Sebastian, Spain
[4] Univ Pais Vasco UPV EHU, ETSF Sci Dev Ctr, Dept Fis Mat, E-20018 San Sebastian, Spain
[5] DIPC, E-20018 San Sebastian, Spain
关键词
Level alignment; HOMO; Wet electron level; Two photon photoemission; Ultraviolet photoemission spectroscopy; Photocatalysis; PHOTOCATALYTIC DISSOCIATION; SURFACE SCIENCE; GREENS-FUNCTION; WATER; PHOTOCHEMISTRY; RUTILE;
D O I
10.1016/j.comptc.2014.03.007
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Electronic level alignment at the interface between an adsorbed molecular layer and a semiconducting substrate determines the activity and efficiency of many photocatalytic materials. We perform G(0)W(0) calculations to determine the coverage dependence of the level alignment for a prototypical photocatalytic interface: 1/2 and 1 monolayer (ML) intact and dissociated CH3OH on rutile TiO2(1 1 0). We find changes in the wavefunction's spatial distribution, and a consequent renormalization of the quasiparticle energy levels, as a function of CH3OH coverage and dissociation. Our results suggest that the occupied molecular levels responsible for hole trapping are not those observed in the ultraviolet photoemission spectroscopy (UPS) spectrum. Rather, they are those of isolated CH3O on the surface. We find the unoccupied molecular levels have either 2D character with weight above the surface at 1 ML coverage, or significant hybridization with the surface at 1/2 ML coverage. These results suggest the resonance observed in the two photon phooemission (2PP) spectrum arises from excitations to unoccupied "Wet electron" levels with 2D character. (C) 2014 Elsevier B.V. All rights reserved.
引用
收藏
页码:259 / 265
页数:7
相关论文
共 50 条
  • [41] Structural Dependence of Competitive Adsorption of Water and Methanol on TiO2 Surfaces
    Wang, Zhengming
    Xiong, Feng
    Sun, Guanghui
    Jin, Yuekang
    Huang, Weixin
    CHINESE JOURNAL OF CHEMISTRY, 2017, 35 (06) : 889 - 895
  • [42] The impact of metalation on adsorption geometry, electronic level alignment and UV-stability of organic macrocycles on TiO2(110)
    Graf, Manuel
    Mette, Gerson
    Leuenberger, Dominik
    Gurdal, Yeliz
    Iannuzzi, Marcella
    Zabka, Wolf-Dietrich
    Schnidrig, Stephan
    Probst, Benjamin
    Hutter, Jurg
    Alberto, Roger
    Osterwalder, Jurg
    NANOSCALE, 2017, 9 (25) : 8756 - 8763
  • [43] Using G0W0 Level Alignment to Identify Catechol's Structure on TiO2(110)
    Mowbray, Duncan J.
    Migani, Annapaola
    JOURNAL OF PHYSICAL CHEMISTRY C, 2015, 119 (34): : 19634 - 19641
  • [44] Using GoWo Level Alignment to Identify Catechol's Structure on TiO2(110) (vol 119, 19634, 2015)
    Mowbray, Duncan J.
    Migani, Annapaola
    JOURNAL OF PHYSICAL CHEMISTRY C, 2016, 120 (07): : 4151 - 4151
  • [45] Photochemistry of NO chemisorbed on TiO2(110) and TiO2 powders
    Rusu, CN
    Yates, JT
    JOURNAL OF PHYSICAL CHEMISTRY B, 2000, 104 (08): : 1729 - 1737
  • [46] Strong Photon Energy Dependence of the Photocatalytic Dissociation Rate Methanol on TiO2(110) (vol 135, pg 19039, 2013)
    Xu, Chenbiao
    Yang, Wenshao
    Ren, Zefeng
    Dai, Dongxu
    Guo, Qing
    Minton, Timothy K.
    Yang, Xueming
    JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (12) : 4794 - 4794
  • [47] Dependence of calcium phosphate formation on nanostructure of rutile TiO2(110) surfaces
    Sasahara, Akira
    Murakami, Tatsuya
    Tomitori, Masahiko
    JAPANESE JOURNAL OF APPLIED PHYSICS, 2018, 57 (11)
  • [48] Anomalous Dependence of Photocarrier Recombination Time on the Polaron Density of TiO2(110)
    Wang, Huimin
    Fu, Huixia
    You, Peiwei
    Zhang, Cui
    Jiang, Ying
    Meng, Sheng
    JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2023, 14 (37): : 8312 - 8319
  • [49] Imaging adsorbate O-H bond cleavage:: Methanol on TiO2(110)
    Zhang, ZR
    Bondarchuk, O
    White, JM
    Kay, BD
    Dohnálek, Z
    JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (13) : 4198 - 4199
  • [50] Enhanced activity for supported Au clusters: Methanol oxidation on Au/TiO2(110)
    Tenney, Samuel A.
    Cagg, Brett A.
    Levine, Mara S.
    He, Wei
    Manandhar, Kedar
    Chen, Donna A.
    SURFACE SCIENCE, 2012, 606 (15-16) : 1233 - 1243