Intense Ultrafast Laser Pulses Research Articles

On-target delivery of intense ultrafast laser pulses through hollow-core anti-resonant fibers.

We report the flexible on-target delivery of 800 nm wavelength, 5 GW peak power, 40 fs duration laser pulses through an evacuated and tightly coiled 10 m long hollow-core nested anti-resonant fiber by positively chirping the input pulses to compensate for the anomalous dispersion of the fiber. Near-transform-limited output pulses with high beam quality and a guided peak intensity of 3 PW/cm2 were achieved by suppressing plasma effects in the residual gas by pre-pumping the fiber with laser pulses after evacuation. This appears to cause a long-term removal of molecules from the fiber core. Identifying the fluence at the fiber core-wall interface as the damage origin, we scaled the coupled energy to 2.1 mJ using a short piece of larger-core fiber to obtain 20 GW at the fiber output. This scheme can pave the way towards the integration of anti-resonant fibers in mJ-level nonlinear optical experiments and laser-source development.

Electron heating and radiation in high aspect ratio sub-micron plasma generated by an ultrafast Bessel pulse within a solid dielectric

When propagating inside dielectrics, an ultrafast Bessel beam creates a high aspect-ratio cylinder of plasma with nanometric diameter that extends over several tens of micrometers to centimeters. We analyze the interaction between the intense ultrafast laser pulse and the plasma rod using particle-in-cell simulations. We show that electrons are heated and accelerated up to keV energies via transit acceleration inside the resonance lobes in the vicinity of the critical surface and compute their radiation pattern.

Electron quantum path control in high harmonic generation via chirp variation of strong laser pulses

The quantum phases of the electron paths driven by an ultrafast laser in high harmonic generation in an atomic gas depends linearly on the instantaneous cycle-averaged laser intensity. Using high laser intensities, a complete single ionisation of the atomic gas may occur before the laser pulse peak. Therefore, high harmonic generation could be localised only in a temporal window at the leading edge of laser pulse envelope. Varying the laser frequency chirp of an intense ultrafast laser pulse, the centre, and the width of the temporal window, that the high harmonic generation phenomenon occurs, could be controlled with high accuracy. This way, both the duration and the phase of the electron trajectories, that generate efficiently high harmonics, is fully controlled. A method of spectral control and selection of the high harmonic extreme ultraviolet light from distinct quantum paths is experimentally demonstrated. Furthermore, a phenomenological numerical model enlightens the physical processes that take place. This novel approach of the electron quantum path selection via laser chirp is a simple and versatile way of controlling the time-spectral characteristics of the coherent extreme ultraviolet light with applications in the fields of attosecond pulses and soft x-ray nano-imaging.

Vibrationally resolved above-threshold ionization in NO molecules by intense ultrafast two-color laser pulses: An experimental and theoretical study

We present above-threshold ionization (ATI) in the molecule nitric oxide, NO, by intense (${10}^{12}--{10}^{13}\phantom{\rule{0.28em}{0ex}}\mathrm{W}/{\mathrm{cm}}^{2}$) two-color femtosecond laser pulses. Vibrationally resolved coherent interference phenomena of multiphoton and multipathway ionization processes have been investigated by measuring experimentally and modeling theoretically the molecular photoionization yields. We find that the ATI photoelectron distribution of NO, initiated from degenerate electronic and vibrational states, depends on the relative phase of the two pulses, the kinetic energy, and emission angle of the photoelectrons. This dependence codes the information of interference effects of molecular electronic states. AC Stark effects modulate interference patterns in ATI spectra. Moreover, the ATI spectra exhibit peak energy dependencies that illustrate interference effects from coherent couplings between various ionization channels. These features reflect the molecular property and the multiple channel ionization interference effects in ATI processes. The results allow to explore coherent electron-vibration processes in ultrafast molecular photoionization.

Evidence for topological defects in a photoinduced phase transition

Upon excitation with an intense ultrafast laser pulse, a symmetry-broken ground state can undergo a non-equilibrium phase transition through pathways dissimilar from those in thermal equilibrium. Determining the mechanism underlying these photo-induced phase transitions (PIPTs) has been a long-standing issue in the study of condensed matter systems. To this end, we investigate the light-induced melting of a unidirectional charge density wave (CDW) material, LaTe$_3$. Using a suite of time-resolved probes, we independently track the amplitude and phase dynamics of the CDW. We find that a quick ($\sim\,$1$\,$ps) recovery of the CDW amplitude is followed by a slower reestablishment of phase coherence. This longer timescale is dictated by the presence of topological defects: long-range order (LRO) is inhibited and is only restored when the defects annihilate. Our results provide a framework for understanding other PIPTs by identifying the generation of defects as a governing mechanism.

Ultrafast electron dynamics in epitaxial graphene investigated with time- and angle-resolved photoemission spectroscopy

In order to exploit the intriguing optical properties of graphene it is essential to gain a better understanding of the light-matter interaction in the material on ultrashort timescales. Exciting the Dirac fermions with intense ultrafast laser pulses triggers a series of processes involving interactions between electrons, phonons and impurities. Here we study these interactions in epitaxial graphene supported on silicon carbide (semiconducting) and iridium (metallic) substrates using ultrafast time- and angle-resolved photoemission spectroscopy (TR-ARPES) based on high harmonic generation. For the semiconducting substrate we reveal a complex hot carrier dynamics that manifests itself in an elevated electronic temperature and an increase in linewidth of the π band. By analyzing these effects we are able to disentangle electron relaxation channels in graphene. On the metal substrate this hot carrier dynamics is found to be severely perturbed by the presence of the metal, and we find that the electronic system is much harder to heat up than on the semiconductor due to screening of the laser field by the metal.

Incorporating real time velocity map image reconstruction into closed-loop coherent control.

We report techniques developed to utilize three-dimensional momentum information as feedback in adaptive femtosecond control of molecular dynamics. Velocity map imaging is used to obtain the three-dimensional momentum map of the dissociating ions following interaction with a shaped intense ultrafast laser pulse. In order to recover robust feedback information, however, the two-dimensional momentum projection from the detector must be inverted to reconstruct the full three-dimensional momentum of the photofragments. These methods are typically slow or require manual inputs and are therefore accomplished offline after the images have been obtained. Using an algorithm based upon an "onion-peeling" (also known as "back projection") method, we are able to invert 1040 × 1054 pixel images in under 1 s. This rapid inversion allows the full photofragment momentum to be used as feedback in a closed-loop adaptive control scheme, in which a genetic algorithm tailors an ultrafast laser pulse to optimize a specific outcome. Examples of three-dimensional velocity map image based control applied to strong-field dissociation of CO and O2 are presented.

Measurement of the Plasma AstrophysicalSFactor for theHe3(d,p)He4Reaction in Exploding Molecular Clusters

The plasma astrophysical S factor for the 3He(d,p)4He fusion reaction was measured for the first time at temperatures of few keV, using the interaction of intense ultrafast laser pulses with molecular deuterium clusters mixed with 3He atoms. Different proportions of D2 and 3He or CD4 and 3He were mixed in the gas target in order to allow the measurement of the cross section for the 3He(d,p)4He reaction. The yield of 14.7 MeV protons from the 3He(d,p)4He reaction was measured in order to extract the astrophysical S factor at low energies. Our result is in agreement with other S factor parametrizations found in the literature.

Study of the yield of D-D, D-3He fusion reactions produced by the interaction of intense ultrafast laser pulses with molecular clusters

The interaction of intense ultrafast laser pulses with molecular clusters produces a Coulomb explosion of the clusters. In this process, the positive ions from the clusters might gain enough kinetic energy to drive nuclear reactions. An experiment to measure the yield of D-D and D-3He fusion reactions was performed at University of Texas Center for High Intensity Laser Science. Laser pulses of energy ranging from 100 to 180 J and duration 150fs were delivered by the Petawatt laser. The temperature of the energetic deuterium ions was measured using a Faraday cup, whereas the yields of the D-D reactions were measured by detecting the characteristic 2.45 MeV neutrons and 3.02 MeV protons. In order to allow the simultaneous measurement of 3He(D,p)4He and D-D reactions, different concentrations of D2 and 3He or CD4 and 3He were mixed in the gas jet target. The 2.45 MeV neutrons from the D(D,n)3He reaction were detecteded as well as the 14.7 MeV protons from the 3He(D,p)4He reaction. The preliminary results will be shown.

Neutral-Ionic State Correlations in Strong-Field Molecular Ionization

We study correlations between neutral and ionic states in strong-field molecular ionization. We compare predictions based on Dyson orbital norms and quasistatic semiclassical tunneling theories (Keldysh and molecular orbital Ammosov-Delone-Krainov) with more detailed calculations of strong-field ionization which take into account (i) the Coulomb interaction between the outgoing continuum electron wave packet and the remaining bound electrons and (ii) electron-core interactions that cause distortions of the electronic continuum states during the ionization event. Our results highlight the prominence of electronic rearrangement effects in strong-field ionization with intense ultrafast laser pulses, where the outgoing continuum electron can cause electronic transitions in the parent ion. Calculations and measurements for excited uracil molecules reveal the breakdown of Keldysh-weighted Dyson norm predictions for ionization to different states of the molecular cation in the strong-field regime.

Time-resolved soft x-ray absorption setup using multi-bunch operation modes at synchrotrons

Here, we report on a novel experimental apparatus for performing time-resolved soft x-ray absorption spectroscopy in the sub-ns time scale using non-hybrid multi-bunch mode synchrotron radiation. The present setup is based on a variable repetition rate Ti:sapphire laser (pump pulse) synchronized with the ~500 MHz x-ray synchrotron radiation bunches and on a detection system that discriminates and singles out the significant x-ray photon pulses by means of a custom made photon counting unit. The whole setup has been validated by measuring the time evolution of the L(3) absorption edge during the melting and the solidification of a Ge single crystal irradiated by an intense ultrafast laser pulse. These results pave the way for performing synchrotron time-resolved experiments in the sub-ns time domain with variable repetition rate exploiting the full flux of the synchrotron radiation.

Control of 1,3-Cyclohexadiene Photoisomerization Using Light-Induced Conical Intersections

We have studied the photoinduced isomerization from 1,3-cyclohexadiene to 1,3,5-hexatriene in the presence of an intense ultrafast laser pulse. We find that the laser field maximally suppresses isomerization if it is both polarized parallel to the excitation dipole and present 50 fs after the initial photoabsorption, at the time when the system is expected to be in the vicinity of a conical intersection that mediates this structural transition. A modified ab initio multiple spawning (AIMS) method shows that the laser induces a resonant coupling between the excited state and the ground state, i.e., a light-induced conical intersection. The theory accounts for the timing and direction of the effect.

Quasi-classical model of non-destructive wavepacket manipulation by intense ultrashort nonresonant laser pulses

A quasi-classical model (QCM) of nuclear wavepacket generation, modification and imaging by three intense ultrafast near-infrared laser pulses has been developed. Intensities in excess of 1013 W cm-2 are studied, the laser radiation is non-resonant and pulse durations are in the few-cycle regime, hence significantly removed from the conditions typical of coherent control and femtochemistry. The 1sσ ground state of the D2 precursor is projected onto the available electronic states in D2+ (1sσg ground and 2pσu dissociative) and D++D+ (Coulomb explosion) by tunnel ionization by an ultrashort ‘pump’ pulse, and relative populations are found numerically. A generalized non-adiabatic treatment allows the dependence of the initial vibrational population distribution on laser intensity to be calculated. The wavepacket is approximated as a classical ensemble of particles moving on the 1sσg potential energy surface (PES), and hence follow trajectories of different amplitudes and frequencies depending on the initial vibrational state. The ‘control’ pulse introduces a time-dependent polarization of the molecular orbital, causing the PES to be modified according to the dynamic Stark effect and the transition dipole. The trajectories adjust in amplitude, frequency and phase-offset as work is done on or by the resulting force; comparing the perturbed and unperturbed trajectories allows the final vibrational state populations and phases to be determined. The action of the ‘probe’ pulse is represented by a discrete internuclear boundary, such that elements of the ensemble at a larger internuclear separation are assumed to be photodissociated. The vibrational populations predicted by the QCM are compared to recent quantum simulations (Niederhausen and Thumm 2008 Phys. Rev. A 77 013404), and a remarkable agreement has been found. The applicability of this model to femtosecond and attosecond time-scale experiments is discussed and the relation to established femtochemistry and coherent control techniques are explored.

Interpreting ultrafast molecular fragmentation dynamics with ab initio electronic structure calculations

High-level ab initio electronic structure calculations are used to interpret the fragmentation dynamics of CHBr(2)COCF(3), following excitation with an intense ultrafast laser pulse. The potential energy surfaces of the ground and excited cationic states along the dissociative C-CF(3) bond have been calculated using multireference second order perturbation theory methods. The calculations confirm the existence of a charge transfer resonance during the evolution of a dissociative wave packet on the ground state potential energy surface of the molecular cation and yield a detailed picture of the dissociation dynamics observed in earlier work. Comparisons of the ionic spectrum for two similar molecules support a general picture in which molecules are influenced by dynamic resonances in the cation during dissociation.

Multiple ionization of ions and atoms by intense ultrafast laser pulses

Non-sequential processes in the multiple ionization of Xe and Xe+ targets subject to intense femtosecond laser pulses have been investigated. A precise ratio has been determined for the direct comparison of ionization using circular and linear polarized fields. Suppression of non-sequential effects where an ionic target is compared to a neutral atom target has been confirmed.

Numerical simulations of self-focusing of ultrafast laser pulses.

Simulation of nonlinear propagation of intense ultrafast laser pulses is a hard problem, because of the steep spatial gradients and the temporal shocks that form during the propagation. In this study we adapt the iterative grid distribution method of Ren and Wang [J. Comput. Phys. 159, 246 (2000)] to solve the two-dimensional nonlinear Schrödinger equation with normal time dispersion, space-time focusing, and self-steepening. Our simulations show that, after the asymmetric temporal pulse splitting, the rear peak self-focuses faster than the front one. As a result, the collapse of the rear peak is arrested before that of the front peak. Unlike what has sometimes been conjectured, however, collapse of the two peaks is not arrested through multiple splittings, but rather through temporal dispersion.

Lasing action in air induced by ultra-fast laser filamentation

The backscattered fluorescence of nitrogen from long filaments generated by intense ultrafast Ti-sapphire laser pulses propagating in air is studied. It shows an exponential increase with increasing filament length, indicating amplified spontaneous emission (ASE).

Deuterium-deuterium fusion dynamics in low-density molecular-cluster jets irradiated by intense ultrafast laser pulses.

Following the interaction of superintense, short pulse lasers and plasmas, ions can be accelerated to velocities sufficient to drive nuclear fusion reactions, in particular, by the process of Coulomb explosion of clusters [T. Ditmire, Nature (London) 398, 491 (1999)]]. We show here how short bursts of neutrons can be produced using a jet of low-density deuterated methane clusters. Ion velocity distributions were simultaneously measured by a Thomson parabola mass spectrometer, demonstrating deuteron energies up to 120 keV. We show that, in such conditions, nuclear fusion will occur not only in the hot plasma core, but also in the cold outer region by collision processes.

Femtosecond laser energy deposition in strongly absorbing cluster gases diagnosed by blast wave trajectory analysis

An intense ultrafast laser pulse can be very strongly absorbed in a moderate density gas composed of van der Waals bonded clusters. In this paper, the deposition of the energy of intense 30 fs light pulses in a gas of deuterium clusters has been diagnosed using a technique based on analysis of the trajectories of the resulting cylindrically symmetric blast waves. Using the well-known relation between blast wave velocity and energy deposition in gas, the laser energy deposited per unit length as a function of distance in gas jet plume was measured. These measurements were conducted in jets containing either deuterium clusters or simple deuterium molecules.

Self-focusing and frequency broadening of an intense short-pulse laser in plasmas.

An intense ultrafast laser pulse propagating through a plasma undergoes self-focusing and self-phase-modulation as a result of relativistic mass nonlinearity. The inclusion of a quartic (r4) term in the expansion of the eikonal in the radial coordinate r allows the modification of the shape of the radial intensity profile. The front of the pulse, under the combined effects of time-dependent self-focusing and frequency downshifting, acquires a severely distorted temporal shape. The radial profile for I(lambda)2(mu) < 2.8 x 1018 W/cm2, where I is the axial laser intensity and lambda(mu), is the laser wavelength in micrometers, is transformed from a Gaussian to a super-Gaussian because of the faster convergence of the marginal rays than the paraxial rays. In the opposite case of I(lambda)(2)(mu) > 2.8 x 10(18) W/cm2 when nonlinear plasma permittivity approaches saturation, the radial profile in the axial region becomes broader than the Gaussian.