COHERENT CONTROL OF HIGH HARMONIC GENERATION USING ATTOSECOND PULSE TRAINS
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1 DOCTORAL THESIS ETH NO COHERENT CONTROL OF HIGH HARMONIC GENERATION USING ATTOSECOND PULSE TRAINS A dissertation submitted to the S WISS F EDERAL I NSTITUTE OF T ECHNOLOGY Z URICH for the degree of D OCTOR OF N ATURAL S CIENCES Submitted by A RNE H EINRICH Dipl. Phys. (Universität Hannover, Germany) born on April 22 nd, 1977 in Einbeck, Germany Accepted on the recommendation of Prof. Dr. U. Keller, Supervisor Prof. Dr. T. Esslinger, Co-Examiner Dr. J. Biegert, Co-Examiner 2006
2 Abstract The physics of atoms in strong laser fields has been a subject of intensive studies in the last twenty years. When an intense laser field, with amplitude comparable to the Coulomb field, is applied to an atomic medium, different strong field effects take place. Under these conditions a semiclassical model can be used to describe the phenomena. In this approach an electron is ionized by tunneling from the ground state, and then it is accelerated in the field of the laser and driven back to the atom. The processes differ in the last step, one possibility is that the electron rescatters elastically leading to the formation of highly energetic electrons, a phenomenon called above threshold ionization (ATI). On the other hand the electron can rescatter inelastically and free another electron, a phenomenon that is called nonsequential double ionization (NSDI). Alternatively it can recombine and generate a high energetic photon, a process known as high harmonic generation (HHG). In this thesis I will concentrate on high harmonic generation, the emphasis being on the theoretical background and an experimental proof of how high harmonic generation can be controlled using an attosecond pulse train (APT). In this method an attosecond pulse train is used in combination with an intense infrared (IR) laser field. The timing of the attosecond pulse train with respect to the infrared laser field can be used to microscopically select a single quantum path contribution to high harmonic generation that would otherwise consist of many interfering components. The attosecond pulse train controls the release of the electron into the continuum and influences the yield and coherence of the harmonics generated. Depending on the chosen time delay between infrared laser and attosecond pulse train, the harmonic spectrum is significantly enhanced, and exhibits either a spectrally resolved plateau of harmonics, or distinct harmonics in the cut-off. - X -
3 - XI - ABSTRACT To investigate, if the microscopic effect persists phase matching, nonadiabatic calculations of the macroscopic harmonic signal created by a gas volume of helium atoms exposed to a strong infrared laser pulse in combination with an attosecond pulse train are presented. It is shown that the harmonic yield can be enhanced by two to four orders of magnitude for the optimal delays between the infrared and the attosecond pulse train. Since attosecond pulse train assisted high harmonic generation survives and even improves phase matching a systematic study of additional degrees of freedom added by the attosecond pulse train on the single atom level is presented. An initial experiment on attosecond pulse train assisted high harmonic generation was carried out. Harmonics in the vacuum ultraviolet (VUV) spectral range are generated in a Xe target, and focused together with the remaining IR field into a He gas jet to generate high harmonics in the extreme ultraviolet (XUV) spectral range. The harmonics generated by both fields show a clear enhancement of a factor of five in the cut-off region compared to the infrared-only case. In the experiment the delay between both fields could not be adjusted and the incoming vacuum ultraviolet harmonics were not temporally characterized. Therefore a direct proof that an attosecond pulse train is formed, could not be provided. For temporal characterization of vacuum ultraviolet or attosecond pulse train assisted high harmonics an imaging electron spectrometer is presented. The spectrometer maps the electron distribution of an ionization event on a phosphor screen in such a way that the full three-dimensional electron momentum distribution can be reconstructed. In this way new insights in strong field processes not possible with conventional electron time of flight (TOF) spectrometers can be gained. In particular the temporal structure of single isolated attosecond pulses and attosecond pulse trains can be measured. Moreover pump-probe measurements with attosecond pulse trains, to investigate attosecond pulse train assisted above threshold ionization and attosecond pulse train assisted nonsequential double ionization become possible with this spectrometer.
4 Die Physik von Atomen in starken Laserfeldern ist ein sich seit 20 Jahren stetig weiterentwickelnder Forschungszweig. Wirkt ein intensiver Laserstrahl mit einer Feldstärke vergleichbar dem Coulombfeld auf ein atomares Medium treten verschiedene Effekte auf, die mit Hilfe eines semiklassischen Modells beschrieben werden können. In diesem Kontext tunnelt ein Elektron aus dem Grundzustand ins Kontinuum. Im elektrischen Feld des Lasers wird es beschleunigt und zum Atom zurückgetrieben. Beim letzten Schritt sind verschiedene Phänomene zu unterscheiden. Das Elektron kann elastisch gestreut werden und somit hochenergetische Elektronen erzeugen. Dieser Prozess wird above threshold ionization (ATI) genannt. Das Elektron kann aber daneben auch inelastisch gestreut werden und ein anderes Elektron ionisieren. Dieser Prozess wird als nonsequential double ionization (NSDI) bezeichnet. Alternativ kann es in den Grundzustand rekombinieren und dabei ein hochenergetisches Photon erzeugen; ein Prozess bekannt als high harmonic generation (HHG). In meiner Dissertation habe ich mich auf HHG konzentriert, wobei der Augenmerk auf der theoretischen Beschreibung und auf dem experimentellen Beweis liegt, dass ein attosecond pulse train (APT) benutzt werden kann um high harmonic generation zu kontrollieren. Dazu wird ein APT in Kombination mit einem intensiven infrarot (IR)-Laserfeld benutzt. Dabei kann der Zeitpunkt des APT im Vergleich zum IR-Laserfeld benutzt werden, um mikroskopisch den Beitrag eines einzelnen Quantenpfades zur HHG auszuwählen, die normalerweise aus vielen interferierenden Komponenten besteht. Der APT kontrolliert die Ionisation des Elektrons und beeinflusst somit den Fluss und die Kohärenz der erzeugten Harmonischen. Abhängig von dem gewählten zeitlichen Abstand zwischen dem IR-Laser und dem APT, ist das harmonischen - XII -
5 - XIII - KURZFASSUNG Spektrum signifikant verstärkt und hat entweder spektral aufgelöste Plateau- Harmonische oder ausgeprägte Harmonische im cut-off. Zur Untersuchung, ob der mikroskopische Effekt phase matching übersteht, werden nicht adiabatische Rechnungen des makroskopisch erzeugen harmonischen Signals von einem mit Heliumatomen ausgefüllten Volumen unter dem Einfluss eines starken IR-Laserpulses in Kombination mit einem APT vorgestellt. Die Rechnungen zeigen, dass das harmonische Signal bei optimalem zeitlichem Abstand zwischen dem IR und dem APT um zwei bis vier Größenordnungen verstärkt wird. Da APT-assisted HHG nicht nur phase matching übersteht sondern sogar verbessert, wird eine systematische Studie auf atomarer Ebene zur Abhängigkeit der Erzeugung von den zusätzlichen Freiheitsgraden des APT vorgestellt. Ein erstes Experiment zur APT-assisted HHG wird präsentiert, wobei Harmonische im vakuum-ultravioletten (VUV) Spektralbereich in Xe erzeugt werden und zusammen mit dem übrig gebliebenen IR-Feld in einen He Gasjet fokussiert werden, um hohe Harmonische im extrem-ultravioletten (XUV) Spektralbereich zu erzeugen. Die von beiden Feldern gemeinsam erzeugten Harmonischen sind gegenüber den von dem IR alleine erzeugten um das Fünffache verstärkt. In dem Experiment konnte der zeitliche Abstand nicht variiert und die VUV Harmonischen zeitlich nicht charakterisiert werden, daher konnte kein direkter Beweis für einen APT erbracht werden. Für die zeitliche Charakterisierung der VUV und APT-assisted HHG Strahlung wird ein abbildendes Elektronenspektrometer vorgestellt, das die Elektronenverteilung eines Ionisationsvorganges auf einen Phosphorschirm derart abbildet, dass die volle dreidimensionale Impulsverteilung rekonstruiert werden kann. Somit können neue Einblicke in strong field Prozesse gewonnen werden, die mit konventionellen Flugzeitspektrometern nicht möglich sind. Im Besonderen kann die zeitliche Struktur von einzelnen isolierten Attosekunden Pulsen und APTs gemessen werden. Zusätzlich macht es das Spektrometer
6 KURZFASSUNG - XIV - möglich Pump-Probe Messungen mit APTs durchzuführen, um APT-assisted ATI und APT-asisted NSDI zu untersuchen.
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