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This content will become publicly available on March 16, 2019

Title: Quasiparticle spectra from molecules to bulk

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:
Grant/Contract Number:
AC02-05CH11231
Type:
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)
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 77 NANOSCIENCE AND NANOTECHNOLOGY
OSTI Identifier:
1426485
Alternate Identifier(s):
OSTI ID: 1426511