Department of Physics and Astronomy and Pittsburgh Quantum Institute, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, USA.
Hefei National Laboratory for Physical Sciences at the Microscale, and Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
Phys Rev Lett. 2018 Mar 23;120(12):126801. doi: 10.1103/PhysRevLett.120.126801.
Charge transfer in transduction of light to electrical or chemical energy at heterojunctions of metals with semiconductors or semimetals is believed to occur by photogenerated hot electrons in metal undergoing incoherent internal photoemission through the heterojunction interface. Charge transfer, however, can also occur coherently by dipole coupling of electronic bands at the heterojunction interface. Microscopic physical insights into how transfer occurs can be elucidated by following the coherent polarization of the donor and acceptor states on the time scale of electronic dephasing. By time-resolved multiphoton photoemission spectroscopy (MPP), we investigate the coherent electron transfer from an interface state that forms upon chemisorption of Ag nanoclusters onto graphite to a σ symmetry interlayer band of graphite. Multidimensional MPP spectroscopy reveals a resonant two-photon transition, which dephases within 10 fs completing the coherent transfer.
在金属与半导体或半金属的异质结中,光向电或化学能的能量转移被认为是通过金属中光生的热电子通过异质结界面进行非相干内光发射而发生的。然而,电荷转移也可以通过异质结界面处电子能带的偶极耦合而相干地发生。通过跟踪电子退相干时间尺度上施主和受主态的相干极化,可以阐明转移是如何发生的。通过时间分辨多光子光电子能谱(MPP),我们研究了从银纳米团簇化学吸附到石墨上形成的界面态到石墨的σ对称性层间带的相干电子转移。多维 MPP 光谱揭示了一个共振的双光子跃迁,该跃迁在 10 fs 内退相,从而完成了相干转移。