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Title: Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells

Abstract

Solution-processed perovskite quantum wells have been utilized to fabricate increasingly efficient and stable optoelectronic devices. Little is known about the dynamics of photogenerated excitons in perovskite quantum wells within the first few hundred femtoseconds-a crucial time scale on which energy and charge transfer processes may compete. In this work we use ultrafast transient absorption and two-dimensional electronic spectroscopy to clarify the movement of excitons and charges in reduced-dimensional perovskite solids. We report excitonic funneling from strongly to weakly confined perovskite quantum wells within 150 fs, facilitated by strong spectral overlap and orientational alignment among neighboring wells. This energy transfer happens on time scales orders of magnitude faster than charge transfer, which we find to occur instead over 10s to 100s of picoseconds. Simulations of both Forster-type interwell exciton transfer and free carrier charge transfer are in agreement with these experimental results, with theoretical exciton transfer calculated to occur in 100s of femtoseconds.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [5];  [6]; ORCiD logo [7]; ORCiD logo [1]; ORCiD logo [2]
  1. Univ. of Toronto, ON (Canada)
  2. Princeton Univ., NJ (United States)
  3. Netherlands eScience Center, Amsterdam (Netherlands)
  4. Univ. of Electronic Science and Technology of China, Chengdu (China); Univ. of Quebec (Canada)
  5. Ohio Univ., Athens, OH (United States)
  6. Argonne National Lab. (ANL), Lemont, IL (United States)
  7. Vrije Univ., Amsterdam (Netherlands)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; Natural Sciences and Engineering Research Council of Canada (NSERC); Netherlands Organisation for Scientific Research (NWO); Canadian Institute for Advanced Research (CIFAR)
OSTI Identifier:
1557832
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 10; Journal Issue: 3; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; carrier dynamics; dynamics; energy transfer; layered perovskite; metal halide perovskite; two-dimensional electronic spectroscopy

Citation Formats

Proppe, Andrew H., Elkins, Madeline H., Voznyy, Oleksandr, Pensack, Ryan D., Zapata, Felipe, Besteiro, Lucas V., Quan, Li Na, Quintero-Bermudez, Rafael, Todorovic, Petar, Kelley, Shana O., Govorov, Alexander O., Gray, Stephen K., Infante, Ivan, Sargent, Edward H., and Scholes, Gregory D. Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells. United States: N. p., 2019. Web. doi:10.1021/acs.jpclett.9b00018.
Proppe, Andrew H., Elkins, Madeline H., Voznyy, Oleksandr, Pensack, Ryan D., Zapata, Felipe, Besteiro, Lucas V., Quan, Li Na, Quintero-Bermudez, Rafael, Todorovic, Petar, Kelley, Shana O., Govorov, Alexander O., Gray, Stephen K., Infante, Ivan, Sargent, Edward H., & Scholes, Gregory D. Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells. United States. https://doi.org/10.1021/acs.jpclett.9b00018
Proppe, Andrew H., Elkins, Madeline H., Voznyy, Oleksandr, Pensack, Ryan D., Zapata, Felipe, Besteiro, Lucas V., Quan, Li Na, Quintero-Bermudez, Rafael, Todorovic, Petar, Kelley, Shana O., Govorov, Alexander O., Gray, Stephen K., Infante, Ivan, Sargent, Edward H., and Scholes, Gregory D. Thu . "Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells". United States. https://doi.org/10.1021/acs.jpclett.9b00018. https://www.osti.gov/servlets/purl/1557832.
@article{osti_1557832,
title = {Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells},
author = {Proppe, Andrew H. and Elkins, Madeline H. and Voznyy, Oleksandr and Pensack, Ryan D. and Zapata, Felipe and Besteiro, Lucas V. and Quan, Li Na and Quintero-Bermudez, Rafael and Todorovic, Petar and Kelley, Shana O. and Govorov, Alexander O. and Gray, Stephen K. and Infante, Ivan and Sargent, Edward H. and Scholes, Gregory D.},
abstractNote = {Solution-processed perovskite quantum wells have been utilized to fabricate increasingly efficient and stable optoelectronic devices. Little is known about the dynamics of photogenerated excitons in perovskite quantum wells within the first few hundred femtoseconds-a crucial time scale on which energy and charge transfer processes may compete. In this work we use ultrafast transient absorption and two-dimensional electronic spectroscopy to clarify the movement of excitons and charges in reduced-dimensional perovskite solids. We report excitonic funneling from strongly to weakly confined perovskite quantum wells within 150 fs, facilitated by strong spectral overlap and orientational alignment among neighboring wells. This energy transfer happens on time scales orders of magnitude faster than charge transfer, which we find to occur instead over 10s to 100s of picoseconds. Simulations of both Forster-type interwell exciton transfer and free carrier charge transfer are in agreement with these experimental results, with theoretical exciton transfer calculated to occur in 100s of femtoseconds.},
doi = {10.1021/acs.jpclett.9b00018},
journal = {Journal of Physical Chemistry Letters},
number = 3,
volume = 10,
place = {United States},
year = {2019},
month = {1}
}

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Works referenced in this record:

Highly Tunable Colloidal Perovskite Nanoplatelets through Variable Cation, Metal, and Halide Composition
journal, July 2016


Quantum Size Effect in Organometal Halide Perovskite Nanoplatelets
journal, September 2015


Colloidal Organohalide Perovskite Nanoplatelets Exhibiting Quantum Confinement
journal, May 2015

  • Tyagi, Pooja; Arveson, Sarah M.; Tisdale, William A.
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 10
  • DOI: 10.1021/acs.jpclett.5b00664

2D Homologous Perovskites as Light-Absorbing Materials for Solar Cell Applications
journal, June 2015

  • Cao, Duyen H.; Stoumpos, Constantinos C.; Farha, Omar K.
  • Journal of the American Chemical Society, Vol. 137, Issue 24
  • DOI: 10.1021/jacs.5b03796

High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells
journal, July 2016

  • Tsai, Hsinhan; Nie, Wanyi; Blancon, Jean-Christophe
  • Nature, Vol. 536, Issue 7616
  • DOI: 10.1038/nature18306

Ligand-Stabilized Reduced-Dimensionality Perovskites
journal, February 2016

  • Quan, Li Na; Yuan, Mingjian; Comin, Riccardo
  • Journal of the American Chemical Society, Vol. 138, Issue 8
  • DOI: 10.1021/jacs.5b11740

Synthetic Control over Quantum Well Width Distribution and Carrier Migration in Low-Dimensional Perovskite Photovoltaics
journal, February 2018

  • Proppe, Andrew H.; Quintero-Bermudez, Rafael; Tan, Hairen
  • Journal of the American Chemical Society, Vol. 140, Issue 8
  • DOI: 10.1021/jacs.7b12551

One-Year stable perovskite solar cells by 2D/3D interface engineering
journal, June 2017

  • Grancini, G.; Roldán-Carmona, C.; Zimmermann, I.
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15684

Selective growth of layered perovskites for stable and efficient photovoltaics
journal, January 2018

  • Cho, Kyung Taek; Grancini, Giulia; Lee, Yonghui
  • Energy & Environmental Science, Vol. 11, Issue 4
  • DOI: 10.1039/C7EE03513F

Efficient ambient-air-stable solar cells with 2D–3D heterostructured butylammonium-caesium-formamidinium lead halide perovskites
journal, August 2017


Observation of Internal Photoinduced Electron and Hole Separation in Hybrid Two-Dimentional Perovskite Films
journal, January 2017

  • Liu, Junxue; Leng, Jing; Wu, Kaifeng
  • Journal of the American Chemical Society, Vol. 139, Issue 4
  • DOI: 10.1021/jacs.6b12581

Perovskite energy funnels for efficient light-emitting diodes
journal, June 2016

  • Yuan, Mingjian; Quan, Li Na; Comin, Riccardo
  • Nature Nanotechnology, Vol. 11, Issue 10
  • DOI: 10.1038/nnano.2016.110

Efficient Visible Quasi-2D Perovskite Light-Emitting Diodes
journal, June 2016

  • Byun, Jinwoo; Cho, Himchan; Wolf, Christoph
  • Advanced Materials, Vol. 28, Issue 34
  • DOI: 10.1002/adma.201601369

Amplified Spontaneous Emission Based on 2D Ruddlesden-Popper Perovskites
journal, February 2018

  • Li, Meili; Gao, Qinggang; Liu, Peng
  • Advanced Functional Materials, Vol. 28, Issue 17
  • DOI: 10.1002/adfm.201707006

Compositional and orientational control in metal halide perovskites of reduced dimensionality
journal, September 2018

  • Quintero-Bermudez, Rafael; Gold-Parker, Aryeh; Proppe, Andrew H.
  • Nature Materials, Vol. 17, Issue 10
  • DOI: 10.1038/s41563-018-0154-x

Excitonic Many-Body Interactions in Two-Dimensional Lead Iodide Perovskite Quantum Wells
journal, March 2015

  • Wu, Xiaoxi; Trinh, M. Tuan; Zhu, X. -Y.
  • The Journal of Physical Chemistry C, Vol. 119, Issue 26
  • DOI: 10.1021/acs.jpcc.5b00148

Glotaran : A Java -Based Graphical User Interface for the R Package TIMP
journal, January 2012

  • Snellenburg, Joris J.; Laptenok, Sergey P.; Seger, Ralf
  • Journal of Statistical Software, Vol. 49, Issue 3
  • DOI: 10.18637/jss.v049.i03

Photocarrier Recombination Dynamics in Perovskite CH 3 NH 3 PbI 3 for Solar Cell Applications
journal, August 2014

  • Yamada, Yasuhiro; Nakamura, Toru; Endo, Masaru
  • Journal of the American Chemical Society, Vol. 136, Issue 33
  • DOI: 10.1021/ja506624n

Unveiling Structurally Engineered Carrier Dynamics in Hybrid Quasi-Two-Dimensional Perovskite Thin Films toward Controllable Emission
journal, September 2017

  • Shang, Qiuyu; Wang, Yunuan; Zhong, Yangguang
  • The Journal of Physical Chemistry Letters, Vol. 8, Issue 18
  • DOI: 10.1021/acs.jpclett.7b01857

Layered 2D alkyldiammonium lead iodide perovskites: synthesis, characterization, and use in solar cells
journal, January 2016

  • Safdari, Majid; Svensson, Per H.; Hoang, Minh Tam
  • Journal of Materials Chemistry A, Vol. 4, Issue 40
  • DOI: 10.1039/C6TA05055G

Biexciton Resonances Reveal Exciton Localization in Stacked Perovskite Quantum Wells
journal, August 2017

  • Elkins, Madeline H.; Pensack, Ryan; Proppe, Andrew H.
  • The Journal of Physical Chemistry Letters, Vol. 8, Issue 16
  • DOI: 10.1021/acs.jpclett.7b01621

Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer
journal, July 2017

  • Duan, Hong-Guang; Prokhorenko, Valentyn I.; Cogdell, Richard J.
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 32
  • DOI: 10.1073/pnas.1702261114

Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides
journal, September 2015

  • Moody, Galan; Kavir Dass, Chandriker; Hao, Kai
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9315

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
  • DOI: 10.1038/s41467-017-00546-z

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
  • DOI: 10.1126/sciadv.1600477

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
  • DOI: 10.1038/ncomms12613

Perovskite light-emitting diodes based on solution-processed self-organized multiple quantum wells
journal, September 2016


Transcending the slow bimolecular recombination in lead-halide perovskites for electroluminescence
journal, February 2017

  • Xing, Guichuan; Wu, Bo; Wu, Xiangyang
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms14558

Dielectric confinement effect on excitons in PbI 4 -based layered semiconductors
journal, March 1992


Exciton state in two-dimensional perovskite semiconductor (C10H21NH3)2PbI4
journal, March 1989


Optical properties due to electronic transitions in two-dimensional semiconductors ( C n H 2 n + 1 NH 3 ) 2 PbI 4
journal, December 1990


Efficient exciton energy transfer between widely separated quantum wells at low temperatures
journal, April 1996


Energy transfer of excitons between quantum wells separated by a wide barrier
journal, November 2000


Evidence for Fast Interlayer Energy Transfer in MoSe 2 /WS 2 Heterostructures
journal, June 2016


Picosecond energy transfer and multiexciton transfer outpaces Auger recombination in binary CdSe nanoplatelet solids
journal, March 2015

  • Rowland, Clare E.; Fedin, Igor; Zhang, Hui
  • Nature Materials, Vol. 14, Issue 5
  • DOI: 10.1038/nmat4231

Beyond Förster Resonance Energy Transfer in Biological and Nanoscale Systems
journal, May 2009

  • Beljonne, David; Curutchet, Carles; Scholes, Gregory D.
  • The Journal of Physical Chemistry B, Vol. 113, Issue 19
  • DOI: 10.1021/jp900708f

L ONG -R ANGE R ESONANCE E NERGY T RANSFER IN M OLECULAR S YSTEMS
journal, October 2003


Excitons in ultrathin organic-inorganic perovskite crystals
journal, July 2015


Excitonic Properties of Chemically Synthesized 2D Organic-Inorganic Hybrid Perovskite Nanosheets
journal, March 2018


Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Lessons from nature about solar light harvesting
journal, September 2011

  • Scholes, Gregory D.; Fleming, Graham R.; Olaya-Castro, Alexandra
  • Nature Chemistry, Vol. 3, Issue 10
  • DOI: 10.1038/nchem.1145

Excitons in nanoscale systems
journal, September 2006

  • Scholes, Gregory D.; Rumbles, Garry
  • Nature Materials, Vol. 5, Issue 9
  • DOI: 10.1038/nmat1710

Low-Intensity Pump-Probe Measurements on the B800 Band of Rhodospirillum molischianum
journal, January 2003


Energy transfer within the bacteriochlorophyll antenna of purple bacteria at 77 K, studied by picosecond absorption recovery
journal, November 1987

  • van Grondelle, R.; Bergström, H.; Sundström, V.
  • Biochimica et Biophysica Acta (BBA) - Bioenergetics, Vol. 894, Issue 2
  • DOI: 10.1016/0005-2728(87)90201-5

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
  • DOI: 10.1021/acs.jpcc.7b00762

Molecularly Engineered Organic-Inorganic Hybrid Perovskite with Multiple Quantum Well Structure for Multicolored Light-Emitting Diodes
journal, September 2016

  • Hu, Hongwei; Salim, Teddy; Chen, Bingbing
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep33546

Direct Observation of Ultrafast Exciton Dissociation in Lead Iodide Perovskite by 2D Electronic Spectroscopy
journal, December 2017


Works referencing / citing this record:

Efficient near-infrared light-emitting diodes based on quantum dots in layered perovskite
journal, January 2020


Modeling nonadiabatic dynamics in condensed matter materials: some recent advances and applications
journal, November 2019

  • Smith, Brendan; Akimov, Alexey V.
  • Journal of Physics: Condensed Matter, Vol. 32, Issue 7
  • DOI: 10.1088/1361-648x/ab5246

Optimization of Low‐Dimensional Components of Quasi‐2D Perovskite Films for Deep‐Blue Light‐Emitting Diodes
journal, September 2019

  • Yuan, Shuai; Wang, Zhao‐Kui; Xiao, Lei‐Xin
  • Advanced Materials, Vol. 31, Issue 44
  • DOI: 10.1002/adma.201904319

Long-lived charge separation in two-dimensional ligand-perovskite heterostructures
journal, January 2020

  • Deng, Shibin; Snaider, Jordan M.; Gao, Yao
  • The Journal of Chemical Physics, Vol. 152, Issue 4
  • DOI: 10.1063/1.5131801

Large-area transparent flexible guanidinium incorporated MAPbI 3 microstructures for high-performance photodetectors with enhanced stability
journal, January 2020

  • Kumar, Gundam Sandeep; Sarkar, Piyush Kanti; Pradhan, Bapi
  • Nanoscale Horizons, Vol. 5, Issue 4
  • DOI: 10.1039/c9nh00774a