Tuning the bandgap of Cs<sub>2</sub>AgBiBr<sub>6</sub> through dilute tin alloying

Lindquist, Kurt P.; Mack, Stephanie; Slavney, Adam H.; Leppert, Linn; Gold‐Parker, Aryeh; Stebbins, Jonathan F.; Salleo, Alberto; Toney, Michael F.; Neaton, Jeffrey B.; Karunadasa, Hemamala I.

doi:10.1039/c9sc02581b

Cited by 74 publications

(81 citation statements)

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“…[ 143,144 ] The aforementioned theoretical analysis gives us a chance to tune the bandgap of HDPs through precise component engineering and unexpected optoelectronic properties will be uncovered. [ 68,145–147 ]…”

Section: Optical Properties Of Hdpsmentioning

confidence: 99%

Lead‐Free Halide Double Perovskites: Structure, Luminescence, and Applications

Zeng

2020

Small Structures

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Organic–inorganic halide perovskites have attracted extensive attention due to their excellent optoelectronic properties. However, the toxicity of heavy atom Pb2+ and instability overshadow further commercial applications, motivating researchers to explore alternative analogues to overcome these disadvantages. Lead‐free halide double perovskites (HDPs), sharing similar crystal structures with organic–inorganic halide perovskites, are promising candidates for optoelectronic applications. However, HDPs possess unique properties that are uncommon in organic–inorganic halide perovskites deriving from feasible component engineering and strong electron–phonon interaction. Bright luminescence in HDPs originates from self‐trapped excitons (STEs) and sensitized dopants can cover the full visible and near‐infrared ray (NIR) gamut by modulating parity‐forbidden transitions and the energy‐transfer process. The superior optoelectronic characteristics of HDPs further extend applications on self‐assembly, white‐light phosphors, NIR bioimaging, and scintillators, in comparison to organic–inorganic halide perovskites. Herein, the structural diversity, tunable luminescence, photophysical mechanism of STEs, charge‐carrier dynamics, size effect, and stability issues of HDPs are discussed. The challenges and outlook for further investigations are also given, which may help in discovering new analogues and boosting the photoluminescence quantum yield and stability of HDPs.

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Section: Optical Properties Of Hdpsmentioning

confidence: 99%

Lead‐Free Halide Double Perovskites: Structure, Luminescence, and Applications

Zeng

2020

Small Structures

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“…Alloying/doping is a simple yet efficient method to tune the bandgaps of a wide range of materials, including traditional inorganic semiconductors, 8,9 oxide-based perovskites, 10 Pbbased perovskites, 11 as well as lead-free halide double perovskites. [12][13][14][15] For example, trivalent Sb 3+ -alloying has been employed to decrease the bandgap of Cs 2 AgBiBr 6 and Cs 2 -AgInCl 6 . However, the bandgaps of the alloys in both cases are still large for photovoltaic applications.…”

Section: Introductionmentioning

confidence: 99%

The atomic-level structure of bandgap engineered double perovskite alloys Cs₂AgIn_1−xFe_xCl₆

Wang

Kobera

et al. 2021

Chem. Sci.

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“…After the first report on the synthesis of Cs 2 AgBiBr 6 and Cs 2 AgBiCl 6 , 16 , 17 the Br-based material has been shown to form high-quality thin films suitable for the fabrication of solar cells with power conversion efficiencies reaching 1, 4, and 2.5% using vacuum deposition and solution processing, respectively. 18 − 20 The material has been further investigated computationally, 18 , 21 as a single crystal, 22 , 23 and its band gap has been shown to be tunable by alloying with Pb 2+ , 24 Sn 2+/4+ , 25 Tl 3+ , 9 In 3+ , and Sb 3+ . 13 Very recently, mixed-halides Cs 2 AgBiCl 6- x Br x have been investigated both theoretically 26 , 27 and experimentally.…”

Section: Introductionmentioning

confidence: 99%

Halide Mixing and Phase Segregation in Cs₂AgBiX₆ (X = Cl, Br, and I) Double Perovskites from Cesium-133 Solid-State NMR and Optical Spectroscopy

et al. 2020

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All-inorganic double perovskites (elpasolites) are a promising potential alternatives to lead halide perovskites in optoelectronic applications. Although halide mixing is a well-established strategy for band gap tuning, little is known about halide mixing and phase segregation phenomena in double perovskites. Here, we synthesize a wide range of single- and mixed-halide Cs 2 AgBiX 6 (X = Cl, Br, and I) double perovskites using mechanosynthesis and probe their atomic-level microstructure using 133 Cs solid-state MAS NMR. We show that mixed Cl/Br materials form pure phases for any Cl/Br ratio while Cl/I and Br/I mixing is only possible within a narrow range of halide ratios (<3 mol % I) and leads to a complex mixture of products for higher ratios. We characterize the optical properties of the resulting materials and show that halide mixing does not lead to an appreciable tunability of the PL emission. We find that iodide incorporation is particularly pernicious in that it quenches the PL emission intensity and radiative charge carrier lifetimes for iodide ratios as low as 0.3 mol %. Our study shows that solid-state NMR, in conjunction with optical spectroscopies, provides a comprehensive understanding of the structure–activity relationships, halide mixing, and phase segregation phenomena in Cs 2 AgBiX 6 (X = Cl, Br, and I) double perovskites.

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Tuning the bandgap of Cs₂AgBiBr₆ through dilute tin alloying

Abstract: Sn alloying tunes a halide double perovskite to absorb visible light, in a nontoxic composition.

Cited by 74 publications

References 43 publications

Lead‐Free Halide Double Perovskites: Structure, Luminescence, and Applications

Lead‐Free Halide Double Perovskites: Structure, Luminescence, and Applications

The atomic-level structure of bandgap engineered double perovskite alloys Cs₂AgIn_1−xFe_xCl₆

Halide Mixing and Phase Segregation in Cs₂AgBiX₆ (X = Cl, Br, and I) Double Perovskites from Cesium-133 Solid-State NMR and Optical Spectroscopy

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Tuning the bandgap of Cs2AgBiBr6 through dilute tin alloying

Abstract: Sn alloying tunes a halide double perovskite to absorb visible light, in a nontoxic composition.

Cited by 74 publications

References 43 publications

Lead‐Free Halide Double Perovskites: Structure, Luminescence, and Applications

Lead‐Free Halide Double Perovskites: Structure, Luminescence, and Applications

The atomic-level structure of bandgap engineered double perovskite alloys Cs2AgIn1−xFexCl6

Halide Mixing and Phase Segregation in Cs2AgBiX6 (X = Cl, Br, and I) Double Perovskites from Cesium-133 Solid-State NMR and Optical Spectroscopy

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Tuning the bandgap of Cs₂AgBiBr₆ through dilute tin alloying

The atomic-level structure of bandgap engineered double perovskite alloys Cs₂AgIn_1−xFe_xCl₆

Halide Mixing and Phase Segregation in Cs₂AgBiX₆ (X = Cl, Br, and I) Double Perovskites from Cesium-133 Solid-State NMR and Optical Spectroscopy