arXiv subjects

Vinod M. Menon

Publications and source records attributed to Vinod M. Menon.

At least 19 recordsLinked to original sources

arXiv2026

Cavity-Enhanced Activation of Radiatively Suppressed Light-Hole Exciton Emission in Colloidal Nanoplatelets

Light-hole (LH) excitons provide access to well-defined polarization and spin degrees of freedom that are central to quantum photonics and chiral light-matter interactions. Achieving LH emission is challenging because LH states are energetically unfavoured and typically relax non-radiatively. Existing strategies to access LH excitons rely on modifying the electronic band structure through strain, shape anisotropy, or piezoelectric fields, approaches that are material-specific and offer limited post-synthesis tunability. Here we demonstrate an all-photonic route to activate LH exciton emission in colloidal CdSe-CdS nanoplatelets (NPLs) using a distributed Bragg reflector (DBR) cavity, without altering the underlying band structure. In the absence of a cavity mode, the system exhibits amplified spontaneous emission from heavy-hole (HH) states without detectable LH emission at low excitation powers. By spectrally matching a cavity resonance to the LH exciton, cavity-coupled LH emission emerges at significantly lower excitation powers. Temperature-dependent spectroscopy reveals reversible switching between LH- and HH-coupled emission through exciton-cavity detuning, while polarization-resolved and spectrally resolved time-resolved photoluminescence measurements provide independent evidence distinguishing the cavity-coupled LH and HH emission channels. These findings establish cavity engineering as a general materials-level approach for accessing radiatively suppressed optical states.

physics.optics↗

arXiv2026

Optical Modulation Due to Energy Exchange Between Photonic and Exciton Modes in the Intermediate Coupling Regime

Actively tunable photonic devices are vital for next-generation optoelectronics requiring rapid switching and high bandwidth. Although organic optoelectronic devices have found wide application, their use as optical modulators has been limited by low absorption in the critical near-infrared (NIR) region, slow response time, and weak nonlinearities. To address these limitations, we developed a scheme based on intermediate exciton-photon coupling in a NIR absorbing squaraine-dye based photonic structure. Using energy-momentum resolved pump-probe spectroscopy, we show that the sign and magnitude of the optical response of our system depends strongly on the energy detuning between the excitonic and photonic modes. These data are analyzed using temporal coupled-mode theory to show that near resonance, a distinct energy exchange process emerges in the cross-over regime between strong and weak light-matter coupling. This effect enables dynamical control over the photoinduced response, providing a pathway for broadband optical signal modulation extending into the NIR spectral region.

physics.optics↗

arXiv2026

Generative modelling powered by room-temperature polariton condensates

Generative modelling requires efficient stochastic nonlinear transformations and physical platforms that can naturally realise them. We experimentally demonstrate that nonlinear optical systems operating in the strong light-matter coupling regime can serve as physical transformation layers for conditional generative modelling. Specifically, we develop a workflow in which room-temperature exciton-polariton condensates formed in organic dye microcavities act as a physical stochastic transform within a generative adversarial network and enable conditional digit-to-image translation. By using the nonlinear many-body dynamics and intrinsic stochasticity of polariton condensates, the workflow outperforms baseline approaches based on digitally injected perturbations. We find that polariton-enabled sampling via generative adversarial network (Polariton GAN) yields improved inception score, digit preservation accuracy and structural similarity compared with both digital sampling and laser-based systems. We further show that spatially correlated output variations can naturally regularise adversarial training and enhance output diversity. Our results establish polariton condensation as a new computational resource for generative modelling, opening a pathway towards physics-enhanced machine learning systems.

cond-mat.dis-nn↗

arXiv2026

Bulk and surface excitons in the van der Waals magnet CrSBr: Magneto-optical studies to 55 tesla

In thin layers of the 2D magnetic semiconductor CrSBr, very recent studies identified two distinct band-edge optical resonances, believed to arise from distinguishable bulk and surface excitons. This behavior reportedly originates from the highly anisotropic nature of CrSBr -- particularly in its antiferromagnetic state -- where excitons are effectively confined within individual monolayers, such that excitons in the two surface layers "see" a different local dielectric environment and have a lower resonance energy. To explore this scenario, here we investigate optical absorption properties of few-layer CrSBr in magnetic fields. In addition to the fundamental exciton resonance at ~1.36eV, we observe an absorption resonance ~20 meV lower in energy. Compared to the fundamental transition, this resonance redshifts only half as much in small magnetic fields that induce ferromagnetic order, while in high fields to 55T it exhibits a smaller diamagnetic shift. Both behaviors point to distinguishable populations of bulk and surface excitons in CrSBr.

cond-mat.mes-hall↗

arXiv2026

Microwave-to-optical transduction using magnon-exciton coupling in a layered antiferromagnet

Coherent interfaces between microwave-frequency quantum systems and low-loss optical links are essential for quantum networks. However, existing microwave-optical transducers often trade conversion efficiency against added noise, bandwidth, and device integrability. Here, we demonstrate coherent microwave-to-optical transduction based on magnon-exciton coupling in the layered antiferromagnet CrSBr. Driving the antiferromagnetic resonance with microwave signals imprints coherent modulation on a reflected optical probe, generating optical sidebands that are resonantly enhanced near excitonic transitions. While prior magnon-based approaches to microwave-to-optical transduction have typically relied on intrinsically weak off-resonant magneto-optical effects (e.g., Faraday rotation), our scheme exploits strong light-matter interactions at exciton resonances. Even in a bulk crystal without cavity enhancement, we observe coherent conversion over an intrinsically broadband window of ~ 300 MHz. We further show that multiple exciton-polariton resonances inherit the magnon-coupled response, suggesting a route to broaden the usable optical detuning range and to mitigate optical dissipation. Our results establish magnon-coupled excitons in layered magnets as a scalable platform for broadband microwave-optical interfaces, with pathways to higher cooperativity via reduced magnetic volume and cavity integration.

cond-mat.mtrl-sci↗

arXiv2026

Excitons in van der Waals magnetic materials

Two-dimensional magnetic semiconductors provide a unique materials platform in which long-range magnetic order coexists with strongly bound excitons. Because excitonic states and magnetic moments originate from the same electronic orbitals and are coupled through intrinsic exchange interactions, optical excitations in these systems exhibit pronounced sensitivity to magnetic order. Recent experiments have revealed unusually strong magneto-optical responses, as well as direct coupling between excitons and magnons, establishing new routes for controlling light-matter interactions with spin degrees of freedom. This Review surveys key developments in the field, focusing on representative material systems, experimental signatures of exciton-magnetism coupling, and the theoretical frameworks used to describe these phenomena. We conclude with perspectives on how this rapidly evolving field could enable next-generation optoelectronic and quantum technologies leveraging the coupled dynamics of light, charge, and spin.

cond-mat.mtrl-sci↗

arXiv2025

Towards coherent polaritonic circuits operating at room temperature

Polariton condensation is a potential system state for performing analog computations, given that it exhibits quantum behavior at macroscopic scales readily probed with low-cost optical methods. Current methods of fabricating devices in polariton microcavities largely involve patterning the devices via e-beam lithography before the cavity is completed, which offers less flexibility in device creation and reduces the maximum possible refractive index contrast. Moreover, the momentum and spatial distributions of the condensate are highly dependent on the host platform, and it has been difficult to preserve the desired behavior when modifying a given cavity. Here we introduce a method that addresses both of these challenges with the creation of polaritonic circuits of arbitrary forms etched via Focused Ion Beam into an organic microcavity based on Rhodamine 3B Perchlorate within a Small Molecule Ionic Isolation Lattices complex. We demonstrate room temperature condensation and propagation of polaritons in rectangular and trapezoidal waveguides by analyzing spatial and angle-resolved photoluminescence. We also discuss the blue-shifting and non-zero momentum of the condensate and show that it is strongly confined up to several higher energy levels. As an example, we report the spatial profiles of condensation in custom devices, such as a ring waveguide, a Y-splitter, and a Mach-Zehnder interferometer. This work represents a first step towards the realization of more complex, fully integrated, coherent polaritonic circuits operating at room temperature.

physics.optics↗

arXiv2025

Directional Flow of Confined Polaritons in CrSBr

Nanoscale control of energy transport is a central challenge in modern photonics. Utilization of exciton-polaritons hybrid light-matter quasiparticles is one viable approach, but it typically demands complex device engineering to enable directional transport. Here, we demonstrate that the van der Waals magnet CrSBr offers an inherent avenue for steering polariton transport leveraging a unique combination of intrinsic optical anisotropy, high refractive index, and excitons dressed by photons. This combination enables low-loss guided modes that propagate tens of microns along the crystal $a$-axis, while simultaneously inducing strong one-dimensional confinement along the orthogonal $b$-axis. By embedding CrSBr flakes in a microcavity, we further enhance the confinement, as evidenced by energy modes that are discretized along the $b$-axis but continuous along the $a$-axis. Moreover, the magneto-exciton coupling characteristic of CrSBr allows unprecedented control over both unidirectional propagation and confinement. Our results establish CrSBr as a versatile polaritonic platform for integrated optoelectronic device applications, including energy-efficient optical modulators and switches.

physics.optics↗

arXiv2025

Free Space Few-Photon Nonlinearity in Critically Coupled Polaritonic Metasurfaces

Few-photon optical nonlinearity in planar solid-state systems is challenging yet crucial for quantum and classical optical information processing. Polaritonic nonlinear metasurfaces have emerged as a promising candidate to push the photon number down -- but have often been hindered by challenges like the poor photon-trapping efficiency and lack of modal overlap. Here, we address these issues in a self-hybridized perovskite metasurface through critical coupling engineering, and report strong polaritonic nonlinear absorption at an ultra-low incident power density of only 519 W/cm2 (2 orders of magnitude lower than the state of art in free-space planar devices), with an estimated photon number of 6.12 per cavity lifetime. Taking advantage of a quasi-bound-state-in-the-continuum design with asymmetry-controlled quality-(Q)-factor, we systematically examine the Q-dependent device nonlinearity and determine the optimal cavity critical coupling condition. With the optimized device, we demonstrate at 6 Kelvin a tunable nonlinear response from reverse saturable absorption to saturable absorption at varying pump powers, with a maximal effective nonlinear absorption coefficient up to 29.4+-5.8 cm/W (6 orders of magnitude larger than unpatterned perovskites) at 560 nm wavelength. In addition, the cavity-exciton detuning dependent device response is analyzed and well explained by a phase-space-filling model, elucidating the underlying physics and the origin of giant nonlinearity. Our study paves the way towards practical flat nonlinear optical devices with large functional areas and massive parallel operation capabilities.

physics.optics↗

arXiv2024

Magnon-mediated exciton-exciton interaction in a van der Waals antiferromagnet

Excitons are fundamental excitations that govern the optical properties of semiconductors. Interacting excitons can lead to various emergent phases of matter and large nonlinear optical responses. In most semiconductors, excitons interact via exchange interaction or phase space filling. Correlated materials that host excitons coupled to other degrees of freedom offer hitherto unexplored pathways for controlling these interactions. Here, we demonstrate magnon-mediated excitonic interactions in CrSBr, an antiferromagnetic semiconductor. This interaction manifests as the dependence of exciton energy on exciton density via a magnonic adjustment of the spin canting angle. Our study demonstrates the emergence of quasiparticle-mediated interactions in correlated quantum materials, leading to large nonlinear optical responses and potential device concepts such as magnon-mediated quantum transducers.

cond-mat.mtrl-sci↗

arXiv2024

Magneto-optics in a van der Waals magnet tuned by self-hybridized polaritons

Controlling quantum materials with light is of fundamental and technological importance. By utilizing the strong coupling of light and matter in optical cavities (1-3), recent studies were able to modify some of their most defining features (4-6). In this work, we study the magneto-optical properties of a van der Waals magnet that supports strong coupling of photons and excitons even in the absence of external cavity mirrors. In this material - the layered magnetic semiconductor CrSBr - emergent light-matter hybrids called polaritons are shown to significantly increase the spectral bandwidth of correlations between the magnetic, electronic, and optical properties, enabling largely tunable optical responses to applied magnetic fields and magnons. Our results highlight the importance of exciton-photon self-hybridization in van der Waals magnets and motivate novel directions for the manipulation of quantum material properties by strong light-matter coupling.

cond-mat.mes-hall↗

arXiv2024

Moiré exciton polaron engineering via twisted hBN

Twisted hexagonal boron nitride (thBN) exhibits emergent ferroelectricity due to the formation of moiré superlattices with alternating AB and BA domains. These domains possess electric dipoles, leading to a periodic electrostatic potential that can be imprinted onto other 2D materials placed in its proximity. Here we demonstrate the remote imprinting of moiré patterns from twisted hexagonal boron nitride (thBN) onto monolayer MoSe2 and investigate the resulting changes in the exciton properties. We confirm the imprinting of moiré patterns on monolayer MoSe2 via proximity using Kelvin probe force microscopy (KPFM) and hyperspectral photoluminescence (PL) mapping. By developing a technique to create large ferroelectric domain sizes ranging from 1 μm to 8.7 μm, we achieve unprecedented potential modulation of 387 +- 52 meV. We observe the formation of exciton polarons due to charge redistribution caused by the antiferroelectric moiré domains and investigate the optical property changes induced by the moiré pattern in monolayer MoSe2 by varying the moiré pattern size down to 110 nm. Our findings highlight the potential of twisted hBN as a platform for controlling the optical and electronic properties of 2D materials for optoelectronic and valleytronic applications.

cond-mat.mtrl-sci↗

arXiv2024

Million-Q Free Space Meta-Optical Resonator at Visible Wavelengths

High-quality (Q)-factor optical resonators with extreme temporal coherence are of both technological and fundamental importance in optical metrology, continuous-wave lasing, and semiconductor quantum optics. Despite extensive efforts in designing high-Q resonators across different spectral regimes, the experimental realization of very large Q-factors at visible wavelengths remains challenging due to the small feature size that is sensitive to fabrication imperfections, and thus is typically implemented in integrated photonics. In the pursuit of free-space optics with the benefits of large space-bandwidth product and massive parallel operations, here we design and fabricate a visible-wavelength etch-free metasurface with minimized fabrication defects and experimentally demonstrate a million-scale ultrahigh-Q resonance. A new laser-scanning momentum-space-resolved spectroscopy technique with extremely high spectral and angular resolution is developed to characterize the record-high Q-factor as well as the dispersion of the million-Q resonance in free space. By integrating monolayer WSe2 into our ultrahigh-Q meta-resonator, we further demonstrate laser-like highly unidirectional and narrow-linewidth exciton emission, albeit without any operating power density threshold. Under continuous-wave laser pumping, we observe pump-power-dependent linewidth narrowing at room temperature, indicating the potential of our meta-optics platform in controlling coherent quantum light-sources. Our result also holds great promise for applications like optical sensing, spectral filtering, and few-photon nonlinear optics.

physics.optics↗

arXiv2024

Efficient and Tunable Photochemical Charge Transfer via Long-Lived Bloch Surface Wave Polaritons

Achieving precise control of photoinduced molecular charge transfer reactions underpins key emerging technologies. As such, the use of hybrid light-matter molecular exciton-polariton states has been proposed as a scheme to directly modify the efficiency and rate of such reactions. However, the efficacy of polariton-driven photochemistry remains an open question. Here, we demonstrate conditions under which photoinduced polaritonic charge transfer can be achieved and directly visualized using momentum resolved ultrafast spectroscopy. Key conditions for charge transfer are satisfied using Bloch surface wave polaritons, which exhibit favorable dispersion characteristics that permit the selective pumping of hybrid states with long lifetimes (100-400 fs) that permit vibrationally assisted molecular charge transfer. Using this approach, we tune the energetic driving force for charge separation, reducing it by as much as 0.5 eV compared to the bare exciton. These results establish that tunable and efficient polariton-driven molecular charge transfer is indeed possible using carefully considered photonic systems.

physics.optics↗

arXiv2024

Direct writing of room temperature polariton condensate lattice by top-down approach

Realizing lattices of exciton polariton condensates has been of much interest owing to the potential of such systems to realize analog Hamiltonian simulators and physical computing architectures. Prior work on polariton condensate lattices has primarily been on GaAs-based systems, with the recent advent of organic molecules and perovskite systems allowing room-temperature operation. However, in most of these room temperature systems, the lattices are defined using a bottom-up approach by patterning the bottom mirrors, significantly limiting the types of lattices and refractive index contrast that can be realized. Here, we report a direct write approach that uses a Focused Ion Beam (FIB) to etch 2D lattice into a planar microcavity. Such etching of the cavity allows for realizing high refractive index contrast lattices. We realize the polariton condensate lattice using the highly photostable host-guest Frenkel excitons of an organic dye small molecular ionic lattice (SMILES).1,2 The lattice structures are defined on a planar microcavity embedded with SMILES using FIB, allowing the realization of lattices with different geometries, including defect sites on demand. The band structure of the lattice and the emergence of condensation are imaged using momentum-resolved spectroscopy. The present approach allows us to study periodic, quasi-periodic, and disordered polariton condensate lattices at room temperature using a top-down approach without compromising on the quantum yield of the organic excitonic material embedded in the cavity.

cond-mat.mtrl-sci↗

arXiv2023

Addressing the Dark State Problem in Strongly Coupled Organic Exciton-Polariton Systems

The manipulation of molecular excited state processes through strong coupling has attracted significant interest for its potential to provide precise control of photochemical phenomena. However, the key limiting factor for achieving this control has been the dark state problem, in which photoexcitation populates long-lived reservoir states with similar energies and dynamics to bare excitons. Here, we use a sensitive ultrafast transient reflection method with momentum and spectral resolution to achieve the selective excitation of organic exciton-polaritons in open photonic cavities. We show that the energy dispersions of these systems allow us to avoid the parasitic effect of reservoir states. Under phase-matching conditions, we observe the direct population and decay of polaritons on time scales of less than 100 fs and find that momentum scattering processes occur on even faster timescales. We establish that it is possible to overcome the dark state problem through careful design of strongly coupled systems.

physics.optics↗

arXiv2023

Spin-correlated exciton-polaritons in a van der Waals magnet

Strong coupling between light and elementary excitations is emerging as a powerful tool to engineer the properties of solid-state systems. Spin-correlated excitations that couple strongly to optical cavities promise control over collective quantum phenomena such as magnetic phase transitions, but their suitable electronic resonances have yet to be found. Here we report strong light-matter coupling in $\textrm{NiPS}_3$, a van der Waals antiferromagnet with highly correlated electronic degrees of freedom. A previously unobserved class of polaritonic quasiparticles emerges from the strong coupling between its spin-correlated excitons and the photons inside a microcavity. Detailed spectroscopic analysis in conjunction with a microscopic theory provides unique insights into the origin and interactions of these exotic magnetically coupled excitations. Our work introduces van der Waals magnets to the field of strong light-matter physics and provides a path towards the design and control of correlated electron systems via cavity quantum electrodynamics.

cond-mat.mtrl-sci↗

arXiv2023

A plug-and-play molecular approach for room temperature polariton condensation

Exciton-polaritons (EP), half-light half-matter quasiparticles that form in optical cavities, are attractive platforms for creating macroscopic coherent states like BECs. EPs based on organic molecules are of particular interest for realizing such states at room temperature while offering the promise of synthetic tunability. However, the demonstrations of such condensates have been limited to a few specific molecular systems1. Here we report a universal platform for realizing molecular polariton condensates using commercial dyes that solves long standing material challenges. This solution is made possible using a new and programable molecular material called small-molecule, ionic isolation lattices (SMILES) with the potential to incorporate a wide array of molecular fluorophores2. We show EP condensation in rhodamine by incorporating it into SMILES lattice placed in a planar microcavity. The SMILES approach overcomes the major drawbacks of organic molecular photophysical systems such as self-quenching, which sets the foundation for realizing practical polaritonic devices operating at ambient temperatures covering wide spectral range.

physics.optics↗