Optical control of ground-state atomic orbital alignment: Cl(P-2(3/2)) atoms from HCl(v=2,J=1) photodissociation

Dimitris Sofikitis, Luis Rubio-Lago, Marion R. Martin, Davida J. Brown Ankeny, Nathaniel C. -M. Bartlett, Andrew J. Alexander, Richard N. Zare, T. Peter Rakitzis

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(HCl)-Cl-35(v=0,J=0) molecules in a supersonic expansion were excited to the (HCl)-Cl-35(v=2,J=1,M=0) state with linearly polarized laser pulses at about 1.7 mu m. These rotationally aligned J=1 molecules were then selectively photodissociated with a linearly polarized laser pulse at 220 nm after a time delay, and the velocity-dependent alignment of the Cl-35(P-2(3/2)) photofragments was measured using 2+1 REMPI and time-of-flight mass spectrometry. The Cl-35(P-2(3/2)) atoms are aligned by two mechanisms: (1) the time-dependent transfer of rotational polarization of the (HCl)-Cl-35(v=2,J=1,M=0) molecule to the Cl-35(P-2(3/2)) nuclear spin [which is conserved during the photodissociation and thus contributes to the total Cl-35(P-2(3/2)) photofragment atomic polarization] and (2) the alignment of the Cl-35(P-2(3/2)) electronic polarization resulting from the photoexcitation and dissociation process. The total alignment of the Cl-35(P-2(3/2)) photofragments from these two mechanisms was found to vary as a function of time delay between the excitation and the photolysis laser pulses, in agreement with theoretical predictions. We show that the alignment of the ground-state Cl-35(P-2(3/2)) atoms, with respect to the photodissociation recoil direction, can be controlled optically. Potential applications include the study of alignment-dependent collision effects. (c) 2007 American Institute of Physics.

Original languageEnglish
Article number144307
Pages (from-to)-
Number of pages7
JournalJournal of Chemical Physics
Issue number14
Publication statusPublished - 14 Oct 2007


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