Optical frequency conversion via the nonlinear effect of third harmonic generation is shown to be resonantly enhanced in few-layer black phosphorus. This feature is believed to be a consequence of exciton-related resonance, as the enhancement is strongly correlated with the observation of exciton-recombination photoluminescence. Few-layer thicknesses are obtained both via mechanical exfoliation and laser thinning.
We report the first detailed characterization of the sheet third-harmonic optical susceptibility, χ(3)s, of tungsten diselenide (WSe2). With a home-built multiphoton microscope setup developed to study harmonics generation, we map the second and third-harmonic intensities as a function of position in the sample, pump power and polarization angle, for single- and few-layers flakes of WSe2. We register a value of |χ(3)s| ≈ 0.9 × 10−28 m3 V−2 at a fundamental excitation frequency of ℏω = 0.8 eV, which is comparable in magnitude to the third-harmonic susceptibility of other group-VI transition metal dichalcogenides. The simultaneously recorded sheet second-harmonic susceptibility is found to be |χ(2)s| ≈ 0.7 × 10−19 m2 V−1 in very good agreement on the order of magnitude with recent reports for WSe2, which asserts the robustness of our values for |χ(3)s|.
A population imbalance at different valleys of an electronic system lowers its effective rotational symmetry. We introduce a technique to measure such imbalance (a valley polarization), which exploits the unique fingerprints of this symmetry reduction in the polarization-dependent secondharmonic generation (SHG). We present the principle and detection scheme in the context of hexagonal two-dimensional crystals, which include graphene-based systems and the family of transition metal dichalcogenides, and provide a direct experimental demonstration using a molybdenum diselenide monolayer with 2H polytype at room temperature. We deliberately use the simplest possible setup, where a single pulsed laser beam simultaneously controls the valley imbalance and tracks the SHG process. We further developed a model of the transient population dynamics, which analytically describes the valley-induced SHG rotation in very good agreement with the experimental data. In addition to providing the first experimental demonstration of the effect, this work establishes a conceptually simple, compact, and transferable way of measuring instantaneous valley polarization, with direct applicability in the nascent field of valleytronics.
We propose a robust photonic platform for encapsulation and addressing of optically active 2D-and nano-materials. Our implementation utilises a monolayer of MoS 2 transition metal dichalcogenide embedded in an elastomeric waveguide chip. The structure is manufactured from PDMS using soft-lithography and capable of sustaining a single mode of guided light. We prove that this setup facilitates addressing of the 2D material flake by pumping it with polarised laser light and gathering polarisation-resolved photoluminescence spectra with the extinction ratio of 31, which highlights the potential for selection-rule dependent measurements. Our results demonstrate improved handling of the material and experimental simplification compared to other techniques.
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