Owing to the predominant merit of tunable bandgaps, tin-lead mixed perovskites have shown great potentials in realizing near-infrared optoelectronics and are receiving increasing attention. However, despite the merit, there is still a lack of fundamental understanding of the bandgap variation as a function of Sn/Pb ratio, mainly because the films are easy to segregate in terms of both composition and phase. Here, we report a fully stoichiometric synthesis of monocrystalline FAPb1-xSnxI3 nanocrystals as well as their atomic-scale imaging. On the basis of the systematic measurements of the monocrystalline materials, strain and Coulomb interaction-induced atomic ordering was revealed to be responsible for the unusual discontinuous bandgap jumping near x = 0.5 from the expected bowing effect. As a result, both FAPb0.6Sn0.4I3 and FAPb0.4Sn0.6I3 have the lowest bandgaps of around 1.27 electron volts, while that of FAPb0.5Sn0.5I3 is 1.33 electron volts. Correspondingly, their based light-emitting diodes can emit infrared lights with the wavelengths reaching 930 nanometers.
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