Resolving the time when an electron exits a tunnelling barrier.

The tunnelling of a particle through a barrier is one of the most fundamental and ubiquitous quantum processes. When induced by an intense laser field, electron tunnelling from atoms and molecules initiates a broad range of phenomena such as the generation of attosecond pulses, laser-induced electron diffraction and holography. These processes evolve on the attosecond timescale (1 attosecond ≡ 1 as = 10(-18) seconds) and are well suited to the investigation of a general issue much debated since the early days of quantum mechanics--the link between the tunnelling of an electron through a barrier and its dynamics outside the barrier. Previous experiments have measured tunnelling rates with attosecond time resolution and tunnelling delay times. Here we study laser-induced tunnelling by using a weak probe field to steer the tunnelled electron in the lateral direction and then monitor the effect on the attosecond light bursts emitted when the liberated electron re-encounters the parent ion. We show that this approach allows us to measure the time at which the electron exits from the tunnelling barrier. We demonstrate the high sensitivity of the measurement by detecting subtle delays in ionization times from two orbitals of a carbon dioxide molecule. Measurement of the tunnelling process is essential for all attosecond experiments where strong-field ionization initiates ultrafast dynamics. Our approach provides a general tool for time-resolving multi-electron rearrangements in atoms and molecules--one of the key challenges in ultrafast science.

Generating Isolated Elliptically Polarized Attosecond Pulses Using Bichromatic Counterrotating Circularly Polarized Laser Fields.

We theoretically demonstrate the possibility to generate both trains and isolated attosecond pulses with high ellipticity in a practical experimental setup. The scheme uses circularly polarized, counterrotating two-color driving pulses carried at the fundamental and its second harmonic. Using a model Ne atom, we numerically show that highly elliptic attosecond pulses are generated already at the single-atom level. Isolated pulses are produced by using few-cycle drivers with controlled time delay between them.

High harmonic interferometry of multi-electron dynamics in molecules.

High harmonic emission occurs when an electron, liberated from a molecule by an incident intense laser field, gains energy from the field and recombines with the parent molecular ion. The emission provides a snapshot of the structure and dynamics of the recombining system, encoded in the amplitudes, phases and polarization of the harmonic light. Here we show with CO(2) molecules that high harmonic interferometry can retrieve this structural and dynamic information: by measuring the phases and amplitudes of the harmonic emission, we reveal 'fingerprints' of multiple molecular orbitals participating in the process and decode the underlying attosecond multi-electron dynamics, including the dynamics of electron rearrangement upon ionization. These findings establish high harmonic interferometry as an effective approach to resolving multi-electron dynamics with sub-Angström spatial resolution arising from the de Broglie wavelength of the recombining electron, and attosecond temporal resolution arising from the timescale of the recombination event.

Three-body bound states in atomic mixtures with resonant p-wave interaction.

We employ the Born-Oppenheimer approximation to find the effective potential in a three-body system consisting of a light particle and two heavy ones when the heavy-light short-range interaction potential has a resonance corresponding to a nonzero orbital angular momentum. In the case of an exact resonance in the p-wave scattering amplitude, the effective potential is attractive and long range; namely, it decreases as the third power of the interatomic distance. Moreover, we show that the range and power of the potential, as well as the number of bound states, are determined by the mass ratio of the particles and the parameters of the heavy-light short-range potential.

Operational dynamic modeling transcending quantum and classical mechanics.

We introduce a general and systematic theoretical framework for operational dynamic modeling (ODM) by combining a kinematic description of a model with the evolution of the dynamical average values. The kinematics includes the algebra of the observables and their defined averages. The evolution of the average values is drawn in the form of Ehrenfest-like theorems. We show that ODM is capable of encompassing wide-ranging dynamics from classical non-relativistic mechanics to quantum field theory. The generality of ODM should provide a basis for formulating novel theories.

Strong-field control and spectroscopy of attosecond electron-hole dynamics in molecules.

Molecular structures, dynamics and chemical properties are determined by shared electrons in valence shells. We show how one can selectively remove a valence electron from either Pi vs. Sigma or bonding vs. nonbonding orbital by applying an intense infrared laser field to an ensemble of aligned molecules. In molecules, such ionization often induces multielectron dynamics on the attosecond time scale. Ionizing laser field also allows one to record and reconstruct these dynamics with attosecond temporal and sub-Angstrom spatial resolution. Reconstruction relies on monitoring and controlling high-frequency emission produced when the liberated electron recombines with the valence shell hole created by ionization.

Tunnel ionization of molecules and orbital imaging.

We study whether tunnel ionization of aligned molecules can be used to map out the electronic structure of the ionizing orbitals. We show that the common view, which associates tunnel ionization rates with the electronic density profile of the ionizing orbital, is not always correct. Using the example of tunnel ionization from the CO(2) molecule, we show how and why the angular structure of the alignment-dependent ionization rate moves with increasing the strength of the electric field. These modifications reflect a general trend for molecules.

Strong-field ionization of clusters using two-cycle pulses at 1.8 µm.

The interaction of intense laser pulses with nanoscale particles leads to the production of high-energy electrons, ions, neutral atoms, neutrons and photons. Up to now, investigations have focused on near-infrared to X-ray laser pulses consisting of many optical cycles. Here we study strong-field ionization of rare-gas clusters (103 to 105 atoms) using two-cycle 1.8 µm laser pulses to access a new interaction regime in the limit where the electron dynamics are dominated by the laser field and the cluster atoms do not have time to move significantly. The emission of fast electrons with kinetic energies exceeding 3 keV is observed using laser pulses with a wavelength of 1.8 µm and an intensity of 1 × 1015 W/cm2, whereas only electrons below 500 eV are observed at 800 nm using a similar intensity and pulse duration. Fast electrons are preferentially emitted along the laser polarization direction, showing that they are driven out from the cluster by the laser field. In addition to direct electron emission, an electron rescattering plateau is observed. Scaling to even longer wavelengths is expected to result in a highly directional current of energetic electrons on a few-femtosecond timescale.

Multielectron correlation in high-harmonic generation: a 2D model analysis.

We analyze the role of multielectron dynamics in high-harmonic generation spectroscopy, using an example of a two-electron system. We identify and systematically quantify the importance of correlation and exchange effects. One of the main sources for correlation is identified to be the polarization of the ion by the recombining continuum electron. This effect, which plays an important qualitative and quantitative role, seriously undermines the validity of the standard approaches to high-harmonic generation, which ignore the contribution of excited ionic states to the radiative recombination of the continuum electron.

Attosecond circular dichroism spectroscopy of polyatomic molecules.

We describe the roles of multiple electronic continua in high-harmonic generation from aligned molecules. First, we show how the circularity of emitted harmonics tracks the interplay of different electronic continua participating in the nonlinear response. Second, we show that the interplay of different continua can lead to large variations of harmonic phases. Finally, we show how multiple electronic continua allow one to shape the polarization of high harmonics and attosecond pulses.

Attosecond photoelectron spectroscopy of electron tunneling in a dissociating hydrogen molecular ion.

We demonstrate the potential of intense-field pump, attosecond probe photoelectron spectroscopy to monitor electron tunneling between the two protons during dissociative ionization of the hydrogen molecule, with attosecond temporal and Angstrom-scale spatial resolution.

Effective fields in laser-driven electron recollision and charge localization.

We propose a model to describe correlated two-electron dynamics in strong laser fields during laser-induced recollision between an electron and its parent ion. We derive an effective interaction potential which describes the effect of the laser-driven electron collision with an ion while retaining the correlation between the colliding and the bound electron. Using dissociative ionization of molecular hydrogen as an example, we analyze the dynamics of correlation-driven electron localization in a dissociating hydrogen molecular ion.

Suppression of decoherence in a wave packet via nonlinear resonance.

We propose a simple approach for suppressing decoherence of a wave packet excited in an anharmonic oscillator. We show that when a resonant external field forces the oscillator to follow the driving force, motion around the resonant trajectory inside a stable resonant island can be made almost completely immune to the environment. As an example, we study suppression of decoherence due to coupling to thermally populated rotations in vibrational wave packets in a Na2 molecule.

Experimental observation of different-order components of a vibrational wave packet in a bulk dielectric using high-order Raman scattering.

We use high-order Raman scattering in a bulk dielectric to characterize coherent dynamics with precision typical for gas phase experiments. The experimental pump-probe approach allows for the simultaneous observation and separation in space and time of the individual contributions of different-order Raman processes to a coherent wave packet without relying on phase-matching conditions and within the same experimental geometry. We propose a novel technique to discriminate between stimulated excitation of vibronic levels in the impulsive and intermediate excitation regimes, futhermore allowing us to distinguish between different pathways contributing to the same fifth-order Raman processes.

Dynamic stark control of photochemical processes.

A method is presented for controlling the outcome of photochemical reactions by using the dynamic Stark effect due to a strong, nonresonant infrared field. The application of a precisely timed infrared laser pulse reversibly modifies potential energy barriers during a chemical reaction without inducing any real electronic transitions. Dynamic Stark control (DSC) is experimentally demonstrated for a nonadiabatic photochemical reaction, showing substantial modification of reaction channel probabilities in the dissociation of IBr. The DSC process is nonperturbative and insensitive to laser frequency and affects all polarizable molecules, suggesting broad applicability.

Optimal generation of single-dispersion precompensated 1-fs pulses by molecular phase modulation.

We show how an optimal control approach can be combined with the pump-probe technique for pulse compression by molecular phase modulation in hollow-core fibers to generate single 1-fs pulses in the visible. Varying the intensity and duration of the Gaussian-shaped pump pulse at the input induces optimal rotational response of the molecules. The probe pulse, which scatters off of the resulting time variation of the refractive index, is shaped at the input for optimal compression at the output, including dispersion to all orders.

Quantum logic approach to wave packet control.

We study control of wave packets with a finite accuracy, approaching it as quantum information processing. For a given control resolution, we define the analogs of several quantum bits within the shape of a single wave packet. These bits are based on wave packet symmetries. Analogs of one- and two-bit gates can be implemented using only free wave packet evolution and coordinate-dependent ac Stark shifts applied at the moments of fractional revivals. As in quantum computation, the gates form a logarithmically small set of basis operations which can be used to approximate any unitary transformation desired for quantum control of the wave packet dynamics. Numerical examples show the application of this approach to control vibrational wave packet revivals.

Coarse-grained controllability of wavepackets by free evolution and phase shifts.

We describe an approach to controlling wavepacket dynamics and a criterion of wavepacket controllability based on discretized properties of the wavepacket's localization on the orbit. The notion of "coarse-grained control" and the coarse-grained description of the controllability in infinite-dimensional Hilbert spaces are introduced and studied using the mathematical apparatus of loop groups. We prove that 2D rotational wavepackets are controllable by only free evolution and phase kicks by AC Stark shift implemented at fractional revivals. This scheme works even if the AC Stark shifts can have only a smooth coordinate dependence, correspondent to the action of a linearly polarized laser field.

Tunable optimal compression of ultrabroadband pulses by cross-phase modulation.

We show how cross-phase modulation between two pulses, combined with optimal pulse shaping at the input of a dielectric medium, can be used to generate nearly single-cycle pulses that are tunable from the ultraviolet to the mid-infrared at the output of the medium, precompensating for dispersion to all orders.

Switched wave packets: a route to nonperturbative quantum control.

The dynamic Stark effect due to a strong nonresonant but nonionizing laser field provides a route to quantum control via the creation of novel superposition states. We consider the creation of a field-free "switched" wave packet through adiabatic turn-on and sudden turn-off of a strong dynamic Stark interaction. There are two limiting cases for such wave packets. The first is a Raman-type coupling, illustrated by the creation of field-free molecular axis alignment. An experimental demonstration is given. The second case is that of dipole-type coupling, illustrated by the creation of charge localization in an array of quantum wells.