Scaling Laws of Exciton Recombination Kinetics in Low Dimensional Halide Perovskite Nanostructures

Gao, Mengyu; Liu, Hao; Yu, Sunmoon; Louisia, Sheena; Zhang, Ye; Nenon, David P.; Alivisatos, A. Paul; Yang, Peidong

doi:10.1021/jacs.0c02000

Title: Scaling Laws of Exciton Recombination Kinetics in Low Dimensional Halide Perovskite Nanostructures

Abstract

Carrier recombination is a crucial process governing the optical properties of a semiconductor. Although various theoretical approaches have been utilized to describe carrier behaviors, a quantitative understanding of the impact of defects and interfaces in low dimensional semiconductor systems is still elusive. Here, we develop a model system consisting of chemically tunable, highly luminescent halide perovskite nanocrystals to illustrate the role of carrier diffusion and material dimensionality on the carrier recombination kinetics and luminescence efficiency. Our advanced synthetic methods provide a well-controlled colloidal system consisting of nanocrystals with different aspect ratios, halide compositions, and surface conditions. Using this system, we reveal the scaling laws of photoluminescence quantum yield and radiative lifetime with respect to the aspect ratio of nanocrystals. The scaling laws derived herein are not only a phenomenological observation but proved a powerful tool disentangling the carrier dynamics of microscopic systems in a quantitative and interpretable manner. The investigation of our model system and theoretical formulation bring to light the dimensionality, as a hidden constraint on carrier dynamics, and identify the diffusion length as an important parameter that distinguishes nanoscale and macroscale carrier behaviors. Furthermore, the conceptual distinction in carrier dynamics in different dimensionality regimes informs new design rulesmore »« less

Authors:

^[1]; Liu, Hao ^[2];

^[1]; Louisia, Sheena ^[1]; Zhang, Ye ^[1];

^[1];

^[3];

^[3]

Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Inst., Berkeley, CA (United States)

Publication Date:: Thu Apr 16 00:00:00 EDT 2020

Research Org.:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1841154

Grant/Contract Number:: AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: Journal of the American Chemical Society

Additional Journal Information:: Journal Volume: 142; Journal Issue: 19; Journal ID: ISSN 0002-7863

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Excitons; Diffusion; Carrier dynamics; Defects; Perovskites

Citation Formats


                    Gao, Mengyu, Liu, Hao, Yu, Sunmoon, Louisia, Sheena, Zhang, Ye, Nenon, David P., Alivisatos, A. Paul, and Yang, Peidong. Scaling Laws of Exciton Recombination Kinetics in Low Dimensional Halide Perovskite Nanostructures.  United States: N. p., 2020. 
Web.  doi:10.1021/jacs.0c02000.

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                    Gao, Mengyu, Liu, Hao, Yu, Sunmoon, Louisia, Sheena, Zhang, Ye, Nenon, David P., Alivisatos, A. Paul, & Yang, Peidong. Scaling Laws of Exciton Recombination Kinetics in Low Dimensional Halide Perovskite Nanostructures.  United States.  https://doi.org/10.1021/jacs.0c02000

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                    Gao, Mengyu, Liu, Hao, Yu, Sunmoon, Louisia, Sheena, Zhang, Ye, Nenon, David P., Alivisatos, A. Paul, and Yang, Peidong. Thu .  
"Scaling Laws of Exciton Recombination Kinetics in Low Dimensional Halide Perovskite Nanostructures".  United States.  https://doi.org/10.1021/jacs.0c02000.  https://www.osti.gov/servlets/purl/1841154.

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@article{osti_1841154,

  title        = {Scaling Laws of Exciton Recombination Kinetics in Low Dimensional Halide Perovskite Nanostructures},

  author       = {Gao, Mengyu and Liu, Hao and Yu, Sunmoon and Louisia, Sheena and Zhang, Ye and Nenon, David P. and Alivisatos, A. Paul and Yang, Peidong},

  abstractNote = {Carrier recombination is a crucial process governing the optical properties of a semiconductor. Although various theoretical approaches have been utilized to describe carrier behaviors, a quantitative understanding of the impact of defects and interfaces in low dimensional semiconductor systems is still elusive. Here, we develop a model system consisting of chemically tunable, highly luminescent halide perovskite nanocrystals to illustrate the role of carrier diffusion and material dimensionality on the carrier recombination kinetics and luminescence efficiency. Our advanced synthetic methods provide a well-controlled colloidal system consisting of nanocrystals with different aspect ratios, halide compositions, and surface conditions. Using this system, we reveal the scaling laws of photoluminescence quantum yield and radiative lifetime with respect to the aspect ratio of nanocrystals. The scaling laws derived herein are not only a phenomenological observation but proved a powerful tool disentangling the carrier dynamics of microscopic systems in a quantitative and interpretable manner. The investigation of our model system and theoretical formulation bring to light the dimensionality, as a hidden constraint on carrier dynamics, and identify the diffusion length as an important parameter that distinguishes nanoscale and macroscale carrier behaviors. Furthermore, the conceptual distinction in carrier dynamics in different dimensionality regimes informs new design rules for optical devices where complex microstructures are involved.},

  doi          = {10.1021/jacs.0c02000},

  journal      = {Journal of the American Chemical Society},

  number       = 19,

  volume       = 142,

  place        = {United States},

  year         = {Thu Apr 16 00:00:00 EDT 2020},

  month        = {Thu Apr 16 00:00:00 EDT 2020}

}

Copy to clipboard

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Title: Scaling Laws of Exciton Recombination Kinetics in Low Dimensional Halide Perovskite Nanostructures

Abstract

Citation Formats

Random Walks on Lattices. III. Calculation of First‐Passage Times with Application to Exciton Trapping on Photosynthetic Units journal, April 1969

Extrinsic and Dynamic Edge States of Two-Dimensional Lead Halide Perovskites journal, February 2019

Synthesis of Composition Tunable and Highly Luminescent Cesium Lead Halide Nanowires through Anion-Exchange Reactions journal, June 2016

Essentially Trap-Free CsPbBr 3 Colloidal Nanocrystals by Postsynthetic Thiocyanate Surface Treatment journal, May 2017

A Solution NMR Toolbox for Characterizing the Surface Chemistry of Colloidal Nanocrystals journal, February 2013

Hybrid organic—inorganic perovskites: low-cost semiconductors with intriguing charge-transport properties journal, January 2016

Rashba Effect in a Single Colloidal CsPbBr 3 Perovskite Nanocrystal Detected by Magneto-Optical Measurements journal, July 2017

Zero-Dimensional and Quasi One-Dimensional Effects in Semiconductor Nanorods journal, May 2004

Aspect Ratio Dependence of Auger Recombination and Carrier Multiplication in PbSe Nanorods journal, February 2013

Quantitative imaging of anion exchange kinetics in halide perovskites journal, June 2019

The emergence of perovskite solar cells journal, July 2014

Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals journal, January 2015

Perovskite light-emitting diodes with external quantum efficiency exceeding 20 per cent journal, October 2018

Melting in Semiconductor Nanocrystals journal, June 1992

Composition-dependent photoluminescence intensity and prolonged recombination lifetime of perovskite CH 3 NH 3 PbBr 3−x Cl x films journal, January 2014

Exciton Recombination in Formamidinium Lead Triiodide: Nanocrystals versus Thin Films journal, June 2017

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

Perspectives on the Physical Chemistry of Semiconductor Nanocrystals journal, January 1996

The Role of Length and Defects on Optical Quantum Efficiency and Exciton Decay Dynamics in Single-Walled Carbon Nanotubes journal, December 2010

High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization journal, July 2015

Visualizing Carrier Diffusion in Individual Single-Crystal Organolead Halide Perovskite Nanowires and Nanoplates journal, September 2015

Interfacial Synthesis of Monodisperse CsPbBr 3 Nanorods with Tunable Aspect Ratio and Clean Surface for Efficient Light-Emitting Diode Applications journal, February 2019

Synthesis and Properties of CdSe/ZnS Core/Shell Nanorods journal, September 2003

Spatially resolved multicolor CsPbX 3 nanowire heterojunctions via anion exchange journal, June 2017

Role of microstructure in the electron–hole interaction of hybrid lead halide perovskites journal, August 2015

Recombination Kinetics in Organic-Inorganic Perovskites: Excitons, Free Charge, and Subgap States journal, September 2014

Exciton Diffusion in Air-Suspended Single-Walled Carbon Nanotubes journal, June 2010

All-inorganic perovskite nanocrystal scintillators journal, August 2018

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

Quantum-size effects on radiative lifetimes and relaxation of excitons in semiconductor nanostructures journal, October 1998

CdSe Nanorod Synthesis: A New Approach journal, November 2007

Controlling the influence of Auger recombination on the performance of quantum-dot light-emitting diodes journal, October 2013

Theoretical study of time-resolved luminescence in semiconductors. III. Trap states in the band gap journal, September 2015

Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites journal, March 2017

Understanding the physical properties of hybrid perovskites for photovoltaic applications journal, July 2017

Spectral and Dynamical Properties of Single Excitons, Biexcitons, and Trions in Cesium–Lead-Halide Perovskite Quantum Dots journal, March 2016

Exciton diffusion, end quenching, and exciton-exciton annihilation in individual air-suspended carbon nanotubes journal, March 2015

Ligand Control of Growth, Morphology, and Capping Structure of Colloidal CdSe Nanorods journal, May 2007

Size Dependence of a First Order Solid-Solid Phase Transition: The Wurtzite to Rock Salt Transformation in CdSe Nanocrystals journal, July 1994

Quantum Dot Luminescent Concentrator Cavity Exhibiting 30-fold Concentration journal, August 2015

Shape control of CdSe nanocrystals journal, March 2000

Enhanced thermoelectric performance of rough silicon nanowires journal, January 2008

Impact of microstructure on local carrier lifetime in perovskite solar cells journal, April 2015

Perovskite light-emitting diodes based on spontaneously formed submicrometre-scale structures journal, October 2018

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

Fast Anion-Exchange in Highly Luminescent Nanocrystals of Cesium Lead Halide Perovskites (CsPbX 3 , X = Cl, Br, I) journal, July 2015

Charge-Carrier Dynamics in Organic-Inorganic Metal Halide Perovskites journal, May 2016

Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber journal, October 2013

Long-Range Balanced Electron- and Hole-Transport Lengths in Organic-Inorganic CH3NH3PbI3 journal, October 2013

Bandgap engineering in semiconductor alloy nanomaterials with widely tunable compositions journal, October 2017

Diffusion Limited Photoluminescence Quantum Yields in 1-D Semiconductors: Single-Wall Carbon Nanotubes journal, November 2010

Coherent single-photon emission from colloidal lead halide perovskite quantum dots journal, February 2019

Recombination in amorphous materials as a continuous-time random-walk problem journal, March 1983

Delayed Exciton Emission and Its Relation to Blinking in CdSe Quantum Dots journal, October 2015

Delayed Luminescence in Lead Halide Perovskite Nanocrystals journal, June 2017

Using Shape to Control Photoluminescence from CdSe/CdS Core/Shell Nanorods journal, May 2011

Length-Dependent Optical Effects in Single Walled Carbon Nanotubes † journal, May 2008

Synthesis and Micrometer-Scale Assembly of Colloidal CdSe/CdS Nanorods Prepared by a Seeded Growth Approach journal, October 2007

Chemical Cutting of Perovskite Nanowires into Single‐Photon Emissive Low‐Aspect‐Ratio CsPbX 3 (X=Cl, Br, I) Nanorods journal, December 2018

Surface- vs Diffusion-Limited Mechanisms of Anion Exchange in CsPbBr 3 Nanocrystal Cubes Revealed through Kinetic Studies journal, September 2016

Design Principles for Trap-Free CsPbX 3 Nanocrystals: Enumerating and Eliminating Surface Halide Vacancies with Softer Lewis Bases journal, November 2018

Single Cesium Lead Halide Perovskite Nanocrystals at Low Temperature: Fast Single-Photon Emission, Reduced Blinking, and Exciton Fine Structure journal, January 2016

Superfluorescence from lead halide perovskite quantum dot superlattices journal, November 2018

Thermal Conductance of Thin Silicon Nanowires journal, September 2008

Synthesis and Optical Properties of PbSe Nanorods with Controlled Diameter and Length journal, August 2015

Random Walks on Lattices. III. Calculation of First‐Passage Times with Application to Exciton Trapping on Photosynthetic Units
journal, April 1969

Extrinsic and Dynamic Edge States of Two-Dimensional Lead Halide Perovskites
journal, February 2019

Synthesis of Composition Tunable and Highly Luminescent Cesium Lead Halide Nanowires through Anion-Exchange Reactions
journal, June 2016

Essentially Trap-Free CsPbBr ₃ Colloidal Nanocrystals by Postsynthetic Thiocyanate Surface Treatment
journal, May 2017

A Solution NMR Toolbox for Characterizing the Surface Chemistry of Colloidal Nanocrystals
journal, February 2013

Hybrid organic—inorganic perovskites: low-cost semiconductors with intriguing charge-transport properties
journal, January 2016

Rashba Effect in a Single Colloidal CsPbBr ₃ Perovskite Nanocrystal Detected by Magneto-Optical Measurements
journal, July 2017

Zero-Dimensional and Quasi One-Dimensional Effects in Semiconductor Nanorods
journal, May 2004

Aspect Ratio Dependence of Auger Recombination and Carrier Multiplication in PbSe Nanorods
journal, February 2013

Quantitative imaging of anion exchange kinetics in halide perovskites
journal, June 2019

The emergence of perovskite solar cells
journal, July 2014

Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals
journal, January 2015

Perovskite light-emitting diodes with external quantum efficiency exceeding 20 per cent
journal, October 2018

Melting in Semiconductor Nanocrystals
journal, June 1992

Composition-dependent photoluminescence intensity and prolonged recombination lifetime of perovskite CH ₃ NH ₃ PbBr _3−x Cl _x films
journal, January 2014

Exciton Recombination in Formamidinium Lead Triiodide: Nanocrystals versus Thin Films
journal, June 2017

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

Perspectives on the Physical Chemistry of Semiconductor Nanocrystals
journal, January 1996

The Role of Length and Defects on Optical Quantum Efficiency and Exciton Decay Dynamics in Single-Walled Carbon Nanotubes
journal, December 2010

High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization
journal, July 2015

Visualizing Carrier Diffusion in Individual Single-Crystal Organolead Halide Perovskite Nanowires and Nanoplates
journal, September 2015

Interfacial Synthesis of Monodisperse CsPbBr ₃ Nanorods with Tunable Aspect Ratio and Clean Surface for Efficient Light-Emitting Diode Applications
journal, February 2019

Synthesis and Properties of CdSe/ZnS Core/Shell Nanorods
journal, September 2003

Spatially resolved multicolor CsPbX ₃ nanowire heterojunctions via anion exchange
journal, June 2017

Role of microstructure in the electron–hole interaction of hybrid lead halide perovskites
journal, August 2015

Recombination Kinetics in Organic-Inorganic Perovskites: Excitons, Free Charge, and Subgap States
journal, September 2014

Exciton Diffusion in Air-Suspended Single-Walled Carbon Nanotubes
journal, June 2010

All-inorganic perovskite nanocrystal scintillators
journal, August 2018

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

Quantum-size effects on radiative lifetimes and relaxation of excitons in semiconductor nanostructures
journal, October 1998

CdSe Nanorod Synthesis: A New Approach
journal, November 2007

Controlling the influence of Auger recombination on the performance of quantum-dot light-emitting diodes
journal, October 2013

Theoretical study of time-resolved luminescence in semiconductors. III. Trap states in the band gap
journal, September 2015

Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites
journal, March 2017

Understanding the physical properties of hybrid perovskites for photovoltaic applications
journal, July 2017

Spectral and Dynamical Properties of Single Excitons, Biexcitons, and Trions in Cesium–Lead-Halide Perovskite Quantum Dots
journal, March 2016

Exciton diffusion, end quenching, and exciton-exciton annihilation in individual air-suspended carbon nanotubes
journal, March 2015

Ligand Control of Growth, Morphology, and Capping Structure of Colloidal CdSe Nanorods
journal, May 2007

Size Dependence of a First Order Solid-Solid Phase Transition: The Wurtzite to Rock Salt Transformation in CdSe Nanocrystals
journal, July 1994

Quantum Dot Luminescent Concentrator Cavity Exhibiting 30-fold Concentration
journal, August 2015

Shape control of CdSe nanocrystals
journal, March 2000

Enhanced thermoelectric performance of rough silicon nanowires
journal, January 2008

Impact of microstructure on local carrier lifetime in perovskite solar cells
journal, April 2015

Perovskite light-emitting diodes based on spontaneously formed submicrometre-scale structures
journal, October 2018

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

Fast Anion-Exchange in Highly Luminescent Nanocrystals of Cesium Lead Halide Perovskites (CsPbX ₃ , X = Cl, Br, I)
journal, July 2015

Charge-Carrier Dynamics in Organic-Inorganic Metal Halide Perovskites
journal, May 2016

Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber
journal, October 2013

Long-Range Balanced Electron- and Hole-Transport Lengths in Organic-Inorganic CH₃NH₃PbI₃
journal, October 2013

Bandgap engineering in semiconductor alloy nanomaterials with widely tunable compositions
journal, October 2017

Diffusion Limited Photoluminescence Quantum Yields in 1-D Semiconductors: Single-Wall Carbon Nanotubes
journal, November 2010

Coherent single-photon emission from colloidal lead halide perovskite quantum dots
journal, February 2019

Recombination in amorphous materials as a continuous-time random-walk problem
journal, March 1983

Delayed Exciton Emission and Its Relation to Blinking in CdSe Quantum Dots
journal, October 2015

Delayed Luminescence in Lead Halide Perovskite Nanocrystals
journal, June 2017

Using Shape to Control Photoluminescence from CdSe/CdS Core/Shell Nanorods
journal, May 2011

Length-Dependent Optical Effects in Single Walled Carbon Nanotubes ^†
journal, May 2008

Synthesis and Micrometer-Scale Assembly of Colloidal CdSe/CdS Nanorods Prepared by a Seeded Growth Approach
journal, October 2007

Chemical Cutting of Perovskite Nanowires into Single‐Photon Emissive Low‐Aspect‐Ratio CsPbX ₃ (X=Cl, Br, I) Nanorods
journal, December 2018

Surface- vs Diffusion-Limited Mechanisms of Anion Exchange in CsPbBr ₃ Nanocrystal Cubes Revealed through Kinetic Studies
journal, September 2016

Design Principles for Trap-Free CsPbX ₃ Nanocrystals: Enumerating and Eliminating Surface Halide Vacancies with Softer Lewis Bases
journal, November 2018

Single Cesium Lead Halide Perovskite Nanocrystals at Low Temperature: Fast Single-Photon Emission, Reduced Blinking, and Exciton Fine Structure
journal, January 2016

Superfluorescence from lead halide perovskite quantum dot superlattices
journal, November 2018

Thermal Conductance of Thin Silicon Nanowires
journal, September 2008

Synthesis and Optical Properties of PbSe Nanorods with Controlled Diameter and Length
journal, August 2015