Dynamic Screening and Slow Cooling of Hot Carriers in Lead Halide Perovskites

Joshi, Prakriti Pradhan; Maehrlein, Sebastian F.; Zhu, Xiaoyang

doi:10.1002/adma.201803054

Title: Dynamic Screening and Slow Cooling of Hot Carriers in Lead Halide Perovskites

Abstract

Abstract Among the exceptional properties of lead halide perovskites (LHPs) is the ultraslow cooling of hot carriers. Carrier densities below the Mott density for large polarons (≤ ≈10 ¹⁸ cm ⁻³ ) are focused on here. As in other semiconductors, a nascent hot electron distribution initially cools down via emission of longitudinal optical (LO) phonons on the 10 ⁻¹⁴ –10 ⁻¹³ s timescale. What distinguishes LHPs from conventional semiconductors is the exceptionally efficient screening in the former. The dielectric screening in LHPs on the 10 ⁻¹³ s timescale results in an order‐of‐magnitude reduction in the Coulomb potential upon the formation of a large polaron, likely with ferroelectric‐like local ordering. Further LO‐phonon emission is inhibited, and this leads to partial retention of hot electron energy on the 10 ⁻¹² s timescale, more so in hybrid LHPs than in their all‐inorganic counterparts. Further cooling of hot polarons occurs on the 10 ⁻¹⁰ s timescale, and this can be attributed to the slow diffusion of heat out of the large polaron volume due to the low thermal conductivity of LHPs. Like other carrier properties, slow hot carrier cooling in LHPs can be intimately related to efficient screening in a soft, anharmonic, and dynamicallymore » disordered lattice.« less

Authors:

Joshi, Prakriti Pradhan ^[1]; Maehrlein, Sebastian F. ^[1];

^[1]

Department of Chemistry Columbia University New York NY 10027 USA

Publication Date:: Wed Jan 23 00:00:00 EST 2019

Sponsoring Org.:: USDOE

OSTI Identifier:: 1491924

Grant/Contract Number:: N00014‐18‐1‐2080; DE‐SC0010692

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Advanced Materials

Additional Journal Information:: Journal Name: Advanced Materials Journal Volume: 31 Journal Issue: 47; Journal ID: ISSN 0935-9648

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Joshi, Prakriti Pradhan, Maehrlein, Sebastian F., and Zhu, Xiaoyang. Dynamic Screening and Slow Cooling of Hot Carriers in Lead Halide Perovskites.  Germany: N. p., 2019. 
Web.  doi:10.1002/adma.201803054.

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                    Joshi, Prakriti Pradhan, Maehrlein, Sebastian F., & Zhu, Xiaoyang. Dynamic Screening and Slow Cooling of Hot Carriers in Lead Halide Perovskites.  Germany.  https://doi.org/10.1002/adma.201803054

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                    Joshi, Prakriti Pradhan, Maehrlein, Sebastian F., and Zhu, Xiaoyang. Wed .  
"Dynamic Screening and Slow Cooling of Hot Carriers in Lead Halide Perovskites".  Germany.  https://doi.org/10.1002/adma.201803054.

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@article{osti_1491924,

  title        = {Dynamic Screening and Slow Cooling of Hot Carriers in Lead Halide Perovskites},

  author       = {Joshi, Prakriti Pradhan and Maehrlein, Sebastian F. and Zhu, Xiaoyang},

  abstractNote = {Abstract Among the exceptional properties of lead halide perovskites (LHPs) is the ultraslow cooling of hot carriers. Carrier densities below the Mott density for large polarons (≤ ≈10 18 cm −3 ) are focused on here. As in other semiconductors, a nascent hot electron distribution initially cools down via emission of longitudinal optical (LO) phonons on the 10 −14 –10 −13 s timescale. What distinguishes LHPs from conventional semiconductors is the exceptionally efficient screening in the former. The dielectric screening in LHPs on the 10 −13 s timescale results in an order‐of‐magnitude reduction in the Coulomb potential upon the formation of a large polaron, likely with ferroelectric‐like local ordering. Further LO‐phonon emission is inhibited, and this leads to partial retention of hot electron energy on the 10 −12 s timescale, more so in hybrid LHPs than in their all‐inorganic counterparts. Further cooling of hot polarons occurs on the 10 −10 s timescale, and this can be attributed to the slow diffusion of heat out of the large polaron volume due to the low thermal conductivity of LHPs. Like other carrier properties, slow hot carrier cooling in LHPs can be intimately related to efficient screening in a soft, anharmonic, and dynamically disordered lattice.},

  doi          = {10.1002/adma.201803054},

  journal      = {Advanced Materials},

  number       = 47,

  volume       = 31,

  place        = {Germany},

  year         = {Wed Jan 23 00:00:00 EST 2019},

  month        = {Wed Jan 23 00:00:00 EST 2019}

}

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It has been ten years since research on lead halide perovskites (LHPs) took off spectacularly and expanded into one of the most active fields today in chemistry, physics, materials science, and engineering. There is no doubt that the rapid growth of this field has been fueled by the exceptional performance of this class of materials in solar cells, light emitting devices, and other electronic, optoelectronic, and photonic devices. Such application oriented advance has been accompanied by major development in mechanistic understanding. Growing mechanistic studies on LHPs have revealed structure–property relationships including, among others, structural instability, unique defect chemistry, dynamic disordermore »« less
https://doi.org/10.1063/5.0020414

Full Text Available
Lead halide perovskites: Crystal-liquid duality, phonon glass electron crystals, and large polaron formation

Journal Article Miyata, Kiyoshi ; Atallah, Timothy L. ; Zhu, X. -Y. - Science Advances

Lead halide perovskites have been demonstrated as high performance materials in solar cells and light-emitting devices. These materials are characterized by coherent band transport expected from crystalline semiconductors, but dielectric responses and phonon dynamics typical of liquids. This “crystal-liquid” duality implies that lead halide perovskites belong to phonon glass electron crystals, a class of materials believed to make the most efficient thermoelectrics. We show that the crystal-liquid duality and the resulting dielectric response are responsible for large polaron formation and screening of charge carriers, leading to defect tolerance, moderate charge carrier mobility, and radiative recombination properties. Large polaron formation, alongmore »« less
Cited by 281
https://doi.org/10.1126/sciadv.1701469

Full Text Available
Decoding ultrafast polarization responses in lead halide perovskites by the two-dimensional optical Kerr effect

Journal Article Maehrlein, Sebastian F. ; Joshi, Prakriti P. ; Huber, Lucas ; ... - Proceedings of the National Academy of Sciences of the United States of America

The ultrafast polarization response to incident light and ensuing exciton/carrier generation are essential to outstanding optoelectronic properties of lead halide perovskites (LHPs). A large number of mechanistic studies in the LHP field to date have focused on contributions to polarizability from organic cations and the highly polarizable inorganic lattice. For a comprehensive understanding of the ultrafast polarization response, we must additionally account for the nearly instantaneous hyperpolarizability response to the propagating light field itself. While light propagation is pivotal to optoelectronics and photonics, little is known about this in LHPs in the vicinity of the bandgap where stimulated emission, polaritonmore »« less
https://doi.org/10.1073/pnas.2022268118

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Title: Dynamic Screening and Slow Cooling of Hot Carriers in Lead Halide Perovskites

Abstract

Citation Formats

Femtosecond hot‐carrier energy relaxation in GaAs journal, November 1987

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

Hot-carrier cooling and photoinduced refractive index changes in organic–inorganic lead halide perovskites journal, September 2015

Local Polar Fluctuations in Lead Halide Perovskite Crystals journal, March 2017

Dynamic disorder, phonon lifetimes, and the assignment of modes to the vibrational spectra of methylammonium lead halide perovskites journal, January 2016

Recent progress in relaxor ferroelectrics with perovskite structure journal, January 2006

Intrinsic Charge Transport across Phase Transitions in Hybrid Organo-Inorganic Perovskites journal, May 2016

Photogeneration of superparaelectric large polarons in dielectrics with soft anharmonic T 1 u phonons journal, May 2003

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

Efficiency of hot‐carrier solar energy converters journal, May 1982

Room-Temperature Coherent Optical Phonon in 2D Electronic Spectra of CH 3 NH 3 PbI 3 Perovskite as a Possible Cooling Bottleneck journal, June 2017

Temperature-Dependent Charge-Carrier Dynamics in CH 3 NH 3 PbI 3 Perovskite Thin Films journal, September 2015

Ultralow thermal conductivity in all-inorganic halide perovskites journal, July 2017

Metal halide perovskites for energy applications journal, May 2016

Quantization of Multiparticle Auger Rates in Semiconductor Quantum Dots journal, February 2000

Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells journal, May 2009

Exceeding the Shockley–Queisser limit in solar energy conversion journal, January 2013

Direct Observation of Dynamic Symmetry Breaking above Room Temperature in Methylammonium Lead Iodide Perovskite journal, October 2016

Trap-Free Hot Carrier Relaxation in Lead–Halide Perovskite Films journal, May 2017

Phonon Speed, Not Scattering, Differentiates Thermal Transport in Lead Halide Perovskites journal, August 2017

Breaking the phonon bottleneck in nanometer quantum dots: Role of Auger-like processes journal, January 1995

Optical phonons in methylammonium lead halide perovskites and implications for charge transport journal, January 2016

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

Slow hot carrier cooling in cesium lead iodide perovskites journal, October 2017

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

Hot-phonon effects in bulk GaAs journal, September 1987

Lead halide perovskites: Crystal-liquid duality, phonon glass electron crystals, and large polaron formation journal, October 2017

Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites journal, January 2017

Anisotropic and Ultralow Phonon Thermal Transport in Organic-Inorganic Hybrid Perovskites: Atomistic Insights into Solar Cell Thermal Management and Thermoelectric Energy Conversion Efficiency journal, May 2016

Phonon anharmonicity, lifetimes, and thermal transport in CH 3 NH 3 PbI 3 from many-body perturbation theory journal, December 2016

Transport Dynamics of a Large Acoustic Polaron in One Dimension journal, December 1983

Long-Lived Hot Carriers in Formamidinium Lead Iodide Nanocrystals journal, May 2017

Theory of super-para-electric large polaron for gigantic photo-enhancements of dielectric constant and electronic conductivity in SrTiO 3 journal, January 2005

Low electron-polar optical phonon scattering as a fundamental aspect of carrier mobility in methylammonium lead halide CH 3 NH 3 PbI 3 perovskites journal, January 2016

Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites journal, July 2017

Mechanical properties of A Pb X 3 ( A = Cs or CH 3 NH 3 ; X = I or Br) perovskite single crystals journal, October 2015

Role of Dielectric Drag in Polaron Mobility in Lead Halide Perovskites journal, October 2017

Direct observation of mode-specific phonon-band gap coupling in methylammonium lead halide perovskites journal, September 2017

Electron Dynamics at the ZnO (101̅0) Surface journal, July 2008

Perovskite Materials for Light-Emitting Diodes and Lasers journal, May 2016

Competition Between Hot-Electron Cooling and Large Polaron Screening in CsPbBr 3 Perovskite Single Crystals journal, December 2017

Interplay between organic cations and inorganic framework and incommensurability in hybrid lead-halide perovskite CH 3 NH 3 PbBr 3 journal, September 2017

Thermal Conductivity of CH 3 NH 3 PbI 3 and CsPbI 3 : Measuring the Effect of the Methylammonium Ion on Phonon Scattering journal, February 2017

Quantifying Polaron Formation and Charge Carrier Cooling in Lead-Iodide Perovskites journal, May 2018

Lattice Dynamics and Central-Mode Phenomena in the Dielectric Response of Ferroelectrics and Related Materials journal, January 2004

Phonon–Electron Scattering Limits Free Charge Mobility in Methylammonium Lead Iodide Perovskites journal, December 2015

Dynamic disorder in methylammoniumtrihalogenoplumbates (II) observed by millimeter‐wave spectroscopy journal, December 1987

Ultrafast Imaging of Carrier Cooling in Metal Halide Perovskite Thin Films journal, January 2018

Exploring Anomalous Polarization Dynamics in Organometallic Halide Perovskites journal, January 2018

Infrared dielectric constant of gallium arsenide journal, December 1996

Semiconductor excitons in new light journal, July 2006

Large polarons in lead halide perovskites journal, August 2017

Extended carrier lifetimes and diffusion in hybrid perovskites revealed by Hall effect and photoconductivity measurements journal, August 2016

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

Improved Understanding of the Electronic and Energetic Landscapes of Perovskite Solar Cells: High Local Charge Carrier Mobility, Reduced Recombination, and Extremely Shallow Traps journal, September 2014

Ultrafast carrier thermalization in lead iodide perovskite probed with two-dimensional electronic spectroscopy journal, August 2017

Dielectric Response: Answer to Many Questions in the Methylammonium Lead Halide Solar Cell Absorbers journal, May 2017

Dynamics of hot carrier cooling in photo-excited GaAs journal, September 1979

Ultra-Low Thermal Conductivity in Organic–Inorganic Hybrid Perovskite CH 3 NH 3 PbI 3 journal, July 2014

GIGANTEA is a co-chaperone which facilitates maturation of ZEITLUPE in the Arabidopsis circadian clock journal, February 2017

Persistent Energetic Electrons in Methylammonium Lead Iodide Perovskite Thin Films journal, November 2016

Screening of hot-carrier relaxation in highly photoexcited semiconductors journal, February 1981

Tetragonal CH 3 NH 3 PbI 3 is ferroelectric journal, June 2017

Making and Breaking of Lead Halide Perovskites journal, January 2016

Dynamical Origin of the Rashba Effect in Organohalide Lead Perovskites: A Key to Suppressed Carrier Recombination in Perovskite Solar Cells? journal, April 2016

Charge transport in hybrid halide perovskites journal, November 2017

Organic-Inorganic Halide Perovskite Photovoltaics book, January 2016

Barrier to recombination of oppositely charged large polarons journal, February 2018

Molecular disorder and translation/rotation coupling in the plastic crystal phase of hybrid perovskites journal, January 2016

Detailed Balance Limit of Efficiency of p‐n Junction Solar Cells journal, March 1961

Slow Cooling of Hot Polarons in Halide Perovskite Solar Cells journal, October 2017

Relaxing with relaxors: a review of relaxor ferroelectrics journal, April 2011

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

Ferroelectric large polarons journal, April 2018

Structural Phase- and Degradation-Dependent Thermal Conductivity of CH 3 NH 3 PbI 3 Perovskite Thin Films journal, March 2016

CH 3 NH 3 PbI 3 perovskites: Ferroelasticity revealed journal, April 2017

Photoinduced Giant Dielectric Constant in Lead Halide Perovskite Solar Cells journal, June 2014

Femtosecond hot‐carrier energy relaxation in GaAs
journal, November 1987

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

Hot-carrier cooling and photoinduced refractive index changes in organic–inorganic lead halide perovskites
journal, September 2015

Local Polar Fluctuations in Lead Halide Perovskite Crystals
journal, March 2017

Dynamic disorder, phonon lifetimes, and the assignment of modes to the vibrational spectra of methylammonium lead halide perovskites
journal, January 2016

Recent progress in relaxor ferroelectrics with perovskite structure
journal, January 2006

Intrinsic Charge Transport across Phase Transitions in Hybrid Organo-Inorganic Perovskites
journal, May 2016

Photogeneration of superparaelectric large polarons in dielectrics with soft anharmonic $T_{1 u}$ phonons
journal, May 2003

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

Efficiency of hot‐carrier solar energy converters
journal, May 1982

Room-Temperature Coherent Optical Phonon in 2D Electronic Spectra of CH ₃ NH ₃ PbI ₃ Perovskite as a Possible Cooling Bottleneck
journal, June 2017

Temperature-Dependent Charge-Carrier Dynamics in CH ₃ NH ₃ PbI ₃ Perovskite Thin Films
journal, September 2015

Ultralow thermal conductivity in all-inorganic halide perovskites
journal, July 2017

Metal halide perovskites for energy applications
journal, May 2016

Quantization of Multiparticle Auger Rates in Semiconductor Quantum Dots
journal, February 2000

Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells
journal, May 2009

Exceeding the Shockley–Queisser limit in solar energy conversion
journal, January 2013

Direct Observation of Dynamic Symmetry Breaking above Room Temperature in Methylammonium Lead Iodide Perovskite
journal, October 2016

Trap-Free Hot Carrier Relaxation in Lead–Halide Perovskite Films
journal, May 2017

Phonon Speed, Not Scattering, Differentiates Thermal Transport in Lead Halide Perovskites
journal, August 2017

Breaking the phonon bottleneck in nanometer quantum dots: Role of Auger-like processes
journal, January 1995

Optical phonons in methylammonium lead halide perovskites and implications for charge transport
journal, January 2016

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

Slow hot carrier cooling in cesium lead iodide perovskites
journal, October 2017

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

Hot-phonon effects in bulk GaAs
journal, September 1987

Lead halide perovskites: Crystal-liquid duality, phonon glass electron crystals, and large polaron formation
journal, October 2017

Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites
journal, January 2017

Anisotropic and Ultralow Phonon Thermal Transport in Organic-Inorganic Hybrid Perovskites: Atomistic Insights into Solar Cell Thermal Management and Thermoelectric Energy Conversion Efficiency
journal, May 2016

Phonon anharmonicity, lifetimes, and thermal transport in ${CH}_{3} {NH}_{3} {PbI}_{3}$ from many-body perturbation theory
journal, December 2016

Transport Dynamics of a Large Acoustic Polaron in One Dimension
journal, December 1983

Long-Lived Hot Carriers in Formamidinium Lead Iodide Nanocrystals
journal, May 2017

Theory of super-para-electric large polaron for gigantic photo-enhancements of dielectric constant and electronic conductivity in SrTiO ₃
journal, January 2005

Low electron-polar optical phonon scattering as a fundamental aspect of carrier mobility in methylammonium lead halide CH ₃ NH ₃ PbI ₃ perovskites
journal, January 2016

Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites
journal, July 2017

Mechanical properties of A Pb X ₃ ( A = Cs or CH ₃ NH ₃ ; X = I or Br) perovskite single crystals
journal, October 2015

Role of Dielectric Drag in Polaron Mobility in Lead Halide Perovskites
journal, October 2017

Direct observation of mode-specific phonon-band gap coupling in methylammonium lead halide perovskites
journal, September 2017

Electron Dynamics at the ZnO (101̅0) Surface
journal, July 2008

Perovskite Materials for Light-Emitting Diodes and Lasers
journal, May 2016

Competition Between Hot-Electron Cooling and Large Polaron Screening in CsPbBr ₃ Perovskite Single Crystals
journal, December 2017

Interplay between organic cations and inorganic framework and incommensurability in hybrid lead-halide perovskite ${CH}_{3} {NH}_{3} {PbBr}_{3}$
journal, September 2017

Thermal Conductivity of CH ₃ NH ₃ PbI ₃ and CsPbI ₃ : Measuring the Effect of the Methylammonium Ion on Phonon Scattering
journal, February 2017

Quantifying Polaron Formation and Charge Carrier Cooling in Lead-Iodide Perovskites
journal, May 2018

Lattice Dynamics and Central-Mode Phenomena in the Dielectric Response of Ferroelectrics and Related Materials
journal, January 2004

Phonon–Electron Scattering Limits Free Charge Mobility in Methylammonium Lead Iodide Perovskites
journal, December 2015

Dynamic disorder in methylammoniumtrihalogenoplumbates (II) observed by millimeter‐wave spectroscopy
journal, December 1987

Ultrafast Imaging of Carrier Cooling in Metal Halide Perovskite Thin Films
journal, January 2018

Exploring Anomalous Polarization Dynamics in Organometallic Halide Perovskites
journal, January 2018

Infrared dielectric constant of gallium arsenide
journal, December 1996

Semiconductor excitons in new light
journal, July 2006

Large polarons in lead halide perovskites
journal, August 2017

Extended carrier lifetimes and diffusion in hybrid perovskites revealed by Hall effect and photoconductivity measurements
journal, August 2016

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

Improved Understanding of the Electronic and Energetic Landscapes of Perovskite Solar Cells: High Local Charge Carrier Mobility, Reduced Recombination, and Extremely Shallow Traps
journal, September 2014

Ultrafast carrier thermalization in lead iodide perovskite probed with two-dimensional electronic spectroscopy
journal, August 2017

Dielectric Response: Answer to Many Questions in the Methylammonium Lead Halide Solar Cell Absorbers
journal, May 2017

Dynamics of hot carrier cooling in photo-excited GaAs
journal, September 1979

Ultra-Low Thermal Conductivity in Organic–Inorganic Hybrid Perovskite CH ₃ NH ₃ PbI ₃
journal, July 2014

GIGANTEA is a co-chaperone which facilitates maturation of ZEITLUPE in the Arabidopsis circadian clock
journal, February 2017

Persistent Energetic Electrons in Methylammonium Lead Iodide Perovskite Thin Films
journal, November 2016

Screening of hot-carrier relaxation in highly photoexcited semiconductors
journal, February 1981

Tetragonal CH ₃ NH ₃ PbI ₃ is ferroelectric
journal, June 2017

Making and Breaking of Lead Halide Perovskites
journal, January 2016

Dynamical Origin of the Rashba Effect in Organohalide Lead Perovskites: A Key to Suppressed Carrier Recombination in Perovskite Solar Cells?
journal, April 2016

Charge transport in hybrid halide perovskites
journal, November 2017

Organic-Inorganic Halide Perovskite Photovoltaics
book, January 2016

Barrier to recombination of oppositely charged large polarons
journal, February 2018

Molecular disorder and translation/rotation coupling in the plastic crystal phase of hybrid perovskites
journal, January 2016

Detailed Balance Limit of Efficiency of p‐n Junction Solar Cells
journal, March 1961

Slow Cooling of Hot Polarons in Halide Perovskite Solar Cells
journal, October 2017

Relaxing with relaxors: a review of relaxor ferroelectrics
journal, April 2011

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

Ferroelectric large polarons
journal, April 2018

Structural Phase- and Degradation-Dependent Thermal Conductivity of CH ₃ NH ₃ PbI ₃ Perovskite Thin Films
journal, March 2016

CH ₃ NH ₃ PbI ₃ perovskites: Ferroelasticity revealed
journal, April 2017

Photoinduced Giant Dielectric Constant in Lead Halide Perovskite Solar Cells
journal, June 2014

Hot carrier cooling mechanisms in halide perovskites
journal, November 2017

Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy
journal, April 2017

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