arXiv subjects

Armando Genco

Publications and source records attributed to Armando Genco.

18 recordsLinked to original sources

arXiv2026

Excitonic Mott transition without population inversion

Exciton dissociation via the excitonic Mott transition (EMT) governs the high-density optical response of semiconductors and sets fundamental limits for optoelectronic devices. The EMT is conventionally linked to the onset of population inversion and the emergence of optical gain. Here, we demonstrate that this paradigm can break down under ultrafast non-equilibrium excitation. Using femtosecond pump-probe optical spectroscopy, we drive a monolayer transition metal dichalcogenide into a dense photoexcited state in which the excitonic resonance is completely quenched within ~100 fs, while the optical gain is entirely absent across the explored fluence range. State-of-the-art real-time ab initio simulations reveal that the EMT is governed by an interplay of strongly nonthermal carrier populations and nonequilibrium dynamical screening of the Coulomb interaction. The quantitative agreement between theory and experiment identifies a distinct, ultrafast pathway to exciton ionization beyond quasi-equilibrium descriptions and demonstrates that population inversion is not a universal prerequisite for the EMT.

cond-mat.mes-hall↗

arXiv2025

Integration of 2D Materials in Radial van der Waals Heterostructure Metasurfaces

Two-dimensional semiconductors, such as monolayer transition metal dichalcogenides (TMDC), exhibit strong excitonic transitions at room temperature and offer a unique platform for exploring light-matter interactions in nanoscale photonic systems. In this work, we demonstrate a compact and polarization-invariant photonic metasurface, fabricated from hexagonal boron-nitride (hBN) and based on radial bound states in the continuum (BIC), which are formed by radially distributed pairs of structurally asymmetric resonators. The metasurface employs multiple symmetry-breaking perturbations to support high quality-(Q-)factor resonances within a footprint smaller than 8 x 8 $\mu m^2$ - one-sixth of the area of previous approaches. Compared to established hBN metasurface designs, the radial geometry furthermore achieves significantly higher Q-factors with a reduced footprint. By integrating the hBN photonic structure with a WS$_2$ monolayer, we observe enhanced photoluminescence when its resonance is spectrally aligned with the exciton resonance, accompanied by signatures of discrete momentum-space patterns that identify the orbital-angular-momentum-carrying ring eigenmodes. These features persist over a wide range of excitation powers and show minimal linewidth broadening, indicating robust and spatially modulated exciton-photon coupling. This work establishes a scalable approach for generating hybrid photonic-excitonic states with momentum-space structure, offering new opportunities for exciton localization, valley emission, spatially programmable light-matter interaction in two-dimensional material platforms and compact luminescent devices based on 2D material-integrated metasurfaces.

physics.optics↗

arXiv2025

Spin injection and emission helicity switching in a 2D perovskite/WSe2 heterostructure

The initialization and control of a long-lived spin population in lead halide perovskites are prerequisites for their use in spintronic applications. Here, we demonstrate circular polarization of the interlayer exciton emission in a (BA)2PbI4/WSe2 monolayer heterostructure. The helicity of this emission is controlled by tuning the energy of the excitation laser through the manifold of exciton resonances of the WSe2 monolayer, together with an emerging interlayer absorption feature of the heterostructure. Theoretical calculations show that this resonance arises from hybridized (BA)2PbI4/WSe2 states in the valence band. This hybrid character enables its observation in both linear absorption and ultrafast pump-probe spectroscopies, and plays a key role in controlling the sign of the helicity of the interlayer exciton emission. The tunable spin polarization demonstrated here, with the WSe2 monolayer effectively acting as a tunable spin filter, represents an important step toward the use of 2D perovskites in opto-spintronic applications.

cond-mat.mtrl-sci↗

arXiv2025

Ultrafast dynamics of coherent exciton-polaritons in van der Waals semiconductor metasurfaces

Enabling coherent light-matter interactions is a critical step toward next-generation quantum technologies. However, achieving this under ambient temperature conditions remains challenging due to rapid dephasing in optically excited systems. Optical metasurfaces based on quasi-bound states in the continuum have recently emerged as a powerful platform for reaching the strong light-matter coupling regime in flat, subwavelength thickness devices. Here, we investigate ultrafast exciton-polariton dynamics in self-hybridized WS$_2$ thin-film metasurfaces. Using hyperspectral momentum-resolved imaging, we reconstruct the highly anisotropic exciton-polariton dispersion, with a transition from positive to negative effective mass along orthogonal symmetry axes. Femtosecond pump-probe and multidimensional spectroscopy reveal detuning-dependent polariton dynamics with a coherence time up to ~110 fs, and allow direct observation of the coherent dynamics through ultrafast Rabi oscillations with ~45 fs period. We describe this behaviour with a three-eigenstate model that couples the photonic resonance with both bright and dark excitons, extending the conventional two-state picture of strong coupling. Our results establish van der Waals metasurfaces as a promising platform for next-generation polaritonic devices, enabling coherent quantum transfer of matter excitations at room temperature.

physics.optics↗

arXiv2025

Electrically tunable ultrafast dynamics and interactions of hybrid excitons in a 2D semiconductor bilayer

Extended efforts have been devoted to the study of strongly-interacting excitons and their dynamics, towards macroscopic quantum states of matter such as Bose-Einstein condensates of excitons and polaritons. Momentum-direct layer-hybridized excitons in transition metal dichalcogenides have attracted considerable attention due to their high oscillator strength and dipolar nature. However, the tunability of their interactions and dynamics remains unexplored. Here, we achieve an unprecedented control over the nonlinear properties of dipolar layer-hybridized excitons in an electrically gated van der Waals homobilayer monitored by transient optical spectroscopy. By applying a vertical electric field, we reveal strong Coulomb interactions of dipolar hybrid excitons, leading to opposite density-dependent energy shifts of the two main hybrid species based on their dipolar orientation, together with a strongly enhanced optical saturation of their absorption. Furthermore, by electrically tuning the interlayer tunneling between the hybridized carriers, we significantly extend the formation time of hybrid excitons, while simultaneously increasing their decay times. Our findings have implications for the search on quantum blockade and condensation of excitons and dipolaritons in two-dimensional materials.

cond-mat.mes-hall↗

arXiv2025

Topological Control of Polaritonic Flatbands in Anisotropic van der Waals Metasurfaces

Anisotropic van der Waals (vdW) materials exhibit direction-dependent optical and electronic properties, making them valuable for tailoring directional light-matter interactions. Rhenium disulfide (ReS$_2$) stands out for its strong in-plane anisotropy and its thickness-independent direct-bandgap excitons, which can hybridize with light to form exciton-polaritons. In parallel, metasurfaces, engineered arrays of nanoscale subwavelength resonators, can support ultra-sharp photonic modes in the form of quasi-bound states in the continuum (qBICs). Topological transformations of photonic modes can give rise to flatbands, i.e., dispersionless states with quenched kinetic energy and vanishing group velocity. Intrinsic material anisotropy offers an unexplored route to robust far-field flatband formation and control. Here, we demonstrate how structuring an intrinsically anisotropic excitonic material into a resonant metasurface fundamentally transforms its photonic topological features and light-matter coupling behavior, allowing us to drive and topologically control extended far-field flatband formation. To this end, we fabricate C$_4$-symmetric metasurfaces directly from bulk ReS$_2$. The intrinsic anisotropy lifts the initial double degeneracy of the qBIC mode and yields two distinctly polarized resonances. It also reshapes the topological landscape: the integer topological charge of the qBIC mode splits into momentum-separated half-integer singularities, thereby flattening the far-field photonic dispersion. The resulting topologically-controlled photonic flatbands are then tuned in resonance with the linearly polarized excitonic transitions of ReS$_2$, resulting in two distinct, directionally hybridized exciton-polariton flatband regimes. These findings establish anisotropic vdW metasurfaces as a new platform for topologically engineered flatbands and flatband-driven light-matter coupling.

physics.optics↗

arXiv2025

Roadmap for Photonics with 2D Materials

Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combination with layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary collection of those directions, where 2D materials contribute with polaritons of unique characteristics such as strong spatial confinement, large optical-field enhancement, long lifetimes, high sensitivity to external stimuli (e.g., electric and magnetic fields, heating, and strain), a broad spectral range from the far infrared to the ultraviolet, and hybridization with spin and momentum textures of electronic band structures. The explosion of photonics with 2D materials as a vibrant research area is producing breakthroughs, including the discovery and design of new materials and metasurfaces with unprecedented properties as well as applications in integrated photonics, light emission, optical sensing, and exciting prospects for applications in quantum information, and nanoscale thermal transport. This Roadmap summarizes the state of the art in the field, identifies challenges and opportunities, and discusses future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

cond-mat.mtrl-sci↗

arXiv2024

Femtosecond switching of strong light-matter interactions in microcavities with two-dimensional semiconductors

Ultrafast all-optical logic devices based on nonlinear light-matter interactions hold the promise to overcome the speed limitations of conventional electronic devices. Strong coupling of excitons and photons inside an optical resonator enhances such interactions and generates new polariton states which give access to unique nonlinear phenomena, such as Bose-Einstein condensation, used for all-optical ultrafast polariton transistors. However, the pulse energies required to pump such devices range from tens to hundreds of pJ, making them not competitive with electronic transistors. Here we introduce a new paradigm for all-optical switching based on the ultrafast transition from the strong to the weak coupling regime in microcavities embedding atomically thin transition metal dichalcogenides. Employing single and double stacks of hBN-encapsulated MoS$_2$ homobilayers with high optical nonlinearities and fast exciton relaxation times, we observe a collapse of the 55-meV polariton gap and its revival in less than one picosecond, lowering the threshold for optical switching below 4 pJ per pulse, while retaining ultrahigh switching frequencies. As an additional degree of freedom, the switching can be triggered pumping either the intra- or the interlayer excitons of the bilayers at different wavelengths, speeding up the polariton dynamics, owing to unique interspecies excitonic interactions. Our approach will enable the development of compact ultrafast all-optical logical circuits and neural networks, showcasing a new platform for polaritonic information processing based on manipulating the light-matter coupling.

physics.optics↗

arXiv2023

Resonant band hybridization in alloyed transition metal dichalcogenide heterobilayers

Bandstructure engineering using alloying is widely utilised for achieving optimised performance in modern semiconductor devices. While alloying has been studied in monolayer transition metal dichalcogenides, its application in van der Waals heterostructures built from atomically thin layers is largely unexplored. Here, we fabricate heterobilayers made from monolayers of WSe$_2$ (or MoSe$_2$) and Mo$_x$W$_{1-x}$Se$_2$ alloy and observe nontrivial tuning of the resultant bandstructure as a function of concentration $x$. We monitor this evolution by measuring the energy of photoluminescence (PL) of the interlayer exciton (IX) composed of an electron and hole residing in different monolayers. In Mo$_x$W$_{1-x}$Se$_2$/WSe$_2$, we observe a strong IX energy shift of $\approx$100 meV for $x$ varied from 1 to 0.6. However, for $x<0.6$ this shift saturates and the IX PL energy asymptotically approaches that of the indirect bandgap in bilayer WSe$_2$. We theoretically interpret this observation as the strong variation of the conduction band K valley for $x>0.6$, with IX PL arising from the K-K transition, while for $x<0.6$, the bandstructure hybridization becomes prevalent leading to the dominating momentum-indirect K-Q transition. This bandstructure hybridization is accompanied with strong modification of IX PL dynamics and nonlinear exciton properties. Our work provides foundation for bandstructure engineering in van der Waals heterostructures highlighting the importance of hybridization effects and opening a way to devices with accurately tailored electronic properties.

cond-mat.mtrl-sci↗

arXiv2023

Strong Coupling of Coherent Phonons to Excitons in Semiconducting Monolayer MoTe$_2$

The coupling of the electron system to lattice vibrations and their time-dependent control and detection provides unique insight into the non-equilibrium physics of semiconductors. Here, we investigate the ultrafast transient response of semiconducting monolayer 2$H$-MoTe$_2$ encapsulated with $h$BN using broadband optical pump-probe microscopy. The sub-40-fs pump pulse triggers extremely intense and long-lived coherent oscillations in the spectral region of the A' and B' exciton resonances, up to $\sim$20% of the maximum transient signal, due to the displacive excitation of the out-of-plane $A_{1g}$ phonon. Ab-initio calculations reveal a dramatic rearrangement of the optical absorption of monolayer MoTe$_2$ induced by an out-of-plane stretching and compression of the crystal lattice, consistent with an $A_{1g}$-type oscillation. Our results highlight the extreme sensitivity of the optical properties of monolayer TMDs to small structural modifications and their manipulation with light.

cond-mat.mes-hall↗

arXiv2022

Nonlinear interactions of dipolar excitons and polaritons in MoS2 bilayers

Nonlinear interactions between excitons strongly coupled to light are key for accessing quantum many-body phenomena in polariton systems. Atomically-thin two-dimensional semiconductors provide an attractive platform for strong light-matter coupling owing to many controllable excitonic degrees of freedom. Among these, the recently emerged exciton hybridization opens access to unexplored excitonic species, with a promise of enhanced interactions. Here, we employ hybridized interlayer excitons (hIX) in bilayer MoS2 to achieve highly nonlinear excitonic and polaritonic effects. Such interlayer excitons possess an out-of-plane electric dipole as well as an unusually large oscillator strength allowing observation of dipolar polaritons(dipolaritons) in bilayers in optical microcavities. Compared to excitons and polaritons in MoS2 monolayers, both hIX and dipolaritons exhibit about 8 times higher nonlinearity, which is further strongly enhanced when hIX and intralayer excitons, sharing the same valence band, are excited simultaneously. This gives rise to a highly nonlinear regime which we describe theoretically by introducing a concept of hole crowding. The presented insight into many-body interactions provides new tools for accessing few-polariton quantum correlations.

cond-mat.mes-hall↗

arXiv2021

Dielectric nano-antennas for strain engineering in atomically thin two-dimensional semiconductors

Atomically thin two-dimensional semiconducting transition metal dichalcogenides (TMDs) can withstand large levels of strain before their irreversible damage occurs. This unique property offers a promising route for control of the optical and electronic properties of TMDs, for instance by depositing them on nano-structured surfaces, where position-dependent strain can be produced on the nano-scale. Here, we demonstrate strain-induced modifications of the optical properties of mono- and bilayer TMD WSe$_2 $ placed on photonic nano-antennas made from gallium phosphide (GaP). Photoluminescence (PL) from the strained areas of the TMD layer is enhanced owing to the efficient coupling with the confined optical mode of the nano-antenna. Thus, by following the shift of the PL peak, we deduce the changes in the strain in WSe$_2$ deposited on the nano-antennas of different radii. In agreement with the presented theory, strain up to $\approx 1.4 \%$ is observed for WSe$_2$ monolayers. We also estimate that $>3\%$ strain is achieved in bilayers, accompanied with the emergence of a direct bandgap in this normally indirect-bandgap semiconductor. At cryogenic temperatures, we find evidence of the exciton confinement in the most strained nano-scale parts of the WSe$_2$ layers, as also predicted by our theoretical model. Our results, of direct relevance for both dielectric and plasmonic nano-antennas, show that strain in atomically thin semiconductors can be used as an additional parameter for engineering light-matter interaction in nano-photonic devices.

cond-mat.mes-hall↗

arXiv2021

Transition metal dichalcogenide dimer nano-antennas with ultra-small gaps

Transition metal dichalcogenides have emerged as promising materials for nano-photonic resonators due to their large refractive index, low absorption within a large portion of the visible spectrum and compatibility with a wide range of substrates. Here we use these properties to fabricate WS$_2$ double-pillar nano-antennas in a variety of geometries enabled by the anisotropy in the crystal structure. Using dark field spectroscopy, we reveal multiple Mie resonances, to which we couple WSe$_2$ monolayer photoluminescence and achieve Purcell enhancement and an increased fluorescence by factors up to 240. We introduce post-fabrication atomic force microscope repositioning and rotation of dimer nano-antennas, achieving gaps as small as 10$\pm$5 nm, opening the possibility to a host of potential applications including strong Purcell enhancement of single photon emitters and optical trapping, which we study in simulations. Our findings highlight the advantages of using transition metal dichalcogenides for nano-photonics by exploring new applications enabled by their unique properties.

physics.app-ph↗

arXiv2020

Strong Exciton-Photon Coupling in Large Area MoSe$_2$ and WSe$_2$ Heterostructures Fabricated from Two-Dimensional Materials Grown by Chemical Vapor Deposition

Two-dimensional semiconducting transition metal dichalcogenides embedded in optical microcavities in the strong exciton-photon coupling regime may lead to promising applications in spin and valley addressable polaritonic logic gates and circuits. One significant obstacle for their realization is the inherent lack of scalability associated with the mechanical exfoliation commonly used for fabrication of two-dimensional materials and their heterostructures. Chemical vapor deposition offers an alternative scalable fabrication method for both monolayer semiconductors and other two-dimensional materials, such as hexagonal boron nitride. Observation of the strong light-matter coupling in chemical vapor grown transition metal dichalcogenides has been demonstrated so far in a handful of experiments with monolayer molybdenum disulfide and tungsten disulfide. Here we instead demonstrate the strong exciton-photon coupling in microcavities comprising large area transition metal dichalcogenide / hexagonal boron nitride heterostructures made from chemical vapor deposition grown molybdenum diselenide and tungsten diselenide encapsulated on one or both sides in continuous few-layer boron nitride films also grown by chemical vapor deposition. These transition metal dichalcogenide / hexagonal boron nitride heterostructures show high optical quality comparable with mechanically exfoliated samples, allowing operation in the strong coupling regime in a wide range of temperatures down to 4 Kelvin in tunable and monolithic microcavities, and demonstrating the possibility to successfully develop large area transition metal dichalcogenide based polariton devices.

physics.optics↗

arXiv2017

Bright polariton OLEDs operating in the ultra-strong coupling regime

The generation and control of exotic phenomena in organic electroluminescent microcavities, such as polariton lasing and non-linear optical effects, operating in strong and ultra-strong coupling regimes, is still a great challenge. The main obstacles originate from the small number of molecular classes investigated as well as from the absence of an efficient strategy aiming at the maximization of polariton states population. Here we report on bright polariton organic light emitting diodes made of a coumarin fluorescent dye emitting layer, working in the ultra-strong coupling regime up to a coupling strength of 33%. Owing to a high radiative decay emission, a large Stokes shift and a fine cavity-exciton tuning, the radiative pumping mechanism of polariton states has been fully optimized, leading a large portion (25%) of the emissive electrically pumped excitons to be converted in polariton emission. The resulting polariton OLEDs showed electro-optical performances up to 0.2% of external quantum efficiency and 700 cd/m2 of luminance, corresponding to the highest values reported so far for this class of devices. Our work gives clear indications for an effective exploitation of organic polariton dynamics towards the development of novel quantum optoelectronic devices.

physics.app-ph↗

arXiv2016

Ultrafast flow of interacting organic polaritons

The strong-coupling of an excitonic transition with an electromagnetic mode results in composite quasi-particles called exciton-polaritons, which have been shown to combine the best properties of their bare components in semiconductor microcavities. However, the physics and applications of polariton flows in organic materials and at room temperature are still unexplored because of the poor photon confinement in such structures. Here we demonstrate that polaritons formed by the hybridization of organic excitons with a Bloch Surface Wave are able to propagate for hundreds of microns showing remarkable third-order nonlinear interactions upon high injection density. These findings pave the way for the studies of organic nonlinear light-matter fluxes and for a technological promising route of dissipation-less on-chip polariton devices working at room temperature.

physics.optics↗

arXiv2015

Localized surface resonances of J-aggregate nanostructures

Metallic nanostructures are able to concentrate light into volumes far below the diffraction limit. Here we show, by accurate scattering calculations, that nanostructures obtained from thin films of J-aggregate dyes, concentrate the electromagnetic field at optical frequencies. Moreover, in contrast to metal nanoparticles, these molecular aggregates display highly attractive nonlinear optical properties that can be exploited for the realization of ultracompact devices for switching light by light on the nanoscale without the need of additional nonlinear materials. These results open new perspectives in plasmonic based nanophotonics.

cond-mat.mes-hall↗

arXiv2014

Polariton Induced Enhanced Emission from an Organic Dye under Strong Coupling Regime

Exciton-polaritons in semiconductors are quasi-particles which have recently shown the capability to undergo phase transition into a coherent hybrid state of light and matter. The observation of such quasi-particles in organic microcavities has attracted increasing attention for their characteristic of reaching condensation at room temperature. In this work we demonstrate that the emission properties of organic polaritons do not depend on the overlap between the absorption and emission states of the molecule and that the emission dynamics are modified in the strong coupling regime, showing a significant enhancement of the photoluminescence intensity as compared to the bare dye. This paves the way to the investigation of molecules with large absorption coefficients but poor emission efficiencies for the realization of polariton condensates and organic electrically injected lasers by exploiting strong exciton-photon coupling regimes.

cond-mat.mes-hall↗