TlSn2I5, a Robust Halide Antiperovskite Semiconductor for γ-Ray Detection at Room Temperature

Lin, Wenwen; Stoumpos, Constantinos C.; Liu, Zhifu; Das, Sanjib; Kontsevoi, Oleg Y.; He, Yihui; Malliakas, Christos D.; Chen, Haijie; Wessels, Bruce W.; Kanatzidis, Mercouri G.

doi:10.1021/acsphotonics.7b00388

Title: TlSn₂I₅, a Robust Halide Antiperovskite Semiconductor for γ-Ray Detection at Room Temperature

Abstract

The semiconductor TlSn₂I₅ with a two-dimensional crystal structure and an antiperovskite topology is a promising novel detection material. The compound crystallizes in the I4/mcm space group, has an indirect band gap of 2.14 eV, and melts congruently at 314 °C. Electronic band structure calculations reveal that the most facile electron transport is along the ab layered plane. Compared to CH₃NH₃PbX₃ (X = Br, I), TlSn₂I₅ features higher long-term stability, higher photon stopping power (average atomic number of 55), higher resistivity (~10¹⁰ Ω·cm), and robust mechanical properties. Centimeter-size TlSn₂I₅ single crystals grown from the melt by the Bridgman method can be used to fabricate detector devices, which detect Ag Kα X-rays (22 keV), ⁵⁷Co γ-rays (122 keV), and ²⁴¹Am α-particles (5.5 MeV). The mobility-lifetime product and mobility for electrons were estimated to be 1.1 × 10^-3 cm²·V^-1 and 94 ± 16 cm²·V^-1·s^-1, respectively. Unlike other halide perovskites, TlSn₂I₅ shows no signs of ionic polarization under long-term, high-voltage bias.

Authors:

Lin, Wenwen ^[1];

^[1]; Liu, Zhifu ^[2];

^[2]; Kontsevoi, Oleg Y. ^[3]; He, Yihui ^[1]; Malliakas, Christos D. ^[1]; Chen, Haijie ^[1];

^[2];

^[1]

Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
Northwestern Univ., Evanston, IL (United States). Dept. of Physics and Astronomy

Publication Date:: Fri Jun 23 00:00:00 EDT 2017

Research Org.:: Northwestern Univ., Evanston, IL (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC)

OSTI Identifier:: 1494820

Alternate Identifier(s):: OSTI ID: 1488927

Grant/Contract Number:: NA0002522; 2014-DN-077-ARI086-01; AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: ACS Photonics

Additional Journal Information:: Journal Volume: 4; Journal Issue: 7; Journal ID: ISSN 2330-4022

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; hard radiation detection; γ-ray; crystal growth; semiconductor detector; halide perovskite and photon detection; halide perovskite; photon detection

Citation Formats


                    Lin, Wenwen, Stoumpos, Constantinos C., Liu, Zhifu, Das, Sanjib, Kontsevoi, Oleg Y., He, Yihui, Malliakas, Christos D., Chen, Haijie, Wessels, Bruce W., and Kanatzidis, Mercouri G. TlSn2I5, a Robust Halide Antiperovskite Semiconductor for γ-Ray Detection at Room Temperature.  United States: N. p., 2017. 
Web.  doi:10.1021/acsphotonics.7b00388.

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                    Lin, Wenwen, Stoumpos, Constantinos C., Liu, Zhifu, Das, Sanjib, Kontsevoi, Oleg Y., He, Yihui, Malliakas, Christos D., Chen, Haijie, Wessels, Bruce W., & Kanatzidis, Mercouri G. TlSn2I5, a Robust Halide Antiperovskite Semiconductor for γ-Ray Detection at Room Temperature.  United States.  https://doi.org/10.1021/acsphotonics.7b00388

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                    Lin, Wenwen, Stoumpos, Constantinos C., Liu, Zhifu, Das, Sanjib, Kontsevoi, Oleg Y., He, Yihui, Malliakas, Christos D., Chen, Haijie, Wessels, Bruce W., and Kanatzidis, Mercouri G. Fri .  
"TlSn2I5, a Robust Halide Antiperovskite Semiconductor for γ-Ray Detection at Room Temperature".  United States.  https://doi.org/10.1021/acsphotonics.7b00388.  https://www.osti.gov/servlets/purl/1494820.

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@article{osti_1494820,

  title        = {TlSn2I5, a Robust Halide Antiperovskite Semiconductor for γ-Ray Detection at Room Temperature},

  author       = {Lin, Wenwen and Stoumpos, Constantinos C. and Liu, Zhifu and Das, Sanjib and Kontsevoi, Oleg Y. and He, Yihui and Malliakas, Christos D. and Chen, Haijie and Wessels, Bruce W. and Kanatzidis, Mercouri G.},

  abstractNote = {The semiconductor TlSn2I5 with a two-dimensional crystal structure and an antiperovskite topology is a promising novel detection material. The compound crystallizes in the I4/mcm space group, has an indirect band gap of 2.14 eV, and melts congruently at 314 °C. Electronic band structure calculations reveal that the most facile electron transport is along the ab layered plane. Compared to CH3NH3PbX3 (X = Br, I), TlSn2I5 features higher long-term stability, higher photon stopping power (average atomic number of 55), higher resistivity (~1010 Ω·cm), and robust mechanical properties. Centimeter-size TlSn2I5 single crystals grown from the melt by the Bridgman method can be used to fabricate detector devices, which detect Ag Kα X-rays (22 keV), 57Co γ-rays (122 keV), and 241Am α-particles (5.5 MeV). The mobility-lifetime product and mobility for electrons were estimated to be 1.1 × 10-3 cm2·V-1 and 94 ± 16 cm2·V-1·s-1, respectively. Unlike other halide perovskites, TlSn2I5 shows no signs of ionic polarization under long-term, high-voltage bias.},

  doi          = {10.1021/acsphotonics.7b00388},

  journal      = {ACS Photonics},

  number       = 7,

  volume       = 4,

  place        = {United States},

  year         = {Fri Jun 23 00:00:00 EDT 2017},

  month        = {Fri Jun 23 00:00:00 EDT 2017}

}

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Title: TlSn2I5, a Robust Halide Antiperovskite Semiconductor for γ-Ray Detection at Room Temperature

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Citation Formats

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Advances in the crystal growth and device fabrication technology of CdZnTe room temperature radiation detectors journal, June 2004

Thallium Bromide Nuclear Radiation Detector Development journal, August 2009

TlBr and TlBrxI1−x crystals for γ-ray detectors journal, April 2010

Purification, crystal growth and detector performance of TlBr conference, August 2008

Developing Larger TlBr Detectors—Detector Performance journal, June 2009

Advances in TlBr detector development journal, September 2013

Improved method for HgI2 crystal growth and detector fabrication journal, February 1996

Growth of PBI2 single crystals from stoichiometric and Pb excess melts journal, January 2008

Improved growth of PbI2 single crystals journal, March 2007

Halide Perovskites: Poor Man's High-Performance Semiconductors journal, May 2016

Crystal Growth of the Perovskite Semiconductor CsPbBr 3 : A New Material for High-Energy Radiation Detection journal, June 2013

Sensitive X-ray detectors made of methylammonium lead tribromide perovskite single crystals journal, March 2016

Detection of gamma photons using solution-grown single crystals of hybrid lead halide perovskites journal, July 2016

Electron-hole diffusion lengths > 175 μm in solution-grown CH 3 NH 3 PbI 3 single crystals journal, January 2015

Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals journal, January 2015

Methylammonium Lead Iodide for Efficient X-ray Energy Conversion journal, November 2015

Detection of X-ray photons by solution-processed lead halide perovskites journal, May 2015

Semiconducting Tin and Lead Iodide Perovskites with Organic Cations: Phase Transitions, High Mobilities, and Near-Infrared Photoluminescent Properties journal, July 2013

Calculation of Photon Mass Energy-Transfer and Mass Energy-Absorption Coefficients journal, November 1993

A Study on AB2X5 Compounds (A: K, In, Tl; B: Sr, Sn, Pb; X: Cl, Br, I) journal, May 1986

Zur Neuuntersuchung des Phasendiagramms TlI?SnI2 journal, February 1992

Certain Physical Properties of Single Crystals of Tungsten, Antimony, Bismuth, Tellurium, Cadmium, Zinc, and Tin journal, January 1925

Electron-Hole-Pair Creation Energies in Semiconductors journal, December 1975

Point Defects in Oxides: Tailoring Materials Through Defect Engineering journal, August 2011

The Renaissance of Halide Perovskites and Their Evolution as Emerging Semiconductors journal, September 2015

Crystal growth, upconversion, and infrared emission properties of Er3+-doped KPb2Br5 journal, May 2005

Electronic structure and fundamental absorption edges of KPb2Br5, K0.5Rb0.5Pb2Br5, and RbPb2Br5 single crystals journal, May 2012

Optical pump-probe processes in Nd^3+-doped KPb2Br5, RbPb2Br5, and KPb2Cl5 journal, January 2005

Inorganic Double Helices in Semiconducting SnIP journal, September 2016

Stability of Metal Halide Perovskite Solar Cells journal, September 2015

Zum Mechanismus des lichtelektrischen Prim�rstromes in isolierenden Kristallen journal, March 1932

Nature of polarization in wide-bandgap semiconductor detectors under high-flux irradiation: Application to semi-insulating Cd 1 − x Zn x Te journal, January 2008

Time of flight experimental studies of CdZnTe radiation detectors journal, June 2000

Dimensional Reduction: A Design Tool for New Radiation Detection Materials journal, August 2011

Investigation of Semi-Insulating Cs 2 Hg 6 S 7 and Cs 2 Hg 6-x Cd x S 7 Alloy for Hard Radiation Detection journal, October 2014

CsCdInQ 3 (Q = Se, Te): New Photoconductive Compounds As Potential Materials for Hard Radiation Detection journal, May 2013

Photo-induced current transient spectroscopy of single crystal Tl 6 I 4 Se journal, August 2014

Cs 2 M II M IV 3 Q 8 (Q = S, Se, Te): An Extensive Family of Layered Semiconductors with Diverse Band Gaps journal, August 2013

Photoconductivity in Tl 6 SI 4 : A Novel Semiconductor for Hard Radiation Detection journal, July 2013

Refined Synthesis and Crystal Growth of Pb 2 P 2 Se 6 for Hard Radiation Detectors journal, August 2016

Hard Radiation Detection from the Selenophosphate Pb 2 P 2 Se 6 journal, July 2015

Crystal Growth of Tl 4 CdI 6 : A Wide Band Gap Semiconductor for Hard Radiation Detection journal, March 2014

Photoconductivity in the Chalcohalide Semiconductor, SbSeI: a New Candidate for Hard Radiation Detection journal, May 2013

Charge Transport and Observation of Persistent Photoconductivity in Tl 6 SeI 4 Single Crystals journal, March 2017

Photoluminescence fatigue and inhomogeneous line broadening in semi-insulating Tl 6 SeI 4 single crystals journal, April 2016

Impurity-induced deep centers in Tl 6 SI 4 journal, April 2017

A short history of SHELX journal, December 2007

Projector augmented-wave method journal, December 1994

Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium journal, May 1994

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

Generalized Gradient Approximation Made Simple journal, October 1996

Structure–Band Gap Relationships in Hexagonal Polytypes and Low-Dimensional Structures of Hybrid Tin Iodide Perovskites journal, December 2016

Deep Level and Near-Band-Edge Recombination in Semiconducting Antiperovskite Hg 3 Se 2 I 2 Single Crystals journal, September 2018

Carrier recombination mechanism in CsPbB r 3 revealed by time-resolved photoluminescence spectroscopy journal, December 2019

Photophysical Pathways in Highly Sensitive Cs 2 AgBiBr 6 Double-Perovskite Single-Crystal X-Ray Detectors journal, September 2018

Room temperature semiconductor detectors for nuclear security journal, July 2019

Title: TlSn₂I₅, a Robust Halide Antiperovskite Semiconductor for γ-Ray Detection at Room Temperature

LaBr3:Ce crystal: The latest advance for scintillation cameras
journal, March 2007

Compound semiconductor radiation detectors
journal, September 2004

Progress in compound semiconductors
conference, March 2003

Room-temperature compound semiconductor radiation detectors
journal, August 1997

A Prototype Three-Dimensional Position Sensitive CdZnTe Detector Array
journal, August 2007

Advances in the crystal growth and device fabrication technology of CdZnTe room temperature radiation detectors
journal, June 2004

Thallium Bromide Nuclear Radiation Detector Development
journal, August 2009

TlBr and TlBrxI1−x crystals for γ-ray detectors
journal, April 2010

Purification, crystal growth and detector performance of TlBr
conference, August 2008

Developing Larger TlBr Detectors—Detector Performance
journal, June 2009

Advances in TlBr detector development
journal, September 2013

Improved method for HgI2 crystal growth and detector fabrication
journal, February 1996

Growth of PBI2 single crystals from stoichiometric and Pb excess melts
journal, January 2008

Improved growth of PbI2 single crystals
journal, March 2007

Halide Perovskites: Poor Man's High-Performance Semiconductors
journal, May 2016

Crystal Growth of the Perovskite Semiconductor CsPbBr ₃ : A New Material for High-Energy Radiation Detection
journal, June 2013

Sensitive X-ray detectors made of methylammonium lead tribromide perovskite single crystals
journal, March 2016

Detection of gamma photons using solution-grown single crystals of hybrid lead halide perovskites
journal, July 2016

Electron-hole diffusion lengths > 175 μm in solution-grown CH ₃ NH ₃ PbI ₃ single crystals
journal, January 2015

Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals
journal, January 2015

Methylammonium Lead Iodide for Efficient X-ray Energy Conversion
journal, November 2015

Detection of X-ray photons by solution-processed lead halide perovskites
journal, May 2015

Semiconducting Tin and Lead Iodide Perovskites with Organic Cations: Phase Transitions, High Mobilities, and Near-Infrared Photoluminescent Properties
journal, July 2013

Calculation of Photon Mass Energy-Transfer and Mass Energy-Absorption Coefficients
journal, November 1993

A Study on AB2X5 Compounds (A: K, In, Tl; B: Sr, Sn, Pb; X: Cl, Br, I)
journal, May 1986

Zur Neuuntersuchung des Phasendiagramms TlI?SnI2
journal, February 1992

Certain Physical Properties of Single Crystals of Tungsten, Antimony, Bismuth, Tellurium, Cadmium, Zinc, and Tin
journal, January 1925

Electron-Hole-Pair Creation Energies in Semiconductors
journal, December 1975

Point Defects in Oxides: Tailoring Materials Through Defect Engineering
journal, August 2011

The Renaissance of Halide Perovskites and Their Evolution as Emerging Semiconductors
journal, September 2015

Crystal growth, upconversion, and infrared emission properties of Er3+-doped KPb2Br5
journal, May 2005

Electronic structure and fundamental absorption edges of KPb2Br5, K0.5Rb0.5Pb2Br5, and RbPb2Br5 single crystals
journal, May 2012

Optical pump-probe processes in Nd^3+-doped KPb2Br5, RbPb2Br5, and KPb2Cl5
journal, January 2005

Inorganic Double Helices in Semiconducting SnIP
journal, September 2016

Stability of Metal Halide Perovskite Solar Cells
journal, September 2015

Zum Mechanismus des lichtelektrischen Prim�rstromes in isolierenden Kristallen
journal, March 1932

Nature of polarization in wide-bandgap semiconductor detectors under high-flux irradiation: Application to semi-insulating ${Cd}_{1 - x} {Zn}_{x} Te$
journal, January 2008

Time of flight experimental studies of CdZnTe radiation detectors
journal, June 2000

Dimensional Reduction: A Design Tool for New Radiation Detection Materials
journal, August 2011

Investigation of Semi-Insulating Cs ₂ Hg ₆ S ₇ and Cs ₂ Hg _6-x Cd _x S ₇ Alloy for Hard Radiation Detection
journal, October 2014

CsCdInQ ₃ (Q = Se, Te): New Photoconductive Compounds As Potential Materials for Hard Radiation Detection
journal, May 2013

Photo-induced current transient spectroscopy of single crystal Tl ₆ I ₄ Se
journal, August 2014

Cs ₂ M ^II M ^IV ₃ Q ₈ (Q = S, Se, Te): An Extensive Family of Layered Semiconductors with Diverse Band Gaps
journal, August 2013

Photoconductivity in Tl ₆ SI ₄ : A Novel Semiconductor for Hard Radiation Detection
journal, July 2013

Refined Synthesis and Crystal Growth of Pb ₂ P ₂ Se ₆ for Hard Radiation Detectors
journal, August 2016

Hard Radiation Detection from the Selenophosphate Pb ₂ P ₂ Se ₆
journal, July 2015

Crystal Growth of Tl ₄ CdI ₆ : A Wide Band Gap Semiconductor for Hard Radiation Detection
journal, March 2014

Photoconductivity in the Chalcohalide Semiconductor, SbSeI: a New Candidate for Hard Radiation Detection
journal, May 2013

Charge Transport and Observation of Persistent Photoconductivity in Tl ₆ SeI ₄ Single Crystals
journal, March 2017

Photoluminescence fatigue and inhomogeneous line broadening in semi-insulating Tl ₆ SeI ₄ single crystals
journal, April 2016

Impurity-induced deep centers in Tl ₆ SI ₄
journal, April 2017

A short history of SHELX
journal, December 2007

Projector augmented-wave method
journal, December 1994

Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium
journal, May 1994

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

Generalized Gradient Approximation Made Simple
journal, October 1996

Structure–Band Gap Relationships in Hexagonal Polytypes and Low-Dimensional Structures of Hybrid Tin Iodide Perovskites
journal, December 2016

Deep Level and Near-Band-Edge Recombination in Semiconducting Antiperovskite Hg ₃ Se ₂ I ₂ Single Crystals
journal, September 2018

Carrier recombination mechanism in $CsPbB r_{3}$ revealed by time-resolved photoluminescence spectroscopy
journal, December 2019

Photophysical Pathways in Highly Sensitive Cs ₂ AgBiBr ₆ Double-Perovskite Single-Crystal X-Ray Detectors
journal, September 2018

Room temperature semiconductor detectors for nuclear security
journal, July 2019