arXiv subjects
Publications and source records attributed to Jan M. Rost.
A Rydberg and a ground-state atom can form ultralong range diatomic molecules provided the interaction between the ground-state atom and the Rydberg electron is attractive [C. H. Greene, et al., Phys. Rev. Lett. 85, 2458 (2000)]. A repulsive interaction does not support bound states. However, as we will show, adding a second ground-state atom, a bound triatomic molecule becomes possible constituting a Borromean Rydberg system.
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.
We investigate the dynamics of diatomic molecules subjected to both a femtosecond mid-infrared laser pulse and Gaussian white noise. The stochastic Schrödinger equation with a Morse potential is used to describe the molecular vibrations under noise and the laser pulse. For weak laser intensity, well below the dissociation threshold, it is shown that one can find an optimum amount of noise that leads to a dramatic enhancement of the dissociation probability. The enhancement landscape which is shown as a function of both the noise and the laser strength, exhibits a global maximum. A frequency-resolved gain profile is recorded with a pump-probe set-up which is experimentally realizable. With this profile we identify the linear and nonlinear multiphoton processes created by the interplay between laser and noise and assess their relative contribution to the dissociation enhancement.
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.
We show that ionization and dissociation can be influenced separately in a molecule with appropriate external noise. Specifically we investigate the hydrogen molecular ion under a stochastic force quantum mechanically beyond the Born-Oppenheimer approximation. We find that up to 30% of dissociation without ionization can be achieved by suitably tuning the forcing parameters.
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.
We investigate the effect of incoherent perturbations on atomic photoionization due to a femtosecond mid-infrared laser pulse by solving the time-dependent stochastic Schrödinger equation. For a weak laser pulse which causes almost no ionization, an addition of a Gaussian white noise to the pulse leads to a significantly enhanced ionization probability. Tuning the noise level, a stochastic resonance-like curve is observed showing the existence of an optimum noise for a given laser pulse. Besides studying the sensitivity of the obtained enhancement curve on the pulse parameters, such as the pulse duration and peak amplitude, we suggest that experimentally realizable broadband chaotic light can also be used instead of the white noise to observe similar features. The underlying enhancement mechanism is analyzed in the frequency-domain by computing a frequency-resolved atomic gain profile, as well as in the time-domain by controlling the relative delay between the action of the laser pulse and noise.
We develop a theoretical approach for the dynamics of Rydberg excitations in ultracold gases, with a realistically large number of atoms. We rely on the reduction of the single-atom Bloch equations to rate equations, which is possible under various experimentally relevant conditions. Here, we explicitly refer to a two-step excitation-scheme. We discuss the conditions under which our approach is valid by comparing the results with the solution of the exact quantum master equation for two interacting atoms. Concerning the emergence of an excitation blockade in a Rydberg gas, our results are in qualitative agreement with experiment. Possible sources of quantitative discrepancy are carefully examined. Based on the two-step excitation scheme, we predict the occurrence of an antiblockade effect and propose possible ways to detect this excitation enhancement experimentally in an optical lattice as well as in the gas phase.
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.
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.
Just as a coherent state may be considered as a quantum point, its restriction to a factor space of the full Hilbert space can be interpreted as a quantum plane. The overlap of such a factor coherent state with a full pure state is akin to a quantum section. It defines a reduced pure state in the cofactor Hilbert space. The collection of all the Wigner functions corresponding to a full set of parallel quantum sections defines the Husimi-Wigner reresentation. It occupies an intermediate ground between drastic suppression of nonclassical features, characteristic of Husimi functions, and the daunting complexity of higher dimensional Wigner functions. After analysing these features for simpler states, we exploit this new representation as a probe of numerically computed eigenstates of chaotic Hamiltonians. The individual two-dimensional Wigner functions resemble those of semiclassically quantized states, but the regular ring pattern is broken by dislocations.
We investigate properties of ultralong-range polyatomic molecules formed with a Rb Rydberg atom and several ground-state atoms whose distance from the Rydberg atom is of the order of n^2a_0, where n is the principle quantum number of the Rydberg electron. In particular, we put emphasis on the splitting of the energy levels, and elucidate the nature of the splitting via the construction of symmetry-adapted orbitals.
The effect of noise on the nonlinear photoionization of an atom due to a femtosecond pulse is investigated in the framework of the stochastic Schrödinger equation. A modest amount of white noise results in an enhancement of the net ionization yield by several orders of magnitude, giving rise to a form of quantum stochastic resonance. We demonstrate that this effect is preserved if the white noise is replaced by broadband chaotic light.
It is shown that the two-step excitation scheme typically used to create an ultracold Rydberg gas can be described with an effective two-level rate equation, greatly reducing the complexity of the optical Bloch equations. This allows us to solve the many-body problem of interacting cold atoms with a Monte Carlo technique. Our results reproduce the Rydberg blockade effect. However, we demonstrate that an Autler-Townes double peak structure in the two-step excitation scheme, which occurs for moderate pulse lengths as used in the experiment, can give rise to an antiblockade effect. It is observable in a lattice gas with regularly spaced atoms. Since the antiblockade effect is robust against a large number of lattice defects it should be experimentally realizable with an optical lattice created by CO$_{2}$ lasers.
Formulating a quasiclassical approach we determine the cross section for the complete four-body break-up of the lithium ground state following single photon absorption from threshold up to 220 eV excess energy. In addition, we develop a new classification scheme for three-electron ionizing trajectories in terms of electron-electron collisions, thereby identifying two main ionization paths which the three electrons in the ground state of lithium follow to escape to the continuum. The dominant escape paths manifest themselves in a characteristic ``T-shape'' break-up pattern of the three electrons which implies observable structures in the electronic angular correlation probability. This break-up pattern prevails for excess energies so low that the Wannier threshold law $σ\propto E^α$ describes already the triple ionization cross section, whose predicted value $α=2.16$ we can confirm quantitatively.
Solving the full classical four-body Coulomb problem numerically using a Wigner initial distribution we formulate a classical-quantum hybrid approach to study triple ionization by single photon absorption from the Li ground state in the threshold region. We confirm the Wannier threshold law $σ\propto E^α$ and we show that the $α$ determined in the interval between 2-5 eV deviates from the analytical threshold value of 2.16 which we find in the interval between $0.1-2$ eV.
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.
In this paper we study the response in time of N$_2$, O$_2$ and F$_2$ to laser pulses having a wavelength of 390nm. We find single ionization suppression in O$_2$ and its absence in F$_2$, in accordance with experimental results at $λ= 800$nm. Within our framework of time-dependent density functional theory we are able to explain deviations from the predictions of Intense-Field Many-Body $S$-Matrix Theory (IMST). We confirm the connection of ionization suppression with destructive interference of outgoing electron waves from the ionized electron orbital. However, the prediction of ionization suppression, justified within the IMST approach through the symmetry of the highest occupied molecular orbital (HOMO), is not reliable since it turns out that, e.g. in the case of F$_2$, the electronic response to the laser pulse is rather complicated and does not lead to dominant depletion of the HOMO. Therefore, the symmetry of the HOMO is not sufficient to predict ionization suppression. However, at least for F$_2$, the symmetry of the dominantly ionized orbital is consistent with the non-suppression of ionization.