INITIAL AND FINAL ORBITAL ALIGNMENT PROBING OF THE FINE-STRUCTURE-CHANGING COLLISIONS AMONG THE CA(4S)(1)(4P)(1),(3)P(J) STATES WITH HE - DETERMINATION OF COHERENCE AND CONVENTIONAL CROSS-SECTIONS
Cj. Smith et al., INITIAL AND FINAL ORBITAL ALIGNMENT PROBING OF THE FINE-STRUCTURE-CHANGING COLLISIONS AMONG THE CA(4S)(1)(4P)(1),(3)P(J) STATES WITH HE - DETERMINATION OF COHERENCE AND CONVENTIONAL CROSS-SECTIONS, Journal of the Chemical Society. Faraday transactions, 89(10), 1993, pp. 1401-1411
Citations number
22
Categorie Soggetti
Chemistry Physical","Physics, Atomic, Molecular & Chemical
A laser pump-probe experiment is used to study the orbital alignment e
ffects, orientation effects and vector correlations of collisonal tran
sfer of the Ca (4s)1(4p)1, P-3(1) state to the Ca (4s)1(4p)1, P-3(2, 0
) levels. The experiment is configured in a single-collision crossed-b
eam arrangement between Ca and He, and multi-structure cross-sections
are determined using appropriate combinations of linear and circular l
aser light for the pump/probe steps. Real and imaginary parts of coher
ence cross-sections are obtained along with the conventional populatio
n cross-sections for the m1 --> m2 magnetic sublevel transitions into
the P-3(2) level. The total relative cross-section ratio for the perpe
ndicular (m1 = +/- 1) to parallel (m1 = 0) polarization preparation of
P-3(1) transferring to P-3(2) is 1.46 +/- 0.15. For initial P-3(1) pr
eparation with laser light linearly polarized perpendicular to the ini
tial relative velocity vector, the transfer into the m2-sublevels of t
he P-3(2) state show a distinct preference for the sign-changing m1 =
+ 1 --> m2 = -1 transition. Preparation of Ca P-3(1) with laser light
linearly polarized parallel to the initial relative velocity vector pr
oduces population transfer into the P-3(2) level that is completely al
igned in the +/- 1 and +/-2 sublevels, consistent with symmetry consid
erations. The magnitudes of the coherence cross-sections range from a
few percent to greater than 100% of some of the population transfer co
nventional cross-sections. Study of the alignment effect into the fina
l P-3(0) state found a very large observed effect (sigma(\m\=1)/sigma\
m\=0) of 23 +/- 0.9. Interpretation of the energy transfer results ind
icates that the energy transfer obeys symmetry rules and follows predi
ctions of curve crossings between the SIGMA and PI potentials, where f
or the transfer into P-3(2) only indirect coupling can occur.