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Bulletin of the American Physical Society

Multi-photon two-color ionization of atoms and ions by femtosecond pulses.

Nicolas Douguet, Joel Venzke, Klaus Bartschat, Alexei N. Grum-Grzhimailo, Грызлова Елена Владимировна, Ekaterina I. Staroselskaya

Published May 25, 2016• 0 citations
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One- and two-color resonance-enhanced two-photon ionization (RETPI) is used to detect ultracold ground-state RbCs molecules which are formed via short-range photoassociation from laser-cooled atoms. The transition from the X1Σ+(v = 0) state to the 21Π(v = 10) state of ultracold RbCs molecules shows the consistence of one- and two-color RETPI. A multi-photon photoionization rate model is introduced to interpret the dependence of molecular ion intensity on photoionized laser energy, and can be used to verify the photoionization scheme. This photoionization rate model can be expanded to multi-color photoionization for all kinds of atoms and molecules, which is a powerful method of determining the photoionization scheme.
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.
Two-photon ionization of atomic helium has been measured by combining femtosecond extreme-ultraviolet pulses from the free-electron laser in Hamburg (FLASH at DESY) with intense light pulses from a synchronized neodymium-doped yttrium lithium fluoride laser. Sidebands appear in the photoelectron spectra when the two laser pulses overlap in both space and time. Their intensity exhibits a characteristic dependence on the relative time delay between the ionizing and the dressing pulses and provides an inherent time marker for time-resolved pump-probe experiments. The measurements of the sidebands are in good agreement with theoretical predictions and allow for a direct analysis of two-photon ionization, free from processes related to interference between multiple quantum paths.