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An Effective Purification Process for the Nuclear Radiation Detector Tl6SeI4
journal contribution
posted on 2018-04-18, 00:00 authored by Wenwen Lin, Oleg Y. Kontsevoi, Zhifu Liu, Sanjib Das, Yihui He, Yadong Xu, Constantinos C. Stoumpos, Kyle M. McCall, Alexander J. E. Rettie, Duck Young Chung, Bruce W. Wessels, Mercouri G. KanatzidisThe
semiconductor Tl6SeI4 was previously
identified as a promising semiconductor for room temperature nuclear
radiation detection. As the detection performance and carrier transport
strongly depend on the concentration of impurity energy levels acting
as scattering centers and carrier trapping, material purification
is a crucial prerequisite step to obtain spectroscopic-grade detector
performance. In this contribution, we present a highly efficient purification
method using a bent ampule for evaporating Se, Tl2Se, and
TlI precursors for Tl6SeI4. On the basis of
impurity analysis performed by glow discharge mass spectroscopy, the
main impurities in Tl2Se were identified to be Pb, Bi,
and Al, while in TlI the main impurities are Al and Sn. The bent-ampule
method successfully reduces or removes the Cl, Pb, and Te impurities
from the Se precursor, the Pb, Bi, and Al impurities from the Tl2Se precursor, and removes Sn from TlI. Informed by the analysis
results, density functional theory calculations were performed to
study the identified impurities and related defects. The calculation
results show that Bi and Al act as deep defect levels, which can be
detrimental to the detector performance of Tl6SeI4. If the growth condition of Tl6SeI4 is Tl-rich/Se-poor,
impurity of Si can introduce deep donors. However, it becomes electrically
benign if growth conditions are Tl-poor/Se-rich, while Sn and Pb impurities
are shallow donors. Centimeter-size Tl6SeI4 crystals
were grown by the two-zone vertical Bridgman method using the purified
precursors. The detector made of Tl6SeI4 crystal
maintains the high resistivity on the order of 1011 Ω·cm
after purification, ideal for suppressing leakage current. The detector
exhibits both full-energy and Tl escape photopeaks upon 122 keV γ-ray
from 57Co radiation source. The electron mobility-lifetime
product μeτe for Tl6SeI4 detector is 8.1 × 10–5 cm2·V–1. On the basis of the carrier rise time
measured from output pulses induced by 5.5 MeV α-particles from 241Am, the electron and hole mobilities were estimated to be
112 ± 22 and 81 ± 16 cm2·V–1·s–1, respectively, comparable to those of
the leading detector materials HgI2 and TlBr. These results
validate the potential of this compound for hard radiation detection,
and the impurity analysis presented here allows future efforts to
focus on reducing the concentration of the identified impurities.
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Keywords
impurity analysis122 keV γ- raydetector materials HgI 2Tl 2 Se precursorsemiconductor Tl 6 SeI 4carrier rise timeTl 2 Seradiation detectionspectroscopic-grade detector performanceimpurity energy levelsTl 6 SeI 4 crystalcalculation results showCentimeter-size Tl 6 SeI 4 crystals5.5 MeV α- particlesTl 6 SeI 4Effective Purification ProcessTl 6 SeI 4 detector57 Co radiation sourceglow discharge mass spectroscopyNuclear Radiation Detector Tl 6 SeI 4electron mobility-lifetime product μ e τ e
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