The precise characterization of ultrashort laser pulses has been of interest to the scientific community for many years. Frequency-resolved optical gating (FROG) has been extensively used to retrieve the temporal and spectral field distributions of ultrashort laser pulses. In this work, we exploit the high, broad-band nonlinear optical response of a WS₂monolayer to simultaneously characterize two ultrashort laser pulses with different frequencies. The relaxed phase-matching conditions in a WS₂monolayer enable the simultaneous acquisition of the spectra resulting from both four-wave mixing (FWM) and sum-frequency generation (SFG) nonlinear processes while varying the time delay between the two ultrashort pulses. Next, we introduce an adjusted double-blind FROG algorithm, based on iterative fast Fourier transforms between two FROG traces, to extract the intensity distribution and phase of two ultrashort pulses from the combination of their FWM and SFG FROG traces. Using this algorithm, we find an agreement between the computed and observed FROG traces for both the FWM and SFG processes. Exploiting the broad-band nonlinear response of a WS₂monolayer, we additionally characterize one of the pulses using a second-harmonic generation (SHG) FROG trace to validate the pulse shapes extracted from the combination of the FWM and SFG FROG traces. The retrieved pulse shape from the SHG FROG agrees well with the pulse shape retrieved from our nondegenerate cross-correlation FROG measurement. In addition to the nonlinear parametric processes, we also observe a nonlinearly generated photoluminescence (PL) signal emitted from the WS₂monolayer. Because of its nonlinear origin, the PL signal can also be used to obtain complementary autocorrelation and cross-correlation traces.

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Currently, the nonlinear optical properties of 2D materials are attracting the attention of an ever-increasing number of research groups due to their large potential for applications in a broad range of scientific disciplines. Here, we investigate the interplay between nonlinear photoluminescence (PL) and several degenerate and nondegenerate nonlinear optical processes of a WS2 monolayer at room temperature. We illuminate the sample using two femtosecond laser pulses at frequencies ω1 and ω2 with photon energies below the optical bandgap. As a result, the sample emits light that shows characteristic spectral peaks of the second-harmonic generation, sum-frequency generation, and four-wave mixing. In addition, we find that both resonant and off-resonant nonlinear excitation via frequency mixing contributes to the (nonlinear) PL emission at the A-exciton frequency. The PL exhibits a clear correlation with the observed nonlinear effects, which we attribute to the generation of excitons via degenerate and nondegenerate multiphoton absorption. Our work illustrates a further step toward understanding the fundamental relation between parametric and nonparametric nondegenerate optical mechanisms in transition-metal dichalcogenides. In turn, such understanding has great potential to expand the range of applicability of nonlinear optical processes of 2D materials in different fields of science and technology, where nonlinear mechanisms are typically limited to degenerate processes.

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Transition metal dichalcogenides such as MoS2 represent promising candidates for building blocks of ultra-thin nanophotonic devices. For such applications, vertically-oriented MoS2 (v-MoS2) nanosheets could be advantageous as compared to conventional horizontal MoS2 (h-MoS2) given that their inherent broken symmetry would favor an enhanced nonlinear response. However, the current lack of a controllable and reproducible fabrication strategy for v-MoS2 limits the exploration of this potential. Here we present a systematic study of the growth of v-MoS2 nanosheets based on the sulfurization of a pre-deposited Mo-metal seed layer. We demonstrate that the sulfurization process at high temperatures is driven by the diffusion of sulfur from the vapor-solid interface to the Mo seed layer. Furthermore, we verify an enhanced nonlinear response in the resulting v-MoS2 nanostructures as compared to their horizontal counterparts. Our results represent a stepping stone towards the fabrication of low-dimensional TMD-based nanostructures for versatile nonlinear nanophotonic devices.

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Nanostructured gratings in a metal surface can highly enhance nonlinear optical processes. The geometrical parameters that characterize a grating can be optimized to achieve intense near-fields, which in turn enhance the nonlinear optical signals. For a nonlinear process that involves multiple frequencies, like four-wave mixing (FWM), the optimization of grating parameters necessary to enhance the radiation in-coupling for both frequencies is not trivial. Here, we propose, compute, and experimentally demonstrate a grating design that is resonant to two excitation frequencies and thus enhances the frequency mixing processes more efficiently. Second- and third-order nonlinear mechanisms are studied using two spatially and temporally overlapped laser pulses with different frequencies. Using our grating design, we achieve an unprecedented nonlinear FWM enhancement factor of 7 × 10 3.

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We study the expansion dynamics of super-heated material during ultra-fast laser ablation of water and gel, using transient-reflectivity microscopy. We find that the expansion dynamics of water and gel, as observed during the first few nanoseconds, are extremely similar over a large range of ablation energies. We measure the crater topography of the gel after irradiation with a single laser shot, using optical interferometric microscopy, and estimate the mass that is ejected during the ablation. We calculate the laser energy deposited during irradiation by simulating the precise spatial distribution of the electron plasma density and temperature. We link the amount of removed mass obtained experimentally with the simulations of the deposited laser energy.@en

We study femtosecond-laser-induced flows of air at a water/air interface, at micrometer length scales. To visualize the flow velocity field, we simultaneously induce two flow fronts using two adjacent laser pump spots. Where the flows meet, a stationary shockwave is produced, the length of which is a measure of the local flow velocity at a given radial position. By changing the distance between the spots using a spatial light modulator, we map out the flow velocity around the pump spots. We find gas front velocities near the speed of sound in air vs for two laser excitation energies. We find an energy scaling that is inconsistent with the Sedov-Taylor model. Due to the flexibility offered by spatial beam shaping, our method can be applied to study subsonic laser-induced gas flow fronts in more complicated geometries.@en

The light–energy coupling during femtosecond laser processing of glass is mediated by non-linear ionization mechanisms through the formation of an electron plasma. Its transient optical properties provide information about the density, temperature and scattering rate of the excited electrons. In turn, these properties strongly condition the features and size of the permanent optical modification near the focal volume that are desirable to fabricate photonic devices, such as optical waveguides inside transparent materials. Here, we report on the spectral response of a fs-laser-induced electron plasma inside fused silica by measuring its transient transmission using a broadband probe. We model the interaction of the probe beam with the plasma by combining Drude–Sommerfeld model with Gaussian optics. In this manner, we take into account both the laser–plasma interaction and the influence of the chromatic aberration inherent to a broadband-based system. We find good agreement between experiments at several processing energies and simulations and provide an estimate of the dielectric function of the excited material.@en

We investigate the interaction of femtosecond (fs) laser pulses with single gold nanoparticles, trapped in a linear Paul trap. We study the scattering response of the particles as a function of the polarization angle of a cw laser at three different wavelengths. These measurements provide a value of the visibility that we compare with Mie theory calculations in order to obtain an estimate of the particle radius. We monitor the particle size during ultrafast laser ablation, obtaining an accurate figure for the mass loss as a function of the fs-laser dose. We discuss the particle mass loss induced by a single fs-laser shot and its relation with the number of absorbed photons.

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