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Title: Spatial localization of excitons and charge carriers in hybrid perovskite thin films

The fundamental photophysics underlying the remarkably high power conversion efficiency of organic-inorganic hybrid perovskite-based solar cells has been increasingly studied using complementary spectroscopic techniques. The spatially heterogeneous polycrystalline morphology of the photoactive layers owing to the presence of distinct crystalline grains has been generally neglected in optical measurements and therefore the reported results are typically averaged over hundreds or even thousands of such grains. Here, we apply femtosecond transient absorption microscopy to spatially and temporally probe ultrafast electronic excited-state dynamics in pristine methylammonium lead tri-iodide (CH3NH3PbI3) thin films and composite structures. We found that the electronic excited-state relaxation kinetics are extremely sensitive to the sample location probed, which was manifested by position-dependent decay timescales and transient signals. As a result, analysis of transient absorption kinetics acquired at distinct spatial positions enabled us to identify contributions of excitons and free charge carriers.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
OSTI Identifier:
1209208
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 6; Journal Issue: 15; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE transient absorption microscopy (TAM); ultrafast electronic excited-state spectroscopy; Auger recombination; exciton-exciton annihilation; time-resolved optical imaging; perovskite