arXiv subjects

Myeongsam Jen

Publications and source records attributed to Myeongsam Jen.

2 recordsLinked to original sources

arXiv2026

Vortex-Beam Transient Absorption Microspectroscopy Resolves Ultrafast Free-Exciton and Polaron Diffusion in 2D Perovskites

Two-dimensional (2D) Ruddlesden Popper perovskites are promising optoelectronic materials with strongly confined excitonic properties; however, probing their ultrafast carrier transport dynamics, particularly the initial nonequilibrium diffusion regime, remains challenging because conventional transient absorption microscopy requires complex spatial imaging and lacks sufficient temporal sensitivity to resolve early time diffusion dynamics. Here, we demonstrate a vortex beam based transient absorption microspectroscopy platform (VTAM) enabling imaging free measurement of carrier transport by encoding spatial diffusion information into the mode dependent pump probe signal. By employing vortex probes with different topological charges, VTAM provides mode selective spatial sensitivity to excitonic dynamics with subpicosecond temporal resolution. Using VTAM, we resolved rapid free exciton (FE) diffusion followed by relaxation toward a slower steady state transport regime. A theoretically derived time dependent diffusion model separated transient and steady state transport contributions, yielding a transient diffusion enhancement (68.84 cm2 per s) and a steady state diffusion coefficient (1.85 cm2 per s), thus providing an initial diffusion coefficient (70.69 cm2 per s), and a cooling time of 0.35 ps. Measurements at the exciton-polaron (EP) resonance revealed strongly suppressed diffusion with nearly time independent signal ratios, indicating lattice-coupled EP transport. These parameters were extracted without spatial scanning or image reconstruction, establishing V-TAM as a powerful imaging free platform for investigating carrier transport in perovskites and other semiconductor systems.

physics.optics↗

arXiv2025

Ultrafast exciton polaron dynamics in 2D Ruddlesden Popper lead halide perovskites

Two dimensional Ruddlesden Popper (2D) RP hybrid perovskites exhibit substantially higher chemical and structural stability than their three dimensional (3D) counterparts, positioning them as promising candidates for next generation optoelectronics. While quasiparticle dynamics in 3D perovskites are well studied, their 2D analogues remain comparatively underexplored. Here we systematically investigate the branching, dynamics, and interactions of free excitons (FEs) and exciton polarons EPs in monolayer 2D RP perovskites using visible range femtosecond transient absorption TA spectroscopy. We prepared monolayer 2D RP perovskite thin films with varied organic spacers and distinct fabrication routes for comparative analysis. We find that the EP binding energy is 50 65 meV in (BA)2PbI4 and 37 39 meV in (PEA)2PbI4, consistent with spacer layer dependent coupling as corroborated by FTIR. We reveal a dynamic equilibrium between FEs and EPs that persists for tens of picoseconds. Notably, the TA signatures differ by fabrication route films from the newly developed process show weaker Auger annihilation and a reduced hot phonon bottleneck than those from the conventional route trends consistent with fewer traps and impurities in the former. Coupled rate equation modeling reproduces the transients and quantifies the processes of hot carrier relaxation, exciton exciton annihilation, exciton phonon coupling, and FE EP interconversion. These results demonstrate that the chemical synthetic process (fabrication route) and spacer choice significantly influence EP stability and population balance, offering practical levers for engineering ultrafast photophysics in 2D perovskites and guiding the design of advanced optoelectronic devices.

cond-mat.mtrl-sci↗