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arXiv:2201.06979

Raman mass-spectrometry via oscillatory motion in deep pulsed optical lattices

Alexandros Gerakis, Mikhail N. Shneider, P. F. Barker

Published Jan 18, 2022• 0 citations
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Abstract

We describe a new optical diagnostic for determining the composition of gases by measuring the motion of atoms and molecules trapped within very deep optical lattices. This non-resonant method is analogous to conventional Raman scattering, except that the observed spectral features relate to the oscillatory center-of-mass motion of each species within the lattice, determined uniquely by their respective polarizability-to-mass ratio. Depending on the density of the probed sample, detection occurs either via optical scattering at the high end or via non-resonant ionization at the lower end. We show that such a technique is complementary to conventional mass spectrometry techniques and envision its implementation in existing instruments.

DOI
10.48550/arxiv.2201.06979

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We describe a new optical diagnostic for determining the composition of gases by measuring the motion of atoms and molecules trapped within very deep optical lattices. This non-resonant method is analogous to conventional Raman scattering, except that the observed spectral features relate to the oscillatory center-of-mass motion of each species within the lattice, determined uniquely by their respective polarizability-to-mass ratio. Depending on the density of the probed sample, detection occurs either via optical scattering at the high end or via non-resonant ionization at the lower end. We show that such a technique is complementary to conventional mass spectrometry techniques and envision its implementation in existing instruments.
We describe a new optical diagnostic for determining the composition of gases by measuring the motion of atoms and molecules trapped within very deep optical lattices. This non-resonant method is analogous to conventional Raman scattering, except that the observed spectral features relate to the oscillatory center-of-mass motion of each species within the lattice, determined uniquely by their respective polarizability-to-mass ratio. Depending on the density of the probed sample, detection occurs either via optical scattering at the high end or via non-resonant ionization at the lower end. We show that such a technique is complementary to conventional mass spectrometry techniques and envision its implementation in existing instruments.
We study the spectral profile of Rayleigh scattered light from molecular species trapped in optical lattices created by strong fields in the ${10}^{16}\text{ }\text{W}\text{ }{\text{m}}^{\ensuremath{-}2}$ range. We show that, for lattices with well depths on the order of 100 K, the motional sidebands imparted on spectra are shifted from the central Dicke-narrowed Rayleigh peak by hundreds of MHz. Our calculations for these short duration (30 ns) lattices show that these spectral features appear even in room temperature gases suggesting a new technique for measuring gas composition based on the frequency offset of the sidebands. Finally, we study the role of field-induced molecular alignment within the lattice and calculate its effect on the shape and position of the sidebands.
We investigate the dynamics of untrapped molecules within a far-off resonant accelerating optical lattice. Our analysis shows that untrapped molecules can be temporarily transported by the lattice, and those that are transported for the longest time reach a unique, well-defined critical velocity that depends on the mass to polarizability ratio of the molecular species. We show that this species-dependent critical velocity leads to a velocity dispersion for different species within a gas mixture. Our numerical simulations show that the velocity distribution of a multicomponent gas evolves to form well-separated peaks in velocity space for each species. We propose a time-of-flight analysis technique that transforms the velocity dispersion to a temporal separation of different species, even for small differences in the mass to polarizability ratio. Separation utilizing this concept is demonstrated for atmospheric species and isotopes of nitrogen. Finally, we present an extension of this concept for both temporal and angular dispersion.
Abstract Precise measurement of the particle number, spatial distribution and internal state is fundamental to all proposed experiments with ultracold molecules both in bulk gases and optical lattices. Here, we demonstrate in-situ detection of individual molecules in a bulk sample of 87 Rb 133 Cs molecules. Extending techniques from atomic quantum gas microscopy, we pin the molecules in a deep two-dimensional optical lattice and, following dissociation, collect fluorescence from the constituent atoms using a high-numerical-aperture objective. This enables detection of individual molecules up to the resolution of the sub-micron lattice spacing. Our approach provides direct access to the density distribution of small samples of molecules, allowing us to obtain precise measurements of density-dependent collisional losses. Further, by mapping two internal states of the molecule to different atomic species, we demonstrate simultaneous detection of the position and rotational state of individual molecules. Finally, we implement local addressing of the sample using a focused beam to induce a spatially-dependent light shift on the rotational transitions of the molecules.
It has recently been demonstrated that quantum degenerate gases of very weakly bound molecules can be produced by atomic gases with Feshbach resonances. More strongly bound molecules can be produced with Raman photoassociation of a quantum gas, although this process has not yet been shown to produce a quantum degenerate molecular gas. In principle, Feshbach resonance and Raman photoassociation can be quantum-mechanically reversible, and lead to collective coherent phenomena such as Rabi cycling between an atomic and a molecular gas. However, such atom-molecular coherence has only partly been realized experimentally. Effects that may limit coherence include thermalizing elastic collisions, inelastic collisions, spontaneous Raman scattering, and pairing field formation. Here, we demonstrate a method that circumvents these limitations, based on Raman photoassociation of atoms in an optical lattice and driven into a Mott insulator state. We find that the Raman photoassociation transition is resolved into discrete lines corresponding to the quantized lattice site occupancies, and demonstrate that this provides a new method to accurately determine the distribution of site occupancies and the atom-molecule scattering length. Furthermore, we observe a Raman-induced oscillation of the central core of the gas, containing about 30% of the atoms, between an atomic and a molecular gas.
We form a 1D optical lattices for Cs atoms using light tuned a few thousand linewidths below the 6S1/2(F equals 4) yields 6P3/2(F' equals 5) transition at 852 nm. In this far-off- resonance lattice the time scale for damping of motional coherences and kinetic energy can be orders of magnitude longer than the vibrational oscillation period for atoms trapped in the lattice potential wells. Atoms are loaded directly into deeply bound states, by adiabatic transfer from a superimposed, near-resonance optical lattice. This yields a mean vibrational excitation n approximately equals 0.3, and localization (Delta) z approximately (lambda) /20 deep in the Lamb-Dicke regime. Light scattering subsequently heats the atoms, but the initial rate is only of order 10-3 vibrational quanta per oscillation period. Low vibrational excitation, localization in the Lamb-Dicke regime and low heating rates make these atoms good candidates for resolved- sideband Raman cooling, and for the generation and study of non-classical states of center-of-mass motion. We propose a scheme for resolved-sideband Raman cooling and quantum state preparation; the scheme employs Raman coupling between magnetic sublevels induced by the lattice light field itself.