Excitonic gain and laser emission from mixed-cation halide perovskite thin films

Chen, Songtao; Nurmikko, Arto

doi:10.1364/OPTICA.5.001141

Title: Excitonic gain and laser emission from mixed-cation halide perovskite thin films

Abstract

Organic–inorganic halide perovskites have recently developed into a potential semiconductor coherent light emitter candidate beyond their promise in solar cell applications. However, despite the ample demonstrations of perovskite lasers, experimental results on the origin of optical gain in perovskites are still elusive. Here, we analyze the excitonic gain in the green from mixed-cation halide perovskites Cs_0.17[CH(NH₂)₂]_0.83PbBr₃ (Cs_0.17FA_0.83PbBr₃) by both low temperature absorption/emission spectroscopies and ultrafast pump–probe transient absorption experiments. The perovskite thin films show a robust excitonic feature up to room temperature, with estimated exciton binding energy E_b = 43.8 meV, which can be maintained under high electronic excitations that are required for lasers. By using a high-quality (Q = 1350) vertical cavity consisting of sputtered dielectric HfO₂/SiO₂ distributed Bragg reflectors with perovskite optical gain medium embedded inside, we have demonstrated excitonic-gain-enabled optically pumped lasing, with improved threshold of 13.5 ± 1.4 μJ/cm² and device longevity lifetime >35 h (10⁸ laser shots) at ambient environment under sustained pulsed optical excitations (3.493 eV, τ_pulse = 0.34 ns, 1 kHz). Understanding and exploiting excitonic gain from perovskite thin film materials may help to further boost the performance of perovskite-based lasers.

Authors:

; Nurmikko, Arto

Publication Date:: 2018-09-20

Research Org.:: Brown Univ., Providence, RI (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1471743

Alternate Identifier(s):: OSTI ID: 1502474

Grant/Contract Number:: FG02-07ER46387

Resource Type:: Published Article

Journal Name:: Optica

Additional Journal Information:: Journal Name: Optica Journal Volume: 5 Journal Issue: 9; Journal ID: ISSN 2334-2536

Publisher:: Optical Society of America

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Chen, Songtao, and Nurmikko, Arto. Excitonic gain and laser emission from mixed-cation halide perovskite thin films.  United States: N. p., 2018. 
Web.  https://doi.org/10.1364/OPTICA.5.001141.

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                    Chen, Songtao, & Nurmikko, Arto. Excitonic gain and laser emission from mixed-cation halide perovskite thin films.  United States.  https://doi.org/10.1364/OPTICA.5.001141

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                    Chen, Songtao, and Nurmikko, Arto. Thu .  
"Excitonic gain and laser emission from mixed-cation halide perovskite thin films".  United States.  https://doi.org/10.1364/OPTICA.5.001141.

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@article{osti_1471743,

  title        = {Excitonic gain and laser emission from mixed-cation halide perovskite thin films},

  author       = {Chen, Songtao and Nurmikko, Arto},

  abstractNote = {Organic–inorganic halide perovskites have recently developed into a potential semiconductor coherent light emitter candidate beyond their promise in solar cell applications. However, despite the ample demonstrations of perovskite lasers, experimental results on the origin of optical gain in perovskites are still elusive. Here, we analyze the excitonic gain in the green from mixed-cation halide perovskites Cs0.17[CH(NH2)2]0.83PbBr3 (Cs0.17FA0.83PbBr3) by both low temperature absorption/emission spectroscopies and ultrafast pump–probe transient absorption experiments. The perovskite thin films show a robust excitonic feature up to room temperature, with estimated exciton binding energy Eb = 43.8 meV, which can be maintained under high electronic excitations that are required for lasers. By using a high-quality (Q = 1350) vertical cavity consisting of sputtered dielectric HfO2/SiO2 distributed Bragg reflectors with perovskite optical gain medium embedded inside, we have demonstrated excitonic-gain-enabled optically pumped lasing, with improved threshold of 13.5 ± 1.4 μJ/cm2 and device longevity lifetime >35 h (108 laser shots) at ambient environment under sustained pulsed optical excitations (3.493 eV, τpulse = 0.34 ns, 1 kHz). Understanding and exploiting excitonic gain from perovskite thin film materials may help to further boost the performance of perovskite-based lasers.},

  doi          = {10.1364/OPTICA.5.001141},

  journal      = {Optica},

  number       = 9,

  volume       = 5,

  place        = {United States},

  year         = {2018},

  month        = {9}

}

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Fig. 1. : (a) Scanning electron microscope image of surface morphology of a Cs_0.17FA_0.83PbBr₃ film on a planar quartz substrate. (b) Grain size distribution of the mixed-cation perovskite film, with Gaussian fit (black line) yielding mean value of 79 nm and standard deviation of 51 nm. (c) Xray diffraction patternmore »

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