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Title: Importance of bulk excitations and coherent electron-photon-phonon scattering in photoemission from PbTe(111): Ab initio theory with experimental comparisons

Journal Article · · Physical Review B
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [4];  [5]
  1. Cornell Univ., Ithaca, NY (United States); DOE awards recipients are H.A. Padmore and S. Karkare (coauthors) through Lawrence Berkeley National Laboratory and through Department of Physics, Arizona State University. (J. Kevin Nangoi is not a direct recipient of the DOE awards.)
  2. Arizona State Univ., Tempe, AZ (United States)
  3. Rensselaer Polytechnic Inst., Troy, NY (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  5. Cornell Univ., Ithaca, NY (United States)
+ Show Author Affiliations

This paper presents a fully ab initio many-body photoemission framework that includes coherent three-body electron-photon-phonon scattering to predict the transverse momentum distributions and the mean transverse energies (MTEs) of bulk photoelectrons from single-crystal photocathodes. The need to develop such a theory stems from the lack of studies that provide complete understanding of the underlying fundamental processes governing the transverse momentum distribution of photoelectrons emitted from single crystals. For example, initial predictions based on density-functional theory calculations of effective electron masses suggested that the (111) surface of PbTe would produce very small MTEs (≤ 15 meV), whereas our experiments yielded MTEs ten to twenty times larger than these predictions and also exhibited a lower photoemission threshold than predicted. The ab initio framework presented in this paper correctly reproduces both the magnitude of the MTEs from our measurements in PbTe(111) and the observed photoemission below the predicted threshold. Our results show that both photoexcitations into states that propagate in the bulk of the material and coherent many-body electron-photon-phonon scattering processes, which initial predictions ignored, play surprisingly important roles in photoemission from PbTe(111). Lastly, from the lessons learned, we recommend a procedure for rapid computational screening of potential single-crystal photocathodes for applications in next-generation ultrafast electron diffraction and X-ray free-electron lasers, which will enable significant advances in condensed matter research.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Arizona State Univ., Tempe, AZ (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0021092; AC02-05CH11231
OSTI ID:
1820969
Journal Information:
Physical Review B, Journal Name: Physical Review B Journal Issue: 11 Vol. 104; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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36 MATERIALS SCIENCE
Monte Carlo methods
Wannier function methods
condensed matter physics
density functional theory
electron sources
electronic structure
first-principles calculations
phonons
photoemission spectroscopy
single crystal materials