Materials for radiation detection are critically important and urgently demanded in diverse fields,starting from fundamental scientific research to medical diagnostics,homeland security,and environmental monitoring.Lo...Materials for radiation detection are critically important and urgently demanded in diverse fields,starting from fundamental scientific research to medical diagnostics,homeland security,and environmental monitoring.Lowdimensional halides(LDHs)exhibiting efficient self-trapped exciton(STE)emission with high photoluminescence quantum yield(PLQY)have recently shown a great potential as scintillators.However,an overlooked issue of excitonexciton interaction in LDHs under ionizing radiation hinders the broadening of its radiation detection applications.Here,we demonstrate an exceptional enhancement of exciton-harvesting efficiency in zero-dimensional(0D)Cs_(3)Cu_(2)I_(5):Tl halide single crystals by forming strongly localized Tl-bound excitons.Because of the suppression of nonradiative exciton-exciton interaction,an excellentα/βpulse-shape-discrimination(PSD)figure-of-merit(FoM)factor of 2.64,a superior rejection ratio of 10^(−9),and a high scintillation yield of 26000 photons MeV−1 under 5.49 MeVα-ray are achieved in Cs_(3)Cu_(2)I_(5):Tl single crystals,outperforming the commercial ZnS:Ag/PVT composites for charged particle detection applications.Furthermore,a radiation detector prototype based on Cs_(3)Cu_(2)I_(5):Tl single crystal demonstrates the capability of identifying radioactive 220Rn gas for environmental radiation monitoring applications.We believe that the exciton-harvesting strategy proposed here can greatly boost the applications of LDHs materials.展开更多
基金the following fundings for support:National Key R&D Program of China(2022YFB3503600)National Natural Science Foundation of China(11975303,12211530561,12305211)+3 种基金Shanghai Municipal Natural Science Foundation(20ZR1473900,21TS1400100)CAS Cooperative Research Project(121631KYSB20210017)CAS Project for Young Scientist in Basic Research(YSBR-024)Partial support received from OP Research,Development,and Education financed by European Structural and Investment Funds,(Czech MEYS project No.SOLID21 CZ.02.1.01/0.0/0.0/16_019/0000760).
文摘Materials for radiation detection are critically important and urgently demanded in diverse fields,starting from fundamental scientific research to medical diagnostics,homeland security,and environmental monitoring.Lowdimensional halides(LDHs)exhibiting efficient self-trapped exciton(STE)emission with high photoluminescence quantum yield(PLQY)have recently shown a great potential as scintillators.However,an overlooked issue of excitonexciton interaction in LDHs under ionizing radiation hinders the broadening of its radiation detection applications.Here,we demonstrate an exceptional enhancement of exciton-harvesting efficiency in zero-dimensional(0D)Cs_(3)Cu_(2)I_(5):Tl halide single crystals by forming strongly localized Tl-bound excitons.Because of the suppression of nonradiative exciton-exciton interaction,an excellentα/βpulse-shape-discrimination(PSD)figure-of-merit(FoM)factor of 2.64,a superior rejection ratio of 10^(−9),and a high scintillation yield of 26000 photons MeV−1 under 5.49 MeVα-ray are achieved in Cs_(3)Cu_(2)I_(5):Tl single crystals,outperforming the commercial ZnS:Ag/PVT composites for charged particle detection applications.Furthermore,a radiation detector prototype based on Cs_(3)Cu_(2)I_(5):Tl single crystal demonstrates the capability of identifying radioactive 220Rn gas for environmental radiation monitoring applications.We believe that the exciton-harvesting strategy proposed here can greatly boost the applications of LDHs materials.
