Band Gap Tuning via Lattice Contraction and Octahedral Tilting in Perovskite Materials for Photovoltaics

Prasanna, Rohit; Gold-Parker, Aryeh; Leijtens, Tomas; Conings, Bert; Babayigit, Aslihan; Boyen, Hans -Gerd; Toney, Michael F.; McGehee, Michael D.

doi:10.1021/jacs.7b04981

Title: Band Gap Tuning via Lattice Contraction and Octahedral Tilting in Perovskite Materials for Photovoltaics

Abstract

Tin and lead iodide perovskite semiconductors of the composition AMX₃, where M is a metal and X is a halide, are leading candidates for high efficiency low cost tandem photovoltaics, in part because they have band gaps that can be tuned over a wide range by compositional substitution. We experimentally identify two competing mechanisms through which the A-site cation influences the band gap of 3D metal halide perovskites. Using a smaller A-site cation can distort the perovskite lattice in two distinct ways: by tilting the MX₆ octahedra or by simply contracting the lattice isotropically. The former effect tends to raise the band gap, while the latter tends to decrease it. Lead iodide perovskites show an increase in band gap upon partial substitution of the larger formamidinium with the smaller cesium, due to octahedral tilting. Perovskites based on tin, which is slightly smaller than lead, show the opposite trend: they show no octahedral tilting upon Cs-substitution but only a contraction of the lattice, leading to progressive reduction of the band gap. We outline a strategy to systematically tune the band gap and valence and conduction band positions of metal halide perovskites through control of the cation composition. Using this strategy, wemore »« less

Authors:

^[1]; Gold-Parker, Aryeh ^[2]; Leijtens, Tomas ^[1];

^[3]; Babayigit, Aslihan ^[3]; Boyen, Hans -Gerd ^[3];

^[4];

^[1]

Stanford Univ., Stanford, CA (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Hasselt Univ., Diepenbeek (Belgium)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

Publication Date:: Thu Jul 13 00:00:00 EDT 2017

Research Org.:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1390619

Grant/Contract Number:: AC02-76SF00515; DGE-1147470; 659225

Resource Type:: Accepted Manuscript

Journal Name:: Journal of the American Chemical Society

Additional Journal Information:: Journal Volume: 139; Journal Issue: 32; Journal ID: ISSN 0002-7863

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 14 SOLAR ENERGY

Citation Formats


                    Prasanna, Rohit, Gold-Parker, Aryeh, Leijtens, Tomas, Conings, Bert, Babayigit, Aslihan, Boyen, Hans -Gerd, Toney, Michael F., and McGehee, Michael D. Band Gap Tuning via Lattice Contraction and Octahedral Tilting in Perovskite Materials for Photovoltaics.  United States: N. p., 2017. 
Web.  doi:10.1021/jacs.7b04981.

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                    Prasanna, Rohit, Gold-Parker, Aryeh, Leijtens, Tomas, Conings, Bert, Babayigit, Aslihan, Boyen, Hans -Gerd, Toney, Michael F., & McGehee, Michael D. Band Gap Tuning via Lattice Contraction and Octahedral Tilting in Perovskite Materials for Photovoltaics.  United States.  https://doi.org/10.1021/jacs.7b04981

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                    Prasanna, Rohit, Gold-Parker, Aryeh, Leijtens, Tomas, Conings, Bert, Babayigit, Aslihan, Boyen, Hans -Gerd, Toney, Michael F., and McGehee, Michael D. Thu .  
"Band Gap Tuning via Lattice Contraction and Octahedral Tilting in Perovskite Materials for Photovoltaics".  United States.  https://doi.org/10.1021/jacs.7b04981.  https://www.osti.gov/servlets/purl/1390619.

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@article{osti_1390619,

  title        = {Band Gap Tuning via Lattice Contraction and Octahedral Tilting in Perovskite Materials for Photovoltaics},

  author       = {Prasanna, Rohit and Gold-Parker, Aryeh and Leijtens, Tomas and Conings, Bert and Babayigit, Aslihan and Boyen, Hans -Gerd and Toney, Michael F. and McGehee, Michael D.},

  abstractNote = {Tin and lead iodide perovskite semiconductors of the composition AMX3, where M is a metal and X is a halide, are leading candidates for high efficiency low cost tandem photovoltaics, in part because they have band gaps that can be tuned over a wide range by compositional substitution. We experimentally identify two competing mechanisms through which the A-site cation influences the band gap of 3D metal halide perovskites. Using a smaller A-site cation can distort the perovskite lattice in two distinct ways: by tilting the MX6 octahedra or by simply contracting the lattice isotropically. The former effect tends to raise the band gap, while the latter tends to decrease it. Lead iodide perovskites show an increase in band gap upon partial substitution of the larger formamidinium with the smaller cesium, due to octahedral tilting. Perovskites based on tin, which is slightly smaller than lead, show the opposite trend: they show no octahedral tilting upon Cs-substitution but only a contraction of the lattice, leading to progressive reduction of the band gap. We outline a strategy to systematically tune the band gap and valence and conduction band positions of metal halide perovskites through control of the cation composition. Using this strategy, we demonstrate solar cells that harvest light in the infrared up to 1040 nm, reaching a stabilized power conversion efficiency of 17.8%, showing promise for improvements of the bottom cell of all-perovskite tandem solar cells. In conclusion, the mechanisms of cation-based band gap tuning we describe are broadly applicable to 3D metal halide perovskites and will be useful in further development of perovskite semiconductors for optoelectronic applications.},

  doi          = {10.1021/jacs.7b04981},

  journal      = {Journal of the American Chemical Society},

  number       = 32,

  volume       = 139,

  place        = {United States},

  year         = {Thu Jul 13 00:00:00 EDT 2017},

  month        = {Thu Jul 13 00:00:00 EDT 2017}

}

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Title: Band Gap Tuning via Lattice Contraction and Octahedral Tilting in Perovskite Materials for Photovoltaics

Abstract

Citation Formats

High-performance photovoltaic perovskite layers fabricated through intramolecular exchange journal, May 2015

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

Perovskite-perovskite tandem photovoltaics with optimized band gaps journal, October 2016

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

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Reversible photo-induced trap formation in mixed-halide hybrid perovskites for photovoltaics journal, January 2015

Light-Induced Phase Segregation in Halide-Perovskite Absorbers journal, November 2016

Steric engineering of metal-halide perovskites with tunable optical band gaps journal, December 2014

Cation-Induced Band-Gap Tuning in Organohalide Perovskites: Interplay of Spin–Orbit Coupling and Octahedra Tilting journal, May 2014

Cesium-doped methylammonium lead iodide perovskite light absorber for hybrid solar cells journal, July 2014

A mixed-cation lead mixed-halide perovskite absorber for tandem solar cells journal, January 2016

Towards enabling stable lead halide perovskite solar cells; interplay between structural, environmental, and thermal stability journal, January 2017

Anomalous Band Gap Behavior in Mixed Sn and Pb Perovskites Enables Broadening of Absorption Spectrum in Solar Cells journal, May 2014

VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data journal, October 2011

Parametric Generalized Mixed Implicit Quasi-Variational Inclusions journal, July 2007

Resolving the Physical Origin of Octahedral Tilting in Halide Perovskites journal, June 2016

Strain Tuning of Tin–Halide and Lead–Halide Perovskites: A First-Principles Atomic and Electronic Structure Study journal, September 2015

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Reentrant Structural and Optical Properties and Large Positive Thermal Expansion in Perovskite Formamidinium Lead Iodide journal, November 2016

Tuning the Band Gap in Hybrid Tin Iodide Perovskite Semiconductors Using Structural Templating journal, June 2005

Minimal Effect of the Hole-Transport Material Ionization Potential on the Open-Circuit Voltage of Perovskite Solar Cells journal, August 2016

The classification of tilted octahedra in perovskites journal, November 1972

Structures, Phase Transitions and Tricritical Behavior of the Hybrid Perovskite Methyl Ammonium Lead Iodide journal, October 2016

Octahedral Tilting in Perovskites. I. Geometrical Considerations journal, February 1997

Efficiency limits for single-junction and tandem solar cells journal, November 2006

High Open-Circuit Voltages in Tin-Rich Low-Bandgap Perovskite-Based Planar Heterojunction Photovoltaics journal, November 2016

Improved light management in planar silicon and perovskite solar cells using PDMS scattering layer journal, December 2017

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Design of low bandgap tin–lead halide perovskite solar cells to achieve thermal, atmospheric and operational stability journal, October 2019

Small-Band-Gap Halide Double Perovskites journal, August 2018

Imaging Metal Halide Perovskites Material and Properties at the Nanoscale journal, December 2019

Constructing moisture-stable hybrid lead iodine semiconductors based on hydrogen-bond-free and dual-iodine strategies journal, January 2019

Strain engineering in perovskite solar cells and its impacts on carrier dynamics journal, February 2019

Influence of Sn/Ge Cation Exchange on Vacancy-Ordered Double Perovskite Cs 2 Sn (1− x ) Ge x I 6 : A First-Principles Theoretical Study journal, November 2018

First‐Principles Simulation of Carrier Recombination Mechanisms in Halide Perovskites journal, April 2020

Tailoring the Band Gap in 3D Hybrid Perovskites by Substitution of the Organic Cations: (CH 3 NH 3 ) 1−2 y (NH 3 (CH 2 ) 2 NH 3 ) 2 y Pb 1− y I 3 (0≤ y ≤0.25) journal, June 2018

Lead‐Free Tin‐Based Perovskite Solar Cells: Strategies Toward High Performance journal, May 2019

Pressures Tuning the Band Gap of Organic–Inorganic Trihalide Perovskites (MAPbBr3): A First-Principles Study journal, September 2018

Structure-controlled optical thermoresponse in Ruddlesden-Popper layered perovskites journal, November 2018

Exciton-band tuning induced by the width of the cation in 2D lead iodide perovskite hybrids journal, January 2020

Low‐Bandgap Mixed Tin‐Lead Perovskites and Their Applications in All‐Perovskite Tandem Solar Cells journal, February 2019

Monolithic all-perovskite tandem solar cells with 24.8% efficiency exploiting comproportionation to suppress Sn(ii) oxidation in precursor ink journal, September 2019

Sn‐Pb Binary Perovskite Films with High Crystalline Quality for High Performance Solar Cells journal, August 2019

Energy Level Tuning of PEDOT:PSS for High Performance Tin-Lead Mixed Perovskite Solar Cells journal, November 2018

Toward Perovskite Solar Cell Commercialization: A Perspective and Research Roadmap Based on Interfacial Engineering journal, June 2018

Water in hybrid perovskites: Bulk MAPbI 3 degradation via super-hydrous state journal, April 2019

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journal, May 2015

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journal, January 2016

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journal, October 2016

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journal, February 2017

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journal, March 2017

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journal, May 2017

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journal, December 2016

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journal, January 2015

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journal, March 2013

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

Self-formed grain boundary healing layer for highly efficient CH3NH3PbI3 perovskite solar cells
journal, June 2016

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

Antagonism between Spin–Orbit Coupling and Steric Effects Causes Anomalous Band Gap Evolution in the Perovskite Photovoltaic Materials CH ₃ NH ₃ Sn _{1– x} Pb _x I ₃
journal, August 2015

Stable Low-Bandgap Pb-Sn Binary Perovskites for Tandem Solar Cells
journal, August 2016

Low-bandgap mixed tin–lead iodide perovskite absorbers with long carrier lifetimes for all-perovskite tandem solar cells
journal, March 2017

Fabrication of Efficient Low-Bandgap Perovskite Solar Cells by Combining Formamidinium Tin Iodide with Methylammonium Lead Iodide
journal, September 2016

Reversible photo-induced trap formation in mixed-halide hybrid perovskites for photovoltaics
journal, January 2015

Light-Induced Phase Segregation in Halide-Perovskite Absorbers
journal, November 2016

Steric engineering of metal-halide perovskites with tunable optical band gaps
journal, December 2014

Cation-Induced Band-Gap Tuning in Organohalide Perovskites: Interplay of Spin–Orbit Coupling and Octahedra Tilting
journal, May 2014

Cesium-doped methylammonium lead iodide perovskite light absorber for hybrid solar cells
journal, July 2014

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journal, January 2016

Towards enabling stable lead halide perovskite solar cells; interplay between structural, environmental, and thermal stability
journal, January 2017

Anomalous Band Gap Behavior in Mixed Sn and Pb Perovskites Enables Broadening of Absorption Spectrum in Solar Cells
journal, May 2014

VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011

Parametric Generalized Mixed Implicit Quasi-Variational Inclusions
journal, July 2007

Resolving the Physical Origin of Octahedral Tilting in Halide Perovskites
journal, June 2016

Strain Tuning of Tin–Halide and Lead–Halide Perovskites: A First-Principles Atomic and Electronic Structure Study
journal, September 2015

Solids and Surfaces: A Chemist's View of Bonding in Extended Structures
report, July 1988

Reentrant Structural and Optical Properties and Large Positive Thermal Expansion in Perovskite Formamidinium Lead Iodide
journal, November 2016

Tuning the Band Gap in Hybrid Tin Iodide Perovskite Semiconductors Using Structural Templating
journal, June 2005

Minimal Effect of the Hole-Transport Material Ionization Potential on the Open-Circuit Voltage of Perovskite Solar Cells
journal, August 2016

The classification of tilted octahedra in perovskites
journal, November 1972

Structures, Phase Transitions and Tricritical Behavior of the Hybrid Perovskite Methyl Ammonium Lead Iodide
journal, October 2016

Octahedral Tilting in Perovskites. I. Geometrical Considerations
journal, February 1997

Efficiency limits for single-junction and tandem solar cells
journal, November 2006

High Open-Circuit Voltages in Tin-Rich Low-Bandgap Perovskite-Based Planar Heterojunction Photovoltaics
journal, November 2016

Improved light management in planar silicon and perovskite solar cells using PDMS scattering layer
journal, December 2017

Opportunities and challenges for tandem solar cells using metal halide perovskite semiconductors
journal, July 2018

Temperature-dependent studies of exciton binding energy and phase-transition suppression in (Cs,FA,MA)Pb(I,Br) ₃ perovskites
journal, March 2019

Effect of High Dipole Moment Cation on Layered 2D Organic–Inorganic Halide Perovskite Solar Cells
journal, December 2018

Interplay of Structural and Optoelectronic Properties in Formamidinium Mixed Tin-Lead Triiodide Perovskites
journal, June 2018

Long-lived hot-carrier light emission and large blue shift in formamidinium tin triiodide perovskites
journal, January 2018

Band gap engineering and transport properties of Ba ₂ In ₂ O ₅ : effect of fluorine doping and hydration
journal, January 2019

Bowing of transport gap in hybrid halide perovskite alloys (CH ₃ NH ₃ Sn ₁₋ _x Pb _x I ₃ ): Which band is responsible?
journal, January 2020

Wide-bandgap, low-bandgap, and tandem perovskite solar cells
journal, July 2019

Integrated Perovskite/Bulk‐Heterojunction Organic Solar Cells
journal, February 2019

Impact of cesium on the phase and device stability of triple cation Pb–Sn double halide perovskite films and solar cells
journal, January 2018

Thin‐film solar cells exceeding 22% solar cell efficiency: An overview on CdTe-, Cu(In,Ga)Se ₂ -, and perovskite-based materials
journal, December 2018

Highly Efficient Sn/Pb Binary Perovskite Solar Cell via Precursor Engineering: A Two-Step Fabrication Process
journal, December 2018

Lewis-Adduct Mediated Grain-Boundary Functionalization for Efficient Ideal-Bandgap Perovskite Solar Cells with Superior Stability
journal, August 2018

Vacuum‐Assisted Growth of Low‐Bandgap Thin Films (FA _0.8 MA _0.2 Sn _0.5 Pb _0.5 I ₃ ) for All‐Perovskite Tandem Solar Cells
journal, December 2019

Photophysics of lead-free tin halide perovskite films and solar cells
journal, August 2019

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journal, January 2018

Significance of hydrogen bonding and other noncovalent interactions in determining octahedral tilting in the CH3NH3PbI3 hybrid organic-inorganic halide perovskite solar cell semiconductor
journal, January 2019

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journal, November 2019

Interfacial Effects of Tin Oxide Atomic Layer Deposition in Metal Halide Perovskite Photovoltaics
journal, June 2018

From Nonluminescent to Blue‐Emitting Cs ₄ PbBr ₆ Nanocrystals: Tailoring the Insulator Bandgap of 0D Perovskite through Sn Cation Doping
journal, May 2019

Design of low bandgap tin–lead halide perovskite solar cells to achieve thermal, atmospheric and operational stability
journal, October 2019

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journal, August 2018

Imaging Metal Halide Perovskites Material and Properties at the Nanoscale
journal, December 2019

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journal, January 2019

Strain engineering in perovskite solar cells and its impacts on carrier dynamics
journal, February 2019

Influence of Sn/Ge Cation Exchange on Vacancy-Ordered Double Perovskite Cs ₂ Sn _{(1− x )} Ge _x I ₆ : A First-Principles Theoretical Study
journal, November 2018

First‐Principles Simulation of Carrier Recombination Mechanisms in Halide Perovskites
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Tailoring the Band Gap in 3D Hybrid Perovskites by Substitution of the Organic Cations: (CH 3 NH 3 ) 1−2 y (NH 3 (CH 2 ) 2 NH 3 ) 2 y Pb 1− y I 3 (0≤ y ≤0.25)
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Lead‐Free Tin‐Based Perovskite Solar Cells: Strategies Toward High Performance
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Pressures Tuning the Band Gap of Organic–Inorganic Trihalide Perovskites (MAPbBr3): A First-Principles Study
journal, September 2018

Structure-controlled optical thermoresponse in Ruddlesden-Popper layered perovskites
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