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Title: An unusual crystal growth method of the chalcohalide semiconductor, β-Hg 3S 2Cl 2: A new candidate for hard radiation detection

Here, we assess the mercury chalcohalide compound, β-Hg 3S 2Cl 2, as a potential semiconductor material for X-ray and γ-ray detection. It has a high density (6.80 g/cm 3) and wide band gap (2.56 eV) and crystallizes in the cubic Pm4$$\bar{3}$$n space group with a three-dimensional structure comprised of [Hg 12S 8] cubes with Cl atoms located within and between the cubes, featuring a trigonal pyramidal SHg3 as the main building block. First-principle electronic structure calculations at the density functional theory level predict that the compound has closely lying indirect and direct band gaps. We have successfully grown transparent, single crystals of β-Hg 3S 2Cl 2 up to 7 mm diameter and 1 cm long using a new approach by the partial decomposition of the quaternary Hg 3Bi 2S 2Cl 8 compound followed by the formation of β-Hg 3S 2Cl 2 and an impermeable top layer, all happening in situ during vertical Bridgman growth. The decomposition process was optimized by varying peak temperatures and temperature gradients using a 2 mm/h translation rate of the Bridgman technique. Formation of the quaternary Hg 3Bi 2S 2Cl 8 followed by its partial decomposition into β-Hg 3S 2Cl 2 was confirmed by in situ temperature-dependent synchrotron powder diffraction studies. The single crystal samples obtained had resistivity of 10 10 Ω·cm and mobility-lifetime products of electron and hole carriers of 1.4(4) × 10 –4 cm 2/V and 7.5(3) × 10 –5 cm 2/V, respectively. Further, an appreciable Ag X-ray photoconductivity response was observed showing the potential of β-Hg 3S 2Cl 2 as a hard radiation detector material.
Authors:
 [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [3] ;  [3] ;  [2]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
  3. Northwestern Univ., Evanston, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Crystal Growth and Design
Additional Journal Information:
Journal Volume: 16; Journal Issue: 5; Journal ID: ISSN 1528-7483
Publisher:
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation (NA-20)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Crystal growth; Mercury chalcohalide; Mobility-lifetime product; Semiconductor; X-ray detector; γ-ray Detector
OSTI Identifier:
1352554

Wibowo, Arief C., Malliakas, Christos D., Li, Hao, Stoumpos, Constantinos C., Chung, Duck Young, Wessels, Bruce W., Freeman, Arthur J., and Kanatzidis, Mercouri G.. An unusual crystal growth method of the chalcohalide semiconductor, β-Hg3S2Cl2: A new candidate for hard radiation detection. United States: N. p., Web. doi:10.1021/acs.cgd.5b01802.
Wibowo, Arief C., Malliakas, Christos D., Li, Hao, Stoumpos, Constantinos C., Chung, Duck Young, Wessels, Bruce W., Freeman, Arthur J., & Kanatzidis, Mercouri G.. An unusual crystal growth method of the chalcohalide semiconductor, β-Hg3S2Cl2: A new candidate for hard radiation detection. United States. doi:10.1021/acs.cgd.5b01802.
Wibowo, Arief C., Malliakas, Christos D., Li, Hao, Stoumpos, Constantinos C., Chung, Duck Young, Wessels, Bruce W., Freeman, Arthur J., and Kanatzidis, Mercouri G.. 2016. "An unusual crystal growth method of the chalcohalide semiconductor, β-Hg3S2Cl2: A new candidate for hard radiation detection". United States. doi:10.1021/acs.cgd.5b01802. https://www.osti.gov/servlets/purl/1352554.
@article{osti_1352554,
title = {An unusual crystal growth method of the chalcohalide semiconductor, β-Hg3S2Cl2: A new candidate for hard radiation detection},
author = {Wibowo, Arief C. and Malliakas, Christos D. and Li, Hao and Stoumpos, Constantinos C. and Chung, Duck Young and Wessels, Bruce W. and Freeman, Arthur J. and Kanatzidis, Mercouri G.},
abstractNote = {Here, we assess the mercury chalcohalide compound, β-Hg3S2Cl2, as a potential semiconductor material for X-ray and γ-ray detection. It has a high density (6.80 g/cm3) and wide band gap (2.56 eV) and crystallizes in the cubic Pm4$\bar{3}$n space group with a three-dimensional structure comprised of [Hg12S8] cubes with Cl atoms located within and between the cubes, featuring a trigonal pyramidal SHg3 as the main building block. First-principle electronic structure calculations at the density functional theory level predict that the compound has closely lying indirect and direct band gaps. We have successfully grown transparent, single crystals of β-Hg3S2Cl2 up to 7 mm diameter and 1 cm long using a new approach by the partial decomposition of the quaternary Hg3Bi2S2Cl8 compound followed by the formation of β-Hg3S2Cl2 and an impermeable top layer, all happening in situ during vertical Bridgman growth. The decomposition process was optimized by varying peak temperatures and temperature gradients using a 2 mm/h translation rate of the Bridgman technique. Formation of the quaternary Hg3Bi2S2Cl8 followed by its partial decomposition into β-Hg3S2Cl2 was confirmed by in situ temperature-dependent synchrotron powder diffraction studies. The single crystal samples obtained had resistivity of 1010 Ω·cm and mobility-lifetime products of electron and hole carriers of 1.4(4) × 10–4 cm2/V and 7.5(3) × 10–5 cm2/V, respectively. Further, an appreciable Ag X-ray photoconductivity response was observed showing the potential of β-Hg3S2Cl2 as a hard radiation detector material.},
doi = {10.1021/acs.cgd.5b01802},
journal = {Crystal Growth and Design},
number = 5,
volume = 16,
place = {United States},
year = {2016},
month = {3}
}