Vacuum-free femtosecond fiber laser microplasma X-ray source for radiography.

Radiographic imaging using X-rays is a tool for basic research and applications in industry, materials science, and medical diagnostics. In this article, we present a novel approach for the generation of X-rays using a vacuum-free microplasma by femtosecond fiber laser. By tightly focusing a laser pulse onto a micrometer-sized solid density near-surface plasma from a rotating copper target, we demonstrate the generation of Cu K-photons (8-9 keV) with high yield ∼ 1.6 × 109 phot/s/2π, and with a source size diameter of approximately 10 microns. Femtosecond fiber laser allows working with a high repetition rate (∼2 MHz) and moderate energy levels (10-40 µJ), ensuring the effective quasi-continuous generation of X-ray photons. Furthermore, we introduce a hybrid scheme that combines the tightly focusing laser-plasma X-ray generator with an online control unit for microplasma size source based on the back-reflected second harmonic generated in the laser-induced microplasma. The compactness and high performance of this vacuum-free femtosecond fiber laser microplasma X-ray source makes it a promising solution for advanced radiographic applications. Our preliminary results on the creation of a microfocus X-ray source provide insights into the feasibility and potential of this innovative approach.

Single-shot femtosecond bulk micromachining of silicon with mid-IR tightly focused beams.

Being the second most abundant element on earth after oxygen, silicon remains the working horse for key technologies for the years. Novel photonics platform for high-speed data transfer and optical memory demands higher flexibility of the silicon modification, including on-chip and in-bulk inscription regimes. These are deepness, three-dimensionality, controllability of sizes and morphology of created modifications. Mid-IR (beyond 4 µm) ultrafast lasers provide the required control for all these parameters not only on the surface (as in the case of the lithographic techniques), but also inside the bulk of the semiconductor, paving the way to an unprecedented variety of properties that can be encoded via such an excitation. We estimated the deposited energy density as 6 kJ cm-3 inside silicon under tight focusing of mid-IR femtosecond laser radiation, which exceeds the threshold value determined by the specific heat of fusion (~ 4 kJ cm-3). In such a regime, we successfully performed single-pulse silicon microstructuring. Using third-harmonic and near-IR microscopy, and molecular dynamics, we demonstrated that there is a low-density region in the center of a micromodification, surrounded by a "ring" with higher density, that could be an evidence of its micro-void structure. The formation of created micromodification could be controlled in situ using third-harmonic generation microscopy. The numerical simulation indicates that single-shot damage becomes possible due to electrons heating in the conduction band up to 8 eV (mean thermal energy) and the subsequent generation of microplasma with an overcritical density of 8.5 × 1021 cm-3. These results promise to be the foundation of a new approach of deep three-dimensional single-shot bulk micromachining of silicon.

Dynamics of ultrafast phase transitions in MgF2 triggered by laser-induced THz coherent phonons.

The advent of free-electron lasers opens new routes for experimental high-pressure physics, which allows studying dynamics of condensed matter with femtosecond resolution. A rapid compression, that can be caused by laser-induced shock impact, leads to the cascade of high-pressure phase transitions. Despite many decades of study, a complete understanding of the lattice response to such a compression remains elusive. Moreover, in the dynamical case (in contrast to quasi-static loading) the thresholds of phase transitions can change significantly. Using the third harmonic pump-probe technique combined with molecular dynamics to simulate the terahertz (THz) spectrum, we revealed the dynamics of ultrafast laser-induced phase transitions in MgF2 in all-optical experiment. Tight focusing of femtosecond laser pulse into the transparent medium leads to the generation of sub-TPa shock waves and THz coherent phonons. The laser-induced shock wave propagation drastically displaces atoms in the lattice, which leads to phase transitions. We registered a cascade of ultrafast laser-induced phase transitions (P42/mnm ⇒ Pa-3 ⇒ Pnam) in magnesium fluoride as a change in the spectrum of coherent phonons. The phase transition has the characteristic time of 5-10 ps, and the lifetime of each phase is on the order of 40-60 ps. In addition, phonon density of states, simulated by molecular dynamics, together with third-harmonic time-resolved spectra prove that laser-excited phonons in a bulk of dielectrics are generated by displacive excitation (DECP) mechanism in plasma mediated conditions.

Dynamics of Ultrafast Phase Transitions in (001) Si on the Shock-Wave Front.

We demonstrate an ultrafast (<0.1 ps) reversible phase transition in silicon (Si) under ultrafast pressure loading using molecular dynamics. Si changes its structure from cubic diamond to ß-Sn on the shock-wave front. The phase transition occurs when the shock-wave pressure exceeds 11 GPa. Atomic volume, centrosymmetry, and the X-ray-diffraction spectrum were revealed as effective indicators of phase-transition dynamics. The latter, being registered in actual experimental conditions, constitutes a breakthrough in the path towards simple X-ray optical cross-correlation and pump-probe experiments.

Time-resolved optical probing of the non-equilibrium supercritical state in molecular media under ns laser-plasma impact.

We proposed a complex method based on a combination of shadow photography and time-resolved Raman spectroscopy to observe the non-stationary laser-induced supercritical state in molecular media. Shadow photography is applied for retrieving pressure values, while Raman spectroscopy with molecular dynamics for temperature estimation. Time resolution of 0.25 ns is achieved by varying the delay between the pump (creating an extreme energy delivery) and the probe laser pulses by the self-made digital delay electronic circuit . The proposed method was employed in liquid carbon dioxide and water. Under nanosecond laser pulse impact, the estimated temperatures and pressures (∼700 K and ∼0.5 GPa) achieved in media are higher than the critical parameters of the samples.

The Anomalous Behavior of Thermodynamic Parameters in the Three Widom Deltas of Carbon Dioxide-Ethanol Mixture.

Using molecular dynamics, we demonstrated that in the mixture of carbon dioxide and ethanol (25% molar fraction) there are three pronounced regions on the p-T diagram characterized by not only high-density fluctuations but also anomalous behavior of thermodynamic parameters. The regions are interpreted as Widom deltas. The regions were identified as a result of analyzing the dependences of density, density fluctuations, isobaric thermal conductivity, and clustering of a mixture of carbon dioxide and ethanol in a wide range of pressures and temperatures. Two of the regions correspond to the Widom delta for pure supercritical carbon dioxide and ethanol, while the third region is in the immediate vicinity of the critical point of the binary mixture. The origin of these Widom deltas is a result of the large mixed linear clusters formation.

Optical Diagnostics of Supercritical CO2 and CO2-Ethanol Mixture in the Widom Delta.

The supercritical CO2 (scCO2) is widely used as solvent and transport media in different technologies. The technological aspects of scCO2 fluid applications strongly depend on spatial-temporal fluctuations of its thermodynamic parameters. The region of these parameters' maximal fluctuations on the p-T (pressure-temperature) diagram is called Widom delta. It has significant practical and fundamental interest. We offer an approach that combines optical measurements and molecular dynamics simulation in a wide range of pressures and temperatures. We studied the microstructure of supercritical CO2 fluid and its binary mixture with ethanol in a wide range of temperatures and pressures using molecular dynamics (MD) simulation. MD is used to retrieve a set of optical characteristics such as Raman spectra, refractive indexes and molecular refraction and was verified by appropriate experimental measurements. We demonstrated that in the Widom delta the monotonic dependence of the optical properties on the CO2 density is violated. It is caused by the rapid increase of density fluctuations and medium-sized (20-30 molecules) cluster formation. We identified the correlation between cluster parameters and optical properties of the media; in particular, it is established that the clusters in the Widom delta acts as a seed for clustering in molecular jets. MD demonstrates that the cluster formation is stronger in the supercritical CO2-ethanol mixture, where the extended binary clusters are formed; that is, the nonlinear refractive index significantly increased. The influence of the supercritical state in the cell on the formation of supersonic cluster jets is studied using the Mie scattering technique.

Role of wavelength in photocarrier absorption and plasma formation threshold under excitation of dielectrics by high-intensity laser field tunable from visible to mid-IR.

The development of high power mid-IR laser applications requires a study on laser induced damage threshold (LIDT) in the mid-IR. In this paper we have measured the wavelength dependence of the plasma formation threshold (PFT) that is a LIDT precursor. In order to interpret the observed trends numerically, a model describing the laser induced electron dynamics, based on multiple rate equations, has been developed. We show both theoretically and experimentally that PFT at mid-IR wavelengths is controlled by a transition from weak- to strong-field regime of free carrier absorption. In the case of MgF[Formula: see text] this transition occurs around 3-4 [Formula: see text]m corresponding to the region of the lowermost PFT. The region of the uppermost PFT is reached around 1 [Formula: see text]m and is governed by an interplay of photoionization and weak-field free carrier absorption which manifests itself in both MgF[Formula: see text] and SiO[Formula: see text]. The PFT observed in considered materials exhibits a universal dependence on the excitation wavelength in dielectrics. Thus, the presented results pave the route towards efficient and controllable laser-induced material modifications and should be of direct interest to laser researchers and application engineers for prevention of laser-induced damage of optical components in high-intensity mid-IR laser systems.

Anomalous behavior of nonlinear refractive indexes of CO2 and Xe in supercritical states.

Direct measurement of pressure dependent nonlinear refractive index of CO2 and Xe in subcritical and supercritical states are reported. In the vicinity of the ridge (or the Widom line), corresponding to the maximum density fluctuations, the nonlinear refractive index reaches a maximum value (up to 4.8*10-20m2/W in CO2 and 3.5*10-20m2/W in Xe). Anomalous behavior of the nonlinear refractive index in the vicinity of a ridge is caused by the cluster formation. That corresponds to the results of our theoretical assumption based on the modified Langevin theory.

Generation of an adjustable multi-octave supercontinuum under near-IR filamentation in gaseous, supercritical, and liquid carbon dioxide.

A new supercontinuum (SC) source from high-pressure gas, liquid, and supercritical fluid CO2 aggregate states that covers more than two octaves (from 400 nm up to 2 µm) is successively reported by using a 200 fs pulsed pump at 1.24 µm under femtosecond filamentation. The key features of the proposed source are the highly adjustable nonlinear properties (comparable with condensed matter) of the medium. This allows an easy-to-achieve filamentation process, even at microjoule laser pulse energies, giving the ultrabright and broadband SC. The molecular vibrations significantly modify the SC spectrum; as a result, a bright peak in a 1.4-1.9 µm is generated. Its position could be finely tuned by the pressure and temperature. We report that the generation of the SC in the monofilamentation regime (unlike multifilamentation) is more stable and promising for seeded optical parametric amplifiers, and the most efficient SC generation is achieved in the liquid phase of CO2.