Light Induced Processes in CsPbBr3–Au Hybrid Nanocrystals: Electron Transfer and Expulsion of Au

Chakkamalayath, Jishnudas; Hartland, Gregory V.; Kamat, Prashant V.

doi:10.1021/acs.jpcc.1c05491

Title: Light Induced Processes in CsPbBr₃–Au Hybrid Nanocrystals: Electron Transfer and Expulsion of Au

Abstract

Semiconductor–metal heterostructures such as CsPbBr₃–Au are useful in photocatalysis. When Au nanoparticles are deposited on the CsPbBr₃ nanocrystal surface, they efficiently quench the photoluminescence of the semiconductor. This process has been studied by femtosecond transient absorption spectroscopy measurements, which indicate that electron transfer to the Au nanoparticles occurs from both hot and relaxed electrons in the conduction band of CsPbBr₃. The electron transfer rate constant is much larger for the hot electrons compared to the relaxed electrons. Under steady state photoirradiation of CsPbBr₃–Au heterostructure, the photogenerated electrons from the excited CsPbBr₃ nanocrystals continue to charge the Au nanoparticles. After sufficient irradiation, the gold nanoparticles dissociate from the CsPbBr₃ surface and aggregate into larger size gold nanoparticles. The expulsion of gold nanoparticles restores the original luminescence behavior of CsPbBr₃ nanocrystals. The spectroscopic and morphological studies provide insight into the expulsion of gold nanoparticles in photoirradiated CsPbBr₃–Au heterostructures.

Authors:

Chakkamalayath, Jishnudas ^[1];

^[1];

^[1]

Univ. of Notre Dame, IN (United States)

Publication Date:: Fri Aug 06 00:00:00 EDT 2021

Research Org.:: University of Notre Dame, IN (United States)

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

OSTI Identifier:: 1830757

Grant/Contract Number:: FC02-04ER15533

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. C

Additional Journal Information:: Journal Volume: 125; Journal Issue: 32; Journal ID: ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 14 SOLAR ENERGY

Citation Formats


                    Chakkamalayath, Jishnudas, Hartland, Gregory V., and Kamat, Prashant V. Light Induced Processes in CsPbBr3–Au Hybrid Nanocrystals: Electron Transfer and Expulsion of Au.  United States: N. p., 2021. 
Web.  doi:10.1021/acs.jpcc.1c05491.

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                    Chakkamalayath, Jishnudas, Hartland, Gregory V., & Kamat, Prashant V. Light Induced Processes in CsPbBr3–Au Hybrid Nanocrystals: Electron Transfer and Expulsion of Au.  United States.  https://doi.org/10.1021/acs.jpcc.1c05491

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                    Chakkamalayath, Jishnudas, Hartland, Gregory V., and Kamat, Prashant V. Fri .  
"Light Induced Processes in CsPbBr3–Au Hybrid Nanocrystals: Electron Transfer and Expulsion of Au".  United States.  https://doi.org/10.1021/acs.jpcc.1c05491.  https://www.osti.gov/servlets/purl/1830757.

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@article{osti_1830757,

  title        = {Light Induced Processes in CsPbBr3–Au Hybrid Nanocrystals: Electron Transfer and Expulsion of Au},

  author       = {Chakkamalayath, Jishnudas and Hartland, Gregory V. and Kamat, Prashant V.},

  abstractNote = {Semiconductor–metal heterostructures such as CsPbBr3–Au are useful in photocatalysis. When Au nanoparticles are deposited on the CsPbBr3 nanocrystal surface, they efficiently quench the photoluminescence of the semiconductor. This process has been studied by femtosecond transient absorption spectroscopy measurements, which indicate that electron transfer to the Au nanoparticles occurs from both hot and relaxed electrons in the conduction band of CsPbBr3. The electron transfer rate constant is much larger for the hot electrons compared to the relaxed electrons. Under steady state photoirradiation of CsPbBr3–Au heterostructure, the photogenerated electrons from the excited CsPbBr3 nanocrystals continue to charge the Au nanoparticles. After sufficient irradiation, the gold nanoparticles dissociate from the CsPbBr3 surface and aggregate into larger size gold nanoparticles. The expulsion of gold nanoparticles restores the original luminescence behavior of CsPbBr3 nanocrystals. The spectroscopic and morphological studies provide insight into the expulsion of gold nanoparticles in photoirradiated CsPbBr3–Au heterostructures.},

  doi          = {10.1021/acs.jpcc.1c05491},

  journal      = {Journal of Physical Chemistry. C},

  number       = 32,

  volume       = 125,

  place        = {United States},

  year         = {Fri Aug 06 00:00:00 EDT 2021},

  month        = {Fri Aug 06 00:00:00 EDT 2021}

}

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Title: Light Induced Processes in CsPbBr3–Au Hybrid Nanocrystals: Electron Transfer and Expulsion of Au

Abstract

Citation Formats

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Effects of Chlorine Mixing on Optoelectronics, Ion Migration, and Gamma-Ray Detection in Bromide Perovskites journal, February 2020

Photophysical, Photochemical and Photocatalytic Aspects of Metal Nanoparticles journal, August 2002

The Monolayer Thickness Dependence of Quantized Double-Layer Capacitances of Monolayer-Protected Gold Clusters journal, September 1999

Progress and Perspectives of Plasmon-Enhanced Solar Energy Conversion journal, February 2016

Theory of Photoinjection of Hot Plasmonic Carriers from Metal Nanostructures into Semiconductors and Surface Molecules journal, July 2013

Photoinduced Ultrafast Charge Separation in Plexcitonic CdSe/Au and CdSe/Pt Nanorods journal, October 2013

Opportunities and Challenges of Solar-Energy-Driven Carbon Dioxide to Fuel Conversion with Plasmonic Catalysts journal, August 2017

Technical and economic feasibility of centralized facilities for solar hydrogen production via photocatalysis and photoelectrochemistry journal, January 2013

Light-induced reactivity of gold and hybrid perovskite as a new possible degradation mechanism in perovskite solar cells journal, January 2018

Visualizing Ultrafast Electron Transfer Processes in Semiconductor–Metal Hybrid Nanoparticles: Toward Excitonic–Plasmonic Light Harvesting journal, January 2021

Sensitive X-ray detectors made of methylammonium lead tribromide perovskite single crystals journal, March 2016

Photocatalytic Events of CdSe Quantum Dots in Confined Media. Electrodic Behavior of Coupled Platinum Nanoparticles journal, November 2010

Synergistic Photochemistry of Alcohols Catalyzed by Plasmonic Nanoparticles and a Metal Complex journal, April 2021

Visible Light-Induced Charge Retention and Photocatalysis with Hybrid CdSe−Au Nanodumbbells journal, February 2008

Is There Anything Better than Pt for HER? journal, March 2021

Ultrafast Charge Separation and Long-Lived Charge Separated State in Photocatalytic CdS–Pt Nanorod Heterostructures journal, June 2012

Challenges and Opportunities for CsPbBr 3 Perovskites in Low- and High-Energy Radiation Detection journal, March 2021

Demonstration of Energy-Resolved γ-Ray Detection at Room Temperature by the CsPbCl 3 Perovskite Semiconductor journal, January 2021

Dynamic Burstein-Moss shift in semiconductor colloids journal, April 1989

Catalysis with TiO 2 /Gold Nanocomposites. Effect of Metal Particle Size on the Fermi Level Equilibration journal, April 2004

Semitransparent Perovskite Solar Cells journal, April 2020

Perovskite Photocatalysis. Methyl Viologen Induces Unusually Long-Lived Charge Carrier Separation in CsPbBr 3 Nanocrystals journal, December 2019

Size-Dependent Energy Transfer between CdSe/ZnS Quantum Dots and Gold Nanoparticles journal, August 2011

CsPbBr 3 /ZnS Core/Shell Type Nanocrystals for Enhancing Luminescence Lifetime and Water Stability journal, May 2020

Perovskite Quantum Dots for Application in High Color Gamut Backlighting Display of Light-Emitting Diodes journal, October 2020

Solution-processed perovskite-colloidal quantum dot tandem solar cells for photon collection beyond 1000 nm journal, January 2019

Probing Perovskite Photocatalysis. Interfacial Electron Transfer between CsPbBr 3 and Ferrocene Redox Couple journal, September 2019

Solar-Driven Metal Halide Perovskite Photocatalysis: Design, Stability, and Performance journal, March 2020

What’s so Hot about Electrons in Metal Nanoparticles? journal, June 2017

Efficient plasmon-hot electron conversion in Ag–CsPbBr3 hybrid nanocrystals journal, March 2019

On the Quenching of Semiconductor Quantum Dot Photoluminescence by Proximal Gold Nanoparticles journal, September 2007

Efficient Hot Electron Transfer from Small Au Nanoparticles journal, May 2020

Reactions at noble metal contacts with methylammonium lead triiodide perovskites: Role of underpotential deposition and electrochemistry journal, April 2019

Electrochemical Quantized Capacitance Charging of Surface Ensembles of Gold Nanoparticles journal, November 1999

Plasmon Resonances of Semiconductor Nanocrystals: Physical Principles and New Opportunities journal, March 2014

Prominent Efficiency Enhancement in Perovskite Solar Cells Employing Silica-Coated Gold Nanorods journal, March 2016

Achieving Near-Unity Photoluminescence Efficiency for Blue-Violet-Emitting Perovskite Nanocrystals journal, November 2018

Ligand Assisted Transformation of Cubic CsPbBr 3 Nanocrystals into Two-Dimensional CsPb 2 Br 5 Nanosheets journal, November 2017

Band Bending in Semiconductors: Chemical and Physical Consequences at Surfaces and Interfaces journal, June 2012

Semiconductor−Metal Composite Nanostructures. To What Extent Do Metal Nanoparticles Improve the Photocatalytic Activity of TiO 2 Films? journal, November 2001

Gold Nanoelectrodes of Varied Size: Transition to Molecule-Like Charging journal, June 1998

Au Exchange or Au Deposition: Dual Reaction Pathways in Au–CsPbBr 3 Heterostructure Nanoparticles journal, August 2017

Photocatalytic Water Splitting: Recent Progress and Future Challenges journal, September 2010

Ultrafast Charge Separation in Two-Dimensional CsPbBr 3 Perovskite Nanoplatelets journal, January 2019

Capture, Store, and Discharge. Shuttling Photogenerated Electrons across TiO 2 –Silver Interface journal, August 2011

Metal Halide Perovskite Nanocrystals: Synthesis, Post-Synthesis Modifications, and Their Optical Properties journal, February 2019

Absorption Enhancement in Organic–Inorganic Halide Perovskite Films with Embedded Plasmonic Gold Nanoparticles journal, July 2015

An overview on enhancing the stability of lead halide perovskite quantum dots and their applications in phosphor-converted LEDs journal, January 2019

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

Au–CsPbBr 3 Hybrid Architecture: Anchoring Gold Nanoparticles on Cubic Perovskite Nanocrystals journal, December 2016

Title: Light Induced Processes in CsPbBr₃–Au Hybrid Nanocrystals: Electron Transfer and Expulsion of Au

Halide Perovskite Nanocrystal Photocatalysts for CO ₂ Reduction: Successes and Challenges
journal, July 2020

Charge Separation and Catalytic Activity of Ag@TiO ₂ Core−Shell Composite Clusters under UV−Irradiation
journal, March 2005

The Effects of Electron and Hole Injection on the Photoluminescence of CdSe/CdS/ZnS Nanocrystal Monolayers
journal, March 2008

Optical Nonlinearities and Ultrafast Carrier Dynamics in Semiconductor Nanocrystals
journal, July 2000

Recent Progress on the Stability of Perovskite Solar Cells in a Humid Environment
journal, November 2020

Materials and Methods for Interface Engineering toward Stable and Efficient Perovskite Solar Cells
journal, July 2020

Visible-light-enhanced catalytic oxidation reactions on plasmonic silver nanostructures
journal, May 2011

Progress in Perovskite Photocatalysis
journal, July 2020

“Hot Electron” Photo-Charging and Electrochemical Discharge Kinetics of Silver Nanocrystals
journal, October 2007

Efficient hot-electron transfer by a plasmon-induced interfacial charge-transfer transition
journal, August 2015

Know Thy Nano Neighbor . Plasmonic versus Electron Charging Effects of Metal Nanoparticles in Dye-Sensitized Solar Cells
journal, April 2012

Ultrafast and Hot Electron Transfer in CdSe QD–Au Hybrid Nanostructures
journal, December 2019

Metal Semiconductor Heterostructures for Photocatalytic Conversion of Light Energy
journal, March 2015

Core–Shell CsPbBr ₃ @CdS Quantum Dots with Enhanced Stability and Photoluminescence Quantum Yields for Optoelectronic Devices
journal, July 2020

Effects of Chlorine Mixing on Optoelectronics, Ion Migration, and Gamma-Ray Detection in Bromide Perovskites
journal, February 2020

Photophysical, Photochemical and Photocatalytic Aspects of Metal Nanoparticles
journal, August 2002

The Monolayer Thickness Dependence of Quantized Double-Layer Capacitances of Monolayer-Protected Gold Clusters
journal, September 1999

Progress and Perspectives of Plasmon-Enhanced Solar Energy Conversion
journal, February 2016

Theory of Photoinjection of Hot Plasmonic Carriers from Metal Nanostructures into Semiconductors and Surface Molecules
journal, July 2013

Photoinduced Ultrafast Charge Separation in Plexcitonic CdSe/Au and CdSe/Pt Nanorods
journal, October 2013

Opportunities and Challenges of Solar-Energy-Driven Carbon Dioxide to Fuel Conversion with Plasmonic Catalysts
journal, August 2017

Technical and economic feasibility of centralized facilities for solar hydrogen production via photocatalysis and photoelectrochemistry
journal, January 2013

Light-induced reactivity of gold and hybrid perovskite as a new possible degradation mechanism in perovskite solar cells
journal, January 2018

Visualizing Ultrafast Electron Transfer Processes in Semiconductor–Metal Hybrid Nanoparticles: Toward Excitonic–Plasmonic Light Harvesting
journal, January 2021

Sensitive X-ray detectors made of methylammonium lead tribromide perovskite single crystals
journal, March 2016

Photocatalytic Events of CdSe Quantum Dots in Confined Media. Electrodic Behavior of Coupled Platinum Nanoparticles
journal, November 2010

Synergistic Photochemistry of Alcohols Catalyzed by Plasmonic Nanoparticles and a Metal Complex
journal, April 2021

Visible Light-Induced Charge Retention and Photocatalysis with Hybrid CdSe−Au Nanodumbbells
journal, February 2008

Is There Anything Better than Pt for HER?
journal, March 2021

Ultrafast Charge Separation and Long-Lived Charge Separated State in Photocatalytic CdS–Pt Nanorod Heterostructures
journal, June 2012

Challenges and Opportunities for CsPbBr ₃ Perovskites in Low- and High-Energy Radiation Detection
journal, March 2021

Demonstration of Energy-Resolved γ-Ray Detection at Room Temperature by the CsPbCl ₃ Perovskite Semiconductor
journal, January 2021

Dynamic Burstein-Moss shift in semiconductor colloids
journal, April 1989

Catalysis with TiO ₂ /Gold Nanocomposites. Effect of Metal Particle Size on the Fermi Level Equilibration
journal, April 2004

Semitransparent Perovskite Solar Cells
journal, April 2020

Perovskite Photocatalysis. Methyl Viologen Induces Unusually Long-Lived Charge Carrier Separation in CsPbBr ₃ Nanocrystals
journal, December 2019

Size-Dependent Energy Transfer between CdSe/ZnS Quantum Dots and Gold Nanoparticles
journal, August 2011

CsPbBr ₃ /ZnS Core/Shell Type Nanocrystals for Enhancing Luminescence Lifetime and Water Stability
journal, May 2020

Perovskite Quantum Dots for Application in High Color Gamut Backlighting Display of Light-Emitting Diodes
journal, October 2020

Solution-processed perovskite-colloidal quantum dot tandem solar cells for photon collection beyond 1000 nm
journal, January 2019

Probing Perovskite Photocatalysis. Interfacial Electron Transfer between CsPbBr ₃ and Ferrocene Redox Couple
journal, September 2019

Solar-Driven Metal Halide Perovskite Photocatalysis: Design, Stability, and Performance
journal, March 2020

What’s so Hot about Electrons in Metal Nanoparticles?
journal, June 2017

Efficient plasmon-hot electron conversion in Ag–CsPbBr3 hybrid nanocrystals
journal, March 2019

On the Quenching of Semiconductor Quantum Dot Photoluminescence by Proximal Gold Nanoparticles
journal, September 2007

Efficient Hot Electron Transfer from Small Au Nanoparticles
journal, May 2020

Reactions at noble metal contacts with methylammonium lead triiodide perovskites: Role of underpotential deposition and electrochemistry
journal, April 2019

Electrochemical Quantized Capacitance Charging of Surface Ensembles of Gold Nanoparticles
journal, November 1999

Plasmon Resonances of Semiconductor Nanocrystals: Physical Principles and New Opportunities
journal, March 2014

Prominent Efficiency Enhancement in Perovskite Solar Cells Employing Silica-Coated Gold Nanorods
journal, March 2016

Achieving Near-Unity Photoluminescence Efficiency for Blue-Violet-Emitting Perovskite Nanocrystals
journal, November 2018

Ligand Assisted Transformation of Cubic CsPbBr ₃ Nanocrystals into Two-Dimensional CsPb ₂ Br ₅ Nanosheets
journal, November 2017

Band Bending in Semiconductors: Chemical and Physical Consequences at Surfaces and Interfaces
journal, June 2012

Semiconductor−Metal Composite Nanostructures. To What Extent Do Metal Nanoparticles Improve the Photocatalytic Activity of TiO ₂ Films?
journal, November 2001

Gold Nanoelectrodes of Varied Size: Transition to Molecule-Like Charging
journal, June 1998

Au Exchange or Au Deposition: Dual Reaction Pathways in Au–CsPbBr ₃ Heterostructure Nanoparticles
journal, August 2017

Photocatalytic Water Splitting: Recent Progress and Future Challenges
journal, September 2010

Ultrafast Charge Separation in Two-Dimensional CsPbBr 3 Perovskite Nanoplatelets
journal, January 2019

Capture, Store, and Discharge. Shuttling Photogenerated Electrons across TiO ₂ –Silver Interface
journal, August 2011

Metal Halide Perovskite Nanocrystals: Synthesis, Post-Synthesis Modifications, and Their Optical Properties
journal, February 2019

Absorption Enhancement in Organic–Inorganic Halide Perovskite Films with Embedded Plasmonic Gold Nanoparticles
journal, July 2015

An overview on enhancing the stability of lead halide perovskite quantum dots and their applications in phosphor-converted LEDs
journal, January 2019

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

Au–CsPbBr ₃ Hybrid Architecture: Anchoring Gold Nanoparticles on Cubic Perovskite Nanocrystals
journal, December 2016