Non-Markovian relaxation in an open quantum system

Non-Markovian dynamics in open quantum systems is characterized by a time-non-locality in the equation of motion valid for the reduced density operator. An expansion of this density matrix equation with respect to Laguerre polynomials is used to tackle the time-non-locality. The applicability and the numerical limitations of the method are discussed in detail. In order to illuminate the characteristics of non-Markovian dynamics the reference example is studied of a single quantum degree of freedom moving in a harmonic potential and being embedded in a heat bath. If interpreted as the photoinduced dynamics of nuclear motion in polyatomic molecules we can suggest two clear signatures of non-Markovian dynamics observable in ultrafast optical experiments, firstly a pronounced and somewhat irregular oscillatory behavior of the vibrational level populations, and secondly a separation of the vibrational wavepacket into a double-structure. Received 12 April 2000 and Received in final form 2 September 2000     

Magnetic Thomas-Fermi-Weizsäcker model for quantum dots: A comparison with Kohn-Sham ground states

The magnetic extension of the Thomas-Fermi-Weizs?cker kinetic energy is used within density-functional-theory to numerically obtain the ground state densities and energies of two-dimensional quantum dots. The results are thoroughly compared with the microscopic Kohn-Sham ones in order to assess the validity of the semiclassical method. Circular as well as deformed systems are considered. Received 26 October 2000 and Received in final form 14 December 2000     

Collective oscillations in quantum rings: A broken symmetry case

We present calculations within density functional theory of the ground state and collective electronic oscillations in small two-dimensional quantum rings. No spatial symmetries are imposed to the solutions and, as in a recent contribution, a transition to a broken symmetry solution in the intrinsic reference frame for an increasingly narrow ring is found. The oscillations are addressed by using real-time simulation. Conspicuous effects of the broken symmetry solution on the spectra are pointed out. Received 6 April 2000 and Received in final form 9 June 2000     

Theoretical investigation of the ultrafast NeNePo spectroscopy of Au 4 and Ag 4 Clusters

Ultrafast ground state nuclear dynamics of Au₄ and Ag₄ is theoretically explored in the framework of negative ion - to neutral - to positive ion (NeNePo) pump-probe spectroscopy based on the ab initio Wigner distribution approach. This involves the preparation of a nonequilibrium neutral ensemble by pump induced photodetachment of a thermal anionic ground state distribution, gradient corrected DFT classical trajectory simulations “on the fly” on the neutral ground state, and detection of the relaxation process of the ensemble in the cationic ground state by a time-delayed probe pulse. In Au₄, the initially prepared linear structure is close to a local minimum of the neutral state giving rise to characteristic vibrations in the signals for probe wavelength near the initial Franck-Condon transition. A timescale of ∼1 ps for the structural relaxation towards the stable rhombic D_2h neutral isomer was determined by the increase of the signal for probe wavelength in vicinity of the vertical ionization energy of the rhombic structure. In contrast, the relaxation dynamics in Ag₄ is characterized by normal mode vibrations since both the initially prepared anionic ground state and the neutral ground state have rhombic minimum geometries. Thus, time-resolved oscillations of pump-probe signals are fingerprints of structural behaviour which can be used experimentally for the identification of particular isomers in the framework of NeNePo spectroscopy. Received 22 December 2000     

Local field corrections for light absorption by fullerenes

Semi-empirical atom-atom potential energy calculations based on pairwise additive interactions are performed and, after applying the Born-Oppenheimer approximation to separate high frequency vibrational modes from low frequency orientational and translational modes, the infrared vibrational spectra of CO₂ and N₂O monomers trapped in an argon matrix at a temperature of 5 K are determined. It is shown that only a double substitutional site in argon can accommodate N₂O, whereas CO₂ is trapped in two distinct sites, of single and double substitutional types. The model shows that splitting of the degenerate mode occurs for both molecules in the double site. In the ground electronic state, the vibrational frequency shifts due to the matrix and the vibrational transition moments for low-lying levels are determined using the contact transformation method, as used for gas phase calculations. Calculated energy levels compare well with observed ones and the theory also predicts some unobserved levels. Moreover, calculations show no significant changes in the dipole moments of both CO₂ and N₂O trapped molecules. Received 22 March 2000 and Received in final form 10 May 2000     

Theoretical exploration of ultrafast spectroscopy of small clusters

We present the ultrafast multistate nuclear dynamics involving adiabatic and nonadiabatic excited states of non-stoichiometric halide deficient clusters (Na_nF_n-1) characterized by strong ionic bonding and one-excess electron for which the “frozen ionic bonds” approximation has been justified allowing to consider the optical response of the single excess electron in the effective field of the other electrons. We combined the Wigner-Moyal representation of the vibronic density matrix with the ab initio multi state molecular dynamics in the ground and excited electronic states including the nonadiabatic couplings calculated “on the fly” at low computational demand. This method allows the simulation of femtosecond pump-probe and pump-dump signals based on an analytical formulation, which utilizes temperature dependent ground state initial conditions, an ensemble of trajectories carried out on the electronic excited state as well as on the ground state after the passage through the conical intersection in the case of nonadiabatic dynamics and for probing either in the cationic state or in the ground state. The choice of the systems we presented has been made in order to determine the timescales of the fast geometric relaxation leaving the bonding frame intact as during the dynamics in the first excited state of Na₄F₃, and of the bond breaking processes leading to conical intersection between the first excited state and the ground state as in Na₃F₂. The former is the smallest finite system prototype for an surface F-center of bulk color centers. The latter allows to study the photo isomerization in full complexity taking into account all degrees of freedom. In the case of Na₄F₃ after the fast geometric relaxation in the excited state leading to deformed cuboidal structure without breaking of bonds, different types of internal vibrational redistribution (IVR) processes have been identified in pump-dump signals by tuning the dump laser. In contrast, from the analysis of the pump-probe signals of Na₃F₂ cluster, the timescales for the metallic and the ionic bond breaking, as well as for the passage through conical intersection have been determined. Finally the conditions under which these processes can be experimentally observed have been identified. Received 22 December 2000     

Ground state phase diagram of a spin-2 antiferromagnet on the square lattice

We use the vertex state model approach to construct optimum ground states for a large class of quantum spin-2 antiferromagnets on the square lattice. Optimum ground states are exact ground states of the model which minimize all local interaction operators. The ground state contains two continuous parameters and exhibits a second order phase transition from a disordered phase with exponentially decaying correlation functions to a Néel ordered phase. The behaviour is very similar to that of the corresponding ground state of a quantum spin-3/2 model on the hexagonal lattice, which has been investigated in an earlier paper. Received 8 April 1999     

Radiative lifetimes of 7d, 8d <Superscript>1</Superscript>D<Subscript>2</Subscript> excited states of Hg I

Radiative lifetimes of 7d, 8d ¹ D ₂ excited states of Hg I are measured using pulsed two-photon excitation from the ground [Xe]5d ¹⁰6s ^{2 1} S ₀ mercury state, detecting the decay of the laser-induced fluorescence. The results are compared with theoretical values, obtained by means of a Hartree-Fock single configuration method, taking into account electron configuration interaction. The radiative lifetime value dependence on the effective principal quantum number for the nd ¹ D ₂ series is analyzed and compared with the quantum defect dependence. Received 25 February 2000 and Received in final form 26 July 2000     

Plaquette ground state in the two-dimensional SU(4) spin-orbital model

In order to understand the properties of Mott insulators with strong ground state orbital fluctuations, we study the zero temperature properties of the SU(4) spin-orbital model on a square lattice. Exact diagonalizations of finite clusters suggest that the ground state is disordered with a singlet-multiplet gap and possibly low-lying SU(4) singlets in the gap. An interpretation in terms of plaquette SU(4) singlets is proposed. The implications for LiNiO₂ are discussed. Received 6 July 2000     

Quantum decoherence from adiabatic entanglement with external one or a few degrees of freedom

Based on the Born-Oppenhemer approximation, the concept of adiabatic quantum entanglement is introduced to account for quantum decoherence of a quantum system due to its interaction with a large system of one or a few degrees of freedom. In the adiabatic limit, it is shown that the wave function of the total system formed by the quantum system plus the large system can be factorized as an entangled state with correlation between adiabatic quantum states and quasi-classical motion configurations of the large system. In association with a novel viewpoint about quantum measurement, which has been directly verified by most recent experiments [e.g., S. Durr et al., Nature 33, 359 (1998)], it is shown that the adiabatic entanglement is indeed responsible for the quantum decoherence and thus can be regarded as a “clean” quantum measurement when the large system behaves as a classical object. By taking the large system respectively to be a macroscopically distinguishable spatial variable, a high spin system and a harmonic oscillator with a coherent initial state, three illustrations are presented with their explicit solutions in this paper. Received 26 February 2000 and Received in final form 14 July 2000     

Ultrafast multidimensional dynamics of strong hydrogen bonds

The laser driven dynamics of the OH(D) stretching vibration in phthalic acid monomethylester is investigated. The combination of a 55-dimensional all-Cartesian reaction surface Hamiltonian and the time-dependent self-consistent field approach is shown to provide a microscopic picture of intramolecular vibrational energy redistribution taking place upon interaction with an external laser field. Choosing suitable zeroth-order vibrational states and combinations thereof a quasi-periodic in-phase and out-of-phase oscillatory behavior is observed manifesting energy flow on different time scales. The fingerprints of this behavior in transient absorption spectroscopy are also discussed. Received 24 August 2000 and Received in final form 11 October 2000     

Coulomb repulsion versus Hubbard repulsion in a disordered chain

We study the difference between on site Hubbard and long range Coulomb repulsions for two interacting particles in a disordered chain. The system size L (in units of the lattice spacing) is of the order of the one particle localization length and the energies are taken near the band center. In the two cases, the limits of weak and strong interactions are characterized by uncorrelated energy levels and are separated by a crossover regime where the states are more extended and the spectra more rigid. U denoting the interaction strength and t the kinetic energy scale, the crossovers take place for interaction energy to kinetic energy ratios U/t and U/(2tL) of order one, for Hubbard and Coulomb repulsions respectively. While Hubbard repulsion can only yield weak critical chaos with intermediate spectral statistics, Coulomb repulsion can drive the two particle system to quantum chaos with Wigner-Dyson spectral statistics. The interaction matrix elements are studied to explain this difference. Received 21 March 2000 and Received in final form 5 February 2001     

Laser cooling with electromagnetically induced transparency: application to trapped samples of ions or neutral atoms

A novel method of ground-state laser cooling of trapped atoms utilizes the absorption profile of a three- (or multi-) level system that is tailored by a quantum interference. With cooling rates comparable to conventional sideband cooling, lower final temperatures may be achieved. The method was experimentally implemented to cool a single Ca⁺ ion to its vibrational ground state. Since a broad band of vibrational frequencies can be cooled simultaneously, the technique will be particularly useful for the cooling of larger ion strings, thereby being of great practical importance for initializing a quantum register based on trapped ions. We also discuss its application to different level schemes and for ground-state cooling of neutral atoms trapped by a far-detuned standing wave laser field. Received: 10 July 2001 / Published online: 23 November 2001     

Time-evolution of cascade processes of muonic atoms in hydrogen-helium mixtures

The time-dependence of the population of muonic hydrogen states in hydrogen-helium mixtures is calculated for principal quantum number n. The number of muons transferred to helium nuclei is also determined. The dependence of the population of the ground state of muonic hydrogen on time and target density and the helium concentration is also considered. The results are in agreement with recent experimental data. The comparison of the calculated yield of K lines of X-ray in pure hydrogen and deuterium with experimental data indicates the essential role of the Coulomb deexcitation process. Possible Stark mixing is also analysed. Received 17 February 1999 and Received in final form 9 June 1999     

Multiple-beam Ramsey interference and quantum decoherence

We study the effect of photon scattering from a path of a four-beam atomic interference setup, which is based on a cesium atomic beam and two subsequent optical Ramsey pulses projecting the atoms onto a multilevel dark state. While in two-beam interference, any attempt to keep track of an interfering path reduces the fringe contrast, we demonstrate that photon scattering in a multiple-path arrangement cannot only lead to a decrease, but - under certain conditions - also to an increase of the interference contrast. The results are confirmed by a density-matrix calculation. We are aware that in all cases the “which-path” information carried away by the scattered photons leads to a loss of information that is contained in the atomic quantum state. An approach to quantify this “which-path” information using observed fringe signals is presented; it allows for an appropriate measure of quantum decoherence in multiple-path interference. Received: 27 July 2000 / Published online: 6 December 2000     

Delocalization effects and charge reorganizations induced by repulsive interactions in strongly disordered chains

We study the delocalization effect of a short-range repulsive interaction on the ground state of a finite density of spinless fermions in strongly disordered one dimensional lattices. The density matrix renormalization group method is used to explore the charge density and the sensitivity of the ground state energy with respect to the boundary condition (the persistent current) for a wide range of parameters (carrier density, interaction and disorder). Analytical approaches are developed and allow to understand some mechanisms and limiting conditions. For weak interaction strength, one has a Fermi glass of Anderson localized states, while in the opposite limit of strong interaction, one has a correlated array of charges (Mott insulator). In the two cases, the system is strongly insulating and the ground state energy is essentially invariant under a twist of the boundary conditions. Reducing the interaction strength from large to intermediate values, the quantum melting of the solid array gives rise to a more homogeneous distribution of charges, and the ground state energy changes when the boundary conditions are twisted. In individual chains, this melting occurs by abrupt steps located at sample-dependent values of the interaction where an (avoided) level crossing between the ground state and the first excitation can be observed. Important charge reorganizations take place at the avoided crossings and the persistent currents are strongly enhanced around the corresponding interaction value. These large delocalization effects become smeared and reduced after ensemble averaging. They mainly characterize half filling and strong disorder, but they persist away of this optimal condition. Received 5 July 2000 and Received in final form 8 November 2000