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Title: Tunable Anisotropic Photon Emission from Self-Organized CsPbBr3 Perovskite Nanocrystals

Journal Article · · Nano Letters
ORCiD logo [1];  [2];  [3];  [4]; ORCiD logo [5];  [2];  [5];  [6];  [4]; ORCiD logo [7];  [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry. Materials Sciences Division
  2. Univ. of Augsburg (Germany). Inst. of Physics
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  5. Univ. of California, Berkeley, CA (United States). College of Chemistry
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Univ. of California, Berkeley, CA (United States). College of Chemistry. Dept. of Materials Science and Engineering; Kavli Energy NanoScience Inst., Berkeley, CA (United States)

In this paper, we report controllable anisotropic light emission of photons originating from vertically aligned transition dipole moments in spun-cast films of CsPbBr3 nanocubes. By depositing films of nanocrystals on precoated substrates we can control the packing density and resultant radiation pattern of the emitted photons. We develop a technical framework to calculate the average orientation of light emitters, i.e., the angle between the transition dipole moment vector (TDM) and the substrate. This model is applicable to any emissive material with a known refractive index. Theoretical modeling indicates that oriented emission originates from an anisotropic alignment of the valence band and conduction band edge states on the ionic crystal lattice and demonstrates a general path to model the experimentally less accessible internal electric field of a nanosystem from the photoluminescent anisotropy. The uniquely accessible surface of the perovskite nanoparticles allows for perturbation of the normally isotropic emissive transition. Finally, the reported sensitive and tunable TDM orientation and control of emitted light will allow for applications of perovskite nanocrystals in a wide range of photonic technologies inaccessible to traditional light emitters.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Advanced Research Projects Agency - Energy (ARPA-E); Bavaria California Technology Center (BaCaTeC); German Federal Ministry of Education and Research (BMBF); German Research Foundation (DFG)
Grant/Contract Number:
AC02-05CH11231; AR0000627; 13N13664; Br 1728/18-1
OSTI ID:
1460297
Journal Information:
Nano Letters, Vol. 17, Issue 7; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 59 works
Citation information provided by
Web of Science

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Strategies to Improve Luminescence Efficiency of Metal‐Halide Perovskites and Light‐Emitting Diodes journal September 2018
Perovskite Light-Emitting Diodes with Improved Outcoupling Using a High-Index Contrast Nanoarray journal January 2019
Incorporation of rubidium cations into blue perovskite quantum dot light-emitting diodes via FABr-modified multi-cation hot-injection method journal January 2019
Ultrathin CsPbX 3 Nanowire Arrays with Strong Emission Anisotropy journal June 2018
Fluorescence Anisotropy Reloaded—Emerging Polarization Microscopy Methods for Assessing Chromophores' Organization and Excitation Energy Transfer in Single Molecules, Particles, Films, and Beyond journal February 2019
Strong Polarized Photoluminescence from Stretched Perovskite-Nanocrystal-Embedded Polymer Composite Films journal October 2017
Scalable photonic sources using two-dimensional lead halide perovskite superlattices journal January 2020
Perovskite nanowire–block copolymer composites with digitally programmable polarization anisotropy journal May 2019
Optical anisotropy of one-dimensional perovskite C 4 N 2 H 14 PbI 4 crystals journal January 2020
Scalable photonic sources using two-dimensional lead halide perovskite superlattices text January 2020
Scalable photonic sources using two-dimensional lead halide perovskite superlattices text January 2020
Investigation into the Photoluminescence Red Shift in Cesium Lead Bromide Nanocrystal Superlattices journal January 2019