Ultrafast Dynamics of Photongenerated Holes at a CH3OH/TiO2 Rutile Interface
文献类型：期刊论文
| 作者 | Chu, Weibin1,2,3,4; Saidi, Wissam A.5; Zheng, Qijing1,2,3,4; Xie, Yu6,7 ; Lan, Zhenggang6,7; Prezhdo, Oleg V.8,9; Petek, Hrvoje10; Zhao, Jin1,2,3,4,10
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| 刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
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| 出版日期 | 2016-10-19 |
| 卷号 | 138期号:41页码:13740-13749 |
| 英文摘要 | Photogenerated charge carrier dynamics near molecule/TiO2 interfaces are important for the photocatalytic and photovoltaic processes. To understand this fundamental aspect, we performed a time-domain ab initio nonadiabatic molecular dynamics study of the photogenerated hole dynamics at the CH3OH/rutile TiO2(110) interface. We studied the forward and reverse hole transfer between TiO2 and CH3OH as well as the hole energy relaxation to the valence band maximum. First, we show that the hole-trapping ability of CH3OH depends strongly on the adsorption structure. Only when the CH3OH is deprotonated to form chemisorbed CH3O will 45% of the hole be trapped by the molecule. Second, we find that strong fluctuations of the HOMO energies of the adsorbed molecules induced by electron phonon coupling provide additional channels, which accelerate the hole energy relaxation. Third, we demonstrate that the charge transfer and energy relaxation processes depend significantly on temperature. When the temperature decreases from 100 to 30 K, the forward hole transfer and energy relaxation processes are strongly suppressed because of the reduction of phonon occupation. These results indicate that the molecule/TiO2 energy level alignment, thermal excitation of a phonon, and electron phonon coupling are the key factors that determine the photogenerated hole dynamics. Our studies provide valuable insights into the photogenerated charge and energy transfer dynamics at molecule/semiconductor interfaces. |
| WOS标题词 | Science & Technology ; Physical Sciences |
| 类目[WOS] | Chemistry, Multidisciplinary |
| 研究领域[WOS] | Chemistry |
| 关键词[WOS] | INITIO MOLECULAR-DYNAMICS ; COUPLED ELECTRON-TRANSFER ; SENSITIZED SOLAR-CELLS ; EXPOSED 001 FACETS ; VISIBLE-LIGHT ; TIO2 NANOPARTICLES ; LEVEL ALIGNMENT ; CHARGE-TRANSFER ; PHOTOCATALYTIC ACTIVITY ; HYDROGEN-PRODUCTION |
| 收录类别 | SCI |
| 语种 | 英语 |
| WOS记录号 | WOS:000385992100044 |
| 源URL | [http://ir.qibebt.ac.cn/handle/337004/9070]  |
| 专题 | 青岛生物能源与过程研究所_先进材料理论与模拟团队 |
| 作者单位 | 1.Univ Sci & Technol China, ICQD Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China 2.Univ Sci & Technol China, Key Lab Strongly Coupled Quantum Matter Phys Chin, Acad Sci, Hefei 230026, Anhui, Peoples R China 3.Univ Sci & Technol China, Dept Phys, Hefei 230026, Anhui, Peoples R China 4.Univ Sci & Technol China, Synerget Innovat Ctr Quantum Informat & Quantum P, Hefei 230026, Anhui, Peoples R China 5.Univ Pittsburgh, Dept Mech Engn & Mat Sci, Pittsburgh, PA 15261 USA 6.Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Key Lab Biobased Mat, Qingdao 266101, Shandong, Peoples R China 7.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 8.Univ Southern Calif, Dept Chem, Los Angeles, CA 90089 USA 9.Univ Southern Calif, Dept Phys & Astron, Los Angeles, CA 90089 USA 10.Univ Pittsburgh, Dept Phys & Astron, Pittsburgh, PA 15260 USA |
| 推荐引用方式 GB/T 7714 | Chu, Weibin,Saidi, Wissam A.,Zheng, Qijing,et al. Ultrafast Dynamics of Photongenerated Holes at a CH3OH/TiO2 Rutile Interface[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2016,138(41):13740-13749. |
| APA | Chu, Weibin.,Saidi, Wissam A..,Zheng, Qijing.,Xie, Yu.,Lan, Zhenggang.,...&Zhao, Jin.(2016).Ultrafast Dynamics of Photongenerated Holes at a CH3OH/TiO2 Rutile Interface.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,138(41),13740-13749. |
| MLA | Chu, Weibin,et al."Ultrafast Dynamics of Photongenerated Holes at a CH3OH/TiO2 Rutile Interface".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 138.41(2016):13740-13749. |
入库方式： OAI收割
来源：青岛生物能源与过程研究所
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