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Title: Perovskite Solar Cells with Near 100% Internal Quantum Efficiency Based on Large Single Crystalline Grains and Vertical Bulk Heterojunctions

Grain boundaries (GBs) as defects in the crystal lattice detrimentally impact the power conversion efficiency (PCE) of polycrystalline solar cells, particularly in recently emerging hybrid perovskites where non-radiative recombination processes lead to significant carrier losses. Here, the beneficial effects of activated vertical GBs are demonstrated by first growing large, vertically-oriented methylammonium lead tri-iodide (CH3NH3PbI3) single-crystalline grains. We show that infiltration of p-type doped 2 -7,7 -tetrakis(N,Ndi-p-methoxyphenylamine)-9,9-spirobifluorene (Spiro-OMeTAD) into CH3NH3PbI3 films along the GBs creates space charge regions to suppress non-radiative recombination and enhance carrier collection efficiency. Solar cells with such activated GBs yielded average PCE of 16.3 ± 0.9%, which are among the best solution-processed perovskite devices. As an important alternative to growing ideal CH3NH3PbI3 single crystal films, which is difficult to achieve for such fast-crystallizing perovskites, activating GBs paves a way to design a new type of bulk heterojunction hybrid perovskite photovoltaics toward theoretical maximum PCE.
 [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [2] ;  [1] ;  [1] ;  [2] ;  [1] ;  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
OSTI Identifier:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 137; Journal Issue: 29; Journal ID: ISSN 0002-7863
American Chemical Society (ACS)
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States