skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Discrete Electronic Bands in Semiconductors and Insulators: Potential High-Light-Yield Scintillators

Abstract

Bulk semiconductors and insulators typically have continuous valence and conduction bands. In this paper, we show that valence and conduction bands of a multinary semiconductor or insulator can be split to narrow discrete bands separated by large energy gaps. This unique electronic structure is demonstrated by first-principles calculations in several quaternary elpasolite compounds, i.e., Cs 2NaInBr 6, Cs 2NaBiCl 6, and Tl 2NaBiCl 6. The narrow discrete band structure in these quaternary elpasolites is due to the large electronegativity difference among cations and the large nearest-neighbor distances in cation sublattices. We further use Cs 2NaInBr 6 as an example to show that the narrow bands can stabilize self-trapped and dopant-bound excitons (in which both the electron and the hole are strongly localized in static positions on adjacent sites) and promote strong exciton emission at room temperature. The discrete band structure should further suppress thermalization of hot carriers and may lead to enhanced impact ionization, which is usually considered inefficient in bulk semiconductors and insulators. Finally, these characteristics can enable efficient room-temperature light emission in low-gap scintillators and may overcome the light-yield bottleneck in current scintillator research.

Authors:
 [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division. Center for Radiation Detection Materials and Systems
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1185880
Alternate Identifier(s):
OSTI ID: 1182797
Grant/Contract Number:  
AC05-00OR22725; DEAC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Applied
Additional Journal Information:
Journal Volume: 3; Journal Issue: 5; Journal ID: ISSN 2331-7019
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Shi, Hongliang, and Du, Mao-Hua. Discrete Electronic Bands in Semiconductors and Insulators: Potential High-Light-Yield Scintillators. United States: N. p., 2015. Web. doi:10.1103/PhysRevApplied.3.054005.
Shi, Hongliang, & Du, Mao-Hua. Discrete Electronic Bands in Semiconductors and Insulators: Potential High-Light-Yield Scintillators. United States. doi:10.1103/PhysRevApplied.3.054005.
Shi, Hongliang, and Du, Mao-Hua. Tue . "Discrete Electronic Bands in Semiconductors and Insulators: Potential High-Light-Yield Scintillators". United States. doi:10.1103/PhysRevApplied.3.054005. https://www.osti.gov/servlets/purl/1185880.
@article{osti_1185880,
title = {Discrete Electronic Bands in Semiconductors and Insulators: Potential High-Light-Yield Scintillators},
author = {Shi, Hongliang and Du, Mao-Hua},
abstractNote = {Bulk semiconductors and insulators typically have continuous valence and conduction bands. In this paper, we show that valence and conduction bands of a multinary semiconductor or insulator can be split to narrow discrete bands separated by large energy gaps. This unique electronic structure is demonstrated by first-principles calculations in several quaternary elpasolite compounds, i.e., Cs2NaInBr6, Cs2NaBiCl6, and Tl2NaBiCl6. The narrow discrete band structure in these quaternary elpasolites is due to the large electronegativity difference among cations and the large nearest-neighbor distances in cation sublattices. We further use Cs2NaInBr6 as an example to show that the narrow bands can stabilize self-trapped and dopant-bound excitons (in which both the electron and the hole are strongly localized in static positions on adjacent sites) and promote strong exciton emission at room temperature. The discrete band structure should further suppress thermalization of hot carriers and may lead to enhanced impact ionization, which is usually considered inefficient in bulk semiconductors and insulators. Finally, these characteristics can enable efficient room-temperature light emission in low-gap scintillators and may overcome the light-yield bottleneck in current scintillator research.},
doi = {10.1103/PhysRevApplied.3.054005},
journal = {Physical Review Applied},
number = 5,
volume = 3,
place = {United States},
year = {2015},
month = {5}
}

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

Citation Metrics:
Cited by: 11 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

High Efficiency Carrier Multiplication in PbSe Nanocrystals: Implications for Solar Energy Conversion
journal, May 2004


Study of pure nai at room and liquid nitrogen temperatures
journal, August 2003

  • Moszynski, M.; Balcerzyk, M.; Czarnacki, W.
  • IEEE Transactions on Nuclear Science, Vol. 50, Issue 4
  • DOI: 10.1109/TNS.2003.815176

Luminescence and scintillation properties of the small band gap compound LaI3:Ce3+
journal, January 2005

  • Bessiere, A.; Dorenbos, P.; van Eijk, C. W. E.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 537, Issue 1-2, p. 22-26
  • DOI: 10.1016/j.nima.2004.07.224

Efficient Photochemical Water Splitting by a Chemically Modified n-TiO2
journal, September 2002


Novel γ- and X-ray scintillator research: on the emission wavelength, light yield and time response of Ce3+ doped halide scintillators
journal, January 2009

  • Birowosuto, M. D.; Dorenbos, P.
  • physica status solidi (a), Vol. 206, Issue 1, p. 9-20
  • DOI: 10.1002/pssa.200723669

Alkali halide crystals containing impurity ions with the ns2 ground-state electronic configuration†
journal, January 1991


Band Gap Narrowing of Titanium Oxide Semiconductors by Noncompensated Anion-Cation Codoping for Enhanced Visible-Light Photoactivity
journal, November 2009


Visible-Light Photocatalysis in Nitrogen-Doped Titanium Oxides
journal, July 2001


Intrinsic mechanism for the poor luminescence properties of quantum-box systems
journal, November 1991


Chemical trends of electronic and optical properties of ns 2 ions in halides
journal, January 2014


Crystal Scintillators
journal, January 1984


Energy resolution and non-proportionality of the light yield of pure CsI at liquid nitrogen temperatures
journal, January 2005

  • Moszyński, M.; Balcerzyk, M.; Czarnacki, W.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 537, Issue 1-2
  • DOI: 10.1016/j.nima.2004.08.043

Engineering the Electronic Band Structure for Multiband Solar Cells
journal, January 2011


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


Understanding intermediate-band solar cells
journal, February 2012

  • Luque, Antonio; Martí, Antonio; Stanley, Colin
  • Nature Photonics, Vol. 6, Issue 3
  • DOI: 10.1038/nphoton.2012.1

Optical and scintillation properties of pure and Ce3+-doped Cs2LiYCl6 and Li3YCl6:Ce3+ crystals
journal, October 1999


Current trends in scintillator detectors and materials
journal, July 2002

  • Moses, William W.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 487, Issue 1-2
  • DOI: 10.1016/S0168-9002(02)00955-5

S PECTROSCOPY AND H OT E LECTRON R ELAXATION D YNAMICS IN S EMICONDUCTOR Q UANTUM W ELLS AND Q UANTUM D OTS
journal, October 2001


Quasiparticle spectra, absorption spectra, and excitonic properties of NaI and SrI 2 from many-body perturbation theory
journal, February 2014


Electronic structure engineering of elpasolites: Case of Cs2AgYCl6
journal, November 2013


Highly Efficient Multiple Exciton Generation in Colloidal PbSe and PbS Quantum Dots
journal, May 2005

  • Ellingson, Randy J.; Beard, Matthew C.; Johnson, Justin C.
  • Nano Letters, Vol. 5, Issue 5, p. 865-871
  • DOI: 10.1021/nl0502672

Radiative and non-radiative inter-subband transition in self assembled quantum dots
journal, July 1998


Intermediate-band photovoltaic solar cell based on ZnTe:O
journal, July 2009

  • Wang, Weiming; Lin, Albert S.; Phillips, Jamie D.
  • Applied Physics Letters, Vol. 95, Issue 1
  • DOI: 10.1063/1.3166863

First-principles study of luminescence in Ce-doped inorganic scintillators
journal, March 2011


Assessment of correction methods for the band-gap problem and for finite-size effects in supercell defect calculations: Case studies for ZnO and GaAs
journal, December 2008


Towards the intermediate band
journal, February 2011


Crystal Growth and Scintillation Properties of Strontium Iodide Scintillators
journal, June 2009

  • van Loef, Edgar V.; Wilson, Cody M.; Cherepy, Nerine J.
  • IEEE Transactions on Nuclear Science, Vol. 56, Issue 3
  • DOI: 10.1109/TNS.2009.2013947

The optical properties of thallium-like impurities in alkali-halide crystals
journal, January 1983


Phonon scattering and energy relaxation in two-, one-, and zero-dimensional electron gases
journal, November 1990


Scintillation characteristics of pure and Tl-doped CsI crystals
journal, April 1990

  • Schotanus, P.; Kamermans, R.
  • IEEE Transactions on Nuclear Science, Vol. 37, Issue 2
  • DOI: 10.1109/23.106614

Rationale for mixing exact exchange with density functional approximations
journal, December 1996

  • Perdew, John P.; Ernzerhof, Matthias; Burke, Kieron
  • The Journal of Chemical Physics, Vol. 105, Issue 22, p. 9982-9985
  • DOI: 10.1063/1.472933

Crystal structure of Cs 2 NaBiCl 6
journal, February 1972


Scintillation mechanisms in Ce3+ doped halide scintillators
journal, January 2005


Spectroscopy and anomalous emission of Ce doped elpasolite Cs 2 LiY Cl 6
journal, March 2004

  • Bessière, A.; Dorenbos, P.; Eijk, C. W. E. van
  • Journal of Physics: Condensed Matter, Vol. 16, Issue 10
  • DOI: 10.1088/0953-8984/16/10/019

The synthesis and structures of complex rare-earth halides
journal, January 1982