DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Effect of chlorination on the TlBr band edges for improved room temperature radiation detectors: Effect of chlorination on the TlBr band edges for radiation detectors

Abstract

Thallium bromide (TlBr) crystals subjected to hydrochloric acid (HCl) chemical treatments have been shown to advantageously affect device performance and longevity in TlBr-based room temperature radiation detectors, yet the exact mechanisms of the improvements remain poorly understood. Here in this paper, we investigate the influence of several HCl chemical treatments on device-grade TlBr and describe the changes in the composition and electronic structure of the surface. Composition analysis and depth profiles obtained from secondary ion mass spectrometry (SIMS) identify the extent to which each HCl etch condition affects the detector surface region and forms of a graded TlBr/TlBr1-xCLx surface heterojunction. Using a combination of X-ray photoemission spectroscopy (XPS) and hybrid density functional calculations, we are able to determine the valence band offsets, band gaps, and conduction band offsets as a function of Cl content over the entire composition range of TIBr1-xC1X. This study establishes a strong correlation between device process conditions, surface chemistry, and electronic structure with the goal of further optimizing the long-term stability and radiation response of TlBr-based detectors.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1418904
Report Number(s):
LLNL-JRNL-661938
Journal ID: ISSN 0370-1972
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Accepted Manuscript
Journal Name:
Physica Status Solidi B. Basic Solid State Physics
Additional Journal Information:
Journal Volume: 252; Journal Issue: 6; Journal ID: ISSN 0370-1972
Publisher:
Wiley-Blackwell
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY; density functional theory; radiation detector; surface treatment; thallium halide; X-ray photoemission spectroscopy

Citation Formats

Varley, J. B., Conway, A. M., Voss, L. F., Swanberg, E., Graff, R. T., Nikolic, R. J., Payne, S. A., Lordi, V., and Nelson, A. J. Effect of chlorination on the TlBr band edges for improved room temperature radiation detectors: Effect of chlorination on the TlBr band edges for radiation detectors. United States: N. p., 2015. Web. doi:10.1002/pssb.201451662.
Varley, J. B., Conway, A. M., Voss, L. F., Swanberg, E., Graff, R. T., Nikolic, R. J., Payne, S. A., Lordi, V., & Nelson, A. J. Effect of chlorination on the TlBr band edges for improved room temperature radiation detectors: Effect of chlorination on the TlBr band edges for radiation detectors. United States. https://doi.org/10.1002/pssb.201451662
Varley, J. B., Conway, A. M., Voss, L. F., Swanberg, E., Graff, R. T., Nikolic, R. J., Payne, S. A., Lordi, V., and Nelson, A. J. Mon . "Effect of chlorination on the TlBr band edges for improved room temperature radiation detectors: Effect of chlorination on the TlBr band edges for radiation detectors". United States. https://doi.org/10.1002/pssb.201451662. https://www.osti.gov/servlets/purl/1418904.
@article{osti_1418904,
title = {Effect of chlorination on the TlBr band edges for improved room temperature radiation detectors: Effect of chlorination on the TlBr band edges for radiation detectors},
author = {Varley, J. B. and Conway, A. M. and Voss, L. F. and Swanberg, E. and Graff, R. T. and Nikolic, R. J. and Payne, S. A. and Lordi, V. and Nelson, A. J.},
abstractNote = {Thallium bromide (TlBr) crystals subjected to hydrochloric acid (HCl) chemical treatments have been shown to advantageously affect device performance and longevity in TlBr-based room temperature radiation detectors, yet the exact mechanisms of the improvements remain poorly understood. Here in this paper, we investigate the influence of several HCl chemical treatments on device-grade TlBr and describe the changes in the composition and electronic structure of the surface. Composition analysis and depth profiles obtained from secondary ion mass spectrometry (SIMS) identify the extent to which each HCl etch condition affects the detector surface region and forms of a graded TlBr/TlBr1-xCLx surface heterojunction. Using a combination of X-ray photoemission spectroscopy (XPS) and hybrid density functional calculations, we are able to determine the valence band offsets, band gaps, and conduction band offsets as a function of Cl content over the entire composition range of TIBr1-xC1X. This study establishes a strong correlation between device process conditions, surface chemistry, and electronic structure with the goal of further optimizing the long-term stability and radiation response of TlBr-based detectors.},
doi = {10.1002/pssb.201451662},
journal = {Physica Status Solidi B. Basic Solid State Physics},
number = 6,
volume = 252,
place = {United States},
year = {Mon Feb 09 00:00:00 EST 2015},
month = {Mon Feb 09 00:00:00 EST 2015}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 3 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

X-ray photoelectron spectroscopy of thallium halide valence bands
journal, June 1978


The epitaxial growth of thallium on copper (100): A study by LEED, AES, UPS and EELS
journal, March 1982


Projector augmented-wave method
journal, December 1994


First-principles study of ternary bcc alloys using special quasi-random structures
journal, September 2009


Hybrid functionals based on a screened Coulomb potential
journal, May 2003

  • Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
  • The Journal of Chemical Physics, Vol. 118, Issue 18
  • DOI: 10.1063/1.1564060

Fabrication Methodology of Enhanced Stability Room Temperature TlBr Gamma Detectors
journal, April 2013

  • Conway, A. M.; Voss, L. F.; Nelson, A. J.
  • IEEE Transactions on Nuclear Science, Vol. 60, Issue 2
  • DOI: 10.1109/TNS.2013.2252363

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


Ionic current and polarization effect in TlBr
journal, February 2013


Characterization of ${\rm TlBr}_{\rm x}{\rm Cl}_{1\mathchar"702D {\rm x}}$ Crystals for Radiation Detectors
journal, August 2012

  • Onodera, Toshiyuki; Hitomi, Keitaro; Onodera, Chikara
  • IEEE Transactions on Nuclear Science, Vol. 59, Issue 4
  • DOI: 10.1109/TNS.2012.2200504

First-principles study of constitutional point defects in B2 NiAl using special quasirandom structures
journal, May 2005


Energy-band alignment of II-VI/Zn 3 P 2 heterojunctions from x-ray photoemission spectroscopy
journal, May 2013

  • Bosco, Jeffrey P.; Scanlon, David O.; Watson, Graeme W.
  • Journal of Applied Physics, Vol. 113, Issue 20
  • DOI: 10.1063/1.4807646

Experimental and theoretical study of the electronic structure of HgO and Tl 2 O 3
journal, June 2005


Electrical properties of point defects in CdS and ZnS
journal, September 2013

  • Varley, J. B.; Lordi, V.
  • Applied Physics Letters, Vol. 103, Issue 10
  • DOI: 10.1063/1.4819492

Influence of crystalline surface quality on TlBr radiation detector performance
journal, October 2005

  • Oliveira, I. B.; Costa, F. E.; Kiyohara, P. K.
  • IEEE Transactions on Nuclear Science, Vol. 52, Issue 5
  • DOI: 10.1109/TNS.2005.856788

Tin dioxide from first principles: Quasiparticle electronic states and optical properties
journal, January 2011


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Thallium Bromide Nuclear Radiation Detector Development
journal, August 2009

  • Churilov, Alexei V.; Ciampi, Guido; Kim, Hadong
  • IEEE Transactions on Nuclear Science, Vol. 56, Issue 4
  • DOI: 10.1109/TNS.2009.2021424

Investigation of pixelated TlBr gamma-ray spectrometers with the depth-sensing technique
journal, June 2008

  • Hitomi, Keitaro; Onodera, Toshiyuki; Shoji, Tadayoshi
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 591, Issue 1
  • DOI: 10.1016/j.nima.2008.03.086

Hydrogen Defect-Level Pinning in Semiconductors: The Muonium Equivalent
journal, September 2008


Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)]
journal, June 2006

  • Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
  • The Journal of Chemical Physics, Vol. 124, Issue 21
  • DOI: 10.1063/1.2204597

Point defects in Cd(Zn)Te and TlBr: Theory
journal, September 2013


Polarization Phenomena in TlBr Detectors
journal, August 2009

  • Hitomi, Keitaro; Kikuchi, Yohei; Shoji, Tadayoshi
  • IEEE Transactions on Nuclear Science, Vol. 56, Issue 4
  • DOI: 10.1109/TNS.2009.2013349

TlBr Gamma-Ray Spectrometers Using the Depth Sensitive Single Polarity Charge Sensing Technique
journal, June 2008

  • Hitomi, Keitaro; Onodera, Toshiyuki; Shoji, Tadayoshi
  • IEEE Transactions on Nuclear Science, Vol. 55, Issue 3
  • DOI: 10.1109/TNS.2008.924086

Developing Larger TlBr Detectors—Detector Performance
journal, June 2009

  • Kim, H.; Cirignano, L.; Churilov, A.
  • IEEE Transactions on Nuclear Science, Vol. 56, Issue 3
  • DOI: 10.1109/TNS.2009.2014756

X-ray photoemission analysis of chemically modified TlBr surfaces for improved radiation detectors
journal, April 2013

  • Nelson, A. J.; Voss, L. F.; Beck, P. R.
  • Journal of Applied Physics, Vol. 113, Issue 14
  • DOI: 10.1063/1.4801793

Universal alignment of hydrogen levels in semiconductors and insulators
journal, April 2006


Universal alignment of hydrogen levels in semiconductors, insulators and solutions
journal, June 2003


Spectroscopie photoelectronique ESCA (XPS) de chalcogenures de thallium
journal, November 1980


High-resolution X-ray luminescence extension imaging
journal, February 2021


Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect
journal, February 2020


The epitaxial growth of thallium on copper (100): A study by LEED, AES, UPS and EELS
journal, March 1982


Polarization phenomena in TlBr detectors
conference, October 2008

  • Hitomi, Keitaro; Kikuchi, Yohei; Shoji, Tadayoshi
  • 2008 IEEE Nuclear Science Symposium and Medical Imaging conference (2008 NSS/MIC), 2008 IEEE Nuclear Science Symposium Conference Record
  • DOI: 10.1109/nssmic.2008.4775149