Chiral Phonons in 2D Halide Perovskites

Abstract

Phonons in chiral crystal structures can be circularly polarized, making them chiral. Chiral phonons carry angular momentum, which is observable in heat currents, and, via coupling to electron spin, in spin currents. Two-dimensional (2D) halide perovskites, versatile direct band gap semiconductors, can easily form chiral structures by incorporating chiral organic cations. As a result, they exhibit phenomena such as chirality-induced spin selectivity (CISS) and the spin Seebeck effect, although the underlying mechanisms remain unclear. Using on-the-fly machine-learning force fields trained against density functional theory calculations, we confirm the presence of chiral phonons, a potential key factor for these effects. Our analysis reveals that low-energy phonons, originating from the inorganic framework, primarily exhibit chirality. Under a temperature gradient, these chiral phonons generate substantial angular momentum, leading to experimentally observable effects. These findings position chiral 2D perovskites as a promising platform for exploring the interplay among phononic, electronic, spintronic, and thermal properties.