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Title: Quasiparticle spectra from molecules to bulk

Journal Article · · Physical Review Materials
 [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

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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1426485
Alternate ID(s):
OSTI ID: 1426511
Journal Information:
Physical Review Materials, Vol. 2, Issue 3; ISSN 2475-9953
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 14 works
Citation information provided by
Web of Science

References (28)

Spectral functions of the uniform electron gas via coupled-cluster theory and comparison to the G W and related approximations journal June 2016
Study of the valence electronic structure of ethyne by electron momentum spectroscopy and Green’s function methods journal March 1991
Singularities in the X-Ray Spectra of Metals journal January 1970
Optische Eigenschaften des einkristallinen Siliziums aus Elektronenenergieverlustmessungen journal December 1978
Photoemission spectroscopy of germanium nanocrystal films journal October 2002
Description of quasiparticle and satellite properties via cumulant expansions of the retarded one-particle Green's function journal August 2016
Physical Origin of Satellites in Photoemission of Doped Graphene: An Ab Initio G W Plus Cumulant Study journal April 2013
New Method for Calculating the One-Particle Green's Function with Application to the Electron-Gas Problem journal August 1965
The GW method journal March 1998
Satellite band structure in silicon caused by electron-plasmon coupling journal May 2015
Stochastic GW Calculations for Molecules journal September 2017
Outer- and inner-valence ionization spectra of NH3, PH3, and AsH3: symmetry-adapted cluster configuration interaction general- R study journal February 2002
Electron correlation in semiconductors and insulators: Band gaps and quasiparticle energies journal October 1986
Band Structures of Plasmonic Polarons journal April 2015
Inhomogeneous Electron Gas journal November 1964
Dispersion and line shape of plasmon satellites in one, two, and three dimensions journal June 2016
XSEDE: Accelerating Scientific Discovery journal September 2014
Multiple Plasmon Satellites in Na and Al Spectral Functions from Ab Initio Cumulant Expansion journal September 1996
Valence Electron Photoemission Spectrum of Semiconductors: Ab Initio Description of Multiple Satellites journal October 2011
Electronic excitations: density-functional versus many-body Green’s-function approaches journal June 2002
Correlation effects in the valence x-ray photoionization spectra of ethylene, butadiene, and hexatriene journal January 1997
Real-time cumulant approach for charge-transfer satellites in x-ray photoemission spectra journal March 2015
Computational studies of satellite peaks of the inner-valence ionization of C2H4, C2H2 and H2S using the SAC CI method journal November 1989
Cumulant expansion of the retarded one-electron Green function journal August 2014
Single-particle spectrum of the degenerate electron gas: I. The structure of the spectral weight function journal September 1967
Interacting Electrons: Theory and Computational Approaches book June 2016
Breaking the Theoretical Scaling Limit for Predicting Quasiparticle Energies: The Stochastic G W Approach journal August 2014
Self-Consistent Equations Including Exchange and Correlation Effects journal November 1965

Figures / Tables (4)