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We investigate the effects of the multielectron polarization of the ion described by the induced dipole potential in photoelectron momentum distributions produced in ionization of the CO molecule by a strong laser field. We present results of the numerical solution of the time-dependent Schr\"{o}dinger equation in three spatial dimensions and semiclassical simulations accounting for quantum interference. We predict the change of the asymmetry and interference patterns in two-dimensional photoelectron momentum distributions as well as longitudinal momentum distributions. By using a semiclassical model we identify the mechanism responsible for the observed effects. It is shown that the modifications of electron momentum distributions are caused by a combined effect of the force acting on photoelectrons due to the induced dipole potential and the linear Stark-shift of the ionization potential., Comment: 28 pages, 10 figures

Clusters and nanodroplets hold the promise of enhancing high-order nonlinear optical effects due to their high local density. However, only moderate enhancement has been demonstrated to date. Here, we report the observation of energetic electrons generated by above-threshold ionization (ATI) of helium (He) nanodroplets which are resonantly excited by ultrashort extreme ultraviolet (XUV) free-electron laser pulses and subsequently ionized by near-infrared (NIR) or near-ultraviolet (UV) pulses. The electron emission due to high-order ATI is enhanced by several orders of magnitude compared to He atoms. The crucial dependence of the ATI intensities with the number of excitations in the droplets suggests a local collective enhancement effect.

We extend the semiclassical two-step model [Phys. Rev. A 94, 013415 (2016)] to include a multielectron polarization-induced dipole potential. Using this model we investigate the imprints of multielectron effects in the momentum distributions of photoelectrons ionized by a linearly polarized laser pulse. We predict narrowing of the longitudinal momentum distributions due to electron focusing by the induced dipole potential. We show that the polarization of the core also modifies interference structures in the photoelectron momentum distributions. Specifically, the number of fanlike interference structures in the low-energy part of the electron momentum distribution may be altered. We analyze the mechanisms underlying this interference effect. The account of the multielectron dipole potential seems to improve the agreement between theory and experiment., Comment: 25 pages, 7 figures

Sensors that are able to detect and track single unlabelled biomolecules are an important tool both to understand biomolecular dynamics and interactions at nanoscale, and for medical diagnostics operating at their ultimate detection limits. Recently, exceptional sensitivity has been achieved using the strongly enhanced evanescent fields provided by optical microcavities and nano-sized plasmonic resonators. However, at high field intensities photodamage to the biological specimen becomes increasingly problematic. Here, we introduce an optical nanofibre based evanescent biosensor that operates at the fundamental precision limit introduced by quantisation of light. This allows a four order-of-magnitude reduction in optical intensity whilst maintaining state-of-the-art sensitivity. It enable quantum noise limited tracking of single biomolecules as small as 3.5 nm, and surface-molecule interactions to be monitored over extended periods. By achieving quantum noise limited precision, our approach provides a pathway towards quantum-enhanced single-molecule biosensors., Comment: 17 pages, 4 figures, supplementary information

We present a semiclassical two-step model for strong-field ionization that accounts for path interferences of tunnel-ionized electrons in the ionic potential beyond perturbation theory. Within the framework of a classical trajectory Monte-Carlo representation of the phase-space dynamics, the model employs the semiclassical approximation to the phase of the full quantum propagator in the exit channel. By comparison with the exact numerical solution of the time-dependent Schr\"odinger equation for strong-field ionization of hydrogen, we show that for suitable choices of the momentum distribution after the first tunneling step, the model yields good quantitative agreement with the full quantum simulation. The two-dimensional photoelectron momentum distributions, the energy spectra, and the angular distributions are found to be in good agreement with the corresponding quantum results. Specifically, the model quantitatively reproduces the fan-like interference patterns in the low-energy part of the two-dimensional momentum distributions as well as the modulations in the photoelectron angular distributions., Comment: 31 pages, 7 figures

We investigate polarization squeezing in squeezed coherent states with varying coherent amplitudes. In contrast to the traditional characterization based on the full Stokes parameters, we experimentally determine the Stokes vector of each excitation manifold separately. Only for states with a fixed photon number do the methods coincide; when the photon number is indefinite, our approach gives a richer and deeper description. By capitalising on the properties of the Husimi Q function, we map this notion onto the Poincare space, providing a full account of the measured squeezing., Comment: 5 pages. 5 color figures. Comments welcome!

We numerically study models of $\mathrm{H}_2$ and $\mathrm{LiH}$ molecules, aligned collinearly with the linear polarization of the external field, to elucidate the possible role of correlation in the enhanced-ionization phenomena. Correlation is considered at different levels of approximation with the time-dependent generalized-active-space configuration-interaction method. The results of our studies show that enhanced ionization occurs in multielectron molecules, that correlation is important and they also demonstrate significant deviations between the results of the single-active-electron approximation and more accurate configuration-interaction methods. With the inclusion of correlation we show strong carrier-envelope-phase effects in the enhanced ionization of the asymmetric heteronuclear $\mathrm{LiH}$-like molecule. The correlated calculation shows an intriguing feature of cross-over in enhanced ionization with two carrier-envelope-phases at critical inter-nuclear separation., Comment: 11 pages, 11 figures

We present a study of multiphoton dissociative ionization from molecules. By solving the time-dependent Schr\"{o}dinger equation for H$_2^+$ and projecting the solution onto double continuum scattering states, we observe the correlated electron-nuclear ionization dynamics in detail. We show --- for the first time --- how multiphoton structure prevails as long as the energies of all fragments are accounted for. Our current work provides a new avenue to analyze strong-field fragmentation that leads to a deeper understanding of the correlated molecular dynamics., Comment: 1 Letter with 4 figures, 1 supplemental material

We provide theoretical investigations of the response of the Ar and H atoms to an intense elliptically polarized few-cycle laser pulse, as a function of light ellipticity. The time-dependent Schr{\"o}dinger equation describing the least-bound electron is solved numerically, and differential quantities such as the momentum distribution, the electron density in the continuum, and the above-threshold ionization spectra are computed. These quantities provide insight into the ionization dynamics and the electron rescattering process as a function of light ellipticity, and reveal great similarities between the response of Ar and H to the applied external field.

We propose an operational degree of polarization in terms of the variance of the projected Stokes vector minimized over all the directions of the Poincar\'e sphere. We examine the properties of this degree and show that some problems associated with the standard definition are avoided. The new degree of polarization is experimentally determined using two examples: a bright squeezed state and a quadrature squeezed vacuum., Comment: 4 pages, 2 figures. Comments welcome.

We solve the three-dimensional time-dependent Schr\"{o}dinger equation for a few-cycle circularly polarized femtosecond laser pulse interacting with an oriented target exemplified by an Argon atom, initially in a $3\text{p}_{x}$ or $3\text{p}_{y}$ state. The photoelectron momentum distributions show distinct signatures of the orbital structure of the initial state as well as the carrier-envelope phase of the applied pulse. Our \textit{ab initio} results are compared with results obtained using the length-gauge strong-field approximation, which allows for a clear interpretation of the results in terms of classical physics. Furthermore, we show that ionization by a circularly polarized pulse completely maps out the angular nodal structure of the initial state, thus providing a potential tool for studying orbital symmetry in individual systems or during chemical reactions.

We present a generic approach for treating the effect of nuclear motion in the high-order harmonic generation from polyatomic molecules. Our procedure relies on a separation of nuclear and electron dynamics where we account for the electronic part using the Lewenstein model and nuclear motion enters as a nuclear correlation function. We express the nuclear correlation function in terms of Franck-Condon factors which allows us to decompose nuclear motion into modes and identify the modes that are dominant in the high-order harmonic generation process. We show results for the isotopes CH$_4$ and CD$_4$ and thereby provide direct theoretical support for a recent experiment [Baker {\it et al.}, Science {\bf 312}, 424 (2006)] that uses high-order harmonic generation to probe the ultra-fast structural nuclear rearrangement of ionized methane., Comment: 6 pages, 6 figures

We present an experimental investigation of alkali atom vapor cells coated with a high quality anti-relaxation coating material based on alkenes. The prepared cells with single compound alkene based coating showed the longest spin relaxation times which have been measured up to now with room temperature vapor cells. Suggestions are made that chemical binding of a cesium atom and an alkene molecule by attack to the C=C bond plays a crucial role in such improvement of anti-relaxation coating quality.

We analyse a novel squeezing and entangling mechanism which is due to correlated Stokes and anti-Stokes photon forward scattering in a multi-level atom vapour. Following the proposal we present an experimental demonstration of 3.5 dB pulsed frequency nondegenerate squeezed (quadrature entangled) state of light using room temperature caesium vapour. The source is very robust and requires only a few milliwatts of laser power. The squeezed state is generated in the same spatial mode as the local oscillator and in a single temporal mode. The two entangled modes are separated by twice the Zeeman frequency of the vapour which can be widely tuned. The narrow-band squeezed light generated near an atomic resonance can be directly used for atom-based quantum information protocols. Its single temporal mode characteristics make it a promising resource for quantum information processing.

A theoretical framework for studying strong-field ionization of aligned molecules is presented, and alignment-dependent ionization yields are computed for CO2. Our calculations are in unprecedented agreement with recent experiments. We find that the ionization process is affected by intermediate resonance states, and the alignment-dependent ionization yields do not follow the electron density of the initial states. The theory explains the breakdown of semi-analytical theories, like the molecular tunneling theory and strong-field approximation, were excited electronic structure is neglected., Comment: 4 pages, 6 figures

It is demonstrated that strong laser pulses can introduce torsional motion in the axially chiral molecule 3,5-diflouro-3',5'-dibromo-biphenyl (DFDBrBPh). A nanosecond laser pulse spatially aligns the stereogenic carbon-carbon (C-C) bond axis allowing a perpendicularly polarized, intense femtosecond pulse to initiate torsional motion accompanied by a rotation about the fixed axis. We monitor the induced motion by femtosecond time-resolved Coulomb explosion imaging. Our theoretical analysis corroborates the experimental findings and on the basis of these results we discuss future applications of laser induced torsion, viz., time-resolved studies of de-racemization and laser controlled molecular junctions based on molecules with torsion., Comment: 10 pages, 9 figures, 2 tables; submitted to J. Chem. Phys.

A proof-of-principle experiment is reported, where torsional motion of a molecule, consisting of a pair of phenyl rings, is induced by strong laser pulses. 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. The induced motion is monitored by femtosecond time-resolved Coulomb explosion imaging. Our theoretical analysis accounts for and generalizes the experimental findings., Comment: 4 pages, 4 figures, submitted to PRL; Major revision of the presentation of the material; Correction of ion labels in Fig. 2(a)

Using a quantum mechanical three-step model we present numerical calculations on the high-harmonic generation from four polyatomic molecules. Ethylene (C$_2$H$_4$) serves as an example where orbital symmetry directly affects the harmonic yield. We treat the case of methane (CH$_4$) to address the high-harmonic generation resulting from a molecule with degenerate orbitals. To this end we illustrate how the single orbital contributions show up in the total high-harmonic signal. This example illustrates the importance of adding coherently amplitude contributions from the individual degenerate orbitals. Finally, we study the high-harmonic generation from propane (C$_3$H$_8$) and butane (C$_4$H$_{10}$). These two molecules, being extended and far from spherical in structure, produce harmonics with non-trivial orientational dependencies. In particular, propane can be oriented so that very high-frequency harmonics are favorized, and thus the molecule contains prospects for the generation of UV attosecond pulses., Comment: 9 pages, 6 figures, 1 table

We present a simple quantum mechanical model to describe Coulomb explosion of H$_2^+$ by short, intense, infrared laser pulses. The model is based on the length gauge version of the molecular strong-field approximation and is valid for pulses shorter than 50 fs where the process of dissociation prior to ionization is negligible. The results are compared with recent experimental results for the proton energy spectrum [I. Ben-Itzhak et al., Phys. Rev. Lett. 95, 073002 (2005), B. D. Esry et al., Phys. Rev. Lett. 97, 013003 (2006)]. The predictions of the model reproduce the profile of the spectrum although the peak energy is slightly lower than the observations. For comparison, we also present results obtained by two different tunneling models for this process., Comment: 8 pages, 4 figures

When molecules interact with intense light sources of femtosecond or shorter duration the rotational degrees of freedom are frozen during the response to the strong nonperturbative interaction. We show how the frozen degrees of freedom affect the measurable signals in high-harmonic generation and above threshold ionization. High-harmonic generation exhibits optical coherence in the signal from different orientations of the molecule. For ionization, the contributions from different orientations are added incoherently. The effects are demonstrated for realistic alignment and orientation schemes., Comment: 4 pages, 2 figures

We present a very efficient technique for solving the three-dimensional time-dependent Schrodinger equation. Our method is applicable to a wide range of problems where a fullly three-dimensional solution is required, i.e., to cases where no symmetries exist that reduce the dimensionally of the problem. Examples include arbitrarily oriented molecules in external fields and atoms interacting with elliptically polarized light. We demonstrate that even in such cases, the three-dimensional problem can be decomposed exactly into two two-dimensional problems at the cost of introducing a trivial rotation transformation. We supplement the theoretical framework with numerical results on strong-field ionization of arbitrarily oriented H2+ molecules., Comment: 5 pages, 4 figures

The Gaussian state description of continuous variables is adapted to describe the quantum interaction between macroscopic atomic samples and continuous-wave light beams. The formalism is very efficient: a non-linear differential equation for the covariance matrix of the atomic system explicitly accounts for both the unitary evolution, the dissipation and noise due to the atom-light interaction, and the back-action due to homodyne optical detection on the beam after its interaction with the atoms. Applications to atomic spin squeezing and estimation of unknown classical parameters are presented, and extensions beyond the Gaussian states are discussed., Comment: 15 pages, 4 figures. Modified version of a contribution to the book "Quantum Information with Continuous Variables", Eds. G. Leuchs, N. Cerf, and E. Polzik. To be published by Imperial College Press

We show how to prepare a single molecular ion in a specific internal quantum state in a situation where the molecule is trapped and sympathetically cooled by an atomic ion and where its internal degrees of freedom are initially in thermal equilibrium with the surroundings. The scheme is based on conditional creation of correlation between the internal state of the molecule and the translational state of the collective motion of the two ions, followed by a projection measurement of this collective mode by atomic ion shelving techniques. State preparation in a large number of internal states is possible., Comment: 4 pages, 2 figures, 2 tables

The exact nondipole minimal-coupling Hamiltonian for an atom interacting with an explicitly time- and space-dependent laser field is transformed into the rest frame of a classical free electron in the laser field, i.e., into the Kramers-Henneberger frame. The new form of the Hamiltonian is used to study nondipole effects in the high-intensity, high-frequency regime. Fully three dimensional nondipole {\it ab initio} wavepacket calculations show that the ionization probability may decrease for increasing field strength. We identify a unique signature for the onset of this dynamical stabilization effect in the photoelectron spectrum., Comment: 4 pages, 3 figures

We present three dimensional time-dependent calculations of ionization of arbitrarily spatially oriented H$_2^+$ by attosecond, intense, high-frequency laser fields. The ionization probability shows a strong dependence on both the internuclear distance and the relative orientation between the laser field and the internuclear axis., Comment: 4 pages, 4 figures

The translational motion of molecular ions can be effectively cooled sympathetically to translational temperatures below 100 mK in ion traps through Coulomb interactions with laser-cooled atomic ions. The ro-vibrational degrees of freedom, however, are expected to be largely unaffected during translational cooling. We have previously proposed schemes for cooling of the internal degrees of freedom of such translationally cold but internally hot heteronuclear diatomic ions in the simplest case of ^1-Sigma electronic ground state molecules. Here we present a significant simplification of these schemes and make a generalization to the most frequently encountered electronic ground states of heteronuclear molecular ions: ^1-Sigma, ^2-Sigma, ^3-Sigma and ^2-Pi. The schemes are relying on one or two laser driven transitions with the possible inclusion of a tailored incoherent far infrared radiation field., Comment: 16 pages, 13 figures

We investigate theoretically the application of tailored incoherent far-infrared fields in combination with laser excitation of a single rovibrational transition for rotational cooling of translationally cold polar diatomic molecules. The cooling schemes are effective on a timescale shorter than typical unperturbed trapping times in ion traps and comparable to obtainable confinement times of neutral molecules., Comment: 5 pages, 2 figures

The translational motion of molecular ions can be effectively cooled sympathetically to temperatures below 100 mK in ion traps through Coulomb interactions with laser-cooled atomic ions. The distribution of internal rovibrational states, however, gets in thermal equilibrium with the typically much higher temperature of the environment within tens of seconds. We consider a concept for rotational cooling of such internally hot, but translationally cold heteronuclear diatomic molecular ions. The scheme relies on a combination of optical pumping from a few specific rotational levels into a ``dark state'' with redistribution of rotational populations mediated by blackbody radiation., Comment: 4 pages, 5 figures