Dimensionality-dependent electronic and vibrational dynamics in low-dimensional organic-inorganic tin halides

Abstract Photo-induced dynamics of electronic processes are driven by the coupling between electronic and nuclear degrees of freedom. Here, we construct one- and two-dimensional organic-inorganic tin halides to investigate how dimensionality controls exciton-phonon coupling and exciton self-trapping. The results show that a one-dimensional system has strong exciton-phonon coupling leading to excitation-independent self-trapped exciton emission, whereas a two-dimensional system exhibits over ten times weaker coupling resulting in free exciton emission. The difference originates from enhanced Anderson localization in a one-dimensional system. Femtosecond transient absorption experiments directly resolve room-temperature vibrational wavepackets in a one-dimensional system, some of which propagate along the self-trapped-exciton potential energy surface. A combination of wagging and asymmetric stretching motions (~106 cm -1 ) in tin iodide is identified as such a mode, inducing exciton self-trapping. While no room-temperature wavepackets are observed in a two-dimensional system. These findings uncover the interplay between dimensionality-dependent exciton-phonon coupling and electronic/nuclear dynamics, offering constructive guidance to develop multifunctional organic-inorganic metal halides.