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Review of Scientific Instruments

Reaction microscope for investigating ionization dynamics of weakly bound alkali dimers

Nathan Kurz, D. Fischer, Thomas Pfeifer, Alexander Dorn

Published Dec 1, 2021• 4 citations
Publisher

Abstract

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.

DOI
10.1063/5.0069506

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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.
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.
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.
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.
We developed a magneto-optical trap reaction microscope (MOTREMI) for strontium atoms by combining multiparticle coincident detection with the laser cooling technique. The present compact injection system enables the production of cold Sr atoms in three modes of two-dimensional (2D) magneto-optical trap (MOT) beam, molasses, and three-dimensional (3D) MOT, providing adjustable densities and ratios of the ground state 5s25{s}^{2}5s2 (1S0^{1}S_{0}1S0​) and the excited states 5s5p1P15s5p{\phantom{\rule{4pt}{0ex}}}^{1}{P}_{1}5s5p1P1​ and 3PJ^{3}P_{J}3PJ​. The target profiles including temperature, density, and size of the 3D MOT as well as the 2D MOT beam cold atomic flux were characterized in detail. Using the present setup, we investigate the single photoionization of Sr atoms with molasses through few-photons absorption in 800 nm, where Sr+{\mathrm{Sr}}^{+}Sr+ and ${e}^{\ensuremath{-}}$ are detected in coincidence and most of the ionization channels are identified. The momentum resolution for coincident Sr+{\mathrm{Sr}}^{+}Sr+ and ${e}^{\ensuremath{-}}$ along time-of-flight direction are achieved up to 0.12 a.u. and 0.02 a.u., respectively. The spectra of photoelectron ionized from the ground state as well as several excited states show distinct structures manifesting prominent contributions from multiphoton absorption. Detecting complete vector momenta of electrons and recoil ions in coincidence paves a way for further investigation of two-electron correlation dynamics and multielectron effects with alkaline-earth atoms.
A reaction microscope (ReMi) has been combined with a magneto-optical trap (MOT) for the kinematically complete investigation of atomic break-up processes. With the novel MOTReMi apparatus, the momentum vectors of the fragments of laser-cooled and state-prepared lithium atoms are measured in coincidence and over the full solid angle. The first successful implementation of a MOTReMi could be realized due to an optimized design of the present setup, a nonstandard operation of the MOT, and by employing a switching cycle with alternating measuring and trapping periods. The very low target temperature in the MOT (∼2 mK) allows for an excellent momentum resolution. Optical preparation of the target atoms in the excited Li 2(2)P3/2 state was demonstrated providing an atomic polarization of close to 100%. While first experimental results were reported earlier, in this work, we focus on the technical description of the setup and its performance in commissioning experiments involving target ionization in 266 nm laser pulses and in collisions with projectile ions.
Photoionization induced by trapping and auxiliary laser fields is an inherent feature of many laser-cooling and optical trapping experiments, yet its microscopic dynamics are rarely investigated directly. In this work, we employ a reaction microscope implementing an event-by-event photoionization time retrieval technique to extend momentum-resolved photoelectron spectroscopy to continuous-wave laser--atom interactions. We investigate low-intensity multicolor photoionization of laser-cooled lithium atoms confined in an all-optical trap. Complete three-dimensional electron momentum distributions and kinetic-energy spectra recorded for different laser wavelengths and polarization configurations identify resonant excitation of the 5p5p5p and 5f5f5f states and reveal an additional ionization channel following spontaneous decay from the 5f5f5f to the 4d4d4d state. A pronounced polarization dependence of the photoionization yield is explained by magnetic-sublevel selection rules and the coherent interference of different virtual excitation pathways. These results demonstrate that reaction microscopy combined with event-by-event time reconstruction provides a powerful approach for investigating microscopic electronic dynamics in laser-cooled atomic systems and offers new insight into photoionization processes occurring during optical trapping.