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We predict a near-threshold ("zero energy") peak in multi-photon ionization for a dynamical regime where the photon frequency is large compared to the binding energy of the electron. The peak position does not depend on the laser frequency, but on the binding energy and the pulse duration. The effect originates from the fact that bound-continuum dipole transitions are stronger than continuum-continuum ones. To clearly observe this zero-energy photoelectric effect, the spectral width of the laser pulse should be comparable to the binding energy of the ionized orbital, and the second ionization potential should be larger than the photon energy. This suggests negative ions as ideal candidates for corresponding experiments., Comment: 5 pages, 5 figures, 1 table

Tailored light-matter interactions in the strong coupling regime enable the manipulation and control of quantum systems with up to unit efficiency, with applications ranging from quantum information to photochemistry. While strong light-matter interactions are readily induced at the valence electron level using long-wavelength radiation, comparable phenomena have been only recently observed with short wavelengths, accessing highly-excited multi-electron and inner-shell electron states. However, the quantum control of strong-field processes at short wavelengths has not been possible, so far, due to the lack of pulse shaping technologies in the extreme ultraviolet (XUV) and X-ray domain. Here, exploiting pulse shaping of the seeded free-electron laser (FEL) FERMI, we demonstrate the strong-field quantum control of ultrafast Rabi dynamics in helium atoms with high fidelity. Our approach unravels a strong dressing of the ionization continuum, otherwise elusive to experimental observables. The latter is exploited to achieve control of the total ionization rate, with prospective applications in many XUV and soft X-ray experiments. Leveraging recent advances in intense few-femtosecond to attosecond XUV to soft X-ray light sources, our results open an avenue to the efficient manipulation and selective control of core electron processes and electron correlation phenomena in real time.

Science is and always has been based on data, but the terms "data-centric" and the "4th paradigm of" materials research indicate a radical change in how information is retrieved, handled and research is performed. It signifies a transformative shift towards managing vast data collections, digital repositories, and innovative data analytics methods. The integration of Artificial Intelligence (AI) and its subset Machine Learning (ML), has become pivotal in addressing all these challenges. This Roadmap on Data-Centric Materials Science explores fundamental concepts and methodologies, illustrating diverse applications in electronic-structure theory, soft matter theory, microstructure research, and experimental techniques like photoemission, atom probe tomography, and electron microscopy. While the roadmap delves into specific areas within the broad interdisciplinary field of materials science, the provided examples elucidate key concepts applicable to a wider range of topics. The discussed instances offer insights into addressing the multifaceted challenges encountered in contemporary materials research., Comment: Review, outlook, roadmap, perspective

Scattering properties and time delays for general (non-symmetric) potentials in terms of the respective S-matrices are discussed paradigmatically in one dimension and in comparison to symmetric potentials. Only for the latter the Wigner and Smith time delays coincide. Considering asymmetric potentials also reveals that only one version of S-matrices used in the literature (the one with reflection coefficients on the diagonal) generalizes to the asymmetric case. Finally, we give a criterion how to identify a potential with intrinsic symmetry which behaves like an asymmetric one if it is merely offset from the scattering center., Comment: 8 pages, 4 figures

We demonstrate that strong-field ionization of atoms driven by circularly polarized light becomes an adiabatic process when described in the frame rotating with the laser field. As a direct consequence, a conservation law emerges: in the rotating frame the energy of the tunneling electron is conserved for rotationally invariant potentials. This conservation law, arising from a classical picture, is retrieved through a proper classical-quantum correspondence when considering the full quantum system, beyond the Strong Field Approximation.

Preservation of coherence is a fundamental yet subtle phenomenon in open systems. We uncover its relation to symmetries respected by the system Hamiltonian and its coupling to the environment. We discriminate between local and global classes of decoherence-free subspaces for many-body systems through the introduction of "ghost variables". The latter are orthogonal to the symmetry and the coupling to the environment does not depend on them. Constructing them is facilitated in classical phase space and can be transferred to quantum mechanics through the equivalent role that Poisson and Lie algebras play for symmetries in classical and quantum mechanics, respectively. Examples are given for an interacting spin system.

Backscattering of delocalized electrons has been recently established [Phys. Rev. A 105, L041101 (2022)] as a mechanism to enhance high-order harmonic generation (HHG) in periodic systems with broken translational symmetry. Here we study this effect for a variable spatial gap in an atomic chain. Propagating the many-electron dynamics numerically, we find enhanced HHG and identify its origin in two mechanisms, depending on the gap size, either backscattering or enhanced tunneling from an impurity state. Since the gapped atomic chain exhibits both impurities and vacancies in a unified setting, it provides insight how periodicity breaks influence HHG in different scenarios., Comment: 11 pages, 9 figures, REVTeX 4.2

We identify and describe how intense short light pulses couple to massless Dirac fermions in two-dimensional systems. The ensuing excitation dynamics exhibits unusual scaling with the wavelength of the light due the linear dispersion of the band structure and the fact that light coupling is efficient only close to the Dirac points. We exploit these features to achieve valley polarization of more than 70 % with simple pulse shapes. Quantitative results are given for pristine graphene., Comment: 5 pages, 4 figures

Non-adiabatic photo-ionization is difficult to control as it relies on the derivatives of the envelope and not on phase-details of the short ionizing pulse. Here, we introduce a catalyzing state, whose presence render non-adiabatic ionization sensitive to phase-details of tailored pulses. Since a catalyzing state is in general easy to create, this opens a perspective for coherent control of ultra-fast ionization., Comment: 9 pages, 5 figures, 2 appendices

It is shown that electron backscattering can enhance high-harmonic generation in periodic systems with broken translational symmetry. Paradigmatically, we derive for a finite chain of atoms the harmonic cutoff due to electrons backscattered from the edges of the chain and demonstrate a maximum in the harmonic yield if twice the quiver amplitude of the driven electrons equals the chain length. For an intuitive understanding of our quantum results we develop a refined semiclassical trajectory model with finite electron-hole separation after tunneling. We demonstrate that the same "tunnel exit" also holds for interband harmonics in conventional periodic solid-state systems., Comment: 5 pages, 3 figures, REVTeX 4.2

We derive the semi-classical Lindblad master equation in phase space for both canonical and non-canonical Poisson brackets using the Wigner-Moyal formalism and the Moyal star-product. The semi-classical limit for canonical dynamical variables, i.e., canonical Poisson brackets, is the Fokker-Planck equation, as derived before. We generalize this limit and show that it holds also for non-canonical Poisson brackets. Examples are gyro-Poisson brackets, which occur in spin ensembles, systems of recent interest in atomic physics and quantum optics. We show that the equations of motion for the collective spin variables are given by the Bloch equations of nuclear magnetization with relaxation. The Bloch and relaxation vectors are expressed in terms of the microscopic operators: The Hamiltonian and the Lindblad functions in the Wigner-Moyal formalism.

We have constructed deep neural networks, which can map fluctuating photo-electron spectra obtained from noisy pulses to spectra from noise-free pulses. The network is trained on spectra from noisy pulses in combination with random Hamilton matrices, representing systems which could exist but do not necessarily exist. In [Giri et al., Phys. Rev. Lett. 124,113201 (2020)] we performed a purification of fluctuating spectra, that is mapping them to those from Fourier-limited Gaussian pulses. Here, we investigate the performance of such neural-network-based maps for predicting spectra of double pulses, pulses with a chirp and even partially-coherent pulses pulses from fluctuating spectra generated by noisy pulses. Secondly, we demonstrate that along with a purification of a fluctuating double-pulse spectrum, one can estimate the time-delay of the underlying double pulse, an attractive feature for single-shot spectra from SASE FELs. We demonstrate our approach with resonant two-photon ionization, a non-linear process, sensitive to details of the laser pulse., Comment: 10 pages, 9 figures

The generation of a streaking spectrogram is based on energy absorption from the streaking laser. Investigating this absorption we show rigorously under which condition the measured time shift is independent of properties of the streaking light. In this case it provides the Wigner-Smith time delay. The latter is infinite for systems with a long-range potential tail, such as Coulomb systems. Here, we suggest to determine the time delay relative to pure hydrogen for meaningful results. Finite delays obtained so far for Coulombic systems without the hydrogen reference are the consequence of a finite streaking frequency and depend on its value as well as on the electron's excess energy. Our analysis also suggests a time-delay measurement technique that avoids the record of a complete streaking scan., Comment: 5 pages, 5 figures

Photo-electron spectra obtained with intense pulses generated by free-electron lasers through self-amplified spontaneous emission are intrinsically noisy and vary from shot to shot. We extract the purified spectrum, corresponding to a Fourier-limited pulse, with the help of a deep neural network. It is trained on a huge number of spectra, which was made possible by an extremely efficient propagation of the Schr\"odinger equation with synthetic Hamilton matrices and random realizations of fluctuating pulses. We show that the trained network is sufficiently generic such that it can purify atomic or molecular spectra, dominated by resonant two- or three-photon ionization, non-linear processes which are particularly sensitive to pulse fluctuations. This is possible without training on those systems., Comment: 5 pages, 4 figures (application extended to a molecular system)

We demonstrate that by changing the direction of the chirp in VUV pulses one can switch between excitation and ionization with very high contrast, if the carrier frequency of the light is resonant with two bound states. This is a surprising consequence if rapid adiabatic passage is extended to include transitions to the continuum. The chirp phase locks the linear combination of two resonantly coupled bound states whose ionization amplitudes interfere constructively or destructively depending on the chirp direction under suitable conditions. We derive the phenomenon in a minimal model and verify the effect with calculations for helium as a realistic example., Comment: 5 pages, 5 figures

We demonstrate that ultrashort pulses carry the possibility for a new regime of light-matter interaction with nonadiabatic electron processes sensitive to the envelope-derivative of the light pulse. A standard single pulse with its two peaks in the derivative separated by the width of the pulse acts in this regime like a traditional double pulse. The two ensuing nonadiabatic ionization bursts have slightly different ionization amplitudes. This difference is due to redistribution of continuum electron energy during the bursts, negligible in standard photo-ionization. A time-dependent close- coupling approach based on cycle-averaged potentials in the Kramers-Henneberger reference frame permits a detailed understanding of light pulse derivative-driven electron dynamics., Comment: 5 pages, 5 figures

We present a two-timescale Floquet method that allows one to apply the Kramers-Henneberger approach to short pulses and arbitrary laser frequencies. An efficient numerical procedure to propagate the Floquet Hamiltonian is provided that relies on the Toeplitz matrix formalism and Fast Fourier Transformations. It enables efficient time propagation with large Floquet expansions, while still taking advantage of the cycle-averaged Kramers-Henneberger basis. Three illustrative cases of ionization with different photon energies are analyzed, where the envelope of a short and intense pulse is crucial to the underlying dynamics., Comment: 39 pages, 11 figures

We develop general quantitative criteria for dynamic interference, a manifestation of double-slit interference in time which should be realizable with brilliant state-of-the-art high-frequency laser sources. Our analysis reveals that the observation of dynamic interference hinges upon maximizing the difference between the dynamic polarization of the initial bound and the final continuum state of the electron during the light pulse, while keeping depletion of the initial state small. Confirmed by numerical results, we predict that this is impossible for the hydrogen ground-state but feasible with excited states explicitly exemplified with the hydrogen 2p-state., Comment: 5 pages, 3 figures

Non-adiabatic charge pumping through a single-level quantum dot with periodically modulated parameters is studied theoretically. By means of a quantum-master-equation approach the full counting statistics of the system is obtained. We find a trinomial-probability distribution of the charge transfer, which adequately describes the reversal of the pumping current by sweeping the driving frequency. Further, we derive equations of motion for current and noise, and solve those numerically for two different driving schemes. Both show interesting features which can be fully analyzed due to the simple and generic model studied., Comment: 7 pages, 4 figures

The dynamics of ultra-slow electrons in the combined potential of an ionic core and a static electric field is discussed. With state-of-the-art detection it is possible to create such electrons through strong intense-field photo-absorption and to detect them via high-resolution time-of-flight spectroscopy despite their very low kinetic energy. The characteristic feature of their momentum spectrum, which emerges at the same position for different laser orientations, is derived and could be revealed experimentally with an energy resolution of the order of 1meV., Comment: 5 pages, 5 figures

For ultrashort VUV pulses with a pulse length comparable to the orbital time of the bound electrons they couple to we propose a simplified envelope Hamiltonian. It is based on the Kramers-Henneberger representation in connection with a Floquet expansion of the strong-field dynamics but keeps the time dependence of the pulse envelope explicit. Thereby, the envelope Hamiltonian captures the essence of the physics, -- light-induced shifts of bound states, single-photon absorption, and non-adiabatic electronic transitions. It delivers quantitatively accurate ionization dynamics and allows for physical insight into the processes occurring. Its minimal requirements for construction in terms of laser parameters make it ideally suited for a large class of atomic and molecular problems., Comment: 5 pages, 3 figures

Intense X-ray photo-absorption from short and intense pulses by a molecule triggers complicated electron and subsequently ion dynamics leading to photo-electron spectra which are difficult to interpret. Illuminating fullerenes offers a way to separate out the electron dynamics. Moreover, the fullerene cage confines spatially the origin of photo and Auger electrons. Together with the sequential nature of the photo processes at intensities available at X-ray free electron lasers, this allows for a remarkably detailed interpretation of the photo-electron spectra as we will demonstrate. The general features derived can serve as a paradigm for less well-defined situations in other large molecules or clusters., Comment: 5 pages, 5 figures

Clusters consisting of small molecules containing hydrogen do eject fast protons when illuminated by short X-ray pulses. A suitable overall charging of the cluster controlled by the X-ray intensity induces electron migration from the surface to the bulk leading to efficient segregation of the protons and to a globally hindered explosion of the heavy atoms even outside the screened volume. We investigate this peculiar effect systematically along the iso-electronic sequence of methane over ammonia and water to the atomic limit of neon as a reference. In contrast to core-shell systems where the outer shell is sacrificed to reduce radiation damage, the intricate proton dynamics of hydride clusters allows one to keep the entire backbone of heavy atoms intact., Comment: 5 pages, 5 figures

We demonstrate that fast removal of many electrons uncovers initial correlations of atoms in a finite sample through a pronounced peak in the kinetic-energy spectrum of the exploding ions. This maximum is the result of an intricate interplay between the composition of the system from discrete particles and its boundary. The formation of the peak can be described analytically, allowing for correlations beyond a mean-field reference model. It can be experimentally detected with short and intense light pulses from 4th-generation light sources., Comment: 5 pages, 5 figures

The response of matter to an optical excitation consists essentially of absorption and emission. Traditional spectroscopy accesses the frequency-resolved and time-integrated response, while the temporal evolution stays concealed. However, we will demonstrate here that the temporal evolution of a virtual single-photon transition can be mapped out by a second pulsed electromagnetic field. The resulting optical signal shows previously unexpected optical gain and loss, which can be gated and controlled via the relative delay of the electromagnetic fields. The model presented here can be applied to any system that assumes a two-level character through near-resonant optical dipole excitation, whether they are of atomic, molecular or even solid-state nature. These theoretical observations are in excellent qualitative agreement with our transient absorption spectroscopy study in helium. The presented results can act as starting point for a new scheme for creating optical gain, which is a prerequisite for the operation of lasers. It may be possible to open the doors to spectral regions, which were difficult to access until now, e.g. in the extreme ultraviolet., Comment: 15 pages, 4 figures

Pumping of electrons through nano-scale devices is one of the fascinating achievements in the field of nano-science with a wide range of applications. To optimize the performance of pumps, operating them at high frequencies is mandatory. We consider the influence of fast periodic driving on the average charge transferred through a quantum dot. We show that it is possible to reverse the average current by sweeping the driving frequency only. In connection with this, we observe a rectification of the average current for high frequencies. Since both effects are very robust, as corroborated by analytical results for harmonic driving, they offer a new way of controlling electron pumps., Comment: 5 pages, 3 figures

Massively parallel ionization of many atoms in a cluster or bio-molecule is identified as new phenomenon of light-matter interaction which becomes feasible through short and intense FEL pulses. Almost simultaneously emitted from the illuminated target the photo-electrons can have such a high density that they interact substantially even after photo-ionization. This interaction results in a characteristic electron spectrum which can be interpreted as convolution of a mean-field electron dynamics and binary electron-electron collisions. We demonstrate that this universal spectrum can be obtained analytically by summing synthetic two-body Coulomb collision events. Moreover, we propose an experiment with hydrogen clusters to observe massively parallel ionization., Comment: 4 pages, 5 figures

We study non-adiabatic charge pumping through single-level quantum dots taking into account Coulomb interactions. We show how a truncated set of equations of motion can be propagated in time by means of an auxiliary-mode expansion. This formalism is capable of treating the time-dependent electronic transport for arbitrary driving parameters. We verify that the proposed method describes very precisely the well-known limit of adiabatic pumping through quantum dots without Coulomb interactions. As an example we discuss pumping driven by short voltage pulses for various interaction strengths. Such finite pulses are particular suited to investigate transient non-adiabatic effects, which may be also important for periodic drivings, where they are much more difficult to reveal., Comment: 11 pages, 4 figures

Soft recollisions are laser-driven distant collisions of an electron with its parent ion. Such collisions may cause an energy bunching, since electrons with different initial drift momenta can acquire impacts, which exactly counterbalance these differences. The bunching generates a series of peaks in the photo-electron spectrum. We will show that this series could be uncovered peak-by-peak experimentally by means of phase-stabilized few-cycle pulses with increasing duration., Comment: 8 pages, 3 figures

We introduce soft recollisions in laser-matter interaction. They are characterized by the electron missing the ion upon recollision in contrast to the well-known head-on collisions responsible for high-harmonic generation or above-threshold ionization. We demonstrate analytically that soft recollisions can cause a bunching of photo-electron energies through which a series of low-energy peaks emerges in the electron yield along the laser polarization axis. This peak sequence is universal, it does not depend on the binding potential, and is found below an excess energy of one fifth of the ponderomotive energy., Comment: 4 pages, 3 figures, 1 table

Time-resolved electron transport in nano-devices is described by means of a time-nonlocal quantum master equation for the reduced density operator. Our formulation allows for arbitrary time dependences of any device or contact parameter. The quantum master equation and the related expression for the electron current through the device are derived in fourth order of the coupling to the contacts. It is shown that a consistent sum up to infinite orders induces level broadening in the device. To facilitate a numerical propagation of the equations we propose to use auxiliary density operators. An expansion of the Fermi function in terms of a sum of simple poles leads to a set of equations of motion, which can be solved by standard methods. We demonstrate the viability of the proposed propagation scheme and consider electron transport through a double quantum dot., Comment: 15 pages, 4 figures

The coherent time evolution of electrons in double quantum dots induced by fast bias-voltage switches is studied theoretically. As it was shown experimentally, such driven double quantum dots are potential devices for controlled manipulation of charge qubits. By numerically solving a quantum master equation we obtain the energy- and time-resolved electron transfer through the device which resembles the measured data. The observed oscillations are found to depend on the level offset of the two dots during the manipulation and, most surprisingly, also the on initialization stage. By means of an analytical expression, obtained from a large-bias model, we can understand the prominent features of these oscillations seen in both the experimental data and the numerical results. These findings strengthen the common interpretation in terms of a coherent transfer of electrons between the dots., Comment: 18 pages, 4 figures

Intense light with frequencies above typical atomic or molecular ionization potentials as provided by free-electron lasers couples many photons into extended targets such as clusters and biomolecules. This implies, in contrast to traditional multi-photon ionization, multiple single-photon absorption. Thereby, many electrons are removed from their bound states and either released or trapped if the target charge has become sufficiently large. We develop a simple model for this photo activation to study electron migration and interaction. It satisfies scaling relations which help to relate quite different scenarios. To understand this type of multi-electron dynamics on very short time scales is vital for assessing the radiation damage inflicted by that type of radiation and to pave the way for coherent diffraction imaging of single molecules., Comment: 14 pages, 6 figures, 1 table

A closed set of coupled equations of motion for the description of time-dependent electron transport is derived. It provides the time evolution of energy-resolved quantities constructed from non-equilibrium Green functions. By means of an auxiliary-mode expansion a viable propagation scheme for finite temperatures is obtained, which allows to study arbitrary time dependences and structured reservoirs. Two illustrative examples are presented., Comment: 10 pages, 6 figures; v2: corrected some typos and replaced one duplicated graph

A partial fraction decomposition of the Fermi function resulting in a finite sum over simple poles is proposed. This allows for efficient calculations involving the Fermi function in various contexts of electronic structure or electron transport theories. The proposed decomposition converges in a well-defined region faster than exponential and is thus superior to the standard Matsubara expansion., Comment: 7 pages, 5 figures

A general scenario for electronic charge migration in finite samples illuminated by an intense laser pulse is given. Microscopic calculations for neon clusters under strong short pulses as produced by X-ray free-electron laser sources confirm this scenario and point to the prominent role of field ionization by strong internal fields. The latter leads to the fast formation of a core-shell system with an almost static core of screened ions while the outer shell explodes. Substituting the shell ions with a different material such as helium as a sacrificial layer leads to a substantial improvement of the diffraction image for the embedded cluster thus reducing the consequences of radiation damage for coherent diffractive imaging., Comment: 5 pages, 4 figures

Doping a helium nanodroplet with a tiny xenon cluster of a few atoms only, sparks complete ionization of the droplet at laser intensities below the ionization threshold of helium atoms. As a result, the intrinsically inert and transparent droplet turns into a fast and strong absorber of infrared light. Microscopic calculations reveal a two-step mechanism to be responsible for the dramatic change: Avalanche-like ionization of the helium atoms on a femtosecond time scale, driven by field ionization due to the quickly charged xenon core is followed by resonant absorption enabled by an unusual cigar-shaped nanoplasma within the droplet., Comment: 4 pages, 4 figures

Laser-driven rescattering of electrons is the basis of many strong-field phenomena in atoms and molecules. Here, we will show how this mechanism operates in extended atomic systems, giving rise to effective energy absorption. Rescattering from extended systems can also lead to energy loss, which in its extreme form results in non-linear photo-association. Intense-laser interaction with atomic clusters is discussed as an example. We explain fast electron emission, seen in experimental and numerically obtained spectra, by rescattering of electrons at the highly charged cluster., Comment: 4 pages, 3 figures, 1 table

Energy absorption of xenon clusters embedded in helium nanodroplets from strong femtosecond laser pulses is studied theoretically. Compared to pure clusters we find earlier and more efficient energy absorption in agreement with experiments. This effect is due to resonant absorption of the helium nanoplasma whose formation is catalyzed by the xenon core. For very short double pulses with variable delay both plasma resonances, due to the helium shell and the xenon core, are identified and the experimental conditions are given which should allow for a simultaneous observation of both of them., Comment: 4 pages, 4 figures

It is shown that the energy absorption of a rare-gas cluster from a vacuum-ultraviolet (VUV) pulse can be traced with time-delayed extreme-ultraviolet (XUV) attosecond probe pulses by measuring the kinetic energy of the electrons detached by the probe pulse. By means of this scheme we demonstrate, that for pump pulses as short as one femtosecond, the charging of the cluster proceeds during the formation of an electronic nano-plasma inside the cluster. Using moderate harmonics for the VUV and high harmonics for the XUV pulse from the same near-infrared laser source, this scheme with well defined time delays between pump and probe pulses should be experimentally realizable. Going to even shorter pulse durations we predict that pump and probe pulses of about 250 attoseconds can induce and monitor non-equilibrium dynamics of the nano-plasma., Comment: 10 pages, 5 figures

We study the electron transport properties through a supported organic molecule styrene (C8H8) on an ideal silicon surface Si[111] and probed by a STM-tip. The I-V characteristics and the differential conductance of the molecule are calculated using a self consistent approach based on non equilibrium Green's functions. Two different adsorption configurations for the molecule on the surface were considered which corresponds to a global and a local minimum of the total energy. In both cases we find a negative differential resistance (NDR) in a given interval of bias voltages. This effect is controlled by the states available close to the Fermi level of the surface and can be manipulated by properly doping the substrate. We also analyze the influence of the tip-shape on the I-V characteristics., Comment: 20 pages, 13 figures

Attosecond laser pulses open the door to resolve microscopic electron dynamics in time. Experiments performed include the decay of a core hole, the time-resolved measurement of photo ionization and electron tunneling. The processes investigated share the coherent character of the dynamics involving very few, ideally one active electron. Here, we introduce a scheme to probe dissipative multi-electron motion in time. In this context attosecond probing enables one to obtain information which is lost at later times and cannot be retrieved by conventional methods in the energy domain due to the incoherent nature of the dynamics. As a specific example we will discuss the charging of a rare-gas cluster during a strong femtosecond pulse with attosecond pulses. The example illustrates the proposed use of attosecond pulses and suggests an experimental resolution of a controversy about the mechanism of energy absorption by rare-gas clusters in strong vacuum-ultraviolet (VUV) pulses., Comment: 4 pages, 3 figures

The quantum-classical hybrid-description of rare-gas clusters interacting with intense light pulses which we have developed is described in detail. Much emphasis is put on the treatment of screening electrons in the cluster which set the time scale for the evolution of the system and form the link between electrons strongly bound to ions and quasi-free plasma electrons in the cluster. As an example we discuss the dynamics of an Ar147 cluster exposed to a short VUV laser pulse of 20eV photon energy., Comment: 8 pages, 9 figures

Low-temperature scanning tunneling spectroscopy allows to probe the electronic properties of clusters at surfaces with unprecedented accuracy. By means of quantum transport theory, using realistic tunneling tips, we obtain conductance curves which considerably deviate from the cluster's density of states. Our study explains the remarkably small number of peaks in the conductance spectra observed in recent experiments. We demonstrate that the unambiguous characterization of the states on the supported clusters can be achieved with energy-resolved images, obtained from a theoretical analysis which mimics the experimental imaging procedure., Comment: 5 pages, 3 figures

We present a detailed theoretical study of scanning tunneling imaging and spectroscopy of \Csixty on silver and gold surfaces, motivated by the recent experiments and discussion by X. Lu et al. [PRL \textbf{90}, 096802 (2003) and PRB \textbf{70}, 115418 (2004)]. The surface/sample/tip system is described within a self--consistent DFT based tight--binding model. The topographic and conductance images are computed at constant current from a full self--consistent transport theory based on nonequilibrium Green's functions and compared with those simulated from the local density of states. The molecular orbitals of \Csixty are clearly identified in the energy resolved maps, in close correspondence with the experimental results. We show how the tip structure and orientation can affect the images. In particular, we consider the effects of truncated tips on the energy resolved maps., Comment: 9 pages, 8 figures

We analyze the dynamics of up to $10^5$ electrons resulting from illuminating a Xenon cluster with 9093 atoms with intense laser pulses of different length and peak intensity. Interesting details of electron motion are identified which can be probed with a time resolution of 100 attoseconds. Corresponding experiments would shed light on unexplored territory in complex electronic systems such as clusters and they would also permit to critically access the present theoretical description of this dynamics., Comment: 6 pages, 4 figures

The motion of electrons and ions in medium-sized rare gas clusters (1000 atoms) exposed to intense laser pulses is studied microscopically by means of classical molecular dynamics using a hierarchical tree code. Pulse parameters for optimum ionization are found to be wavelength dependent. This resonant behavior is traced back to a collective electron oscillation inside the charged cluster. It is shown that this dynamics can be well described by a driven and damped harmonic oscillator allowing for a clear discrimination against other energy absorption mechanisms., Comment: 4 pages (4 figures)

The effect of intense X-ray laser interaction on argon clusters is studied theoretically with a mixed quantum/classical approach. In comparison to a single atom we find that ionization of the cluster is suppressed, which is in striking contrast to the observed behavior of rare-gas clusters in intense optical laser pulses. We have identified two effects responsible for this phenomenon: A high space charge of the cluster in combination with a small quiver amplitude and delocalization of electrons in the cluster. We elucidate their impact for different field strengths and cluster sizes., Comment: 4 pages, 4 figures