Switching Exciton Pulses Through Conical Intersections

Exciton pulses transport excitation and entanglement adiabatically through Rydberg aggregates, assemblies of highly excited light atoms, which are set into directed motion by resonant dipole-dipole interaction. Here, we demonstrate the coherent splitting of such pulses as well as the spatial segregation of electronic excitation and atomic motion. Both mechanisms exploit local nonadiabatic effects at a conical intersection, turning them from a decoherence source into an asset. The intersection provides a sensitive knob controlling the propagation direction and coherence properties of exciton pulses. The fundamental ideas discussed here have general implications for excitons on a dynamic network.Comment: Letter with 4 pages and 4 figures. Supplemental material with 4 pages and 4 figure

Approaches and tools to manipulate the carbonate chemistry

Although the chemistry of ocean acidifi cation is very well understood (see chapter 1), its impact on marine organisms and ecosystems remains poorly known. The biological response to ocean acidifi cation is a recent field of research, the fi rst purposeful experiments have only been carried out as late as the 1980s (Agegian, 1985) and most were not performed until the late 1990s. The potentially dire consequences of ocean acidifi cation have attracted the interest of scientists and students with a limited knowledge of the carbonate chemistry and its experimental manipulation. Perturbation experiments are one of the key approaches used to investigate the biological response to elevated p(CO2). Such experiments are based on measurements of physiological or metabolic processes in organisms and communities exposed to seawater with normal and altered carbonate chemistry. The basics of the carbonate chemistry must be understood to perform meaningful CO2 perturbation experiments (see chapter 1). Briefl y, the marine carbonate system considers € CO2 ∗(aq) [the sum of CO2 and H2CO3], € HCO3 −, € CO3 2−, H+, € OH− , and several weak acid-base systems of which borate-boric acid (€ B(OH)4 − , B(OH)3) is the most important. As discussed by Dickson (chapter 1), if two components of the carbonate chemistry are known, all the other components can be calculated for seawater with typical nutrient concentrations at given temperature, salinity, and pressure. One of the possible pairs is of particular interest because both components can be measured with precision, accuracy, and are conservative in the sense that their concentrations do not change with temperature or pressure. Dissolved inorganic carbon (DIC) is the sum of all dissolved inorganic carbon species while total alkalinity (AT) equals € [HCO3 − ] + 2 € [CO3 2− ] + € [B(OH)4 − ] + € [OH− ] - [H+] + minor components, and refl ects the excess of proton acceptors over proton donors with respect to a zero level of protons (see chapter 1 for a detailed defi nition). AT is determined by the titration of seawater with a strong acid and thus can also be regarded as a measure of the buffering capacity. Any changes in any single component of the carbonate system will lead to changes in several, if not all, other components. In other words, it is not possible to vary a single component of the carbonate system while keeping all other components constant. This interdependency in the carbonate system is important to consider when performing CO2 perturbation experiments. To adjust seawater to different p(CO2) levels, the carbonate system can be manipulated in various ways that usually involve changes in AT or DIC. The goal of this chapter is (1) to examine the benefi ts and drawbacks of various manipulation methods used to date and (2) to provide a simple software package to assist the design of perturbation experiments

Dynamics of photo-activated Coulomb complexes

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 tabl

Magnetotransport in Sr3PbO antiperovskite with three-dimensional massive Dirac electrons

Novel topological phenomena are anticipated for three-dimensional (3D) Dirac electrons. The magnetotransport properties of cubic ${\rm Sr_{3}PbO}$ antiperovskite, theoretically proposed to be a 3D massive Dirac electron system, are studied. The measurements of Shubnikov-de Haas oscillations and Hall resistivity indicate the presence of a low density ($\sim 1 \times 10^{18}$ ${\rm cm^{-3}}$) of holes with an extremely small cyclotron mass of 0.01-0.06$m_{e}$. The magnetoresistance $\Delta\rho_{xx}(B)$ is linear in magnetic field $B$ with the magnitude independent of temperature. These results are fully consistent with the presence of 3D massive Dirac electrons in ${\rm Sr_{3}PbO}$. The chemical flexibility of the antiperovskites and our findings in the family member, ${\rm Sr_{3}PbO}$, point to their potential as a model system in which to explore exotic topological phases

Multiple ionization of neon by soft X-rays at ultrahigh intensity

At the free-electron laser FLASH, multiple ionization of neon atoms was quantitatively investigated at 93.0 eV and 90.5 eV photon energy. For ion charge states up to 6+, we compare the respective absolute photoionization yields with results from a minimal model and an elaborate description. Both approaches are based on rate equations and take into acccout a Gaussian spatial intensity distribution of the laser beam. From the comparison we conclude, that photoionization up to a charge of 5+ can be described by the minimal model. For higher charges, the experimental ionization yields systematically exceed the elaborate rate based prediction.Comment: 10 pages, 3 figure

Comment on: `Pipe Network Model for Scaling of Dynamic Interfaces in Porous Media'

We argue that a proposed exponent identity [Phys. Rev. Lett 85, 1238 (2000)] for interface roughening in spontaneous imbibition is wrong. It rests on the assumption that the fluctuations are controlled by a single time scale, but liquid conservation imposes two distinct time scales.Comment: 1 page, to appear in Phys. Rev. Let

Inelastic semiclassical Coulomb scattering

We present a semiclassical S-matrix study of inelastic collinear electron-hydrogen scattering. A simple way to extract all necessary information from the deflection function alone without having to compute the stability matrix is described. This includes the determination of the relevant Maslov indices. Results of singlet and triplet cross sections for excitation and ionization are reported. The different levels of approximation -- classical, semiclassical, and uniform semiclassical -- are compared among each other and to the full quantum result.Comment: 9 figure

Molecular effects in the ionization of N2_2, O2_2 and F2_2 by intense laser fields

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 $\lambda = 800$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.Comment: 19 pages, 5 figure

Semiclassical initial value calculations of collinear helium atom

Semiclassical calculations using the Herman-Kluk initial value treatment are performed to determine energy eigenvalues of bound and resonance states of the collinear helium atom. Both the $eZe$ configuration (where the classical motion is fully chaotic) and the $Zee$ configuration (where the classical dynamics is nearly integrable) are treated. The classical motion is regularized to remove singularities that occur when the electrons collide with the nucleus. Very good agreement is obtained with quantum energies for bound and resonance states calculated by the complex rotation method.Comment: 24 pages, 3 figures. Submitted to J. Phys.

On the recombination in high-order harmonic generation in molecules

We show that the dependence of high-order harmonic generation (HHG) on the molecular orientation can be understood within a theoretical treatment that does not involve the strong field of the laser. The results for H_2 show excellent agreement with time-dependent strong field calculations for model molecules, and this motivates a prediction for the orientation dependence of HHG from the N_2 3s_g valence orbital. For both molecules, we find that the polarization of recombination photons is influenced by the molecular orientation. The variations are particularly pronounced for the N_2 valence orbital, which can be explained by the presence of atomic p-orbitals.Comment: 6 pages 7 figure