Size Dependence and Role of Decoherence in Hot Electron Relaxation within Fluorinated Silicon Quantum Dots: A First-Principles Study

Wong, Jian Cheng; Li, Lesheng; Kanai, Yosuke

doi:10.1021/acs.jpcc.8b08030

Title: Size Dependence and Role of Decoherence in Hot Electron Relaxation within Fluorinated Silicon Quantum Dots: A First-Principles Study

Journal Article · 01 December 2018 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.8b08030 · OSTI ID:1543655

^[1];

^[2]; Kanai, Yosuke ^[1]

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

Reeves et al. in their recent work on small silicon quantum dots found that surface passivation with fluorine atoms results in a significant slow down of hot electron relaxation because there exist particular electronic states that retain the hot electron for an extended time, and the relaxation time scale is largely influenced by shuttling of the hot electron between energetically adjacent states by such unique electronic states. In this work, we investigate how the quantum dot size changes this observation associated with the fluorine passivation and also consider the effect of decoherence. With the larger size of silicon quantum dot, the distinct hot electron shuttling behavior is no longer observed, and the relaxation time constant is much shorter. At the same time, decoherence can significantly slow down the hot electron relaxation by a factor of two or more. Lastly, our study reveals that slow hot electron relaxation can result from the quantum Zeno effect, in addition to the surface-specific vibronic effect for small quantum dots.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Oakland, CA (United States); Univ. of North Carolina, Chapel Hill, NC (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

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

OSTI ID:: 1543655

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 51 Vol. 122; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Size Dependence and Role of Decoherence in Hot Electron Relaxation within Fluorinated Silicon Quantum Dots: A First-Principles Study

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