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Advances in atomic, molecular, and optical physics

Studies of electron-excited targets using recoil momentum spectroscopy with laser probing of the excited state

Andrew James Murray, P. R. Hammond

Published Jan 1, 2001• 3 citations
Publisher
DOI
10.1016/s1049-250x(01)80057-4

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An experimental continuous-wave (cw) pump-probe scheme is demonstrated by investigating the population and photoionization dynamics of an atomic system. In particular, 6Li atoms are initially prepared in optically pumped 22S1/2 and 22P3/2 states before being excited via multi-photon absorption from a tunable femtosecond laser. The subsequent cascade back to the ground state is analyzed by ionizing the atoms in the field of a cw optical dipole trap laser. Conventional spectroscopic methods, such as standard cold-target recoil ion momentum spectroscopy or velocity map imaging, cannot provide simultaneous momentum and time-resolved information on an event-by-event basis for the system investigated here. The new approach overcomes this limitation by leveraging electron-recoil ion coincidences, momentum conservation, and the cyclotron motion of the photoelectron in the magnetic spectrometer field. This enables the reconstruction of ionization times and time-of-flight of the charged target fragments with nanosecond resolution. As a result, not only can three-dimensional photoelectron momentum vectors be determined, but the (incoherent) population dynamics of the atomic system also become accessible. Future applications exploring coherent atomic dynamics on the nanosecond timescale would not only expand the scope of time-resolved spectroscopy but can also aid in developing coherent control schemes for precise atomic manipulation.
An experimental continuous-wave (cw) pump-probe scheme is demonstrated by investigating the population and photoionization dynamics of an atomic system. Specifically, 6^66Li atoms are initially prepared in optically pumped 22S1/22^{2}S_{1/2}22S1/2​ and 22P3/22^{2}P_{3/2}22P3/2​ states before being excited via multi-photon absorption from a tunable femtosecond laser. The subsequent cascade back to the ground state is analyzed by ionizing the atoms in the field of a cw optical dipole trap laser. Conventional spectroscopic methods such as standard cold-target recoil-ion momentum spectroscopy (COLTRIMS) or velocity map imaging (VMI) cannot provide simultaneous momentum and time-resolved information on an event-by-event basis for the system investigated here. The new approach overcomes this limitation by leveraging electron-recoil ion coincidences, momentum conservation, and the cyclotron motion of the photoelectron in the magnetic spectrometer field. This enables the reconstruction of ionization times and time-of-flight of the charged target fragments with nanosecond resolution. As a result, not only can three-dimensional photoelectron momentum vectors be determined, but the (incoherent) population dynamics of the atomic system also become accessible. Future applications exploring coherent atomic dynamics on the nanosecond timescale would not only expand the scope of time-resolved spectroscopy but can also aid in developing coherent control schemes for precise atomic manipulation.
Resolution plays a vital role in spectroscopic studies. In the usual recoil-ion momentum spectroscopy (RIMS), Q-value resolution is relied upon to distinguish between different collision channels: The better the Q-value resolution, the better one is able to resolve energetically similar channels. Although traditional COLTRIMS greatly improves Q-value resolution by cooling the target and thus greatly reducing the initial target momentum spread, the resolution of the technique is still limited by target temperature. However, with the recent development in RIMS, namely, magneto-optical trap recoil ion momentum spectroscopy (MOTRIMS) superior recoil ion momentum resolution as well as charge transfer measurements with laser excited targets have become possible. Through MOTRIMS, methods for the measurements of target excited state fraction and kinematically complete relative charge transfer cross sections have been developed, even for some systems having energetically degenerate or nearly degenerate channels. In the present work, the systems of interest having energy degeneracies or near degeneracies are Rb+{\mathrm{Rb}}^{+}Rb+, K+{\mathrm{K}}^{+}K+, and Li+{\mathrm{Li}}^{+}Li+ colliding with trapped Rb(5l)\mathrm{Rb}(5l)Rb(5l), where l=sl=sl=s and ppp.