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We investigate the influence of relativistic nondipole effects on the photoelectron spectra of argon, particularly in the low kinetic energy region (0 eV - 5 eV). In our experiment, we use intense linearly polarised 800 nm laser pulse to ionise Ar from a jet and we record photoelectron energy and momentum distributions using a reaction microscope (REMI). Our measurements show that nondipole effect can cause an energy-dependent asymmetry along the laser propagation direction in the photoelectron energy and momentum spectra. Model simulation based on time-dependent Dirac equation (TDDE) can reproduce our measurement results. The electron trajectory analysis based on classical model reveals that the photoelectron which obtains negative momentum shift along laser propagation direction is caused by the interplay between the Lorenz force induced radiation pressure during its free propagation in continuum and re-scattering by Coulomb potential of the parent ion when it is driven back by the laser field., Comment: 11 pages, 15 Figures

Atom-Trap Trace-Analysis (ATTA) is a technique aimed at a measuring the relative (in comparison to the common isotope) abundance of exceedingly rare noble gas radio-isotopes (Ar-39, Kr-81 and Kr-85), for the purposes of dating water, ice and other materials that contain trapped gases. These isotopes exist with an extremely low natural abundance and require measurement capability down to parts in 1017. The noble gas dating protocol is similar to that of radio-carbon dating but, the three isotopes together, allow dating of materials in complementary ranges to that possible with the radiocarbon technique. In a facility jointly created by CSIRO, Griffith and Adelaide Universities, we use laser guidance, cooling and trapping to perform isotopic separation using the isotopic dependence of atomic energy levels. The facility is currently undergoing construction but has been shown to be able to produce metastable Ne and Ar, which can then be laser cooled and trapped. When combined with the existing gas separation facility at the CSIRO Waite facility, which efficiently extracts pure noble gases from that are dissolved in water or ice samples, we should be in a position to start measuring the age of real-world samples in the early part of 2020. In addition, to describing the current state of construction, we will also discuss two more efficient approaches for creating metastable atoms that can reduce samples size and avoid unwanted cross-contamination between samples.

We investigate AC Stark-shifted resonances in argon with ultrashort near-infrared pulses. Using 30 fs pulses we observe periodic enhancements of the excitation yield in the intensity regions corresponding to the absorption of 13 and 14 photons. By reducing the pulse duration to 6 fs with only a few optical cycles, we also demonstrate that the enhancements are significantly reduced beyond what is measurable in the experiment. Comparing these to numerical predictions, which are in quantitative agreement with experimental results, we find that even though the quantum-state distribution can be broad, the enhancements are largely due to efficient population of a select few AC Stark-shifted resonant states rather than the closing of an ionization channel. Because these resonances are dependent on the frequency and intensity of the laser field, the broad bandwidth of the 6 fs pulses means that the resonance condition is fulfilled across a large range of intensities. This is further exaggerated by volume-averaging effects, resulting in excitation of the $5g$ state at almost all intensities and reducing the apparent magnitude of the enhancements. For 30 fs pulses, volume averaging also broadens the quantum state distribution but the enhancements are still large enough to survive. In this case, selectivity of excitation to a single state is reduced below 25% of the relative population. However, an analysis of TDSE simulations indicates that excitation of up to 60% into a single state is possible if volume averaging can be eliminated and the intensity can be precisely controlled., 7 pages, 5 figures

The tunnelling of a particle through a potential barrier is a key feature of quantum mechanics that goes to the core of wave–particle duality. The phenomenon has no counterpart in classical physics, and there are no well constructed dynamical observables that could be used to determine ‘tunnelling times’. The resulting debate1–5 about whether a tunnelling quantum particle spends a finite and measurable time under a potential barrier was reignited in recent years by the advent of ultrafast lasers and attosecond metrology6. Particularly important is the attosecond angular streaking (‘attoclock’) technique7, which can time the release of electrons in strong-field ionization with a precision of a few attoseconds. Initial measurements7–10 confirmed the prevailing view that tunnelling is instantaneous, but later studies11,12 involving multi-electron atoms—which cannot be accurately modelled, complicating interpretation of the ionization dynamics—claimed evidence for finite tunnelling times. By contrast, the simplicity of the hydrogen atom enables precise experimental measurements and calculations13–15 and makes it a convenient benchmark. Here we report attoclock and momentum-space imaging16 experiments on atomic hydrogen and compare these results with accurate simulations based on the three-dimensional time-dependent Schrodinger equation and our experimental laser pulse parameters. We find excellent agreement between measured and simulated data, confirming the conclusions of an earlier theoretical study17 of the attoclock technique in atomic hydrogen that presented a compelling argument for instantaneous tunnelling. In addition, we identify the Coulomb potential as the sole cause of the measured angle between the directions of electron emission and peak electric field: this angle had been attributed11,12 to finite tunnelling times. We put an upper limit of 1.8 attoseconds on any tunnelling delay, in agreement with recent theoretical findings18 and ruling out the interpretation of all commonly used ‘tunnelling times’19 as ‘time spent by an electron under the potential barrier’20. Simulation and measurement of the photoionization of atomic hydrogen at attosecond resolution confirm that the tunnelling of the ejected electron is instantaneous.

We present a technique for generating phase-locked two-colour pulses with controllable electric field waveform, whereby the polarization states of the two frequency components, as well as their intensities, relative phase and pulse delay can be completely controlled. To characterize the phase stability and the waveform of the output two-colour pulse in situ, we measured the momentum spectra of protons from dissociative ionization of the hydrogen molecule for different combinations of polarizations.

We present a detailed experimental and theoretical study on the relativistic non-dipole effects in strong-field atomic ionisation by near-infrared linearly-polarised few-cycle laser pulses in the intensity range 1014 -1015 W/cm2. We record high-resolution photoelectron momentum distributions of argon using a reaction microscope and compare our measurements with a truly ab-initio fully relativistic 3D model based on the time-dependent Dirac equation. We observe counter-intuitive peak shifts of the transverse electron momentum distribution in the direction opposite to that of laser propagation as a function of laser intensity and demonstrate an excellent agreement between experimental results and theoretical predictions., 6 pages, 6 figures, Manuscript prepared for submission to Physical Review Letters

Using asymmetric two-color laser fields composed of 1800 and 900nm, we have simultaneously controlled four well identified fragmentation channels in dissociative ionization of the hydrogen molecule, resulting in enhanced electron-localization sensitivities of up to 65%.

The debate on tunnelling times have always been full of contradictions and the attoclock experiments that measure tunnelling delays in strong-field ionization are no exception. The current review presents the debate and discussions concerning the studies of tunnelling times based only on the attoclock technique. We review them with their implications and pitfalls identified due to lack of accurate strong field models that validate the observations in interpreting the measurements performed on noble gases. In order to provide a complete picture, the review begins with a background on some of the popular tunnelling time definitions, most of them conceived during the late 1980s debate, which are often cited in the attoclock literature. We then discuss various attoclock experiments on noble gas atoms and their interpretations in context of the tunneling time debate. The recently performed attoclock experiment and numerical modelling using atomic hydrogen are also presented as an attempt at resolving the controversy. We conclude with the current status of the debate.

Measurements to control the morphology and characteristics of a picosecond laser produced chromium plasma plume upon double-pulse (DP) irradiation are presented and compared to their single-pulse (SP) counterpart. DP schemes are implemented by employing two geometries where the inter-pulse delay and the spatial separation are the control parameters. The ratio of plume length to plume width decreases upon increasing the inter-pulse delay and/or the energy of the second pulse in the collinear DP scheme. Interestingly, plasmas generated in the DP scheme at lower pressures resemble the expansion features of the plasma generated in the SP scheme at higher pressures. We find that DP schemes are advantageous for applications such as high harmonic generation and the production of quality thin films.

In strong-field ionization, the combined influence of nondipole and Coulomb focusing effects leave unique signatures on the photoelectron momentum distributions, which may have direct implications on many important strong-field phenomena. We present a comprehensive review of the experimental and theoretical investigations on these effects. We classify these investigations by relativistic and non-relativistic modelling based on different theoretical approaches, e.g. classical, semiclassical, strong-field approximation (SFA), time-dependent Schrodinger equation (TDSE), and time-dependent Dirac equation (TDDE). Finally, we discuss the latest experimental and theoretical development on this subject that has undergone so far to deeply understand the underlying physics.

Synopsis We present the first experimental evidence which qualitatively shows that frustrated tunnel ionization results in a larger number of excited neutrals per a tunnelling event for 6 fs pulses compared to 30 fs pulses. In addition, we also observe a less severe dependence on elliptical polarization for the 6 fs pulses. Furthermore, by varying the carrier envelope phase of the shorter pulse, we observe a modulation in the yield of excited neutrals which indicates possible control of electron trajectories.

Synopsis Quantum mechanical description of the relativistic non-dipole effects is of fundamental interest in strong-field physics community, as they may have direct implications on the processes relying on re-collision dynamics. Here, we present a detailed experimental and theoretical study on the relativistic non-dipole effects in strong-field ionisation at moderate intensities. We compare our precise measurements with a truly ab-initio fully relativistic 3D model based on the time-dependent Dirac equation and demonstrate an excellent agreement between experimental results and theoretical predictions.

Frustrated tunnel ionization (FTI) is one of the dominant channels in strong field ionization that results in the excitation of atoms. Recent studies have shown that there is a significant number of FTI events for multi-cycle pulses with the theory predicting that the excitation efficiency increases with pulse duration decreasing into the few-cycle regime. Our work concentrates on experimentally investigating the effect of few-cycle pulses on the FTI excitation process. We use pulses with duration 6 fs centred at 800 nm at intensities up to 0.8 PW crossed with an atomic Ar beam. We find that with few-cycle pulses there is more FTI per tunneling event and that for the same pulse energy more FTI is generated.

Time-resolved optical emission spectroscopic measurements of a plasma generated by irradiating a Cr target using 60 picosecond (ps) and 300 ps laser pulses is carried out to investigate the variation in the linewidth ($\delta\lambda$) of emission from neutrals and ions for increasing ambient pressures. Measurements ranging from 10$^{-6}$ Torr to 10$^2$ Torr show a distinctly different variation in the $\delta\lambda$ of neutrals (Cr I) compared to that of singly ionized Cr (Cr II), for both irradiations. $\delta\lambda$ increases monotonously with pressure for Cr II, but an oscillation is evident at intermediate pressures for Cr I. This oscillation does not depend on the laser pulse widths used. In spite of the differences in the plasma formation mechanisms, it is experimentally found that there is an optimum intermediate background pressure for which $\delta\lambda$ of neutrals drops to a minimum. Importantly, these results underline the fact that for intermediate pressures, the usual practice of calculating the plasma number density from the $\delta\lambda$ of neutrals needs to be judiciously done, to avoid reaching inaccurate conclusions.

In this Letter, the statement 'I.I. and A.B. performed computations at the NCI Australia' was missing from the Acknowledgements section. This has been corrected online.

We have investigated nuclear dynamics in bound and dissociating acetylene molecular ions in a time-resolved reaction microscopy experiment with a pair of few-cycle pulses. Different ionization processes were observed for acetylene. These time-dependent ionization processes are simulated using semi-classical on-the-fly dynamics revealing the underling mechanisms.

We generated and characterized plasma with single and double picosecond laser pulses in order to study the plume dynamics and to control the plasma properties. The double-pulse scheme was found to be superior for the generation of a homogeneous plasma. The lateral expansion was prominent for irradiation schemes wherein energy of the first pulse is lower/equal to that of the second pulse. While the velocities of the fast and slow species were found to be nearly equal, the emission counts corresponding to slow species are larger for single pulse compared to the double pulse.

We report on a systematic investigation of the dissociation dynamics of ${{\mathrm{H}}_{2}}^{+}$ in intense laser fields, and study how the kinetic energy spectrum of the dissociating proton can be modulated by the wavelength and intensity of the driving laser field. In the experiment, ${\mathrm{H}}_{2}$ is dissociatively ionized by an intense laser pulse with varying carrier wavelengths ranging from 800 to 1800 nm and varying peak intensities. A model based on Floquet theory and Landau-Zener theory is adopted to explain the experimental observations. The intensity effect is further explored in a few-cycle pump-probe experiment. We observed a significant intensity-dependent proton kinetic energy shift, which can also be well explained by the theoretical simulation. The wavelength- and intensity-dependent proton spectra reveal the mechanism of selective excitation of vibrational levels of ${{\mathrm{H}}_{2}}^{+}$ in intense laser fields.

This work describes the first observations of the ionisation of neon in a metastable atomic state utilising a strong-field, few-cycle light pulse. We compare the observations to theoretical predictions based on the Ammosov-Delone-Krainov (ADK) theory and a solution to the time-dependent Schrödinger equation (TDSE). The TDSE provides better agreement with the experimental data than the ADK theory. We optically pump the target atomic species and measure the ionisation rate as the a function of different steady-state populations in the fine structure of the target state which shows significant ionisation rate dependence on populations of spin-polarised states. The physical mechanism for this effect is unknown.

Ionization of atoms and molecules in strong laser fields is a fundamental process in many fields of research, especially in the emerging field of attosecond science. So far, demonstrably accurate data have only been acquired for atomic hydrogen (H), a species that is accessible to few investigators. Here we present measurements of the ionization yield for argon, krypton, and xenon with percentlevel accuracy, calibrated using H, in a laser regime widely used in attosecond science. We derive a transferrable calibration standard for laser peak intensity, accurate to 1.3%, that is based on a simple reference curve. In addition, our measurements provide a much-needed benchmark for testing models of ionisation in noble-gas atoms, such as the widely employed single-active electron approximation., Article: 5 pages, 2 figures, submitted to PRL (manuscript number LZ14457). Supplementary information: 7 pages, 6 figures, appended to end of main Article

We demonstrate that the coherent control of unimolecular reactions by using a waveform-controlled laser fields can lead to a strong modulation on the yield of the reaction. By using a synthesized \ensuremath{\omega} (1800-nm) and 3\ensuremath{\omega} (600-nm) two-color laser field, the probability of photodissociation of ${\mathrm{H}}_{2}{}^{+}$ can be strongly modulated by varying the relative phase between the two colors. The dissociation probability maximizes at different relative phases for protons with different kinetic energy, and such energy dependence can also be qualitatively reproduced by our simulation. We attribute the observed dissociation probability modulation to the interference between two different dissociation pathways which start from the same electronic states and end with the same kinetic energy.

International audience; Steering the electrons during an ultrafast photo-induced process in a molecule influences the chemical behavior of the system, opening the door to the control of photochemical reactions and photobiological processes. Electrons can be efficiently localized using a strong laser field with a well-designed temporal shape of the electric component. Consequently, many experiments have been performed with laser sources in the near-infrared region (800 nm) in the interest of studying and enhancing the electron localization. However, due to its limited accessibility, the mid-infrared (MIR) range has barely been investigated, although it allows to efficiently control small molecules and even more complex systems. To push further the manipulation of basic chemical mechanisms, we used a MIR two-color (1800 and 900 nm) laser field to ionize H$_2$ and D$_2$ molecules and to steer the remaining electron during the photo-induced dissociation. The study of this prototype reaction led to the simultaneous control of four fragmentation channels. The results are well reproduced by a theoretical model solving the time-dependent Schrödinger equation for the molecular ion, identifying the involved dissociation mechanisms. By varying the relative phase between the two colors, asymmetries (i.e., electron localization selectivity) of up to 65% were obtained, corresponding to enhanced or equivalent levels of control compared to previous experiments. Experimentally easier to implement, the use of a two-color laser field leads to a better electron localization than carrier-envelope phase stabilized pulses and applying the technique in the MIR range reveals more dissociation channels than at 800 nm.

We studied the dynamics of dissociative double ionization of acetylene using pump-probe technique with few-cycle laser pulses and Reaction Microscope detection system.

We present initial phase shift measurements of high-order harmonic radiation generated from hydrogen isotopes using Gouy Phase interferometer. We will study the nuclear dynamics of molecules after they undergo strong-field ionization by ultrashort laser pulses.

We present accurate measurements of carrier-envelope phase effects on ionisation of the noble gases with few-cycle laser pulses. The experimental apparatus is calibrated by using atomic hydrogen data to remove any systematic offsets and thereby obtain accurate CEP data on other generally used noble gases such as Ar, Kr and Xe. Experimental results for H are well supported by exact TDSE theoretical simulations however significant differences are observed in case of noble gases., Comment: 4 pages, 5 figures, submitted to PRL (manuscript number LH15031)

We have investigated nuclear dynamics in bound and dissociating acetylene molecular ions in a time-resolved reaction microscopy experiment with a pair of few-cycle pulses. Vibrating bound acetylene cations or dissociating dications are produced by the first pulse. The second pulse probes the nuclear dynamics by ionization to higher charge states and Coulomb explosion of the molecule. For the bound cations, we observed vibrations in acetylene (HCCH) and its isomer vinylidene (CCHH) along the CC-bond with a periodicity of around 26 fs. For dissociating dication molecules, a clear indication of enhanced ionization is found to occur along the CH- and CC-bonds after 10 fs to 40 fs. The time-dependent ionization processes are simulated using semi-classical on-the-fly dynamics revealing the underling mechanisms.

We describe an extreme ultraviolet (XUV) interferometric technique that can resolve ~100 zeptoseconds (10−21 s) delay between high harmonic emissions from two successive sources separated spatially along the laser propagation in a single Gaussian beam focus. Several improvements on our earlier work have been implemented in the advanced interferometer. In this paper, we report on the design, characterization and optimization of the advanced Gouy phase interferometer. Temporal coherence for both atomic argon and molecular hydrogen gases has been observed for several harmonic orders. It has been shown that phase shift of XUV pulses mainly originates from the emission time delay due to the Gouy phase in the laser focus and the observed interference is independent of the generating medium. This interferometer can be a useful tool for measuring the relative phase shift between any two gas species and for studying ultrafast dynamics of their electronic and nuclear motion.

When a diatomic molecule is ionized by an intense laser field, the ionization rate depends very strongly on the inter-nuclear separation. That dependence exhibits a pronounced maximum at the inter-nuclear separation known as the “critical distance”. This phenomenon was first demonstrated theoretically in H2+ and became known as “charge-resonance enhanced ionization” (CREI, in reference to a proposed physical mechanism) or simply “enhanced ionization”(EI). All theoretical models of this phenomenon predict a double-peak structure in the R-dependent ionization rate of H2+. However, such double-peak structure has never been observed experimentally. It was even suggested that it is impossible to observe due to fast motion of the nuclear wavepackets. Here we report a few-cycle pump-probe experiment which clearly resolves that elusive double-peak structure. In the experiment, an expanding H2+ ion produced by an intense pump pulse is probed by a much weaker probe pulse. The predicted double-peak structure is clearly seen in delay-dependent kinetic energy spectra of protons when pump and probe pulses are polarized parallel to each other. No structure is seen when the probe is polarized perpendicular to the pump.

We study transverse electron momentum distribution (TEMD) in strong field atomic ionization driven by laser pulses with varying ellipticity. We show, both experimentally and theoretically, that the TEMD in the tunneling and over the barrier ionization regimes evolves in a qualitatively different way when the ellipticity parameter describing polarization state of the driving laser pulse increases., Comment: 5 pages, 6 figures

It has been recently predicted theoretically that due to nuclear motion light and heavy hydrogen molecules exposed to strong electric field should exhibit substantially different tunneling ionization rates (O.I. Tolstikhin, H.J. Worner and T. Morishita, Phys. Rev. A 87, 041401(R) (2013) [1]). We studied that isotope effect experimentally by measuring relative ionization yields for each species in a mixed H2/D2 gas jet interacting with intense femtosecond laser pulses. In a reaction microscope apparatus we detected ionic fragments from all contributing channels (single ionization, dissociation, and sequential double ionization) and determined the ratio of total single ionization yields for H2 and D2. The measured ratio agrees quantitatively with the prediction of the generalized weak-field asymptotic theory in an apparent failure of the frozen-nuclei approximation., Comment: 11 pages, 4 figures

We studied ionization of neon and argon by intense linearly polarized femtosecond laser pulses of different wavelengths (400 nm and 800 nm) and peak intensities, and by measuring momentum distributions of singly charged positive ions in the direction parallel to laser polarization. For Ne the momentum distributions exhibited a characteristic dip at zero momentum at 800 nm and a complex multipeak structure at 400 nm. Similarly, for Ar the momentum distributions evolved from a complex multipeak structure with a pronounced dip in the centre at 400 nm, to a smooth distribution characteristic of pure tunneling ionization (800 nm, high intensities). In the intermediate regime (800 nm, medium to low intensities), for both atoms we observed recoil ion momentum distributions modulated by quasi-periodic structures usually seen in the photoelectron energy spectra in a multi-photon regime (ATI spectra). Ne did show a characteristic 'dip' at low momentum, while the longitudinal momentum distribution for Ar exhibited a spike at zero momentum instead. The spectra did dramatically change at 400 nm, where both ions show the pronounced dip near zero momentum. Based on our results, we conclude that the structures observed in Ne and Ar momentum distributions reflect the specifics of atomic structure of the two targets and should not be attributed to effects of electron recollision, as was suggested earlier. Instead, as our results indicate, they are due to the effects of multi-photon resonant enhancement of strong-field ionization.

We present momentum images of the ionic products from the ionization of D2 and C2H2 by short laser pulses. For D2, we use a pump–probe approach to investigate the dependence of the enhanced ionization on the internuclear distance. Evidence for two (not well separated) regions of enhancement is found near internuclear distances of 6 and 10 au. In the case of acetylene, we report clear evidence for the production of both acetylene and vinylidene dications with kinetic energy releases similar to those reported earlier by core electron removal. We also find very different angular distributions for the fragments in the two channels, consistent with a finite time for the isomerization.

We have measured momentum-space images of low-energy electrons generated by the interaction of short intense laser pulses with argon atoms at high intensities. We have done this over a wavelength range from 400 to 800 nm. The spectra show considerable structure in both the energy and angular distributions of the electrons. Some, but not all, energy features can be identified as multi-photon resonances. The angular structure shows a regularity which transcends the resonant structure and may be due instead to diffraction. The complexity of the results defies easy model-dependent interpretations and invites full solutions to Schrodinger's equation for these systems.

Field-free alignment of gas-phase molecules can be achieved by creating rotational wavepackets with a short laser pulse. We demonstrate that the degree of alignment can be improved by illuminating the molecules with a second laser pulse at a specific time during the evolution of the original rotational wavepacket.

Interaction of atoms and molecules with strong electric fields is a fundamental process in many fields of research, particularly in the emerging field of attosecond science. Therefore, understanding the physics underpinning those interactions is of significant interest to the scientific community. One crucial step in this understanding is accurate knowledge of the few-cycle laser field driving the process. Atomic hydrogen (H), the simplest of all atomic species, plays a key role in benchmarking strong-field processes. Its wide-spread use as a testbed for theoretical calculations allows the comparison of approximate theoretical models against nearly-perfect numerical solutions of the three-dimensional time-dependent Schrodinger equation. Until recently, relatively little experimental data in atomic H was available for comparison to these models, and was due mostly due to the difficulty in the construction and use of atomic H sources. Here, we review our most recent experimental results from atomic H interaction with few-cycle laser pulses and how they have been used to calibrate important laser pulse parameters such as peak intensity and the carrier-envelope phase (CEP). Quantitative agreement between experimental data and theoretical predictions for atomic H has been obtained at the 10% uncertainty level, allowing for accurate laser calibration intensity at the 1% level. Using this calibration in atomic H, both accurate CEP data and an intensity calibration standard have been obtained Ar, Kr, and Xe; such gases are in common use for strong-field experiments. This calibration standard can be used by any laboratory using few-cycle pulses in the 1014 W cm−2 intensity regime centered at 800 nm wavelength to accurately calibrate their peak laser intensity to within few-percent precision.

Synopsis We present an intensity dependent study of transverse electron momentum distribution obtained from strong field ionization of argon using linearly polarized few-cycle (6 fs) laser pulses in the intensity range 1015W/cm2-1016W/cm2.

We present the results of attosecond angular streaking of atomic Hydrogen using elliptically polarized, 5.5 fs pulses that are centered around 770 nm, within the intensity range of 1.65 to 4 × 1014 W/cm2. We measure angular offsets in the photo-electron momentum distribution relative to the peak of the electric field of light in the polarization plane. We find a strong agreement in these results with the solutions of complete 3D-TDSE simulations. Further, we compute the contribution of coulomb effects (between the ionized electron-parent ion) to the measured angular offsets using Yukawa potential, subtracting which yields the real 'tunneling delays'.

We explore the effect of nuclear mass on the laser-driven electron localization process. We dissociate a mixed H2 and D2 target with intense, carrier-envelope-phase (CEP) stable 6 fs laser pulses and detect the products in a reaction microscope. We observe a very strong CEP-dependent asymmetry in proton and deuteron emission for low dissociation energy channels. This asymmetry is stronger for H2 than for D2. We also observe a large CEP offset between the asymmetry spectra for H2 and D2. Our theoretical simulations, based on a one-dimensional two-channel model, agree very well with the asymmetry spectra, but fail to account properly for the phase difference between the two isotopes.

The transition between two distinct mechanisms for the laser-induced field-free orientation of CO molecules is observed via measurements of orientation revival times and subsequent comparison to theoretical calculations. In the first mechanism, which we find responsible for the orientation of CO up to peak intensities of 8 x 10^13 W/cm^2, the molecules are impulsively oriented through the hyperpolarizability interaction. At higher intensities, asymmetric depletion through orientation-selective ionization is the dominant orienting mechanism. In addition to the clear identification of the two regimes of orientation, we propose that careful measurements of the onset of the orientation depletion mechanism as a function of the laser intensity will provide a relatively simple route to calibrate absolute rates of non-perturbative strong-field molecular ionization., Comment: 5 pages, 2 figures

It is shown that electrons in molecules behave in an essentially orbital-like fashion and that imaging of the spherically averaged orbital electron density can be achieved in momentum space by electron momentum spectroscopy (EMS). EMS measurements, using the binary (e,2e) reaction under binary encounter collision conditions, are demonstrated to effectively probe valence electron (frontier orbital) electron transfer out of a molecule by providing imaging of the spherically averaged Dyson orbital electron momentum density distribution corresponding to the ionization process. Experimental EMS cross-sections for the outermost valence (frontier) electrons of HF, H 2 O, NH 3 , CH 4 , H 2 S and a range of other molecules are found to be in excellent agreement with MRSD-CI calculations of the respective Dyson orbital densities using the plane wave impulse approximation. High level Hartree–Fock and density functional theory (DFT) (B3LYP and B3PW91) calculations, with large, saturated and diffuse basis sets, demonstrate that the Dyson orbital densities and thus the EMS experiments are also extremely well described by the respective initial state (i.e. neutral molecule) canonical molecular orbital (CMO) Hartree–Fock independent particle electron density distributions, with as good or sometimes an even better description being given by the respective (correlated) Kohn–Sham orbital (KSO) densities of DFT. In this sense EMS is shown to provide experimental imaging of orbital electron densities, with the emerging electrons having a delocalised orbital character immediately prior to `knock-out'. The present experimental and theoretical findings also lend support to the earlier predictions of Fukui as to the possibility of observing the `orbital pattern' experimentally [Int. J. Quant. Chem. 12 (Suppl. 1) (1977) 277] as well as to the recent views of Stowasser and Hoffmann [J. Am. Chem. Soc. 121 (1999) 3414] concerning the `reality' of KSOs. Further supporting evidence for the present findings is provided by a consideration of the results of frontier orbital theory applied to chemical reactions involving electron transfer, such as electrophilic attack [J. Chem. Phys. 20 (1952) 722]. The present results and interpretation are also strongly supported by scanning tunneling microscopy (STM) theory [Phys. Rev. B 31 (1985) 805] and in particular by recent STM experiments on adsorbed C 60 molecules [Chem. Phys. Lett. 321 (2000) 78] which show images which correspond very closely with DFT calculations of the electron density distribution in the HOMO orbital of the neutral molecule. The EMS measurements and associated theoretical calculations, together with the evidence from frontier orbital theory and the STM experiments, strongly suggest that delocalised CMO, or often, even better, the KSO, densities provide an operational definition of orbital electron densities, and thus of orbitals, appropriate for use in discussions of chemical bonding as well as for predicting the outcome of chemical reactions and physical processes involving electron transfer.

Measurements of electron binding energy spectra and electron momentum profiles (electron momentum distribu-tions) for the valence orbitals of the cage molecule adamantane (C 10 H 16 ) using electron momentum spectroscopy arereported. Theoretical momentum profiles are calculated using the plane-wave impulse approximation (PWIA) withinthe target Hartree–Fock and also the target Kohn–Sham approximations (density functional theory, DFT) with the4-31G and 6-311++G** basis sets and compared with the experimental results. The Hartree–Fock and the DFT cal-culations using the 6-311++G** basis set are in good quantitative agreement with the experimental momentum profiles.The experimental and the calculated orbital momentum distributions confirm the tentative orbital assignments made inthe earlier published studies of adamantane by photoelectron spectroscopy. Small e•ects at low momenta, with themeasured cross-section being above the PWIA calculations for molecular orbitals of e and t 1 symmetry, are attributedto distorted-wave e•ects. O 2000 Elsevier Science B.V. All rights reserved.

A method is suggested that allows separation of the contributions from homogeneous and inhomogeneous broadening (IB) to a total spectral contour of rigid systems. Based upon a simple convolution model of inhomogeneous broadening, the method allows calculation of homogeneously broadened spectra and an inhomogeneous distribution function (IDF) from the measured excitation-wavelength-dependent fluorescence spectra of the system. The method is applied successfully to the solid solution of coumarin 334 (C334) in poly(methyl methacrylate) (PMMA) glass at 293 K.

We experimentally optimize the yield of attosecond XUV pulses, with pulse duration inferred from carrier-envelope-phase resolved spectral measurements. We also demonstrate generation of dual attosecond pulses with timing resolution of 90 zeptoseconds.

We present the measured photoionization yield of atomic hydrogen as a function of laser intensity for few-cycle pulses. Fits with exact ab-initio simulations produce better agreement than analytical theories and enable accurate intensity calibration.

Accurate knowledge of the intensity of focused ultrashort laser pulses is crucial to the correct interpretation of experimental results in strong-field physics. We have developed a technique to measure laser intensities approaching ${10}^{15}\phantom{\rule{0.28em}{0ex}}\text{W}/{\text{cm}}^{2}$ with an accuracy of 1$%$. This accuracy is achieved by comparing experimental photoelectron yields from atomic hydrogen with predictions from exact numerical solutions of the three-dimensional time-dependent Schr\"odinger equation. Our method can be extended to relativistic intensities and to the use of other atomic species.

Laser produced plasmas are transient in nature, and their properties, which depend on the laser parameters as well as the material properties and the irradiation conditions, can be tailored for different applications. Highly ionized Al plasmas generated using 7 ns and negatively chirped 60 ps pulses are optimized for the purpose of generating Al IV and Al III, respectively. The plasma is optimized spatio-temporally for Al IV or Al III with irradiation energy as the control parameter using time-resolved optical emission spectroscopy. Plasmas attuned for higher charged states could be utilized as a good alternative source for the generation of high order harmonics.