Excitons in ultrathin organic-inorganic perovskite crystals

Yaffe, Omer; Chernikov, Alexey; Norman, Zachariah M.; Zhong, Yu; Velauthapillai, Ajanthkrishna; van der Zande, Arend; Owen, Jonathan S.; Heinz, Tony F.

doi:10.1103/PhysRevB.92.045414

Title: Excitons in ultrathin organic-inorganic perovskite crystals

Abstract

In this work, we demonstrate the formation of large sheets of layered organic-inorganic perovskite (OIPC) crystals, as thin as a single unit cell, prepared by mechanical exfoliation. The resulting two-dimensional OIPC nanosheets of 2.4 nm thickness are direct semiconductors with an optical band gap of 2.4 eV. They exhibit unusually strong light-matter interaction with an optical absorption as high as 25% at the main excitonic resonance, as well as bright photoluminescence. We extract an exciton binding energy of 490 meV from measurement of the series of excited exciton states. The properties of the excitons are shown to be strongly influenced by the changes in the dielectric surroundings. The environmental sensitivity of these ultrathin OIPC sheets is further reflected in the strong suppression of a thermally driven phase transition present in the bulk crystals.

Authors:

Yaffe, Omer ^[1]; Chernikov, Alexey ^[1]; Norman, Zachariah M. ^[1]; Zhong, Yu ^[1]; Velauthapillai, Ajanthkrishna ^[1]; van der Zande, Arend ^[1]; Owen, Jonathan S. ^[1]; Heinz, Tony F. ^[2]

Columbia Univ., New York, NY (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Publication Date:: Tue Jul 14 00:00:00 EDT 2015

Research Org.:: Energy Frontier Research Centers (EFRC) (United States). Re-Defining Photovoltaic Efficiency Through Molecule Scale Control (RPEMSC); Columbia Univ., New York, NY (United States)

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

OSTI Identifier:: 1385960

Alternate Identifier(s):: OSTI ID: 1194264

Grant/Contract Number:: SC0001085

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review. B, Condensed Matter and Materials Physics

Additional Journal Information:: Journal Volume: 92; Journal Issue: 4; Related Information: RPEMSC partners with Columbia University (lead); Brookhaven National Laboratory; Purdue University; Journal ID: ISSN 1098-0121

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; solar (photovoltaic); electrodes - solar; charge transport; materials and chemistry by design; optics; synthesis (novel materials)

Citation Formats


                    Yaffe, Omer, Chernikov, Alexey, Norman, Zachariah M., Zhong, Yu, Velauthapillai, Ajanthkrishna, van der Zande, Arend, Owen, Jonathan S., and Heinz, Tony F. Excitons in ultrathin organic-inorganic perovskite crystals.  United States: N. p., 2015. 
Web.  doi:10.1103/PhysRevB.92.045414.

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                    Yaffe, Omer, Chernikov, Alexey, Norman, Zachariah M., Zhong, Yu, Velauthapillai, Ajanthkrishna, van der Zande, Arend, Owen, Jonathan S., & Heinz, Tony F. Excitons in ultrathin organic-inorganic perovskite crystals.  United States.  https://doi.org/10.1103/PhysRevB.92.045414

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                    Yaffe, Omer, Chernikov, Alexey, Norman, Zachariah M., Zhong, Yu, Velauthapillai, Ajanthkrishna, van der Zande, Arend, Owen, Jonathan S., and Heinz, Tony F. Tue .  
"Excitons in ultrathin organic-inorganic perovskite crystals".  United States.  https://doi.org/10.1103/PhysRevB.92.045414.  https://www.osti.gov/servlets/purl/1385960.

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@article{osti_1385960,

  title        = {Excitons in ultrathin organic-inorganic perovskite crystals},

  author       = {Yaffe, Omer and Chernikov, Alexey and Norman, Zachariah M. and Zhong, Yu and Velauthapillai, Ajanthkrishna and van der Zande, Arend and Owen, Jonathan S. and Heinz, Tony F.},

  abstractNote = {In this work, we demonstrate the formation of large sheets of layered organic-inorganic perovskite (OIPC) crystals, as thin as a single unit cell, prepared by mechanical exfoliation. The resulting two-dimensional OIPC nanosheets of 2.4 nm thickness are direct semiconductors with an optical band gap of 2.4 eV. They exhibit unusually strong light-matter interaction with an optical absorption as high as 25% at the main excitonic resonance, as well as bright photoluminescence. We extract an exciton binding energy of 490 meV from measurement of the series of excited exciton states. The properties of the excitons are shown to be strongly influenced by the changes in the dielectric surroundings. The environmental sensitivity of these ultrathin OIPC sheets is further reflected in the strong suppression of a thermally driven phase transition present in the bulk crystals.},

  doi          = {10.1103/PhysRevB.92.045414},

  journal      = {Physical Review. B, Condensed Matter and Materials Physics},

  number       = 4,

  volume       = 92,

  place        = {United States},

  year         = {Tue Jul 14 00:00:00 EDT 2015},

  month        = {Tue Jul 14 00:00:00 EDT 2015}

}

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Cortecchia, D.; Neutzner, S.; Yin, J.
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Title: Excitons in ultrathin organic-inorganic perovskite crystals

Abstract

Citation Formats

Quantum Theory of the Optical and Electronic Properties of Semiconductors book, January 2009

Exciton state in two-dimensional perovskite semiconductor (C10H21NH3)2PbI4 journal, March 1989

Analytical approach to excitonic properties of MoS 2 journal, March 2014

Semiconductor Optics book, March 2007

Influence of the image charge effect on excitonic energy structure in organic-inorganic multiple quantum well crystals journal, March 2013

Progress, Challenges, and Opportunities in Two-Dimensional Materials Beyond Graphene journal, March 2013

Excitons in self-organized semiconductor/insulator superlattices: PbI-based perovskite compounds journal, May 1995

Relativistic GW calculations on CH3NH3PbI3 and CH3NH3SnI3 Perovskites for Solar Cell Applications journal, March 2014

Dielectric screening in two-dimensional insulators: Implications for excitonic and impurity states in graphane journal, August 2011

Optical spectroscopy of two-dimensional layered (C_6H_5C_2H_4-NH_3)_2-PbI_4 perovskite journal, January 2010

Graphene: Status and Prospects journal, June 2009

Electronic and Excitonic Structures of Inorganic–Organic Perovskite-Type Quantum-Well Crystal (C 4 H 9 NH 3 ) 2 PbBr 4 journal, August 2005

High Open-Circuit Voltage Solar Cells Based on Organic–Inorganic Lead Bromide Perovskite journal, March 2013

Optical Spectrum of MoS 2 : Many-Body Effects and Diversity of Exciton States journal, November 2013

Probing excitonic dark states in single-layer tungsten disulphide journal, August 2014

Synthesis of Large-Area MoS2 Atomic Layers with Chemical Vapor Deposition journal, March 2012

Synthesis and optical properties of novel organic–inorganic hybrid nanolayer structure semiconductors journal, June 2009

Semiconducting Tin and Lead Iodide Perovskites with Organic Cations: Phase Transitions, High Mobilities, and Near-Infrared Photoluminescent Properties journal, July 2013

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

Large excitonic effects in monolayers of molybdenum and tungsten dichalcogenides journal, September 2012

Synthetic Three-and Lower-Dimensional Semiconductors Based on Inorganic Units journal, July 1996

Organic-inorganic electronics journal, January 2001

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

Absorption coefficients and exciton oscillator strengths in AlGaAs-GaAs superlattices journal, December 1985

Influence of dielectric confinement on excitonic nonlinearity in inorganic-organic layered semiconductors journal, May 2005

Electronic model for self-assembled hybrid organic/perovskite semiconductors: Reverse band edge electronic states ordering and spin-orbit coupling journal, November 2012

Grains and grain boundaries in highly crystalline monolayer molybdenum disulphide journal, May 2013

Making graphene visible journal, August 2007

Strong exciton-photon coupling in microcavities containing new fluorophenethylamine based perovskite compounds journal, January 2012

Tightly Bound Excitons in Monolayer WSe 2 journal, July 2014

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

Van der Waals heterostructures journal, July 2013

Efficient inorganic–organic hybrid heterojunction solar cells containing perovskite compound and polymeric hole conductors journal, May 2013

Electronics and optoelectronics of two-dimensional transition metal dichalcogenides journal, November 2012

Photoconductivity and electroluminescence in lead iodide based natural quantum well structures journal, November 1992

Dielectric confinement effect on excitons in PbI 4 -based layered semiconductors journal, March 1992

Exciton band structure of monolayer MoS 2 journal, February 2015

Emerging Device Applications for Semiconducting Two-Dimensional Transition Metal Dichalcogenides journal, January 2014

Synthesis, Crystal Structure, and Optical and Thermal Properties of (C4H9NH3)2MI4 (M = Ge, Sn, Pb) journal, January 1996

Optical Identification of Single- and Few-Layer MoS2 Sheets journal, January 2012

Efficient planar heterojunction perovskite solar cells by vapour deposition journal, September 2013

A roadmap for graphene journal, October 2012

Absorption spectroscopy on Ga 0.47 In 0.53 As/ Al 0 . 4 8 L In 0.52 As multi-quantum-well heterostructures. I. Excitonic transitions journal, September 1987

The rise of graphene journal, March 2007

Image charge effect on two-dimensional excitons in an inorganic-organic quantum-well crystal journal, January 2005

Electron−Hole Interaction in Carbon Nanotubes: Novel Screening and Exciton Excitation Spectra journal, April 2009

Optical properties due to electronic transitions in two-dimensional semiconductors ( C n H 2 n + 1 NH 3 ) 2 PbI 4 journal, December 1990

Understanding Quantum Confinement of Charge Carriers in Layered 2D Hybrid Perovskites journal, September 2014

Exfoliation of self-assembled 2D organic-inorganic perovskite semiconductors journal, April 2014

Magnetoabsorption of the lowest exciton in perovskite-type compound (CH3NH3)PbI3 journal, July 1994

Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS 2 journal, August 2014

Theory of neutral and charged excitons in monolayer transition metal dichalcogenides journal, July 2013

Quasiparticle band structures and optical properties of strained monolayer MoS 2 and WS 2 journal, April 2013

Quasiparticle band structure calculation of monolayer, bilayer, and bulk MoS 2 journal, May 2012

Fine Structure Constant Defines Visual Transparency of Graphene journal, June 2008

Semiconductor Optics book, January 2012

The rise of graphene book, August 2009

Semiconductor Optics book, January 2005

Theory of Neutral and Charged Excitons in Monolayer Transition Metal Dichalcogenides text, January 2013

Emerging Device Applications for Semiconducting Two-Dimensional Transition Metal Dichalcogenides text, January 2014

Probing Excitonic Dark States in Single-layer Tungsten Disulfide text, January 2014

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Ultrathin Two-Dimensional Organic-Inorganic Hybrid Perovskite Nanosheets with Bright, Tunable Photoluminescence and High Stability journal, March 2017

Ultrafast Carrier Transfer Promoted by Interlayer Coulomb Coupling in 2D/3D Perovskite Heterostructures journal, September 2018

Intrinsic Carrier Transport of Phase-Pure Homologous 2D Organolead Halide Hybrid Perovskite Single Crystals journal, November 2018

Quantum Theory of the Optical and Electronic Properties of Semiconductors
book, January 2009

Exciton state in two-dimensional perovskite semiconductor (C10H21NH3)2PbI4
journal, March 1989

Analytical approach to excitonic properties of MoS $_{2}$
journal, March 2014

Semiconductor Optics
book, March 2007

Influence of the image charge effect on excitonic energy structure in organic-inorganic multiple quantum well crystals
journal, March 2013

Progress, Challenges, and Opportunities in Two-Dimensional Materials Beyond Graphene
journal, March 2013

Excitons in self-organized semiconductor/insulator superlattices: PbI-based perovskite compounds
journal, May 1995

Relativistic GW calculations on CH3NH3PbI3 and CH3NH3SnI3 Perovskites for Solar Cell Applications
journal, March 2014

Dielectric screening in two-dimensional insulators: Implications for excitonic and impurity states in graphane
journal, August 2011

Optical spectroscopy of two-dimensional layered (C_6H_5C_2H_4-NH_3)_2-PbI_4 perovskite
journal, January 2010

Graphene: Status and Prospects
journal, June 2009

Electronic and Excitonic Structures of Inorganic–Organic Perovskite-Type Quantum-Well Crystal (C ₄ H ₉ NH ₃ ) ₂ PbBr ₄
journal, August 2005

High Open-Circuit Voltage Solar Cells Based on Organic–Inorganic Lead Bromide Perovskite
journal, March 2013

Optical Spectrum of ${MoS}_{2}$ : Many-Body Effects and Diversity of Exciton States
journal, November 2013

Probing excitonic dark states in single-layer tungsten disulphide
journal, August 2014

Synthesis of Large-Area MoS₂ Atomic Layers with Chemical Vapor Deposition
journal, March 2012

Synthesis and optical properties of novel organic–inorganic hybrid nanolayer structure semiconductors
journal, June 2009

Semiconducting Tin and Lead Iodide Perovskites with Organic Cations: Phase Transitions, High Mobilities, and Near-Infrared Photoluminescent Properties
journal, July 2013

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

Large excitonic effects in monolayers of molybdenum and tungsten dichalcogenides
journal, September 2012

Synthetic Three-and Lower-Dimensional Semiconductors Based on Inorganic Units
journal, July 1996

Organic-inorganic electronics
journal, January 2001

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

Absorption coefficients and exciton oscillator strengths in AlGaAs-GaAs superlattices
journal, December 1985

Influence of dielectric confinement on excitonic nonlinearity in inorganic-organic layered semiconductors
journal, May 2005

Electronic model for self-assembled hybrid organic/perovskite semiconductors: Reverse band edge electronic states ordering and spin-orbit coupling
journal, November 2012

Grains and grain boundaries in highly crystalline monolayer molybdenum disulphide
journal, May 2013

Making graphene visible
journal, August 2007

Strong exciton-photon coupling in microcavities containing new fluorophenethylamine based perovskite compounds
journal, January 2012

Tightly Bound Excitons in Monolayer ${WSe}_{2}$
journal, July 2014

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

Van der Waals heterostructures
journal, July 2013

Efficient inorganic–organic hybrid heterojunction solar cells containing perovskite compound and polymeric hole conductors
journal, May 2013

Electronics and optoelectronics of two-dimensional transition metal dichalcogenides
journal, November 2012

Photoconductivity and electroluminescence in lead iodide based natural quantum well structures
journal, November 1992

Dielectric confinement effect on excitons in ${PbI}_{4}$ -based layered semiconductors
journal, March 1992

Exciton band structure of monolayer ${MoS}_{2}$
journal, February 2015

Emerging Device Applications for Semiconducting Two-Dimensional Transition Metal Dichalcogenides
journal, January 2014

Synthesis, Crystal Structure, and Optical and Thermal Properties of (C₄H₉NH₃)₂MI₄ (M = Ge, Sn, Pb)
journal, January 1996

Optical Identification of Single- and Few-Layer MoS2 Sheets
journal, January 2012

Efficient planar heterojunction perovskite solar cells by vapour deposition
journal, September 2013

A roadmap for graphene
journal, October 2012

Absorption spectroscopy on ${Ga}_{0.47}$ ${In}_{0.53}$ As/ ${Al}_{0.48 L}$ ${In}_{0.52}$ As multi-quantum-well heterostructures. I. Excitonic transitions
journal, September 1987

The rise of graphene
journal, March 2007

Image charge effect on two-dimensional excitons in an inorganic-organic quantum-well crystal
journal, January 2005

Electron−Hole Interaction in Carbon Nanotubes: Novel Screening and Exciton Excitation Spectra
journal, April 2009

Optical properties due to electronic transitions in two-dimensional semiconductors ( $C_{n}$ $H_{2 n + 1}$ ${NH}_{3}$ $)_{2}$ ${PbI}_{4}$
journal, December 1990

Understanding Quantum Confinement of Charge Carriers in Layered 2D Hybrid Perovskites
journal, September 2014

Exfoliation of self-assembled 2D organic-inorganic perovskite semiconductors
journal, April 2014

Magnetoabsorption of the lowest exciton in perovskite-type compound (CH3NH3)PbI3
journal, July 1994

Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer ${WS}_{2}$
journal, August 2014

Theory of neutral and charged excitons in monolayer transition metal dichalcogenides
journal, July 2013

Quasiparticle band structures and optical properties of strained monolayer MoS $_{2}$ and WS $_{2}$
journal, April 2013

Quasiparticle band structure calculation of monolayer, bilayer, and bulk MoS $_{2}$
journal, May 2012

Fine Structure Constant Defines Visual Transparency of Graphene
journal, June 2008

Semiconductor Optics
book, January 2012

The rise of graphene
book, August 2009

Semiconductor Optics
book, January 2005

Theory of Neutral and Charged Excitons in Monolayer Transition Metal Dichalcogenides
text, January 2013

Emerging Device Applications for Semiconducting Two-Dimensional Transition Metal Dichalcogenides
text, January 2014

Probing Excitonic Dark States in Single-layer Tungsten Disulfide
text, January 2014

Halide Perovskites: Poor Man's High-Performance Semiconductors
journal, May 2016

Efficient Visible Quasi-2D Perovskite Light-Emitting Diodes
journal, June 2016

Two-Dimensional Materials for Halide Perovskite-Based Optoelectronic Devices
journal, March 2017

van der Waals Metal-Organic Framework as an Excitonic Material for Advanced Photonics
journal, January 2017

Excitonic Properties of Chemically Synthesized 2D Organic-Inorganic Hybrid Perovskite Nanosheets
journal, March 2018

Improving the Stability of Metal Halide Perovskite Materials and Light-Emitting Diodes
journal, January 2018

Two-Dimensional Organic-Inorganic Hybrid Perovskites: A New Platform for Optoelectronic Applications
journal, September 2018

Merits and Challenges of Ruddlesden-Popper Soft Halide Perovskites in Electro-Optics and Optoelectronics
journal, October 2018

Compositional Control in 2D Perovskites with Alternating Cations in the Interlayer Space for Photovoltaics with Efficiency over 18%
journal, September 2019

2D Perovskites with Giant Excitonic Optical Nonlinearities for High‐Performance Sub‐Bandgap Photodetection
journal, October 2019

Catalyst‐Free and Morphology‐Controlled Growth of 2D Perovskite Nanowires for Polarized Light Detection
journal, May 2019

Hybrid Perovskites: Effective Crystal Growth for Optoelectronic Applications
journal, May 2017

Understanding Film Formation Morphology and Orientation in High Member 2D Ruddlesden-Popper Perovskites for High-Efficiency Solar Cells
journal, September 2017

Ultrathin Two-Dimensional Organic-Inorganic Hybrid Perovskite Nanosheets with Bright, Tunable Photoluminescence and High Stability
journal, March 2017

Ultrafast Carrier Transfer Promoted by Interlayer Coulomb Coupling in 2D/3D Perovskite Heterostructures
journal, September 2018

Intrinsic Carrier Transport of Phase-Pure Homologous 2D Organolead Halide Hybrid Perovskite Single Crystals
journal, November 2018

Two-Dimensional Metal Halide Perovskites: Theory, Synthesis, and Optoelectronics
journal, January 2017

Synthesis and Photoluminescence Properties of 2D Phenethylammonium Lead Bromide Perovskite Nanocrystals
journal, September 2017

Recent advances in controlling the crystallization of two-dimensional perovskites for optoelectronic device
journal, May 2019