Nowadays, the accurate and full temporal characterization of ultrabroadband few-cycle laser pulses with pulse durations below 7 fs is of great importance in fields of science that investigate ultrafast dynamic processes. There are several indirect methods that use nonlinear optical signals to retrieve the complex electric field of femtosecond lasers. However, the precise characterization of few-cycle femtosecond laser sources with an ultrabroadband spectrum presents additional difficulties, such as reabsorption of nonlinear signals, partial phase matching, and spatiotemporal mismatches. In this work, we combine the dispersion scan (d-scan) method with atomically thin WS2 flakes to overcome these difficulties and fully characterize ultrabroadband laser pulses with a pulse duration of 6.9 fs and a spectrum that ranges from 650 to 1050 nm. Two-dimensional WS2 acts as a remarkably efficient nonlinear medium that offers a broad transparency range and allows for achieving relaxed phase-matching conditions due to its atomic thickness. Using mono- and trilayers of WS2, we acquire d-scan traces by measuring the second-harmonic generation (SHG) signal, originated via laser-WS2 interaction, as a function of optical dispersion (i.e., glass thickness) and wavelength. Our retrieval algorithm extracts a pulse duration at full-width half-maximum of 6.9 fs and the same spectral phase function irrespective of the number of layers. We benchmark and validate our results obtained using WS2 by comparing them with those obtained using a 10-μm-thick BBO crystal. Our findings show that atomically thin media can be an interesting alternative to micrometer-thick bulk crystals to characterize ultrabroadband femtosecond laser pulses using SHG-d-scan with an error below 100 as (attoseconds).

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In this thesis, we explore the interaction between multiple optical light fields. Although these light fields can interfere with each other in a vacuum, actual interaction can only occur in a medium. This interaction can be amplified in materials with nanoscale dimensions such as a monolayer of WS2 and metallic nanostructures. The shapes of these materials have characteristic length scales smaller than the wavelength of light and influence the interaction between light and matter. There are three main reasons why studying light field interactions in nanoscale materials is interesting. First, by investigating the interaction between different light waves we have a tool to probe the light behavior in, e.g., a monolayerWS2 or metallic nanostructures. Secondly, by studying the interaction of multiple light waves we can probe the characteristics of the light waves themselves. Finally, the interaction of light waves can be utilized in novel applications such as frequency conversion and photonic nanocircuitry. This thesis is divided into four parts which will be discussed in the following sections… @en

The fabrication of 2D materials, such as transition metal dichalcogenides (TMDs), in geometries beyond the standard platelet-like configuration exhibits significant challenges which severely limit the range of available morphologies. These challenges arise due to the anisotropic character of their bonding van der Waals out-of-plane while covalent in-plane. Furthermore, industrial applications based on TMD nanostructures with non-standard morphologies require full control on the size-, morphology-, and position on the wafer scale. Such a precise control remains an open problem of which solution would lead to the opening of novel directions in terms of optoelectronic applications. Here, a novel strategy to fabricate position-controlled Mo/MoS₂ core–shell nanopillars (NPs) is reported on. Metal-Mo NPs are first patterned on a silicon wafer. These Mo NPs are then used as scaffolds for the synthesis of Mo/MoS₂ core/shell NPs by exposing them to a rich sulfur environment. Transmission electron microscopy analysis reveals the core/shell nature of the NPs. It is demonstrated that individual Mo/MoS₂ NPs exhibits significant nonlinear optical processes driven by the MoS₂ shell, realizing a precise localization of the nonlinear signal. These results represent an important step towards realizing 1D TMD-based nanostructures as building blocks of a new generation of nanophotonic devices.

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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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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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Silicon spin qubits are one of the leading platforms for quantum computation^1,2. As with any qubit implementation, a crucial requirement is the ability to measure individual quantum states rapidly and with high fidelity. Since the signal from a single electron spin is minute, the different spin states are converted to different charge states^3,4. Charge detection, so far, has mostly relied on external electrometers^5–7, which hinders scaling to two-dimensional spin qubit arrays^2,8,9. Alternatively, gate-based dispersive read-out based on off-chip lumped element resonators has been demonstrated^10–13, but integration times of 0.2–2 ms were required to achieve single-shot read-out^14–16. Here, we connect an on-chip superconducting resonant circuit to two of the gates that confine electrons in a double quantum dot. Measurement of the power transmitted through a feedline coupled to the resonator probes the charge susceptibility, distinguishing whether or not an electron can oscillate between the dots in response to the probe power. With this approach, we achieve a signal-to-noise ratio of about six within an integration time of only 1 μs. Using Pauli’s exclusion principle for spin-to-charge conversion, we demonstrate single-shot read-out of a two-electron spin state with an average fidelity of >98% in 6 μs. This result may form the basis of frequency-multiplexed read-out in dense spin qubit systems without external electrometers, therefore simplifying the system architecture.

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In the version of this Letter originally published, the second, third and fourth exponential terms in equation (3) were incorrect; the corrected equation is shown below. (Formula presented.). The correct equation was used for data analysis. The online versions have been amended.

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We demonstrate the strong coupling between a single electron spin in silicon and a single photon in a superconducting microwave cavity. Using the same cavity we perform rapid high-fidelity single-shot readout of two-electron spin states.

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