arXiv subjects

Jamie M. Fitzgerald

Publications and source records attributed to Jamie M. Fitzgerald.

17 recordsLinked to original sources

arXiv2026

Coherent interaction of WS$_2$ and quasi-2D perovskite excitons over micrometer distances via a cavity field

The coherent coupling of cavity-confined photons and excitonic matter resonances leads to the formation of cavity polaritons, hybrid light-matter quasi-particles. If multiple exciton resonances couple to the same photonic mode, the resulting polariton constitutes a coherent interaction between matter resonances that can be spatially separated without any direct electronic coupling. In this work, we demonstrate the formation of such a coherent coupling at room temperature using an open optical cavity containing two distinct van der Waals materials - monolayer WS2 and layered quasi-2D halide perovskites (HaPs) - separated by $1.5 \mu\rm m$. The system forms three polariton branches, with the middle branch possessing nearly equal fractions of both excitons and the photonic mode. White-light reflectivity and luminescence measurements are in good agreement with simulations using a coupled harmonic oscillator and a microscopic Wannier-Hopfield framework. Our results lay the foundation to combine highly complementary degrees of freedom in 2D materials in an in-situ tunable fashion to enable new polaritonic functionalities.

cond-mat.mes-hall↗

arXiv2026

Perfect Absorption in the Strong Coupling Regime via Degenerate Critical Coupling

Perfect absorption (PA) represents a fundamental limit of light-matter interaction and a means to maximize nanoscale energy conversion. While PA is now a well-established phenomenon, both the theoretical feasibility and a practical mechanism for achieving it under single-beam excitation within the strong coupling regime is unknown. Through rigorous solution of Maxwells equations for a compact photonic crystal (PhC) architecture incorporating a two-dimensional semiconductor, we present a general method based on degenerate critical coupling for single-port PA of exciton-polaritons. At the crossing of two polariton branches, we achieve near-unity absorption exceeding 99.8 \% in a structure thinner than $100\,$nm. This effect is robust under realistic Gaussian beam excitation, and can be realized across different temperatures and excitonic materials by tailoring the PhC geometry. Our results establish a strategy for enabling efficient light-matter coupling, with direct implications for the development of metal-free, ultra-compact polaritonic logic devices, sensors, and energy-harvesting platforms.

cond-mat.mes-hall↗

arXiv2026

Engineering strong coupling in ultra-compact photonic crystal/2D material platforms

Sub-wavelength thick photonic crystal (PhC) slabs coupled to 2D excitonic materials, such as transition metal dichalcogenides (TMDs), are a promising platform for highly tunable, room-temperature, on-chip optoelectronic devices. Unlike conventional Fabry-Perot microcavities, these compact open cavities exhibit non-trivial electric field profiles, leading to spatially distinct regions of weak and strong coupling with excitons within the PhC unit cell. Using coupled mode theory and rigorous solutions to Maxwell's equations, we investigate how the PhC geometry can be used to control these coexisting exciton/polariton contributions and tailor the resulting optical spectra. For large filling factors, i.e., small air gaps, we show that PhC polaritons can be modeled as dark waveguide modes brightened via the periodicity of the PhC slab. Furthermore, by spatially patterning the TMD monolayer based on the local field intensity, we reveal the simultaneous presence of excitons in both the weak and strong coupling regimes. Overall, this work provides fundamental insights into the strong light-matter coupling regime in structured photonic environments, offering a pathway to design and optimize metal-free, ultra-compact polaritonic devices.

physics.optics↗

arXiv2025

Polariton transport in 2D semiconductors: Phonon-mediated transitions between ballistic, superdiffusive and exciton-limited regimes

Exciton transport in 2D semiconductors holds promise for room-temperature, ultra-compact optoelectronic devices, but it is limited by short propagation distances. Hybridization of excitons with cavity photons to form exciton-polaritons can enhance the propagation by orders of magnitude, enabling a coherent, ballistic transport. However, a microscopic understanding of the role of phonons is still lacking, particularly regarding their influence on the crossover from the ballistic to the diffusive polariton transport regime. Here, we investigate the spatiotemporal polariton dynamics in \ce{MoSe2} monolayers at moderate to high temperatures, explicitly including the phonon-mediated coupling to the intervalley exciton reservoir. We identify three distinct transport regimes: (i) an initial sub-ps ballistic-like regime characterized by a phonon-induced velocity renormalization, (ii) a transient, few-ps superdiffusive regime characterized by strongly enhanced diffusion, and (iii) a slower, exciton-limited diffusion following thermalization. The gained microscopic insights will trigger and guide future experimental studies on the phonon-mediated polariton transport in atomically thin semiconductors.

cond-mat.mes-hall↗

arXiv2025

Tuning relaxation and nonlinear upconversion of valley-exciton-polaritons in a monolayer semiconductor

Controlling exciton relaxation and energy conversion pathways via their coupling to photonic modes is a central task in cavity-mediated quantum materials research. In this context, the light-matter hybridization in optical cavities can lead to intriguing effects, such as modified carrier transport, enhancement of optical quantum yield, and control of chemical reaction pathways. Here, we investigate the impact of the strong light-matter coupling regime on energy conversion, both in relaxation and upconversion schemes, by utilizing a strongly charged MoSe2 monolayer embedded in a spectrally tunable open-access cavity. We find that the charge carrier gas yields a significantly modified photoluminescence response of cavity exciton-polaritons, dominated by an intra-cavity like pump scheme. In addition, upconversion luminescence emerges from a population transfer from fermionic trions to bosonic exciton-polaritons. Due to the availability of multiple optical modes in the tunable open cavity, it seamlessly meets the cavity-enhanced double resonance condition required for an efficient upconversion. The latter can be actively tuned via the cavity length in-situ, displaying nonlinear scaling in intensity and fingerprints of the valley polarization. This suggests mechanisms that include both trion-trion Auger scattering and phonon absorption as its underlying microscopic origin.

cond-mat.mes-hall↗

arXiv2025

Magneto-Optics of Anisotropic Exciton Polaritons in Two-Dimensional Perovskites

Layered 2D organic-inorganic perovskite semiconductors support strongly confined excitons that offer significant potential for ultrathin polaritonic devices due to their tunability and huge oscillator strength. The application of a magnetic field has proven to be an invaluable tool for investigating the exciton fine structure observed in these materials. Yet, the combination of an in-plane magnetic field and the strong coupling regime has remained largely unexplored. In this work, we combine microscopic theory with a rigorous solution of Maxwell's equations to model the magneto-optics of exciton polaritons in 2D perovskites. We predict that the brightened dark exciton state can enter the strong coupling regime. Furthermore, the magnetic-field-induced mixing of polarization selection rules and the breaking of in-plane symmetry lead to highly anisotropic polariton branches. This study contributes to a better understanding of the exciton fine structure in 2D perovskites and demonstrates the cavity control of highly anisotropic and polarization-sensitive exciton polaritons.

cond-mat.mes-hall↗

arXiv2024

Infrared magneto-polaritons in MoTe$_2$ mono- and bilayers

MoTe$_2$ monolayers and bilayers are unique within the family of van-der-Waals materials since they pave the way towards atomically thin infrared light-matter quantum interfaces, potentially reaching the important telecommunication windows. Here, we report emergent exciton-polaritons based on MoTe$_2$ monolayer and bilayer in a low-temperature open micro-cavity in a joint experiment-theory study. Our experiments clearly evidence both the enhanced oscillator strength and enhanced luminescence of MoTe$_2$ bilayers, signified by a 38 \% increase of the Rabi-splitting and a strongly enhanced relaxation of polaritons to low-energy states. The latter is distinct from polaritons in MoTe$_2$ monolayers, which feature a bottleneck-like relaxation inhibition. Both the polaritonic spin-valley locking in monolayers and the spin-layer locking in bilayers are revealed via the Zeeman effect, which we map and control via the light-matter composition of our polaritonic resonances.

cond-mat.mes-hall↗

arXiv2024

Revealing dark exciton signatures in polariton spectra of 2D materials

Dark excitons in transition metal dichalcogenides (TMD) have been so far neglected in the context of polariton physics due to their lack of oscillator strength. However, in tungsten-based TMDs, dark excitons are known to be the energetically lowest states and could thus provide important scattering partners for polaritons. In this joint theory-experiment work, we investigate the impact of the full exciton energy landscape on polariton absorption and reflectance. By changing the cavity detuning, we vary the polariton energy relative to the unaffected dark excitons in such a way that we open or close specific phonon-driven scattering channels. We demonstrate both in theory and experiment that this controlled switching of scattering channels manifests in characteristic sharp changes in optical spectra of polaritons. These spectral features can be exploited to extract the position of dark excitons. Our work suggests new possibilities for exploiting polaritons for fingerprinting nanomaterials via their unique exciton landscape.

cond-mat.mes-hall↗

arXiv2024

Circumventing the polariton bottleneck via dark excitons in 2D semiconductors

Efficient scattering into the exciton polariton ground state is a key prerequisite for generating Bose-Einstein condensates and low-threshold polariton lasing. However, this can be challenging to achieve at low densities due to the polariton bottleneck effect that impedes phonon-driven scattering into low-momentum polariton states. The rich exciton landscape of transition metal dichalcogenides (TMDs) provides potential intervalley scattering pathways via dark excitons to rapidly populate these polaritons. Here, we present a microscopic study exploring the time- and momentum-resolved relaxation of exciton polaritons supported by a \ce{MoSe2} monolayer integrated within a Fabry-Perot cavity. By exploiting phonon-assisted transitions between momentum-dark excitons and the lower polariton branch, we demonstrate that it is possible to circumvent the bottleneck region and efficiently populate the polariton ground state. Furthermore, this intervalley pathway is predicted to give rise to, yet unobserved, angle-resolved phonon sidebands in low-temperature photoluminescence spectra that are associated with momentum-dark excitons. This represents a distinctive experimental signature for efficient phonon-mediated polariton-dark-exciton interactions.

cond-mat.mes-hall↗

arXiv2022

Interlayer exciton polaritons in homobilayers of transition metal dichalcogenides

Transition metal dichalcogenides integrated within a high-quality microcavity support well-defined exciton polaritons. While the role of intralayer excitons in 2D polaritonics is well studied, interlayer excitons have been largely ignored due to their weak oscillator strength. Using a microscopic and material-realistic Wannier-Hopfield model, we demonstrate that MoS$_2$ homobilayers in a Fabry-Perot cavity support polaritons that exhibit a large interlayer exciton contribution, while remaining visible in linear optical spectra. Interestingly, with suitable tuning of the cavity length, the hybridization between intra- and interlayer excitons can be 'unmixed' due to the interaction with photons. We predict formation of polaritons where > 90% of the total excitonic contribution is stemming from the interlayer exciton. Furthermore, we explore the conditions on the tunneling strength and exciton energy landscape to push this to even 100%. Despite the extremely weak oscillator strength of the underlying interlayer exciton, optical energy can be effectively fed into the polaritons once the critical coupling condition of balanced radiative and scattering decay channels is met. These findings have a wide relevance for fields ranging from nonlinear optoelectronic devices to Bose-Einstein condensation.

cond-mat.mes-hall↗

arXiv2022

Exciton optics, dynamics and transport in atomically thin semiconductors

Atomically thin semiconductors such as transition metal dichalcogenide (TMD) monolayers exhibit a very strong Coulomb interaction, giving rise to a rich exciton landscape. This makes these materials highly attractive for efficient and tunable optoelectronic devices. In this article, we review the recent progress in the understanding of exciton optics, dynamics and transport, which crucially govern the operation of TMD-based devices. We highlight the impact of hBN-encapsulation, which reveals a plethora of many-particle states in optical spectra, and we outline the most novel breakthroughs in the field of exciton-polaritonics. Moreover, we underline the direct observation of exciton formation and thermalization in TMD monolayers and heterostructures in recent time-resolved ARPES studies. We also show the impact of exciton density, strain and dielectric environment on exciton diffusion and funneling. Finally, we put forward relevant research directions in the field of atomically thin semiconductors for the near future.

cond-mat.mes-hall↗

arXiv2022

Signatures of dark excitons in exciton-polariton optics of transition metal dichalcogenides

Integrating 2D materials into high-quality optical microcavities opens the door to fascinating many-particle phenomena including the formation of exciton-polaritons. These are hybrid quasi-particles inheriting properties of both the constituent photons and excitons. In this work, we investigate the so-far overlooked impact of dark excitons on the momentum-resolved absorption spectra of hBN-encapsulated WSe$_2$ and MoSe$_2$ monolayers in the strong-coupling regime. In particular, thanks to the efficient phonon-mediated scattering of polaritons into energetically lower dark exciton states, the absorption of the lower polariton branch in WSe$_2$ is much higher than in MoSe$_2$. It shows unique step-like increases in the momentum-resolved profile indicating opening of specific scattering channels. We study how different externally accessible quantities, such as temperature or mirror reflectance, change the optical response of polaritons. Our study contributes to an improved microscopic understanding of exciton-polaritons and their interaction with phonons, potentially suggesting experiments that could determine the energy of dark exciton states via momentum-resolved polariton absorption.

cond-mat.mes-hall↗

arXiv2022

Twist Angle Tuning of Moiré Exciton Polaritons in van der Waals Heterostructures

Twisted atomically thin semiconductors are characterized by moiré excitons. Their optical signatures and selection rules are well understood. However, their hybridization with photons in the strong coupling regime for heterostructures integrated in an optical cavity has not been in the focus of research yet. Here, we combine an excitonic density matrix formalism with a Hopfield approach to provide microscopic insights into moiré exciton polaritons. In particular, we show that exciton-light coupling, polariton energy, and even the number of polariton branches can be controlled via the twist angle. We find that these new hybrid light-exciton states become delocalized relative to the constituent excitons due to the mixing with light and higher-energy excitons. The system can be interpreted as a natural quantum metamaterial with a periodicity that can be engineered via the twist angle. Our study presents a significant advance in microscopic understanding and control of moiré exciton polaritons in twisted atomically thin semiconductors.

cond-mat.mes-hall↗

arXiv2020

Suspended photonic crystal membranes in AlGaAs heterostructures for integrated multi-element optomechanics

We present high-reflectivity mechanical resonators fabricated from AlGaAs heterostructures for use in free-space optical cavities operating in the telecom wavelength regime. The mechanical resonators are fabricated in slabs of GaAs and patterned with a photonic crystal to increase their out-of-plane reflectivity. Characterization of the mechanical modes reveals residual tensile stress in the GaAs device layer. This stress results in higher mechanical frequencies than in unstressed GaAs and can be used for strain engineering of mechanical dissipation. Simultaneously, we find that the finite waist of the incident optical beam leads to a dip in the reflectance spectrum. This feature originates from coupling to a guided resonance of the photonic crystal, an effect that must be taken into account when designing slabs of finite size. The single- and sub-$\upmu$m-spaced double-layer slabs demonstrated here can be directly fabricated on top of a distributed Bragg reflector mirror in the same material platform. Such a platform opens a route for realizing integrated multi-element cavity optomechanical devices and optomechanical microcavities on chip.

physics.app-ph↗

arXiv2020

Cavity Optomechanics with Photonic Bound States in the Continuum

We propose a versatile, free-space cavity optomechanics platform built from two photonic crystal membranes, one of which is freely suspended, and designed to form a microcavity less than one wavelength long. This cavity features a series of photonic bound states in the continuum that, in principle, trap light forever and can be favorably used together with evanescent coupling for realizing various types of optomechanical couplings, such as linear or quadratic coupling of either dispersive or dissipative type, by tuning the photonic crystal patterning and cavity length. Crucially, this platform allows for a quantum cooperativity exceeding unity in the ultrastrong single-photon coupling regime, surpassing the performance of conventional Fabry-Perot-based cavity optomechanical devices in the non-resolved sideband regime. This conceptually novel platform allows for exploring new regimes of the optomechanical interaction, in particular in the framework of pulsed and single-photon optomechanics.

quant-ph↗

arXiv2017

Battling Retardation And Nonlocality: The hunt For The Ultimate Plasmonic Cascade Nanolens

We perform a study of the achievable field enhancement of plasmonic cascade nanolenses in the quantum and classical regimes, and explore the limits enforced at larger sizes by retardation and at smaller sizes by nonlocality and other quantum effects. We compare the near field response of a sodium nanolens within a local and nonlocal formalism and find that the increased electron- surface scattering decreases the field enhancements by over an order of magnitude. The large parameter space is explored, within the local approximation, for a number of plasmonic metals as well as the polar dielectric SiC. Using localised surface phonon polaritons, which can be excited in polar dielectrics, is an effective strategy for overcoming retardation due to the lower energy phonon frequency. Finally, we compare the nanolens against the more usual dimer configuration, we find that the superior geometry depends crucially on the material used, with noble metal nanolenses unlikely to offer better performance to equivalent dimers. Interestingly SiC nanolenses can offer a larger maximum field enhancement compared to the corresponding dimer configuration, suggesting that future endeavours in constructing a nanolens should be based on polar dielectrics.

physics.optics↗

arXiv2017

Quantum Plasmonic Nanoantennas

We study plasmonic excitations in the limit of few electrons, in one-atom thick sodium chains, and characterize them based on collectivity. We also compare the excitations to classical localised plasmon modes and find for the longitudinal mode a quantum-classical transition around 10 atoms. The transverse mode appears at much higher energies than predicted classically for all chain lengths. The electric field enhancement is also considered which is made possible by considering the effects of electron-phonon coupling on the broadening of the electronic spectra. Large field enhancements are possible on the molecular level allowing us to consider the validity of using molecules as the ultimate small size limit of plasmonic antennas. Additionally, we consider the case of a dimer system of two sodium chains, where the gap can be considered as a picocavity, and we analyse the charge-transfer states and their dependence on the gap size as well as chain size. Our results and methods are useful for understanding and developing ultra-small, tunable and novel plasmonic devices that utilise quantum effects that could have applications in quantum optics, quantum metamaterials, cavity-quantum electrodynamics and controlling chemical reactions, as well as deepening our understanding of localised plasmons in low dimensional molecular systems.

cond-mat.mes-hall↗