Phase-Control of Single-Crystalline Inorganic Halide Perovskites via Molecular Coordination Engineering

Lin Qingdong; Bernardi Stefano; Shabbir BabarOu QingdongWang MingchaoYin WenpingLiu ShiqiChesman Anthony S. R.Furer Sebastian O.Si GuangyuanMedhekar NikhilJasieniak JacekWidmer-Cooper AsaphMao WenxinBach Udo

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Phase-Control of Single-Crystalline Inorganic Halide Perovskites via Molecular Coordination Engineering

机译：Phase-Control of Single-Crystalline Inorganic Halide Perovskites via Molecular Coordination Engineering

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The excellent optoelectronic properties and structural stability of inorganic cesium lead halide perovskites make them promising candidates for multiple types of optoelectronic devices. However, it remains a challenge to fabricate monocrystalline phase-pure perovskite microstructures by facile low-temperature solution-based methods. Herein, a solution-based method is demonstrated for controlling the crystallization of cesium halide perovskite microstructures. The structure of perovskite crystals is successfully tuned from non-corner sharing Cs4PbBr6 (0D) to corner-sharing CsPbBr3 (3D) to layered CsPb2Br5 (2D) by controlling water (H2O) to dimethylsulfoxide (DMSO) ratios. Molecular dynamics simulations and thermodynamic analysis indicate that the relative stability of Pb2+ and Br- ions in solution is the key factor in determining which crystals form at different H2O/DMSO ratios, with Cs+ simply incorporated as needed. The phase-pure 0D crystals exhibit a high photoluminescence quantum yield of 41, whilst the 2D crystals have an onset of absorption at 350 nm. Furthermore, the as-synthesized, highly uniform 3D perovskite single crystals are coupled with nanofabricated interdigitated electrodes to show excellent X-ray detection, with a high sensitivity of 8000 mu C Gy(air)(-1)cm(-2) obtained under a 0.5V external bias. This is comparable to many commercial X-ray detectors (Si, alpha-Se) and several times higher than other reported inorganic perovskite materials (CsPbBr3 quantum dots, Cs2AgBiBr6).

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《Advanced functional materials》 |2022年第16期|2109442.1-2109442.10|共10页
作者
Lin Qingdong; Bernardi Stefano; Shabbir BabarOu QingdongWang MingchaoYin WenpingLiu ShiqiChesman Anthony S. R.Furer Sebastian O.Si GuangyuanMedhekar NikhilJasieniak JacekWidmer-Cooper AsaphMao WenxinBach Udo;
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作者单位

Monash Univ, ARC Ctr Excellence Exciton Sci, Clayton, Vic 3800, Australia|Monash Univ, Dept Mat Sci & Engn, Clayton, Vic 3800, Australia;

Monash Univ, Dept Mat Sci & Engn, Clayton, Vic 3800, Australia;

CSIRO, CSIRO Mfg, Clayton, Vic 3168, Australia|Melbourne Ctr Nanofabricat, Victorian Node Australian Natl Fabricat, Clayton, Vic 3168, AustraliaMonash Univ, Dept Chem Engn, Clayton, Vic 3800, Australia|Monash Univ, ARC Ctr Excellence Exciton Sci, Clayton, Vic 3800, AustraliaCSIRO, CSIRO Mfg, Clayton, Vic 3168, AustraliaUniv Sydney, Sch Chem, Sydney, NSW 2006, Australia|Univ Sydney, ARC Ctr Excellence Exciton Sci, Sydney, NSW 2006, Australia|Univ Sydney, Nano Inst, Sydney, NSW 2006, AustraliaMonash Univ, Dept Chem Engn, Clayton, Vic 3800, Australia|Monash Univ, ARC Ctr Excellence Exciton Sci, Clayton, Vic 3800, Australia|Monash Univ, Australian Ctr Adv Photovolta ACAP, Clayton, Vic 3800, Australia;

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正文语种英语
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molecular dynamic simulation; perovskite; phase transformation; single crystals; X-ray detector;

Phase-Control of Single-Crystalline Inorganic Halide Perovskites via Molecular Coordination Engineering

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