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Establishing charge-transfer excitons in 2D perovskite heterostructures

Journal Article · · Nature Communications
 [1];  [2];  [3];  [3]
  1. Beijing Jiaotong Univ. (China). Optical Information Ministry of Education. Key Lab. of Luminescence; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering; OSTI
  2. Beijing Jiaotong Univ. (China). Optical Information Ministry of Education. Key Lab. of Luminescence; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
  3. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
Charge-transfer excitons (CTEs) immensely enrich property-tuning capabilities of semiconducting materials. However, such concept has been remaining as unexplored topic within halide perovskite structures. Here, we report that CTEs can be effectively formed in heterostructured 2D perovskites prepared by mixing PEA2PbI4:PEA2SnI4, functioning as host and guest components. Remarkably, a broad emission can be demonstrated with quick formation of 3 ps but prolonged lifetime of ~0.5 μs. This broad PL presents the hypothesis of CTEs, verified by the exclusion of lattice distortion and doping effects through demonstrating double-layered PEA2PbI4/PEA2SnI4 heterostructure when shearing-away PEA2SnI4 film onto the surface of PEA2PbI4 film by using hand-finger pressing method. The below-bandgap photocurrent indicates that CTEs are vital states formed at PEA2PbI4:PEA2SnI4 interfaces in 2D perovskite heterostructures. Electroluminescence shows that CTEs can be directly formed with electrically injected carriers in perovskite LEDs. Clearly, the CTEs presents a new mechanism to advance the multifunctionalities in 2D perovskites.
Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1816873
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 11; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (59)

Electron Transfer-from Isolated Molecules to Biomolecules book January 2007
Charge Transfer Excitons in Bulk Heterojunctions of a Polyfluorene Copolymer and a Fullerene Derivative journal July 2007
Employing ∼100% Excitons in OLEDs by Utilizing a Fluorescent Molecule with Hybridized Local and Charge-Transfer Excited State journal October 2013
Novel Direct Nanopatterning Approach to Fabricate Periodically Nanostructured Perovskite for Optoelectronic Applications journal January 2017
Design Rules for Donors in Bulk-Heterojunction Solar Cells—Towards 10 % Energy-Conversion Efficiency journal March 2006
Polymer-Fullerene Bulk-Heterojunction Solar Cells journal April 2009
Structure-Tuned Lead Halide Perovskite Nanocrystals journal November 2015
Self-Calibrating Mechanochromic Fluorescent Polymers Based on Encapsulated Excimer-Forming Dyes journal January 2018
Broadband Extrinsic Self‐Trapped Exciton Emission in Sn‐Doped 2D Lead‐Halide Perovskites journal December 2018
Revealing the Cooperative Relationship between Spin, Energy, and Polarization Parameters toward Developing High‐Efficiency Exciplex Light‐Emitting Diodes journal September 2019
Excimer Emission in Self‐Assembled Organic Spherical Microstructures: An Effective Approach to Wavelength Switchable Microlasers journal April 2016
Long-Lived Charge-Transfer States in Compact Donor-Acceptor Dyads journal November 2005
Intramolecular exciplex formation in naphthylalkylamines journal June 1971
Reinterpretation of the anomalous fluorescense of p-n,n-dimethylamino-benzonitrile journal April 1973
Enabling Self-passivation by Attaching Small Grains on Surfaces of Large Grains toward High-Performance Perovskite LEDs journal September 2019
Reversible, Full-Color Luminescence by Post-treatment of Perovskite Nanocrystals journal October 2018
Bandgap and exciton binding energies in lead-iodide-based natural quantum-well crystals journal March 2004
Small Cyclic Diammonium Cation Templated (110)-Oriented 2D Halide (X = I, Br, Cl) Perovskites with White-Light Emission journal April 2019
Tuning the Luminescence of Layered Halide Perovskites journal January 2019
Overcoming Short-Circuit in Lead-Free CH 3 NH 3 SnI 3 Perovskite Solar Cells via Kinetically Controlled Gas–Solid Reaction Film Fabrication Process journal February 2016
Mechanism for Broadband White-Light Emission from Two-Dimensional (110) Hybrid Perovskites journal May 2016
Ultrafast Exciton Dissociation and Long-Lived Charge Separation in a Photovoltaic Pentacene–MoS 2 van der Waals Heterojunction journal December 2016
Study of Perovskite QD Down-Converted LEDs and Six-Color White LEDs for Future Displays with Excellent Color Performance journal July 2016
Donor/Acceptor Charge-Transfer States at Two-Dimensional Metal Halide Perovskite and Organic Semiconductor Interfaces journal October 2018
Charge-Transfer Excitons at Organic Semiconductor Surfaces and Interfaces journal November 2009
Strategies for Increasing the Efficiency of Heterojunction Organic Solar Cells: Material Selection and Device Architecture journal November 2009
Molecular Understanding of Organic Solar Cells: The Challenges journal November 2009
Structural Changes Accompanying Intramolecular Electron Transfer:  Focus on Twisted Intramolecular Charge-Transfer States and Structures journal October 2003
Tuning the Light Emission Properties by Band Gap Engineering in Hybrid Lead Halide Perovskite
  • D’Innocenzo, Valerio; Srimath Kandada, Ajay Ram; De Bastiani, Michele
  • Journal of the American Chemical Society, Vol. 136, Issue 51 https://doi.org/10.1021/ja511198f
journal December 2014
Broadband Tunable Microlasers Based on Controlled Intramolecular Charge-Transfer Process in Organic Supramolecular Microcrystals journal January 2016
Magneto-Optical Investigations on the Formation and Dissociation of Intermolecular Charge-Transfer Complexes at Donor−Acceptor Interfaces in Bulk-Heterojunction Organic Solar Cells journal May 2010
Efficient and Ultrafast Formation of Long-Lived Charge-Transfer Exciton State in Atomically Thin Cadmium Selenide/Cadmium Telluride Type-II Heteronanosheets journal January 2015
Scalable fabrication of perovskite solar cells journal March 2018
Compositional engineering of perovskite materials for high-performance solar cells journal January 2015
Hot charge-transfer excitons set the time limit for charge separation at donor/acceptor interfaces in organic photovoltaics journal December 2012
Nanoscale transport of charge-transfer states in organic donor–acceptor blends journal September 2015
Ultrafast charge transfer in atomically thin MoS2/WS2 heterostructures journal August 2014
Perovskite energy funnels for efficient light-emitting diodes journal June 2016
Organic light-emitting diodes employing efficient reverse intersystem crossing for triplet-to-singlet state conversion journal March 2012
The emergence of perovskite solar cells journal July 2014
Efficient green light-emitting diodes based on quasi-two-dimensional composition and phase engineered perovskite with surface passivation journal February 2018
Tailoring exciton and excimer emission in an exfoliated ultrathin 2D metal-organic framework journal June 2018
Solution-processed perovskite light emitting diodes with efficiency exceeding 15% through additive-controlled nanostructure tailoring journal September 2018
Trifluoroacetate induced small-grained CsPbBr3 perovskite films result in efficient and stable light-emitting devices journal February 2019
High-efficiency perovskite–polymer bulk heterostructure light-emitting diodes journal November 2018
Efficient blue light-emitting diodes based on quantum-confined bromide perovskite nanostructures journal August 2019
Perovskite light-emitting diodes with external quantum efficiency exceeding 20 per cent journal October 2018
Efficient and stable emission of warm-white light from lead-free halide double perovskites journal November 2018
Planar perovskite solar cells with long-term stability using ionic liquid additives journal July 2019
Determination of the exciton binding energy and effective masses for methylammonium and formamidinium lead tri-halide perovskite semiconductors journal January 2016
Organic–inorganic hybrid perovskite quantum dots with high PLQY and enhanced carrier mobility through crystallinity control by solvent engineering and solid-state ligand exchange journal January 2018
Detection of explosive vapors with a charge transfer molecule: self-assembly assisted morphology tuning and enhancement in sensing efficiency journal January 2010
Exciplex emission in bilayer polymer light-emitting devices journal March 1997
Electron mobility measurement using exciplex-type organic light-emitting diodes journal July 2002
Tuning emission color of electroluminescence from two organic interfacial exciplexes by modulating the thickness of middle gadolinium complex layer journal February 2006
Magnetic field effects on excited states, charge transport, and electrical polarization in organic semiconductors in spin and orbital regimes journal April 2019
Highly mobile charge-transfer excitons in two-dimensional WS 2 /tetracene heterostructures journal January 2018
Interface engineering of highly efficient perovskite solar cells journal July 2014
Overcoming the electroluminescence efficiency limitations of perovskite light-emitting diodes journal December 2015

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