The authors have used laser cooling and trapping techniques to investigate photoionization and cold collisions. With laser-trapped Rb, they have measured the photoionization cross section from the first excited (5P) level by observing the photoionization-induced loss rate of neutral atoms from the trap. This technique has the advantage that it directly measures the photoionization rate per atom. Knowing the ionizing laser intensity and the excited-state fraction, the measured loss rate gives the absolute cross section. Using this technique, the Rb 5P photoionization cross section at {approximately}400 nm has been determined with an uncertainty of 9%. The authors are currently attempting to extend this method to the 5D level. Using time-ordered pulses of diode-laser light (similar to the STIRAP technique), they have performed very efficient two-photon excitation of trapped Rb atoms to 5D. Finally, they will present results from a recent collaboration which combines measurements form conventional molecular spectroscopy (single photon and double resonance) with photoassociation collisions of ultracold Na atoms to yield a precise ({le}1 ppm) value for the dissociation energy of the X {Sigma}{sub g}{sub +} ground state of the Na{sub 2} molecule.
The authors have used laser cooling and trapping techniques to investigate photoionization and cold collisions. With laser-trapped Rb, they have measured the photoionization cross section from the first excited (5P) level by observing the photoionization-induced loss rate of neutral atoms from the trap. This technique has the advantage that it directly measures the photoionization rate per atom. Knowing the ionizing laser intensity and the excited-state fraction, the measured loss rate gives the absolute cross section. Using this technique, the Rb 5P photoionization cross section at {approximately}400 nm has been determined with an uncertainty of 9%. The authors are currently attempting to extend this method to the 5D level. Using time-ordered pulses of diode-laser light (similar to the STIRAP technique), they have performed very efficient two-photon excitation of trapped Rb atoms to 5D. Finally, they will present results from a recent collaboration which combines measurements form conventional molecular spectroscopy (single photon and double resonance) with photoassociation collisions of ultracold Na atoms to yield a precise ({le}1 ppm) value for the dissociation energy of the X {Sigma}{sub g}{sub +} ground state of the Na{sub 2} molecule.
A series of experiments is performed on cold 85Rb atoms confined in a magneto-optical trap. A variation of Stimulated Raman adiabatic passage (STIRAP) is used to transfer population from the 5S 1/2 ground state to the 5D5/2 state with an efficiency exceeding 80%. This process relies on moderately intense pulses arriving in the counterintuitive order, i.e., the upper transition (5P → 5D) driven before the lower transition (5S → 5P ). There is reasonable agreement with computer simulations, excepting a marked discrepancy between measured intensities and those used in the simulations. With a large ensemble of 5D atoms available, the 5D photoionization cross section at four different laser wavelengths (1064, 788, 647 and 532 nm) is determined via trap loss measurements. The theoretical calculations agree well with the experimental results (17.7, 10.9, 7.6 and 5.2 Mb, respectively). An experiment to measure the 5S-5D collisional rate constant sets an order-of-magnitude upper bound of 10−10 cm3/s, assuming all atoms are 5S-5D pairs. ^
We describe a new technique for accurate measurement of absolute photoionization cross sections. By measuring the loss rateof atoms from a laser trap in the presence of ionizing light, we directly measure the photoionization rate. The only quantities requiring absolute calibration are the ionizing laser intensity and the fractional population in the relevant state. Our technique is capable of detecting extremely small ionization rates, which means that low-power cw sources can be used. We have applied this method to photoionization from the 5P(3/2) state of rubidium at wavelengths of 413 and 407 nm.The cross sections are 1.36(12) x 10(-17) and 1.25(11) x 10(-17) cm(2) , respectively.
Advances in laser cooling of neutral atoms have made possible a new form of high resolution spectoscopy: photoassociation of ultracold atoms. Colliding neutral atoms, confined in a laser trap, are photoassociated to bound excited states of the dimer molecule by absorbing a photon from a tunable laser. The technique can probe long range and {open_quote}purely long range{close_quote} molecular states that are difficult or impossible to detect by traditional means and, because of the extremely low energy of the colliding atoms (1 mK), is capable of high resolution (0.001 cm{minus}1). Recent results include, the first direct (and most precise) measurement of a molecular dissociation limit, the first observation of retardation effects in atom-atom interactions, high precision measurements of atomic lifetimes, and the study of exotic states of alkali dimers.
We report on measurements of the cross section for photoionization of Rb atoms in the highly excited 5D5/2 level at wavelengths ranging from 1064 to 532 nm (photoelectron energies of 0.175 to 1.34 eV). We efficiently populate the 5D5/2 level using coherent two-photon excitation of trapped atoms with pulses in the counterintuitive order. The absolute photoionization cross sections are then measured via the increased loss of atoms from the magneto-optical trap when it is illuminated by the photoionizing light. Our results are in good agreement with new calculations based on the valence-electron parametric potential method.
This work presents various novel results in the field of experimental and theoretical trapped ion studies. All investigations involve laser-cooled 138Ba+ ions confined in a linear quadrupole ion trap, which serve as coolant for complex molecular ions, as target for collisions with neutral atoms, or as model system in theoretical analyses. The special feature of the apparatus used in this work, is a molecular ion source based on electrospray ionization that allows for the production of gas-phase molecular ions of almost arbitrary species with a maximum mass-to-charge ratio of 2,000 Da. Trapped together with laser-cooled 138Ba+ ions, the molecular ions can be cooled down, kept cold and investigated for many minutes and in principle for up to hours in a nearly collisionless environment.
In this work, the sympathetic cooling of complex molecular ions to translational temperatures below 1 K is demonstrated for different types of molecules covering a mass range from 182 to 12,400 Da. Using the example of the protein cytochrome c, with a mass of about 12,400 Da the most massive molecular species sympathetically cooled in an ion trap so far, the methods for detection of successful trapping and cooling, and temperature determination are presented in detail. In one case, multiply protonated molecules of the protein cytochrome c have been cooled to less than 0.75 K. Furthermore, two methods for measuring photodestruction rates of cold, trapped complex molecular ions have been developed that can, for example, be applied in destructive spectroscopy schemes. Both techniques are demonstrated using the example of singly protonated glycyrrhetinic acid molecules (GAH+) dissociated by an ultraviolet (UV) laser. Measurements of the photodestruction rate were performed at different intensities of the UV laser, and rates as low as 0.05 s-1 and less have been determined, which is only possible due to the long ion storage times that can be achieved with this apparatus. For the UV laser wavelength of 266 nm, a destruction cross section of (1.1±0.1)∙10E-17 cm2 for GAH+ has been determined.
In this work, feasibility studies towards internal cooling of trapped complex molecular ions have been performed. Such an additional internal cooling could be realized via collisions with laser-cooled neutral atoms. To test their suitability, neutral atoms of Li, Na, K, Rb, Cs, and Yb have been collided with trapped laser-cooled and not cooled Ba+ ions as well as with complex molecular ions. For all species charge exchange reactions with Ba+ ions have been observed excluding these species for collisional cooling. While K, Rb, and Cs showed charge exchange reactions with ground state and laser-excited Ba+ ions, the charge exchange rates of Yb and Ba+ were found to be state dependent. Collisions of neutral Yb atoms were found to be reactive and lead to the formation of adducts and fragments, in contrast to the alkali metals for which no such reactions have been observed. In addition, the motion of cooled, trapped ions has been studied theoretically via simulations. When the translational energy of a trapped ion ensemble is sufficiently reduced, a first-order phase transition from a liquid to a solid state occurs with the ion ensemble changing from a disordered ion cloud to an ordered ion crystal. As ions in a linear quadrupole trap arrange in shell structures, a free motion in radial direction is disabled, and ions can only move to neighboring shells when their kinetic energy is high enough to overcome a certain potential barrier. The simulations have shown that intershell diffusion rates in the considered ion crystals increase exponentially when the ion temperatures exceed values that well agree with the predictions of other established models. Ion ensembles of different ion numbers (300, 500, and 1000 138Ba+ ions) and symmetries (prolate and spherical) have been investigated showing a clear tendency for the phase transition temperatures: The higher the ion number, the lower is the transition temperature.
Photoionization of a cold atomic sample offers intriguing possibilities for observing collective effects at extremely low temperatures. Irradiation of a rubidium condensate and of cold rubidium atoms within a magneto-optical trap (MOT) with laser pulses ionizing through one-photon and two-photon absorption processes was performed. Losses and modifications in the density profile of the remaining trapped cold cloud or the remaining condensate sample were examined as functions of the ionizing laser parameters. Ionization cross sections were measured for atoms in a MOT, while in magnetic traps losses larger than those expected for ionization process were measured.