arXiv subjects

Sankaran Ramesh

Publications and source records attributed to Sankaran Ramesh.

5 recordsLinked to original sources

arXiv2026

Franson-Interferometric Bounds on Entangled Two-Photon Absorption

Entangled photons offer quantum correlations with no classical analogue. In entangled pair two-photon absorption (ETPA), absorption rate is predicted to scale linearly rather than quadratically with photon flux, promising molecular excitation at fluxes far below the classical threshold. Reported ETPA cross sections nevertheless vary widely across experiments, largely since the observable, the differential of the transmitted flux or weak fluorescence, is difficult to separate from scattering and linear losses. We present a method which uses Franson interference to study entangled two-photon absorption through delay-dependent coincidence measurements on dye molecules. Applying the method to Rhodamine 6G, we observe a small asymmetry in the Franson interference envelope and obtain a model-derived effective cross section of approximately 2.1 E(-21) centimeter squared for Rhodamine 6G. However, the estimated systematic uncertainty does not allow a definitive ETPA assignment. Instead, the experiment establishes a quantitative bound on the ETPA response and provides a background-free benchmark for future measurements.

physics.chem-ph↗

arXiv2026

Helicity-Resolved Spatiotemporal Mapping of Chiral Plexcitons in Helicoids

Plasmon-exciton hybrids, or plexcitons, offer deeply subwavelength light-matter interactions with versatile pathways for energy redistribution. Incorporating chirality into such systems is particularly compelling, enabling spin-sensitive optical functionality that can operate on ultrafast timescales and within ultracompact volumes. Despite recent progress in chiral plexcitonic systems, how structural chirality and plasmon-exciton coupling determine chiroptical spectra and ultrafast energy flow remains elusive. Here we realize chiral plexcitons by functionalizing intrinsically chiral gold helicoid nanoparticles with molecular J-aggregates. Within a non-Hermitian framework, we trace the microscopic origin of the helicoid chiroptical response and its coupling to the excitonic transition, revealing how the helicity of light selectively addresses distinct hybrid responses. At the spatiotemporal extreme, we find that the gap-localized response not only enhances polarization-sensitive contrast but also strengthens the local hybrid interaction, leading to accelerated ultrafast relaxation. Together, these space-, time-, and polarization-resolved measurements provide a physically grounded and experimentally benchmarked picture of chiral plexcitonic coupling, identifying chirality as a practical control parameter for selectively steering nanoscale energy pathways and dynamics.

physics.optics↗

arXiv2025

Phonon-Mediated Chirality Transfer from Organic Cation to Inorganic lattice in Hybrid Perovskites

Two-dimensional hybrid metal halide perovskites combine spin-orbit coupling, soft lattice dynamics, and molecular tunability, making them promising platforms for chiral optoelectronics. While chiral organic spacers are known to induce optical activity in the inorganic framework, the microscopic mechanism by which molecular chirality couples to the inorganic lattice is actively studied. Here, we investigate coherent vibrational dynamics in chiral ($R$-MBA)$_2$PbI$_4$ and its racemic analogue using circular-polarized transient absorption spectroscopy. A vibrational mode at ~5.7 meV is present in the chiral material and not observed in the racemic counterpart, confirmed as a lattice phonon by agreement between time-domain and steady-state measurements. Ab-initio calculations reveal correlated libration of the organic spacer and bending displacement of the Pb-I framework analogous to a classical Wilberforce pendulum whose sense is locked to the structural handedness of the lattice. Polarization-resolved measurements reveal a transient circular dichroism whose exact sign reversal between ($R$-MBA)$_2$PbI$_4$ and ($S$-MBA)$_2$PbI$_4$ is consistent with a periodic modulation of the excitonic rotational strength driven by the coupled lattice displacement. These results establish dynamic chirality transfer through the coupled librational-bending mechanism, with direct implications for phonon-driven chiral optical responses and spin-selective transport.

cond-mat.mtrl-sci↗

arXiv2025

Dimensionality-dependent electronic and vibrational dynamics in low-dimensional organic-inorganic tin halides

Photo-induced dynamics of electronic processes in materials are driven by the coupling between electronic and nuclear degrees of freedom. Here we construct 1D and 2D organic-inorganic tin halides to investigate the functional role of dimensionality to exciton-phonon coupling (EPC) and exciton self-trapping. The results show that the 1D system has strong EPC leading to excitation-independent self-trapped exciton (STE) emission, while the 2D system exhibits over ten times weaker EPC resulting in free exciton emission. By performing femtosecond transient absorption experiments, we directly resolve the room-temperature vibrational wavepackets in the 1D system, some of which propagate along the STE potential energy surface. A combination of wagging and asymmetric stretching motions (~106 cm-1) in tin iodide is identified as such a mode inducing exciton self-trapping. While no room-temperature wavepackets are observed in the 2D system. These findings uncover the interplay between the dimensionality-dependent EPC and electronic/nuclear dynamics, offering constructive guidance to develop multifunctional organic-inorganic metal halides.

physics.chem-ph↗

arXiv2024

Coherent Phonons, Localization and Slow Polaron Formation in Lead-free Gold Perovskite

Lead-free metal halide perovskites are emerging as less-toxic alternatives to their lead-based counterparts. However, their applicability in optoelectronic devices is limited, and the charge transport dynamics remain poorly understood. Understanding photo-induced charge and structural dynamics is critical for unlocking the potential of these novel systems. In this work, we employ ultrafast optical and Raman spectroscopy combined with band structure calculations to investigate the coupled electronic and vibrational dynamics in Caesium gold bromide, a promising lead-free perovskite. We find that the band-edge charge transfer states are strongly coupled to Au-Br stretching phonon modes, leading to frequency modulation of absorption by impulsively excited coherent phonons. Early-stage relaxation is characterized by dynamics of delocalized charge transfer excitation and slowly decaying coherent phonons. The electronic and vibrational relaxation reveals a slow formation of a localized polaronic state in the 10-20 ps timescale. Using a displaced harmonic oscillator model, the polaronic binding energy is estimated to be ~80 meV following lattice relaxation along the phonon modes. Strong exciton-phonon coupling and slow polaron formation via coupling to lattice modes make this material a promising testbed for the control of coherent phonons and localized polaronic states using light.

cond-mat.mtrl-sci↗