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Ultra-fast Dynamics of Small Molecules in Strong Fields

dc.contributor.advisorHill, Wendell Ten_US
dc.contributor.authorZhao, Kunen_US
dc.date.accessioned2006-06-14T05:45:17Z
dc.date.available2006-06-14T05:45:17Z
dc.date.issued2006-04-24en_US
dc.identifier.urihttp://hdl.handle.net/1903/3444
dc.description.abstractCorrelation detection techniques (image labeling, coincidence imaging, and joint variance) are developed with an image spectrometer capable of collecting charges ejected over 4\pi sr and a digital camera synchronized with the laser repetition rate at up to 735 Hz. With these techniques, molecular decay channels ejecting atomic fragments with different momenta (energies) can be isolated; thus the initial molecular configurations (bond lengths and/or bond angles) and orientations as well as their distributions can be extracted. These techniques are applied to study strong-field induced dynamics of diatomic and triatomic molecules. Specific studies included the measurements of the Coulomb explosion energy as a function of bond angle in linear (CO_2) and bent (NO_2) triatomics and the ejection anisotropy relative to the laser polarization axis during Coulomb explosions in both triatomic (CO_2 and NO_2) and diatomic (H_2, N_2 and O_2) systems. The experiments were performed with 100 fs, 800 nm laser pulses focused to 0.1 ~ 5 \times 10^15 W/cm^2. The explosion energy of NO_2 decreases monotonically by more than 25% from the smallest to the largest bond angle. By contrast, the CO_2 explosion energies are nearly independent of bond angle. The enhanced-ionization and static-screening models in two-dimension with three charge centers were developed to simulate the explosion energies as a function of bond angle. The predictions are consistent with the measurements of CO_2 and NO_2. The observed explosion signals as a function of bond angle for both triatomics show large-amplitude vibrations. The ejection angular distributions in triatomic (CO_2 and NO_2) and diatomic (H_2, N_2, and O_2) Coulomb explosions were measured; the contribution made to the ejection anisotropy by dynamic alignment was studied by comparing the images obtained with linearly and circularly polarized fields. Different angular distributions of the molecules are consistent with different ionization stages, induced dipole moments and rotational constants. The dynamic alignment of H_2 is found to be nearly complete. A larger dynamic alignment of CO_2 than that of N_2 or O_2 is consistent with that more electrons have been removed from CO_2 and the precursor molecular ion spends more time in the field prior to the explosion.en_US
dc.format.extent3961782 bytes
dc.format.extent27851 bytes
dc.format.extent50137 bytes
dc.format.mimetypeapplication/pdf
dc.format.mimetypeapplication/pdf
dc.format.mimetypeapplication/pdf
dc.language.isoen_US
dc.titleUltra-fast Dynamics of Small Molecules in Strong Fieldsen_US
dc.typeDissertationen_US
dc.contributor.publisherDigital Repository at the University of Marylanden_US
dc.contributor.publisherUniversity of Maryland (College Park, Md.)en_US
dc.contributor.departmentChemical Physicsen_US
dc.subject.pqcontrolledPhysics, Molecularen_US
dc.subject.pqcontrolledPhysics, Opticsen_US
dc.subject.pquncontrolledultra-fasten_US
dc.subject.pquncontrolledmolecular dynamicsen_US
dc.subject.pquncontrolledintense fielden_US
dc.subject.pquncontrolledCoulomb explosionen_US
dc.subject.pquncontrolledimagingen_US
dc.subject.pquncontrolledcorrelation detectionen_US


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