Degradation of Alkali-Based Photocathodes from Exposure to Residual Gases: A First-Principles Study

Wang, Gaoxue; Pandey, Ravindra; Moody, Nathan A.; Batista, Enrique R.

doi:10.1021/acs.jpcc.6b12796

Title: Degradation of Alkali-Based Photocathodes from Exposure to Residual Gases: A First-Principles Study

Journal Article · Fri Mar 31 00:00:00 EDT 2017 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.6b12796· OSTI ID:1407878

Wang, Gaoxue ^[1]; Pandey, Ravindra ^[2];

^[3];

^[3]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Michigan Technological Univ., Houghton, MI (United States). Dept. of Physics
Michigan Technological Univ., Houghton, MI (United States). Dept. of Physics
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Photocathodes are a key component in the production of electron beams in systems such as X-ray free-electron lasers and X-ray energy-recovery linacs. Alkali-based materials display high quantum efficiency (QE), however, their QE undergoes degradation faster than metal photocathodes even in the high vacuum conditions where they operate. The high reactivity of alkali-based surfaces points to surface reactions with residual gases as one of the most important factors for the degradation of QE. In order to advance the understanding on the degradation of the QE, we investigated the surface reactivity of common residual gas molecules (e.g., O₂, CO₂, CO, H₂O, N₂, and H₂) on one of the best-known alkali-based photocathode materials, cesium antimonide (Cs₃Sb), using first-principles calculations based on density functional theory. Furthermore, the reaction sites, adsorption energy, and effect in the local electronic structure upon reaction of these molecules on (001), (110), and (111) surfaces of Cs₃Sb were computed and analyzed. The adsorption energy of these molecules on Cs3Sb follows the trend of O₂ (-4.5 eV) > CO₂ (-1.9 eV) > H₂O (-1.0 eV) > CO (-0.8 eV) > N₂ (-0.3 eV) ≈ H₂ (-0.2 eV), which agrees with experimental data on the effect of these gases on the degradation of QE. The interaction strength is determined by the charge transfer from the surfaces to the molecules. The adsorption and dissociation of O containing molecules modify the surface chemistry such as the composition, structure, charge distribution, surface dipole, and work function of Cs₃Sb, resulting in the degradation of QE with exposure to O₂, CO₂, H₂O, and CO.

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Research Organization:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-06NA25396; 20150394DR

OSTI ID:: 1407878

Report Number(s):: LA-UR-16-29612; TRN: US1703158

Journal Information:: Journal of Physical Chemistry. C, Vol. 121, Issue 15; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 22 works

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Cited By (2)

Overcoming the quantum efficiency-lifetime tradeoff of photocathodes by coating with atomically thin two-dimensional nanomaterials Wang, Gaoxue; Yang, Ping; Moody, Nathan A. npj 2D Materials and Applications, Vol. 2, Issue 1 https://doi.org/10.1038/s41699-018-0062-6	journal	June 2018
Photoemission and Degradation of Semiconductor Photocathode Huang, Pengwei; Qian, Houjun; Du, Yingchao Deutsches Elektronen-Synchrotron, DESY, Hamburg https://doi.org/10.3204/pubdb-2019-05676	text	January 2019

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