Exciton Fine Structure in 2D Perovskites: The Out‐of‐Plane Excitonic State

Posmyk, Katarzyna; Dyksik, Mateusz; Surrente, Alessandro; Maude, Duncan K.; Zawadzka, Natalia; Babiński, Adam; Molas, Maciej R.; Paritmongkol, Watcharaphol; Mączka, Mirosław; Tisdale, William A.; Plochocka, Paulina; Baranowski, Michał

doi:10.1002/adom.202300877

Exciton Fine Structure in 2D Perovskites: The Out‐of‐Plane Excitonic State (in EN)

Journal Article · Sun Jul 23 00:00:00 EDT 2023 · Advanced Optical Materials

DOI:https://doi.org/10.1002/adom.202300877· OSTI ID:2575787

^[1]; ^[2]; ^[2]; Maude, Duncan K. ^[3]; Zawadzka, Natalia ^[4]; ^[4]; ^[4]; ^[5]; ^[6]; ^[5]; ^[1]; ^[2]

Wroclaw Univ. of Science and Technology (Poland); Laboratoire National des Champs Magnétiques Intenses (LNCMI), Grenoble (France)
Wroclaw Univ. of Science and Technology (Poland)
Laboratoire National des Champs Magnétiques Intenses (LNCMI), Grenoble (France)
Univ. of Warsaw (Poland)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Polish Academy of Sciences (PAS), Wrocław (Poland)

2D Ruddlesden‐Popper metal‐halide perovskites feature particularly strong excitonic effects, making them a fascinating playground for studying exciton physics. A complete understanding of the properties of this quasi‐particle is crucial to fully exploit the tremendous potential of 2D perovskites (2DP) in light emission applications. Despite intense investigations, some of the exciton properties remain elusive to date, for example, the energy‐ordering of the exciton states within the so‐called fine structure manifold. Using optical spectroscopy, it demonstrates that in the archetypical 2DP (PEA)₂PbI₄, in contradiction to theoretical predictions, the energy of the bright out‐of‐plane exciton state is higher than that of two in‐plane states. Having elucidated the order of exciton fine structure, it determines the g‐factor of the dark exciton transition, together with the values of the electron and hole g‐factors in the direction parallel to the c‐axis of the crystal. In this way, it provides for the first time, a complete picture of the exciton fine structure in (PEA)₂PbI₄ 2DP.

View Accepted Manuscript (DOE)

Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Agence Nationale de la Recherche

Grant/Contract Number:: SC0019345

OSTI ID:: 2575787

Journal Information:: Advanced Optical Materials, Journal Name: Advanced Optical Materials Journal Issue: 8 Vol. 12; ISSN 2195-1071

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: EN

References (57)

Band‐Edge Exciton Fine Structure and Exciton Recombination Dynamics in Single Crystals of Layered Hybrid Perovskites Fang, Hong‐Hua; Yang, Jie; Adjokatse, Sampson Advanced Functional Materials, Vol. 30, Issue 6 https://doi.org/10.1002/adfm.201907979	journal	December 2019
2D Ruddlesden-Popper Perovskites for Optoelectronics Chen, Yani; Sun, Yong; Peng, Jiajun Advanced Materials, Vol. 30, Issue 2 https://doi.org/10.1002/adma.201703487	journal	October 2017
Exciton Ground State Fine Structure and Excited States Landscape in Layered Halide Perovskites from Combined BSE Simulations and Symmetry Analysis Quarti, Claudio; Giorgi, Giacomo; Katan, Claudine Advanced Optical Materials https://doi.org/10.1002/adom.202202801	journal	February 2023
Dark and Bright Excitons in Halide Perovskite Nanoplatelets Gramlich, Moritz; Swift, Michael W.; Lampe, Carola Advanced Science https://doi.org/10.1002/advs.202103013	journal	December 2021
Exciton state in two-dimensional perovskite semiconductor (C10H21NH3)2PbI4 Ishihara, Teruya; Takahashi, Jun; Goto, Takenari Solid State Communications, Vol. 69, Issue 9 https://doi.org/10.1016/0038-1098(89)90935-6	journal	March 1989
Photoconductivity and electroluminescence in lead iodide based natural quantum well structures Hong, X.; Ishihara, T.; Nurmikko, A. V. Solid State Communications, Vol. 84, Issue 6 https://doi.org/10.1016/0038-1098(92)90210-Z	journal	November 1992
Magneto-optical study on the excitonic spectrum of (C6H13NH3)2PbI4 Kataoka, T.; Kondo, T.; Ito, R. Physica B: Condensed Matter, Vol. 184, Issue 1-4 https://doi.org/10.1016/0921-4526(93)90336-5	journal	February 1993
Synthetic Variation and Structural Trends in Layered Two-Dimensional Alkylammonium Lead Halide Perovskites Paritmongkol, Watcharaphol; Dahod, Nabeel S.; Stollmann, Alexia Chemistry of Materials, Vol. 31, Issue 15 https://doi.org/10.1021/acs.chemmater.9b01318	journal	July 2019
Excitons and Their Fine Structure in Lead Halide Perovskite Nanocrystals from Atomistic GW/BSE Calculations Biffi, Giulia; Cho, Yeongsu; Krahne, Roman The Journal of Physical Chemistry C, Vol. 127, Issue 4 https://doi.org/10.1021/acs.jpcc.2c07111	journal	January 2023
Revealing Excitonic Phonon Coupling in (PEA) ₂ (MA) _{n −1} Pb _n I _{3 n +1} 2D Layered Perovskites Urban, Joanna M.; Chehade, Gabriel; Dyksik, Mateusz The Journal of Physical Chemistry Letters, Vol. 11, Issue 15 https://doi.org/10.1021/acs.jpclett.0c01714	journal	June 2020
Two Origins of Broadband Emission in Multilayered 2D Lead Iodide Perovskites Paritmongkol, Watcharaphol; Powers, Eric R.; Dahod, Nabeel S. The Journal of Physical Chemistry Letters, Vol. 11, Issue 20 https://doi.org/10.1021/acs.jpclett.0c02214	journal	September 2020
Tuning the Excitonic Properties of the 2D (PEA) ₂ (MA) _{n −1} Pb _n I _{3 n +1} Perovskite Family via Quantum Confinement Dyksik, Mateusz; Wang, Shuli; Paritmongkol, Watcharaphol The Journal of Physical Chemistry Letters, Vol. 12, Issue 6 https://doi.org/10.1021/acs.jpclett.0c03731	journal	February 2021
Quantification of Exciton Fine Structure Splitting in a Two-Dimensional Perovskite Compound Posmyk, Katarzyna; Zawadzka, Natalia; Dyksik, Mateusz The Journal of Physical Chemistry Letters, Vol. 13, Issue 20 https://doi.org/10.1021/acs.jpclett.2c00942	journal	May 2022
Unraveling the Exciton Binding Energy and the Dielectric Constant in Single-Crystal Methylammonium Lead Triiodide Perovskite Yang, Zhuo; Surrente, Alessandro; Galkowski, Krzysztof The Journal of Physical Chemistry Letters, Vol. 8, Issue 8 https://doi.org/10.1021/acs.jpclett.7b00524	journal	April 2017
Electrons, Excitons, and Phonons in Two-Dimensional Hybrid Perovskites: Connecting Structural, Optical, and Electronic Properties Straus, Daniel B.; Kagan, Cherie R. The Journal of Physical Chemistry Letters, Vol. 9, Issue 6 https://doi.org/10.1021/acs.jpclett.8b00201	journal	February 2018
Multiband k·p Model for Tetragonal Crystals: Application to Hybrid Halide Perovskite Nanocrystals Ben Aich, R.; Ben Radhia, S.; Boujdaria, K. The Journal of Physical Chemistry Letters, Vol. 11, Issue 3 https://doi.org/10.1021/acs.jpclett.9b02179	journal	January 2020
Exciton Polarons in Two-Dimensional Hybrid Metal-Halide Perovskites Srimath Kandada, Ajay Ram; Silva, Carlos The Journal of Physical Chemistry Letters, Vol. 11, Issue 9 https://doi.org/10.1021/acs.jpclett.9b02342	journal	March 2020
Bright Exciton Fine-Structure in Two-Dimensional Lead Halide Perovskites Do, T. Thu Ha; Granados del Águila, Andrés; Zhang, Dong Nano Letters, Vol. 20, Issue 7 https://doi.org/10.1021/acs.nanolett.0c01364	journal	May 2020
Thickness-Dependent Dark-Bright Exciton Splitting and Phonon Bottleneck in CsPbBr₃-Based Nanoplatelets Revealed via Magneto-Optical Spectroscopy Wang, Shuli; Dyksik, Mateusz; Lampe, Carola Nano Letters, Vol. 22, Issue 17 https://doi.org/10.1021/acs.nanolett.2c01826	journal	August 2022
Revealing Giant Exciton Fine-Structure Splitting in Two-Dimensional Perovskites Using van der Waals Passivation Canet-Albiach, Rodolfo; Kreĉmarová, Marie; Bailach, José Bosch Nano Letters, Vol. 22, Issue 18 https://doi.org/10.1021/acs.nanolett.2c02729	journal	September 2022
Coherent Spin Dynamics of Electrons in Two-Dimensional (PEA)₂PbI₄ Perovskites Kirstein, Erik; Zhukov, Evgeny A.; Yakovlev, Dmitri R. Nano Letters, Vol. 23, Issue 1 https://doi.org/10.1021/acs.nanolett.2c03975	journal	December 2022
Neutral and Charged Exciton Fine Structure in Single Lead Halide Perovskite Nanocrystals Revealed by Magneto-optical Spectroscopy Fu, Ming; Tamarat, Philippe; Huang, He Nano Letters, Vol. 17, Issue 5 https://doi.org/10.1021/acs.nanolett.7b00064	journal	April 2017
Exciton Fine Structure in Perovskite Nanocrystals Sercel, Peter C.; Lyons, John L.; Wickramaratne, Darshana Nano Letters, Vol. 19, Issue 6 https://doi.org/10.1021/acs.nanolett.9b01467	journal	April 2019
Giant Fine Structure Splitting of the Bright Exciton in a Bulk MAPbBr₃ Single Crystal Baranowski, Michał; Galkowski, Krzysztof; Surrente, Alessandro Nano Letters, Vol. 19, Issue 10 https://doi.org/10.1021/acs.nanolett.9b02520	journal	September 2019
Broad Tunability of Carrier Effective Masses in Two-Dimensional Halide Perovskites Dyksik, Mateusz; Duim, Herman; Zhu, Xiangzhou ACS Energy Letters, Vol. 5, Issue 11 https://doi.org/10.1021/acsenergylett.0c01758	journal	October 2020
Excitonic and Polaronic Properties of 2D Hybrid Organic–Inorganic Perovskites Yin, Jun; Li, Hong; Cortecchia, Daniele ACS Energy Letters, Vol. 2, Issue 2 https://doi.org/10.1021/acsenergylett.6b00659	journal	January 2017
Toward Engineering Intrinsic Line Widths and Line Broadening in Perovskite Nanoplatelets Liu, Albert; Nagamine, Gabriel; Bonato, Luiz G. ACS Nano, Vol. 15, Issue 4 https://doi.org/10.1021/acsnano.0c09244	journal	March 2021
Excitons at the Phase Transition of 2D Hybrid Perovskites Ziegler, Jonas D.; Lin, Kai-Qiang; Meisinger, Barbara ACS Photonics, Vol. 9, Issue 11 https://doi.org/10.1021/acsphotonics.2c01035	journal	October 2022
Tunable Out-of-Plane Excitons in 2D Single-Crystal Perovskites Fieramosca, Antonio; De Marco, Luisa; Passoni, Marco ACS Photonics, Vol. 5, Issue 10 https://doi.org/10.1021/acsphotonics.8b00984	journal	September 2018
Direct Observation of Electron–Phonon Coupling and Slow Vibrational Relaxation in Organic–Inorganic Hybrid Perovskites Straus, Daniel B.; Hurtado Parra, Sebastian; Iotov, Natasha Journal of the American Chemical Society, Vol. 138, Issue 42 https://doi.org/10.1021/jacs.6b08175	journal	October 2016
A semiconductor source of triggered entangled photon pairs Stevenson, R. M.; Young, R. J.; Atkinson, P. Nature, Vol. 439, Issue 7073 https://doi.org/10.1038/nature04446	journal	January 2006
High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells Tsai, Hsinhan; Nie, Wanyi; Blancon, Jean-Christophe Nature, Vol. 536, Issue 7616 https://doi.org/10.1038/nature18306	journal	July 2016
Bright triplet excitons in caesium lead halide perovskites Becker, Michael A.; Vaxenburg, Roman; Nedelcu, Georgian Nature, Vol. 553, Issue 7687 https://doi.org/10.1038/nature25147	journal	January 2018
High-performance semiconductor quantum-dot single-photon sources Senellart, Pascale; Solomon, Glenn; White, Andrew Nature Nanotechnology, Vol. 12, Issue 11 https://doi.org/10.1038/nnano.2017.218	journal	November 2017
Spin-polarized exciton quantum beating in hybrid organic–inorganic perovskites Odenthal, Patrick; Talmadge, William; Gundlach, Nathan Nature Physics, Vol. 13, Issue 9 https://doi.org/10.1038/nphys4145	journal	May 2017
Scaling law for excitons in 2D perovskite quantum wells Blancon, J. -C.; Stier, A. V.; Tsai, H. Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04659-x	journal	June 2018
Exciton diffusion in two-dimensional metal-halide perovskites Seitz, Michael; Magdaleno, Alvaro J.; Alcázar-Cano, Nerea Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15882-w	journal	April 2020
Anomalous collapses of Nares Strait ice arches leads to enhanced export of Arctic sea ice Moore, G. W. K.; Howell, S. E. L.; Brady, M. Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-020-20314-w	journal	January 2021
The Landé factors of electrons and holes in lead halide perovskites: universal dependence on the band gap Kirstein, E.; Yakovlev, D. R.; Glazov, M. M. Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-30701-0	journal	June 2022
The ground exciton state of formamidinium lead bromide perovskite nanocrystals is a singlet dark state Tamarat, Philippe; Bodnarchuk, Maryna I.; Trebbia, Jean-Baptiste Nature Materials, Vol. 18, Issue 7 https://doi.org/10.1038/s41563-019-0364-x	journal	May 2019
Ultrastructural Characterization of the Lower Motor System in a Mouse Model of Krabbe Disease Cappello, Valentina; Marchetti, Laura; Parlanti, Paola Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/s41598-016-0001-8	journal	December 2016
Fine structure of excitons and electron–hole exchange energy in polymorphic CsPbBr ₃ single nanocrystals Ramade, Julien; Andriambariarijaona, Léon Marcel; Steinmetz, Violette Nanoscale, Vol. 10, Issue 14 https://doi.org/10.1039/C7NR09334A	journal	January 2018
On the optical anisotropy in 2D metal-halide perovskites Steger, Mark; Janke, Svenja M.; Sercel, Peter C. Nanoscale, Vol. 14, Issue 3 https://doi.org/10.1039/D1NR06899G	journal	January 2022
Perspective on the physics of two-dimensional perovskites in high magnetic field Surrente, Alessandro; Baranowski, Michał; Plochocka, Paulina Applied Physics Letters, Vol. 118, Issue 17 https://doi.org/10.1063/5.0048490	journal	April 2021
Polymorphous nature of cubic halide perovskites Zhao, Xin-Gang; Dalpian, Gustavo M.; Wang, Zhi Physical Review B, Vol. 101, Issue 15 https://doi.org/10.1103/PhysRevB.101.155137	journal	April 2020
Dielectric confinement effect on excitons in PbI 4 -based layered semiconductors Hong, X.; Ishihara, T.; Nurmikko, A. V. Physical Review B, Vol. 45, Issue 12 https://doi.org/10.1103/PhysRevB.45.6961	journal	March 1992
Huge exchange energy and fine structure of excitons in an organic-inorganic quantum well material Ema, K.; Umeda, K.; Toda, M. Physical Review B, Vol. 73, Issue 24 https://doi.org/10.1103/PhysRevB.73.241310	journal	June 2006
Optical orientation and alignment of excitons in ensembles of inorganic perovskite nanocrystals Nestoklon, M. O.; Goupalov, S. V.; Dzhioev, R. I. Physical Review B, Vol. 97, Issue 23 https://doi.org/10.1103/PhysRevB.97.235304	journal	June 2018
Bright-Exciton Fine-Structure Splittings in Single Perovskite Nanocrystals Yin, Chunyang; Chen, Liyang; Song, Nan Physical Review Letters, Vol. 119, Issue 2 https://doi.org/10.1103/PhysRevLett.119.026401	journal	July 2017
Exciton-polaron spectral structures in two-dimensional hybrid lead-halide perovskites Neutzner, Stefanie; Thouin, Félix; Cortecchia, Daniele Physical Review Materials, Vol. 2, Issue 6 https://doi.org/10.1103/PhysRevMaterials.2.064605	journal	June 2018
Quantifying anisotropic thermal transport in two-dimensional perovskite (PEA2PbI4) through cross-sectional scanning thermal microscopy Maiti, Abhishek; Agarwal, Khushboo; Gonzalez-Munoz, Sergio Physical Review Materials, Vol. 7, Issue 2 https://doi.org/10.1103/PhysRevMaterials.7.023801	journal	February 2023
Colloquium : Excitons in atomically thin transition metal dichalcogenides Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M. Reviews of Modern Physics, Vol. 90, Issue 2 https://doi.org/10.1103/RevModPhys.90.021001	journal	April 2018
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data Momma, Koichi; Izumi, Fujio Journal of Applied Crystallography, Vol. 44, Issue 6 https://doi.org/10.1107/S0021889811038970	journal	October 2011
Multidimensional coherent spectroscopy reveals triplet state coherences in cesium lead-halide perovskite nanocrystals Liu, Albert; Almeida, Diogo B.; Bonato, Luiz G. Science Advances, Vol. 7, Issue 1 https://doi.org/10.1126/sciadv.abb3594	journal	January 2021
Brightening of dark excitons in 2D perovskites Dyksik, Mateusz; Duim, Herman; Maude, Duncan K. Science Advances, Vol. 7, Issue 46 https://doi.org/10.1126/sciadv.abk0904	journal	November 2021
Electronic and Excitonic Structures of Inorganic–Organic Perovskite-Type Quantum-Well Crystal (C ₄ H ₉ NH ₃ ) ₂ PbBr ₄ Tanaka, Kenichiro; Takahashi, Takayuki; Kondo, Takashi Japanese Journal of Applied Physics, Vol. 44, Issue 8 https://doi.org/10.1143/JJAP.44.5923	journal	August 2005
Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)2PbI4 Two-Dimensional Perovskites Posmyk, Katarzyna; Dyksik, Mateusz; Surrente, Alessandro Nanomaterials, Vol. 13, Issue 6 https://doi.org/10.3390/nano13061119	journal	March 2023

Similar Records

Quantification of Exciton Fine Structure Splitting in a Two-Dimensional Perovskite Compound

Journal Article · Fri May 13 00:00:00 EDT 2022 · Journal of Physical Chemistry Letters · OSTI ID:1904339

Related Subjects

2D perovskites
excitons
fine structure splitting

Exciton Fine Structure in 2D Perovskites: The Out‐of‐Plane Excitonic State (in EN)

Citation Formats

References (57)

Similar Records

Related Subjects