Search

In the strong-coupling regime, the interaction between light and matter reaches a hybridization state where the photonic and material components become inseparably linked. Using tailored states of light to break symmetries in such systems can underpin the development of novel non-equilibrium quantum materials. Chiral optical cavities offer a promising way for this, enabling either temporal or spatial symmetry-breaking, both of which are unachievable with conventional mirror cavities. For spatial symmetry-breaking a cavity needs to discriminate the handedness of circularly polarized light, a functionality that can only be achieved with metamaterials. Here, we suggest and demonstrate experimentally a chiral transition metal dichalcogenide (TMDC) metasurface with broken out-of-plane symmetry, allowing for a selective formation of self-hybridized exciton-polaritons with specific chirality. Our metasurface cavity maintains maximum chirality for oblique incidence up to 20{\deg}, significantly outperforming all previously known designs, thereby turning the angle of incidence from a constraint to a new degree of freedom for sub-nanometer precise control of resonance wavelengths. Moreover, we study the chiral strong-coupling regime in nonlinear experiments and show the polariton-driven nature of chiral third-harmonic generation. Our results demonstrate a clear pathway towards novel quantum material engineering with implications in a wide range of photonics research, such as superconductivity and valleytronics., Comment: 34 pages, 4 figures, and 12 supporting figures

Photonics has been revolutionized by breakthroughs in optical metasurfaces and layered two-dimensional materials. Yet, integrating these two fields in a singular system has remained challenging. Here, we introduce the concept of van der Waals (vdW) heterostructure metasurfaces, where ultrathin multilayer vdW material stacks are shaped into precisely engineered resonant nanostructures for boosting light-matter interactions. By leveraging quasi-bound states in the continuum to create intrinsic cavities from WS$_2$ monolayers encapsulated in hexagonal boron nitride, we observe room-temperature strong coupling and polaritonic luminescence, which further unveils a saturation of the strong-coupling regime at ultralow fluences <1 nJ/cm2, more than three orders of magnitude smaller than in previous 2D-cavity systems. Our approach, seamlessly merging metasurfaces and vdW materials, unlocks new avenues for ultrathin optical devices with atomic-scale precision and control., Comment: main + supplementary (28 pages, 4 main figures, 9 supplementary figures)

We studied the frequency and quality factor of mechanical plasmonic nanoresonators as a function of temperature, ranging from ambient to 4 K. Our investigation focused on individual gold nanorods and nanodisks of various sizes. We observed that oscillation frequencies increase linearly as temperature decreases until saturation is reached at cryogenic temperatures. This behavior is explained by the temperature dependence of the elastic modulus, with a Debye temperature compatible with reported bulk values for gold. To describe the behavior of the quality factor, we developed a model considering the nanostructures as anelastic solids, identifying a dissipation peak around 150 K due to a thermally activated process, likely of the Niblett-Wilks mechanism type. Importantly, our findings suggest that external dissipation factors are more critical to improving quality factors than internal friction, which can be increased by modifying the nanoresonator's environment. Our results enable the design of structures with high vibration frequencies and quality factors by effectively controlling external losses., Comment: Main text and supporting information, 18 pages, 6 figures

Dielectric metasurfaces supporting quasi-bound states in the continuum (qBICs) enable high field enhancement with narrow-linewidth resonances in the visible and near-infrared ranges. The resonance emerges when distorting the meta-atom's geometry away from a symmetry-protected BIC condition and, usually, a given design can sustain one or two of these states. In this work, we introduce a silicon-on-silica metasurface that simultaneously supports up to four qBIC resonances in the near-infrared region. This is achieved by combining multiple symmetry-breaking distortions on an elliptical cylinder array. By pumping two of these resonances, the nonlinear process of degenerate four-wave mixing is experimentally realized. By comparing the nonlinear response with that of an unpatterned silicon film, the near-field enhancement inside the nanostructured dielectric is revealed. The presented results demonstrate independent geometric control of multiple qBICs and their interaction trough wave mixing processes, opening new research pathways in nanophotonics, with potential applications in information multiplexing, multi-wavelength sensing and nonlinear imaging., Comment: 25 pages, 12 figures

Resonances are usually associated with finite systems - the vibrations of clamped strings in a guitar or the optical modes in a cavity defined by mirrors. In optics, resonances may be induced in infinite continuous media via periodic modulations of their optical properties. Here we demonstrate that periodic modulations of the permittivity of a featureless thin film can also act as a symmetry breaking mechanism, allowing the excitation of photonic $\textit{quasi}$-bound states in the continuum ($\textit{q}$BICs). By interfering two ultrashort laser pulses in the unbounded film, transient resonances can be tailored through different parameters of the pump beams. We show that the system offers resonances tunable in wavelength and quality-factor, and spectrally selective enhancement of third harmonic generation. Due to a fast decay of the permittivity asymmetry, we observe ultrafast dynamics, enabling time-selective near-field enhancement with picosecond precision. Optically-induced permittivity asymmetries may be exploited in on-demand weak to ultrastrong light-matter interaction regimes and light manipulation at dynamically chosen wavelengths in lithography-free metasurfaces.

Metasurfaces have unlocked significant advancements across photonics, yet their efficient active control remains challenging. The active materials required often lack continuous tunability, exhibit inadequate refractive index (RI) changes, or suffer from high losses. These aspects pose an inherent limitation for resonance-shifting based switching: when RI changes are small, the resulting shift is also minor. Conversely, high RI changes typically come with high intrinsic losses necessitating broad modes because narrow ones cannot tolerate such losses. Therefore, larger spectral shifts are required to effectively detune the modes. This paper introduces a novel active metasurface approach that converts the constraint of high intrinsic losses into a beneficial feature. This is achieved by controlling the losses in a hybrid vanadium dioxide (VO$_{2}$) - silicon metasurface, supporting symmetry-protected bound states in the continuum (BICs) within the infrared spectrum. By leveraging the temperature-controlled losses in VO$_{2}$ and combining them with the inherent far-field-coupling tunability of BICs, we gain unprecedented precision in independently controlling both the radiative and nonradiative losses of the resonant system. Our dual-control mechanism allows us to optimize our metasurfaces and we experimentally demonstrate quality factors above 200, a maximum reflectance amplitude of 90%, a relative switching contrast of 78%, and continuous tuning from under- to over-coupling within the infrared spectral range. This study provides a foundation for experimentally and technologically simple, fine-tunable, active metasurfaces for applications ranging from molecular sensors to filters and optical modulators., Comment: 25 pages, 4 figures, 4 supplementary figures

High-index Mie-resonant dielectric nanostructures provide a new framework to manipulate light at the nanoscale. In particular their local field confinement together with their inherently low losses at frequencies below their band-gap energy allows to efficiently boost and control linear and nonlinear optical processes. Here, we investigate nanoantennas composed of a thin indium-tin oxide layer in the center of a dielectric Gallium Phosphide nanodisk. While the linear response is similar to that of a pure GaP nanodisk, we show that the second and third-harmonic signals of the nanogap antenna are boosted at resonance. Linear and nonlinear finite-difference time-domain simulations show that the high refractive index contrast leads to strong field confinement inside the antenna's ITO layer. Measurement of ITO and GaP nonlinear susceptibilities deliver insight on how to engineer nonlinear nanogap antennas for higher efficiencies for future nanoscale devices., Comment: main: 18 pages, 4 figues, supplemental: 8 pages, 4 figures, 1 table

Two-dimensional (2D) semiconductors possess strongly bound excitons, opening novel opportunities for engineering light-matter interaction at the nanoscale. However, their in-plane confinement leads to large non-radiative exciton-exciton annihilation (EEA) processes, setting a fundamental limit for their photonic applications. In this work, we demonstrate suppression of EEA via enhancement of light-matter interaction in hybrid 2D semiconductor-dielectric nanophotonic platforms, by coupling excitons in WS$ _2 $ monolayers with optical Mie resonances in dielectric nanoantennas. The hybrid system reaches an intermediate light-matter coupling regime, with photoluminescence enhancement factors up to 10$ ^2 $. Probing the exciton ultrafast dynamics reveal suppressed EEA for coupled excitons, even under high exciton densities $>$ 10$^{12}$ cm$^{-2} $. We extract EEA coefficients in the order of 10$^{-3} $, compared to 10$^{-2} $ for uncoupled monolayers, as well as absorption enhancement of 3.9 and a Purcell factor of 4.5. Our results highlight engineering the photonic environment as a route to achieve higher quantum efficiencies for low-power hybrid devices, and larger exciton densities, towards strongly correlated excitonic phases in 2D semiconductors., Comment: Main text and supporting information, 32 pages, 4 Figures manuscript + 13 Supporting Figures

Structured light has proven useful for numerous photonic applications. However, the current use of structured light in optical fiber science and technology is severely limited by mode mixing or by the lack of optical elements that can be integrated onto fiber end-faces for complex wavefront control, and hence generation of structured light is still handled outside the fiber via bulky optics in free space. We report a metafiber platform capable of creating arbitrarily structured light on the hybrid-order Poincar\'e sphere. Polymeric metasurfaces, with unleashed height degree of freedom and a greatly expanded 3D meta-atom library, were laser nanoprinted and interfaced with polarization-maintaining single-mode fibers. Multiple metasurfaces were interfaced on the fiber end-faces, transforming the fiber output into different structured-light fields, including cylindrical vector beams, circularly polarized vortex beams, and an arbitrary vector field. Our work provides a new paradigm for advancing optical fiber science and technology towards fiber-integrated light shaping, which may find important applications in fiber communications, fiber lasers and sensors, endoscopic imaging, fiber lithography, and lab-on-fiber technology.

Broken symmetries lie at the heart of nontrivial physical phenomena. Breaking the in-plane geometrical symmetry of optical systems allows to access a set of electromagnetic states termed symmetry-protected quasi-bound states in the continuum (qBICs). Here we demonstrate, theoretically, numerically and experimentally, that such optical states can also be accessed in metasurfaces by breaking the in-plane symmetry in the permittivity of the comprising materials, showing a remarkable equivalence to their geometrically-asymmetric counterparts. However, while the physical size of atoms imposes a limit on the lowest achievable geometrical asymmetry, weak permittivity modulations due to carrier doping and electro-optical Pockels and Kerr effects, usually considered insignificant, open up the possibility of infinitesimal permittivity asymmetries for on-demand, and dynamically tuneable optical resonances of extremely high quality factors. We probe the excitation of permittivity-asymmetric qBICs (${\varepsilon}$-qBICs) using a prototype Si/TiO$_{2}$ metasurface, in which the asymmetry in the unit cell is provided by the refractive index contrast of the dissimilar materials, surpassing any unwanted asymmetries from nanofabrication defects or angular deviations of light from normal incidence. ${\varepsilon}$-qBICs can also be excited in 1D gratings, where quality-factor enhancement and tailored interference phenomena via the interplay of geometrical and permittivity asymmetries are numerically demonstrated. The emergence of ${\varepsilon}$-qBICs in systems with broken symmetries in their permittivity may enable to test time-energy uncertainties in quantum mechanics, and lead to a whole new class of low-footprint optical and optoelectronic devices, from arbitrarily narrow filters and topological sources, biosensing and ultrastrong light-matter interaction platforms, to tuneable optical switches., Comment: Manuscript and Supplementary Information, 27 pages, 4 Figures manuscript + 4 Supplementary Figures

The realization of lossless metasurfaces with true chirality crucially requires the fabrication of three-dimensional structures, constraining their feasibility for experiments and hampering practical implementations. Even though the three-dimensional assembly of metallic nanostructures has been demonstrated previously, the resulting plasmonic resonances suffer from high intrinsic and radiative losses. The concept of photonic bound states in the continuum (BICs) is instrumental for tailoring radiative losses in diverse geometries, especially when implemented using lossless dielectrics, but applications have so far been limited to planar and intrinsically achiral structures. Here, we introduce a novel nanofabrication approach to unlock the height of generally flat all-dielectric metasurfaces as an accessible parameter for efficient resonance and functionality control. In particular, we realize out-of-plane symmetry breaking in quasi-BIC metasurfaces and leverage this design degree of freedom to demonstrate, for the first time, an optical all-dielectric quasi-BIC metasurface with maximum intrinsic chirality that responds selectively to light of a particular circular polarization depending on the structural handedness. Our experimental results not only open a new paradigm for all-dielectric BICs and chiral nanophotonics but also promise advances in the realization of efficient generation of optical angular momentum, holographic metasurfaces, and parity-time symmetry-broken optical systems., Comment: Main text and supporting information, 35 pages, 3 Figures manuscript + 13 Supporting Figures

We propose a new approach based on random matrix theory to calculate the temporal second-order intensity correlation function $g^{(2)}(t)$ of the radiation emitted by random lasers and random fiber lasers. The multimode character of these systems, with a relevant degree of disorder in the active medium, and large number of random scattering centers substantially hinder the calculation of $g^{(2)}(t)$. Here we apply for the first time in a photonic system the universal statistical properties of Ginibre's non-Hermitian random matrix ensemble to obtain $g^{(2)}(t)$. Excellent agreement is found with time-resolved measurements for several excitation powers of an erbium-based random fiber laser. We also discuss the extension of the random matrix approach to address the statistical properties of general disordered photonic systems with various Hamiltonian symmetries., Comment: 5 pages, 4 figures

The capability to dynamically control the nonlinear refractive index of plasmonic suspensions may enable innovative nonlinear sensing and signaling nanotechnologies. Here, we experimentally determine the effective nonlinear refractive index for gold nanorods suspended in an index matching oil aligned using electric fields, demonstrating an approach to modulate the nonlinear optical properties of the suspension. The nonlinear optical experiments were carried out using a Hartmann-Shack wavefront aberrometer in a collimated beam configuration with a high repetition rate femtosecond laser. The suspensions were probed at 800 nm, overlapping with the long-axis absorption peak of the nanorods. We find that the effective nonlinear refractive index of the gold nanorods suspension depends linearly on the orientational order parameter, S, which can be understood by a thermally induced nonlinear response. We also show the magnitude of the nonlinear response can be varied by ~60%.

Turbulence is a challenging feature common to a wide range of complex phenomena. Random fibre lasers are a special class of lasers in which the feedback arises from multiple scattering in a one-dimensional disordered cavity-less medium. Here, we report on statistical signatures of turbulence in the distribution of intensity fluctuations in a continuous-wave-pumped erbium-based random fibre laser, with random Bragg grating scatterers. The distribution of intensity fluctuations in an extensive data set exhibits three qualitatively distinct behaviours: a Gaussian regime below threshold, a mixture of two distributions with exponentially decaying tails near the threshold, and a mixture of distributions with stretched-exponential tails above threshold. All distributions are well described by a hierarchical stochastic model that incorporates Kolmogorov's theory of turbulence, which includes energy cascade and the intermittence phenomenon. Our findings have implications for explaining the remarkably challenging turbulent behaviour in photonics, using a random fibre laser as the experimental platform., Comment: 9 pages, 5 figures

We investigate the effects of two dimensional confinement on the lasing properties of a classical random laser system operating in the incoherent feedback (diffusive) regime. A suspension of 250nm rutile (TiO2) particles in a Rhodamine 6G solution was inserted into the hollow core of a photonic crystal fiber (PCF) generating the first random fiber laser and a novel quasi-one-dimensional RL geometry. Comparison with similar systems in bulk format shows that the random fiber laser presents an efficiency that is at least two orders of magnitude higher., Comment: 15 pages, 3 figures