Due to their high photovoltaic efficiency and low-cost synthesis, lead halide
perovskites have attracted wide interest for application in new solar cell
technologies. The most stable and efficient ABX3β perovskite solar cells
employ mixed A-site cations, however the impact of cation mixing on carrier
trapping and recombination -- key processes that limit photovoltaic performance
-- is not fully understood. Here we analyse non-radiative carrier trapping in
the mixed A-cation hybrid halide perovskite MA1βxβCsxβPbI3β. By using
rigorous first-principles simulations combined with techniques initially
developed for organic molecular materials, we show that cation mixing leads to
a hole trapping rate at the iodine interstitial that is seven orders of
magnitude greater than in the single cation system. We demonstrate that the
same defect in the same material can display a wide variety of defect activity
-- from electrically inactive to recombination centre -- and, in doing so,
resolve conflicting reports in the literature. Finally, we propose a new
mechanism in which composition can be used to determine the rate of carrier
trapping; this is achieved by controlling the phase and dynamical response of
the lattice through the steric size of the A-site cations. Our findings
elucidate crucial links between chemical composition, defect activity and
optoelectronic performance, and present a general approach that can help to
rationalise the development of new materials with target defect properties