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Title: Generalizable density functional theory based photoemission model for the accelerated development of photocathodes and other photoemissive devices

Abstract

In this work, we have developed an ab initio photoemission model that accurately describes the photoemission process for the most diverse range of photocathode materials to date. Compared to previous photoemission models, this is accomplished by considerably reducing the number of approximations and assumptions used in representing the photoemission process and the photoemitting material itself. Notably, our model directly includes the full electronic structure of the material, photoexcitation probabilities for all direct optical transitions, and an improved surface-vacuum barrier transmission probability. To test the performance of our model, we perform validations with experimental measurements for all photocathode materials studied in this work. Whereas previous models have often qualitatively disagreed with the measured photoemission properties of some materials, our model is found to provide quantitative agreement with experimental measurements for all tested materials. As an example, our method predicts the root-mean-square transverse momentum of electrons emitted from PbTe up to an excess energy of 1.0 eV with a mean absolute error that is ~5× less than from previously derived expressions. Perhaps more importantly, our model is able to match experimentally observed decreases in intrinsic emittance with increasing photon energy—a feat that current analytical models are unable to achieve. We expect thatmore » the broad applicability of our model will greatly accelerate the rate of discovery, characterization, and scientific understanding of photocathodes and other photonic devices.« less

Authors:
; ; ; ORCiD logo; ; ; ; ;
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF); Austrian Science Fund (FWF)
OSTI Identifier:
1635318
Alternate Identifier(s):
OSTI ID: 1647100
Grant/Contract Number:  
AC02-76SF00515; SC0017621; PHYS-1535279; J3980-N27
Resource Type:
Published Article
Journal Name:
Physical Review B
Additional Journal Information:
Journal Name: Physical Review B Journal Volume: 101 Journal Issue: 23; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; electron sources; free-electron lasers; Bloch wave theory; density functional theory; condensed matter & materials physics; accelerators & beams

Citation Formats

Antoniuk, Evan R., Yue, Yumeng, Zhou, Yao, Schindler, Peter, Schroeder, W. Andreas, Dunham, Bruce, Pianetta, Piero, Vecchione, Theodore, and Reed, Evan J. Generalizable density functional theory based photoemission model for the accelerated development of photocathodes and other photoemissive devices. United States: N. p., 2020. Web. doi:10.1103/physrevb.101.235447.
Antoniuk, Evan R., Yue, Yumeng, Zhou, Yao, Schindler, Peter, Schroeder, W. Andreas, Dunham, Bruce, Pianetta, Piero, Vecchione, Theodore, & Reed, Evan J. Generalizable density functional theory based photoemission model for the accelerated development of photocathodes and other photoemissive devices. United States. doi:https://doi.org/10.1103/physrevb.101.235447
Antoniuk, Evan R., Yue, Yumeng, Zhou, Yao, Schindler, Peter, Schroeder, W. Andreas, Dunham, Bruce, Pianetta, Piero, Vecchione, Theodore, and Reed, Evan J. Mon . "Generalizable density functional theory based photoemission model for the accelerated development of photocathodes and other photoemissive devices". United States. doi:https://doi.org/10.1103/physrevb.101.235447.
@article{osti_1635318,
title = {Generalizable density functional theory based photoemission model for the accelerated development of photocathodes and other photoemissive devices},
author = {Antoniuk, Evan R. and Yue, Yumeng and Zhou, Yao and Schindler, Peter and Schroeder, W. Andreas and Dunham, Bruce and Pianetta, Piero and Vecchione, Theodore and Reed, Evan J.},
abstractNote = {In this work, we have developed an ab initio photoemission model that accurately describes the photoemission process for the most diverse range of photocathode materials to date. Compared to previous photoemission models, this is accomplished by considerably reducing the number of approximations and assumptions used in representing the photoemission process and the photoemitting material itself. Notably, our model directly includes the full electronic structure of the material, photoexcitation probabilities for all direct optical transitions, and an improved surface-vacuum barrier transmission probability. To test the performance of our model, we perform validations with experimental measurements for all photocathode materials studied in this work. Whereas previous models have often qualitatively disagreed with the measured photoemission properties of some materials, our model is found to provide quantitative agreement with experimental measurements for all tested materials. As an example, our method predicts the root-mean-square transverse momentum of electrons emitted from PbTe up to an excess energy of 1.0 eV with a mean absolute error that is ~5× less than from previously derived expressions. Perhaps more importantly, our model is able to match experimentally observed decreases in intrinsic emittance with increasing photon energy—a feat that current analytical models are unable to achieve. We expect that the broad applicability of our model will greatly accelerate the rate of discovery, characterization, and scientific understanding of photocathodes and other photonic devices.},
doi = {10.1103/physrevb.101.235447},
journal = {Physical Review B},
number = 23,
volume = 101,
place = {United States},
year = {2020},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
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DOI: https://doi.org/10.1103/physrevb.101.235447

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