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Time-invariant photonic structures amplify or absorb light based on their intrinsic material gain or loss. The coherent interference of multiple beams in space, e.g., in a resonator, can be exploited to tailor the wave interaction with material gain or loss, respectively maximizing lasing or coherent perfect absorption. By contrast, a time-varying system is not bound to conserve energy, even in the absence of material gain or loss, and can support amplification or absorption of a probe wave through parametric phenomena. Here, we demonstrate theoretically and experimentally how a subwavelength film of indium tin oxide, whose bulk permittivity is homogeneously and periodically modulated via optical pumping, can be dynamically tuned to act both as a non-resonant amplifier and a perfect absorber, by manipulating the relative phase of two counterpropagating probe beams. This extends the concept of coherent perfect absorption to the temporal domain. We interpret this result as selective switching between the gain and loss modes present in the momentum bandgap of a periodically modulated medium. By tailoring the relative intensity of the two probes, high-contrast modulation can be achieved with up to 80% absorption and 400% amplification. Our results demonstrate control of gain and loss in time-varying media at optical frequencies and pave the way towards coherent manipulation of light in Floquet-engineered complex photonic systems.

The interaction of light with superluminally moving matter entails unconventional phenomena, from Fresnel drag to Hawking radiation and to light amplification. While relativity makes these effects inaccessible using objects in motion, synthetic motion - enabled via space-time modulated internal degrees of freedom - is free from these constraints. Here we observe synthetic velocity of a reflectivity modulation travelling on an Indium-Tin-Oxide (ITO) interface, generated by ultrafast laser illumination at multiple positions and times. The interaction of the moving reflectivity modulation with a probe light beam acts as a non-separable spatio-temporal transformation that diffracts the light, changing its frequency and momentum content. The recorded frequency-momentum diffraction pattern is defined by the velocity of the diffracted probe wave relative to the modulation. Our experiments open a path towards mimicking relativistic mechanics and developing programmable spatio-temporal transformations of light., Comment: 9 pages, 3 figures

Time-varying metamaterials rely on large and fast changes of the linear permittivity. Beyond the linear terms, however, the effect of a non-perturbative modulation of the medium on harmonic generation and the associated nonlinear susceptibilities remains largely unexplored. In this work, we study second harmonic generation at an optically pumped time-varying interface between air and a 310 nm Indium Tin Oxide film. We observe an enhancement of the modulation contrast at the second harmonic wavelength, up to 93% for a pump intensity of 100 GW/cm$^2$, leading to large frequency broadening and shift. We demonstrate that, in addition to the quadratic dependence on the fundamental field, a significant contribution to the enhancement comes from the temporal modulation of the second order nonlinear susceptibility, whose relative change is double that of the linear term. Moreover, the spectra resulting from single and double-slit time diffraction show significantly enhanced frequency shift, broadening and modulation depth, when compared to the infrared fundamental beam, and could be exploited for optical computing and sensing. Enhanced time-varying effects on the harmonic signal extends the application of materials to the visible range and calls for further theoretical exploration of non-perturbative nonlinear optics., Comment: 19 pages, 3 figures, 8 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

Coupled nanolasers are of growing interest for on-chip optical computation and data transmission, which requires an understanding of how lasers interact to form complex systems. The non-Hermitian interaction between two coupled resonators, when excited selectively, can lead to parity-time symmetry, the formation of exceptional points, and subsequently spectral control and increased sensitivity. These investigations have been limited to pump energies close to the lasing threshold, and large or narrow-line lasers. Here, by programmable optical excitation we study two coupled nanolasers significantly above threshold, where mode instability plays an important role. We map the mode evolution around two exceptional points, and observe lasing gaps due to reversed pump dependence which compare well with nonlinear theory. Finally, the coupling can be exploited to control the lasing threshold and wavelength, and for frequency switching around the lasing gap. Controlled and integrated nanolasers constitutes a promising platform for future highly sensitive and programmable on-chip laser sources., Comment: 8 pages, 4 figures

The final performance of a molecular electronic device is determined by the chemical structure of the molecular wires used in its assembly. Molecular place-exchange was used to incorporate di-thioacetate terminated molecules into ordered arrays of dodecanethiol capped gold nanoparticles. X-ray photoelectron spectroscopy confirmed successful molecular replacement. Room-temperature molecular conductance of a statistically large number of devices reveals that conductance is enhanced by up to two orders of magnitude for the di-thioacetate terminated molecules. Density functional theory transport calculations were performed on five different configurations of the di-thioacetate molecules between gold electrodes, and the calculated average conductance values are in good agreement with the conductance experimentally-observed trend. Our findings highlight important cooperative effects of bridging neighboring gold nanoparticles and choice of appropriate molecular wires when designing devices for efficient transport.

Numerous optical phenomena and applications have been enabled by nanophotonic structures. Their current fabrication from high refractive index dielectrics, such as silicon or gallium phosphide, pose restricting fabrication challenges, while metals, relying on plasmons and thus exhibiting high ohmic losses, limit the achievable applications. Here, we present an emerging class of layered so-called van der Waals (vdW) crystals as a viable nanophotonics platform. We extract the dielectric response of 11 mechanically exfoliated thin-film (20-200 nm) van der Waals crystals, revealing high refractive indices up to n = 5, pronounced birefringence up to $\Delta$n = 3, sharp absorption resonances, and a range of transparency windows from ultraviolet to near-infrared. We then fabricate nanoantennas on SiO$_2$ and gold utilizing the compatibility of vdW thin films with a variety of substrates. We observe pronounced Mie resonances due to the high refractive index contrast on SiO$_2$ leading to a strong exciton-photon coupling regime as well as largely unexplored high-quality-factor, hybrid Mie-plasmon modes on gold. We demonstrate further vdW-material-specific degrees of freedom in fabrication by realizing nanoantennas from stacked twisted crystalline thin-films, enabling control of nonlinear optical properties, and post-fabrication nanostructure transfer, important for nano-optics with sensitive materials.

The wave nature of light is revealed by diffraction from physical structures. We report a time-domain version of the classic Young's double-slit experiment: a beam of light twice gated in time produces an interference in the frequency spectrum. The 'time slits', narrow enough to produce diffraction at optical frequencies, are generated from a thin film of Indium-Tin-Oxide illuminated with high-power infrared pulses, inducing a fast reflectivity rise, followed by a slower decay. Separation between the time slits determines the period of oscillations in the frequency spectrum, while the decay of fringe visibility in frequency reveals the shape of the time slits. Here we find a surprise: many more oscillations are visible than expected from existing theory, implying a rise time for the leading edge of around 1-10 fs, approaching an optical cycle of 4.4 fs. This is over an order of magnitude faster than the width of the pump and can be inferred from the decay of the frequency oscillations., Comment: 12 pages, 2 figures, 4 supplementary figures - submitted

We report a switchable time-varying mirror, composed of an ITO-Au stack, which can be efficiently modulated in time with over a ten-fold increase in reflectivity, with a change of 0.6. Upon interacting with the time-varying mirror, the frequency content of a reflected pulse is extended to 31 THz. This originates from the shortening of the response time of the mirror beyond saturation, as confirmed by a time-varying model and by further four-wave mixing experiments. A temporal response unbounded by the pump bandwidth opens new avenues for spectral manipulation from time-varying systems with impact for communication networks, optical switching and computing. We report a switchable time-varying mirror, composed of an ITO-Au bilayer, displaying a ten-fold modulation of reflectivity ($\Delta R \approx 0.6$), which saturates for a driving pump intensity $I_{\mathrm{pump}}\approx 100$~GW/cm$^2$. Upon interacting with the saturated time-varying mirror, the frequency content of a reflected pulse is extended up to 31 THz, well beyond the pump spectral content (2.8 THz). We interpret the spectral broadening as a progressive shortening of the mirror rise time from 110 fs to sub 30 fs with increasing pump power, which is confirmed by four-wave mixing experiments and partially captured by a linear time-varying model of the mirror. A temporal response unbounded by the pump bandwidth opens new avenues for spectral manipulation from time-varying systems with impact for communication networks, optical switching and computing., Comment: 6 pages, 4 figures Supplemental: 7 pages, 5 figures update: resubmitted version following referee feedback - removed red-colored sentences

Researchers have shown that children's social-emotional growth is inextricably connected to academic learning. We developed the Social-Emotional Learning Foundations (SELF) intervention, a Grade K-1 curriculum merging social-emotional learning (SEL) and literacy instruction, to promote language supported self-regulation, specifically for primary grade children at early risk for emotional or behavioral difficulties. We report findings from a pretest-posttest cluster randomized efficacy trial with one fixed between-subjects factor to test the effects of teacher-delivered SEL instruction against those of business as usual (BAU). We recruited 163 kindergarten (K) and 141 first grade teachers from 52 schools across 11 school districts within one southeastern state. Our student sample (n=1154) consisted of 627 kindergarteners and 527 first graders identified by teachers as at risk for internalizing or externalizing emotional and behavioral problems using the "Systematic Screening for Behavioral Disorders"; 613 of these students participated in the SELF condition and 541 participated in the BAU condition. We randomly assigned schools to SELF or BAU and used a multilevel model with three levels (i.e., children, classrooms, schools) to analyze data on subscales of six (four teacher-report and two direct) assessments related to self-regulation, social-emotional learning, social-emotional vocabulary, and general behavioral functioning. We found positive main effects of SELF compared to BAU on all but one measure, with effect sizes (calculated using Hedges' "g") ranging from 0.20 to 0.65. Findings provide evidence for guiding future SEL intervention research and informing practice to improve student outcomes, particularly for children at risk for behavior problems. [This is the online first version of an article published in "Journal of School Psychology."]

Giant shell CdSe/CdS quantum dots are bright and flexible emitters, with near-unity quantum yield and suppressed blinking, but their single photon purity is reduced by efficient multiexcitonic emission. We report the observation, at the single dot level, of a large blueshift of the photoluminescence biexciton spectrum ($24\pm5$ nm over a sample of 32 dots) for pure-phase wurtzite quantum dots. By spectral filtering, we demonstrate a 2.3 times reduction of the biexciton quantum yield relative to the exciton emission, while preserving as much as 60% of the exciton single photon emission, thus improving the purity from $g_2(0)=0.07\pm0.01$ to $g_2(0)=0.03\pm0.01$. At larger pump fluency the spectral purification is even more effective with up to a 6.6 times reduction in $g_2(0)$, which is due to the suppression of higher order excitons and shell states experiencing even larger blueshift. Our results indicate the potential for synthesis engineered giant shell quantum dots, with further increased biexciton blueshift, for quantum optical applications requiring both high purity and brightness., Comment: Supporting information is available

Time-varying media have recently emerged as a new paradigm for wave manipulation, thanks to thesynergy between the discovery of novel, highly nonlinear materials, such as epsilon-near-zero materials, and the questfor novel wave applications, such as magnet-free nonreciprocity, multi-mode light shaping, and ultrafast switching. Inthis review we provide a comprehensive discussion of the recent progress achieved with photonic metamaterials whoseproperties stem from their modulation in time. We review the basic concepts underpinning temporal switching and itsrelation with spatial scattering, and deploy the resulting insight to review photonic time-crystals and their emergentresearch avenues such as topological and non-Hermitian physics. We then extend our discussion to account for spa-tiotemporal modulation and its applications to nonreciprocity, synthetic motion, giant anisotropy, amplification andother effects. Finally, we conclude with a review of the most attractive experimental avenues recently demonstrated,and provide a few perspectives on emerging trends for future implementations of time-modulation in photonics.

Electron transfer to an individual quantum dot promotes the formation of charged excitons with enhanced recombination pathways and reduced lifetimes. Excitons with only one or two extra charges have been observed and exploited for very efficient lasing or single quantum dot LEDs. Here, by room-temperature time-resolved experiments on individual giant-shell CdSe/CdS quantum dots, we show the electrochemical formation of highly charged excitons containing more than twelve electrons and one hole. We report the control over intensity blinking, along with a deterministic manipulation of quantum dot photodynamics, with an observed 210-fold increase of the decay rate, accompanied by 12-fold decrease of the emission intensity, while preserving single-photon emission characteristics. These results pave the way for deterministic control over the charge state, and room-temperature decay-rate engineering for colloidal quantum dot-based classical and quantum communication technologies.

The efficient excitation of quantum sources such as quantum dots or single molecules requires high NA optics which is often a challenge in cryogenics, or in ultrafast optics. Here we propose a 3.2 um wide parabolic mirror, with a 0.8 um focal length, fabricated by direct laser writing on CdSe/CdS colloidal quantum dots, capable of focusing the excitation light to a sub-wavelength spot and to extract the generated emission by collimating it into a narrow beam. This mirror is fabricated via in-situ volumetric optical lithography, which can be aligned to individual emitters, and it can be easily adapted to other geometries beyond the paraboloid. This compact solid-state transducer from far-field to the emitter has important applications in objective-free quantum technologies.

The ultrafast changes of material properties induced by short laser pulses can lead to frequency shift of reflected and transmitted radiation. Recent reports highlight how such a frequency shift is enhanced in the spectral regions where the material features a near-zero real part of the permittivity. Here we investigate the frequency shift for fields generated by four-wave mixing with a nonlinear polarisation oscillating at twice the pump frequency. In our experiment we observe a frequency shift of more than 60 nm (compared to the pulse width of ~40 nm) for the phase conjugated radiation generated by a 500 nm Aluminium-doped Zinc Oxide (AZO) film pumped close to the epsilon-near-zero wavelength. Our results indicate applications of time-varying media for nonlinear optics and frequency conversion.

Time-varying metasurfaces are emerging as a powerful instrument for the dynamical control of the electromagnetic properties of a propagating wave. Here we demonstrate an efficient time-varying metasurface based on plasmonic nano-antennas strongly coupled to an epsilon-near-zero (ENZ) deeply sub-wavelength film. The plasmonic resonance of the metal resonators strongly interacts with the optical ENZ modes, providing a Rabi level spitting of ~30%. Optical pumping at frequency {\omega} induces a nonlinear polarisation oscillating at 2{\omega} responsible for an efficient generation of a phase conjugate and a negative refracted beam with a conversion efficiency that is more than four orders of magnitude greater compared to the bare ENZ film. The introduction of a strongly coupled plasmonic system therefore provides a simple and effective route towards the implementation of ENZ physics at the nanoscale

The dynamical Casimir effect is the generation of pairs of real particles or photons from the vacuum as a result of a non-adiabatic change of a system parameter or boundary condition. As opposed to standard parametric amplification where the modulation occurs both in space and in time, this fundamental process requires a pure modulation in time, which makes its detection particularly challenging at optical frequencies. In this paper we experimentally demonstrate a realisation of the optical analogue of the mechanical dynamical Casimir effect in the near-infrared optical regime in a dispersion-oscillating photonic crystal fibre. The experiments are based on the equivalence of the spatial modulation of the fibre core diameter to a pure temporal modulation when this is considered in the co-moving frame of the travelling pump pulse. We provide evidence of optical dynamical Casimir effect by measuring quantum correlations between the spectrally resolved photon pairs. The non-classical nature of the measured light is supported by evidence of anti-bunching photon statistics.

We propose a design concept for tailoring the local density of optical states (LDOS) in dielectric nanostructures, based on the phase distribution of the scattered optical fields induced by point-like emitters. First we demonstrate that the LDOS can be expressed in terms of a coherent summation of constructive and destructive contributions. By using an iterative approach, dielectric nanostructures can be designed to effectively remove the destructive terms. In this way dielectric Mie resonators, featuring low LDOS for electric dipoles, can be reshaped to enable enhancements of three orders of magnitude. To demonstrate the generality of the method, we also design nanocavities that enhance the radiated power of a circular dipole, a quadrupole and an arbitrary collection of coherent dipoles. Our concept provides a powerful tool for high-performance dielectric resonators, and affords fundamental insights into light-matter coupling at the nanoscale.

The blinking dynamics of colloidal core-shell CdSe/CdS dot-in-rods is studied in detail at the single particle level. Analyzing the autocorrelation function of the fluorescence intensity, we demonstrate that these nanoemitters are characterized by a short value of the mean duration of bright periods (ten to a few hundreds of microseconds). The comparison of the results obtained for samples with different geometries shows that not only the shell thickness is crucial but also the shape of the dot- in-rods. Increasing the shell aspect ratio results in shorter bright periods suggesting that surface traps impact the stability of the fluorescence intensity.