arXiv subjects

Katherine A Koch

Publications and source records attributed to Katherine A Koch.

3 recordsLinked to original sources

arXiv2026

Temperature-Induced Crossover of Coherent Phonon Mechanisms in Chiral 2D Perovskites

The coupling between electronic excitations and lattice degrees of freedom fundamentally dictates the optoelectronic functionality of hybrid perovskites. While the potential energy surfaces (PESs) of the electronic excited states are typically considered static, albeit modulated by thermal disorder, the exact nature of their structural evolution with temperature remains elusive. Here, we demonstrate that the excited-state structural reconfiguration in two-dimensional metal-halide perovskites is explicitly temperature-evolving, governed by lattice compliance. We select a chiral perovskite framework with an exceptionally large, temperature-dependent bond angle variance to maximize the structural compliance. Through phase-resolved resonant impulsive stimulated Raman scattering, we measure the coherent phonon dynamics and resolve the real-time structural pathways of exciton-lattice dressing. We observe a temperature-induced crossover from field-driven Impulsive Stimulated Raman Scattering (ISRS) to population-driven Displacive Excitation of Coherent Phonons (DECP). While momentum-driven ISRS pathways dominate at low temperatures, increasing thermal energy softens the lattice and enhances coordinate-driven displacive pathways, allowing excitons to sample steeper, highly anharmonic regions of the excited-state PES. Our results show that temperature can actively modulate the excited-state structural coordinates of flexible 2D frameworks, offering a practical strategy to tune exciton-lattice interactions in chiral optoelectronics.

cond-mat.mtrl-sci↗

arXiv2025

Nonlinear Dynamics in the Formation of Molecular Polariton Condensates

Exciton-polaritons - hybrid light-matter quasiparticles - can undergo Bose-Einstein-like condensation at elevated temperatures owing to their lower effective mass. This becomes even more pronounced in the context of molecular polariton condensates where the large exciton binding energy of Frenkel excitons facilitates condensation at room temperature. While widely studied as low-threshold coherent light sources, the dynamics of their condensation remain poorly understood, partly due to the limitations of existing kinetic models. Here, we use excitation correlation photoluminescence (ECPL), a nonlinear optical technique with 220fs resolution, to probe molecular polariton condensation in Rhodamine-B-doped small-molecule ionic isolation lattices (SMILES). This platform promotes dipole alignment and suppresses detrimental intermolecular interactions. ECPL reveals condensate formation within hundreds of femtoseconds, driven by radiative scattering from the reservoir. A sustained population beyond the polariton lifetime suggests an additional feeding mechanism from higher momentum states in the lower polariton dispersion. These results provide quantitative insight into condensation timescales and mechanisms, advancing our control over polariton dynamics.

cond-mat.mtrl-sci↗

arXiv2025

Fine-Tuning Exciton Polaron Characteristics via Lattice Engineering in 2D Hybrid Perovskites

The layered structure of 2D metal halide perovskites (MHPs) consisting of an ionic metal halide octahedral layer electronically separated by an organic cation, exhibits strong coupling between high-binding-energy excitons and low-energy lattice phonons. Photoexcitations in these systems are believed to be exciton polarons, Coulombically bound electron-hole pairs dressed by lattice vibrations. Understanding and controlling the structural and chemical factors that govern this interaction is crucial for optimizing exciton recombination, transport, and many-body interactions. Our study examines the role of the organic cation in a prototypical 2D-MHP system, phenylethylammonium lead iodide, (PEA)2PbI4, and its halogenated derivatives, (F/Cl-PEA)2PbI4. These substitutions allow us to probe polaronic effects while maintaining the average lattice and electronic structure. Using resonant impulsive stimulated Raman scattering (RISRS), we analyze the metal-halide sub-lattice motion coupled to excitons. We apply formalism based on a perturbative expansion of the nonlinear response function on the experimental data to estimate the Huang-Rhys parameter, $S=1/2 Δ^2$, to quantify the lattice displacement ($Δ$) due to exciton-phonon coupling. A direct correlation emerges between lattice displacement and octahedral distortion, with F-PEA exhibiting the largest shift and Cl-PEA exhibiting the least, significantly influencing the fine structure features in absorption. Additionally, 2D electronic spectroscopy reveals that F-PEA, with the strongest polaronic coupling, exhibits the least thermal dephasing, supporting the polaronic protection hypothesis. Our findings suggest that systematic organic cation substitution serves as a tunable control for the fine structure in 2D-MHPs, and offers a pathway to mitigate many-body scattering effects by tailoring the polaronic coupling.

cond-mat.mtrl-sci↗