We predict theoretically a regime of photon-pair generation driven by the interplay of multiple bound states in the continuum resonances in nonlinear metasurfaces. This nondegenerate photon-pair generation is derived from the hyperbolic topology of the transverse phase matching and can enable orders-of-magnitude enhancement of the photon rate and spectral brightness, as compared to the degenerate regime. We show through comprehensive simulations that the entanglement of the photon pairs can be tuned by varying the pump polarization, which can underpin future advances and applications of ultracompact quantum light sources.

We investigate, with a combination of ultrafast optical spectroscopy and semiclassical modeling, the photothermal properties of various water-soluble nanocrystal assemblies. Broadband pump-probe experiments with ∼100-fs time resolution in the visible and near infrared reveal a complex scenario for their transient optical response that is dictated by their hybrid composition at the nanoscale, comprising metallic (Au) or semiconducting (Fe 3 O 4 ) nanostructures and a matrix of organic ligands. We track the whole chain of energy flow that starts from light absorption by the individual nanocrystals and subsequent excitation of out-ofequilibrium carriers followed by the electron-phonon equilibration, occurring in a few picoseconds, and then by the heat release to the matrix on the 100-ps timescale. Two-dimensional finiteelement method electromagnetic simulations of the composite nanostructure and multitemperature modeling of the energy flow dynamics enable us to identify the key mechanism presiding over the light-heat conversion in these kinds of nanomaterials. We demonstrate that hybrid (organic-inorganic) nanocrystal assemblies can operate as efficient nanoheaters by exploiting the high absorption from the individual nanocrystals, enabled by the dilution of the inorganic phase that is followed by a relatively fast heating of the embedding organic matrix, occurring on the 100-ps timescale.

No abstract

We study the optical properties of an anisotropic ripple-shaped two-dimensional molybdenum disulfide (MoS2) nanosheet deposited by chemical vapor deposition onto a nanopatterned silica (SiO2) substrate. We unveil a giant anisotropic optical response in the linear and nonlinear regime by a combination of optical extinction measurements, ultrafast broadband transient absorption experiments, and finite element method numerical simulations. In steady state optical measurements, such anisotropy appears as a polarization-dependent extinction in correspondence with the characteristic excitonic peaks (A, B, C, and D) of MoS2. Along with spectral changes, ultrafast measurements strikingly exhibit the onset of an anisotropic relaxation dynamic in the region of the C exciton. Numerical simulations indicate that the observed polarization-dependent optical response is dictated by the nanopattering of MoS2, with peculiar features belonging to the out-of-plane component of the dielectric tensor of MoS2 that is made effective through the rippled configuration. Our findings give a rationale to the anisotropic exciton response and show that morphology manipulation represents a valuable option for the tuning of optical and electronic properties in transition-metal dichalcogenides.

Nanofabrication of flat optic silica gratings conformally layered with two-dimensional (2D) MoS 2 is demonstrated over large area (cm 2 ), achieving a strong amplification of the photon absorption in the active 2D layer. The anisotropic subwavelength silica gratings induce a highly ordered periodic modulation of the MoS 2 layer, promoting the excitation of Guided Mode Anomalies (GMA) at the interfaces of the 2D layer. We show the capability to achieve a broadband tuning of these lattice modes from the visible (VIS) to the near-infrared (NIR) by simply tailoring the illumination conditions and/or the period of the lattice. Remarkably, we demonstrate the possibility to strongly confine resonant and nonresonant light into the 2D MoS 2 layers via GMA excitation, leading to a strong absorption enhancement as high as 240% relative to a flat continuous MoS 2 film. Due to their broadband and tunable photon harvesting capabilities, these large area 2D MoS 2 metastructures represent an ideal scalable platform for new generation devices in nanophotonics, photo- detection and -conversion, and quantum technologies.

The enhancement of nonlinear optical effects via nanoscale engineering is a hot topic of research. Optical nanoantennas increase light–matter interaction and provide, simultaneously, a high throughput of the generated harmonics in the scattered light. However, nanoscale nonlinear optics has dealt so far with static or quasi-static configurations, whereas advanced applications would strongly benefit from high-speed reconfigurable nonlinear nanophotonic devices. Here we propose and experimentally demonstrate ultrafast all-optical modulation of the second harmonic (SH) from a single nanoantenna. Our design is based on a subwavelength AlGaAs nanopillar driven by a control femtosecond light pulse in the visible range. The control pulse photoinjects free carriers in the nanostructure, which in turn induce dramatic permittivity changes at the band edge of the semiconductor. This results in an efficient modulation of the SH signal generated at 775 nm by a second femtosecond pulse at the 1.55 μm telecommunications (telecom) wavelength. Our results can lead to the development of ultrafast, all optically reconfigurable, nonlinear nanophotonic devices for a broad class of telecom and sensing applications.

We demonstrate optically tunable control of secondharmonic generation in all-dielectric nanoantennas: by using a control beam which is absorbed by the nanoresonator, we thermo-optically change the refractive index of the radiating element to modulate the amplitude of the second-harmonic signal. For a moderate temperature increase of roughly 40 K, modulation of the efficiency up to 60% is demonstrated; this large tunability of the single meta-atom response paves the way to exciting avenues for reconfigurable homogeneous and heterogeneous metasurfaces.

Plasmonic nanoparticles (NPs) are exploited to concentrate light, provide local heating and enhance drug release when coupled to smart polymers. However, the role of NP assembling in these processes is poorly investigated, although their superior performance as nanoheaters has been theoretically predicted since a decade. Here we report on a compound hydrogel (agarose and carbomer 974P) loaded with gold NPs of different configurations. We investigate the dynamics of light-heat conversion in these hybrid plasmonic nanomaterials via a combination of ultrafast pump-probe spectroscopy and hot-electrons dynamical modeling. The photothermal study ascertains the possibility to control the degree of assembling via surface functionalization of the NPs, thus enabling a tuning of the photothermal response of the plasmon-enhanced gel under continuous wave excitation. We exploit these assemblies to enhance photothermal release of drug mimetics with large steric hindrance loaded in the hydrogel. Using compounds with an effective hydrodynamic diameter bigger than the mesh size of the gel matrix, we find that the nanoheaters assemblies enable a two orders of magnitude faster cumulative drug release toward the surrounding environment compared to isolated NPs, under the same experimental conditions. Our results pave the way for a new paradigm of nanoplasmonic control over drug release.