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Title: Tunable Anisotropic Photon Emission from Self-Organized CsPbBr 3 Perovskite Nanocrystals

In this paper, we report controllable anisotropic light emission of photons originating from vertically aligned transition dipole moments in spun-cast films of CsPbBr 3 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.
Authors:
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)
Publication Date:
Grant/Contract Number:
AC02-05CH11231; AR0000627; 13N13664; Br 1728/18-1
Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal Issue: 7; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States); Univ. of Augsburg (Germany)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); 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)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; CsPbBr3; nanocrystal; oriented emission; perovskite
OSTI Identifier:
1460297