Giant spin-selective bandgap renormalization in CsPbBr 3 colloidal nanocrystals
Abstract
The spin-dependence of the strongly correlated phenomena and many-body interactions play an important role in quantum information science. In particular, it is quite interesting but unclear how the spin degree of freedom ramifies the bandgap renormalization, one of the fundamental many-body phenomena. We report the first room-temperature observation of giant spin-selective bandgap renormalization (SS-BGR) in CsPbBr3 colloidal nanocrystals using time-resolved circularly polarized femtosecond pump-probe spectroscopy. The SS-BGR results from many-body interactions among carriers with the same spin that renormalize their joint density of states by 57+/- 1 meV, visualized here as photoinduced absorption (PIA) below band-edge transition energy when the pump and probe are co-polarized. The hallmark result of spectrally resolved SS-BGR is in stark contrast to the usually submerged signal in II-VI and III-V semiconductors and is 3 orders of magnitude larger than that observed in Ge/SiGe quantum wells, highlighting the unique and beneficial band structure of the metal-halide semiconductors. We propose that the PIA, due to SS-BGR, can be used to describe the spin-polarization and spin-relaxation dynamics. The experimental and theoretical findings open up new possibilities for optical manipulation of spin degrees of freedom and their many-body interactions in metal-halide perovskite nanocrystals for potential room-temperature applications.
- Authors:
-
[1];
[3];
[1]
- Indian Inst. of Science Education and Research, Bhopal (India)
- National Renewable Energy Lab. (NREL), Golden, CO (United States); Indian Inst. of Chemical Technology, Tarnaka (India)
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1882927
- Report Number(s):
- NREL/JA-5900-82268
Journal ID: ISSN 2469-9950; MainId:83041;UUID:00c74667-f6db-40ec-b7fb-af416cde76e2;MainAdminID:64828; TRN: US2307951
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review. B
- Additional Journal Information:
- Journal Volume: 106; Journal Issue: 4; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; bandgap renormalization; CsPbBr3; spin polarization; spin-selective; room-temperature
Citation Formats
Shrivastava, Megha, Hazarika, Abhijit, Aneesh, J., Mandal, Dipendranath, Beard, Matthew C., and Adarsh, K. V. Giant spin-selective bandgap renormalization in CsPbBr3 colloidal nanocrystals. United States: N. p., 2022.
Web. doi:10.1103/physrevb.106.l041404.
Shrivastava, Megha, Hazarika, Abhijit, Aneesh, J., Mandal, Dipendranath, Beard, Matthew C., & Adarsh, K. V. Giant spin-selective bandgap renormalization in CsPbBr3 colloidal nanocrystals. United States. https://doi.org/10.1103/physrevb.106.l041404
Shrivastava, Megha, Hazarika, Abhijit, Aneesh, J., Mandal, Dipendranath, Beard, Matthew C., and Adarsh, K. V. Tue .
"Giant spin-selective bandgap renormalization in CsPbBr3 colloidal nanocrystals". United States. https://doi.org/10.1103/physrevb.106.l041404. https://www.osti.gov/servlets/purl/1882927.
@article{osti_1882927,
title = {Giant spin-selective bandgap renormalization in CsPbBr3 colloidal nanocrystals},
author = {Shrivastava, Megha and Hazarika, Abhijit and Aneesh, J. and Mandal, Dipendranath and Beard, Matthew C. and Adarsh, K. V.},
abstractNote = {The spin-dependence of the strongly correlated phenomena and many-body interactions play an important role in quantum information science. In particular, it is quite interesting but unclear how the spin degree of freedom ramifies the bandgap renormalization, one of the fundamental many-body phenomena. We report the first room-temperature observation of giant spin-selective bandgap renormalization (SS-BGR) in CsPbBr3 colloidal nanocrystals using time-resolved circularly polarized femtosecond pump-probe spectroscopy. The SS-BGR results from many-body interactions among carriers with the same spin that renormalize their joint density of states by 57+/- 1 meV, visualized here as photoinduced absorption (PIA) below band-edge transition energy when the pump and probe are co-polarized. The hallmark result of spectrally resolved SS-BGR is in stark contrast to the usually submerged signal in II-VI and III-V semiconductors and is 3 orders of magnitude larger than that observed in Ge/SiGe quantum wells, highlighting the unique and beneficial band structure of the metal-halide semiconductors. We propose that the PIA, due to SS-BGR, can be used to describe the spin-polarization and spin-relaxation dynamics. The experimental and theoretical findings open up new possibilities for optical manipulation of spin degrees of freedom and their many-body interactions in metal-halide perovskite nanocrystals for potential room-temperature applications.},
doi = {10.1103/physrevb.106.l041404},
journal = {Physical Review. B},
number = 4,
volume = 106,
place = {United States},
year = {Tue Jul 05 00:00:00 EDT 2022},
month = {Tue Jul 05 00:00:00 EDT 2022}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Perovskite Nanocrystal Heterostructures: Synthesis, Optical Properties, and Applications
journal, August 2020
- Bera, Suman; Pradhan, Narayan
- ACS Energy Letters, Vol. 5, Issue 9
An Insightful Picture of Multi-Particle Recombination in Few-Layer MoS2 Nanosheets
journal, January 2022
- Taank, Pravrati; Karmakar, Riyanka; Sharma, Rituraj
- The Journal of Physical Chemistry C, Vol. 126, Issue 1
Spin-orbit–coupled exciton-polariton condensates in lead halide perovskites
journal, December 2021
- Spencer, Michael S.; Fu, Yongping; Schlaus, Andrew P.
- Science Advances, Vol. 7, Issue 49
Many-body and correlation effects in semiconductors
journal, May 2001
- Chemla, D. S.; Shah, Jagdeep
- Nature, Vol. 411, Issue 6837
Band filling with free charge carriers in organometal halide perovskites
journal, August 2014
- Manser, Joseph S.; Kamat, Prashant V.
- Nature Photonics, Vol. 8, Issue 9
Observation of Exciton Redshift–Blueshift Crossover in Monolayer WS 2
journal, June 2017
- Sie, E. J.; Steinhoff, A.; Gies, C.
- Nano Letters, Vol. 17, Issue 7
Rashba Effect in a Single Colloidal CsPbBr 3 Perovskite Nanocrystal Detected by Magneto-Optical Measurements
journal, July 2017
- Isarov, Maya; Tan, Liang Z.; Bodnarchuk, Maryna I.
- Nano Letters, Vol. 17, Issue 8
High-Yield Exfoliation of Monolayer 1T’-MoTe2 as Saturable Absorber for Ultrafast Photonics
journal, October 2021
- Yu, Wei; Dong, Zikai; Abdelwahab, Ibrahim
- ACS Nano, Vol. 15, Issue 11
Highly Spin-Polarized Carrier Dynamics and Ultralarge Photoinduced Magnetization in CH 3 NH 3 PbI 3 Perovskite Thin Films
journal, February 2015
- Giovanni, David; Ma, Hong; Chua, Julianto
- Nano Letters, Vol. 15, Issue 3
Intervalley polaronic biexcitons in metal halide perovskite quantum dots
journal, October 2021
- Poonia, Ajay K.; Shrivastava, Megha; Mir, Wasim J.
- Physical Review B, Vol. 104, Issue 16
Coherent spin dynamics of electrons and holes in CsPbBr3 perovskite crystals
journal, February 2019
- Belykh, Vasilii V.; Yakovlev, Dmitri R.; Glazov, Mikhail M.
- Nature Communications, Vol. 10, Issue 1
Room‐Temperature Magnetic Field Effect on Excitonic Photoluminescence in Perovskite Nanocrystals
journal, June 2021
- Zhang, Kun; Zhao, Jian; Hu, Qingsong
- Advanced Materials, Vol. 33, Issue 30
Observation of Intervalley Biexcitonic Optical Stark Effect in Monolayer WS 2
journal, November 2016
- Sie, Edbert J.; Lui, Chun Hung; Lee, Yi-Hsien
- Nano Letters, Vol. 16, Issue 12
Population inversion and giant bandgap renormalization in atomically thin WS2 layers
journal, June 2015
- Chernikov, Alexey; Ruppert, Claudia; Hill, Heather M.
- Nature Photonics, Vol. 9, Issue 7
Exciton fission in monolayer transition metal dichalcogenide semiconductors
journal, October 2017
- Steinhoff, A.; Florian, M.; Rösner, M.
- Nature Communications, Vol. 8, Issue 1
Valley-selective optical Stark effect in monolayer WS2
journal, December 2014
- Sie, Edbert J.; McIver, James W.; Lee, Yi-Hsien
- Nature Materials, Vol. 14, Issue 3
Investigation of Exciton-Plasma Mott Transition in Si
journal, June 1977
- Shah, Jagdeep; Combescot, M.; Dayem, A. H.
- Physical Review Letters, Vol. 38, Issue 25
Bright triplet excitons in caesium lead halide perovskites
journal, January 2018
- Becker, Michael A.; Vaxenburg, Roman; Nedelcu, Georgian
- Nature, Vol. 553, Issue 7687
Resonant optical Stark effect in monolayer WS2
journal, December 2019
- Cunningham, Paul D.; Hanbicki, Aubrey T.; Reinecke, Thomas L.
- Nature Communications, Vol. 10, Issue 1
Biexciton fine structure in monolayer transition metal dichalcogenides
journal, October 2018
- Steinhoff, Alexander; Florian, Matthias; Singh, Akshay
- Nature Physics, Vol. 14, Issue 12
The ground exciton state of formamidinium lead bromide perovskite nanocrystals is a singlet dark state
journal, May 2019
- Tamarat, Philippe; Bodnarchuk, Maryna I.; Trebbia, Jean-Baptiste
- Nature Materials, Vol. 18, Issue 7
State of the Art and Prospects for Halide Perovskite Nanocrystals
journal, June 2021
- Dey, Amrita; Ye, Junzhi; De, Apurba
- ACS Nano, Vol. 15, Issue 7
High Defect Tolerance in Lead Halide Perovskite CsPbBr 3
journal, January 2017
- Kang, Jun; Wang, Lin-Wang
- The Journal of Physical Chemistry Letters, Vol. 8, Issue 2
Experimental observation of spin-dependent electron many-body effects in CdTe
journal, August 2014
- Horodyská, P.; Němec, P.; Novotný, T.
- Journal of Applied Physics, Vol. 116, Issue 5
Intervalley biexcitons and many-body effects in monolayer
journal, September 2015
- Sie, Edbert J.; Frenzel, Alex J.; Lee, Yi-Hsien
- Physical Review B, Vol. 92, Issue 12
Room-Temperature Anomalous Coherent Excitonic Optical Stark Effect in Metal Halide Perovskite Quantum Dots
journal, January 2022
- Shrivastava, Megha; Krieg, Franziska; Mandal, Dipendranath
- Nano Letters, Vol. 22, Issue 2
Strong spin-orbit coupling inducing Autler-Townes effect in lead halide perovskite nanocrystals
journal, May 2021
- Yumoto, Go; Hirori, Hideki; Sekiguchi, Fumiya
- Nature Communications, Vol. 12, Issue 1
Effect of Composition on the Spin Relaxation of Lead Halide Perovskites
journal, February 2020
- Zhou, Meng; Sarmiento, Julio S.; Fei, Chengbin
- The Journal of Physical Chemistry Letters, Vol. 11, Issue 4
Setting an Upper Bound to the Biexciton Binding Energy in CsPbBr 3 Perovskite Nanocrystals
journal, August 2019
- Shulenberger, Katherine E.; Ashner, Matthew N.; Ha, Seung Kyun
- The Journal of Physical Chemistry Letters, Vol. 10, Issue 18
Strong Spin-Selective Optical Stark Effect in Lead Halide Perovskite Quantum Dots
journal, April 2020
- Li, Yulu; He, Shan; Luo, Xiao
- The Journal of Physical Chemistry Letters, Vol. 11, Issue 9
Ultrafast Exciton Dynamics in Colloidal CsPbBr 3 Perovskite Nanocrystals: Biexciton Effect and Auger Recombination
journal, February 2017
- Aneesh, J.; Swarnkar, Abhishek; Kumar Ravi, Vikash
- The Journal of Physical Chemistry C, Vol. 121, Issue 8
Room temperature long-range coherent exciton polariton condensate flow in lead halide perovskites
journal, October 2018
- Su, Rui; Wang, Jun; Zhao, Jiaxin
- Science Advances, Vol. 4, Issue 10
Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
journal, August 2014
- Ugeda, Miguel M.; Bradley, Aaron J.; Shi, Su-Fei
- Nature Materials, Vol. 13, Issue 12
Spin band-gap renormalization and hole spin dynamics in Ge/SiGe quantum wells
journal, June 2012
- Lange, C.; Isella, G.; Chrastina, D.
- Physical Review B, Vol. 85, Issue 24
Dynamic polaronic screening for anomalous exciton spin relaxation in two-dimensional lead halide perovskites
journal, November 2020
- Tao, Weijian; Zhou, Qiaohui; Zhu, Haiming
- Science Advances, Vol. 6, Issue 47
Bose-Einstein condensation of excitons in a single quantum well
journal, March 2000
- Koinov, Z. G.
- Physical Review B, Vol. 61, Issue 12
Optical band gap and the Burstein–Moss effect in iodine doped PbTe using diffuse reflectance infrared Fourier transform spectroscopy
journal, July 2013
- Gibbs, Zachary M.; LaLonde, Aaron; Snyder, G. Jeffrey
- New Journal of Physics, Vol. 15, Issue 7
Atomlike interaction and optically tunable giant band-gap renormalization in large-area atomically thin
MoS 2
journal, November 2021
- Bera, Santu K.; Shrivastava, Megha; Bramhachari, Khamari
- Physical Review B, Vol. 104, Issue 20
Large polarization-dependent exciton optical Stark effect in lead iodide perovskites
journal, August 2016
- Yang, Ye; Yang, Mengjin; Zhu, Kai
- Nature Communications, Vol. 7, Issue 1
Lasing in Bose-Fermi mixtures
journal, January 2016
- Kochereshko, Vladimir P.; Durnev, Mikhail V.; Besombes, Lucien
- Scientific Reports, Vol. 6, Issue 1
Ultrafast exciton many-body interactions and hot-phonon bottleneck in colloidal cesium lead halide perovskite nanocrystals
journal, September 2018
- Mondal, Anirban; Aneesh, J.; Kumar Ravi, Vikash
- Physical Review B, Vol. 98, Issue 11
Spin Polarization Dynamics of Free Charge Carriers in CsPbI 3 Nanocrystals
journal, May 2020
- Strohmair, Simone; Dey, Amrita; Tong, Yu
- Nano Letters, Vol. 20, Issue 7
Tunable room-temperature spin-selective optical Stark effect in solution-processed layered halide perovskites
journal, June 2016
- Giovanni, David; Chong, Wee Kiang; Dewi, Herlina Arianita
- Science Advances, Vol. 2, Issue 6
Electrical Tuning of Exciton Binding Energies in Monolayer
journal, September 2015
- Chernikov, Alexey; van der Zande, Arend M.; Hill, Heather M.
- Physical Review Letters, Vol. 115, Issue 12
Visualizing the Anomalous Charge Density Wave States in Graphene/NbSe
2
Heterostructures
journal, October 2020
- Chen, Yu; Wu, Lishu; Xu, Hai
- Advanced Materials, Vol. 32, Issue 45
Size- and Composition-Dependent Exciton Spin Relaxation in Lead Halide Perovskite Quantum Dots
journal, April 2020
- Li, Yulu; Luo, Xiao; Liu, Yuan
- ACS Energy Letters, Vol. 5, Issue 5
Spin-dependent electron many-body effects in GaAs
journal, December 2005
- Nemec, P.; Kerachian, Y.; van Driel, H. M.
- Physical Review B, Vol. 72, Issue 24
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
Organic Cations Might Not Be Essential to the Remarkable Properties of Band Edge Carriers in Lead Halide Perovskites
journal, October 2016
- Zhu, Haiming; Trinh, M. Tuan; Wang, Jue
- Advanced Materials, Vol. 29, Issue 1
Polaron and Spin Dynamics in Organic–Inorganic Lead Halide Perovskite Nanocrystals
journal, October 2020
- Shrivastava, Megha; Bodnarchuk, Maryna I.; Hazarika, Abhijit
- Advanced Optical Materials, Vol. 8, Issue 24
Proximity Effects on the Charge Density Wave Order and Superconductivity in Single-Layer NbSe2
journal, November 2021
- Dreher, Paul; Wan, Wen; Chikina, Alla
- ACS Nano, Vol. 15, Issue 12
Biexcitonic optical Stark effects in monolayer molybdenum diselenide
journal, July 2018
- Yong, Chaw-Keong; Horng, Jason; Shen, Yuxia
- Nature Physics, Vol. 14, Issue 11
Mott Transition of Excitons in Coupled Quantum Wells
journal, June 2008
- Stern, M.; Garmider, V.; Umansky, V.
- Physical Review Letters, Vol. 100, Issue 25
Individual contribution of electrons and holes to photocarrier-induced bandgap renormalization in intrinsic bulk GaAs
journal, September 2020
- Chen, Yicun; Lu, Haiming; Lai, Tianshu
- Journal of Applied Physics, Vol. 128, Issue 11
Intensity of Optical Absorption by Excitons
journal, December 1957
- Elliott, R. J.
- Physical Review, Vol. 108, Issue 6
Transient circular dichroism and exciton spin dynamics in all-inorganic halide perovskites
journal, November 2020
- Zhao, Weijie; Su, Rui; Huang, Yuqing
- Nature Communications, Vol. 11, Issue 1
Band-gap renormalization in InP/Gax 1 − x
journal, June 2011
- Nowak, A. K.; Gallardo, E.; van der Meulen, H. P.
- Physical Review B, Vol. 83, Issue 24
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