Tan Ryan, Dryzhakov Bogdan, Higgins Kate, Charest Jessica, Dancoes Zachary, Kandlakunta Praneeth, Cao Lei R, Ahmadi Mahshid, Hu Bin, Lukosi Eric
Department of Nuclear Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States.
Institute for Advanced Materials & Manufacturing, University of Tennessee, Knoxville, Tennessee 37996, United States.
ACS Appl Mater Interfaces. 2022 Aug 3;14(30):34571-34582. doi: 10.1021/acsami.2c05024. Epub 2022 Jul 22.
Dual γ/neutron radiation sensors are a critical component of the nuclear security mission to prevent the proliferation of a special nuclear material (SNM). While high-performing semiconductors such as high purity germanium (HPGe) and CdZnTe (CZT) already exist in the nuclear security enterprise, their high cost and/or logistical burdens make widespread deployment difficult to achieve. Metal lead halide perovskites (MHPs) have attracted interest in recent years to address this challenge. In particular, methylammonium lead tribromide (CHNHPbBr, MAPbBr, or MAPB) has been widely evaluated for its radiation sensing capabilities. While previous studies have demonstrated low-energy X-ray and α particle sensing of MAPB-based detectors and several studies discuss the potential for γ ray sensing, neutron sensing of this material has been rarely explored. Here, we explore the incorporation of lithium in the form of LiCl into the MAPB structure to add thermal neutron sensitivity. Characterizations of the lithium-doped MAPB crystals demonstrate that quality growths are achievable with single crystals that exhibit high crystallinity, no phase change, and high macroscopic bulk quality. Finally, we report on the first demonstrated γ ray and thermal neutron sensing based on lithium-doped MAPB single crystals, which is a significant milestone in the development of 3D dual γ/neutron MHP sensors.
双γ/中子辐射传感器是防止特殊核材料(SNM)扩散的核安全任务的关键组成部分。虽然核安全领域已经存在诸如高纯度锗(HPGe)和碲锌镉(CZT)等高性能半导体,但它们的高成本和/或后勤负担使得难以实现广泛部署。近年来,金属卤化铅钙钛矿(MHP)已引起人们对解决这一挑战的关注。特别是,三溴化甲基铵铅(CH₃NH₃PbBr₃,MAPbBr₃或MAPB)因其辐射传感能力而受到广泛评估。虽然先前的研究已经证明了基于MAPB的探测器对低能X射线和α粒子的传感能力,并且有几项研究讨论了γ射线传感的潜力,但这种材料的中子传感很少被探索。在这里,我们探索以LiCl的形式将锂掺入MAPB结构中,以增加热中子敏感性。锂掺杂MAPB晶体的表征表明,高质量的生长可以通过具有高结晶度、无相变和高宏观整体质量的单晶来实现。最后,我们报告了首次基于锂掺杂MAPB单晶的γ射线和热中子传感,这是3D双γ/中子MHP传感器开发中的一个重要里程碑。