Excited Electron Dynamics at Semiconductor–Molecule Type-II Heterojunction Interface: First-Principles Dynamics Simulation

Li, Lesheng; Kanai, Yosuke

doi:10.1021/acs.jpclett.6b00436

Title: Excited Electron Dynamics at Semiconductor–Molecule Type-II Heterojunction Interface: First-Principles Dynamics Simulation

Journal Article · Sat Apr 02 00:00:00 EDT 2016 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.6b00436· OSTI ID:1371353

Li, Lesheng ^[1]; Kanai, Yosuke ^[1]

Univ. of North Carolina, Chapel Hill, NC (United States)

Excited electron dynamics at semiconductor–molecule interfaces is ubiquitous in various energy conversion technologies. However, a quantitative understanding of how molecular details influence the quantum dynamics of excited electrons remains a great scientific challenge because of the complex interplay of different processes with various time scales. Here in this paper, we employ first-principles electron dynamics simulations to investigate how molecular features govern the dynamics in a representative interface between the hydrogen-terminated Si(111) surface and a cyanidin molecule. Hot electron transfer to the chemisorbed molecule was observed but was short-lived on the molecule. Interfacial electron transfer to the chemisorbed molecule was found to be largely decoupled from hot electron relaxation within the semiconductor surface. While the hot electron relaxation was found to take place on a time scale of several hundred femtoseconds, the subsequent interfacial electron transfer was slower by an order of magnitude. Finally, at the same time, this secondary process of picosecond electron transfer is comparable in time scale to typical electron trapping into defect states in the energy gap.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001011; AC02-05CH11231

OSTI ID:: 1371353

Journal Information:: Journal of Physical Chemistry Letters, Vol. 7, Issue 8; Related Information: UNC partners with University of North Carolina (lead); Duke University; University of Florida; Georgia Institute of Technology; University; North Carolina Central University; Research Triangle Institute; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 16 works

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Title: Excited Electron Dynamics at Semiconductor–Molecule Type-II Heterojunction Interface: First-Principles Dynamics Simulation

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