arXiv subjects

Andrea Mancini

Publications and source records attributed to Andrea Mancini.

12 recordsLinked to original sources

arXiv2026

Ultrafast Control of Lifetime in High Q Anisotropic Plasmon Polaritons

Losses are a major roadblock in the technological implementation of surface plasmons at optical frequencies. The recent emergence of MoOCl2, a correlated van-der-Waals material with strongly anisotropic optical properties, offers new avenues to circumvent this limit. We report the far-field observation of high-Q surface plasmon polaritons in this material, arising from the anisotropic hybridisation of surface plasmons and dielectric modes. We then explore nonlinear pumping of intraband electrons to the conduction band in these structures, leading, contrary to intuition, to an abrupt increase in the lifetime of the polariton resonance, despite the injection of hot electrons. This counterintuitive phenomenon stems from the competition between photon and plasmon excitations in a lenticular polariton resonance, yielding a largely tuneable lifetime at ultrafast speeds.

physics.optics↗

arXiv2026

Intrinsic plasmon canalization in the biaxial van der Waals crystal MoOCl$_2$

Anisotropic polaritons in low-symmetry crystals allow for subwavelength confinement and directional routing of light. The most extreme form of such anisotropy arises at the topological transition between elliptical and hyperbolic dispersion, where the isofrequency contours collapse into parallel lines and polaritons propagate in a diffractionless, beam-like fashion. This canalization regime has previously been accessed through twisted heterostructures or engineered metasurfaces. Here we show that natural canalization can be achieved without any fabrication or structuring by exploiting the intrinsic elliptical-to-hyperbolic transition in the van der Waals crystal MoOCl$_2$ at room temperature. Using near-field imaging, we directly visualize plasmon-polariton canalization emerging at the low-loss Drude crossing point along the [010] crystal axis. Owing to the moderate slope of the Drude permittivity, the resulting polaritons remain highly directional across a broad spectral window. This weak dispersion also enables robust thickness-dependent tuning, and we demonstrate, both experimentally and theoretically, that the canalization wavelength can be adjusted by more than 1 {\mu}m simply by varying the flake thickness. This work brings canalized polariton propagation into the 4.5 - 6 {\mu}m range, beyond the frequency limits of phonon-polariton platforms and overlapping with important molecular vibrations, opening new opportunities for mid-IR nanophotonics and sensing.

physics.optics↗

arXiv2026

Phonon-polaritonic skyrmions: Transition from bubble- to N\'eel-type

Optical skyrmions are members of the emerging topological branch of solid-state physics and photonics, allowing for control over topological light textures through light-matter interactions. However, in nanophotonics their practical application has been severely limited by high inherent losses in plasmonic materials, resulting in the lack of tunability between different topological properties. Here, we utilize the strong dispersion of silicon carbide thin films to realize highly confined surface phonon-polariton skyrmion lattices, which we image via near-field microscopy. We experimentally demonstrate topological tuning between bubble- and N\'eel-type skyrmions, a unique advantage that polar dielectrics offer over most existing approaches. Changing the excitation wavelength by only 10% switches the skyrmion type, revealed by examination of the skyrmion number density contrast. Analysis of domain wall size and steepness in analogy to magnetic materials also confirms this transition. Our results are a starting point to investigate other topological features in phononic systems such as merons, skyrmion bags, and other complex structured light fields. Furthermore, strong light-matter hybridization and nonlinear effects owing to anharmonicity of the phonons may be observed in the future, possibly leading towards the discovery of polaritonic skyrmion-skyrmion interactions and hence applications in topology-based information processing.

physics.optics↗

arXiv2026

Anisotropic electron gas in a hyperbolic van der Waals material

Electron gases in low dimensional materials exhibit unconventional transport and optical phenomena due to reduced phase space, enhanced interactions, and strong sensitivity to lattice symmetry. While commonly realized in quantum confined systems and engineered heterostructures, such states are rare in naturally occurring materials. Hyperbolic materials provide a compelling alternative, as extreme lattice anisotropy can host unconventional electronic states and novel electron-phonon interactions. Here, we investigate the angle resolved polarized Raman (ARPR) response of MoOCl2, the first naturally occurring hyperbolic material whose hyperbolicity originates from a highly anisotropic electron gas. We observe pronounced polarization dependent Fano line shapes, revealing coherent coupling between phonons and an anisotropic electronic continuum. We characterize the directional response of this continuum, incorporating it into effective Raman tensors that quantitatively reproduce the ARPR measurements and capture the distinct Raman fingerprint of MoOCl2. Excitation energy and thickness dependent ARPR measurements further demonstrate a tunable quasi 1D electronic continuum with weak interlayer coupling, establishing MoOCl2 as a model system for Raman studies of electron-phonon coupling in hyperbolic materials

cond-mat.mes-hall↗

arXiv2024

Visible-frequency hyperbolic plasmon polaritons in a natural van der Waals crystal

Controlling light at subwavelength scales is one of the main challenges of nanophotonics. Leveraging hyperbolic polaritons supporting arbitrarily large wavevectors can lead to extreme light confinement, effectively overcoming the diffraction limit. Hyperbolicity was initially realized in artificial metamaterials, but their performances are limited by high losses in the metallic components. While recently discovered natural low-loss hyperbolic phonon polaritons initiated a revival in the interest for hyperbolic materials, they are confined to the mid-infrared frequency range, limiting their use for several applications. Some hyperbolic materials at visible frequencies have been studied, but they are either very lossy or only feature out-of-plane hyperbolicity. Here, we demonstrate the presence of low-loss, in-plane hyperbolic plasmon polaritons in the visible and near-infrared in thin films of $\mathrm{MoOCl}_2$, a natural van der Waals crystal. The polariton dispersion is predicted based on the framework of light propagation in biaxial media, and experimentally confirmed by real space nano imaging on exfoliated flakes. $\mathrm{MoOCl}_2$ constitutes a novel material platform for visible-range applications leveraging the unboundedness of hyperbolic modes, such as hyperlensing, Purcell factor enhancement and super-resolution imaging, without the drawbacks of metamaterials.

physics.optics↗

arXiv2024

Revealing mode formation in quasi-bound states in the continuum metasurfaces via near-field optical microscopy

Photonic metasurfaces offer exceptional control over light at the nanoscale, facilitating applications spanning from biosensing, and nonlinear optics to photocatalysis. Many metasurfaces, especially resonant ones, rely on periodicity for the collective mode to form, which makes them subject to the influences of finite size effects, defects, and edge effects, all of which have considerable negative impact at the application level. These aspects are especially important for quasi-bound state in the continuum (BIC) metasurfaces, for which the collective mode is highly sensitive to perturbations due to high quality factors and strong near-field enhancement. Here, we quantitatively investigate the mode formation in quasi-BIC metasurfaces on the individual resonator level using scattering scanning near-field optical microscopy (s-SNOM) in combination with a new image processing technique. We find that the quasi-BIC mode is formed at a minimum size of 10 x 10-unit cells much smaller than expected from far-field measurements. Furthermore, we show that the coupling direction of the resonators, defects and edge states have pronounced influence on the quasi-BIC mode. This study serves as a link between the far-field and near-field responses of metasurfaces, offering crucial insights for optimizing spatial footprint and active area, holding promise for augmenting applications such as catalysis and biospectroscopy.

physics.optics↗

arXiv2024

Highly confined incident-angle-robust surface phonon polariton bound states in the continuum metasurfaces

Squeezing light into subwavelength dimensions is vital for on-chip integration of photonic technologies. One approach to overcome the diffraction limit is coupling light to material excitations, leading to polariton states. Here, we showcase how low-loss mid-infrared surface phonon polaritons enable metasurfaces supporting quasi-bound states in the continuum (qBICs) with deeply subwavelength unit cells. Utilizing 100 nm thick free-standing silicon carbide membranes, we achieve highly confined qBIC states with a unit cell volume ~ 10^4 times smaller than the diffraction limit. This results in remarkable robustness of the platform against the incident angle that is unique among qBIC systems. We also demonstrate vibrational strong coupling with a thin layer of spin-coated molecules, leveraging the small mode volume. This work introduces phononic qBICs as a novel ultra-confined nanophotonic platform, paving a way for the miniaturization of mid-infrared devices for molecular sensing and thermal radiation engineering.

physics.optics↗

arXiv2023

Multiplication of the orbital angular momentum of phonon polaritons via sublinear dispersion

Optical vortices (OVs) promise to greatly enhance optical information capacity via orbital angular momentum (OAM) multiplexing. The need for on-chip integration of OAM technologies has prompted research into subwavelength-confined polaritonic OVs. However, the topological order imprinted by the structure used for the transduction from free-space beams to surface polaritons is inherently fixed after fabrication. Here, we overcome this limitation via dispersion-driven topological charge multiplication. We switch the OV topological charge within a small $\sim 3 \%$ frequency range by leveraging the strong sublinear dispersion of low-loss surface phonon polaritons (SPhP) on silicon carbide membranes. Applying the Huygens principle we quantitatively evaluate the topological order of the experimental OVs detected by near-field imaging. We further explore the deuterogenic effect, which predicts the coexistence of multiple topological charges in higher-order polaritonic OVs. Our work demonstrates a viable method to manipulate the topological charge of polaritonic OVs, paving the way for the exploration of novel OAM-enabled light-matter interactions at mid-infrared frequencies.

physics.optics↗

arXiv2021

Second harmonic generation in germanium quantum wells for nonlinear silicon photonics

Second-harmonic generation (SHG) is a direct measure of the strength of second-order nonlinear optical effects, which also include frequency mixing and parametric oscillations. Natural and artificial materials with broken center-of-inversion symmetry in their unit cell display high SHG efficiency, however the silicon-foundry compatible group-IV semiconductors (Si, Ge) are centrosymmetric, thereby preventing full integration of second-order nonlinearity in silicon photonics platforms. Here we demonstrate strong SHG in Ge-rich quantum wells grown on Si wafers. The symmetry breaking is artificially realized with a pair of asymmetric coupled quantum wells (ACQW), in which three of the quantum-confined states are equidistant in energy, resulting in a double resonance for SHG. Laser spectroscopy experiments demonstrate a giant second-order nonlinearity at mid-infrared pump wavelengths between 9 and 12 microns. Leveraging on the strong intersubband dipoles, the nonlinear susceptibility almost reaches 10^5 pm/V

physics.optics↗

arXiv2019

Pump-probe Spectroscopy Study of Ultrafast Temperature Dynamics in Nanoporous Gold

We explore the influence of the nanoporous structure on the thermal relaxation of electrons and holes excited by ultrashort laser pulses ($\sim 7$ fs) in thin gold films. Plasmon decay into hot electron-hole pairs results in the generation of a Fermi-Dirac distribution thermalized at a temperature $T_{\mathrm{e}}$ higher than the lattice temperature $T_{\mathrm{l}}$. The relaxation times of the energy exchange between electrons and lattice, here measured by pump-probe spectroscopy, is slowed down by the nanoporous structure, resulting in much higher peak $T_{\mathrm{e}}$ than for bulk gold films. The electron-phonon coupling constant and the Debye temperature are found to scale with the metal filling factor $f$ and a two-temperature model reproduces the data. The results open the way for electron temperature control in metals by engineering of the nanoporous geometry.

cond-mat.mtrl-sci↗

arXiv2018

Surface Thermal Gradients Activated by Enhanced Molecular Absorption in Mid-infrared Vertical Antenna Arrays

We investigate local heat generation by molecules at the apex of polymer-embedded vertical antennas excited at resonant mid-infrared wavelengths, exploiting the surface enhanced infrared absorption (SEIRA) effect. The embedding of vertical nanoantennas in a non-absorbing polymer creates thermal isolation between the apical hotspot, the locus of heat generation, and the heat sink represented by the substrate. Vibrational mid-infrared absorption by strongly absorbing molecules located at the antenna apex then generates nanoscale temperature gradients at the surface. We imaged the thermal gradients by using a nano-photothermal expansion microscope, and we found values up to 10 K/microm in conditions where the radiation wavelength resonates with both the molecule vibrations and the plasmonic mode of the antennas. Values up to 1000 K/microm can be foreseen at maximum quantum cascade laser power. The presented system provides a promising thermoplasmonic platform for antenna-assisted thermophoresis and resonant mid-infrared photocatalysis.

physics.app-ph↗

arXiv2018

Thermoplasmonic Effect of Surface Enhanced Infrared Absorption in Vertical Nanoantenna Arrays

The temperature increase and temperature gradients induced by mid-infrared laser illumination of vertical gold nanoantenna arrays embedded into polymer layers was measured directly with a photothermal expansion nanoscope. Nanoscale thermal hotspot images and local temperature increase spectra were both obtained, the latter by broadly tuning the emission wavelength of a quantum cascade laser. The spectral analysis indicates that plasmon-enhanced mid-infrared vibrations of molecules located in the antenna hotspots are responsible for some of the thermoplasmonic resonances, while Joule heating in gold is responsible for the remaining resonances. In particular, plasmonic dark modes with low scattering cross-section mostly produce surface-enhanced infrared absorption (SEIRA), while bright modes with strong radiation coupling produce Joule heating. The dark modes do not modify the molecular absorption lineshape and the related temperature increase is chemically triggered by the presence of molecules with vibrational fingerprints resonant with the plasmonic dark modes. The bright modes, instead, are prone to Fano interference, display an asymmetric molecular absorption lineshape and generate heat also at frequencies far from molecular vibrations, insofar lacking chemical specificity. For focused mid-infrared laser power of 50 mW, the measured nanoscale temperature increases are in the range of 10 K and temperature gradients reach 5 K/$μ$m in the case of dark modes resonating with strong infrared vibrations such as the C=O bond of poly-methylmethacrylate at 1730 cm$^{-1}$.

physics.app-ph↗