Halide perovskites offer great promise for optoelectronic applications, but stability issues continue to hinder its implementation and long-term stability. The stability of all-inorganic halide perovskites and the inherent quantum confinement of low dimensional perovskites can be harnessed to synthesize materials with high PL efficiency. An example of such materials is the recently reported new family of layered double perovskites, Cs4Mn1−xCdxBi2Cl12. Herein, we report a new synthetic procedure that enhances the maximum PLQY of this family materials to up 79.5%, a 20% enhancement from previous reports and the highest reported for a Mn-doped halide perovskite. Importantly, stability tests demonstrate that these materials are very stable towards humidity, UV irradiation, and temperature. Finally, we investigated the photophysics, the effects of magnetic coupling and temperature in the PL efficiency and proposed a mechanism for the emission process. Our results highlight the potential of this family of materials and related layered all-inorganic perovskites for solid-state lighting and optoelectronic applications.
Layered halide perovskites and double perovskites optoelectronic properties have recently been the subject of intense research. Layered double perovskites represent the merging of both worlds, and as such, have the potential to further expand the already vast space of optoelectronic properties and applications of halide perovskites. Despite having more than 40 known members, to date, only the <111>-oriented layered double perovskites: Cs4Cd1-xMnxBi2Cl12, have shown efficient photoluminescence (PL). In this work, we replaced Bi with Sb to further investigate the electronic structure and PL properties of these materials, resulting in two new families of layered inorganic perovskites alloys with full solubility. The first family, Cs4Cd1-xMnSb2Cl12, exhibits a PL emission at 605 nm ascribed to Mn 2+ centers in octahedral coordination, and a maximum photoluminescence quantum yield PLQY of 28.5%. The second family of alloys, also with full solubility, Cs4Cd0.8Mn0.2(Sb1-yBiy)2Cl12, contains a fixed amount of Mn 2+ and Cd 2+ cations but different concentrations of the trivalent metals. This variability allows the tuning of the PL emission from 603 nm to 614 nm. We show that the decreased efficiency of the Cs4Cd1-xMnxSb2Cl12family compared to Cs4Cd1-xMnxBi2Cl12, is mostly due to a decreased spin-orbit coupling in Sb and the subsequent increased electronic delocalization compared to the Bi alloys, reducing the energy transfer to Mn 2+ centers. This work lays out a roadmap to understand and achieve high photoluminescence efficiencies in layered double perovskites.
Layered halide perovskites and double perovskites optoelectronic properties have recently been the subject of intense research. Layered double perovskites represent the merging of both worlds, and as such, have the potential to further expand the already vast space of optoelectronic properties and applications of halide perovskites. Despite having more than 40 known members, to date, only the <111>-oriented layered double perovskites: Cs<sub>4</sub>Cd<sub>1</sub>–<sub>x</sub>Mn<sub>x</sub><b>Bi</b><sub>2</sub>Cl<sub>12</sub>, have shown efficient photoluminescence (PL). In this work, we replaced Bi with Sb to further investigate the electronic structure and PL properties of these materials, resulting in two new families of layered inorganic perovskites alloys with full solubility. The first family, Cs<sub>4</sub>Cd<sub>1</sub>–<sub>x</sub>Mn<b>Sb</b><sub>2</sub>Cl<sub>12</sub>, exhibits a PL emission at 605 nm ascribed to Mn<sup>2+</sup> centers in octahedral coordination, and a maximum photoluminescence quantum yield PLQY of 28.5%. The second family of alloys, also with full solubility, Cs<sub>4</sub>Cd<sub>0.8</sub>Mn<sub>0.2</sub>(Sb<sub>1</sub>–<sub>y</sub>Bi<sub>y</sub>)<sub>2</sub>Cl<sub>12</sub>, contains a fixed amount of Mn<sup>2+</sup> and Cd<sup>2+</sup> cations but different concentrations of the trivalent metals. This variability allows the tuning of the PL emission from 603 nm to 614 nm. We show that the decreased efficiency of the Cs<sub>4</sub>Cd<sub>1</sub>–<sub>x</sub>Mn<sub>x</sub>Sb<sub>2</sub>Cl<sub>12</sub>family compared to Cs<sub>4</sub>Cd<sub>1</sub>–<sub>x</sub>Mn<sub>x</sub><b>Bi</b><sub>2</sub>Cl<sub>12</sub>, is mostly due to a decreased spin-orbit coupling in Sb and the subsequent increased electronic delocalization compared to the Bi alloys, reducing the energy transfer to Mn<sup>2+</sup> centers. This work lays out a roadmap to understand and achieve high photoluminescence efficiencies in layered double perovskites.<p></p>
Halide perovskites offer great promise for optoelectronic applications, but stability issues continue to hinder its implementation and long-term stability. The stability of all-inorganic halide perovskites and the inherent quantum confinement of low dimensional perovskites can be harnessed to synthesize materials with high PL efficiency. An example of such materials is the recently reported new family of layered double perovskites, Cs4Mn1−xCdxBi2Cl12. Herein, we report a new synthetic procedure that enhances the maximum PLQY of this family materials to up 79.5%, a 20% enhancement from previous reports and the highest reported for a Mn-doped halide perovskite. Importantly, stability tests demonstrate that these materials are very stable towards humidity, UV irradiation, and temperature. Finally, we investigated the photophysics, the effects of magnetic coupling and temperature in the PL efficiency and proposed a mechanism for the emission process. Our results highlight the potential of this family of materials and related layered all-inorganic perovskites for solid-state lighting and optoelectronic applications<p></p>
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