  Owing to their high energy-conversion efficiency and inexpensive fabrication
routes, solar cells based on metal-organic halide perovskites have rapidly
gained prominence as a disruptive technology. An attractive feature of
perovskite absorbers is the possibility of tailoring their properties by
changing the elemental composition through the chemical precursors. In this
context, rational in silico design represents a powerful tool for mapping the
vast materials landscape and accelerating discovery. Here we show that the
optical band gap of metal-halide perovskites, a key design parameter for solar
cells, strongly correlates with a simple structural feature, the largest
metal-halide-metal bond angle. Using this descriptor we suggest continuous
tunability of the optical gap from the mid-infrared to the visible. Precise
band gap engineering is achieved by controlling the bond angles through the
steric size of the molecular cation. Based on these design principles we
predict novel low-gap perovskites for optimum photovoltaic efficiency, and we
demonstrate the concept of band gap modulation by synthesising and
characterising novel mixed-cation perovskites.
