Phase-pure 2D tin halide perovskite thin flakes for stable lasing.

Ruddlesden-Popper tin halide perovskites are a class of two-dimensional (2D) semiconductors with exceptional optoelectronic properties, high carrier mobility, and low toxicity. However, the synthesis of phase-pure 2D tin perovskites is still challenging, and the fundamental understanding of their optoelectronic properties is deficient compared to their lead counterparts. Here, we report the synthesis of a series of 2D tin perovskite bulk crystals with high phase purity via a mixed-solvent strategy. By engineering the quantum-well thickness (related to n value) and organic ligands, the optoelectronic properties, including photoluminescence emission, exciton-phonon coupling strength, and exciton binding energy, exhibit a wide tunability. In addition, these 2D tin perovskites exhibited excellent lasing performance. Both high-n value tin perovskite (n > 1) and n = 1 tin perovskite thin flakes were successfully optically pumped to lase. Furthermore, the lasing from 2D tin perovskites could be maintained up to room temperature. Our findings highlight the tremendous potential of 2D tin perovskites as promising candidates for high-performance lasers.

[1]  A. Petrozza,et al.  Lasing in Two-Dimensional Tin Perovskites , 2022, ACS nano.

[2]  Joo Sung Kim,et al.  Ultra-bright, efficient and stable perovskite light-emitting diodes , 2022, Nature.

[3]  D. Nordlund,et al.  Low Exciton Binding Energies and Localized Exciton–Polaron States in 2D Tin Halide Perovskites , 2022, Advanced Optical Materials.

[4]  Thomas G. Allen,et al.  Damp heat–stable perovskite solar cells with tailored-dimensionality 2D/3D heterojunctions , 2022, Science.

[5]  Jun Wang,et al.  Regulation of the luminescence mechanism of two-dimensional tin halide perovskites , 2022, Nature Communications.

[6]  Kyung-In Jang,et al.  Perovskite superlattices with efficient carrier dynamics , 2021, Nature.

[7]  Libai Huang,et al.  Ligand-Driven Grain Engineering of High Mobility Two-Dimensional Perovskite Thin-Film Transistors. , 2021, Journal of the American Chemical Society.

[8]  C. Grigoropoulos,et al.  Actively variable-spectrum optoelectronics with black phosphorus , 2021, Nature.

[9]  S. Mandal,et al.  Refractive index of different perovskite materials , 2021, Journal of Materials Research.

[10]  Yingtang Zhou,et al.  First-principles investigation on the thickness-dependent optoelectronic properties of two-dimensional perovskite BA2SnI4 , 2021 .

[11]  S. Stupp,et al.  Tunable exciton binding energy in 2D hybrid layered perovskites through donor–acceptor interactions within the organic layer , 2020, Nature Chemistry.

[12]  Hongjun Gao,et al.  Universal mechanical exfoliation of large-area 2D crystals , 2020, Nature Communications.

[13]  M. Baranowski,et al.  Excitons in Metal‐Halide Perovskites , 2020, Advanced Energy Materials.

[14]  Libai Huang,et al.  Long-range exciton transport and slow annihilation in two-dimensional hybrid perovskites , 2020, Nature Communications.

[15]  M. Zeller,et al.  Molecular engineering of organic–inorganic hybrid perovskites quantum wells , 2019, Nature Chemistry.

[16]  Liyun Zhao,et al.  Lasing from Mechanically Exfoliated 2D Homologous Ruddlesden–Popper Perovskite Engineered by Inorganic Layer Thickness , 2019, Advanced materials.

[17]  Song Jin,et al.  Metal halide perovskite nanostructures for optoelectronic applications and the study of physical properties , 2019, Nature Reviews Materials.

[18]  L. Chu,et al.  Molecularly thin two-dimensional hybrid perovskites with tunable optoelectronic properties due to reversible surface relaxation , 2018, Nature Materials.

[19]  Edward P. Booker,et al.  Vertical Cavity Biexciton Lasing in 2D Dodecylammonium Lead Iodide Perovskites , 2018, Advanced Optical Materials.

[20]  X. Zhang,et al.  Single-crystalline layered metal-halide perovskite nanowires for ultrasensitive photodetectors , 2018, Nature Electronics.

[21]  O. Voznyy,et al.  Electron–phonon interaction in efficient perovskite blue emitters , 2018, Nature Materials.

[22]  Wei‐Liang Chen,et al.  Low-Threshold Lasing from 2D Homologous Organic-Inorganic Hybrid Ruddlesden-Popper Perovskite Single Crystals. , 2018, Nano letters.

[23]  Libai Huang,et al.  Electron-Phonon Scattering in Atomically Thin 2D Perovskites. , 2016, ACS nano.

[24]  Oleksandr Voznyy,et al.  Perovskite energy funnels for efficient light-emitting diodes. , 2016, Nature nanotechnology.

[25]  Sergei Tretiak,et al.  High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells , 2016, Nature.

[26]  Feliciano Giustino,et al.  Electron–phonon coupling in hybrid lead halide perovskites , 2016, Nature Communications.

[27]  D. J. Clark,et al.  Ruddlesden-Popper Hybrid Lead Iodide Perovskite 2D Homologous Semiconductors , 2016 .

[28]  Omar K Farha,et al.  2D Homologous Perovskites as Light-Absorbing Materials for Solar Cell Applications. , 2015, Journal of the American Chemical Society.

[29]  Yuan Wang,et al.  Monolayer excitonic laser , 2015, Nature Photonics.

[30]  Arka Majumdar,et al.  Monolayer semiconductor nanocavity lasers with ultralow thresholds , 2015, Nature.

[31]  Xiang Zhang,et al.  Edge Nonlinear Optics on a MoS2 Atomic Monolayer , 2014, Science.

[32]  Likai Li,et al.  Black phosphorus field-effect transistors. , 2014, Nature nanotechnology.

[33]  Qing Hua Wang,et al.  Electronics and optoelectronics of two-dimensional transition metal dichalcogenides. , 2012, Nature nanotechnology.

[34]  Pierre Lefebvre,et al.  Influence of electron-phonon interaction on the optical properties of III nitride semiconductors , 2001 .

[35]  Cherie R. Kagan,et al.  Organic-inorganic hybrid materials as semiconducting channels in thin-film field-effect transistors , 1999, Science.

[36]  David B. Mitzi,et al.  Electroluminescence from an Organic−Inorganic Perovskite Incorporating a Quaterthiophene Dye within Lead Halide Perovskite Layers , 1999 .

[37]  D. Mitzi,et al.  Conducting tin halides with a layered organic-based perovskite structure , 1994, Nature.

[38]  P. Bhattacharya,et al.  Absorption and photoluminescence studies of the temperature dependence of exciton life time in lattice-matched and strained quantum well systems , 1987 .