RESUMEN
The increasing role of two-dimensional (2D) devices requires the development of new techniques for ultrafast control of physical properties in 2D van der Waals (vdW) nanolayers. A special feature of heterobilayers assembled from vdW monolayers is femtosecond separation of photoexcited electrons and holes between the neighboring layers, resulting in the formation of Coulomb force. Using laser pulses, we generate a 0.8 THz coherent breathing mode in MoSe2/WSe2 heterobilayers, which modulates the thickness of the heterobilayer and should modulate the photogenerated electric field in the vdW gap. While the phonon frequency and decay time are independent of the stacking angle between the MoSe2 and WSe2 monolayers, the amplitude decreases at intermediate angles, which is explained by a decrease in the photogenerated electric field between the layers. The modulation of the vdW gap by coherent phonons enables a new technology for the generation of THz radiation in 2D nanodevices with vdW heterobilayers.
RESUMEN
We investigate the non-degenerate two-photon absorption coefficient ß(ω1, ω2) as a function of the non-degeneracy parameter ω1/ω2 for bulk GaAs and Si at a constant transition energy â ω 1+â ω 2=1.57eV. In both materials, the two-photon absorption strength increases with increasing ω1/ω2 regardless of the direct and indirect character of the bandgap. The GaAs measurement data agrees well with corresponding theoretical predictions for direct semiconductors. The Si data reveals similar trends albeit with smaller overall absorption strength. In addition, different crystallographic orientations and polarization configurations are analyzed.
RESUMEN
Transient changes of the optical response of WS2 monolayers are studied by femtosecond broadband pump-probe spectroscopy. Time-dependent absorption spectra are analyzed by tracking the line width broadening, bleaching, and energy shift of the main exciton resonance as a function of time delay after the excitation. Two main sources for the pump-induced changes of the optical response are identified. Specifically, we find an interplay between modifications induced by many-body interactions from photoexcited carriers and by the subsequent transfer of the excitation to the phonon system followed by cooling of the material through the heat transfer to the substrate.
RESUMEN
We propose and implement a new concept for thermochromic plasmonic elements. It is based on vanadium dioxide (VO2) nanocrystals located in the near field of surface plasmon polaritons supported by an otherwise unstructured gold thin film. When the VO2 undergoes the metal-insulator phase transition, the coupling conditions for conversion of light into propagating surface plasmon polaritons change markedly. In particular, we realize thermochromic plasmonic grating couplers with substantial switching contrast as well as tunable plasmonic couplers in a Kretschmann configuration. The use of VO2 nanocrystals permits highly repetitive switching and room temperature operation. Simulations based on the actual dielectric function of our VO2 nanocrystals agree well with the experiment.
RESUMEN
Single- and few-layer crystals of exfoliated MoTe2 have been characterized spectroscopically by photoluminescence, Raman scattering, and optical absorption measurements. We find that MoTe2 in the monolayer limit displays strong photoluminescence. On the basis of complementary optical absorption results, we conclude that monolayer MoTe2 is a direct-gap semiconductor with an optical band gap of 1.10 eV. This new monolayer material extends the spectral range of atomically thin direct-gap materials from the visible to the near-infrared.
RESUMEN
We propose and implement a versatile scheme to analyze the phase structure of femtosecond pulses. It relies on second harmonic generation in combination with phase-sensitive χ(3)-current injection driven by two time-delayed portions of the emerging ω/2ω pulse pair. Most strikingly, the group velocity dispersions of both the ω and 2ω components can be unambiguously determined from a simple Fourier transformation of the resulting current interferogram. We test the concept for 45 fs pulses at 1.45 µm and directly compare it to second harmonic frequency resolved optical gating. By choosing appropriate frequency doublers and semiconductor detectors, the scheme is applicable to many wavelength regimes and to pulses as short as a few optical cycles.
RESUMEN
Acoustic nanocavities (ANCs) with resonance frequencies much above 1 GHz are prospective to be exploited in sensors and quantum operating devices. Nowadays, acoustic nanocavities fabricated from van der Waals (vdW) nanolayers allow them to exhibit resonance frequencies of the breathing acoustic mode up to f â¼ 1 THz and quality factors up to Q â¼ 103. For such high acoustic frequencies, electrical methods fail, and optical techniques are used for the generation and detection of coherent phonons. Here, we study experimentally acoustic nanocavities fabricated from WSe2 layers with thicknesses from 8 up to 130 nm deposited onto silica colloidal crystals. The substrate provides a strong mechanical support for the layers while keeping their acoustic properties the same as in membranes. We concentrate on experimental and theoretical studies of the amplitude of the optically measured acoustic signal from the breathing mode, which is the most important characteristic for acousto-optical devices. We probe the acoustic signal optically with a single wavelength in the vicinity of the exciton resonance and measure the relative changes in the reflectivity induced by coherent phonons up to 3 × 10-4 for f â¼ 100 GHz. We reveal the enhancement of photon-phonon interaction for a wide range of acoustic frequencies and show high sensitivity of the signal amplitude to the photoelastic constants governed by the deformation potential and dielectric function for photon energies near the exciton resonance. We also reveal a resonance in the photoelastic response (we call it photoelastic resonance) in the nanolayers with thickness close to the Bragg condition. The estimates show the capability of acoustic nanocavities with an exciton resonance for operations with high-frequency single phonons at an elevated temperature.
RESUMEN
We implement a versatile concept to time-resolve optical nonlinearities of semiconductors in amplitude and phase. A probe pulse transmitted through the optically pumped sample is superimposed with first subharmonic spectral components derived from the same laser source. This effective ω/2ω pulse pair induces a coherently controlled current in a time-integrating semiconductor detector. Current interferograms obtained by scanning the ω/2ω time delay then reveal the electric field of the 2ω part as well as its pump-induced modifications. As a paradigm we analyze the excitonic optical nonlinearity of a CdTe thin film at frequencies around 385 THz. We then move on to resolve the pump-induced amplitude- and phase-distortions of a probe pulse related to two-photon absorption and cross-phase modulation in ZnSe.
RESUMEN
We propose and demonstrate an ultrabroadband concept to characterize amplitude and phase changes of femtosecond pulses. The radiation is superimposed with the first subharmonic spectral components from the same laser source. This effective ω/2ω pulse pair induces a coherently controlled charge current in a time-integrating semiconductor detector. An interferometric variation of the time delay between the harmonically related components then reveals the electric field of the 2ω part. This method is realized with the second harmonic of a compact Er:fiber source centered at 390 THz and a GaAs-based detector. Most strikingly, it is sensitive to â¼π/20 phase changes and can be utilized to analyze femtojoule pulses.
RESUMEN
The nonlinear process of second harmonic generation (SHG) in monolayer (1L) transition metal dichalcogenides (TMD), like WS2, strongly depends on the polarization state of the excitation light. By combination of plasmonic nanostructures with 1L-WS2 by transferring it onto a plasmonic nanoantenna array, a hybrid metasurface is realized impacting the polarization dependency of its SHG. Here, we investigate how plasmonic dipole resonances affect the process of SHG in plasmonic-TMD hybrid metasurfaces by nonlinear spectroscopy. We show that the polarization dependency is affected by the lattice structure of plasmonic nanoantenna arrays as well as by the relative orientation between the 1L-WS2 and the individual plasmonic nanoantennas. In addition, such hybrid metasurfaces show SHG in polarization states, where SHG is usually forbidden for either 1L-WS2 or plasmonic nanoantennas. By comparing the SHG in these channels with the SHG generated by the hybrid metasurface components, we detect an enhancement of the SHG signal by a factor of more than 40. Meanwhile, an attenuation of the SHG signal in usually allowed polarization states is observed. Our study provides valuable insight into hybrid systems where symmetries strongly affect the SHG and enable tailored SHG in 1L-WS2 for future applications.
RESUMEN
A 58 MHz femtosecond Ti:sapphire oscillator is optimized for long wavelength operation beyond 900 nm. Sub 30 fs, approximately 3 nJ pulses with a bandwidth exceeding 20 THz are realized for central wavelengths 900 nm < or = lambda < or = 960 nm. This laser opens up new perspectives for the sensitive time-resolved spectroscopy of various semiconductor nanostructures. Moreover, its second harmonic serves as a source of visible multi-milliwatt femtosecond pulses tunable around 475 nm.