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Reversible Triple-Mode Photo- and Radioluminescence and Nonlinear Optical Switching in Highly Efficient 0D Hybrid Cuprous Halides
Chemistry of Materials ( IF 7.2 ) Pub Date : 2023-08-16 , DOI: 10.1021/acs.chemmater.3c00038 Dong-Yang Li 1, 2 , Jia-Hang Wu 3 , Xing-Yu Wang 1 , Xiao-Yang Zhang 1 , Cheng-Yang Yue 1, 2 , Xiao-Wu Lei 1, 2
Chemistry of Materials ( IF 7.2 ) Pub Date : 2023-08-16 , DOI: 10.1021/acs.chemmater.3c00038 Dong-Yang Li 1, 2 , Jia-Hang Wu 3 , Xing-Yu Wang 1 , Xiao-Yang Zhang 1 , Cheng-Yang Yue 1, 2 , Xiao-Wu Lei 1, 2
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Multifunctional stimuli-responsive luminescent and optical switching is extremely crucial for wide advanced photonic applications, but it remains a challenging objective for halide perovskites. Herein, by performing single-crystal to single-crystal (SC–SC) transformation as a dynamic molecular strategy, we realized a reversible triple-mode photoluminescence, radioluminescence (PL and RL), and nonlinear optical (NLO) switching in a pair of zero-dimensional (0D) hybrid cuprous halides of [ETPP]2Cu4Br6 and [ETPP]CuBr2. Specifically, [ETPP]2Cu4Br6 and [ETPP]CuBr2 display highly efficient yellow and green light emissions under UV light excitation with the highest quantum yield of up to near unity. Simultaneously, identical radioluminescence can also be activated by using X-ray as RL with a light yield of up to 57,974 photons MeV–1, surpassing most of the previously reported hybrid cuprous halides. Most remarkably, reversible SC–SC transformation between them can be realized in an ethanol impregnation-heating process, which provides reversible PL/RL transitions in two light-emitting states. Additionally, this process is also accompanied by transition between the centrosymmetric NLO-inactive [ETPP]2Cu4Br6 and noncentrosymmetric NLO-active [ETPP]CuBr2 through reversible second harmonic generation (SHG) “silent-active” switching. To the best of our knowledge, this is the first reported triple-mode reversible PL, RL, and SHG switching in halide perovskite chemistry, which can realize advanced applications in data storage, information security, optical logic gates, etc.
中文翻译：
高效 0D 混合卤化亚铜中的可逆三模光致发光和辐射发光以及非线性光开关
多功能刺激响应发光和光学开关对于广泛的先进光子应用极其重要，但对于卤化物钙钛矿来说仍然是一个具有挑战性的目标。在此，通过将单晶到单晶（SC-SC）转变作为动态分子策略，我们在一对[ETPP] 2 Cu 4 Br 6和[ETPP]CuBr 2的零维（0D）杂化卤化亚铜。具体地，[ETPP] 2 Cu 4 Br 6和[ETPP]CuBr 2在紫外光激发下显示高效的黄光和绿光发射，最高量子产率高达接近1。同时，使用X射线作为RL也可以激活相同的放射发光，光产量高达57,974个光子MeV –1，超过了大多数先前报道的混合卤化亚铜。最值得注意的是，它们之间的可逆 SC-SC 转变可以在乙醇浸渍加热过程中实现，从而提供两种发光态的可逆 PL/RL 跃迁。此外，该过程还伴随着中心对称NLO非活性[ETPP] 2 Cu 4 Br 6和非中心对称NLO活性[ETPP]CuBr 2之间的转变通过可逆二次谐波发生（SHG）“静音-主动”切换。据我们所知，这是卤化物钙钛矿化学中首次报道的三模可逆 PL、RL 和 SHG 开关，可实现数据存储、信息安全、光逻辑门等方面的高级应用。
更新日期：2023-08-16
中文翻译：
高效 0D 混合卤化亚铜中的可逆三模光致发光和辐射发光以及非线性光开关
多功能刺激响应发光和光学开关对于广泛的先进光子应用极其重要，但对于卤化物钙钛矿来说仍然是一个具有挑战性的目标。在此，通过将单晶到单晶（SC-SC）转变作为动态分子策略，我们在一对[ETPP] 2 Cu 4 Br 6和[ETPP]CuBr 2的零维（0D）杂化卤化亚铜。具体地，[ETPP] 2 Cu 4 Br 6和[ETPP]CuBr 2在紫外光激发下显示高效的黄光和绿光发射，最高量子产率高达接近1。同时，使用X射线作为RL也可以激活相同的放射发光，光产量高达57,974个光子MeV –1，超过了大多数先前报道的混合卤化亚铜。最值得注意的是，它们之间的可逆 SC-SC 转变可以在乙醇浸渍加热过程中实现，从而提供两种发光态的可逆 PL/RL 跃迁。此外，该过程还伴随着中心对称NLO非活性[ETPP] 2 Cu 4 Br 6和非中心对称NLO活性[ETPP]CuBr 2之间的转变通过可逆二次谐波发生（SHG）“静音-主动”切换。据我们所知，这是卤化物钙钛矿化学中首次报道的三模可逆 PL、RL 和 SHG 开关，可实现数据存储、信息安全、光逻辑门等方面的高级应用。
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