Optical probing of ultrafast laser-induced solid-to-overdense-plasma transitions.

Understanding the solid target dynamics resulting from the interaction with an ultrashort laser pulse is a challenging fundamental multi-physics problem involving atomic and solid-state physics, plasma physics, and laser physics. Knowledge of the initial interplay of the underlying processes is essential to many applications ranging from low-power laser regimes like laser-induced ablation to high-power laser regimes like laser-driven ion acceleration. Accessing the properties of the so-called pre-plasma formed as the laser pulse's rising edge ionizes the target is complicated from the theoretical and experimental point of view, and many aspects of this laser-induced transition from solid to overdense plasma over picosecond timescales are still open questions. On the one hand, laser-driven ion acceleration requires precise control of the pre-plasma because the efficiency of the acceleration process crucially depends on the target properties at the arrival of the relativistic intensity peak of the pulse. On the other hand, efficient laser ablation requires, for example, preventing the so-called "plasma shielding". By capturing the dynamics of the initial stage of the interaction, we report on a detailed visualization of the pre-plasma formation and evolution. Nanometer-thin diamond-like carbon foils are shown to transition from solid to plasma during the laser rising edge with intensities < 1016 W/cm². Single-shot near-infrared probe transmission measurements evidence sub-picosecond dynamics of an expanding plasma with densities above 1023 cm-3 (about 100 times the critical plasma density). The complementarity of a solid-state interaction model and kinetic plasma description provides deep insight into the interplay of initial ionization, collisions, and expansion.

THz to far-infrared spectra of the known crystal polymorphs of phenylalanine.

There is renewed interest in the structure of the essential amino acid phenylalanine in the solid state. Three new polymorphs were found in the years 2012 to 2014. Here, we investigate the structure, stability, and energetical ordering of these phases using first-principles simulations at the level of density functional theory incorporating van der Waals interactions. Two of the distinct crystal forms are found to be structurally similar and energetically very close after vibrational free energy corrections have been taken into account. Infrared absorption spectra are likewise calculated and compared to experimental measurements. By combining measurements obtained with a commercial Fourier transform infra-red spectrometer and a homemade air-photonics-based THz time domain spectrometer, we could carry out this comparison in the vibrational frequency region from 1 to 40 THz. The excellent agreement of the line positions and the established energy ranking allow us to identify the most stable polymorph of phenylalanine.

Terahertz pulse generation by multi-color laser fields with linear versus circular polarization: erratum.

We present an erratum to our Letter [Opt. Lett.46, 5906 (2021)10.1364/OL.442519]. This erratum corrects the caption of Fig. 2, which contains confusing information. This correction does not affect any of the results or the conclusions of the original Letter.

Frequency-resolved characterization of broadband two-color air-plasma terahertz beam profiles.

The frequency-resolved terahertz (THz) beam profile characteristics of a two-color air-plasma THz source were investigated in the broadband frequency range (1-15 THz). The frequency resolution is achieved by combining THz waveform measurements and the knife-edge technique. Our results show that the THz focal spot size is strongly frequency dependent. This has important implications on nonlinear THz spectroscopy applications where accurate knowledge of the applied THz electrical field strength onto the sample is important. In addition, the transition between the solid and hollow beam profile of the air-plasma THz beam was carefully identified. Far from the focus, the features across the 1-15 THz range have also been carefully examined, revealing the characteristic conical emission patterns at all frequencies.

Terahertz pulse generation by multi-color laser fields with linear versus circular polarization.

We study the influence of the polarization state of multi-color femtosecond laser pulses ionizing air or noble gases on the emitted terahertz radiation. A local-current model and plane wave evaluations predict a cross-over in the THz energy yields with increasing number of pump harmonics, for which circular laser polarization is more efficient for a few harmonics, and linear polarization is favorable for more than six pump colors. Comprehensive 3D numerical simulations of gas jet experiments confirm this property for singly and multiply ionized gases. Rotation of the THz polarization ellipse in the case of circular laser polarization is explained by phase shifts that may alter the phase angle between the harmonics.

Shaping convex edges in borosilicate glass by single pass perforation with an Airy beam.

We demonstrate curved modifications with lengths of up to 2 mm within borosilicate glass produced by single 1030 nm picosecond laser shots with an Airy beam profile. Plasma ignition in the sidelobes of the beam as well as surface damage prove to be the crucial limitations for confined bulk energy deposition on a curved trajectory. A combined experimental and numerical analysis reveals optimum laser parameters for confined bulk energy deposition. This way, we achieved single pass perforation of a 525 µm thick glass sheet and separation by a subsequent etching step, resulting in a well-defined convex edge down to a radius of curvature of 774 µm.

Intensity modulated terahertz vortex wave generation in air plasma by two-color femtosecond laser pulses.

We investigate the generation of broadband terahertz (THz) pulses with phase singularity from air plasmas created by fundamental and second harmonic laser pulses. We show that when the second harmonic beam carries a vortex charge, the THz beam acquires a vortex structure as well. A generic feature of this THz vortex is that the intensity is modulated along the azimuthal angle, which can be attributed to the spatially varying relative phase difference between the two pump harmonics. Fully space- and time-resolved numerical simulations reveal that transverse instabilities of the pump further affect the emitted THz field along nonlinear propagation, which may produce additional singularities resulting in a rich vortex structure. The predicted intensity modulation is experimentally demonstrated with a thermal camera, in excellent agreement with simulation results. The presence of phase singularities in the experiment is revealed by astigmatic transformation of the beam using a cylindrical mirror.

Spatiotemporal rogue events in optical multiple filamentation.

The transient appearance of bright spots in the beam profile of optical filaments formed in xenon is experimentally investigated. Fluence profiles are recorded with high-speed optical cameras at the kilohertz repetition rate of the laser source. A statistical analysis reveals a thresholdlike appearance of heavy-tailed fluence distributions together with the transition from single to multiple filamentation. The multifilament scenario exhibits near-exponential probability density functions, with extreme events exceeding the significant wave height by more than a factor of 10. The extreme events are isolated in space and in time. The macroscopic origin of these experimentally observed heavy-tail statistics is shown to be local refractive index variations inside the nonlinear medium, induced by multiphoton absorption and subsequent plasma thermalization. Microscopically, mergers between filament strings appear to play a decisive role in the observed rogue wave statistics.

3D numerical simulations of THz generation by two-color laser filaments.

Terahertz (THz) radiation produced by the filamentation of two-color pulses over long distances in argon is numerically investigated using a comprehensive model in full space-time-resolved geometry. We show that the dominant physical mechanism for THz generation in the filamentation regime at clamping intensity is based on quasi-dc plasma currents. The calculated THz spectra for different pump pulse energies and pulse durations are in agreement with previously reported experimental observations. For the same pulse parameters, near-infrared pump pulses at 2 µm are shown to generate a more than 1 order of magnitude greater THz yield than pumps centered at 800 nm.

Azimuthons in weakly nonlinear waveguides of different symmetries.

We show that weakly guiding nonlinear waveguides support stable propagation of rotating spatial solitons (azimuthons). We investigate the role of waveguide symmetry on the soliton rotation. We find that azimuthons in circular waveguides always rotate rigidly during propagation and the analytically predicted rotation frequency is in excellent agreement with numerical simulations. On the other hand, azimuthons in square waveguides may experience spatial deformation during propagation. Moreover, we show that there is a critical value for the modulation depth of azimuthons above which solitons just wobble back and forth, and below which they rotate continuously. We explain these dynamics using the concept of energy difference between different orientations of the azimuthon.

Self-pinching of pulsed laser beams during filamentary propagation.

Competing nonlinear optical effects that act on femtosecond laser pulses propagating in a self-generated light filament may give rise to a pronounced radial beam deformation, similar to the z-pinch contraction of pulsed high-current discharges. This self-generated spatial beam contraction is accompanied by a pulse break-up that can be beneficially exploited for on-axis temporal compression of the pulse. The pinching mechanism therefore explains the recently observed self-compression and the complicated spatio-temporal shapes typical for filament propagation experiments.

Stable rotating dipole solitons in nonlocal optical media.

We reveal that nonlocality can provide a simple physical mechanism for stabilization of multihump optical solitons and present what we believe to be the first example of stable rotating dipole solitons and soliton spiraling, which are known to be unstable in all types of realistic nonlinear media with a local response.

Self-compression by femtosecond pulse filamentation: experiments versus numerical simulations.

We analyze pulse self-compression in femtosecond filaments, both experimentally and numerically. We experimentally demonstrate the compression of 45 fs pulses down to a duration of 7.4 fs at millijoule pulse energies. This sixfold compression in a self-generated filament does not require any means for dispersion compensation and is highly efficient. We compare our results to numerical simulations, providing a complete propagation model that accounts for full dispersion, pressure variations, Kerr nonlinearity and plasma generation in multiphoton and tunnel regimes. The equations are numerically integrated and allow for a quantitative comparison with the experiment. Our experiments and numerical simulations reveal a characteristic spectrotemporal structure of the self-compressed pulses, consisting of a compressible blue wing and an incompressible red pedestal. We explain the underlying mechanism that leads to this structure and examine the scalability of filament self-compression with respect to pulse energy and gas pressure.

Chirp-induced dynamics of femtosecond filaments in air.

We investigate the influence of a chirped phase on femtosecond pulses propagating in air. Pulses with an initially negative chirp are temporally compressed by compensation with group-velocity dispersion. We demonstrate that this property, combined with plasma defocusing, can be used to trigger filamentation at different foci, increase self-guiding ranges, or even shorten pulse duration.

Intense pulses in air: breakup of rotational symmetry.

We investigate azimuthal instabilities of intense rotationally symmetric pulsed beams propagating in air. Although the spatial-temporal evolution of the field is strongly influenced by the onset of plasma generation, the instabilities are caused chiefly by the Kerr effect. We conclude that calculations that assume rotational symmetry become unrealistic because of the fast growth of azimuthal instabilities shortly after the onset of plasma generation.