Note: Position dependence of time signals picked off a microchannel plate detector

Citation: Ablikim, U., Zohrabi, M., Jochim, B., Berry, B., Severt, T., Carnes, K. D., & Ben-Itzhak, I. (2015). Note: Position dependence of time signals picked off a microchannel plate detector. Review of Scientific Instruments, 86(1), 3. doi:10.1063/1.4906327Using an ultrafast laser and a precision mask, we demonstrate that time signals picked off directly from a microchannel plate detector depend on the position of the hit. This causes a time spread of about 280 ps, which can affect the quality of imaging measurements using large detectors. (C) 2015 AIP Publishing LLC

Note: Determining the detection efficiency of excited neutral atoms by a microchannel plate detector

Citation: Berry, B., Zohrabi, M., Hayes, D., Ablikim, U., Jochim, B., Severt, T., . . . Ben-Itzhak, I. (2015). Note: Determining the detection efficiency of excited neutral atoms by a microchannel plate detector. Review of Scientific Instruments, 86(4), 3. doi:10.1063/1.4916953We present a method for determining the detection efficiency of neutral atoms relative to keV ions. Excited D* atoms are produced by D-2 fragmentation in a strong laser field. The fragments are detected by a micro-channel plate detector either directly as neutrals or as keV ions following field ionization and acceleration by a static electric field. Moreover, we propose a new mechanism by which neutrals are detected. We show that the ratio of the yield of neutrals and ions can be related to the relative detection efficiency of these species. (C) 2015 AIP Publishing LLC

Tracking ultrafast non-adiabatic dissociation dynamics of the deuterated water dication molecule

We applied reaction microscopy to elucidate fast non-adiabatic dissociation dynamics of deuterated water molecules after direct photo-double ionization at 61 eV with synchrotron radiation. For the very rare D+ + O+ + D breakup channel, the particle momenta, angular, and energy distributions of electrons and ions, measured in coincidence, reveal distinct electronic dication states and their dissociation pathways via spin-orbit coupling and charge transfer at crossings and seams on the potential energy surfaces. Notably, we could distinguish between direct and fast sequential dissociation scenarios. For the latter case, our measurements reveal the geometry and orientation of the deuterated water molecule with respect to the polarization vector that leads to this rare 3-body molecular breakup channel. Aided by multi-reference configuration-interaction calculations, the dissociation dynamics could be traced on the relevant potential energy surfaces and particularly their crossings and seams. This approach also unraveled the ultrafast time scales governing these processes

Mechanisms and dynamics of the NH⁺₂ + H⁺ and NH⁺ + H⁺ + H fragmentation channels upon single-photon double ionization of NH₃

We present state-selective measurements on the NH$_2^{+}$ + H$^{+}$ and NH$^{+}$ + H$^{+}$ + H dissociation channels following single-photon double ionization at 61.5 eV of neutral NH$_{3}$, where the two photoelectrons and two cations are measured in coincidence using 3-D momentum imaging. Three dication electronic states are identified to contribute to the NH$_2^{+}$ + H$^{+}$ dissociation channel, where the excitation in one of the three states undergoes intersystem crossing prior to dissociation, producing a cold NH$_2^+$ fragment. In contrast, the other two states directly dissociate, producing a ro-vibrationally excited NH$_2^+$ fragment with roughly 1 eV of internal energy. The NH$^{+}$ + H$^{+}$ + H channel is fed by direct dissociation from three intermediate dication states, one of which is shared with the NH$_2^{+}$ + H$^{+}$ channel. We find evidence of autoionization contributing to each of the double ionization channels. The distributions of the relative emission angle between the two photoelectrons, as well as the relative angle between the recoil axis of the molecular breakup and the polarization vector of the ionizing field, are also presented to provide insight on both the photoionization and photodissociation mechanisms for the different dication states

Unambiguous observation of F-atom core-hole localization in CF4 through body-frame photoelectron angular distributions

Citation: McCurdy, C. W., Rescigno, T. N., Trevisan, C. S., Lucchese, R. R., Gaire, B., Menssen, A., . . . Weber, T. (2017). Unambiguous observation of F-atom core-hole localization in CF4 through body-frame photoelectron angular distributions. Physical Review A, 95(1). doi:10.1103/PhysRevA.95.011401A dramatic symmetry breaking in K-shell photoionization of the CF4 molecule in which a core-hole vacancy is created in one of four equivalent fluorine atoms is displayed in the molecular frame angular distribution of the photoelectrons. Observing the photoejected electron in coincidence with an F+ atomic ion after Auger decay is shown to select the dissociation path where the core hole was localized almost exclusively on that atom. A combination of measurements and ab initio calculations of the photoelectron angular distribution in the frame of the recoiling CF3+ and F+ atoms elucidates the underlying physics that derives from the Ne-like valence structure of the F(1s-1) core-excited atom. © 2017 American Physical Society

The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields

Much of our intuition about strong-field processes is built upon studies of diatomic molecules, which typically have electronic states that are relatively well separated in energy. In polyatomic molecules, however, the electronic states are closer together, leading to more complex interactions. A combined experimental and theoretical investigation of strong-field ionization followed by hydrogen elimination in the hydrocarbon series C2D2, C2D4 and C2D6 reveals that the photofragment angular distributions can only be understood when the field-dressed orbitals rather than the field-free orbitals are considered. Our measured angular distributions and intensity dependence show that these field-dressed orbitals can have strong Rydberg character for certain orientations of the molecule relative to the laser polarization and that they may contribute significantly to the hydrogen elimination dissociative ionization yield. These findings suggest that Rydberg contributions to field-dressed orbitals should be routinely considered when studying polyatomic molecules in intense laser fields

Fragmentation of CD+ induced by intense ultrashort laser pulses

Citation: Graham, L., Zohrabi, M., Gaire, B., Ablikim, U., Jochim, B., Berry, B., . . . Ben-Itzhak, I. (2015). Fragmentation of CD+ induced by intense ultrashort laser pulses. Physical Review A, 91(2), 11. doi:10.1103/PhysRevA.91.023414The fragmentation of CD[superscript +] in intense ultrashort laser pulses was investigated using a coincidence three-dimensional momentum imaging technique improved by employing both transverse and longitudinal electric fields. This allowed clear separation of all fragmentation channels and the determination of the kinetic energy release down to nearly zero, for a molecule with significant mass asymmetry. The most probable dissociation pathways for the two lowest dissociation limits, C[superscript +]+D and C+D[superscript +], were identified for both 22-fs, 798-nm and 50-fs, 392-nm pulses. Curiously, the charge asymmetric dissociation of CD[superscript 2+] was not observed for 392-nm photons, even though it was clearly visible for the fundamental 798 nm at the same peak intensity

Strong-field dissociation dynamics of molecular dications

Citation: Jochim, B., Severt, T., Zohrabi, M., Ablikim, U., Berry, B., Gaire, B., . . . Ben-Itzhak, I. (2015). Strong-field dissociation dynamics of molecular dications. 635(11). doi:10.1088/1742-6596/635/11/112044We focus on the dissociation of metastable molecular dications induced by intense, ultrafast laser pulses. In particular, we demonstrate the dominant role of commonly-neglected permanent-dipole transitions and drive dissociation via a pump-dump-like mechanism within a single laser pulse. © Published under licence by IOP Publishing Ltd

The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense few-cycle laser pulses

Citation: Jochim, B., Siemering, R., Zohrabi, M., Voznyuk, A., Mahowald, J. B., Schmitz, D. G., . . . De Vivie-Riedle, R. (2015). The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense few-cycle laser pulses. 635(11). doi:10.1088/1742-6596/635/11/112043We demonstrate the importance of ionization from Rydberg orbitals via experimental and theoretical work focusing on the strong-field dissociative single ionization of small hydrocarbons. Our findings suggest that Rydberg states should be routinely considered when studying polyatomic molecules in intense laser fields. © Published under licence by IOP Publishing Ltd.Additional Authors: Wells, E.;De Vivie-Riedle, R