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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.
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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.
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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.
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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.
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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.
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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.
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We numerically study the filamentation of ultrashort laser pulses at 2 microm carrier wavelength in noble gases (argon, xenon) and in air. Compared with filamentation in the near-visible domain (800 nm), mid-infrared optical sources with durations close to a single cycle can be generically produced at various pressures and powers near the self-focusing threshold. The mechanism by which self-compression takes place mainly involves optical self-focusing, pulse steepening and plasma defocusing. On-axis spectra and spectral phases are discussed. Delivering single-cycled pulses at long wavelengths has important applications in the generation of high-order harmonics and isolated attosecond pulses.
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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.
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An optical self-guiding of femtosecond filaments in air is identified in a regime where plasma generation ceases to support the self-channeling process. Group-velocity dispersion is shown to keep the beam temporally and spatially localized upon a few meters by taking over the ionization of air molecules, once the pulse peak power becomes close to the self-focusing threshold. In this regime, the pulse undergoes slow splitting events that maintain a residual self-guiding with light intensities as high as 10 TW/cm2, as soon as the electron plasma density has fallen down below 10(15) cm(-3).
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Two femtosecond pulses in convergent geometry are combined with an appropriate time delay, in order to double the length of the plasma channel created by multiphoton ionization of air. Suitable parameters are estimated analytically and tested by direct numerical simulations.
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The nonlinear propagation of femtosecond pulses in pressure-gas cells filled with argon is investigated. By increasing the pressure for reaching peak power levels close to the threshold for self-focusing, it is shown that either group-velocity dispersion or multiphoton ionizing (MPI) sources can become key players for arresting the beam collapse. For input powers noticeably above critical, MPI rapidly dominates and the formation of self-guided filaments of light occurs. We discuss the dynamical role of MPI in shortening the pulse duration up to the optical cycle limit. Two different wavelength domains are commented. The influence of space-time focusing and self-steepening effects is furthermore discussed. Their respective roles in promoting shock structures are studied and shown to still promote pulse shortening in suitable power regimes. Finally, spectral broadening is analyzed and proven to be more important for large laser wavelengths. Numerical integration of the propagation equations is explained in the light of analytical arguments.
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We analyze the shape and stability of localized states in nonlinear cubic media with space-dependent potentials modeling an inhomogeneity. By means of a static variational approach, we describe the ground states and vortexlike stationary solutions, either in dilute atom gases or in optical cavities, with an emphasis on parabolic-type potentials. First, we determine the existence conditions for soliton and vortex structures for both focusing and defocusing nonlinearity. It is shown that, even for a defocusing medium, soliton modes can exist with a confining potential. Second, step potentials and boundedness effects in hollow capillaries are investigated, which both proceed from a similar analysis. Finally, we discuss applications of this procedure to charged vortices in dilute quantum gases and to Bose-Einstein condensates trapped in the presence of a light-induced Gaussian barrier.
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We examine the nonlinear dynamics of femtosecond filaments in air at different pressures. Emphasis is placed on the changes in multiple filamentation patterns produced by terawatt laser pulses. Principal modifications induced by pressure variations apply to the onset distance, size, and number of the filaments inside the laser bundle.
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We examine the robustness of ultrashort optical vortices propagating freely in the atmosphere. We first approximate the stability regions of femtosecond spinning pulses as a function of their topological charge. Next, we numerically demonstrate that atmospheric optical vortices are capable of conveying high power levels in air over hundreds of meters before they break up into filaments.
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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.
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Femtosecond light pulses interacting with solids are studied. With a power close to the self-focusing threshold, an optical pulse evolves like a solitary wave with a temporal duration shrunk to a few femtoseconds through the defocusing action of multiphoton ionization. Self-steepening and space-time focusing are shown to form shock profiles, which do not prevent the pulse from keeping a shorter duration over one Rayleigh length. Theoretical estimates justify the key mechanisms leading to pulse compression, whose influence on the power spectra is finally discussed.