Phonon-Mediated Chirality Transfer from Organic Cation to Inorganic lattice in Hybrid Perovskites

Abstract

Two-dimensional hybrid metal halide perovskites combine spin-orbit coupling, soft lattice dynamics, and molecular tunability, making them promising platforms for chiral optoelectronics. While chiral organic spacers are known to induce optical activity in the inorganic framework, the microscopic mechanism by which molecular chirality couples to the inorganic lattice is actively studied. Here, we investigate coherent vibrational dynamics in chiral ($R$-MBA)$_2$PbI$_4$ and its racemic analogue using circular-polarized transient absorption spectroscopy. A vibrational mode at ~5.7 meV is present in the chiral material and not observed in the racemic counterpart, confirmed as a lattice phonon by agreement between time-domain and steady-state measurements. Ab-initio calculations reveal correlated libration of the organic spacer and bending displacement of the Pb-I framework analogous to a classical Wilberforce pendulum whose sense is locked to the structural handedness of the lattice. Polarization-resolved measurements reveal a transient circular dichroism whose exact sign reversal between ($R$-MBA)$_2$PbI$_4$ and ($S$-MBA)$_2$PbI$_4$ is consistent with a periodic modulation of the excitonic rotational strength driven by the coupled lattice displacement. These results establish dynamic chirality transfer through the coupled librational-bending mechanism, with direct implications for phonon-driven chiral optical responses and spin-selective transport.