Spatial–temporal spectroscopy characterizations and electronic structure of methylammonium perovskites

Liu, Zhaoyu; Bhamu, K. C.; Luo, Liang; Shah, Satvik; Park, Joong -Mok; Cheng, Di; Long, Men; Biswas, Rana; Fungara, F.; Shinar, Ruth; Shinar, Joseph; Vela, Javier; Wang, Jigang

doi:10.1557/mrc.2018.114

Title: Spatial–temporal spectroscopy characterizations and electronic structure of methylammonium perovskites

Abstract

Using time-resolved laser-scanning confocal microscopy and ultrafast optical pump/THz probe spectroscopy, we measure photoluminescence (PL) and THz-conductivity in perovskite micro-crystals and films. PL quenching and lifetime variations occur from local heterogeneity. Ultrafast THz-spectra measure sharp quantum transitions from excitonic Rydberg states, providing weakly bound excitons with a binding energy of ~13.5 meV at low temperatures. Ab-initio electronic structure calculations give a direct band gap of 1.64 eV, a dielectric constant of ~18, heavy electrons, and light holes, resulting in weakly bound excitons, consistent with the binding energies from the experiment. Here, the complementary spectroscopy and simulations reveal fundamental insights into perovskite light-matter interactions.

Authors:

Liu, Zhaoyu ^[1]; Bhamu, K. C. ^[2]; Luo, Liang ^[1]; Shah, Satvik ^[3]; Park, Joong -Mok ^[1]; Cheng, Di ^[1]; Long, Men ^[1];

^[1]; Fungara, F. ^[1]; Shinar, Ruth ^[3]; Shinar, Joseph ^[1]; Vela, Javier ^[1]; Wang, Jigang ^[1]

Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
CSIR-National Chemical Lab., Maharashtra (India)
Iowa State Univ., Ames, IA (United States)

Publication Date:: Mon Jul 09 00:00:00 EDT 2018

Research Org.:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1461658

Report Number(s):: IS-J-9714
Journal ID: ISSN 2159-6859; PII: S2159685918001143

Grant/Contract Number:: 61771402; 61505164; 11674266; 11372248; 51575297; AC02-07CH11358

Resource Type:: Accepted Manuscript

Journal Name:: MRS Communications

Additional Journal Information:: Journal Volume: 10; Journal Issue: 25; Journal ID: ISSN 2159-6859

Publisher:: Materials Research Society - Cambridge University Press

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; ultrafast spectroscopy; perovskites; excitonic spectra; electronic structure

Citation Formats


                    Liu, Zhaoyu, Bhamu, K. C., Luo, Liang, Shah, Satvik, Park, Joong -Mok, Cheng, Di, Long, Men, Biswas, Rana, Fungara, F., Shinar, Ruth, Shinar, Joseph, Vela, Javier, and Wang, Jigang. Spatial–temporal spectroscopy characterizations and electronic structure of methylammonium perovskites.  United States: N. p., 2018. 
Web.  doi:10.1557/mrc.2018.114.

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                    Liu, Zhaoyu, Bhamu, K. C., Luo, Liang, Shah, Satvik, Park, Joong -Mok, Cheng, Di, Long, Men, Biswas, Rana, Fungara, F., Shinar, Ruth, Shinar, Joseph, Vela, Javier, & Wang, Jigang. Spatial–temporal spectroscopy characterizations and electronic structure of methylammonium perovskites.  United States.  https://doi.org/10.1557/mrc.2018.114

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                    Liu, Zhaoyu, Bhamu, K. C., Luo, Liang, Shah, Satvik, Park, Joong -Mok, Cheng, Di, Long, Men, Biswas, Rana, Fungara, F., Shinar, Ruth, Shinar, Joseph, Vela, Javier, and Wang, Jigang. Mon .  
"Spatial–temporal spectroscopy characterizations and electronic structure of methylammonium perovskites".  United States.  https://doi.org/10.1557/mrc.2018.114.  https://www.osti.gov/servlets/purl/1461658.

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@article{osti_1461658,

  title        = {Spatial–temporal spectroscopy characterizations and electronic structure of methylammonium perovskites},

  author       = {Liu, Zhaoyu and Bhamu, K. C. and Luo, Liang and Shah, Satvik and Park, Joong -Mok and Cheng, Di and Long, Men and Biswas, Rana and Fungara, F. and Shinar, Ruth and Shinar, Joseph and Vela, Javier and Wang, Jigang},

  abstractNote = {Using time-resolved laser-scanning confocal microscopy and ultrafast optical pump/THz probe spectroscopy, we measure photoluminescence (PL) and THz-conductivity in perovskite micro-crystals and films. PL quenching and lifetime variations occur from local heterogeneity. Ultrafast THz-spectra measure sharp quantum transitions from excitonic Rydberg states, providing weakly bound excitons with a binding energy of ~13.5 meV at low temperatures. Ab-initio electronic structure calculations give a direct band gap of 1.64 eV, a dielectric constant of ~18, heavy electrons, and light holes, resulting in weakly bound excitons, consistent with the binding energies from the experiment. Here, the complementary spectroscopy and simulations reveal fundamental insights into perovskite light-matter interactions.},

  doi          = {10.1557/mrc.2018.114},

  journal      = {MRS Communications},

  number       = 25,

  volume       = 10,

  place        = {United States},

  year         = {Mon Jul 09 00:00:00 EDT 2018},

  month        = {Mon Jul 09 00:00:00 EDT 2018}

}

Copy to clipboard

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The Journal of Chemical Physics, Vol. 151, Issue 24
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Title: Spatial–temporal spectroscopy characterizations and electronic structure of methylammonium perovskites

Abstract

Citation Formats

Generalized Gradient Approximation Made Simple journal, October 1996

Metal-halide perovskites for photovoltaic and light-emitting devices journal, May 2015

Principles of the Theory of Solids book, January 1972

Perovskite solar cells join the major league journal, November 2015

Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite journal, June 2017

Direct Observation of Long Electron-Hole Diffusion Distance in CH3NH3PbI3 Perovskite Thin Film journal, September 2015

The Effects of the Organic–Inorganic Interactions on the Thermal Transport Properties of CH 3 NH 3 PbI 3 journal, March 2016

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

Iodine Migration and its Effect on Hysteresis in Perovskite Solar Cells journal, January 2016

Organometal Perovskite Light Absorbers Toward a 20% Efficiency Low-Cost Solid-State Mesoscopic Solar Cell journal, July 2013

Impact of Monovalent Cation Halide Additives on the Structural and Optoelectronic Properties of CH 3 NH 3 PbI 3 Perovskite journal, March 2016

Reversible Structural Swell–Shrink and Recoverable Optical Properties in Hybrid Inorganic–Organic Perovskite journal, July 2016

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

Ionic polarization-induced current–voltage hysteresis in CH3NH3PbX3 perovskite solar cells journal, February 2016

Interface engineering of highly efficient perovskite solar cells journal, July 2014

Imaging the Long Transport Lengths of Photo-generated Carriers in Oriented Perovskite Films journal, December 2016

Growth of CH3NH3PbI3 cuboids with controlled size for high-efficiency perovskite solar cells journal, August 2014

Structures and Electronic Properties of Different CH3NH3PbI3/TiO2 Interface: A First-Principles Study journal, February 2016

Structural, optical, and electrical properties of phase-controlled cesium lead iodide nanowires journal, February 2017

Lead iodide perovskite light-emitting field-effect transistor journal, June 2015

Cesium-containing triple cation perovskite solar cells: improved stability, reproducibility and high efficiency journal, January 2016

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

Crystal Structures, Optical Properties, and Effective Mass Tensors of CH 3 NH 3 PbX 3 (X = I and Br) Phases Predicted from HSE06 journal, March 2014

Solvent engineering for high-performance inorganic–organic hybrid perovskite solar cells journal, July 2014

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

High efficiency sequentially vapor grown n-i-p CH 3 NH 3 PbI 3 perovskite solar cells with undoped P3HT as p-type heterojunction layer journal, January 2015

CH 3 NH 3 PbI 3– x Cl x under Different Fabrication Strategies: Electronic Structures and Energy-Level Alignment with an Organic Hole Transport Material journal, February 2017

Computed and Experimental Absorption Spectra of the Perovskite CH 3 NH 3 PbI 3 journal, August 2014

Elucidating the role of disorder and free-carrier recombination kinetics in CH3NH3PbI3 perovskite films journal, July 2015

Electronic Structure of TiO 2 /CH 3 NH 3 PbI 3 Perovskite Solar Cell Interfaces journal, January 2014

Density functional theory analysis of structural and electronic properties of orthorhombic perovskite CH 3 NH 3 PbI 3 journal, January 2014

Characterization of an abnormal photoluminescence behavior upon crystal-phase transition of perovskite CH 3 NH 3 PbI 3 journal, January 2015

Accurate Band Gaps of Semiconductors and Insulators with a Semilocal Exchange-Correlation Potential journal, June 2009

Structural and optical properties of methylammonium lead iodide across the tetragonal to cubic phase transition: implications for perovskite solar cells journal, January 2016

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

First-Principles Study of Lead Iodide Perovskite Tetragonal and Orthorhombic Phases for Photovoltaics journal, August 2014

Brighter pieces of the puzzle journal, July 2015

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

Efficient organometal trihalide perovskite planar-heterojunction solar cells on flexible polymer substrates journal, November 2013

Phonon Mode Transformation Across the Orthohombic–Tetragonal Phase Transition in a Lead Iodide Perovskite CH 3 NH 3 PbI 3 : A Terahertz Time-Domain Spectroscopy Approach journal, December 2015

Surface Properties of CH 3 NH 3 PbI 3 for Perovskite Solar Cells journal, February 2016

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

Principles of the theory of solids journal, July 1965

Helicity-dependent terahertz photocurrent and phonon dynamics in hybrid metal halide perovskites journal, December 2019

Generalized Gradient Approximation Made Simple
journal, October 1996

Metal-halide perovskites for photovoltaic and light-emitting devices
journal, May 2015

Principles of the Theory of Solids
book, January 1972

Perovskite solar cells join the major league
journal, November 2015

Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite
journal, June 2017

Direct Observation of Long Electron-Hole Diffusion Distance in CH3NH3PbI3 Perovskite Thin Film
journal, September 2015

The Effects of the Organic–Inorganic Interactions on the Thermal Transport Properties of CH ₃ NH ₃ PbI ₃
journal, March 2016

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

Iodine Migration and its Effect on Hysteresis in Perovskite Solar Cells
journal, January 2016

Organometal Perovskite Light Absorbers Toward a 20% Efficiency Low-Cost Solid-State Mesoscopic Solar Cell
journal, July 2013

Impact of Monovalent Cation Halide Additives on the Structural and Optoelectronic Properties of CH ₃ NH ₃ PbI ₃ Perovskite
journal, March 2016

Reversible Structural Swell–Shrink and Recoverable Optical Properties in Hybrid Inorganic–Organic Perovskite
journal, July 2016

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

Ionic polarization-induced current–voltage hysteresis in CH3NH3PbX3 perovskite solar cells
journal, February 2016

Interface engineering of highly efficient perovskite solar cells
journal, July 2014

Imaging the Long Transport Lengths of Photo-generated Carriers in Oriented Perovskite Films
journal, December 2016

Growth of CH3NH3PbI3 cuboids with controlled size for high-efficiency perovskite solar cells
journal, August 2014

Structures and Electronic Properties of Different CH3NH3PbI3/TiO2 Interface: A First-Principles Study
journal, February 2016

Structural, optical, and electrical properties of phase-controlled cesium lead iodide nanowires
journal, February 2017

Lead iodide perovskite light-emitting field-effect transistor
journal, June 2015

Cesium-containing triple cation perovskite solar cells: improved stability, reproducibility and high efficiency
journal, January 2016

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

Crystal Structures, Optical Properties, and Effective Mass Tensors of CH ₃ NH ₃ PbX ₃ (X = I and Br) Phases Predicted from HSE06
journal, March 2014

Solvent engineering for high-performance inorganic–organic hybrid perovskite solar cells
journal, July 2014

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

High efficiency sequentially vapor grown n-i-p CH ₃ NH ₃ PbI ₃ perovskite solar cells with undoped P3HT as p-type heterojunction layer
journal, January 2015

CH ₃ NH ₃ PbI _{3– x} Cl _x under Different Fabrication Strategies: Electronic Structures and Energy-Level Alignment with an Organic Hole Transport Material
journal, February 2017

Computed and Experimental Absorption Spectra of the Perovskite CH ₃ NH ₃ PbI ₃
journal, August 2014

Elucidating the role of disorder and free-carrier recombination kinetics in CH3NH3PbI3 perovskite films
journal, July 2015

Electronic Structure of TiO ₂ /CH ₃ NH ₃ PbI ₃ Perovskite Solar Cell Interfaces
journal, January 2014

Density functional theory analysis of structural and electronic properties of orthorhombic perovskite CH ₃ NH ₃ PbI ₃
journal, January 2014

Characterization of an abnormal photoluminescence behavior upon crystal-phase transition of perovskite CH ₃ NH ₃ PbI ₃
journal, January 2015

Accurate Band Gaps of Semiconductors and Insulators with a Semilocal Exchange-Correlation Potential
journal, June 2009

Structural and optical properties of methylammonium lead iodide across the tetragonal to cubic phase transition: implications for perovskite solar cells
journal, January 2016

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

First-Principles Study of Lead Iodide Perovskite Tetragonal and Orthorhombic Phases for Photovoltaics
journal, August 2014

Brighter pieces of the puzzle
journal, July 2015

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

Efficient organometal trihalide perovskite planar-heterojunction solar cells on flexible polymer substrates
journal, November 2013

Phonon Mode Transformation Across the Orthohombic–Tetragonal Phase Transition in a Lead Iodide Perovskite CH ₃ NH ₃ PbI ₃ : A Terahertz Time-Domain Spectroscopy Approach
journal, December 2015

Surface Properties of CH ₃ NH ₃ PbI ₃ for Perovskite Solar Cells
journal, February 2016

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

Principles of the theory of solids
journal, July 1965

Helicity-dependent terahertz photocurrent and phonon dynamics in hybrid metal halide perovskites
journal, December 2019