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Title: Cesium intercalation of graphene: A 2D protective layer on alkali antimonide photocathode

Abstract

Alkali antimonide photocathodes have wide applications in free-electron lasers and electron cooling. The short lifetime of alkali antimonide photocathodes necessitates frequent replacement of the photocathodes during a beam operation. Furthermore, exposure to mediocre vacuum causes loss of photocathode quantum efficiency due to the chemical reaction with residual gas molecules. Theoretical analyses have shown that covering an alkali antimonide photocathode with a monolayer graphene or hexagonal boron nitride protects it in a coarse vacuum environment due to the inhibition of chemical reactions with residual gas molecules. Alkali antimonide photocathodes require an ultra-high vacuum environment, and depositing a monolayer 2D material on it poses a serious challenge. In the present work, we have incorporated a novel method known as intercalation, in which alkali atoms pass through the defects of a graphene thin film to create a photocathode material underneath. Initially, Sb was deposited on a Si substrate, and a monolayer graphene was transferred on top of the Sb film. Heat cleaning around 550–600 °C effectively removed the Sb oxides, leaving metallic Sb underneath the graphene layer. Depositing Cs on top of a monolayer graphene enabled the intercalation process. Atomic force microscopy, Raman spectroscopy, x-ray photoelectron spectroscopy, low energy electron microscopy, and x-raymore » diffraction measurements were performed to evaluate photocathode formation underneath the monolayer graphene. Our analysis shows that Cs penetrated the graphene and reacted with Sb and formed Cs3Sb.« less

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2];  [2]; ORCiD logo [3];  [4]; ORCiD logo [1];  [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Euclid Techlabs, Bolingbrook, IL (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
Euclid Techlabs, LLC, Bolingbrook, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1898420
Alternate Identifier(s):
OSTI ID: 1898175; OSTI ID: 1907828
Report Number(s):
BNL-223841-2023-JAAM
Journal ID: ISSN 2166-532X; TRN: US2310898
Grant/Contract Number:  
SC0021511; SC0012704; AC02-06CH11357; AC02−76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
APL Materials
Additional Journal Information:
Journal Volume: 10; Journal Issue: 11; Journal ID: ISSN 2166-532X
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
43 PARTICLE ACCELERATORS; photocathodes; intercalation; 2D materials; graphene; electron microscopy; thin films; intercalation compounds; atomic force microscopy; x-ray photoelectron spectroscopy; x-ray diffraction; ultra-high vacuum; 36 MATERIALS SCIENCE; GaAs; photocatodes; electron affinity; low energy electron microscopy

Citation Formats

Biswas, Jyoti, Gaowei, Mengjia, Liu, Ao, Poddar, Shashi, Stan, Liliana, Smedley, John, Sadowski, Jerzy T., and Tong, Xiao. Cesium intercalation of graphene: A 2D protective layer on alkali antimonide photocathode. United States: N. p., 2022. Web. doi:10.1063/5.0122937.
Biswas, Jyoti, Gaowei, Mengjia, Liu, Ao, Poddar, Shashi, Stan, Liliana, Smedley, John, Sadowski, Jerzy T., & Tong, Xiao. Cesium intercalation of graphene: A 2D protective layer on alkali antimonide photocathode. United States. https://doi.org/10.1063/5.0122937
Biswas, Jyoti, Gaowei, Mengjia, Liu, Ao, Poddar, Shashi, Stan, Liliana, Smedley, John, Sadowski, Jerzy T., and Tong, Xiao. Tue . "Cesium intercalation of graphene: A 2D protective layer on alkali antimonide photocathode". United States. https://doi.org/10.1063/5.0122937. https://www.osti.gov/servlets/purl/1898420.
@article{osti_1898420,
title = {Cesium intercalation of graphene: A 2D protective layer on alkali antimonide photocathode},
author = {Biswas, Jyoti and Gaowei, Mengjia and Liu, Ao and Poddar, Shashi and Stan, Liliana and Smedley, John and Sadowski, Jerzy T. and Tong, Xiao},
abstractNote = {Alkali antimonide photocathodes have wide applications in free-electron lasers and electron cooling. The short lifetime of alkali antimonide photocathodes necessitates frequent replacement of the photocathodes during a beam operation. Furthermore, exposure to mediocre vacuum causes loss of photocathode quantum efficiency due to the chemical reaction with residual gas molecules. Theoretical analyses have shown that covering an alkali antimonide photocathode with a monolayer graphene or hexagonal boron nitride protects it in a coarse vacuum environment due to the inhibition of chemical reactions with residual gas molecules. Alkali antimonide photocathodes require an ultra-high vacuum environment, and depositing a monolayer 2D material on it poses a serious challenge. In the present work, we have incorporated a novel method known as intercalation, in which alkali atoms pass through the defects of a graphene thin film to create a photocathode material underneath. Initially, Sb was deposited on a Si substrate, and a monolayer graphene was transferred on top of the Sb film. Heat cleaning around 550–600 °C effectively removed the Sb oxides, leaving metallic Sb underneath the graphene layer. Depositing Cs on top of a monolayer graphene enabled the intercalation process. Atomic force microscopy, Raman spectroscopy, x-ray photoelectron spectroscopy, low energy electron microscopy, and x-ray diffraction measurements were performed to evaluate photocathode formation underneath the monolayer graphene. Our analysis shows that Cs penetrated the graphene and reacted with Sb and formed Cs3Sb.},
doi = {10.1063/5.0122937},
journal = {APL Materials},
number = 11,
volume = 10,
place = {United States},
year = {Tue Nov 15 00:00:00 EST 2022},
month = {Tue Nov 15 00:00:00 EST 2022}
}

Works referenced in this record:

Interaction of Cesium-Potassium Antimonide Photocathode Materials with Oxygen: an X-Ray Photoelectron Spectroscopy Study
journal, October 1993

  • Soriano, Leonardo; Galán, Luis
  • Japanese Journal of Applied Physics, Vol. 32, Issue Part 1, No. 10
  • DOI: 10.1143/jjap.32.4737

Preparation and study of properties of a few alkali antimonide photocathodes
journal, August 1978

  • Ghosh, C.; Varma, B. P.
  • Journal of Applied Physics, Vol. 49, Issue 8
  • DOI: 10.1063/1.325465

Raman scattering of monolayer graphene: the temperature and oxygen doping effects
journal, April 2011


Codeposition of ultrasmooth and high quantum efficiency cesium telluride photocathodes
journal, July 2019


Photoelectron transport in CsI and CsBr coating films of alkali antimonide and CsI photocathodes
journal, October 2002

  • Shefer, E.; Breskin, A.; Boutboul, T.
  • Journal of Applied Physics, Vol. 92, Issue 8
  • DOI: 10.1063/1.1505684

Stoichiometry control and automated growth of alkali antimonide photocathode films by molecular beam deposition
journal, February 2022

  • Pavlenko, Vitaly; Smedley, John; Scheinker, Alexander
  • Applied Physics Letters, Vol. 120, Issue 9
  • DOI: 10.1063/5.0080948

Temperature-dependent quantum efficiency degradation of K-Cs-Sb bialkali antimonide photocathodes grown by a triple-element codeposition method
journal, November 2017


Preparation of InSb substrates for molecular beam epitaxy
journal, July 1995

  • Liu, W. K.
  • Journal of Vacuum Science & Technology B: Microelectronics and Nanometer Structures, Vol. 13, Issue 4
  • DOI: 10.1116/1.588184

Photocathode behavior during high current running in the Cornell energy recovery linac photoinjector
journal, December 2011

  • Cultrera, Luca; Maxson, Jared; Bazarov, Ivan
  • Physical Review Special Topics - Accelerators and Beams, Vol. 14, Issue 12
  • DOI: 10.1103/physrevstab.14.120101

Photoemission from Bialkali Photocathodes through an Atomically Thin Protection Layer
journal, December 2021

  • Liu, Fangze; Guo, Lei; DeFazio, Jeffrey
  • ACS Applied Materials & Interfaces, Vol. 14, Issue 1
  • DOI: 10.1021/acsami.1c19393

Record high-average current from a high-brightness photoinjector
journal, January 2013

  • Dunham, Bruce; Barley, John; Bartnik, Adam
  • Applied Physics Letters, Vol. 102, Issue 3
  • DOI: 10.1063/1.4789395

X-ray Photoemission Spectroscopy Studies of Cesium Antimonide Photocathodes for Photoinjector Applications
journal, January 2015


X-ray photoemission studies of cesium antimonide photoemitters
journal, June 1980


Cathode R&D for future light sources
journal, October 2010

  • Dowell, D. H.; Bazarov, I.; Dunham, B.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 622, Issue 3
  • DOI: 10.1016/j.nima.2010.03.104

Cold electron beams from cryocooled, alkali antimonide photocathodes
journal, November 2015

  • Cultrera, L.; Karkare, S.; Lee, H.
  • Physical Review Special Topics - Accelerators and Beams, Vol. 18, Issue 11
  • DOI: 10.1103/physrevstab.18.113401

The mechanism of caesium intercalation of graphene
journal, November 2013

  • Petrović, M.; Šrut Rakić, I.; Runte, S.
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3772

Direct synthesis of graphene on any nonmetallic substrate based on KrF laser ablation of ordered pyrolytic graphite
journal, June 2014


Overcoming the quantum efficiency-lifetime tradeoff of photocathodes by coating with atomically thin two-dimensional nanomaterials
journal, June 2018

  • Wang, Gaoxue; Yang, Ping; Moody, Nathan A.
  • npj 2D Materials and Applications, Vol. 2, Issue 1
  • DOI: 10.1038/s41699-018-0062-6

Kinetics of alkali-based photocathode degradation
journal, November 2016

  • Pavlenko, Vitaly; Liu, Fangze; Hoffbauer, Mark A.
  • AIP Advances, Vol. 6, Issue 11
  • DOI: 10.1063/1.4967349

Direct CVD Growth of Graphene on Technologically Important Dielectric and Semiconducting Substrates
journal, September 2018

  • Khan, Afzal; Islam, Sk Masiul; Ahmed, Shahzad
  • Advanced Science, Vol. 5, Issue 11
  • DOI: 10.1002/advs.201800050

Reduced work function of graphene by metal adatoms
journal, February 2017


Degradation of Alkali-Based Photocathodes from Exposure to Residual Gases: A First-Principles Study
journal, April 2017

  • Wang, Gaoxue; Pandey, Ravindra; Moody, Nathan A.
  • The Journal of Physical Chemistry C, Vol. 121, Issue 15
  • DOI: 10.1021/acs.jpcc.6b12796

Ultra low emittance electron beams from multi-alkali antimonide photocathode operated with infrared light
journal, March 2016

  • Cultrera, L.; Gulliford, C.; Bartnik, A.
  • Applied Physics Letters, Vol. 108, Issue 13
  • DOI: 10.1063/1.4945091

Inner-orbital binding-energy shifts of antimony and bismuth compounds
journal, April 1973

  • Morgan, Wayne E.; Stec, Wojciech J.; Van Wazer, John R.
  • Inorganic Chemistry, Vol. 12, Issue 4
  • DOI: 10.1021/ic50122a054

Synthesis and x-ray characterization of sputtered bi-alkali antimonide photocathodes
journal, November 2017

  • Gaowei, M.; Ding, Z.; Schubert, S.
  • APL Materials, Vol. 5, Issue 11
  • DOI: 10.1063/1.5010950

X‐ray photoemission studies of superficially oxidized cesium antimonide photoemitters
journal, March 1981

  • Bates, C. W.; van Atekum, Th. M.; Wertheim, G. K.
  • Applied Physics Letters, Vol. 38, Issue 5
  • DOI: 10.1063/1.92348

Transfer of CVD-Grown Monolayer Graphene onto Arbitrary Substrates
journal, August 2011

  • Suk, Ji Won; Kitt, Alexander; Magnuson, Carl W.
  • ACS Nano, Vol. 5, Issue 9
  • DOI: 10.1021/nn201207c

The effects of oxygen-induced phase segregation on the interfacial electronic structure and quantum efficiency of Cs 3 Sb photocathodes
journal, October 2020

  • Galdi, Alice; DeBenedetti, William J. I.; Balajka, Jan
  • The Journal of Chemical Physics, Vol. 153, Issue 14
  • DOI: 10.1063/5.0024020

Protection of cesium-antimony photocathodes
journal, March 1997

  • Buzulutskov, A.; Breskin, A.; Chechik, R.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 387, Issue 1-2
  • DOI: 10.1016/s0168-9002(96)00984-9

Fine Structure Constant Defines Visual Transparency of Graphene
journal, June 2008