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High Resolution Spectroscopy

Two-Color Photo-Associative Ionization Collisions between Sodium Atoms

Vanderlei Salvador Bagnato, Luís Gustavo Marcassa, C. Tao, Yanping Wang, J. Weiner

Published Jan 1, 1993• 0 citations
Publisher

Abstract

Collisions of ultracold trapped atoms ( T< 1mK) have opened a new field of atomic collisions with abundant opportunities for theory and experiments. Photo-associative ionization (PAI) in sodium atoms has been the first two-body collision Studied in optical traps3. In this process two ground state Na atoms absorb two photons during the course of the collisional encounter. The first absorption at long range put the colliding system on an attractive C3/R3 potential curve, and the two atoms begin to accelerate toward each other. A second absorption promotes the system to a doubly excited Na(3p)+Na(3p) potential curve from which the PAI process takes place at short range.

DOI
10.1364/hrs.1993.pd6

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Physical Review A•Jan 1, 1995•11 citations
Collisions of ultracold trapped atoms ( T< 1mK) have opened a new field of atomic collisions with abundant opportunities for theory and experiments. Photo-associative ionization (PAI) in sodium atoms has been the first two-body collision Studied in optical traps3. In this process two ground state Na atoms absorb two photons during the course of the collisional encounter. The first absorption at long range put the colliding system on an attractive C3/R3 potential curve, and the two atoms begin to accelerate toward each other. A second absorption promotes the system to a doubly excited Na(3p)+Na(3p) potential curve from which the PAI process takes place at short range.
We report new calculations of two-body associative ionization collisions between sodium atoms confined in a magneto-optic trap at ultracold temperatures. These collisions represent a new kind of {open_quotes}open{close_quotes} or dissipative collision for which the energy of the atom + applied light field need not be conserved due to spontaneous emission coupling to the vacuum modes of the radiation field and require density matrix methods rather than wavefunction methods to describe the collision. In these collisions the Na atoms must absorb a photon when they are in close enough proximity that a significant fraction of the excited population survives relaxation back to the ground state. The Na atoms accelerate towards each other on the excited molecular state and absorbs a second photon to a doubly excited state which then proceeds to associatively ionize at close range. Our calculations incorporate a molecular picture of the atomic collision, laser optical-field dressing of the molecular states participating in the dynamics, and population and coherence decay due to spontaneous emission. The effect of excited state hyperfine structure, which plays a critical role in the dynamics, is simulated by simplified models with a reduced number of states based on the full set of molecular-hyperfine adiabatic potentialmore » curves. Comparison is made with recent measurements of photo-associative ionization. rates as a function of optical field intensity from about 20 to 130 mW cm{sup -2}.« less
We study photo-associative ionization (PAI) for sodium atoms held in a magneto-optical trap (T < 1 mK). The process is investigated using one and two laser frequencies. For a single color PAI, we measure the rate constant as a function of light intensity and the result is compared with calculation based on semiclassical Bloch equation theory. The measured rate constant appears to saturate sooner than theory. In the two-color PAI (TCPAI) we investigate individual steps of the process. Different combinations of laser frequencies prepare different populations in each of the hyperfine ground state and the contribution of each one in this collisional process is investigated. The comparison with theory allows a fairly clear understanding of PAI and TCPAI.
The rate coefficient for the laser-induced associative-ionization reaction of ultracold Na in an optical trap is calculated as a function of the trap laser detuning from the Na(2{(}^{2}(2S1/2{\mathit{S}}_{1/2}S1/2​,F=2)\ensuremath{\rightarrow}Na(2{(}^{2}(2P3/2{\mathit{P}}_{3/2}P3/2​,F=3) resonance. Aided by a knowledge of the excited-state potential-energy curves and of the nature of the free-atom optical-pumping process, we propose the following mechanism, which we call photoassociative ionization (PAI): 2Na(3{(}^{3}(3${\mathrm{\ensuremath{\Sigma}}}_{\mathit{u}}^{+}$)${\ensuremath{\rightarrow}}^{\mathrm{\ensuremath{\Elzxh}}\mathrm{\ensuremath{\omega}}}$Na2∗{\mathrm{Na}}_{2}^{\mathrm{*}}Na2∗​(${0}_{\mathit{g}}^{\mathrm{\ensuremath{-}}}$ and 1g{1}_{\mathit{g}}1g​)${\ensuremath{\rightarrow}}^{\mathrm{\ensuremath{\Elzxh}}\mathrm{\ensuremath{\omega}}}$Na2∗∗{\mathrm{Na}}_{2}^{\mathrm{*}\mathrm{*}}Na2∗∗​(1u{1}_{\mathit{u}}1u​)\ensuremath{\rightarrow}Na2+{\mathrm{Na}}_{2}^{+}Na2+​+${\mathit{e}}^{\mathrm{\ensuremath{-}}}$. Maxima in the calculated PAI rate coefficient occur at detunings that are simultaneously one-photon resonant with bound levels of the long-range ${0}_{\mathit{g}}^{\mathrm{\ensuremath{-}}}$ state and two-photon resonant with the lower rotational levels of a vibrational level lying 9 GHz below the dissociation threshold of the autoionizing 1u{1}_{\mathit{u}}1u​ state. The calculated PAI spectrum (PAI rate coefficient versus trap-laser detuning) displays a series of broad peaks between -0.5 and -4 GHz detuning and a cutoff at -5 GHz detuning, as does the experimentally measured spectrum of Lett et al. [Phys. Rev. Lett. 67, 2139 (1991)].The broad widths of the peaks in the PAI spectrum is due in part to the orientation averaging of the collision vector with respect to the electric-field vector and to the optical pumping of the Na2{\mathrm{Na}}_{2}Na2​\ensuremath{\rightarrow}Na2∗{\mathrm{Na}}_{2}^{\mathrm{*}}Na2∗​ rovibronic transition. The calculated PAI rate coefficient at -0.6 GHz detuning is a factor of 4 higher than the experimental value. Fine-structure-changing transitions play a role in the doubly excited states, because of the 1u{1}_{\mathit{u}}1u​ avoided crossing, but not in the intermediate states, because they have gerade symmetry and the only states that have been shown to undergo fine-structure-changing transitions with large probability have ungerade symmetry. Several predictions based on the proposed model and suggestions for future experiments are discussed.
We have studied polarization effects in the photoassociation of two colliding ultra-cold Na-atoms. In a first step the two colliding atoms absorb a laser photon to associate to a singly excited molecule in a bound state of the 0g− or 1g potential. In a second step the excited molecule absorbs a second photon and is further excited to a bound level in a doubly excited potential (0u− or 1u which are autoionizing). By measuring the produced ions with parallel and perpendicular polarizations of the two laser beams used possible polarization effects can be studied. We find strong polarization effects if a 0g− state is used as the intermediate state and very little or no effects at all if a 1g state is used.
We report here measurements of two-body photoassociative ionization collisions between sodium atoms within an ultranarrow velocity class selected from a well-collimated, thermal atomic beam. Doppler-shifted excitation of the Na(3s2{\mathrm{}}^{2}2S1/2{\mathit{S}}_{1/2}S1/2​;F=1)\ensuremath{\rightarrow}Na(5p2{\mathrm{}}^{2}2P3/2{\mathit{P}}_{3/2}P3/2​) transition at 285 nm by a single-mode laser defines the narrow velocity class that subsequently populates the F=2 hyperfine level of the Na ground state by optical pumping. Probe laser beam excitation tuned near the Na(3s2{\mathrm{}}^{2}2S1/2{\mathit{S}}_{1/2}S1/2​;F=2)\ensuremath{\rightarrow}Na(3p2{\mathrm{}}^{2}2P3/2{\mathit{P}}_{3/2}P3/2​;F=3) transition produced photoassociative ionization with an average collision energy EK{\mathit{E}}_{\mathit{K}}EK​ corresponding to a temperature of 5.3 mK (EK{\mathit{E}}_{\mathit{K}}EK​=3/2kT). We determine the rate constant for the process as a function of probe beam intensity and polarization.