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Title: Manipulating the Transition Dipole Moment of CsPbBr 3 Perovskite Nanocrystals for Superior Optical Properties

Abstract

Colloidal cesium lead halide perovskite nanocrystals exhibit unique photophysical properties including high quantum yields, tunable emission colors, and narrow photoluminescence spectra that have marked them as promising light emitters for applications in diverse photonic devices. Randomly oriented transition dipole moments have limited the light outcoupling efficiency of all isotropic light sources, including perovskites. In this report we design and synthesize deep blue emitting, quantum confined, perovskite nanoplates and analyze their optical properties by combining angular emission measurements with back focal plane imaging and correlating the results with physical characterization. By reducing the dimensions of the nanocrystals and depositing them face down onto a substrate by spin coating, we orient the average transition dipole moment of films into the plane of the substrate and improve the emission properties for light emitting applications. We then exploit the sensitivity of the perovskite electronic transitions to the dielectric environment at the interface between the crystal and their surroundings to reduce the angle between the average transition dipole moment and the surface to only 14° and maximize potential light emission efficiency. Furthermore, this tunability of the electronic transition that governs light emission in perovskites is unique and, coupled with their excellent photophysical properties, introduces amore » valuable method to extend the efficiencies and applications of perovskite based photonic devices beyond those based on current materials.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [5];  [5];  [2]; ORCiD logo [6];  [3];  [7];  [4]; ORCiD logo [8]; ORCiD logo [2]; ORCiD logo [1]
  1. Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
  2. Institute of Physics, University of Augsburg, 86135 Augsburg, Germany
  3. Department of Chemistry and Materials Science and Engineering, University of California, Berkeley, California 94720, United States
  4. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
  5. Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
  6. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States; Department of Chemistry and Materials Science and Engineering, University of California, Berkeley, California 94720, United States
  7. SSRL Materials Science Division, SLAC National Accelerator Laboratory, 2575 Sand Hill Rd MS 69, Menlo Park, California 94025, United States
  8. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States; Department of Chemistry and Materials Science and Engineering, University of California, Berkeley, California 94720, United States; Kavli Energy NanoScience Institute, Berkeley, California 94720, United States
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1503670
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 19; Journal Issue: 4; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 2D materials; anisotropic; back focal plane imaging; lead halide perovskite; LED; transition dipole moment

Citation Formats

Jurow, Matthew J., Morgenstern, Thomas, Eisler, Carissa, Kang, Jun, Penzo, Erika, Do, Mai, Engelmayer, Manuel, Osowiecki, Wojciech T., Bekenstein, Yehonadav, Tassone, Christopher, Wang, Lin-Wang, Alivisatos, A. Paul, Brütting, Wolfgang, and Liu, Yi. Manipulating the Transition Dipole Moment of CsPbBr 3 Perovskite Nanocrystals for Superior Optical Properties. United States: N. p., 2019. Web. doi:10.1021/acs.nanolett.9b00122.
Jurow, Matthew J., Morgenstern, Thomas, Eisler, Carissa, Kang, Jun, Penzo, Erika, Do, Mai, Engelmayer, Manuel, Osowiecki, Wojciech T., Bekenstein, Yehonadav, Tassone, Christopher, Wang, Lin-Wang, Alivisatos, A. Paul, Brütting, Wolfgang, & Liu, Yi. Manipulating the Transition Dipole Moment of CsPbBr 3 Perovskite Nanocrystals for Superior Optical Properties. United States. https://doi.org/10.1021/acs.nanolett.9b00122
Jurow, Matthew J., Morgenstern, Thomas, Eisler, Carissa, Kang, Jun, Penzo, Erika, Do, Mai, Engelmayer, Manuel, Osowiecki, Wojciech T., Bekenstein, Yehonadav, Tassone, Christopher, Wang, Lin-Wang, Alivisatos, A. Paul, Brütting, Wolfgang, and Liu, Yi. Fri . "Manipulating the Transition Dipole Moment of CsPbBr 3 Perovskite Nanocrystals for Superior Optical Properties". United States. https://doi.org/10.1021/acs.nanolett.9b00122. https://www.osti.gov/servlets/purl/1503670.
@article{osti_1503670,
title = {Manipulating the Transition Dipole Moment of CsPbBr 3 Perovskite Nanocrystals for Superior Optical Properties},
author = {Jurow, Matthew J. and Morgenstern, Thomas and Eisler, Carissa and Kang, Jun and Penzo, Erika and Do, Mai and Engelmayer, Manuel and Osowiecki, Wojciech T. and Bekenstein, Yehonadav and Tassone, Christopher and Wang, Lin-Wang and Alivisatos, A. Paul and Brütting, Wolfgang and Liu, Yi},
abstractNote = {Colloidal cesium lead halide perovskite nanocrystals exhibit unique photophysical properties including high quantum yields, tunable emission colors, and narrow photoluminescence spectra that have marked them as promising light emitters for applications in diverse photonic devices. Randomly oriented transition dipole moments have limited the light outcoupling efficiency of all isotropic light sources, including perovskites. In this report we design and synthesize deep blue emitting, quantum confined, perovskite nanoplates and analyze their optical properties by combining angular emission measurements with back focal plane imaging and correlating the results with physical characterization. By reducing the dimensions of the nanocrystals and depositing them face down onto a substrate by spin coating, we orient the average transition dipole moment of films into the plane of the substrate and improve the emission properties for light emitting applications. We then exploit the sensitivity of the perovskite electronic transitions to the dielectric environment at the interface between the crystal and their surroundings to reduce the angle between the average transition dipole moment and the surface to only 14° and maximize potential light emission efficiency. Furthermore, this tunability of the electronic transition that governs light emission in perovskites is unique and, coupled with their excellent photophysical properties, introduces a valuable method to extend the efficiencies and applications of perovskite based photonic devices beyond those based on current materials.},
doi = {10.1021/acs.nanolett.9b00122},
journal = {Nano Letters},
number = 4,
volume = 19,
place = {United States},
year = {Fri Mar 08 00:00:00 EST 2019},
month = {Fri Mar 08 00:00:00 EST 2019}
}

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Works referenced in this record:

The Bright Side of Perovskites
journal, October 2016

  • Colella, Silvia; Mazzeo, Marco; Rizzo, Aurora
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 21
  • DOI: 10.1021/acs.jpclett.6b01799

Perovskite photonic sources
journal, April 2016


Colloidal CsPbBr 3 Perovskite Nanocrystals: Luminescence beyond Traditional Quantum Dots
journal, November 2015

  • Swarnkar, Abhishek; Chulliyil, Ramya; Ravi, Vikash Kumar
  • Angewandte Chemie International Edition, Vol. 54, Issue 51
  • DOI: 10.1002/anie.201508276

Study of Perovskite QD Down-Converted LEDs and Six-Color White LEDs for Future Displays with Excellent Color Performance
journal, July 2016

  • Yoon, Hee Chang; Kang, Heejoon; Lee, Soyoung
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 28
  • DOI: 10.1021/acsami.6b05468

General Strategy for the Preparation of Stable Luminous Nanocomposite Inks Using Chemically Addressable CsPbX 3 Peroskite Nanocrystals
journal, March 2018


What future for quantum dot-based light emitters?
journal, December 2015


Nanocrystals of Cesium Lead Halide Perovskites (CsPbX 3 , X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut
journal, February 2015

  • Protesescu, Loredana; Yakunin, Sergii; Bodnarchuk, Maryna I.
  • Nano Letters, Vol. 15, Issue 6
  • DOI: 10.1021/nl5048779

Highly Luminescent Colloidal Nanoplates of Perovskite Cesium Lead Halide and Their Oriented Assemblies
journal, December 2015

  • Bekenstein, Yehonadav; Koscher, Brent A.; Eaton, Samuel W.
  • Journal of the American Chemical Society, Vol. 137, Issue 51
  • DOI: 10.1021/jacs.5b11199

Genesis, challenges and opportunities for colloidal lead halide perovskite nanocrystals
journal, February 2018

  • Akkerman, Quinten A.; Rainò, Gabriele; Kovalenko, Maksym V.
  • Nature Materials, Vol. 17, Issue 5
  • DOI: 10.1038/s41563-018-0018-4

Benzoyl Halides as Alternative Precursors for the Colloidal Synthesis of Lead-Based Halide Perovskite Nanocrystals
journal, January 2018

  • Imran, Muhammad; Caligiuri, Vincenzo; Wang, Mengjiao
  • Journal of the American Chemical Society, Vol. 140, Issue 7
  • DOI: 10.1021/jacs.7b13477

Colloidal Synthesis of Quantum Confined Single Crystal CsPbBr 3 Nanosheets with Lateral Size Control up to the Micrometer Range
journal, June 2016

  • Shamsi, Javad; Dang, Zhiya; Bianchini, Paolo
  • Journal of the American Chemical Society, Vol. 138, Issue 23
  • DOI: 10.1021/jacs.6b03166

Solution-Phase Synthesis of Cesium Lead Halide Perovskite Nanowires
journal, July 2015

  • Zhang, Dandan; Eaton, Samuel W.; Yu, Yi
  • Journal of the American Chemical Society, Vol. 137, Issue 29
  • DOI: 10.1021/jacs.5b05404

Origin of the stability of two-dimensional perovskites: a first-principles study
journal, January 2018

  • Yang, Yi; Gao, Fei; Gao, Shiwu
  • Journal of Materials Chemistry A, Vol. 6, Issue 30
  • DOI: 10.1039/C8TA01496E

Boosting Tunable Blue Luminescence of Halide Perovskite Nanoplatelets through Postsynthetic Surface Trap Repair
journal, July 2018


High Defect Tolerance in Lead Halide Perovskite CsPbBr 3
journal, January 2017


Highly Dynamic Ligand Binding and Light Absorption Coefficient of Cesium Lead Bromide Perovskite Nanocrystals
journal, January 2016


Tunable Anisotropic Photon Emission from Self-Organized CsPbBr 3 Perovskite Nanocrystals
journal, June 2017


Mirrors of Bonding in Metal Halide Perovskites
journal, September 2018

  • Goesten, Maarten G.; Hoffmann, Roald
  • Journal of the American Chemical Society, Vol. 140, Issue 40
  • DOI: 10.1021/jacs.8b08038

Band Gap Tuning of CH 3 NH 3 Pb(Br 1– x Cl x ) 3 Hybrid Perovskite for Blue Electroluminescence
journal, June 2015

  • Kumawat, Naresh K.; Dey, Amrita; Kumar, Aravindh
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 24
  • DOI: 10.1021/acsami.5b02159

Electron–phonon interaction in efficient perovskite blue emitters
journal, May 2018


Single-Layer Halide Perovskite Light-Emitting Diodes with Sub-Band Gap Turn-On Voltage and High Brightness
journal, October 2016

  • Li, Junqiang; Shan, Xin; Bade, Sri Ganesh R.
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 20
  • DOI: 10.1021/acs.jpclett.6b01942

50-Fold EQE Improvement up to 6.27% of Solution-Processed All-Inorganic Perovskite CsPbBr 3 QLEDs via Surface Ligand Density Control
journal, November 2016


Quantum Dot Light-Emitting Diodes Based on Inorganic Perovskite Cesium Lead Halides (CsPbX 3 )
journal, October 2015


Highly Efficient Light-Emitting Diodes of Colloidal Metal–Halide Perovskite Nanocrystals beyond Quantum Size
journal, June 2017


Ligand Engineering to Improve the Luminance Efficiency of CsPbBr 3 Nanocrystal Based Light-Emitting Diodes
journal, December 2017

  • Kumawat, Naresh Kumar; Swarnkar, Abhishek; Nag, Angshuman
  • The Journal of Physical Chemistry C, Vol. 122, Issue 25
  • DOI: 10.1021/acs.jpcc.8b00723

High-efficiency perovskite–polymer bulk heterostructure light-emitting diodes
journal, November 2018


Bright triplet excitons in caesium lead halide perovskites
journal, January 2018

  • Becker, Michael A.; Vaxenburg, Roman; Nedelcu, Georgian
  • Nature, Vol. 553, Issue 7687
  • DOI: 10.1038/nature25147

Emitter Orientation as a Key Parameter in Organic Light-Emitting Diodes
journal, September 2017


Organic Light-Emitting Diodes with 30% External Quantum Efficiency Based on a Horizontally Oriented Emitter
journal, March 2013

  • Kim, Sei-Yong; Jeong, Won-Ik; Mayr, Christian
  • Advanced Functional Materials, Vol. 23, Issue 31
  • DOI: 10.1002/adfm.201300104

Crystal Organic Light-Emitting Diodes with Perfectly Oriented Non-Doped Pt-Based Emitting Layer
journal, February 2016

  • Kim, Kwon-Hyeon; Liao, Jia-Ling; Lee, Si Woo
  • Advanced Materials, Vol. 28, Issue 13
  • DOI: 10.1002/adma.201504451

Understanding and predicting the orientation of heteroleptic phosphors in organic light-emitting materials
journal, October 2015

  • Jurow, Matthew J.; Mayr, Christian; Schmidt, Tobias D.
  • Nature Materials, Vol. 15, Issue 1
  • DOI: 10.1038/nmat4428

Solution-processed, high-performance light-emitting diodes based on quantum dots
journal, October 2014

  • Dai, Xingliang; Zhang, Zhenxing; Jin, Yizheng
  • Nature, Vol. 515, Issue 7525
  • DOI: 10.1038/nature13829

The Evolution of Quantum Confinement in CsPbBr 3 Perovskite Nanocrystals
journal, April 2017


Colloidal Halide Perovskite Nanoplatelets: An Exciting New Class of Semiconductor Nanomaterials
journal, May 2017


Color-Pure Violet-Light-Emitting Diodes Based on Layered Lead Halide Perovskite Nanoplates
journal, June 2016


On the crystal structure of colloidally prepared CsPbBr 3 quantum dots
journal, January 2016

  • Cottingham, Patrick; Brutchey, Richard L.
  • Chemical Communications, Vol. 52, Issue 30
  • DOI: 10.1039/C6CC01088A

Characterizing Photon Reabsorption in Quantum Dot-Polymer Composites for Use as Displacement Sensors
journal, January 2017


Small-Angle Scattering from Polymeric Mass Fractals of Arbitrary Mass-Fractal Dimension
journal, April 1996


CdSe Nanoplatelet Films with Controlled Orientation of their Transition Dipole Moment
journal, May 2017


Fluorescence near interfaces: The role of photonic mode density
journal, April 1998


Increased light outcoupling efficiency in dye-doped small molecule organic light-emitting diodes with horizontally oriented emitters
journal, May 2011


Orientation of luminescent excitons in layered nanomaterials
journal, March 2013

  • Schuller, Jon A.; Karaveli, Sinan; Schiros, Theanne
  • Nature Nanotechnology, Vol. 8, Issue 4
  • DOI: 10.1038/nnano.2013.20

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
  • DOI: 10.1038/ncomms9056

Light–Matter Interactions in Cesium Lead Halide Perovskite Nanowire Lasers
journal, September 2016

  • Park, Kidong; Lee, Jong Woon; Kim, Jun Dong
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 18
  • DOI: 10.1021/acs.jpclett.6b01821

Densities and refractive indices of pure organic acids as a function of temperature
journal, April 1990

  • Bernardo-Gil, Gabriela; Esquivel, Mercedes; Ribeiro, Albertina
  • Journal of Chemical & Engineering Data, Vol. 35, Issue 2
  • DOI: 10.1021/je00060a032

CsPbBr 3 QD/AlO x Inorganic Nanocomposites with Exceptional Stability in Water, Light, and Heat
journal, June 2017

  • Loiudice, Anna; Saris, Seryio; Oveisi, Emad
  • Angewandte Chemie International Edition, Vol. 56, Issue 36
  • DOI: 10.1002/anie.201703703

High‐Efficiency Deep‐Blue‐Emitting Organic Light‐Emitting Diodes Based on Iridium(III) Carbene Complexes
journal, August 2018

  • Pal, Amlan K.; Krotkus, Simonas; Fontani, Mattia
  • Advanced Materials, Vol. 30, Issue 50
  • DOI: 10.1002/adma.201804231

Rational Molecular Design for Deep‐Blue Thermally Activated Delayed Fluorescence Emitters
journal, January 2018

  • Chan, Chin‐Yiu; Cui, Lin‐Song; Kim, Jong Uk
  • Advanced Functional Materials, Vol. 28, Issue 11
  • DOI: 10.1002/adfm.201706023

Colloidal nanoplatelets with two-dimensional electronic structure
journal, October 2011

  • Ithurria, S.; Tessier, M. D.; Mahler, B.
  • Nature Materials, Vol. 10, Issue 12
  • DOI: 10.1038/nmat3145

Device efficiency of organic light-emitting diodes: Progress by improved light outcoupling
journal, September 2012

  • Brütting, Wolfgang; Frischeisen, Jörg; Schmidt, Tobias D.
  • physica status solidi (a), Vol. 210, Issue 1
  • DOI: 10.1002/pssa.201228320

Dipole radiation within one-dimensional anisotropic microcavities: a simulation method
journal, January 2011

  • Penninck, Lieven; De Visschere, Patrick; Beeckman, Jeroen
  • Optics Express, Vol. 19, Issue 19
  • DOI: 10.1364/OE.19.018558

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
  • DOI: 10.1021/acs.jpclett.5b02597

Works referencing / citing this record:

Effect of dimensionality on the optical absorption properties of CsPbI 3 perovskite nanocrystals
journal, November 2019

  • Liu, Albert; Bonato, Luiz G.; Sessa, Francesco
  • The Journal of Chemical Physics, Vol. 151, Issue 19
  • DOI: 10.1063/1.5124399

Device Engineering for All-Inorganic Perovskite Light-Emitting Diodes
journal, July 2019

  • Luo, Dongxiang; Chen, Qizan; Qiu, Ying
  • Nanomaterials, Vol. 9, Issue 7
  • DOI: 10.3390/nano9071007

Scalable photonic sources using two-dimensional lead halide perovskite superlattices
journal, January 2020


Scalable photonic sources using two-dimensional lead halide perovskite superlattices
text, January 2020

  • Jakub, Jagielski,; F., Solari, Simon; Lucie, Jordan,
  • Nature Publishing Group
  • DOI: 10.21256/zhaw-19629

Scalable photonic sources using two-dimensional lead halide perovskite superlattices
text, January 2020


Device Engineering for All-Inorganic Perovskite Light-Emitting Diodes
journal, July 2019

  • Luo, Dongxiang; Chen, Qizan; Qiu, Ying
  • Nanomaterials, Vol. 9, Issue 7
  • DOI: 10.3390/nano9071007

Scalable photonic sources using two-dimensional lead halide perovskite superlattices
text, January 2020