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Title: Advances and Promises of Layered Halide Hybrid Perovskite Semiconductors

Abstract

Layered halide hybrid organic–inorganic perovskites (HOP) have been the subject of intense investigation before the rise of three-dimensional (3D) HOP and their impressive performance in solar cells. Recently, layered HOP have also been proposed as attractive alternatives for photostable solar cells and revisited for light-emitting devices. Here, we combine classical solid-state physics concepts with simulation tools based on density functional theory to overview the main features of the optoelectronic properties of layered HOP. A detailed comparison between layered and 3D HOP is performed to highlight differences and similarities. In the same way as the cubic phase was established for 3D HOP, here we introduce the tetragonal phase with D4h symmetry as the reference phase for 2D monolayered HOP. It allows for detailed analysis of the spin–orbit coupling effects and structural transitions with corresponding electronic band folding. We further investigate the effects of octahedral tilting on the band gap, loss of inversion symmetry and possible Rashba effect, quantum confinement, and dielectric confinement related to the organic barrier, up to excitonic properties. Altogether, this paper aims to provide an interpretive and predictive framework for 3D and 2D layered HOP optoelectronic properties.

Authors:
 [1];  [2];  [2];  [3];  [4];  [4];  [5];  [5];  [5];  [5]; ORCiD logo [5]; ORCiD logo [5];  [2];  [1];  [2]
  1. National Inst. of Applied Sciences of Rennes (INSA), CNRS/UMR 6082, Rennes (France). Optical Functions for Information Technologies (FOTON)
  2. Univ. of Rennes, CNRS/UMR 6226, Rennes (France). Inst. of Chemical Sciences of Rennes (ICRH)
  3. The Barcelona Institute of Science and Technology (BIST), CSIC, Barcelona (Spain). Catalan Inst. of Nanoscience and Nanotechnology (ICN2)
  4. Univ. of Groningen (Netherlands). Zernike Inst. for Advanced Materials
  5. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; USDOE Laboratory Directed Research and Development (LDRD) Program; National Research Agency (ANR) (France); BPO Foundation (France); European Research Council (ERC); Netherlands Organization for Scientific Research (NWO); Ministry of Economy and Enterprise (MINECO) (Spain); European Union (EU)
OSTI Identifier:
1459816
Report Number(s):
LA-UR-16-26260
Journal ID: ISSN 1936-0851
Grant/Contract Number:  
AC52-06NA25396; 2016-c2012096724; PEROPHOT 2015; 306983; SEV-2013-0295; 687008
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 10; Journal Issue: 11; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; Bethe−Salpeter equation; density functional theory; dielectric confinement; exciton; halide perovskites; k·p; layered materials; quantum confinement; Rashba

Citation Formats

Pedesseau, Laurent, Sapori, Daniel, Traore, Boubacar, Robles, Roberto, Fang, Hong-Hua, Loi, Maria Antonietta, Tsai, Hsinhan, Nie, Wanyi, Blancon, Jean-Christophe, Neukirch, Amanda, Tretiak, Sergei, Mohite, Aditya D., Katan, Claudine, Even, Jacky, and Kepenekian, Mikael. Advances and Promises of Layered Halide Hybrid Perovskite Semiconductors. United States: N. p., 2016. Web. doi:10.1021/acsnano.6b05944.
Pedesseau, Laurent, Sapori, Daniel, Traore, Boubacar, Robles, Roberto, Fang, Hong-Hua, Loi, Maria Antonietta, Tsai, Hsinhan, Nie, Wanyi, Blancon, Jean-Christophe, Neukirch, Amanda, Tretiak, Sergei, Mohite, Aditya D., Katan, Claudine, Even, Jacky, & Kepenekian, Mikael. Advances and Promises of Layered Halide Hybrid Perovskite Semiconductors. United States. https://doi.org/10.1021/acsnano.6b05944
Pedesseau, Laurent, Sapori, Daniel, Traore, Boubacar, Robles, Roberto, Fang, Hong-Hua, Loi, Maria Antonietta, Tsai, Hsinhan, Nie, Wanyi, Blancon, Jean-Christophe, Neukirch, Amanda, Tretiak, Sergei, Mohite, Aditya D., Katan, Claudine, Even, Jacky, and Kepenekian, Mikael. Wed . "Advances and Promises of Layered Halide Hybrid Perovskite Semiconductors". United States. https://doi.org/10.1021/acsnano.6b05944. https://www.osti.gov/servlets/purl/1459816.
@article{osti_1459816,
title = {Advances and Promises of Layered Halide Hybrid Perovskite Semiconductors},
author = {Pedesseau, Laurent and Sapori, Daniel and Traore, Boubacar and Robles, Roberto and Fang, Hong-Hua and Loi, Maria Antonietta and Tsai, Hsinhan and Nie, Wanyi and Blancon, Jean-Christophe and Neukirch, Amanda and Tretiak, Sergei and Mohite, Aditya D. and Katan, Claudine and Even, Jacky and Kepenekian, Mikael},
abstractNote = {Layered halide hybrid organic–inorganic perovskites (HOP) have been the subject of intense investigation before the rise of three-dimensional (3D) HOP and their impressive performance in solar cells. Recently, layered HOP have also been proposed as attractive alternatives for photostable solar cells and revisited for light-emitting devices. Here, we combine classical solid-state physics concepts with simulation tools based on density functional theory to overview the main features of the optoelectronic properties of layered HOP. A detailed comparison between layered and 3D HOP is performed to highlight differences and similarities. In the same way as the cubic phase was established for 3D HOP, here we introduce the tetragonal phase with D4h symmetry as the reference phase for 2D monolayered HOP. It allows for detailed analysis of the spin–orbit coupling effects and structural transitions with corresponding electronic band folding. We further investigate the effects of octahedral tilting on the band gap, loss of inversion symmetry and possible Rashba effect, quantum confinement, and dielectric confinement related to the organic barrier, up to excitonic properties. Altogether, this paper aims to provide an interpretive and predictive framework for 3D and 2D layered HOP optoelectronic properties.},
doi = {10.1021/acsnano.6b05944},
journal = {ACS Nano},
number = 11,
volume = 10,
place = {United States},
year = {2016},
month = {10}
}

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Edge stabilization in reduced-dimensional perovskites
journal, January 2020


Band‐Edge Exciton Fine Structure and Exciton Recombination Dynamics in Single Crystals of Layered Hybrid Perovskites
journal, December 2019

  • Fang, Hong‐Hua; Yang, Jie; Adjokatse, Sampson
  • Advanced Functional Materials, Vol. 30, Issue 6
  • DOI: 10.1002/adfm.201907979

(C 3 H 9 NI) 4 AgBiI 8 : a direct-bandgap layered double perovskite based on a short-chain spacer cation for light absorption
journal, January 2020

  • Yao, Yunpeng; Kou, Bo; Peng, Yu
  • Chemical Communications, Vol. 56, Issue 21
  • DOI: 10.1039/c9cc07796k

Excited-state vibrational dynamics toward the polaron in methylammonium lead iodide perovskite
journal, June 2018

  • Park, Myeongkee; Neukirch, Amanda J.; Reyes-Lillo, Sebastian E.
  • Nature Communications, Vol. 9, Issue 1
  • DOI: 10.1038/s41467-018-04946-7

Aqueous acid-based synthesis of lead-free tin halide perovskites with near-unity photoluminescence quantum efficiency
journal, January 2019

  • Wang, Aifei; Guo, Yanyan; Zhou, Zhaobo
  • Chemical Science, Vol. 10, Issue 17
  • DOI: 10.1039/c9sc00453j

Recombination at high carrier density in methylammonium lead iodide studied using time-resolved microwave conductivity
journal, August 2017

  • Labram, John G.; Chabinyc, Michael L.
  • Journal of Applied Physics, Vol. 122, Issue 6
  • DOI: 10.1063/1.4990802

Searching for stability at lower dimensions: current trends and future prospects of layered perovskite solar cells
journal, January 2019

  • Thrithamarassery Gangadharan, Deepak; Ma, Dongling
  • Energy & Environmental Science, Vol. 12, Issue 10
  • DOI: 10.1039/c9ee01591d

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

  • Cortecchia, D.; Neutzner, S.; Yin, J.
  • APL Materials, Vol. 6, Issue 11
  • DOI: 10.1063/1.5045782

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

  • Tremblay, Marie-Hélène; Bacsa, John; Barlow, Stephen
  • Materials Chemistry Frontiers
  • DOI: 10.1039/d0qm00118j

Two-dimensional halide perovskite nanomaterials and heterostructures
journal, January 2018

  • Shi, Enzheng; Gao, Yao; Finkenauer, Blake P.
  • Chemical Society Reviews, Vol. 47, Issue 16
  • DOI: 10.1039/c7cs00886d

Progress in Theoretical Study of Metal Halide Perovskite Solar Cell Materials
journal, August 2017


Scaling law for excitons in 2D perovskite quantum wells
journal, June 2018


Tuning the optical bandgap in layered hybrid perovskites through variation of alkyl chain length
journal, April 2019

  • Sichert, Jasmina A.; Hemmerling, Annick; Cardenas-Daw, Carlos
  • APL Materials, Vol. 7, Issue 4
  • DOI: 10.1063/1.5087296

Extremely reduced dielectric confinement in two-dimensional hybrid perovskites with large polar organics
journal, November 2018


Tailoring Organic Cation of 2D Air-Stable Organometal Halide Perovskites for Highly Efficient Planar Solar Cells
journal, May 2017


Dimensionality engineering of hybrid halide perovskite light absorbers
journal, November 2018

  • Gao, Peng; Bin Mohd Yusoff, Abd Rashid; Nazeeruddin, Mohammad Khaja
  • Nature Communications, Vol. 9, Issue 1
  • DOI: 10.1038/s41467-018-07382-9

Recent advances toward efficient and stable tin‐based perovskite solar cells
journal, December 2019

  • Tai, Qidong; Cao, Jiupeng; Wang, Tianyue
  • EcoMat, Vol. 1, Issue 1
  • DOI: 10.1002/eom2.12004

In-Plane Ferroelectricity in Thin Flakes of Van der Waals Hybrid Perovskite
journal, October 2018


Flexible Quasi‐2D Perovskite/IGZO Phototransistors for Ultrasensitive and Broadband Photodetection
journal, December 2019


Designing a new family of oxonium-cation based structurally diverse organic–inorganic hybrid iodoantimonate crystals
journal, January 2019

  • Parmar, Swati; Pal, Shiv; Biswas, Abhijit
  • Chemical Communications, Vol. 55, Issue 52
  • DOI: 10.1039/c9cc03485d

Enhanced Exciton and Photon Confinement in Ruddlesden-Popper Perovskite Microplatelets for Highly Stable Low-Threshold Polarized Lasing
journal, April 2018


Distinct conducting layer edge states in two-dimensional (2D) halide perovskite
journal, July 2019


Multiscale in modelling and validation for solar photovoltaics
journal, January 2018


Highly Emissive Self-Trapped Excitons in Fully Inorganic Zero-Dimensional Tin Halides
journal, July 2018

  • Benin, Bogdan M.; Dirin, Dmitry N.; Morad, Viktoriia
  • Angewandte Chemie, Vol. 130, Issue 35
  • DOI: 10.1002/ange.201806452

Structural and thermodynamic limits of layer thickness in 2D halide perovskites
journal, December 2018

  • Soe, Chan Myae Myae; Nagabhushana, G. P.; Shivaramaiah, Radha
  • Proceedings of the National Academy of Sciences, Vol. 116, Issue 1
  • DOI: 10.1073/pnas.1811006115

Fabrication of single phase 2D homologous perovskite microplates by mechanical exfoliation
journal, January 2018


Controllable growth of two-dimensional perovskite microstructures
journal, January 2018

  • Fang, Chen; Li, Junze; Wang, Jun
  • CrystEngComm, Vol. 20, Issue 41
  • DOI: 10.1039/c8ce01087k

Growth mechanism of strongly emitting CH3NH3PbBr3 perovskite nanocrystals with a tunable bandgap
journal, October 2017


An overview on enhancing the stability of lead halide perovskite quantum dots and their applications in phosphor-converted LEDs
journal, January 2019

  • Wei, Yi; Cheng, Ziyong; Lin, Jun
  • Chemical Society Reviews, Vol. 48, Issue 1
  • DOI: 10.1039/c8cs00740c

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


Does Rashba splitting in CH 3 NH 3 PbBr 3 arise from 2 × 2 surface reconstruction?
journal, January 2018

  • Che, Xiaoyang; Traore, Boubacar; Katan, Claudine
  • Physical Chemistry Chemical Physics, Vol. 20, Issue 14
  • DOI: 10.1039/c8cp00745d

Preface: Two dimensional (2D) hybrid organic-inorganic perovskites
journal, November 2018

  • Li, Wei; Docampo, Pablo; Mohite, Aditya D.
  • APL Materials, Vol. 6, Issue 11
  • DOI: 10.1063/1.5079945

Free-electron effects on the optical absorption of the hybrid perovskite CH 3 NH 3 PbI 3 from first principles
journal, July 2019


Perovskite‐Based Phototransistors and Hybrid Photodetectors
journal, August 2019

  • Xie, Chao; Liu, Chun‐Ki; Loi, Hok‐Leung
  • Advanced Functional Materials, Vol. 30, Issue 20
  • DOI: 10.1002/adfm.201903907

Stable biexcitons in two-dimensional metal-halide perovskites with strong dynamic lattice disorder
journal, March 2018


Two-dimensional hybrid perovskites sustaining strong polariton interactions at room temperature
journal, May 2019


Bright magnetic dipole radiation from two-dimensional lead-halide perovskites
journal, February 2020

  • DeCrescent, Ryan A.; Venkatesan, Naveen R.; Dahlman, Clayton J.
  • Science Advances, Vol. 6, Issue 6
  • DOI: 10.1126/sciadv.aay4900

Realization of “warm” white light via halide substitution in polar two-dimensional hybrid perovskites (2meptH 2 )PbCl x Br 4−x
journal, January 2018

  • Wang, Sasa; Yao, Yunpeng; Wu, Zhenyue
  • Journal of Materials Chemistry C, Vol. 6, Issue 45
  • DOI: 10.1039/c8tc03167c

Fluorination of Organic Spacer Impacts on the Structural and Optical Response of 2D Perovskites
journal, January 2020

  • García-Benito, Inés; Quarti, Claudio; Queloz, Valentin I. E.
  • Frontiers in Chemistry, Vol. 7
  • DOI: 10.3389/fchem.2019.00946

Multilayered 2D Cesium‐Based Hybrid Perovskite with Strong Polarization Sensitivity: Dimensional Reduction of CsPbBr 3
journal, March 2020

  • Liu, Yi; Wang, Jiaqi; Han, Shiguo
  • Chemistry – A European Journal, Vol. 26, Issue 16
  • DOI: 10.1002/chem.201905531

Lead-free hybrid perovskites for photovoltaics
journal, January 2018


First-principles characterization of two-dimensional (CH 3 (CH 2 ) 3 NH 3 ) 2 (CH 3 NH 3 ) n−1 Ge n I 3n+1 perovskite
journal, January 2018

  • Wu, Liyuan; Lu, Pengfei; Li, Yuheng
  • Journal of Materials Chemistry A, Vol. 6, Issue 47
  • DOI: 10.1039/c8ta10055a

Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites
journal, March 2017


Unravelling Light-Induced Degradation of Layered Perovskite Crystals and Design of Efficient Encapsulation for Improved Photostability
journal, April 2018

  • Fang, Hong-Hua; Yang, Jie; Tao, Shuxia
  • Advanced Functional Materials, Vol. 28, Issue 21
  • DOI: 10.1002/adfm.201800305

Spintronics of Hybrid Organic–Inorganic Perovskites: Miraculous Basis of Integrated Optoelectronic Devices
journal, June 2019

  • Liao, Kun; Hu, Xiaoyong; Cheng, Yinke
  • Advanced Optical Materials, Vol. 7, Issue 15
  • DOI: 10.1002/adom.201900350

Design principles for electronic charge transport in solution-processed vertically stacked 2D perovskite quantum wells
journal, May 2018


Surface Termination, Morphology, and Bright Photoluminescence of Cesium Lead Halide Perovskite Nanocrystals
journal, November 2016


Unveiling the operation mechanism of layered perovskite solar cells
text, January 2019

  • M. M., Nahid,; S. J., Stuard,; J., Huang,
  • The University of North Carolina at Chapel Hill University Libraries
  • DOI: 10.17615/dstf-da41

Highly Emissive Self-Trapped Excitons in Fully Inorganic Zero-Dimensional Tin Halides
journal, July 2018

  • Benin, Bogdan M.; Dirin, Dmitry N.; Morad, Viktoriia
  • Angewandte Chemie International Edition, Vol. 57, Issue 35
  • DOI: 10.1002/anie.201806452

Stable Light-Emitting Diodes Using Phase-Pure Ruddlesden-Popper Layered Perovskites
conference, February 2018

  • Tsai, Hsinhan; Mohite, Aditya; Blancon, Jean-Christophe
  • Proceedings of the 3rd International Conference on Perovskite Thin Film Photovoltaics, Photonics and Optoelectronics
  • DOI: 10.29363/nanoge.abxpvperopto.2018.053