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Unlocking the true potential of optical spectroscopy on the nanoscale requires development of stable and low-noise laser sources. Here, we have developed a low-noise supercontinuum (SC) source based on an all-normal dispersion fiber pumped by a femtosecond fiber laser and demonstrate high resolution, spectrally resolved near-field measurements in the near-infrared (NIR) region. Specifically, we explore the reduced-noise requirements for aperture-less scattering-type scanning near-field optical microscopy (s-SNOM), including inherent pulse-to-pulse fluctuation of the SC. We use our SC light source to demonstrate the first NIR, spectrally resolved s-SNOM measurement, a situation where state-of-the-art commercial SC sources are too noisy to be useful. We map the propagation of surface plasmon polariton (SPP) waves on monocrystalline gold platelets in the wavelength region of 1.34-1.75 μm in a single measurement, thereby characterizing experimentally the dispersion curve of the SPP in the NIR. Our results represent a technological breakthrough that has the potential to enable a wide range of new applications of low-noise SC sources in near-field studies.

We demonstrate the first megahertz (MHz) repetition-rate, broadband terahertz (THz) source based on optical rectification in the organic crystal HMQ-TMS driven by a femtosecond Yb:fibre laser. Pumping at 1035 nm with 30 fs pulses, we achieve few-cycle THz emission with a smooth multi-octave spectrum that extends up to 6 THz at -30 dB, with conversion efficiencies reaching 10-4 and an average output power of up to 0.38 mW. We assess the thermal damage limit of the crystal and conclude a maximum fluence of ∼1.8 mJ·cm-2 at 10 MHz with a 1/e2 pump beam diameter of 0.10 mm. We compare the performance of HMQ-TMS with the prototypical inorganic crystal gallium phosphide (GaP), yielding a tenfold electric field increase with a peak on-axis field strength of 7 kV·cm-1 and almost double the THz bandwidth. Our results further demonstrate the suitability of organic crystals in combination with fibre lasers for repetition-rate scaling of broadband, high-power THz sources for time-domain spectroscopic applications.

We use mono-crystalline gold platelets with ultra-smooth surfaces and superior plasmonic properties to investigate the formation of interference patterns caused by surface plasmon polaritons (SPPs) with scattering-type scanning near-field microscopy at 521 and 633 nm. By applying a Fourier analysis approach, we can identify and separate several signal channels related to SPPs launched and scattered by the atomic force microscopy tip and the edges of the platelet. Especially at the excitation wavelength of 633 nm, we can isolate a region in the center of the platelets where we find only contributions of SPPs which are launched by the tip and reflected at the edges. These signatures are used to determine the SPP wavelength of λSPP = 606 nm in good agreement with theoretical predictions. Furthermore, we were still able to measure SPP signals after 20 μm propagation, which demonstrates impressively the superior plasmonic quality of these mono-crystalline gold platelets.

We demonstrate the first megahertz (MHz) repetition-rate, broadband terahertz (THz) source based on optical rectification in the organic crystal HMQ-TMS driven by a femtosecond Yb:fibre laser. Pumping at 1035 nm with 30 fs pulses, we achieve few-cycle THz emission with a smooth multi-octave spectrum that extends up to 6 THz at -30 dB, with conversion efficiencies reaching 10-4 and an average output power of up to 0.38 mW.We assess the thermal damage limit of the crystal and conclude a maximum fluence of ∼1.8 mJ cm-2 at 10 MHz with a 1/e2 pump beam diameter of 0.10 mm. We compare the performance of HMQ-TMS with the prototypical inorganic crystal gallium phosphide (GaP), yielding a tenfold electric field increase with a peak on-axis field strength of 7 kV cm-1 and almost double the THz bandwidth. Our results further demonstrate the suitability of organic crystals in combination with fibre lasers for repetition-rate scaling of broadband, high-power THz sources for time-domain spectroscopic applications.

We investigate single-cycle terahertz (THz) field-induced nonlinear absorption in doped silicon carbide. We find that the nonlinear response is ultrafast, and we observe up to 20% reduction of transmission of single THz pulses at peak field strengths of 280 kV/cm. We model the field and temperature dependence of the nonlinear response by a finite-difference time-domain simulation that incorporates the temporally nonlocal nonlinear conductivity of the silicon carbide. Nonlinear two-dimensional THz spectroscopy reveals that the nonlinear absorption has an ultrafast subpicosecond recovery time, with contributions from both sum-frequency generation and four-wave mixing, in the form of a photon-echo signal. The ultrafast nonlinearity with its equally fast recovery time makes silicon carbide an interesting candidate material for extremely fast nonlinear THz modulators.

Terahertz pulses are very popular because of their numerous applications, for example in security. Located between microwaves and optical waves in the electromagnetic spectrum, their spectral domain can now be exploited for molecular spectroscopy using terahertz emission from plasmas formed by femtosecond laser pulses ionizing gases such as air. Downconversion of broadband optical spectra in a plasma produces intense radiation suitable for the detection of suspect materials remotely. The different physical mechanisms involved to create terahertz radiation by laser-matter interaction are reviewed. The new potentialities offered by intense ultrafast lasers allow the acquisition of unique spectral signatures characterizing various materials.