Publication date: 22nd July 2026
Two-dimensional (2D) Ruddlesden–Popper metal halide perovskites exhibit one of the most intriguing optical responses among layered semiconductors. Their spectra frequently display multiple sidebands, broad quasi-plateaus, and pronounced thickness-dependent features that challenge straightforward excitonic interpretations. Here, we critically reassess the optical response of 2D perovskites by examining the intertwined roles of electronic structure, exciton fine structure, exciton–phonon coupling, and photonic effects. We show that the exceptionally large excitonic oscillator strength and high refractive index of these materials naturally give rise to polaritonic stop bands and interference phenomena that can dominate reflection, transmission, and absorption spectra, even in nominally freestanding crystals. These photonic contributions, often overlooked, substantially reshape spectral line shapes and complicate the identification of distinct excitonic resonances, calling for a more integrated electronic–photonic framework for interpreting the optical response of two-dimensional perovskites.
In the second part of my talk, I will revisit the lattice dynamics of 2D layered perovskites and show that Raman active modes, involve substantial motion of the organic sublattice. This finding challenges the conventional assignment of low-frequency modes to predominantly inorganic framework motion and instead reveals their intrinsically hybrid organic–inorganic character. Moreover, these modes can be selectively engineered through chemical substitution of the organic spacer, establishing an additional degree of freedom for controlling lattice dynamics in 2D perovskites. We next probe the lattice response under electronic excitation and identify signatures consistent with polaron formation. These polarons are hybrid in nature: their stabilization requires the coupled response of both organic and inorganic sublattices. Such coupling provides a route to tune the polaronic state through hybrid phonon modes. This hybrid polarons shape the linear optical response of layered 2D perovskites
