Highlights of 2016

We investigate the process of circularly polarized high harmonic generation in molecules using a bicircular laser field. In this context, we show that molecules offer a very robust framework for the production of circularly polarized harmonics, provided their symmetry is compatible with that of the laser field. Using a discrete time-dependent symmetry analysis, we show how all the features (harmonic order and polarization) of spectra can be explained and predicted. The symmetry analysis is generic and can easily be applied to other target and/or field configurations.

A few-body approach relying on static line broadening theory is developed to treat the spectroscopy of a single Rydberg excitation to a trilobite-like state immersed in a high density ultracold medium. The present theoretical framework implements the recently developed compact treatment of polyatomic Rydberg molecules, allowing for an accurate treatment of a large number of perturbers within the Rydberg orbit. This system exhibits two unique spectral signatures: its lineshape depends on the Rydberg quantum number n but, strikingly, is independent of the density of the medium, and it is characterized by sharply peaked features reflecting the oscillatory structure of the potential energy landscape.

Photoelectron circular dichroism is investigated experimentally as a function of the number of absorbed circularly polarized photons. Three structurally different chiral molecules yet showing similar absorption spectra are studied. They are isotropically distributed in the gas phase and ionized with femtosecond laser pulses. We measure and analyze the photoelectron angular distribution of threshold electrons ionized with three photons and compare them to those of above-threshold (ATI) electrons ionized with four photons. Additionally to an increase in high even order Legendre polynomials the coefficients of the high odd order Legendre polynomials rise with increasing photon number. Consequently, the ATI electrons also carry the chirality signature. All investigated chiral molecules reveal an individual set of coefficients for the threshold and ATI signatures despite their similarities in chemical structure. The presented data set can serve as a guideline for theoretical modeling of the interaction of circularly polarized light with chiral molecules in the multiphoton regime.

Considering the photoionization of Ar@${{rm{C}}}_{60}$ and Kr@${{rm{C}}}_{60}$ endofullerenes, the decay of ${{rm{C}}}_{60}$ innershell excitations through the outershell continuum of the confined atom via the inter-Coulombic decay (ICD) pathway is detailed. Excitations to atom-${{rm{C}}}_{60}$ hybrid states, when these states exist, can induce coherence between ICD and electron-transfer mediated decay (ETMD). This should be the dominant above-threshold decay process for a variety of confined systems, and the strength of these resonances is such that they should be amenable for study by photoelectron spectroscopy.

We have performed a kinematically complete experiment on ionization of H₂ by 75 keV proton impact for electrons ejected with a speed close to the projectile speed. The fully differential data are compared to a three-body distorted wave and a continuum distorted wave—eikonal initial state calculation. Large discrepancies between experiment and theory, as well as between both calculations, are found. These probably arise from a strong coupling between the ionization and capture channels, which is not accounted for by theory.

Electron emission caused by extreme ultraviolet (XUV) radiation in the presence of a strong near infrared (NIR) field leads to multiphoton interactions that depend on several parameters. Here, a comprehensive study of the influence of the angle between the polarization directions of the NIR and XUV fields on the two-color angle-resolved photoelectron spectra of He and Ne is presented. The resulting photoelectron angular distribution strongly depends on the orientation of the NIR polarization plane with respect to that of the XUV field. The prevailing influence of the intense NIR field over the angular emission characteristics for He(1s) and Ne(2p) ionization lines is shown. The underlying processes are modeled in the frame of the strong field approximation (SFA) which shows very consistent agreement with the experiment reaffirming the power of the SFA for multicolor-multiphoton ionization in this regime.

We present an investigation of resonances with natural and unnatural parities in the positron-potassium system using the complex scaling method. A model potential is used to represent the interaction between the core and the valence electron. Explicitly correlated Gaussian wave functions are used to represent the correlation effects between the valence electron, the positron and the K⁺ core. Resonance energies and widths for two partial waves (S- and P-wave) below the ${rm{K}}(4p,5;s,5p,4;d,4f)$ excitation thresholds and positronium n = 2 formation threshold are calculated for natural parity. Resonance states for P^e below the ${rm{K}}(4d)$ excitation threshold and positronium n = 2, 3 formation thresholds are calculated for unnatural parity which has not been previously reported. Below both positronium thresholds we have found a dipole series of resonances, with binding energies scaling in good agreement with exceptions from an analytical calculation. The present results are compared with those in the literature.

We propose a method to create higher orbital states of ultracold atoms in the Mott regime of an optical lattice. This is done by periodically modulating the position of the trap minima (known as shaking) and controlling the interference term of the lasers creating the lattice. These methods are combined with techniques of shortcuts to adiabaticity. As an example of this, we show specifically how to create an anti-ferromagnetic type ordering of angular momentum states of atoms. The specific pulse sequences are designed using Lewis–Riesenfeld invariants and a four-level model for each well. The results are compared with numerical simulations of the full Schrödinger equation.

The coherent interaction with ultrashort light pulses is a powerful strategy for monitoring and controlling the dynamics of wave packets in all states of matter. As light presents an oscillation period of a few femtoseconds (T = 2.6 fs in the near infrared spectral range), an external optical field can induce changes in a medium on the sub-cycle timescale, i.e. in a few hundred attoseconds. In this work, we resolve the dynamics of autoionizing states on the femtosecond timescale and observe the sub-cycle evolution of a coherent electronic wave packet in a diatomic molecule, exploiting a tunable ultrashort extreme ultraviolet pulse and a synchronized infrared field. The experimental observations are based on measuring the variations of the extreme ultraviolet radiation transmitted through the molecular gas. The different mechanisms contributing to the wave packet dynamics are investigated through theoretical simulations and a simple three level model. The method is general and can be extended to the investigation of more complex systems.

Over the years many He–He interaction potentials have been developed, some very sophisticated, including various corrections beyond the Born–Oppenheimer approximation. Most of them were used to predict properties of helium dimers and trimers, examples of exotic quantum states, whose experimental study proved to be very challenging. Recently, detailed structural properties of helium trimers were measured for the first time, allowing a comparison with theoretical predictions and possibly enabling the evaluation of different interaction potentials. The comparisons already made included adjusting the maxima of both theoretical and experimental correlation functions to one, so the overall agreement between theory and experiment appeared satisfactory. However, no attempt was made to evaluate the quality of the interaction potentials used in the calculations. In this work, we calculate the experimentally measured correlation functions using both new and old potentials, compare them with experimental data and rank the potentials. We use diffusion Monte Carlo simulations at T = 0, which give within statistical noise exact results of the ground state properties. All models predict both trimers ⁴He₃ and ⁴He${}_{2}{}^{3}$He to be in a quantum halo state.

Molecular frame photoelectron angular distributions (MFPADs) are measured in electron–ion momentum imaging experiments and compared with complex Kohn variational calculations for carbon K-shell ionization of carbon tetrafluoride (CF₄), ethane (C₂H₆) and 1,1-difluoroethylene (C₂H₂F₂). While in ethane the polarization averaged MFPADs show a tendency at low energies for the photoelectron to be emitted in the directions of the bonds, the opposite effect is seen in CF₄. A combination of these behaviors is seen in difluoroethylene where ionization from the two carbons can be distinguished experimentally because of their different K-shell ionization potentials. Excellent agreement is found between experiment and simple static-exchange or coupled two-channel theoretical calculations. However, simple electrostatics do not provide an adequate explanation of the suggestively simple angular distributions at low electron ejection energies.

An electrostatic beam has been used to perform scattering measurements with an angular-discrimination of $lesssim 2^circ$. The total cross sections of positrons scattering from helium and krypton have been determined in the energy range (10–300) eV. This work was initially stimulated by the investigations of Nagumo et al (2011 J. Phys. Soc. Japan 80 064301), the first positron field-free measurements performed with a similarly high resolution, which found significant discrepancies at low energies with most other experiments and theories. The present results show good agreement with theories and several other measurements, even those characterized by a much poorer angular discrimination, implying a small contribution from particles elastically scattered at forward angles, as theoretically predicted for He but not for Kr.

Experimental and theoretical results are reported for single-photon single ionization of ${{rm{W}}}^{2+}$ and W³⁺ tungsten ions. Experiments were performed at the photon–ion merged-beam setup of the Advanced Light Source in Berkeley. Absolute cross sections and detailed energy scans were measured over an energy range 20–90 eV at a bandwidth of 100 meV. Broad peak features with widths typically around 5 eV have been observed with almost no narrow resonances present in the investigated energy range. Theoretical results were obtained from a Dirac–Coulomb R-matrix approach. The calculations were carried out for the lowest-energy terms of the investigated tungsten ions with levels ${5{{rm{s}}}^{2}5{{rm{p}}}^{6}5{{rm{d}}}^{4}{}^{5}{rm{D}}}_{J}$ $J=0,1,2,3,4$ for ${{rm{W}}}^{2+}$ and ${5{{rm{s}}}^{2}5{{rm{p}}}^{6}5{{rm{d}}}^{3}{}^{4}{rm{F}}}_{{J}^{prime }}$ ${J}^{prime }=3/2,5/2,7/2,9/2$ for ${{rm{W}}}^{3+}$. Assuming a statistically weighted distribution of ions in the initial ground-term levels there is good agreement of theory and experiment for ${{rm{W}}}^{3+}$ ions. However, for ${{rm{W}}}^{2+}$ ions at higher energies there is a factor of approximately two difference between experimental and theoretical cross sections.

We explore the Casimir effect on an interacting Bose–Einstein condensate (BEC) inside a cylindrical tube. The Casimir force for the confined BEC consists of (i) a mean-field part arising from the spatial inhomogeneity of the condensate order parameter, and (ii) a quantum fluctuation part arising from the confinement of Bogoliubov excitations in the condensate. Our analytical result predicts Casimir force on a cylindrical shallow of ⁴He well below the λ-point, and can be tested experimentally.

We have developed and implemented a compact transparent nozzle for use in laser vaporization sources. This nozzle eliminates the need for an ablation aperture, allowing for a more intense molecular beam. We use this nozzle to prepare a molecular beam of aluminum monohydride (AlH) suitable for ion trap loading of AlH⁺ via photoionization in ultra-high vacuum. We demonstrate stable AlH production over hour time scales using a liquid ablation target. The long-term stability, low heat load and fast ion production rate of this source are well-suited to molecular ion experiments employing destructive state readout schemes requiring frequent trap reloading.

Heteronuclear alkali-metal dimers represent the class of molecules of choice for creating samples of ultracold molecules exhibiting an intrinsic large permanent electric dipole moment. Among them, the KCs molecule, with a permanent dipole moment of 1.92 Debye still remains to be observed in ultracold conditions. Based on spectroscopic studies available in the literature completed by accurate quantum chemistry calculations, we propose several optical coherent schemes to create ultracold bosonic and fermionic KCs molecules in their absolute rovibrational ground level, starting from a weakly bound level of their electronic ground state manifold. The processes rely on the existence of convenient electronically excited states allowing an efficient stimulated Raman adiabatic transfer of the level population.

There is increasing interest in cold heavy polar molecular species for their applications in fundamental physics, such as the tests of the electron's electric dipole moment. Here we propose a switched ring Stark decelerator suitable for slowing both light and heavy polar molecules. Two typical polar molecular species, ND₃ and ²⁰⁵TlF, are employed to test the feasibility of our scheme with the help of trajectory calculation. Our proposed scheme is found to share many advantages with the state-of-the-art traveling wave decelerator, yet with relatively simple electronics and flexible operation modes. Sub-millikelvin molecular samples can be conveniently obtained in our decelerator using a combined operation mode. These monochromatic beams are ideal starting points for precise studies of molecular collision, cold chemistry and high-resolution spectroscopy.

We investigate the interplay of diffraction and nonlinear effects during the propagation of very short light pulses. Adapting the factorization approach to the problem at hand by keeping the transverse-derivative terms apart from the residual nonlinear contributions we derive an unidirectional propagation equation which is valid for weak dispersion and reduces to the slowly-evolving-wave-approximation in the case of paraxial rays. A comparison of the numerical simulation results for the two equations shows pronounced differences when self-focusing plays an important role. We devote special attention to modelling the propagation of ultrashort terahertz pulses taking into account diffraction as well as Kerr-type and second-order nonlinearities. Comparing the measured and simulated wave forms we deduce the value of the nonlinear refractive index of lithium niobate in the terahertz region to be three orders of magnitude larger than in the visible part of the spectrum.

The dynamics of the Dicke model, which describes the interaction of N two-level atoms with a resonant field mode, is studied in the presence of dissipation and in strong non-equilibrium for a moderate number of atoms. Starting from a highly excited state, it is investigated to what extent signatures of superradient phenomena known from the thermodynamic limit $Nto infty$, namely, superradiant light emission and atom-field correlations characteristic for the superradiant phase, appear on transient time scales. Attention is also paid to subtleties of modeling dissipation in the weak coupling limit and to the dynamics in phase space. The latter allows phase space correlators to be defined as indicators for collective behavior on transient time scales. These findings may be of relevance for the realization of Dicke physics with superconducting circuits.

We investigate a hybrid optomechanical system consisting of an ensemble of quantum emitters inside a standard optomechanical cavity with a moving end mirror, in which the motion of the mirror changes the transition rate of each emitter and therefore leads to a direct coupling between the internal state of the quantum emitter and the mechanical mode. We analyzed the steady-state characteristics of the optomechanical system and found that the bistability of the system depends strongly on the distance between the emitter ensemble and the mirror. Further, we also analyze in detail the influences of the distance and other system parameters, i.e., the effective detunings, the driving power, the decay rates of the cavity, and the emitter ensemble and the thermal phonons on the steady-state entanglement by considering fluctuation of the mechanical oscillator, the cavity field, and the emitter ensemble. It is found that the degree of the steady-state entanglement can be greatly enhanced in a certain range of parameters by increasing the vacuum-induced emitter–mirror coupling, which can be realized by decreasing the emitter–mirror distance and increasing properly the free-space spontaneous emission rate of the emitter.

We report the generation of coherent water-window soft x-ray harmonics in a neon-filled semi-infinite gas cell driven by a femtosecond multi-mJ mid-infrared optical parametric chirped-pulse amplification (OPCPA) system at a 1 kHz repetition rate. The cutoff energy was extended to ∼450 eV with a 2.1 μm driver wavelength and a photon flux of $sim 1.5times {10}^{6}$ photons/s/1% bandwidth was obtained at 350 eV. A comparable photon flux of $sim 1.0times {10}^{6}$ photons/s/1% bandwidth was observed at the nitrogen K-edge of 410 eV. This is the first demonstration of water-window harmonic generation up to the nitrogen K-edge from a kHz OPCPA system. Finally, this system is suitable for time-resolved soft x-ray near-edge absorption spectroscopy. Further scaling of the driving pulse's energy and repetition rate is feasible due to the availability of high-power picosecond Yb-doped pump laser technologies, thereby enabling ultrafast, tabletop water-window x-ray imaging.

Time-delays in the photoionization of molecules are investigated. As compared to atomic ionization, the time-delays expected from molecular ionization present a much richer phenomenon, with a strong spatial dependence due to the anisotropic nature of the molecular scattering potential. We investigate this from a scattering theory perspective, and make use of molecular photoionization calculations to examine this effect in representative homonuclear and hetronuclear diatomic molecules, nitrogen and carbon monoxide. We present energy and angle-resolved maps of the Wigner delay time for single-photon valence ionization, and discuss the possibilities for experimental measurements.

A proposed new method of cooling positronium is to realize the Bose–Einstein condensation (BEC) of positronium. We perform detailed studies of three processes: (1) thermalization processes between positronium and the silica walls of a cavity, (2) Ps–Ps scattering and (3) laser cooling. The thermalization process is shown to be not sufficient for BEC. Ps–Ps collision is shown to have a big effect on the cooling performance. We combine both methods and establish an efficient cooling process for BEC. We also propose a new optical laser system for the cooling.

The Virtual Atomic and Molecular Data Centre (VAMDC) Consortium is a worldwide consortium which federates atomic and molecular databases through an e-science infrastructure and an organisation to support this activity. About 90% of the inter-connected databases handle data that are used for the interpretation of astronomical spectra and for modelling in many fields of astrophysics. Recently the VAMDC Consortium has connected databases from the radiation damage and the plasma communities, as well as promoting the publication of data from Indian institutes. This paper describes how the VAMDC Consortium is organised for the optimal distribution of atomic and molecular data for scientific research. It is noted that the VAMDC Consortium strongly advocates that authors of research papers using data cite the original experimental and theoretical papers as well as the relevant databases.

In this review we summarize the recent calculations and improvements of atomic data that we have carried out for the analysis of astrophysical spectroscopy within the atomic processes for astrophysical plasmas network. We briefly discuss the various methods used for the calculations, and highlight several issues that we have uncovered during such extensive work. We discuss the completeness and accuracy of the cross sections for ionic excitation by electron impact for the main isoelectronic sequences, which we have obtained with large-scale calculations. Given its astrophysical importance, we emphasize the work on iron. Some examples on the significant improvement that has been achieved over previous calculations are provided.

We demonstrate multiple photon cycling and radiative force deflection on the triatomic free radical strontium monohydroxide (SrOH). Optical cycling is achieved on SrOH in a cryogenic buffer-gas beam by employing the rotationally closed $P(N^{primeprime} =1)$ branch of the vibronic transition ${tilde{X}}^{2}{{rm{Sigma }}}^{+}(000)leftrightarrow {tilde{A}}^{2}{{rm{Pi }}}_{1/2}(000)$. A single repumping laser excites the Sr–O stretching vibrational mode, and photon cycling of the molecule deflects the SrOH beam by an angle of $0.2^circ$ via scattering of ∼100 photons per molecule. This approach can be used for direct laser cooling of SrOH and more complex, isoelectronic species.

Laser slowing of CaF molecules down to the capture velocity of a magneto-optical trap for molecules is achieved. Starting from a two-stage buffer gas beam source, we apply frequency-broadened 'white-light' slowing and observe approximately $6times {10}^{4}$ CaF molecules in a single pulse with velocities 10 ± 4 m s⁻¹. CaF is a candidate for collisional studies in the mK regime. This work represents a significant step towards magneto-optical trapping of CaF.

The role of the geometric phase effect on chemical reaction dynamics is explored by examining the hydrogen exchange process in the fundamental H+HD reaction. Results are presented for vibrationally excited HD molecules in the v = 4 vibrational level and for collision energies ranging from 1 μK to 100 K. It is found that, for collision energies below 3 K, inclusion of the geometric phase leads to dramatic enhancement or suppression of the reaction rates depending on the final quantum state of the HD molecule. The effect was found to be the most prominent for rotationally resolved integral and differential cross sections but it persists to a lesser extent in the vibrationally resolved and total reaction rate coefficients. However, no significant GP effect is present in the reactive channel leading to the D+H₂ product or in the D+H₂$(v=4,j=0),to$ HD+H reaction. A simple interference mechanism involving inelastic (nonreactive) and exchange scattering amplitudes is invoked to account for the observed GP effects. The computed results also reveal a shape resonance in the H+HD reaction near 1 K and the GP effect is found to influence the magnitude of the resonant part of the cross section. Experimental detection of the resonance may allow a sensitive probe of the GP effect in the H+HD reaction.

Mixtures of polarized fermions of two different masses can form weakly bound clusters, such as dimers and trimers, that are universally described by the scattering length between the heavy and light fermions. We use the resonating group method to investigate the low-energy scattering processes involving dimers or trimers. The method reproduces approximately the known particle–dimer and dimer–dimer scattering lengths. We use it to estimate the trimer–trimer scattering length, which is presently unknown, and find it to be positive.

Using the multipolar expansion of electrostatic and magnetostatic potential energies, we characterize the long-range interactions between two weakly-bound diatomic molecules, taking as an example the paramagnetic Er₂ Feshbach molecules which were produced recently. Since inside each molecule individual atoms conserve their identity, the intermolecular potential energy can be expanded as the sum of pairwise atomic potential energies. In the case of Er₂ Feshbach molecules, we show that the interaction between atomic magnetic dipoles gives rise to the usual ${R}^{-3}$ term of the multipolar expansion, where R is the intermolecular distance, but also to additional terms scaling as ${R}^{-5},$ ${R}^{-7},$ and so on. Those terms are due to the interaction between effective molecular multipole moments, and are strongly anisotropic with respect to the orientation of the molecules. Similarly, the atomic pairwise van der Waals interaction results in ${R}^{-6},$ ${R}^{-8},$ ... terms in the intermolecular potential energy. By calculating the reduced electric-quadrupole moment of erbium ground level $langle {}^{3}{H}_{6}| | {hat{Q}}_{2}| | {}^{3}{H}_{6}rangle =-1.305$ a.u., we also demonstrate that the electric–quadrupole interaction energy is negligible with respect to the magnetic dipole and van der Waals interaction energies. The general formalism presented in this article can be applied to calculate the long-range potential energy between arbitrary charge distributions composed of almost free subsystems.

We describe a gas-phase x-ray scattering experiment capable of capturing molecular motions with atomic spatial resolution and femtosecond time resolution. X-ray free electron lasers can deliver intense x-ray pulses of ultrashort duration, making them suitable to study ultrafast chemical reaction dynamics in an ultraviolet pump, x-ray probe scheme. A cell diffractometer balances sample flow with gas density and laser focusing conditions to provide adequate scattering vector resolution with high signal intensity and near-uniform excitation probability. Images from a pixel-array x-ray detector, spatially and electronically calibrated, allow for detection of scattering intensity changes below 1%. First experiments on the ring-opening reaction of 1,3-cyclohexadiene to form 1, 3, 5-hexatriene show a rapid initial reaction on an 80 fs time scale.

We present the design and optimization of a new instrument for ultrafast electron diffraction and imaging. The proposed instrument merges the high peak current and relativistic electron energies of radio-frequency guns, with the high average electron flux of static electron microscopes, extending the beam parameter space achievable with relativistic electrons by many orders of magnitude. An immediate consequence of this work is a broader range of accessible science by using electron probes, enabling techniques as femtosecond nano-diffraction and coherent diffraction imaging, and paving the way to direct observation of ultrafast dynamics in complex and isolated samples, from nanocrystals, to nano/micro droplets and organic molecules.

Here we propose a miniaturized electron source driven by recent experimental results of laser-triggered electron emission from tungsten nanotips and dielectric laser acceleration of sub relativistic electrons with velocities as low as $5.7times {10}^{7};{rm{m}};{{rm{s}}}^{-1}$ or energies as low as 9.6 keV, less than 20% of the speed of light. The recently observed laser-triggered emission of coherent low-emittance electron pulses from tungsten nanotips naturally lends itself towards incorporation with subrelativistic dielectric laser accelerators (DLAs). These structures have previously been shown to accelerate 28 keV electrons and here we report on the utilization of the 4th and 5th spatial harmonics of near fields in the single grating DLA to achieve acceleration of electrons with kinetic energies of 15.2 and 9.6 keV. We then propose the combination of needle tip emitters with subrelativistic accelerators to form a mm-scale device capable of producing electrons with arbitrary energies.

We selectively create p-wave Feshbach molecules in the ${m}_{l}=pm 1$ orbital angular momentum projection state of ⁶Li. We use an optical lattice potential to restrict the relative momentum of the atoms such that only the ${m}_{l}=pm 1$ molecular state couples to the atoms at the Feshbach resonance. We observe the hollow-centered dissociation profile, which is a clear indication of the selective creation of p-wave molecules in the ${m}_{l}=pm 1$ states. We also measure the dissociation energy of the p-wave molecules created in the optical lattice and develop a theoretical formulation to explain the dissociation energy as a function of the magnetic field ramp rate for dissociation. The capability of selecting one of the two closely-residing p-wave Feshbach resonances is useful for the precise characterization of the p-wave Feshbach resonances.

We show that the singlet fraction p_s and total magnetisation (or polarisation) m can bound the minimum concurrence in an ensemble of spins. We identify ${p}_{{rm{s}}}gt (1-{m}^{2})/2$ as a sufficient and tight condition for bipartite entanglement. Our proof makes no assumptions about the state of the system or symmetry of the particles, and can therefore be used as a witness for spin entanglement between fermions. We discuss the implications for recent experiments in which spin correlations were observed, and the prospect to study entanglement dynamics in the demagnetisation of a cold Fermi gas.

We present quantum mechanical calculations of autoionization rates for two rubidium Rydberg atoms with weakly overlapping electron clouds. We neglect exchange effects and consider tensor products of independent atom states forming an approximate basis of the two-electron state space. We consider large sets of two-atom states with randomly chosen quantum numbers and find that the charge overlap between the two Rydberg electrons allows one to characterise the magnitude of the autoionization rates. If the electron clouds overlap by more than one percent, the autoionization rates increase approximately exponentially with the charge overlap. This finding is independent of the energy of the initial state.

We experimentally characterize the optical nonlinear response of a cold atomic medium placed inside an optical cavity, and excited to Rydberg states. The excitation to S and D Rydberg levels is carried out via a two-photon transition in an electromagnetically induced transparency configuration, with a weak (red) probe beam on the lower transition, and a strong (blue) coupling beam on the upper transition. The observed optical nonlinearities induced by S states for the probe beam can be explained using a semi-classical model with van der Waals' interactions. For the D states, it appears necessary to take into account a dynamical decay of Rydberg excitations into a long-lived dark state. We show that the measured nonlinearities can be explained by using a Rydberg bubble model with a dynamical decay.

We investigate the coherent manipulation of interacting Rydberg atoms placed inside a high-finesse optical cavity for the deterministic preparation of strongly coupled light-matter systems. We consider a four-level diamond scheme with one common Rydberg level for N interacting atoms. One side of the diamond is used to excite the atoms into a collective 'superatom' Rydberg state using either π-pulses or stimulated Raman adiabatic passage (STIRAP) pulses. The upper transition on the other side of the diamond is used to transfer the collective state to one that is coupled to a field mode of an optical cavity. Due to the strong interaction between the atoms in the Rydberg level, the Rydberg blockade mechanism plays a key role in the deterministic quantum state synthesis of the atoms in the cavity. We use numerical simulation to show that non-classical states of light can be generated and that the state that is coupled to the cavity field is a collective one. We also investigate how different decay mechanisms affect this interacting many-body system. We also analyze our system in the case of two Rydberg excitations within the blockade volume. The simulations are carried out with parameters corresponding to realizable high-finesse optical cavities and alkali atoms like rubidium.

Sufficiently high densities in Bose–Einstein condensates provide favorable conditions for the production of ultralong-range polyatomic molecules consisting of one Rydberg atom and a number of neutral ground state atoms. The chemical binding properties and electronic wave functions of these exotic molecules are investigated analytically via hybridized diatomic states. The effects of the molecular geometry on the system's properties are studied through comparisons of the adiabatic potential curves and electronic structures for both symmetric and randomly configured molecular geometries. General properties of these molecules with increasing numbers of constituent atoms and in different geometries are presented. These polyatomic states have spectral signatures that lead to non-Lorentzian line-profiles.

Beams of helium atoms in Rydberg–Stark states with principal quantum number n = 48 and electric dipole moments of 4600 D have been decelerated from a mean initial longitudinal speed of 2000 m s⁻¹ to zero velocity in the laboratory-fixed frame-of-reference in the continuously moving electric traps of a transmission-line decelerator. In this process accelerations up to $-1.3times {10}^{7}$ m s⁻² were applied, and changes in kinetic energy of ${rm{Delta }}{E}_{mathrm{kin}}=1.3times {10}^{-20}$ J (${rm{Delta }}{E}_{mathrm{kin}}/e=83$ meV) per atom were achieved. Guided and decelerated atoms, and those confined in stationary electrostatic traps, were detected in situ by pulsed electric field ionisation. The results of numerical calculations of particle trajectories within the decelerator have been used to characterise the observed deceleration efficiencies, and aid in the interpretation of the experimental data.

Phase matching of circularly polarized high-order harmonics driven by counter-rotating bi-chromatic lasers was recently predicted theoretically and demonstrated experimentally. In that work, phase matching was analyzed by assuming that the total energy, spin angular momentum and linear momentum of the photons participating in the process are conserved. Here we propose a new perspective on phase matching of circularly polarized high harmonics. We derive an extended phase matching condition by requiring a new propagation matching condition between the classical vectorial bi-chromatic laser pump and harmonics fields. This allows us to include the influence of the laser pulse envelopes on phase matching. We find that the helicity dependent phase matching facilitates generation of high harmonics beams with a high degree of chirality. Indeed, we present an experimentally measured chiral spectrum that can support a train of attosecond pulses with a high degree of circular polarization. Moreover, while the degree of circularity of the most intense pulse approaches unity, all other pulses exhibit reduced circularity. This feature suggests the possibility of using a train of attosecond pulses as an isolated attosecond probe for chiral-sensitive experiments.

Attosecond science offers formidable tools for the investigation of electronic processes at the heart of important physical processes in atomic, molecular and solid-state physics. In the last 15 years impressive advances have been obtained from both the experimental and theoretical points of view. Attosecond pulses, in the form of isolated pulses or of trains of pulses, are now routinely available in various laboratories. In this review recent advances in attosecond science are reported and important applications are discussed. After a brief presentation of various techniques that can be employed for the generation and diagnosis of sub-femtosecond pulses, various applications are reported in atomic, molecular and condensed-matter physics.

We present a review of quantum computation with neutral atom qubits. After an overview of architectural options and approaches to preparing large qubit arrays we examine Rydberg mediated gate protocols and fidelity for two- and multi-qubit interactions. Quantum simulation and Rydberg dressing are alternatives to circuit based quantum computing for exploring many body quantum dynamics. We review the properties of the dressing interaction and provide a quantitative figure of merit for the complexity of the coherent dynamics that can be accessed with dressing. We conclude with a summary of the current status and an outlook for future progress.

In this review we will discuss the topic of high order harmonic generation (HHG) from samples of organic and bio-molecules. The possibility to extract useful dynamical and structural information from the measurement of the HHG emission, a technique termed high harmonic generation spectroscopy (HHGS), will be the special focus of our discussions. We will begin by introducing the salient facts of HHG from atoms and simple molecules and explaining the principles behind HHGS. Next the technical difficulties associated with HHG from samples of organic molecules and biomolecules, principally the low sample density and the low ionization potential, will be examined. Then we will present some recent experiments where HHG spectra from samples of these molecules have been measured and discuss what has been learned from these measurements. Finally we will look at the future prospects for HHG spectroscopy of organic molecules, discussing some of the technical and in principle limits of the technique and methods that may ameliorate these limits.

The subject of optomechanics involves interactions between optical and mechanical degrees of freedom, and is currently of great interest as an enabler of fundamental investigations in quantum mechanics, as well as a platform for ultrasensitive measurement devices. The majority of optomechanical configurations rely on the exchange of linear momentum between light and matter. We will begin this tutorial with a brief description of such systems. Subsequently, we will introduce optomechanical systems based on angular momentum exchange. In this context, optical fields carrying polarization and orbital angular momentum will be considered, while for the mechanics, torsional and free rotational motion will be of relevance. Our overall aims will be to supply basic analyses of some of the existing theoretical proposals, to provide functional descriptions of some of the experiments conducted thus far, and to consider some directions for future research. We hope this tutorial will be useful to both theorists and experimentalists interested in the subject.

In recent years intense mid-infrared lasers with wavelength of a few microns have become the standard tools for research in strong field physics laboratories worldwide. These lasers offer the opportunities to extend the traditional study of high-order harmonics generation and attosecond sciences from the extreme ultraviolet to soft x-rays. In this tutorial we revisit the familiar strong field approximation and its simplification—the quantum orbits theory. We draw special emphasis on the factorization of laser induced dipole moment as the product of a returning electron wave packet with the photo-recombination dipole transition matrix element. The former depends on the laser properties only (up to a normalization constant) while the latter is related to laser-free photoionization transition dipole. The factorization leads to the suggested modification beyond the strong field approximation—the quantitative rescattering theory. In applying these theories to mid-infrared lasers, we analyze the behavior of the returning electron wave packet and its scaling properties vs the wavelength of the laser. A few examples are given to demonstrate how the quantitative rescattering theory is capable of reproducing experimental harmonic spectra under various conditions. Future opportunities in employing harmonics generated by optimized mid-infrared lasers for probing molecular structure and for serving as useful table-top coherent light sources up to the x-ray region are also discussed.

A primer on the Floquet theory of periodically time-dependent quantum systems is provided, and it is shown how to apply this framework for computing the quasienergy band structure governing the dynamics of ultracold atoms in driven optical cosine lattices. Such systems are viewed here as spatially and temporally periodic structures living in an extended Hilbert space, giving rise to spatio-temporal Bloch waves whose dispersion relations can be manipulated at will by exploiting ac-Stark shifts and multiphoton resonances. The elements required for numerical calculations are introduced in a tutorial manner, and some example calculations are discussed in detail, thereby illustrating future prospects of Floquet engineering.