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Kinematically complete multiphoton ionization studies on optically trapped 6Li and 6Li_2 created by single-color photoassociation

Niels Kurz

Published Jan 1, 2021• 0 citations
Publisher

Abstract

In this work, a reaction microscope with a magneto-optical trap for 6Li atoms, was extended by an optical dipole trap in order to be able to investigate in detail laser-induced atomic and molecular ionization dynamics in a cold quantum gas. \nThe optical dipole trap was operated at a full trap depth of 2.3 mK for 6Li atoms and about \n1% of the atoms in the MOT could be transferred into the dipole trap, with 1/e storage times \nexceeding 5 s. The optically trapped ensemble of 6Li atoms was used as a target for ionisation with intensive and broadband femtosecond laser pulses (λ = 750−820 nm, P = 10^11−10^14 W/cm2, Δt = 30 fs) and allowed to perform kinematically complete experiments, in which 6Li+ ions \nas well as photoelectrons were measured coincidentically. \nAs a first application, in this work, a series of association- and ionization mechanisms, which \nled to production of molecular 6Li2+ ions, were investigated with trapped lithium atoms. \nIn photoassociative ionization, two atoms collide, which were previously lifted into the asymptotic 2p − 3s potential energy curve by ladder excitation. During the collision the atoms autoionize into the 12Σg+(6Li2+) groundstate of the molecular ion, since these two potential energy curves exhibit an avoided crossing. This process was observed when magneto-optically trapped atoms were illuminated with the femtosecond laser. \nIn the dipole trap, using single-color photoassociation, excited state molecules were produced \nin high-lying vibrational states 11Σg+(ν = 65) and 13Σg+(v = 57) and spectroscopically investigated. A fraction of the excited state molecules decay via fluorescence into the molecular ground state. The 11Σg+(ν = 38)(6Li2) ground state molecules created via the singlet res- \nonance 11Σu+(ν = 65)(Li∗2) were detected via direct 3 photon ionisation. The momentum spectra show very low kinetic energies for the photo electrons of below 100 meV. Therefore \nin the molecular ion only vibrational states of Li2+ are getting populated, which are directly below the 3-photon transition energy. \nFinally, a stepwise ionization mechanism was identified, which leads into the continuum via \nan intermediate molecular state of 6Li2∗ after photoassociation. The starting point is a pho- \ntoassociated excited state molecule 11Σu+(ν = 65)(6Li∗2), which absorbs two photons of the dipole trap laser (λ = 1070 nm ± 2 nm). This happens via an intermediate molecular state \n31Σg+(2s + 3s), after which it leads into the 12Σg+(6Li2+) potential.

DOI
10.11588/heidok.00029072

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In this work, a reaction microscope with a magneto-optical trap for 6Li atoms, was extended by an optical dipole trap in order to be able to investigate in detail laser-induced atomic and molecular ionization dynamics in a cold quantum gas. \nThe optical dipole trap was operated at a full trap depth of 2.3 mK for 6Li atoms and about \n1% of the atoms in the MOT could be transferred into the dipole trap, with 1/e storage times \nexceeding 5 s. The optically trapped ensemble of 6Li atoms was used as a target for ionisation with intensive and broadband femtosecond laser pulses (λ = 750−820 nm, P = 10^11−10^14 W/cm2, Δt = 30 fs) and allowed to perform kinematically complete experiments, in which 6Li+ ions \nas well as photoelectrons were measured coincidentically. \nAs a first application, in this work, a series of association- and ionization mechanisms, which \nled to production of molecular 6Li2+ ions, were investigated with trapped lithium atoms. \nIn photoassociative ionization, two atoms collide, which were previously lifted into the asymptotic 2p − 3s potential energy curve by ladder excitation. During the collision the atoms autoionize into the 12Σg+(6Li2+) groundstate of the molecular ion, since these two potential energy curves exhibit an avoided crossing. This process was observed when magneto-optically trapped atoms were illuminated with the femtosecond laser. \nIn the dipole trap, using single-color photoassociation, excited state molecules were produced \nin high-lying vibrational states 11Σg+(ν = 65) and 13Σg+(v = 57) and spectroscopically investigated. A fraction of the excited state molecules decay via fluorescence into the molecular ground state. The 11Σg+(ν = 38)(6Li2) ground state molecules created via the singlet res- \nonance 11Σu+(ν = 65)(Li∗2) were detected via direct 3 photon ionisation. The momentum spectra show very low kinetic energies for the photo electrons of below 100 meV. Therefore \nin the molecular ion only vibrational states of Li2+ are getting populated, which are directly below the 3-photon transition energy. \nFinally, a stepwise ionization mechanism was identified, which leads into the continuum via \nan intermediate molecular state of 6Li2∗ after photoassociation. The starting point is a pho- \ntoassociated excited state molecule 11Σu+(ν = 65)(6Li∗2), which absorbs two photons of the dipole trap laser (λ = 1070 nm ± 2 nm). This happens via an intermediate molecular state \n31Σg+(2s + 3s), after which it leads into the 12Σg+(6Li2+) potential.
We report on the implementation of a far-off-resonant, optical dipole force trap in a reaction microscope combined with a magneto-optical trap. Kinematically complete multi-photon ionization experiments were performed on optically trapped 6Li atoms and photo-associated 6Li2 molecules in their highest vibrational state. The apparatus allows us to distinguish different ionization mechanisms related to the presence of the IR field of the optical dipole trap that can occur during ionization of 6Li and 6Li2 in strong fields. In a series of proof-of-principle experiments, we detect weakly bound dimers via three-photon ionization with femtosecond pulses (τ = 30 fs) at a central wavelength of 780 nm and measure directly the momenta of the photoelectrons in coincidence with recoil ions.
Synopsis We report on performing high resolution recoil ion momentum spectroscopy in a reaction microscope (ReMi) on a target of dipole-force trapped cold 6Li atoms in a non-interacting |1〉-|2〉 spin mixture and coincident detection of recoil ions and photoelectrons. Photo-ionization occurs from the electronic ground state of the 6Li atoms and IR photons significantly contribute to the ion yield via 3-photon resonances. High resolution time-of-flight spectra are obtained by modulating the trap depth synced with the arrival of the fs laser pulses.
We present the results of a spectroscopic study LiRb molecules created via photoassociation (PA) to vibration levels of the 4(1) potential. Atoms are first cooled and trapped in a dual species 7Li/ 85Rb magneto-optical trap (MOT) at temperatures of ≈ 1 mK or less. In a cold sample of sufficient density, PA occurs when a resonant laser field induces a free-bound transition to create molecules in an excited electronic potential. After spontaneous emission the molecules decay to a mixture of free atoms and bound molecules depending on the Franck-Condon factors (FCFs) of the excited and ground state vibrational wavefunctions. While excited LiRb * has been previously detected by trap loss fluorescence detection, ionization spectroscopy is required to determine the population of ground state levels after decay. We detect ground state molecules via resonantly enhanced multiphoton ionization (REMPI) where a two photon ionization transition is enhanced by an intermediate resonance. The intermediate resonances match progressions from the D1Π and possibly B1&Pgr; potentials, many of which have known energies obtained from previous heat pipe experiments. This is contrary to the expectation that weakly bound LiRb * should primarily decay to weakly bound levels of the ground state and could point to a possible path for creating molecules in the rovibronic ground state.
Reaction microscopes enable kinematically complete measurements of atomic and molecular fragmentation. An ultracold atomic target is usually provided by a supersonic gas jet. The apparatus developed in the course of this thesis for the first time combines the principle of the reaction microscope with a magneto-optical trap. This allows for the preparation of lithium atoms in the sub-mK range. Being a three-electron system, its simple atomic structure makes lithium a model system of great topical interest for all kinds of ionization reactions. In order not to deteriorate the determination of the momenta of the charged fragments by the magnetic field of the trap, a pulsed mode of operation is adopted, creating field-free conditions during data acquisition and making efficient use of the stored target. The novel apparatus provides a versatile target for investigations on fragmentation of lithium by electron, ion and photon impact. For the first time, momentum-resolved measurements on multiphoton ionization in intense laser fields with pulse durations of 25~fs and peak intensities in the range between 1011^{11}11~W/cm2^22 and 1016^{16}16~W/cm2^22 were performed. The acquired photoelectron spectra exhibit unexpected structures such as a preferred emission in the direction perpendicular to the laser polarization axis, which are not fully understood yet. Presently, corresponding calculations are being done in several theory groups.
This thesis describes the production of molecular Bose-Einstein condensates (BEC) of 6Li2 dimers and binding energy measurements of p-wave Feshbach molecules. A σ− Zeeman slower is used to produce a continuous beam of isotopically enriched 6Li atoms at speeds low enough to load a magneto-optical trap (MOT). We currently have a flux of slowed atoms of ~ 5 · 106 atoms/s loading the MOT with more than 108 atoms. We then transfer up to 106 atoms in an almost equal spin mixture of the two lowest hyperfine states into an optical dipole trap. We achieved condensates in three different crossed optical dipole trap geometries. The initial low power optical dipole trap was formed using light from a 25WVersaDisk Yb:YAG laser at 1030 nm. It consisted of a 15 W beam crossed with a 13 W beam at about 80 degrees with a waist of approximately 30 μm in each beam. By translating the focus of the second beam we could change the trap geometry from near symmetric to elongated. Nowadays, we produce condensates in a crossed dipole trap formed by a 100 W fibre laser. Both arms are focussed to a waist of 40 μm, cross each other at 14 degrees and have laser powers of ~80 W and ~70 W, respectively. Evaporative cooling is achieved by reducing the laser power near the broad s-wave Feshbach resonance at 834 G. By tuning to the low magnetic field side (770 G) of the Feshbach resonance molecules are formed through three-body recombination at sufficiently low temperatures. Further evaporation leads to the creation of a molecular BEC. After reducing the laser power by a factor of about 1000 in approximately 3 s we have observed more than 30 000 condensed molecules. During the evaporation the temperature decreases from about 100 μK to below 100 nK. We present measurements of the binding energies of 6Li p-wave Feshbach molecules formed in combinations of the |F = 1/2,mF = +1/2i (|1i) and |F = 1/2,mF = −1/2i (|2i) states. The binding energies scale linearly with magnetic field detuning for all three resonances. The relative molecular magnetic moments are found to be 113 ± 7 μK/G, 111 ± 6 μK/G and 118 ± 8 μK/G for the |1i − |1i, |1i − |2i and |2i − |2i resonances, respectively, in good agreement with theoretical predictions.
For this Master thesis, multiphoton ionisation processes of Lithium-6 atoms from an optical dipole trap have been investigated and the momentum distributions of the resulting ions over the whole solid angle in a Reaction Microscope have been obtained for the first time. The atoms have first been trapped in a magneto-optical trap, before being transferred into the purely optical dipole trap. Measurements for five different peak intensities in the range of 6:5 x 1013 W=cm2 to 6:5 x 1014 W=cm2 have been carried out, where a femtosecond laser has been used as the projectile beam. The experimentally obtained momentum distributions are consistent with formerly executed comparable experiments and offer a basis for future experiments.