Few-cycle pulses of intense 800 nm light are used to probe ionization and dissociation of carbon disulfide in the intensity and temporal regime where rescattering is expected to dominate the laser-molecule interaction. The wavepacket of the rescattered electron destructively interferes with the anti-bonding $π$-orbital of CS$_2^+$ such that rescattering is effectively "switched off". Direct signature of enhanced ionization being "switched off" in the ultrashort domain is also obtained. Consequently, dissociation becomes an almost non-existent channel when few-cycle pulses are used, with only long-lived singly-, doubly-, and triply-charged molecular ions dominating the mass spectrum. Few-cycle optical pulses help reveal that quantum-mechanically determined molecular symmetry contributes to strong field molecular ionization.
We revisit a recently proposed scheme [M.F. Ciappina et al 2019 Phys. Rev. A 99 043405] for accurate measurement of electromagnetic radiation intensities in a focus of high-power laser beams. The method is based on the observation of multiple sequential tunneling ionization of atoms and suggests the determination of the peak intensity value from the appearance in the focal area ions with a certain charge number. Here we study the sensitivity of the approach to two essential factors: the focal volume effect and the tunneling ionization model chosen to calculate ionization rates. We show, on the…
Intense, 100 fs laser pulses at 3.2 and 3.6 um are used to generate, by multi-photon ionization, broadband wave packets with up to 400 eV of kinetic energy and charge states up to Xe+6. The multiple ionization pathways are well described by a white electron wave packet and field-free inelastic cross sections, averaged over the intensity-dependent energy distribution for (e,ne) electron impact ionization. The analysis also suggests a contribution from a 4d core excitation in xenon.
Intense attosecond magnetic field pulses are predicted to be produced by intense few cycle circularly polarized UV pulses. Numerical solutions of the time dependent Schrödinger equation for H$_2^+$ are used to study the dynamical process. Spiralling attosecond circular electron wave packets are created with nanometer molecular dimensions, thus generating magnetic fields of several tens of Teslas ($10^5$ Gauss). Simulations show that the induced magnetic field is critically dependent on the pulse wavelength $λ$ and pulse duration $nτ$ ($n$ number of cycle) as predicted by a classical model. For…
We report on tunnel ionization of Xe by 2-cycle, intense, infrared laser pulses and its dependence on carrier-envelope-phase (CEP). At low values of optical field ($E$), the ionization yield is maximum for cos-like pulses with the dependence becoming stronger for higher charge states. At higher $E$-values, the CEP dependence either washes out or flips. A simple phenomenological model is developed that predicts and confirms the observed results. CEP effects are seen to persist for 8-cycle pulses. Unexpectedly, electron rescattering plays an unimportant role in the observed CEP dependence. Our r…
Intense extreme-ultraviolet (XUV) pulses enable the investigation of XUV-induced nonlinear processes and are a prerequisite for the development of attosecond pump - attosecond probe experiments. While highly nonlinear processes in the XUV range have been studied at free-electron lasers (FELs), high-harmonic generation (HHG) has allowed the investigation of low-order nonlinear processes. Here we suggest a concept to optimize the HHG intensity, which surprisingly requires a scaling of the experimental parameters that differs substantially from optimizing the HHG pulse energy. As a result, we are…
Using the frequency-domain theory, the high-order above threshold ionization (HATI) of a molecule is treated as a two-step transition: an above threshold ionization (ATI) followed by a laser-assisted collision (LAC). It is found that the HATI spectrum carries three pieces of information: the fingerprint of the molecular wave function lying in the ATI transition, the geometry structure of the molecule lying in the potential scattering between two plane waves, and the interaction between the ionized electron and the laser field lying in a phase factor in the LAC transition, where the phase facto…
Ionization is a fundamental process in intense laser-matter interactions, and is known to cause plasma defocusing and intensity clamping. Here, we investigate theoretically the propagation dynamics of an intense laser pulse in a helium gas jet in the ionization saturation regime, and we find that the pulse undergoes self-focusing and self-compression through ionization-induced reshaping, resulting in a manyfold increase in the laser intensity. This unconventional behavior is associated with the spatiotemporal frequency variation mediated by ionization and spatiotempral coupling. Our results il…
By using perturbation theory we derive an expression for the electrical field of a Gaussian laser pulse propagating in a gas medium. This expression is used as a trial solution in a variational method to get quasianalytical solutions for the width, intensity and self-focusing distance of ultrashort pulse. The approximation gives an improved agreement with results of numerical simulations for a broad range of values of the input power of the pulse than previous analytical results available in the literature.
We report on the generation of intense extreme ultraviolet (EUV) supercontinuum with photon energies spanning from 35 eV to 50 eV (i. e., supporting an isolated attosecond pulse with a duration of ~271 as) by loosely focusing 35 fs, 11 mJ pulses from a femtosecond laser amplifier into a 10-mm long gas cell filled with krypton gas. The dramatic change of spectral and temporal properties of the driver pulses after passing through the gas cell indicates that propagation effects play a significant role in promoting the generation of the EUV supercontinuum.
We use classical electron ensembles and the aligned-electron approximation to examine the effect of laser pulse duration on the dynamics of strong-field double ionization. We cover the range of intensities $10^{14}-10^{16} W/cm^2$ for the laser wavelength 780 nm. The classical scenario suggests that the highest rate of recollision occurs early in the pulse and promotes double ionization production in few-cycle pulses. In addition, the purely classical ensemble calculation predicts an exponentially decreasing recollision rate with each subsequent half cycle. We confirm the exponential behavior …
We theoretically analyze the quantum vortices - the zeros of electron wave function which are formed through atom ionization by ultrashort laser pulse. In 2D space we consider the case of above-threshold ionization of hydrogen atom and in 3D space the ionization of the atom in the zero-radius-potential approximation. With the help of obtained analytical results we make the assumption that localization of quantum vortices in 3D space can be predicted by analysis of 2D model.
We theoretically study the scaling with the driving wavelength of the high-order harmonic generation (HHG) under the simultaneous irradiation of an extreme ultraviolet (XUV) pulse. Surprisingly, when the cutoff energy and ionization yield are fixed, the harmonic yield is nearly independent of the driving wavelength. We identify its origin as the combination of the initial spatial width of the states excited by the XUV pulse, making the wavepacket spreading less prominent, and the shallowing of the ionization potential, which suggests complex nature of the wavelength dependence of HHG.
The process of ionization of a hydrogen atom by a short infrared laser pulse is studied in the regime of very large pulse intensity, in the dipole approximation. Let $A$ denote the integral of the electric field of the pulse over time at the location of the atomic nucleus. It is shown that, in the limit where $|A| \to \infty$, the ionization probability approaches unity and the electron is ejected into a cone opening in the direction of $-A$ and of arbitrarily small opening angle. Asymptotics of various physical quantities in $|A|^{-1}$ is studied carefully. Our results are in qualitative agre…
Polyatomic molecules in strong laser fields can undergo substantial nuclear motion within tens of femtoseconds. Ion imaging methods based on dissociation or Coulomb explosion therefore have difficulty faithfully recording the geometry dependence of the field ionization that initiates the dissociation process. Here we compare the strong-field double ionization and subsequent dissociation of water (both H$_2$O and D$_2$O) in 10-fs and 40-fs 800-nm laser pulses. We find that 10-fs pulses turn off before substantial internuclear motion occurs, whereas rapid internuclear motion can take place durin…
Intense few cycle terahertz pulses exhibit complex non-linear behavior under interaction with heavily n-doped Si. Fast increase in the transmission of a 700 fs pulse (central frequency 1.5 THz) through the Si sample (low field transmission of 0:02 %) saturates at 8 % for the external field of 5 MV/cm and then drops twofold at 20 MV/cm. An electro-optical sampling measurements revealed formation of a single cycle terahertz pulse at this field due to formation of a thin ionized layer by the first intense oscillation of the terahertz field.
The equations of motion of charged particles under the influence of short electromagnetic pulses are investigated. The subcycle regime is considered, and the delta function approximation is applied. The effects of the self force are also considered, and the threshold where radiation becomes important is discussed. A dimensionless parameter is defined that signals the onset of radiation reaction effects.
Sources of intense, ultra-short electromagnetic pulses enable applications such as attosecond pulse generation, control of electron motion in solids and the observation of reaction dynamics at the electronic level. For such applications both high-intensity and carrier envelope phase~(CEP) tunability are beneficial, yet hard to obtain with current methods. In this work we present a new scheme for generation of isolated CEP-tunable intense sub-cycle pulses with central frequencies that range from the midinfrared to the ultraviolet. It utilizes an intense laser pulse which drives a wake in a plas…
Octave-spanning, 12.5 fs, (1.9 cycle) pulses with 115 μJ energy in the short-wavelength mid-infrared spectral range (1-2.5 μm) have been generated via phase-mismatched cascaded nonlinear frequency conversion using organic DAST crystal. Such ultra-fast cascading effect is ensured by the interaction of a pump pulse with the exceptionally large effective nonlinearity of the DAST crystal and experiencing non-resonant, strongly phase mismatched, Kerr-like negative nonlinearity.
We theoretically investigate the generation of intense keV attosecond pulses in an orthogonally polarized multicycle midinfrared two-color laser field. It is demonstrated that multiple continuum-like humps, which have a spectral width of about twenty orders of harmonics and an intensity of about one order higher than adjacent normal harmonic peaks, are generated under proper two-color delays, owing to the reduction of the number of electron-ion recollisions and suppression of inter-half-cycle interference effect of multiple electron trajectories when the long wavelength midinfrared driving fie…
We theoretically study the generation of terahertz (THz) radiation by two-color filamentation of ultrashort laser pulses with different wavelengths. We consider wavelengths in the range from 0.6 to 10.6 $μ$m, thus covering the whole range of existing and future powerful laser sources in the near, mid and far-infrared. We show how different parameters of two-color filaments and generated THz pulses depend on the laser wavelength. We demonstrate that there is an optimal laser wavelength for two-color filamentation that provides the highest THz conversion efficiency and results in generation of e…
The speed of magnetization reversal is a key feature in magnetic data storage. Magnetic fields from intense THz pulses have been recently shown to induce small magnetization dynamics in Cobalt thin film on the sub-picosecond time scale. Here, we show that at higher field intensities, the THz electric field starts playing a role, strongly changing the dielectric properties of the cobalt thin film. Both the electronic and magnetic responses are found to occur simultaneously, with the electric field response persistent on a time scale orders of magnitude longer than the THz stimulus
Energy transfer processes from a high-intensity ultrashort laser pulse to electrons in simple dielectrics, silicon, diamond, and $α$-quartz are theoretically investigated by first-principles calculations based on time-dependent density functional theory (TDDFT). Dependences on frequency as well as intensity of the laser pulse are examined in detail, making a comparison with the Keldysh theory. Although the Keldysh theory reliably reproduces the main features of the TDDFT calculation, we find some deviations between results by the two theories. The origin of the differences is examined in detai…
The intense terahertz (THz) pulses facilitate the observation of various nonlinear optical effects and manipulation of material properties. In this work, we report a convenient approach that can produce strong broadband terahertz pulses with center frequency tunable between 2-4 THz. The coherent THz light source with pulse energy of 1.2 microjoule can be generated from a low-cost crystalline quartz pumped by an ultrashort tilted wave-front pulse. Thanks to the wide transparent spectral window and high damage threshold, our theoretical analysis and experiment show that the optical rectification…
The results of high-field terahertz transmission experiments on n-doped silicon (carrier concentration of $8.7\times10^{16}$ cm$^{-3}$) are presented. We use terahertz pulses with electric field strengths up to 3.1 MV cm$^{-1}$ and a pulse duration of 700 fs. Huge transmittance enhancement of $\sim$90 times is observed with increasing of the terahertz electric field strengths within the range of 1.5--3.1 MV cm$^{-1}$.
Air turns into a nonlinear medium for electromagnetic waves under exceptionally strong fields. However up to present, its minuscule nonlinear response has limited the exploration to the optical frequency regime owing to the availability of intense near-infrared lasers. Here, we report on the observation of large-amplitude nonlinearity in air induced by an extremely intense light bullet at Terahertz frequencies (0.1-10 THz) provoking strong air birefringence. The observed nonlinearity manifests itself as third order susceptibility. The presented nonlinear observations break the barrier for the …
Propagation of few-cycle laser pulses in optical fiber is investigated beyond the unidirectional approximation. Considered medium parameters include dispersion, Kerr and Raman nonlinearities. High intensities of ~10^10 kW/cm^2 lead to generation of the octave-spanning continuum. The error of the unidirectional approximation is seen in simulations as two pulses propagating forwards and backwards, both remain weak under the considered conditions. Direct analytical estimate of the error is derived and verified numerically. It can be applied to a priory justification of the unidirectional approach…
We investigate the prospects of creating broad rotational wave packets by means of molecular interaction with long sequences of intense femtosecond pulses. Using state-resolved rotational Raman spectroscopy of oxygen, subject to a sequence of more than 20 laser pulses with peak intensities exceeding $10^{13}$ W/cm$^{2}$ per pulse, we show that the centrifugal distortion is the main obstacle on the way to reaching high rotational states. We demonstrate that the timing of the pulses can be optimized to partially mitigate the centrifugal limit. The cumulative effect of a long pulse sequence resul…
Intense, ultrashort pulses of 800 nm laser light (12 fs, $\sim$4 optical cycles) of peak intensity 5$\times$10$^{14}$ W cm$^{-2}$ have been used to irradiate gas-phase Xe$_n$ clusters ($n$=500-25,000) so as to induce multiple ionization and subsequent Coulomb explosion. Energy distributions of exploding ions are measured in the few-cycle domain that does not allow sufficient time for the cluster to undergo Coulomb-driven expansion. This results in overall dynamics that appear to be significantly different to those in the many-cycle regime. One manifestation is that the maximum ion energies are…
This article presents: 1) The theoretical background of strong field physics and vacuum structure and stability; 2) The instrumental developments in the area of pulse lasers and considers the physics case for ultra intense laser facilities; and 3) Discussion of the applied and fundamental uses of ultra-intense lasers.
Intense single-cycle THz pulses resonantly interacting with molecular rotations are shown to induce significant field-free orientation under ambient conditions. We calculate and measure the angular distribution associated with THz-driven rotational motion and correlate the THz-induced orientation and alignment in an OCS gas sample.
We show theoretically that an intense femtosecond optical pulse incident normally on a metal surface tends to decay into a pair of counter-propagating surface plasmon-polaritons (SPPs). The interference field heats the medium periodically, which causes a periodic permittivity perturbation and resonantly amplifies the magnitudes of SPPs. The instability growth time is only 10-50 fs for typical metals at damaging laser fluences. This mechanism is promising for the interpretation of laser-induced periodic surface structures formation in a single-pulse pumping regime.
Non-linear Compton scattering in ultra-short intense laser pulses is discussed with the focus on angular distributions of the emitted photon energy. This is an observable which is accessible easily experimentally. Asymmetries of the azimuthal distributions are predicted for both linear and circular polarization. We present a systematic survey of the influence of the laser intensity, the carrier envelope phase and the laser polarization on the emission spectra for single-cycle and few-cycle laser pulses. For linear polarization, the dominant direction of the emission changes from a perpendicula…
We propose a novel measurement technique capable of determining the temporal duration of an intense laser pulse directly in its focus at full intensity. We show that the electromagnetic radiation pattern emitted by an electron bunch with a temporal energy chirp colliding perpendicularly with the laser pulse exhibits a distinct dependence on the pulse's duration. As the electrons emit radiation into an angular region determined by the ratio of their instantaneous energy to the laser's local field strength, the temporal change of the electrons' energy imprints information about the laser's pulse…
The spectra of Compton radiation emitted during electron scattering off an intense laser beam are calculated using the framework of strong-field quantum electrodynamics. We model these intense laser beams as finite length plane-wave-fronted pulses, similar to Neville and Rohrlich [Phys. Rev. D {\bf 3}, 1692 (1971)], or as trains of such pulses. Expressions for energy and angular distributions of Compton photons are derived such that a comparison of both situations becomes meaningful. Comparing frequency distributions for both an isolated laser pulse and a laser pulse train, we find a very good…
The electric field ionization of gallium acceptors in germanium was studied by using terahertz time-domain spectroscopy after single-cycle terahertz pulse excitation. As the peak electric field of the excitation pulse increases, the distinct absorptions due to acceptor transitions centered at 2.0 and 2.2 THz decrease, and simultaneously, absorption emerges in the lower frequency region. These behaviors clearly show that the terahertz pulse ionizes neutral acceptors. The electric field dependence of the released hole density is well reproduced by a model assuming direct field-assisted tunneling…
Single strand breaks are induced in DNA plasmids, pBR322 and pUC19, in aqueous media by intense ultrashort laser pulses (820 nm wavelength, 45 fs pulse duration, 1 kHz repetition rate) at intensities of 1-12 TW cm$^{-2}$. The intense laser radiation generates, {\it in situ}, electrons that induce transformation of supercoiled DNA into relaxed DNA. The extent of electron-mediated relaxation of DNA structure is quantified. Introduction of electron and radical scavengers inhibits DNA damage.
A propagation of an ultra-intense short laser pulse in a fiber is investigated with two dimensional Particle-in-Cell simulations. The fiber is a narrow hollow channel with walls consisting of overdense plasma. In the nonlinear interaction of the laser pulse with fiber walls high order harmonics are generated. Sufficiently high harmonics, for which the fiber walls are transparent, propagate outwards at certain angle. This is a scheme of a generator of ultra-short pulses of coherent light with a very short wavelength.
