Relativistic origin of slow electron-hole recombination in hybrid halide perovskite solar cells

Abstract

The hybrid perovskite CH3NH3PbI3 (MAPI) exhibits long minority-carrier lifetimes and diffusion lengths. We show that slow recombination originates from a spin-split indirect-gap. Large internal electric fields act on spin-orbit-coupled band extrema, shifting band-edges to inequivalent wavevectors, making the fundamental gap indirect. From a description of photoluminescence within the quasiparticle self-consistent GW (QSGW) approximation for MAPI, CdTe and GaAs, we predict carrier lifetime as a function of light intensity and temperature. At operating conditions we find radiative recombination in MAPI is reduced by a factor of more than 350 compared to direct gap behavior. The indirect gap is retained with dynamic disorder.

19 pages, 2 figures. V3 updates text and SI

References in corpus (3)

• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Revealing the role of organic cations in hybrid halide perovskites CH3NH3PbI3

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