Lars Bojer Madsen

Measurement and laser control of attosecond charge migration in ionized iodoacetylene.

Electronic movement flashing into view Numerous chemical processes begin with ionization: the ejection of an electron from a molecule. What happens in the immediate aftermath of that event? Kraus et al. explored this question in iodoacetylene by detecting and analyzing the spectrum of emitted high harmonics (see the Perspective by Ueda). They traced the migration of the residual positively charged hole along the molecular axis on a time scale faster than a quadrillionth of a second. They thereby characterized the capacity of a laser field to steer the holes motion in appropriately oriented molecules. Science, this issue p. 790; see also p. 740 High harmonics reveal fine details of electronic rearrangement in a molecule in the first instants after ionization. [Also see Perspective by Ueda] The ultrafast motion of electrons and holes after light-matter interaction is fundamental to a broad range of chemical and biophysical processes. We advanced high-harmonic spectroscopy to resolve spatially and temporally the migration of an electron hole immediately after ionization of iodoacetylene while simultaneously demonstrating extensive control over the process. A multidimensional approach, based on the measurement and accurate theoretical description of both even and odd harmonic orders, enabled us to reconstruct both quantum amplitudes and phases of the electronic states with a resolution of ~100 attoseconds. We separately reconstructed quasi–field-free and laser-controlled charge migration as a function of the spatial orientation of the molecule and determined the shape of the hole created by ionization. Our technique opens the prospect of laser control over electronic primary processes.

Photoelectron angular distributions from strong-field ionization of oriented molecules

An experimental study shows how a polar molecule can be oriented in three dimensions by using a combination of laser and electrostatic fields. The approach should help to obtain molecular-frame information about strong-field ionization processes in molecules for which the orientation cannot be determined after ionization.

Quantum gates and multiparticle entanglement by Rydberg excitation blockade and adiabatic passage.

We propose to apply stimulated adiabatic passage to transfer atoms from their ground state into Rydberg excited states. Atoms a few micrometers apart experience a dipole-dipole interaction among Rydberg states that is strong enough to shift the atomic resonance and inhibit excitation of more than a single atom. We show that the adiabatic passage in the presence of this interaction between two atoms leads to robust creation of maximally entangled states and to two-bit quantum gates. For many atoms, the excitation blockade leads to an effective implementation of collective-spin and Jaynes-Cummings-like Hamiltonians, and we show that the adiabatic passage can be used to generate collective J_{x}=0 eigenstates and Greenberger-Horne-Zeilinger states of tens of atoms.

Manipulating the torsion of molecules by strong laser pulses.

We demonstrate that strong laser pulses can induce torsional motion in a molecule consisting of a pair of phenyl rings. A nanosecond laser pulse spatially aligns the carbon-carbon bond axis, connecting the two phenyl rings, allowing a perpendicularly polarized, intense femtosecond pulse to initiate torsional motion accompanied by an overall rotation about the fixed axis. We monitor the induced motion by femtosecond time-resolved Coulomb explosion imaging. Our theoretical analysis accounts for and generalizes the experimental findings.

Spin squeezing and precision probing with light and samples of atoms in the Gaussian description

We consider an ensemble of trapped atoms interacting with a continuous-wave laser field. For sufficiently polarized atoms and for a polarized light field, we may approximate the nonclassical components of the collective spin angular momentum operator for the atoms and the Stokes vectors of the field by effective position and momentum variables for which we assume a Gaussian state. Within this approximation, we present a theory for the squeezing of the atomic spin by polarization rotation measurements on the probe light. We derive analytical expressions for the squeezing with and without inclusion of the noise effects introduced by atomic decay and by photon absorption. The theory is readily adapted to the case of inhomogeneous light-atom coupling [A. Kuzmich and T.A.B. Kennedy, Phys. Rev. Lett. 92, 030407 (2004)]. As a special case, we show how to formulate the theory for an optically thick sample by slicing the gas into pieces, each having only small photon absorption probability. Our analysis of a realistic probing and measurement scheme shows that it is the maximally squeezed component of the atomic gas that determines the accuracy of the measurement.

Extending the strong-field approximation of high-order harmonic generation to polar molecules: gating mechanisms and extension of the harmonic cutoff

Polar molecules such as CO are interesting target systems for high-order harmonic generation (HHG) as they can be oriented with current laser techniques, thus allowing the study of systems without inversion symmetry. However, the asymmetry of the molecule also means that the molecular orbitals are Stark shifted in energy due to their interaction with the driving laser. We extend the strong-field approximation of HHG by incorporating the Stark shift into the Lewenstein model and discuss its impact on two different gating mechanisms in CO. In system-induced gating an oriented target molecule serves as a gate by selecting every other half-cycle due to an increased (decreased) ionization rate. In field-induced gating the waveform of the driving laser is tailored such that the harmonic emission from an aligned molecule is damped (enhanced) every other half-cycle. We show that the Stark shift weakens the strength of system-induced gating and also determines the relative contribution from opposite orientations in field-induced gating. Finally, we propose a novel scheme for extending the high-order harmonic cutoff by letting the two gating mechanisms counteract each other, thus allowing for a higher laser intensity without increased ionization of the target gas.

Symmetry of Carrier-Envelope Phase Difference Effects in Strong-Field, Few-Cycle Ionization of Atoms and Molecules

In few-cycle pulses, the exact value of the carrier-envelope phase difference (CEPD) has a pronounced influence on the ionization dynamics of atoms and molecules. We show that, for atoms in circularly polarized light, a change in the CEPD is mapped uniquely to an overall rotation of the system, and results for arbitrary CEPD are obtained by rotation of the results from a single calculation with fixed CEPD. For molecules, this is true only for linear molecules aligned parallel with the propagation direction of the field. The effects of CEPD are classified as geometric or nongeometric. The observations are exemplified by strong-field calculations on hydrogen.

Time-dependent restricted-active-space self-consistent-field theory for laser-driven many-electron dynamics

We present the time-dependent restricted-active-space self-consistent field (TD-RASSCF) theory as a new framework for the time-dependent many-electron problem. The theory generalizes the multiconfigurational time-dependent Hartree-Fock (MCTDHF) theory by incorporating the restricted-active-space scheme well known in time-independent quantum chemistry. Optimization of the orbitals as well as the expansion coefficients at each time step makes it possible to construct the wave function accurately while using only a relatively small number of electronic configurations. In numerical calculations of high-order harmonic generation spectra of a one-dimensional model of atomic beryllium interacting with a strong laser pulse, the TD-RASSCF method is reasonably accurate while largely reducing the computational complexity. The TD-RASSCF method has the potential to treat large atoms and molecules beyond the capability of the MCTDHF method.

High-order harmonic generation from arbitrarily oriented diatomic molecules including nuclear motion and field-free alignment

We present a theoretical model of high-harmonic generation from diatomic molecules. The theory includes effects of alignment as well as nuclear motion and is used to predict results for N{sub 2}, O{sub 2}, H{sub 2}, and D{sub 2}. The results show that the alignment dependence of high-harmonics is governed by the symmetry of the highest occupied molecular orbital and that the inclusion of the nuclear motion in the theoretical description generally reduces the intensity of the harmonic radiation. We compare our model with experimental results on N{sub 2} and O{sub 2}, and obtain very good agreement.

Probing the longitudinal momentum spread of the electron wave packet at the tunnel exit.

We present an ellipticity resolved study of momentum distribution arising from strong-field ionization of helium. The influence of the ion potential on the departing electron is considered within a semi-classical model consisting of an initial tunneling step and subsequent classical propagation. We find that the momentum distribution can be explained by including the longitudinal momentum spread of the electron at the exit from the tunnel. Our combined experimental and theoretical study provides an estimate of this momentum spread.