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Title: Quasiparticle spectra from molecules to bulk

Abstract

We present a stochastic cumulant GW method, allowing us to map the evolution of photoemission spectra, quasiparticle energies, lifetimes, and emergence of collective excitations from molecules to bulklike systems with up to thousands of valence electrons, including Si nanocrystals and nanoplatelets. The quasiparticle energies rise due to their coupling with collective shake-up (plasmon) excitations, and this coupling leads to significant spectral weight loss (up to 50% for the low-energy states), shortening the lifetimes and shifting the spectral features to lower energies by as much as 0.6 eV. Such features are common to all the systems studied irrespective of their sizes and shapes. For small and low-dimensional systems the surface plasmon resonances affect the frequency of the collective excitation and position of the satellites.

Authors:
 [1];  [2];  [1]
  1. Univ. of California, Los Angeles, CA (United States). Dept. of Chemistry and Biochemistry
  2. Univ. of California, Berkeley, CA (United States). Materials Science Division, Dept. of Chemistry
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1426485
Alternate Identifier(s):
OSTI ID: 1426511
Grant/Contract Number:
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 3; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Vlček, Vojtěch, Rabani, Eran, and Neuhauser, Daniel. Quasiparticle spectra from molecules to bulk. United States: N. p., 2018. Web. doi:10.1103/PhysRevMaterials.2.030801.
Vlček, Vojtěch, Rabani, Eran, & Neuhauser, Daniel. Quasiparticle spectra from molecules to bulk. United States. doi:10.1103/PhysRevMaterials.2.030801.
Vlček, Vojtěch, Rabani, Eran, and Neuhauser, Daniel. Fri . "Quasiparticle spectra from molecules to bulk". United States. doi:10.1103/PhysRevMaterials.2.030801.
@article{osti_1426485,
title = {Quasiparticle spectra from molecules to bulk},
author = {Vlček, Vojtěch and Rabani, Eran and Neuhauser, Daniel},
abstractNote = {We present a stochastic cumulant GW method, allowing us to map the evolution of photoemission spectra, quasiparticle energies, lifetimes, and emergence of collective excitations from molecules to bulklike systems with up to thousands of valence electrons, including Si nanocrystals and nanoplatelets. The quasiparticle energies rise due to their coupling with collective shake-up (plasmon) excitations, and this coupling leads to significant spectral weight loss (up to 50% for the low-energy states), shortening the lifetimes and shifting the spectral features to lower energies by as much as 0.6 eV. Such features are common to all the systems studied irrespective of their sizes and shapes. For small and low-dimensional systems the surface plasmon resonances affect the frequency of the collective excitation and position of the satellites.},
doi = {10.1103/PhysRevMaterials.2.030801},
journal = {Physical Review Materials},
number = 3,
volume = 2,
place = {United States},
year = {Fri Mar 16 00:00:00 EDT 2018},
month = {Fri Mar 16 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on March 16, 2019
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