arXiv subjects

Rohit Rana

Publications and source records attributed to Rohit Rana.

3 recordsLinked to original sources

arXiv2026

Influence Functional Approach to Non-Perturbative Exciton Binding Renormalization from Phonons

We construct a many-body model Hamiltonian to capture how phonons renormalize exciton binding as a function of temperature. By using the GW approximation and density functional perturbation theory, we are able to parameterize this Hamiltonian completely from first principles. To capture static quasiparticle properties non-perturbatively, we evolve this Hamiltonian in imaginary time with path integral Monte Carlo using an influence functional based approach. For a class of Wannier-Mott type excitons, our binding energies are in quantitative agreement with experiment. We find that in addition to long-range dipolar interactions from longitudinal optical modes, short-ranged deformation potentials from acoustic modes and transverse optical modes can significantly renormalize electron and hole polaron binding energies at elevated temperature. However, exciton binding energies are only appreciably renormalized by coupling to optical phonons.

cond-mat.mtrl-sci↗

arXiv2025

Theoretical insights into the role of lattice fluctuations on the excited behavior of lead halide perovskites

Lead halide perovskites have been extensively studied as a class of materials with unique optoelectronic properties. A fundamental aspect that governs optical and electronic behaviors within these materials is the intricate coupling between charges and their surrounding lattice. Unravelling the role of charge-lattice interactions on the optoelectronic properties in lead halide perovskites is necessary to understand their photophysics. Unlike traditional semiconductors where a harmonic approximation often suffices to capture lattice fluctuations, lead halide perovskites have a significant anharmonicity attributed from the rocking and tilting motions of inorganic framework. Thus, while there is broad consensus on the importance of the structural deformations and polar fluctuations on the behavior of charge carriers and quasiparticles, the strongly anharmonic nature of these fluctuations and their strong interactions render theoretical descriptions of lead halides perovskites challenging. In this Account, we review our recent efforts to understand how the soft, polar lattice of this class of materials alter their quasiparticle binding energies and fine structure, charge mobilities, and lifetimes of phonons and excess charges. Throughout, these are aimed at characterizing the interplay between lattice fluctuations and optoelectronic properties of lead halide perovskites and are reviewed in the context of the effective models we have built, and the novel theoretical methods we have developed to understand bulk crystalline materials, as well as nanostructures, and lower dimensionality lattices. By integrating theoretical advances with experimental observations, the perspective we detail in this account provides a comprehensive picture that serves as both design principles for optoelectronic materials and a set of theoretical tools to study them when charge-lattice interactions are important.

cond-mat.mtrl-sci↗

arXiv2025

On the interplay of electronic and lattice screening on exciton binding in two-dimensional lead halide perovskites

We use path integral Monte Carlo to study the energetics of excitons in layered, hybrid organic-inorganic perovskites in order to elucidate the relative contributions of dielectric confinement and electron-phonon coupling. While the dielectric mismatch between polar perovskite layers and non-polar ligand layers significantly increases the exciton binding energy relative to their three dimensional bulk crystal counterparts, formation of exciton polarons attenuates this effect. The contribution from polaron formation is found to be a non-monotonic function of the lead halide layer thickness, which is clarified by a general variational theory. Accounting for both of these effects provides a description of exciton binding energies in good agreement with experimental measurements. By studying isolated layers and stacked layered crystals of various thicknesses, with ligands of varying polarity, we provide a systematic understanding of the excitonic behavior of this class of materials and how to engineer their photophysics.

cond-mat.mtrl-sci↗