Quasiparticle spectra from molecules to bulk
- Univ. of California, Los Angeles, CA (United States). Dept. of Chemistry and Biochemistry
- 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
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