Why lead-halide perovskites keep long carrier lifetimes despite defects · revision history

Revision 2

Accepted · core change · record

Changes against revision 1:

Title
Why lead-halide perovskites keep long carrier lifetimes despite defects
Plain
Solution-made perovskite films have many defects, yet light-generated charges in them survive for millionths of a second, much longer than in comparably imperfect ordinary semiconductors. Proposed reasons include charges wrapped in lattice distortions (polarons), a constantly fluctuating lattice, and defects whose energy levels lie harmlessly near the band edges.
Precise · changed · core
Revision 1: In MAPbI3, FAPbI3 and CsPbBr3, nonradiative lifetimes reach about 1e-6 s at trap densities of order $1e15\ \text{to}\ 1e16\,\mathrm{cm}^{-3}$ despite modest mobilities. Determine which mechanism dominates the suppression of Shockley-Read-Hall (defect-mediated) recombination: shallow intrinsic defect levels from antibonding valence-band character, large-polaron screening of capture, dynamic disorder reducing capture cross sections, or spin-split (Rashba) band edges. An answer is a ranking of mechanisms with first-principles nonadiabatic capture rates matching measured lifetimes versus $T$ and composition.
Revision 2: In MAPbI3, FAPbI3 and $\mathrm{CsPbBr_3}$, nonradiative lifetimes reach about $10^{-6}$ s at trap densities of order $10^{15}\ \text{to}\ 10^{16}\,\mathrm{cm}^{-3}$ despite modest mobilities. Determine which mechanism dominates the suppression of Shockley-Read-Hall (defect-mediated) recombination: shallow intrinsic defect levels from antibonding valence-band character, large-polaron screening of capture, dynamic disorder reducing capture cross sections, or spin-split (Rashba) band edges. An answer is a ranking of mechanisms with first-principles nonadiabatic capture rates matching measured lifetimes versus $T$ and composition.
Settled by
Computed capture coefficients for the dominant defects, including anharmonic lattice dynamics, that reproduce measured lifetimes and their temperature dependence.
Kind
phenomenon
Answer type
mechanism
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Literature status
contested
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Decisions