Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors CsPbBr3 and CsPbCl3

Sebastian, M.; Peters, J. A.; Stoumpos, C. C.; Im, J.; Kostina, S. S.; Liu, Z.; Kanatzidis, M. G.; Freeman, A. J.; Wessels, B. W.

doi:10.1103/PhysRevB.92.235210

Title: Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors $CsPbB r_{3}$ and $CsPbC l_{3}$

Abstract

The ternary compounds CsPbX₃ (X = Br or Cl) have perovskite structures that are being considered for optical and electronic applications such as lasing and gamma-ray detection. An above-band-gap excitonic photoluminescence (PL) band is seen in both CsPbX₃ compounds. An excitonic emission peak centered at 2.98 eV, ~0.1 eV above the room-temperature band gap, is observed for CsPbCl₃. The thermal quenching of the excitonic luminescence is well described by a two-step quenching model, yielding activation energies of 0.057 and 0.0076 eV for high- and low-temperature regimes, respectively. CsPbBr₃ exhibits bound excitonic luminescence peaks located at 2.29 and 2.33 eV that are attributed to recombination involving Br vacancy centers. Activation energies for thermal quenching of the excitonic luminescence of 0.017 and 0.0007 eV were calculated for CsPbBr₃. Temperature-dependent PL experiments reveal unexpected blueshifts for all excitonic emission peaks in CsPbX₃ compounds. A phonon-assisted step-up process leads to the blueshift in CsPbBr₃ emission, while there is a contribution from band-gap widening in CsPbCl₃. Finally, the absence of significant deep level defect luminescence in these compounds makes them attractive candidates for high-resolution, room-temperature radiation detection.

Authors:

Sebastian, M. ^[1]; Peters, J. A. ^[1]; Stoumpos, C. C. ^[2]; Im, J. ^[3]; Kostina, S. S. ^[1]; Liu, Z. ^[1]; Kanatzidis, M. G. ^[2]; Freeman, A. J. ^[3]; Wessels, B. W. ^[1]

Northwestern Univ., Evanston, IL (United States). Dept. of Material Science and Engineering
Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
Northwestern Univ., Evanston, IL (United States). Dept. of Physics and Astronomy

Publication Date:: Tue Dec 29 00:00:00 EST 2015

Research Org.:: Northwestern Univ., Evanston, IL (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1494838

Alternate Identifier(s):: OSTI ID: 1234041

Grant/Contract Number:: NA0002522; AC02-06CH11357

Resource Type:: Accepted Manuscript

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

Additional Journal Information:: Journal Volume: 92; Journal Issue: 23; Journal ID: ISSN 1098-0121

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; photoluminescence (PL); exciton emission; gamma-ray detection; perovskite halides; CsPbBr3; CsPbCl3

Citation Formats


                    Sebastian, M., Peters, J. A., Stoumpos, C. C., Im, J., Kostina, S. S., Liu, Z., Kanatzidis, M. G., Freeman, A. J., and Wessels, B. W. Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors CsPbBr3 and CsPbCl3.  United States: N. p., 2015. 
Web.  doi:10.1103/PhysRevB.92.235210.

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                    Sebastian, M., Peters, J. A., Stoumpos, C. C., Im, J., Kostina, S. S., Liu, Z., Kanatzidis, M. G., Freeman, A. J., & Wessels, B. W. Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors CsPbBr3 and CsPbCl3.  United States.  https://doi.org/10.1103/PhysRevB.92.235210

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                    Sebastian, M., Peters, J. A., Stoumpos, C. C., Im, J., Kostina, S. S., Liu, Z., Kanatzidis, M. G., Freeman, A. J., and Wessels, B. W. Tue .  
"Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors CsPbBr3 and CsPbCl3".  United States.  https://doi.org/10.1103/PhysRevB.92.235210.  https://www.osti.gov/servlets/purl/1494838.

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@article{osti_1494838,

  title        = {Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors CsPbBr3 and CsPbCl3},

  author       = {Sebastian, M. and Peters, J. A. and Stoumpos, C. C. and Im, J. and Kostina, S. S. and Liu, Z. and Kanatzidis, M. G. and Freeman, A. J. and Wessels, B. W.},

  abstractNote = {The ternary compounds CsPbX3 (X = Br or Cl) have perovskite structures that are being considered for optical and electronic applications such as lasing and gamma-ray detection. An above-band-gap excitonic photoluminescence (PL) band is seen in both CsPbX3 compounds. An excitonic emission peak centered at 2.98 eV, ~0.1 eV above the room-temperature band gap, is observed for CsPbCl3. The thermal quenching of the excitonic luminescence is well described by a two-step quenching model, yielding activation energies of 0.057 and 0.0076 eV for high- and low-temperature regimes, respectively. CsPbBr3 exhibits bound excitonic luminescence peaks located at 2.29 and 2.33 eV that are attributed to recombination involving Br vacancy centers. Activation energies for thermal quenching of the excitonic luminescence of 0.017 and 0.0007 eV were calculated for CsPbBr3. Temperature-dependent PL experiments reveal unexpected blueshifts for all excitonic emission peaks in CsPbX3 compounds. A phonon-assisted step-up process leads to the blueshift in CsPbBr3 emission, while there is a contribution from band-gap widening in CsPbCl3. Finally, the absence of significant deep level defect luminescence in these compounds makes them attractive candidates for high-resolution, room-temperature radiation detection.},

  doi          = {10.1103/PhysRevB.92.235210},

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

  number       = 23,

  volume       = 92,

  place        = {United States},

  year         = {Tue Dec 29 00:00:00 EST 2015},

  month        = {Tue Dec 29 00:00:00 EST 2015}

}

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Figures / Tables:

Table 1: Crystal data and structure refinement for CsPbCl₃ at 293(2) K. 364

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Zhao, Wei; Qin, Zhengyuan; Zhang, Chunfeng
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Makarov, Sergey; Furasova, Aleksandra; Tiguntseva, Ekaterina
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Materials Discovery of Stable and Nontoxic Halide Perovskite Materials for High-Efficiency Solar Cells
text, January 2019

Jacobs, Ryan; Luo, Guangfu; Morgan, Dane
arXiv
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Title: Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors CsPbB r 3 and CsPbC l 3

Abstract

Citation Formats

Figures / Tables:

Generalized Gradient Approximation Made Simple journal, October 1996

The Renaissance of Halide Perovskites and Their Evolution as Emerging Semiconductors journal, September 2015

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Excitation intensity and temperature-dependent photoluminescence and optical absorption in Tl4Ga3InSe8 layered crystals journal, August 2006

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

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High intensity photoluminescence of microcrystalline CsPbBr3 films: Evidence for enhanced stimulated emission at room temperature journal, January 2007

Bound excitons and resonant Raman scattering in Cd x Zn 1 − x Te ( 0.9 ≤ x ≤ 1 ) journal, December 1983

Luminescence Spectroscopy of Semiconductors book, February 2012

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Crystal Growth of the Perovskite Semiconductor CsPbBr 3 : A New Material for High-Energy Radiation Detection journal, June 2013

Assessment of correction methods for the band-gap problem and for finite-size effects in supercell defect calculations: Case studies for ZnO and GaAs journal, December 2008

Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)] journal, June 2006

Does the low-temperature Arrhenius plot of the photoluminescence intensity in CdTe point towards an erroneous activation energy? journal, February 1997

Ab initiomolecular dynamics for liquid metals journal, January 1993

Lead bromide and ternary alkali lead bromide single crystals — growth and emission properties journal, August 1996

Polarization Phenomena in TlBr Detectors journal, August 2009

Crystal Structure and Photoconductivity of Cæsium Plumbohalides journal, November 1958

Photoluminescence and stimulated emission from microcrystalline Cs Pb Cl 3 films prepared by amorphous-to-crystalline transformation journal, November 2004

Identification of the symmetry of phonon modes in CsPbCl3 in phase IV by Raman and resonance-Raman scattering journal, December 1997

Luminescence of CsPbBr3-like quantum dots in CsBr single crystals journal, October 1999

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

Phase transitions in ABX3 type halides journal, March 1971

Low-energy excitation in CsPbX3 (X=Cl, Br) journal, December 2002

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New Evidence for Defect Creation by High Optical Excitation in Glow Discharge Amorphous Silicon journal, July 1980

Phase Transitions in CsPbCl 3 journal, December 1971

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Shallow halogen vacancies in halide optoelectronic materials journal, November 2014

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

Structure validation in chemical crystallography journal, January 2009

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Ionic conductivity of CsPbCl3 and CsPbBr3 journal, January 1987

A short history of SHELX journal, December 2007

Temperature dependence of the photoinduced fatigue-recovery phenomena of photoluminescence under prolonged irradiation in GeS2 chalcogenide glass journal, March 2008

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Temperature dependence of band gaps in Si and Ge journal, February 1985

First principle study of the structural and optoelectronic properties of cubic perovskites CsPbM3 (M=Cl, Br, I) journal, September 2011

Ionic conduction of the perovskite-type halides journal, November 1983

Time-dependent photoluminescence fatigue-recovery phenomena in germanium sulfide glasses journal, June 2013

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

Heavy metal ternary halides for room-temperature x-ray and gamma-ray detection conference, September 2013

Further Contribution to the Theory of the Line-Shape of the Exciton Absorption Band journal, January 1962

Reinterpretation of degradation kinetics of amorphous silicon journal, March 1989

First-principles calculations for point defects in solids journal, March 2014

Photoluminescence Associated with Multivalley Resonant Impurity States above the Fundamental Band Edge: N Isoelectronic Traps in Ga As 1 − x P x journal, July 1971

A neutron diffraction study of anharmonic thermal vibrations in cubic CsPb X 3 journal, January 1980

Excitation-power dependence of the near-band-edge photoluminescence of semiconductors journal, April 1992

Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites journal, October 2012

Photoluminescence from the nitrogen-perturbed above-bandgap states in dilute GaAs1−xNx alloys: A microphotoluminescence study journal, May 2006

Intrinsic point defects in aluminum antimonide journal, April 2008

Temperature-dependent excitonic photoluminescence of hybrid organometal halide perovskite films journal, January 2014

Neutron Diffraction Study of the Structure of Cubic CsPbBr 3 journal, July 1979

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

Excitation Intensity and Temperature-Dependent Photoluminescence and Optical Absorption in Tl4Ga3InSe8 Layered Crystals. journal, October 2006

Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect journal, February 2020

Polarization phenomena in TlBr detectors conference, October 2008

Intrinsic point defects in aluminum antimonide text, January 2010

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Title: Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors $CsPbB r_{3}$ and $CsPbC l_{3}$

Generalized Gradient Approximation Made Simple
journal, October 1996

The Renaissance of Halide Perovskites and Their Evolution as Emerging Semiconductors
journal, September 2015

Projector augmented-wave method
journal, December 1994

Hybrid functionals based on a screened Coulomb potential
journal, May 2003

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journal, November 2000

WinGX and ORTEP for Windows : an update
journal, July 2012

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journal, May 2012

Luminescence of CsPbCl3 Nanocrystals Dispersed in a CsCl Crystal under High-Energy Excitation
journal, May 2001

Evidence for the direct population of solid-state bands by non-bonding electron pairs in compounds of the type CsM II X3(M II = Ge, Sn, Pb; X = Cl, Br, I)
journal, January 1995

Excitation intensity and temperature-dependent photoluminescence and optical absorption in Tl4Ga3InSe8 layered crystals
journal, August 2006

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

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journal, January 1979

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journal, September 1971

Linear Network Model of Gene Regulation for the Yeast Cell Cycle
journal, March 2004

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journal, July 2014

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journal, December 1979

Structural Phase Transitions in CsPbBr ₃
journal, November 1974

Radiative recombination via intrinsic defects in CuxGaySe2
journal, April 2001

Excitons in CsPbX3 (X=Cl, Br, I) ternary nanocrystallites in thin film matrices
journal, December 2001

Mesoscopic CH₃NH₃PbI₃/TiO₂ Heterojunction Solar Cells
journal, October 2012

High intensity photoluminescence of microcrystalline CsPbBr3 films: Evidence for enhanced stimulated emission at room temperature
journal, January 2007

Bound excitons and resonant Raman scattering in ${Cd}_{x} {Zn}_{1 - x} Te (0.9 \leq x \leq 1)$
journal, December 1983

Luminescence Spectroscopy of Semiconductors
book, February 2012

Temperature and Excitation Power Dependences of the Photoluminescencein CdMnTe Crystals
journal, May 2011

Crystal Growth of the Perovskite Semiconductor CsPbBr ₃ : A New Material for High-Energy Radiation Detection
journal, June 2013

Assessment of correction methods for the band-gap problem and for finite-size effects in supercell defect calculations: Case studies for ZnO and GaAs
journal, December 2008

Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)]
journal, June 2006

Does the low-temperature Arrhenius plot of the photoluminescence intensity in CdTe point towards an erroneous activation energy?
journal, February 1997

Ab initiomolecular dynamics for liquid metals
journal, January 1993

Lead bromide and ternary alkali lead bromide single crystals — growth and emission properties
journal, August 1996

Polarization Phenomena in TlBr Detectors
journal, August 2009

Crystal Structure and Photoconductivity of Cæsium Plumbohalides
journal, November 1958

Photoluminescence and stimulated emission from microcrystalline $Cs Pb {Cl}_{3}$ films prepared by amorphous-to-crystalline transformation
journal, November 2004

Identification of the symmetry of phonon modes in CsPbCl3 in phase IV by Raman and resonance-Raman scattering
journal, December 1997

Luminescence of CsPbBr3-like quantum dots in CsBr single crystals
journal, October 1999

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

Phase transitions in ABX3 type halides
journal, March 1971

Low-energy excitation in CsPbX3 (X=Cl, Br)
journal, December 2002

Partial recovery of the fatigued photoluminescence in germanium sulfide glass
journal, June 2003

New Evidence for Defect Creation by High Optical Excitation in Glow Discharge Amorphous Silicon
journal, July 1980

Phase Transitions in CsPbCl ₃
journal, December 1971

Crystal Growth of Tl ₄ CdI ₆ : A Wide Band Gap Semiconductor for Hard Radiation Detection
journal, March 2014

Optical properties of Zn-terminated ZnO bulk
journal, February 2004

Shallow halogen vacancies in halide optoelectronic materials
journal, November 2014

Thermal Dissociation of Excitons Bounds to Neutral Acceptors in High-Purity GaAs
journal, November 1971

Strongly Enhanced Free-Exciton Luminescence in Microcrystalline CsPbBr ₃ Films
journal, July 2003

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

Structure validation in chemical crystallography
journal, January 2009

Free-to-bound recombination in near stoichiometric Cu $_{2}$ ZnSnS $_{4}$ single crystals
journal, July 2012

Ionic conductivity of CsPbCl3 and CsPbBr3
journal, January 1987

A short history of SHELX
journal, December 2007

Temperature dependence of the photoinduced fatigue-recovery phenomena of photoluminescence under prolonged irradiation in GeS2 chalcogenide glass
journal, March 2008

Unusual defect physics in CH ₃ NH ₃ PbI ₃ perovskite solar cell absorber
journal, February 2014

Temperature dependence of band gaps in Si and Ge
journal, February 1985

First principle study of the structural and optoelectronic properties of cubic perovskites CsPbM3 (M=Cl, Br, I)
journal, September 2011

Ionic conduction of the perovskite-type halides
journal, November 1983

Time-dependent photoluminescence fatigue-recovery phenomena in germanium sulfide glasses
journal, June 2013

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Heavy metal ternary halides for room-temperature x-ray and gamma-ray detection
conference, September 2013

Further Contribution to the Theory of the Line-Shape of the Exciton Absorption Band
journal, January 1962

Reinterpretation of degradation kinetics of amorphous silicon
journal, March 1989

First-principles calculations for point defects in solids
journal, March 2014

Photoluminescence Associated with Multivalley Resonant Impurity States above the Fundamental Band Edge: N Isoelectronic Traps in $Ga {As}_{1 - x} P_{x}$
journal, July 1971

A neutron diffraction study of anharmonic thermal vibrations in cubic CsPb X ₃
journal, January 1980

Excitation-power dependence of the near-band-edge photoluminescence of semiconductors
journal, April 1992

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journal, October 2012

Photoluminescence from the nitrogen-perturbed above-bandgap states in dilute GaAs1−xNx alloys: A microphotoluminescence study
journal, May 2006

Intrinsic point defects in aluminum antimonide
journal, April 2008

Temperature-dependent excitonic photoluminescence of hybrid organometal halide perovskite films
journal, January 2014

Neutron Diffraction Study of the Structure of Cubic CsPbBr ₃
journal, July 1979

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

Excitation Intensity and Temperature-Dependent Photoluminescence and Optical Absorption in Tl4Ga3InSe8 Layered Crystals.
journal, October 2006

Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect
journal, February 2020

Polarization phenomena in TlBr detectors
conference, October 2008

Intrinsic point defects in aluminum antimonide
text, January 2010

High-Temperature Photoluminescence of CsPbX ₃ (X = Cl, Br, I) Nanocrystals
journal, March 2017

Low-Temperature Absorption, Photoluminescence, and Lifetime of CsPbX ₃ (X = Cl, Br, I) Nanocrystals
journal, May 2018

Light Emitting Diodes Based on Inorganic Composite Halide Perovskites
journal, December 2018

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