Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways

Manger, Lydia H.; Rowley, Matthew B.; Fu, Yongping; Foote, Alexander K.; Rea, Morgan T.; Wood, Sharla L.; Jin, Song; Wright, John C.; Goldsmith, Randall H.

doi:10.1021/acs.jpcc.6b11547

Title: Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways

Abstract

Hybrid organic-inorganic perovskites demonstrate desirable photophysical behaviors and promising applications from efficient photovoltaics to lasing, but the fundamental nature of excited state species is still under debate. We also collected time-resolved photoluminescence of single-crystal nanoplates of methylammonium lead iodide perovskite (MAPbI3), with excitation over a range of fluences and repetition rates, to provide a more complete photophysical picture. A fundamentally different way of simulating the photophysics is developed that relies on unnormalized decays, global analysis over a large array of conditions, and inclusion of steady-state behavior; these details are critical to capturing observed behaviors. These additional constraints require inclusion of spatially-correlated pairs, along with free carriers and traps, demonstrating the importance of our comprehensive analysis. Modeling geminate and non-geminate pathways shows geminate processes are dominant at high carrier densities and early times. This combination of data and simulation provides a detailed picture of perovskite photophysics across multiple excitation regimes that was not previously available.

Authors:

Manger, Lydia H. ^[1]; Rowley, Matthew B. ^[1]; Fu, Yongping ^[1]; Foote, Alexander K. ^[1]; Rea, Morgan T. ^[1]; Wood, Sharla L. ^[1];

^[1]; Wright, John C. ^[1];

^[1]

Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemistry

Publication Date:: Tue Dec 20 00:00:00 EST 2016

Research Org.:: Univ. of Wisconsin, Madison, WI (United States)

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

OSTI Identifier:: 1393446

Grant/Contract Number:: FG02-09ER46664; SC0002162

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. C

Additional Journal Information:: Journal Volume: 121; Journal Issue: 2; Journal ID: ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 14 SOLAR ENERGY; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Manger, Lydia H., Rowley, Matthew B., Fu, Yongping, Foote, Alexander K., Rea, Morgan T., Wood, Sharla L., Jin, Song, Wright, John C., and Goldsmith, Randall H. Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways.  United States: N. p., 2016. 
Web.  doi:10.1021/acs.jpcc.6b11547.

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                    Manger, Lydia H., Rowley, Matthew B., Fu, Yongping, Foote, Alexander K., Rea, Morgan T., Wood, Sharla L., Jin, Song, Wright, John C., & Goldsmith, Randall H. Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways.  United States.  https://doi.org/10.1021/acs.jpcc.6b11547

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                    Manger, Lydia H., Rowley, Matthew B., Fu, Yongping, Foote, Alexander K., Rea, Morgan T., Wood, Sharla L., Jin, Song, Wright, John C., and Goldsmith, Randall H. Tue .  
"Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways".  United States.  https://doi.org/10.1021/acs.jpcc.6b11547.  https://www.osti.gov/servlets/purl/1393446.

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@article{osti_1393446,

  title        = {Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways},

  author       = {Manger, Lydia H. and Rowley, Matthew B. and Fu, Yongping and Foote, Alexander K. and Rea, Morgan T. and Wood, Sharla L. and Jin, Song and Wright, John C. and Goldsmith, Randall H.},

  abstractNote = {Hybrid organic-inorganic perovskites demonstrate desirable photophysical behaviors and promising applications from efficient photovoltaics to lasing, but the fundamental nature of excited state species is still under debate. We also collected time-resolved photoluminescence of single-crystal nanoplates of methylammonium lead iodide perovskite (MAPbI3), with excitation over a range of fluences and repetition rates, to provide a more complete photophysical picture. A fundamentally different way of simulating the photophysics is developed that relies on unnormalized decays, global analysis over a large array of conditions, and inclusion of steady-state behavior; these details are critical to capturing observed behaviors. These additional constraints require inclusion of spatially-correlated pairs, along with free carriers and traps, demonstrating the importance of our comprehensive analysis. Modeling geminate and non-geminate pathways shows geminate processes are dominant at high carrier densities and early times. This combination of data and simulation provides a detailed picture of perovskite photophysics across multiple excitation regimes that was not previously available.},

  doi          = {10.1021/acs.jpcc.6b11547},

  journal      = {Journal of Physical Chemistry. C},

  number       = 2,

  volume       = 121,

  place        = {United States},

  year         = {Tue Dec 20 00:00:00 EST 2016},

  month        = {Tue Dec 20 00:00:00 EST 2016}

}

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Works referencing / citing this record:

Inhibition of light emission from the metastable tetragonal phase at low temperatures in island-like films of lead iodide perovskites
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Title: Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways

Abstract

Citation Formats

A vacuum flash–assisted solution process for high-efficiency large-area perovskite solar cells journal, June 2016

The emergence of perovskite solar cells journal, July 2014

Formamidinium lead trihalide: a broadly tunable perovskite for efficient planar heterojunction solar cells journal, January 2014

Lead Iodide Perovskite Sensitized All-Solid-State Submicron Thin Film Mesoscopic Solar Cell with Efficiency Exceeding 9% journal, August 2012

Solution Growth of Single Crystal Methylammonium Lead Halide Perovskite Nanostructures for Optoelectronic and Photovoltaic Applications journal, April 2015

Sequential deposition as a route to high-performance perovskite-sensitized solar cells journal, July 2013

Electron-hole diffusion lengths > 175 μm in solution-grown CH 3 NH 3 PbI 3 single crystals journal, January 2015

Low-Temperature Solution-Processed Perovskite Solar Cells with High Efficiency and Flexibility journal, January 2014

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

Low-temperature solution-processed wavelength-tunable perovskites for lasing journal, March 2014

Spatially Non-uniform Trap State Densities in Solution-Processed Hybrid Perovskite Thin Films journal, February 2016

Band filling with free charge carriers in organometal halide perovskites journal, August 2014

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

From organic single crystals to solution processed thin-films: Charge transport and trapping with varying degree of order journal, April 2013

Chemical Management for Colorful, Efficient, and Stable Inorganic–Organic Hybrid Nanostructured Solar Cells journal, March 2013

Lead halide perovskite nanowire lasers with low lasing thresholds and high quality factors journal, April 2015

High Photoluminescence Efficiency and Optically Pumped Lasing in Solution-Processed Mixed Halide Perovskite Semiconductors journal, March 2014

Nanowire Lasers of Formamidinium Lead Halide Perovskites and Their Stabilized Alloys with Improved Stability journal, January 2016

Excited State Properties of Hybrid Perovskites journal, December 2015

Photon recycling in lead iodide perovskite solar cells journal, March 2016

Charge Carriers in Hybrid Organic–Inorganic Lead Halide Perovskites Might Be Protected as Large Polarons journal, November 2015

Perovskite solar cells with a planar heterojunction structure prepared using room-temperature solution processing techniques journal, December 2013

Exciton versus Free Carrier Photogeneration in Organometal Trihalide Perovskites Probed by Broadband Ultrafast Polarization Memory Dynamics journal, March 2015

Perovskite solar cells employing organic charge-transport layers journal, December 2013

Perovskite Solar Cells: From Materials to Devices journal, October 2014

Correlated electron–hole plasma in organometal perovskites journal, September 2014

Lasing in robust cesium lead halide perovskite nanowires journal, February 2016

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

Analysis of Multivalley and Multibandgap Absorption and Enhancement of Free Carriers Related to Exciton Screening in Hybrid Perovskites journal, May 2014

Excitons versus free charges in organo-lead tri-halide perovskites journal, April 2014

Electro-optics of perovskite solar cells journal, December 2014

Observation of a hot-phonon bottleneck in lead-iodide perovskites journal, October 2015

Comparison of Recombination Dynamics in CH 3 NH 3 PbBr 3 and CH 3 NH 3 PbI 3 Perovskite Films: Influence of Exciton Binding Energy journal, November 2015

Comparative study on the excitons in lead-halide-based perovskite-type crystals CH3NH3PbBr3 CH3NH3PbI3 journal, September 2003

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

Dynamic Optical Properties of CH 3 NH 3 PbI 3 Single Crystals As Revealed by One- and Two-Photon Excited Photoluminescence Measurements journal, August 2015

Dual nature of the excited state in organic–inorganic lead halide perovskites journal, January 2015

Enhanced Photoluminescence and Solar Cell Performance via Lewis Base Passivation of Organic–Inorganic Lead Halide Perovskites journal, September 2014

Homogeneous Emission Line Broadening in the Organo Lead Halide Perovskite CH 3 NH 3 PbI 3– x Cl x journal, March 2014

Luminescence Spectroscopy of Semiconductors book, February 2012

Photophysics of Organic-Inorganic Hybrid Lead Iodide Perovskite Single Crystals journal, February 2015

Organometal Halide Perovskite Solar Cell Materials Rationalized: Ultrafast Charge Generation, High and Microsecond-Long Balanced Mobilities, and Slow Recombination journal, February 2014

Revealing the ultrafast charge carrier dynamics in organo metal halide perovskite solar cell materials using time resolved THz spectroscopy journal, January 2016

Geminate Charge Recombination in Alternating Polyfluorene Copolymer/Fullerene Blends journal, July 2007

Thermally Activated Exciton Dissociation and Recombination Control the Carrier Dynamics in Organometal Halide Perovskite journal, June 2014

High Charge Carrier Mobilities and Lifetimes in Organolead Trihalide Perovskites journal, December 2013

Amplified spontaneous emission-application to Nd:YAG lasers journal, January 1999

Nonradiative recombination of excitons in carbon nanotubes mediated by free charge carriers journal, October 2008

Direct–indirect character of the bandgap in methylammonium lead iodide perovskite journal, October 2016

Electron–phonon coupling in hybrid lead halide perovskites journal, May 2016

Exciton formation rates in GaAs/ Al x Ga 1 − x As quantum wells journal, January 1997

Screening in crystalline liquids protects energetic carriers in hybrid perovskites journal, September 2016

Real-Time Observation of Organic Cation Reorientation in Methylammonium Lead Iodide Perovskites journal, August 2015

Photo-induced halide redistribution in organic–inorganic perovskite films journal, May 2016

Tuning the Light Emission Properties by Band Gap Engineering in Hybrid Lead Halide Perovskite journal, December 2014

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

Enhanced Organo-Metal Halide Perovskite Photoluminescence from Nanosized Defect-Free Crystallites and Emitting Sites journal, September 2015

Mechanistic insights into perovskite photoluminescence enhancement: light curing with oxygen can boost yield thousandfold journal, January 2015

Inhibition of light emission from the metastable tetragonal phase at low temperatures in island-like films of lead iodide perovskites journal, January 2019

Perovskite Excitonics: Primary Exciton Creation and Crossover from Free Carriers to a Secondary Exciton Phase journal, December 2017

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

Perovskites for Light Emission journal, August 2018

Characterization of trap states in perovskite films by simultaneous fitting of steady-state and transient photoluminescence measurements journal, August 2018

Exciton Recombination in Formamidinium Lead Triiodide: Nanocrystals versus Thin Films text, January 2017

A vacuum flash–assisted solution process for high-efficiency large-area perovskite solar cells
journal, June 2016

The emergence of perovskite solar cells
journal, July 2014

Formamidinium lead trihalide: a broadly tunable perovskite for efficient planar heterojunction solar cells
journal, January 2014

Lead Iodide Perovskite Sensitized All-Solid-State Submicron Thin Film Mesoscopic Solar Cell with Efficiency Exceeding 9%
journal, August 2012

Solution Growth of Single Crystal Methylammonium Lead Halide Perovskite Nanostructures for Optoelectronic and Photovoltaic Applications
journal, April 2015

Sequential deposition as a route to high-performance perovskite-sensitized solar cells
journal, July 2013

Electron-hole diffusion lengths > 175 μm in solution-grown CH ₃ NH ₃ PbI ₃ single crystals
journal, January 2015

Low-Temperature Solution-Processed Perovskite Solar Cells with High Efficiency and Flexibility
journal, January 2014

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

Low-temperature solution-processed wavelength-tunable perovskites for lasing
journal, March 2014

Spatially Non-uniform Trap State Densities in Solution-Processed Hybrid Perovskite Thin Films
journal, February 2016

Band filling with free charge carriers in organometal halide perovskites
journal, August 2014

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

From organic single crystals to solution processed thin-films: Charge transport and trapping with varying degree of order
journal, April 2013

Chemical Management for Colorful, Efficient, and Stable Inorganic–Organic Hybrid Nanostructured Solar Cells
journal, March 2013

Lead halide perovskite nanowire lasers with low lasing thresholds and high quality factors
journal, April 2015

High Photoluminescence Efficiency and Optically Pumped Lasing in Solution-Processed Mixed Halide Perovskite Semiconductors
journal, March 2014

Nanowire Lasers of Formamidinium Lead Halide Perovskites and Their Stabilized Alloys with Improved Stability
journal, January 2016

Excited State Properties of Hybrid Perovskites
journal, December 2015

Photon recycling in lead iodide perovskite solar cells
journal, March 2016

Charge Carriers in Hybrid Organic–Inorganic Lead Halide Perovskites Might Be Protected as Large Polarons
journal, November 2015

Perovskite solar cells with a planar heterojunction structure prepared using room-temperature solution processing techniques
journal, December 2013

Exciton versus Free Carrier Photogeneration in Organometal Trihalide Perovskites Probed by Broadband Ultrafast Polarization Memory Dynamics
journal, March 2015

Perovskite solar cells employing organic charge-transport layers
journal, December 2013

Perovskite Solar Cells: From Materials to Devices
journal, October 2014

Correlated electron–hole plasma in organometal perovskites
journal, September 2014

Lasing in robust cesium lead halide perovskite nanowires
journal, February 2016

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

Analysis of Multivalley and Multibandgap Absorption and Enhancement of Free Carriers Related to Exciton Screening in Hybrid Perovskites
journal, May 2014

Excitons versus free charges in organo-lead tri-halide perovskites
journal, April 2014

Electro-optics of perovskite solar cells
journal, December 2014

Observation of a hot-phonon bottleneck in lead-iodide perovskites
journal, October 2015

Comparison of Recombination Dynamics in CH ₃ NH ₃ PbBr ₃ and CH ₃ NH ₃ PbI ₃ Perovskite Films: Influence of Exciton Binding Energy
journal, November 2015

Comparative study on the excitons in lead-halide-based perovskite-type crystals CH₃NH₃PbBr₃ CH₃NH₃PbI₃
journal, September 2003

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

Dynamic Optical Properties of CH ₃ NH ₃ PbI ₃ Single Crystals As Revealed by One- and Two-Photon Excited Photoluminescence Measurements
journal, August 2015

Dual nature of the excited state in organic–inorganic lead halide perovskites
journal, January 2015

Enhanced Photoluminescence and Solar Cell Performance via Lewis Base Passivation of Organic–Inorganic Lead Halide Perovskites
journal, September 2014

Homogeneous Emission Line Broadening in the Organo Lead Halide Perovskite CH ₃ NH ₃ PbI _{3– x} Cl _x
journal, March 2014

Luminescence Spectroscopy of Semiconductors
book, February 2012

Photophysics of Organic-Inorganic Hybrid Lead Iodide Perovskite Single Crystals
journal, February 2015

Organometal Halide Perovskite Solar Cell Materials Rationalized: Ultrafast Charge Generation, High and Microsecond-Long Balanced Mobilities, and Slow Recombination
journal, February 2014

Revealing the ultrafast charge carrier dynamics in organo metal halide perovskite solar cell materials using time resolved THz spectroscopy
journal, January 2016

Geminate Charge Recombination in Alternating Polyfluorene Copolymer/Fullerene Blends
journal, July 2007

Thermally Activated Exciton Dissociation and Recombination Control the Carrier Dynamics in Organometal Halide Perovskite
journal, June 2014

High Charge Carrier Mobilities and Lifetimes in Organolead Trihalide Perovskites
journal, December 2013

Amplified spontaneous emission-application to Nd:YAG lasers
journal, January 1999

Nonradiative recombination of excitons in carbon nanotubes mediated by free charge carriers
journal, October 2008

Direct–indirect character of the bandgap in methylammonium lead iodide perovskite
journal, October 2016

Electron–phonon coupling in hybrid lead halide perovskites
journal, May 2016

Exciton formation rates in GaAs/ ${Al}_{x}$ ${Ga}_{1 - x}$ As quantum wells
journal, January 1997

Screening in crystalline liquids protects energetic carriers in hybrid perovskites
journal, September 2016

Real-Time Observation of Organic Cation Reorientation in Methylammonium Lead Iodide Perovskites
journal, August 2015

Photo-induced halide redistribution in organic–inorganic perovskite films
journal, May 2016

Tuning the Light Emission Properties by Band Gap Engineering in Hybrid Lead Halide Perovskite
journal, December 2014

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

Enhanced Organo-Metal Halide Perovskite Photoluminescence from Nanosized Defect-Free Crystallites and Emitting Sites
journal, September 2015

Mechanistic insights into perovskite photoluminescence enhancement: light curing with oxygen can boost yield thousandfold
journal, January 2015

Inhibition of light emission from the metastable tetragonal phase at low temperatures in island-like films of lead iodide perovskites
journal, January 2019

Perovskite Excitonics: Primary Exciton Creation and Crossover from Free Carriers to a Secondary Exciton Phase
journal, December 2017

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

Perovskites for Light Emission
journal, August 2018

Characterization of trap states in perovskite films by simultaneous fitting of steady-state and transient photoluminescence measurements
journal, August 2018

Exciton Recombination in Formamidinium Lead Triiodide: Nanocrystals versus Thin Films
text, January 2017