Kohärente transiente und effiziente Endzustandskontrolle in Atomen und Molekülen

Es ist ein lang gehegter Traum in der Chemie, den Ablauf einer chemischen Reaktion zu kontrollieren und das Aufbrechen und Bilden chemischer Bindungen zu steuern. Diesem Ziel verschreibt sich auch das Forschungsgebiet der Femtochemie. Hier werden Femtosekunden Laserpulse eingesetzt um auf dem Quantenlevel molekulare Dynamiken auf ihren intrinsischen Zeitskalen zu kontrollieren und das System selektiv und effizient von einem Anfangs- in einen Zielzustand zu überführen. Der Wunsch, mit geformten Femtosekunden Laserpulsen Kontrolle über transiente Dynamiken und finale Populationen auszuüben, zu beobachten und zu verstehen, bildet auch die Motivation für diese Arbeit. Hierzu wurden mit Hilfe der Photoelektronenspektroskopie Untersuchungen zur Wechselwirkung atomarer und molekularer Prototypsysteme mit intensiven, geformten Femtosekunden Laserpulsen durchgeführt. Die Verwendung von Modelsystemen ermöglicht es, grundlegende Mechanismen der kohärenten Kontrolle in intensiven Laserfeldern zu analysieren, ohne dass sie durch komplexe Wechselwirkungen verschleiert werden. Zunächst wurde die Wechselwirkung von Kaliumatomen mit gechirpten Femtosekunden Laserpulsen untersucht. In den Experimenten wurden sowohl transiente Dynamiken als auch die Endbesetzungen der elektronischen Zustände abgebildet. In den folgenden Experimenten wurde das Quantenkontrollszenario SPODS auf die gekoppelte Elektronen-Kern-Dynamik in Molekülen übertragen. Die Kontrolle basiert auf der Erzeugung und Manipulation von Ladungsoszillationen durch Pulssequenzen. Der letzte Teil widmet sich der Entwicklung adiabatischer Kontrollmechanismen in Molekülen. Bei den Experimenten wurden gechirpte Airypulse eingesetzt um robuste Starkfeldanregung in molekularen Systemen zu induzieren. In Zukunft wird die Erforschung immer komplexerer Moleküle im Rahmen der transienten Kontrolle im Fokus stehen. Dabei werden nicht nur die effiziente Besetzung gebundener Zustände von Interesse sein, sondern auch die gezielte Dissoziation in spezifische Fragmente, photoinduzierte Isomerisierungsreaktionen oder die Kontrolle über transiente Dynamiken, die Einfluss auf andere molekulare Eigenschaften haben. Vor dem Hintergrund dieses übergeordneten Wunsches, photochemische Reaktionen immer komplexerer Moleküle, bis hin zu großen, biologisch relevanten Molekülen, zu kontrollieren, ist es umso wichtiger, die zugrundeliegenden Anregungsmechanismen in einfachen Systemen nachzuvollziehen. In den hier präsentierten Experimenten wurde gezeigt, wie die simultane Beobachtung der bekleideten und der stationären Zustände in atomaren Systemen zu einem umfassenden Bild der lichtinduzierte Dynamiken führen kann. Die gewonnenen Erkenntnisse können auf die Steuerung gekoppelter Dynamiken übertragen werden, durch die Kontrolle auch in molekularen Systemen möglich wird.

Generation of strong quasistatic magnetic fields in interactions of ultraintense and short laser pulses with overdense plasma targets

An analytical fluid model is proposed for the generation of strong quasistatic magnetic fields during normal incidence of a short ultraintense Gaussian laser pulse with a finite spot size on an overdense plasma. The steepening of the electron density profile in the originally homogeneous overdense plasma and the formation of electron cavitation as the electrons are pushed inward by the laser are included self-consistently. It is shown that the appearance of the cavitation plays an important role in the generation of quasistatic magnetic fields: the strong plasma inhomogeneities caused by the formation of the electron cavitation lead to the generation of a strong axial quasistatic magnetic field B-z. In the overdense regime, the generated quasistatic magnetic field increases with increasing laser intensity, while it decreases with increasing plasma density. It is also found that, in a moderately overdense plasma, highly intense laser pulses can generate magnetic fields similar to 100 MG and greater due to the transverse linear mode conversion process.

A discrete time-dependent method for metastable atoms and molecules in intense fields

The full-dimensional time-dependent Schrodinger equation for the electronic dynamics of single-electron systems in intense external fields is solved directly using a discrete method. Our approach combines the finite-difference and Lagrange mesh methods. The method is applied to calculate the quasienergies and ionization probabilities of atomic and molecular systems in intense static and dynamic electric fields. The gauge invariance and accuracy of the method is established. Applications to multiphoton ionization of positronium, the hydrogen atom and the hydrogen molecular ion are presented. At very high laser intensity, above the saturation threshold, we extend the method using a scaling technique to estimate the quasienergies of metastable states of the hydrogen molecular ion. The results are in good agreement with recent experiments. (C) 2004 American Institute of Physics.

The RMT method for many-electron atomic systems in intense short-pulse laser light

We describe a new ab initio method for solving the time-dependent Schrödinger equation for multi-electron atomic systems exposed to intense short-pulse laser light. We call the method the R-matrix with time-dependence (RMT) method. Our starting point is a finite-difference numerical integrator (HELIUM), which has proved successful at describing few-electron atoms and atomic ions in strong laser fields with high accuracy. By exploiting the R-matrix division-of-space concept, we bring together a numerical method most appropriate to the multi-electron finite inner region (R-matrix basis set) and a different numerical method most appropriate to the one-electron outer region (finite difference). In order to exploit massively parallel supercomputers efficiently, we time-propagate the wavefunction in both regions by employing Arnoldi methods, originally developed for HELIUM.

Fundamental interactions of molecules (Na_2, Na_3) with intense femtosecond laser pulses

The real-time dynamics of multiphoton ionization and fragmentation of molecules Na_2 and Na_3 has been studied in molecular beam experiments employing ion and electron spectroscopy together with femtosecond pump-probe techniques. Experiments with Na_2 and Na_3 reveal unexpected features of the dynamics of the absorption of several photons as seen in the one- and three-dimensional vibrational wave packet motion in different potential surfaces and in high laser fields: In Na_2 a second major resonance-enhanced multiphoton ionization (REMPI) process is observed, involving the excitation of two electrons and subsequent electronic autoionization. The possibility of controlling a reaction by controlling the duration of propagation of a wave packet on an electronically-excited surface is demonstrated. In high laser fields, the contributions from direct photoionization and from the second REMPI process to the total ion yield change, due to different populations in the electronic states participating in the multiphoton ionization (MPI) processes. In addition, a vibrational wave packet motion in the electronic ground state is induced through stimulated emission pumping by the pump laser. The 4^1 \summe^+_g shelf state of Na_2 is given as an example for performing frequency spectroscopy of highlying electronic states in the time domain. Pure wave packet effects, such as the spreading and the revival of a vibrational wave packet, are investigated. The three-dimensional wave packet motion in the Na_3 reflects the normal modes in the X and B states, and shows in addition the pseudorotational motion in the B state in real time.

Methods of generating carrier-envelope-phase stabilized, intense, few-cycle laser pulses

Ultrafast laser pulses have become an integral part of the toolbox of countless laboratories doing physics, chemistry, and biological research. The work presented here is motivated by a section in the ever-growing, interdisciplinary research towards understanding the fundamental workings of light-matter interactions. Specifically, attosecond pulses can be useful tools to obtain the desired insight. However access to, and the utility of, such pulses is dependent on the generation of intense, few-cycle, carrier-envelope-phase stabilized laser pulses. The presented work can be thought of as a sort of roadmap towards the latter. From the oscillator which provides the broadband seed to amplification methods, the integral pieces necessary for the generation of attosecond pulses are discussed. A range of topics from the fundamentals to design challenges is presented, outfitting the way towards the practical implementation of an intense few-cycle carrier-envelope-phase stabilized laser source.

A plasma channel scheme for the interaction of an intense femtosecond laser pulse with a deuterium cluster jet

We propose a plasma channel scheme to obtain an improved table-top laser driven fusion neutron yield as a result of explosions of large deuterium clusters irradiated by an intense laser pulse. A cylindrical plasma channel is created by two moderate intensity laser prepulses at the edge of a deuterium cluster jet along which an intense main laser pulse propagates several nanoseconds later. With the aid of this plasma channel, the main laser pulse will be allowed to deposit its energy into the central region of the deuterium gas jet where the cluster sizes are larger and the atomic density is higher. The plasma channel formation and its impact on the deuterium ion energy spectrum and the consequent fusion neutron yield have been investigated. The calculated results show that a remarkable increase of the table-top laser driven fusion neutron yield would be expected.

Guiding and confining fast electrons by transient electric and magnetic fields with a plasma inverse cone

The fast electron propagation in an inverse cone target is investigated computationally and experimentally. Two-dimensional particle-in-cell simulation shows that fast electrons with substantial numbers are generated at the outer tip of an inverse cone target irradiated by a short intense laser pulse. These electrons are guided and confined to propagate along the inverse cone wall, forming a large surface current. The propagation induces strong transient electric and magnetic fields which guide and confine the surface electron current. The experiment qualitatively verifies the guiding and confinement of the strong electron current in the wall surface. The large surface current and induced strong fields are of importance for fast ignition related researches.

Origin of the double-peak structure in longitudinal momentum distributions for single ionization of an He atom in strong laser field

The single ionization of an He atom by intense linearly polarized laser field in the tunneling regime is studied by S- matrix theory. When only the first term of the expansion of the S matrix is considered and time, spatial distribution, and fluctuation of the laser pulse are taken into account, the obtained momentum distribution in the polarization direction of laser field is consistent with the semiclassical calculation, which only considers tunneling and the interaction between the free electron and external field. When the second term, which includes the interaction between the core and the free electron, is considered, the momentum distribution shows a complex multipeak structure with the central minimum and the positions of some peaks are independent of the intensity in some intensity regime, which is consistent with the recent experimental result. Based on our analysis, we found that the structures observed in the momentum distribution of an He atom are attributed to the " soft" collision of the tunneled electron with the core.

Suppression of multiple ionization of atomic ions in intense ultrafast laser pulses

The interaction of an intense laser field with a beam of atomic ions has been investigated experimentally for the first time. The ionization dynamics of Ar+ ions and Ar neutrals in a 60 fs, 790 nm laser pulse have been compared and contrasted at intensities up to 10(16) W cm (-2). Our results show that nonsequential ionization from an Ar+ target is strongly suppressed compared with that from the corresponding neutral target. We have also observed for the first time the strong field ionization of high lying target metastable levels in the Ar+ beam.

Fast-beam study of H2+ ions in an intense femtosecond laser field

A fast beam of H-2(+) ions, produced from a low energy ion accelerator, has been used for the first time in intense laser field experiments. The technique has enabled neutral dissociation products to be analysed and detected for the first time in such studies. Energy spectra of neutral and ionized fragments, product yields as a function of focused laser intensity and angular distributions of neutral dissociation products have been measured. Significant differences are observed between the present results and those obtained from experiments involving neutral H-2 molecules. These differences are indicative of the precursor H-2 molecule playing an important and hitherto neglected formative role in the laser-induced fragmentation processes.

Dynamic control of laser-produced proton beams

The emission characteristics of intense laser driven protons are controlled using ultrastrong (of the order of 10(9) V/m) electrostatic fields varying on a few ps time scale. The field structures are achieved by exploiting the high potential of the target (reaching multi-MV during the laser interaction). Suitably shaped targets result in a reduction in the proton beam divergence, and hence an increase in proton flux while preserving the high beam quality. The peak focusing power and its temporal variation are shown to depend on the target characteristics, allowing for the collimation of the inherently highly divergent beam and the design of achromatic electrostatic lenses.

Simulation of relativistically colliding laser-generated electron flows

The plasma dynamics resulting from the simultaneous impact, of two equal, ultra-intense laser pulses, in two spatially separated spots, onto a dense target is studied via particle-in-cell simulations. The simulations show that electrons accelerated to relativistic speeds cross the target and exit at its rear surface. Most energetic electrons are bound to the rear surface by the ambipolar electric field and expand along it. Their current is closed by a return current in the target, and this current configuration generates strong surface magnetic fields. The two electron sheaths collide at the midplane between the laser impact points. The magnetic repulsion between the counter-streaming electron beams separates them along the surface normal direction, before they can thermalize through other beam instabilities. This magnetic repulsion is also the driving mechanism for the beam-Weibel (filamentation) instability, which is thought to be responsible for magnetic field growth close to the internal shocks of gamma-ray burst jets. The relative strength of this repulsion compared to the competing electrostatic interactions, which is evidenced by the simulations, suggests that the filamentation instability can be examined in an experimental setting. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4768426]

Investigations of ultrafast charge dynamics in laser-irradiated targets by a self probing technique employing laser driven protons

The divergent and broadband proton beams produced by the target normal sheath acceleration mechanism provide the unique opportunity to probe, in a point-projection imaging scheme, the dynamics of the transient electric and magnetic fields produced during laser-plasma interactions. Commonly such experimental setup entails two intense laser beams, where the interaction produced by one beam is probed with the protons produced by the second. We present here experimental studies of the ultra-fast charge dynamics along a wire connected to laser irradiated target carried out by employing a ‘self’ proton probing arrangement – i.e. by connecting the wire to the target generating the probe protons. The experimental data shows that an electromagnetic pulse carrying a significant amount of charge is launched along the wire, which travels as a unified pulse of 10s of ps duration with a velocity close to speed of light. The experimental capabilities and the analysis procedure of this specific type of proton probing technique are discussed.

Physical characterization of laser interaction and shock generation in laser shock processing: coupled theoretical-experimental analysis

Laser Shock Processing is developing as a key technology for the improvement of surface mechanical and corrosion resistance properties of metals due to its ability to introduce intense compressive residual stresses fields into high elastic limit materials by means of an intense laser driven shock wave generated by laser with intensities exceeding the 109 W/cm2 threshold, pulse energies in the range of 1 Joule and interaction times in the range of several ns. However, because of the relatively difficult-to-describe physics of shock wave formation in plasma following laser-matter interaction in solid state, only limited knowledge is available in the way of full comprehension and predictive assessment of the characteristic physical processes and material transformations with a specific consideration of real material properties. In the present paper, an account of the physical issues dominating the development of LSP processes from a moderately high intensity laser-matter interaction point of view is presented along with the theoretical and computational methods developed by the authors for their predictive assessment and new experimental contrast results obtained at laboratory scale.