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Title: Direct experimental evidence for photoinduced strong-coupling polarons in organolead halide perovskite nanoparticles

Echoing the roaring success of their bulk coun-terparts, nano-objects built from organolead halide perov-skites (OLHP) present bright prospects for surpassing the performances of their conventional organic and inorganic analogues in photodriven technologies. Unraveling the pho-toinduced charge dynamics is essential for optimizing OLHP optoelectronic functionalities. However, mapping the carri-er-lattice interactions remains challenging, owing to their manifestations on multiple length scales and time scales. By correlating ultrafast time-resolved optical and X-ray absorp-tion measurements, this work reveals the photoinduced formation of strong-coupling polarons in CH 3NH 3PbBr 3 nanoparticles. Such polarons originate from the self-trapping of electrons in the net Coulombic field caused by the dis-placed inorganic nuclei and the oriented organic cations. The transient structural change detected at the Pb L 3 X-ray ab-sorption edge is well captured by a distortion with average bond elongation in the [PbBr 6] 2- motif. As a result, general implications for designing novel OLHP nanomaterials targeting the active utilization of these quasi-particles are outlined.
Authors:
 [1] ;  [2] ;  [1] ;  [3] ;  [1] ;  [2] ;  [4] ;  [4] ;  [4] ;  [1] ;  [1] ;  [4] ;  [5] ;  [4] ;  [1] ;  [6]
  1. Lund Univ., Lund (Sweden)
  2. (Qatar)
  3. (Egypt)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Qatar Univ., Doha (Qatar)
  6. Univ. of Hamburg, Hamburg (Germany)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 7; Journal Issue: 22; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Scientific User Facilities Division; Knut and Alice Wallenberg Foundation; Swedish Research Council (SRC)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; CH3NH3PBI3; exciton binding-energy; lead-iodide perovskites; charge-carriers; molecules; solar-cells; trap states
OSTI Identifier:
1369031