Following the Nonthermal Phase Transition in Niobium Dioxide by Time-Resolved Harmonic Spectroscopy.

Photoinduced phase transitions in correlated materials promise diverse applications from ultrafast switches to optoelectronics. Resolving those transitions and possible metastable phases temporally are key enablers for these applications, but challenge existing experimental approaches. Extreme nonlinear optics can help probe phase changes, as higher-order nonlinearities have higher sensitivity and temporal resolution to band structure and lattice deformations. Here the ultrafast transition from the semiconducting to the metallic phases in polycrystalline thin-film NbO_{2} is investigated by time-resolved harmonic spectroscopy. The emission strength of all harmonic orders shows a steplike suppression when the excitation fluence exceeds a threshold (∼11-12 mJ/cm^{2}), below the fluence required for the thermal transition-a signature of the nonthermal emergence of a metallic phase within 100±20 fs. This observation is backed by full ab initio simulations as well as a 1D chain model of high-harmonic generation from both phases. Our results demonstrate femtosecond harmonic probing of phase transitions and nonthermal dynamics in solids.

Ultrafast laser-induced strain waves in thin ruthenium layers.

We report on the time-dependent optical diffraction from ultra-high frequency laser-induced acoustic waves in thin layers of ruthenium deposited on glass substrates. We show that the thermo-optic and strain-optic effects dominate the optical response of Ru layers to a traveling longitudinal strain wave. In addition, we show the generation and detection of acoustic waves with a central frequency ranging from 130 GHz to 750 GHz on ultra-thin layers with thicknesses in the range of 1.2 - 20 nm. For these ultra-thin layers we measure a strong dependency of the speed of sound on the layer thickness and, thus, the frequency. This frequency-dependent speed of sound results in a frequency-dependent acoustic impedance mismatch between the ruthenium and the glass substrate, leading to a faster decay of the measured signals for increasing frequency. Furthermore, for these extremely high-frequency oscillations, we find that the frequency and phase remain constant for times longer than about 2 ps after optical excitation. Back extrapolation of the acquired acoustic signals to t = 0 gives a starting phase of -π/2. As this seems unlikely, we interpret this as an indication of possible dynamic changes in the phase/frequency of the acoustic wave in the first 2 ps after excitation.

Femtosecond time-resolved pump-probe measurements on percolating gold in the ablation regime.

We report on femtosecond laser ablation experiments on percolating gold layers deposited on a glass substrate. In our experiments, we measure changes in optical transmission and reflection induced by single, high-intensity infrared laser pulses as a function of the time delay between the pump and the probe. For the highest pump intensities we find that on a time scale of about 150 ps after excitation, the transmission and reflection approach values close to the substrate values. We attribute this rapid ablation to vaporization of the entire layer when the injected energy exceeds the cohesive energy of the material. This vaporization results in the rapid transformation of the gold layer into a sufficiently dilute mist of atoms and nano-particles which renders the material almost optically transparent to the probe pulse. SEM images of the surfaces show how the morphology of the films changes at relatively low excitation intensities and show the complete removal of the gold at high intensities. We find that the ablation threshold for percolating Au on glass is 2.3 × 1011 W/cm2, which is two orders of magnitude lower than the damage threshold for continuous gold layers as reported in the literature.

Detection of periodic structures through opaque metal layers by optical measurements of ultrafast electron dynamics.

We report on femtosecond optical pump-probe measurements of ultrafast electron dynamics to detect the presence of gratings buried underneath optically opaque gold layers. Electron energy diffusion and cooling are found to be strongly affected by the presence and type of metal buried below the gold layer. As a result, the spatially periodic buried grating is encoded on the electron temperature near the top surface, leading to a spatially periodic modulation of the optical properties near the gold surface from which a delayed probe pulse can be diffracted. Our measurements show that these effects may be useful for optical detection and alignment applications in semiconductor device manufacturing.

Terahertz near-field spectroscopy of filled subwavelength sized apertures in thin metal films.

We have measured terahertz near-field spectra of cesium iodide crystals as small as ~10 µm in diameter, which were deposited on single, sub-wavelength-sized apertures created in thin gold films on a substrate. The advantage of using small apertures for terahertz microspectroscopy is that only terahertz light that has interacted with the cesium iodide is observed. We find that around the transverse optical phonon frequency of cesium iodide, the amplitude transmission is as much influenced by the refractive index as by the absorption. We show that the ability to measure in the near-field of the apertures, where signals are relatively strong, allows us to measure on sample volumes as small as ~5×10(-16) m(3).

Electromagnetic spin-orbit interactions via scattering of subwavelength apertures.

Circularly polarized electric fields incident on subwavelength apertures produce near-field phase singularities with phase vorticity +/-1 depending on the polarization handedness. These near-field phase singularities combine with those associated with orbital angular momentum and result in polarization-dependent transmission. We produce arbitrary phase vorticity in the longitudinal component of scattered electric fields by varying the incident beam and aperture configuration.

Influence of the dielectric substrate on the terahertz electric near-field of a hole in a metal.

We have studied theoretically and experimentally the influence of a dielectric substrate on the frequency-dependent terahertz electric near-field of a small hole in a metal layer. We find that the near-field transmission spectrum and the two-dimensional field distribution of an empty hole in a thin metal layer on a substrate are almost identical to that of a hole which is also filled with the same dielectric material as the substrate. For thicker metal layers, however, the near-field spectra of filled and unfilled holes become very different. In addition, for thick metal layers, the two-dimensional field distributions are more strongly affected by the substrate, especially if we allow for an air gap between the metal and the substrate. Our results validate the -somewhat unusual- two-dimensional field distribution measured beneath a hole in a thick metal foil and highlight the effect that a substrate can have on the measurement of the near-field of an object.

Terahertz near-field vectorial imaging of subwavelength apertures and aperture arrays.

We present measurements of the complete terahertz (THz) electric near-field distribution, E(x), E(y) and E(z), in both the time- and frequency-domains, for subwavelength apertures and subsections of subwavelength aperture arrays. Measuring the individual components of the THz near-field with subwavelength spatial resolution, as they emerge from these structures, illustrates how the field interacts with the apertures. We observe the small but measurable y- and z-components of the electric field for both single apertures and arrays. Resonant contributions, attributed to Bloch modes, are detected and we observe the presence of a longitudinal field component, E(z), within the different array apertures, which can be attributed to a diffractive effect. These measurements illustrate in detail the individual THz field components emerging from subwavelength apertures and provide a direct measure of two important mechanisms that contribute to the net transmission of light through arrays.

Near field imaging of terahertz focusing onto rectangular apertures.

We performed terahertz near-field experiments on single rectangular holes with various lengths grown on an electro-optic crystal substrate with lambda/100 resolution. We find that the near-field amplitude becomes proportionally larger as the rectangle becomes narrower, strongly suggesting that a constant energy passes through even for a very narrow slit. The occurrence of a large field enhancement at the fundamental localized resonance is discussed confirming the funneling of energy at the near-field.

Advanced terahertz electric near-field measurements at sub-wavelength diameter metallic apertures.

Using terahertz-light excitation, we have measured with sub-wavelength spatial, and sub-cycle temporal resolution the time- and frequency-dependent electric-field and surface-charge density in the vicinity of small metallic holes. In addition to a singularity like concentration of the electric field near the hole edges, we observe, that holes can act as differential operators whose near-field output is the time-derivative of the incident electric field. Our results confirm the well-known predictions made by Bouwkamp, Philips Res. Rep. 5, 321-332 (1950), and reveal, with unprecedented detail, what physically happens when light passes through a small hole.

Fourier-transform terahertz near-field imaging of one-dimensional slit arrays: mapping of electric-field-, magnetic-field-, and Poynting vectors.

We present 2D measurements of the full THz electric field behind a sample consisting of multiple slits in a metal foil. Our measurements, which have a sub-wavelength spatial, and a sub-period temporal resolution, reveal electric field lines, electric field vortices and saddle points. From our measurements we are able to reconstruct the magnetic field and, finally, the position and time-dependent Poynting vector which shows the flow of energy behind the sample. Our results show that it is possible to study the flow of light near sub-wavelength plasmonic structures such as slit-arrays and, by implication, other metamaterial samples.

Spot-size reduction in terahertz apertureless near-field imaging.

We show measurements and calculations of the terahertz (THz) near field of a metal tip with a specially formed, semicircular apex that allows us to identify the separate contributions of the tip apex and shaft to the measured signal. We find that when the tip-crystal distance is not modulated the measured near-field signal is overwhelmed by contributions from the tip shaft, resulting in a relatively large THz spot size. When the tip-crystal distance is modulated, with subsequent lock-in detection at the modulation frequency, only the near-field distribution of the semicircular apex is observed, resulting in a much smaller THz spot size and thus improved spatial resolution.

Towards terahertz near-field microscopy.

We have detected sub-wavelength spot sizes in the near-field of a metal tip, which is illuminated with terahertz (THz) pulses. The THz near-field is detected by using electro-optic detection in a (100) oriented GaP crystal. Contrary to conventional electro-optic detection, which uses (110) oriented detection crystals, (100) crystals only allow the detection of THz light, polarized perpendicular to our crystal surface. This component is strongly localized near the apex of the tip, which has sub-wavelength dimensions. The detection process is blind to the incident THz radiation, which is polarized parallel to the crystal surface. As a result, a sub-wavelength THz spot size with an intensity full-width half maximum (FWHM) diameter of lambda/200 is observed.

Measurement of THz Spot Sizes with a λ/200 Diameter in the Near-Field of a Metal Tip.

We report on a method to obtain asub-wavelength resolution in terahertz time-domain imaging. In our method,a sharp copper tip is used to locallydistort and concentrate the THz electricfield. The distorted electric field, presentmainly in the near field of the tip, iselectro-optically measured in an (100)oriented GaP crystal. By raster scanning the tipalong the surface of the crystal we find asmallest THz spot size of 10 µm forfrequencies from 0.1 to 2.5 THz. For ourpeak frequency of 0.15 THz this corresponds to aresolution of λ/200. Our setup has thepotential to reach a resolution down to afew µm, and is a promising candidate tostudy single, living cells in the THzfrequency range.

A terahertz system using semi-large emitters: noise and performance characteristics.

We have built a relatively simple, highly efficient, terahertz (THz) emission and detection system centred around a 15 fs Ti:sapphire laser. In the system, 200 mW of laser power is focused on a 120 microm diameter spot between two silverpaint electrodes on the surface of a semi-insulating GaAs crystal, kept at a temperature near 300 K, biased with a 50 kHz, +/- 400 V square wave. Using rapid delay scanning and lock-in detection at 50 kHz, we obtain probe laser quantum-noise limited signals using a standard electro-optic detection scheme with a 1 mm thick (110) oriented ZnTe crystal. The maximum THz-induced differential signal that we observe is deltaP/P = 7 x 10(-3), corresponding to a THz peak amplitude of 95 V cm(-1). The THz average power was measured to be about 40 microW, to our knowledge the highest power reported so far generated with Ti:sapphire oscillators as a pump source. The system uses off-the-shelf electronics and requires no microfabrication techniques.