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Role of Stoichiometry in the Growth of Large Pb2P2Se6 Crystals for Nuclear Radiation Detection
ACS Photonics ( IF 6.5 ) Pub Date : 2017-12-05 00:00:00 , DOI: 10.1021/acsphotonics.7b01119 Yadong Xu 1 , Xu Fu 1 , Hongjian Zheng 1 , Yihui He , Wenwen Lin , Kyle M. McCall , Zhifu Liu , Sanjib Das , Bruce W. Wessels , Mercouri G. Kanatzidis
ACS Photonics ( IF 6.5 ) Pub Date : 2017-12-05 00:00:00 , DOI: 10.1021/acsphotonics.7b01119 Yadong Xu 1 , Xu Fu 1 , Hongjian Zheng 1 , Yihui He , Wenwen Lin , Kyle M. McCall , Zhifu Liu , Sanjib Das , Bruce W. Wessels , Mercouri G. Kanatzidis
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Pb2P2Se6 as a heavy element, chemically robust semiconductor, has been identified as a promising material for cost-effective room temperature X/γ-ray detection. Here, we report the properties of Pb2P2Se6 crystals grown by a vertical Bridgman method under off-stoichiometric Se-rich and Pb-rich conditions. Regardless of the conditions the resulting single crystals exhibited high bulk resistivity on the order of 1011 Ω·cm. However, the photoconductivity and charge transport properties varied based on growth condition indicating the different dominant defects associated with the type of stoichiometric deviation. The formation and nature of intrinsic defects in Pb2P2Se6 crystals were also studied by first-principles density functional theory (DFT) calculations as well as thermally stimulated current (TSC) spectroscopy. The TSC results indicated that four traps were common to both Se-rich and Pb-rich Pb2P2Se6, while a higher density of shallow defects were observed in Se-rich Pb2P2Se6. DFT calculations predict that the antisite defects PPb+, PSe– and PbP– are the dominant deep donors and acceptors in Se-rich and Pb-rich Pb2P2Se6, respectively, which leads to the degradation of mobility lifetime product (μτ) on the order of 10–5 cm2·V–1 as measured under 241Am (5.48 MeV) alpha particles irradiation. Nevertheless, Pb2P2Se6 detectors with a thickness of 2 mm show reliable linear response under a series of radiation sources, including 241Am and 57Co γ-ray sources. A high X-ray sensitivity comparable to that of amorphous Se for Pb-rich Pb2P2Se6 detectors was realized, with the value of 68.3 μC·Gyair–1 cm–2 under 40 kVp Ag X-rays at an electrical field of 50 V·cm–1.
中文翻译：
化学计量在核辐射检测用大Pb 2 P 2 Se 6晶体生长中的作用
Pb 2 P 2 Se 6作为重元素，化学上稳健的半导体，已被确定为具有成本效益的室温X /γ射线检测的有前途的材料。在这里，我们报告了在垂直化学计量的富硒和富铅条件下通过垂直Bridgman方法生长的Pb 2 P 2 Se 6晶体的性能。不论条件如何，所得的单晶均表现出约10 11的高体电阻率Ω·cm。然而，光电导率和电荷传输性质根据生长条件而变化，这表明与化学计量偏差类型相关的不同主要缺陷。还通过第一原理密度泛函理论（DFT）计算以及热激电流（TSC）光谱研究了Pb 2 P 2 Se 6晶体中固有缺陷的形成和性质。的TSC结果表明，4个陷阱是共同的富硒和富铅的Pb既2 P 2硒6，而浅的缺陷的较高密度在富硒铅观察2 P 2硒6。DFT计算预测，反位缺陷P的Pb +，P硒-和Pb P -是占主导地位的深施主和受主在富硒和Pb-富铅2 P 2硒6分别，这导致流动性寿命的劣化在241 Am（5.48 MeV）α粒子辐照下测得的乘积（μ）约为10 –5 cm 2 ·V –1。尽管如此，厚度为2 mm的Pb 2 P 2 Se 6检测器在一系列辐射源（包括241 Am和57 Coγ射线源。对于富Pb 2 P 2 Se 6探测器，实现了与非晶态硒相当的高X射线敏感性，在40 kVp Ag X射线下，在电气条件下其值为68.3μC·Gy空气–1 cm –2 50 V·cm –1的电场。
更新日期：2017-12-05
中文翻译：
化学计量在核辐射检测用大Pb 2 P 2 Se 6晶体生长中的作用
Pb 2 P 2 Se 6作为重元素，化学上稳健的半导体，已被确定为具有成本效益的室温X /γ射线检测的有前途的材料。在这里，我们报告了在垂直化学计量的富硒和富铅条件下通过垂直Bridgman方法生长的Pb 2 P 2 Se 6晶体的性能。不论条件如何，所得的单晶均表现出约10 11的高体电阻率Ω·cm。然而，光电导率和电荷传输性质根据生长条件而变化，这表明与化学计量偏差类型相关的不同主要缺陷。还通过第一原理密度泛函理论（DFT）计算以及热激电流（TSC）光谱研究了Pb 2 P 2 Se 6晶体中固有缺陷的形成和性质。的TSC结果表明，4个陷阱是共同的富硒和富铅的Pb既2 P 2硒6，而浅的缺陷的较高密度在富硒铅观察2 P 2硒6。DFT计算预测，反位缺陷P的Pb +，P硒-和Pb P -是占主导地位的深施主和受主在富硒和Pb-富铅2 P 2硒6分别，这导致流动性寿命的劣化在241 Am（5.48 MeV）α粒子辐照下测得的乘积（μ）约为10 –5 cm 2 ·V –1。尽管如此，厚度为2 mm的Pb 2 P 2 Se 6检测器在一系列辐射源（包括241 Am和57 Coγ射线源。对于富Pb 2 P 2 Se 6探测器，实现了与非晶态硒相当的高X射线敏感性，在40 kVp Ag X射线下，在电气条件下其值为68.3μC·Gy空气–1 cm –2 50 V·cm –1的电场。
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