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 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.
- Authors:
- Publication Date:
- 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. doi:10.1364/OPTICA.5.001141.
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
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.
@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 = {Thu Sep 20 00:00:00 EDT 2018},
month = {Thu Sep 20 00:00:00 EDT 2018}
}
https://doi.org/10.1364/OPTICA.5.001141
Web of Science
Figures / Tables:
Works referenced in this record:
Intriguing Optoelectronic Properties of Metal Halide Perovskites
journal, June 2016
- Manser, Joseph S.; Christians, Jeffrey A.; Kamat, Prashant V.
- Chemical Reviews, Vol. 116, Issue 21
Exciton Binding Energy and the Nature of Emissive States in Organometal Halide Perovskites
journal, July 2015
- Zheng, Kaibo; Zhu, Qiushi; Abdellah, Mohamed
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 15
Metal-halide perovskites for photovoltaic and light-emitting devices
journal, May 2015
- Stranks, Samuel D.; Snaith, Henry J.
- Nature Nanotechnology, Vol. 10, Issue 5
Red, Yellow, Green, and Blue Amplified Spontaneous Emission and Lasing Using Colloidal CdSe Nanoplatelets
journal, September 2015
- She, Chunxing; Fedin, Igor; Dolzhnikov, Dmitriy S.
- ACS Nano, Vol. 9, Issue 10
Dynamic disorder, phonon lifetimes, and the assignment of modes to the vibrational spectra of methylammonium lead halide perovskites
journal, January 2016
- Leguy, Aurélien M. A.; Goñi, Alejandro R.; Frost, Jarvist M.
- Physical Chemistry Chemical Physics, Vol. 18, Issue 39
Ultrafast photonic crystal nanocavity laser
journal, July 2006
- Altug, Hatice; Englund, Dirk; Vučković, Jelena
- Nature Physics, Vol. 2, Issue 7
Efficient perovskite light-emitting diodes featuring nanometre-sized crystallites
journal, January 2017
- Xiao, Zhengguo; Kerner, Ross A.; Zhao, Lianfeng
- Nature Photonics, Vol. 11, Issue 2
On the Absorption Cross Section of CdSe Nanocrystal Quantum Dots
journal, August 2002
- Leatherdale, C. A.; Woo, W. -K.; Mikulec, F. V.
- The Journal of Physical Chemistry B, Vol. 106, Issue 31
Theory of light absorption and non-radiative transitions in F-centres
journal, December 1950
- Huang, Kun; Rhys, Avril
- Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, Vol. 204, Issue 1078, p. 406-423
Diode-Pumped Organo-Lead Halide Perovskite Lasing in a Metal-Clad Distributed Feedback Resonator
journal, June 2016
- Jia, Yufei; Kerner, Ross A.; Grede, Alex J.
- Nano Letters, Vol. 16, Issue 7
Green Perovskite Distributed Feedback Lasers
journal, September 2017
- Harwell, J. R.; Whitworth, G. L.; Turnbull, G. A.
- Scientific Reports, Vol. 7, Issue 1
Direct measurement of the exciton binding energy and effective masses for charge carriers in organic–inorganic tri-halide perovskites
journal, June 2015
- Miyata, Atsuhiko; Mitioglu, Anatolie; Plochocka, Paulina
- Nature Physics, Vol. 11, Issue 7
High-performance photovoltaic perovskite layers fabricated through intramolecular exchange
journal, May 2015
- Yang, W. S.; Noh, J. H.; Jeon, N. J.
- Science, Vol. 348, Issue 6240
Overcoming the electroluminescence efficiency limitations of perovskite light-emitting diodes
journal, December 2015
- Cho, H.; Jeong, S. -H.; Park, M. -H.
- Science, Vol. 350, Issue 6265
Lead halide perovskite nanowire lasers with low lasing thresholds and high quality factors
journal, April 2015
- Zhu, Haiming; Fu, Yongping; Meng, Fei
- Nature Materials, Vol. 14, Issue 6
Red, green and blue lasing enabled by single-exciton gain in colloidal quantum dot films
journal, April 2012
- Dang, Cuong; Lee, Joonhee; Breen, Craig
- Nature Nanotechnology, Vol. 7, Issue 5
Size- and Wavelength-Dependent Two-Photon Absorption Cross-Section of CsPbBr 3 Perovskite Quantum Dots
journal, May 2017
- Chen, Junsheng; Žídek, Karel; Chábera, Pavel
- The Journal of Physical Chemistry Letters, Vol. 8, Issue 10
Free Carriers versus Excitons in CH 3 NH 3 PbI 3 Perovskite Thin Films at Low Temperatures: Charge Transfer from the Orthorhombic Phase to the Tetragonal Phase
journal, June 2016
- Phuong, Le Quang; Yamada, Yasuhiro; Nagai, Masaya
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 13
Absorption cross sections and Auger recombination lifetimes in inverted core-shell nanocrystals: Implications for lasing performance
journal, February 2006
- Nanda, J.; Ivanov, S. A.; Htoon, H.
- Journal of Applied Physics, Vol. 99, Issue 3
Absorption coefficient, energy gap, exciton binding energy, and recombination lifetime of GaN obtained from transmission measurements
journal, November 1997
- Muth, J. F.; Lee, J. H.; Shmagin, I. K.
- Applied Physics Letters, Vol. 71, Issue 18
High- Q , Low-Threshold Monolithic Perovskite Thin-Film Vertical-Cavity Lasers
journal, February 2017
- Chen, Songtao; Zhang, Cheng; Lee, Joonhee
- Advanced Materials, Vol. 29, Issue 16
Efficient and Air-Stable Mixed-Cation Lead Mixed-Halide Perovskite Solar Cells with n-Doped Organic Electron Extraction Layers
journal, December 2016
- Wang, Zhiping; McMeekin, David P.; Sakai, Nobuya
- Advanced Materials, Vol. 29, Issue 5
CsPbBr 3 Perovskite Quantum Dot Vertical Cavity Lasers with Low Threshold and High Stability
journal, August 2017
- Huang, Chun-Ying; Zou, Chen; Mao, Chenyi
- ACS Photonics, Vol. 4, Issue 9
Stable Green Perovskite Vertical-Cavity Surface-Emitting Lasers on Rigid and Flexible Substrates
journal, September 2017
- Chen, Songtao; Nurmikko, Arto
- ACS Photonics, Vol. 4, Issue 10
A Photonic Crystal Laser from Solution Based Organo-Lead Iodide Perovskite Thin Films
journal, March 2016
- Chen, Songtao; Roh, Kwangdong; Lee, Joonhee
- ACS Nano, Vol. 10, Issue 4
Charge-separation energy in films of π-conjugated organic molecules
journal, September 2000
- Hill, I. G.; Kahn, A.; Soos, Z. G.
- Chemical Physics Letters, Vol. 327, Issue 3-4
Excited State Properties of Hybrid Perovskites
journal, December 2015
- Saba, Michele; Quochi, Francesco; Mura, Andrea
- Accounts of Chemical Research, Vol. 49, Issue 1
Excitonic gain and laser emission in ZnSe-based quantum wells
journal, September 1992
- Ding, J.; Jeon, H.; Ishihara, T.
- Physical Review Letters, Vol. 69, Issue 11
Improving Optical Gain Performance in Semiconductor Quantum Dots via Coupled Quantum Shells
journal, February 2012
- Dias, Eva A.; Saari, Jonathan I.; Tyagi, Pooja
- The Journal of Physical Chemistry C, Vol. 116, Issue 9
Patterning Multicolored Microdisk Laser Arrays of Cesium Lead Halide Perovskite
journal, January 2017
- He, Xianxiong; Liu, Peng; Zhang, Haihua
- Advanced Materials, Vol. 29, Issue 12
High Photoluminescence Efficiency and Optically Pumped Lasing in Solution-Processed Mixed Halide Perovskite Semiconductors
journal, March 2014
- Deschler, Felix; Price, Michael; Pathak, Sandeep
- The Journal of Physical Chemistry Letters, Vol. 5, Issue 8
Hydrogen-like Wannier–Mott Excitons in Single Crystal of Methylammonium Lead Bromide Perovskite
journal, May 2016
- Tilchin, Jenya; Dirin, Dmitry N.; Maikov, Georgy I.
- ACS Nano, Vol. 10, Issue 6
Photonic Nanostructures Patterned by Thermal Nanoimprint Directly into Organo-Metal Halide Perovskites
journal, January 2017
- Pourdavoud, Neda; Wang, Si; Mayer, André
- Advanced Materials, Vol. 29, Issue 12
Continuous-Wave Lasing in Cesium Lead Bromide Perovskite Nanowires
journal, December 2017
- Evans, Tyler J. S.; Schlaus, Andrew; Fu, Yongping
- Advanced Optical Materials, Vol. 6, Issue 2
Thermally Activated Exciton Dissociation and Recombination Control the Carrier Dynamics in Organometal Halide Perovskite
journal, June 2014
- Savenije, Tom J.; Ponseca, Carlito S.; Kunneman, Lucas
- The Journal of Physical Chemistry Letters, Vol. 5, Issue 13
Slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals
journal, February 2017
- Li, Mingjie; Bhaumik, Saikat; Goh, Teck Wee
- Nature Communications, Vol. 8, Issue 1
Excitonic gain and stimulated emission in ZnSe-based quantum wells up to room temperature
journal, January 1992
- Ding, J.; Jeon, H.; Ishihara, T.
- Surface Science, Vol. 267, Issue 1-3
Ultrafast carrier thermalization in lead iodide perovskite probed with two-dimensional electronic spectroscopy
journal, August 2017
- Richter, Johannes M.; Branchi, Federico; Valduga de Almeida Camargo, Franco
- Nature Communications, Vol. 8, Issue 1
Resolving the ambiguity in the relation between Stokes shift and Huang–Rhys parameter
journal, January 2015
- de Jong, Mathijs; Seijo, Luis; Meijerink, Andries
- Physical Chemistry Chemical Physics, Vol. 17, Issue 26
Correlated electron–hole plasma in organometal perovskites
journal, September 2014
- Saba, Michele; Cadelano, Michele; Marongiu, Daniela
- Nature Communications, Vol. 5, Issue 1
Spectroscopy of optical gain in low threshold colloidal quantum dot laser media: dominance of single-exciton states at room temperature
journal, January 2016
- Roh, Kwangdong; Lee, Joonhee; Dang, Cuong
- Optical Materials Express, Vol. 6, Issue 12
Excitons versus free charges in organo-lead tri-halide perovskites
journal, April 2014
- D’Innocenzo, Valerio; Grancini, Giulia; Alcocer, Marcelo J. P.
- Nature Communications, Vol. 5, Issue 1
Solution-Processed Low Threshold Vertical Cavity Surface Emitting Lasers from All-Inorganic Perovskite Nanocrystals
journal, February 2017
- Wang, Yue; Li, Xiaoming; Nalla, Venkatram
- Advanced Functional Materials, Vol. 27, Issue 13
Cesium Enhances Long-Term Stability of Lead Bromide Perovskite-Based Solar Cells
journal, December 2015
- Kulbak, Michael; Gupta, Satyajit; Kedem, Nir
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 1
Low-threshold amplified spontaneous emission and lasing from colloidal nanocrystals of caesium lead halide perovskites
journal, August 2015
- Yakunin, Sergii; Protesescu, Loredana; Krieg, Franziska
- Nature Communications, Vol. 6, Issue 1
Surface-emitting red, green, and blue colloidal quantum dot distributed feedback lasers
journal, January 2014
- Roh, Kwangdong; Dang, Cuong; Lee, Joonhee
- Optics Express, Vol. 22, Issue 15
Direct Measurement of Conjugated Polymer Electronic Excitation Energies Using Metal/Polymer/Metal Structures
journal, March 1996
- Campbell, I. H.; Hagler, T. W.; Smith, D. L.
- Physical Review Letters, Vol. 76, Issue 11
Two-dimensional photonic crystal bandedge laser with hybrid perovskite thin film for optical gain
journal, May 2016
- Cha, Hyungrae; Bae, Seunghwan; Lee, Myungjae
- Applied Physics Letters, Vol. 108, Issue 18
Quantum States of Confined Carriers in Very Thin -GaAs- Heterostructures
journal, September 1974
- Dingle, R.; Wiegmann, W.; Henry, C. H.
- Physical Review Letters, Vol. 33, Issue 14
Strong Carrier–Phonon Coupling in Lead Halide Perovskite Nanocrystals
journal, September 2017
- Iaru, Claudiu M.; Geuchies, Jaco J.; Koenraad, Paul M.
- ACS Nano, Vol. 11, Issue 11
Continuous-wave lasing in an organic–inorganic lead halide perovskite semiconductor
journal, November 2017
- Jia, Yufei; Kerner, Ross A.; Grede, Alex J.
- Nature Photonics, Vol. 11, Issue 12
Giant Bandgap Renormalization and Exciton-Phonon Scattering in Perovskite Nanocrystals
journal, June 2017
- Saran, Rinku; Heuer-Jungemann, Amelie; Kanaras, Antonios G.
- Advanced Optical Materials, Vol. 5, Issue 17
Femtosecond Dynamics of Resonantly Excited Excitons in Room-Temperature GaAs Quantum Wells
journal, March 1985
- Knox, W. H.; Fork, R. L.; Downer, M. C.
- Physical Review Letters, Vol. 54, Issue 12
A mixed-cation lead mixed-halide perovskite absorber for tandem solar cells
journal, January 2016
- McMeekin, D. P.; Sadoughi, G.; Rehman, W.
- Science, Vol. 351, Issue 6269
High Charge Carrier Mobilities and Lifetimes in Organolead Trihalide Perovskites
journal, December 2013
- Wehrenfennig, Christian; Eperon, Giles E.; Johnston, Michael B.
- Advanced Materials, Vol. 26, Issue 10
Determination of the exciton binding energy and effective masses for methylammonium and formamidinium lead tri-halide perovskite semiconductors
journal, January 2016
- Galkowski, Krzysztof; Mitioglu, Anatolie; Miyata, Atsuhiko
- Energy & Environmental Science, Vol. 9, Issue 3
Intensity of Optical Absorption by Excitons
journal, December 1957
- Elliott, R. J.
- Physical Review, Vol. 108, Issue 6
Unraveling Charge Carriers Generation, Diffusion, and Recombination in Formamidinium Lead Triiodide Perovskite Polycrystalline Thin Film
journal, December 2015
- Piatkowski, Piotr; Cohen, Boiko; Ponseca, Carlito S.
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 1
Highly stable solution processed metal-halide perovskite lasers on nanoimprinted distributed feedback structures
journal, October 2016
- Brenner, Philipp; Stulz, Mareike; Kapp, Dorothee
- Applied Physics Letters, Vol. 109, Issue 14
Temperature dependence of the energy gap in semiconductors
journal, January 1967
- Varshni, Y. P.
- Physica, Vol. 34, Issue 1
Lead Salt Quantum Dots: the Limit of Strong Quantum Confinement
journal, November 2000
- Wise, Frank W.
- Accounts of Chemical Research, Vol. 33, Issue 11
Temperature-dependent exciton linewidths in semiconductors
journal, December 1990
- Rudin, S.; Reinecke, T. L.; Segall, B.
- Physical Review B, Vol. 42, Issue 17
Observation of a hot-phonon bottleneck in lead-iodide perovskites
journal, October 2015
- Yang, Ye; Ostrowski, David P.; France, Ryan M.
- Nature Photonics, Vol. 10, Issue 1
A solvent- and vacuum-free route to large-area perovskite films for efficient solar modules
journal, September 2017
- Chen, Han; Ye, Fei; Tang, Wentao
- Nature, Vol. 550, Issue 7674
Electron–phonon coupling in hybrid lead halide perovskites
journal, May 2016
- Wright, Adam D.; Verdi, Carla; Milot, Rebecca L.
- Nature Communications, Vol. 7, Issue 1
Works referencing / citing this record:
Effects of External Magnetic Fields on Optical Properties of an Oxide Quantum Dot Using the Smorodinsky–Winternitz Potential
journal, January 2020
- Peter, A. John; Karthikeyan, N.; Lee, Chang Woo
- Journal of Electronic Materials, Vol. 49, Issue 3
Deprotonation and vacancies at the CH 3 NH 3 PbI 3 /ZnO and CH 3 NH 3 PbI 3 /GaN interfaces, detected in their theoretical XANES
journal, January 2019
- Wierzbowska, Małgorzata
- Journal of Materials Chemistry C, Vol. 7, Issue 18
Amplified Spontaneous Emission and Lasing in Lead Halide Perovskites: State of the Art and Perspectives
journal, October 2019
- De Giorgi, Maria Luisa; Anni, Marco
- Applied Sciences, Vol. 9, Issue 21
Figures / Tables found in this record: