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The d 3 state of LiRb

Ian Stevenson, David Blasing, Adeel Altaf, Y. P. Chen, Daniel S. Elliott

Published Jan 1, 2016• 1 citation
OpenAlex

Abstract

We report our spectroscopic studies of the $d ^3\Pi$ state of ultra-cold $^7$Li$^{85}$Rb using resonantly-enhanced multi-photon ionization and depletion spectroscopy with bound-to-bound transitions originating from the metastable $a ^3\Sigma^+$ state. We evaluate the potential of this state for use as the intermediate state in a STIRAP transfer scheme from triplet Feshbach LiRb molecules to the $X ^1\Sigma^+$ ground state, and find that the lowest several vibrational levels possess the requisite overlap with initial and final states, as well as convenient energies. Using depletion measurements, we measured the well depth and spin-orbit splitting. We suggest possible pathways for short-range photoassociation using deeply-bound vibrational levels of this electronic state.

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Short-range photoassociation of LiRb

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We have observed short-range photoassociation of $^{7}\mathrm{Li}^{85}\mathrm{Rb}$ to the two lowest vibrational states of the $d{\phantom{\rule{0.16em}{0ex}}}^{3}\mathrm{\ensuremath{\Pi}}$ potential. We have also observed several ${a}^{3}\phantom{\rule{0.16em}{0ex}}{\mathrm{\ensuremath{\Sigma}}}^{+}$ vibrational levels with generation rates between $\ensuremath{\sim}{10}^{2}$ and $\ensuremath{\sim}{10}^{3}$ molecules per second, resulting from the spontaneous decay of these $d{\phantom{\rule{0.16em}{0ex}}}^{3}\mathrm{\ensuremath{\Pi}}$ molecules. We observe an alternation of the peak heights in the rotational photoassociation spectrum that depends on the parity of the excited molecular state. Franck-Condon overlap calculations predict that photoassociation to higher vibrational levels of the $d{\phantom{\rule{0.16em}{0ex}}}^{3}\mathrm{\ensuremath{\Pi}}$ potential, in particular, the sixth vibrational level, should populate the lowest vibrational level of the $a{\phantom{\rule{0.16em}{0ex}}}^{3}{\mathrm{\ensuremath{\Sigma}}}^{+}$ state at a rate as high as ${10}^{4}$ molecules per second. This work also motivates an experimental search for short-range photoassociation to other bound molecular states, such as $c{\phantom{\rule{0.16em}{0ex}}}^{3}{\mathrm{\ensuremath{\Sigma}}}^{+}$ or $b{\phantom{\rule{0.16em}{0ex}}}^{3}\mathrm{\ensuremath{\Pi}}$, as prospects for preparing ground-state molecules.

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We report our spectroscopic studies of the d3Πd ^3\Pid3Π state of ultra-cold 7^77Li85^{85}85Rb using resonantly-enhanced multi-photon ionization and depletion spectroscopy with bound-to-bound transitions originating from the metastable a3Σ+a ^3\Sigma^+a3Σ+ state. We evaluate the potential of this state for use as the intermediate state in a STIRAP transfer scheme from triplet Feshbach LiRb molecules to the X1Σ+X ^1\Sigma^+X1Σ+ ground state, and find that the lowest several vibrational levels possess the requisite overlap with initial and final states, as well as convenient energies. Using depletion measurements, we measured the well depth and spin-orbit splitting. We suggest possible pathways for short-range photoassociation using deeply-bound vibrational levels of this electronic state.
We report our spectroscopic studies of the d 3Π state of ultra-cold 7Li85Rb using resonantly enhanced multi-photon ionization and depletion spectroscopy with bound-to-bound transitions originating from the metastable a 3Σ+ state. We evaluate the potential of this state for use as the intermediate state in a stimulated-Raman-adiabatic-passage transfer scheme from triplet Feshbach LiRb molecules to the X 1Σ+ ground state and find that the lowest several vibrational levels possess the requisite overlap with initial and final states, as well as convenient energies. Using depletion measurements, we measured the well depth and spin-orbit splitting. We suggest possible pathways for short-range photoassociation using deeply bound vibrational levels of this electronic state.
We report the formation of ultracold (7)Li(85)Rb molecules in the a(3)Σ(+) electronic state by photoassociation (PA) and their detection via resonantly enhanced multiphoton ionization (REMPI). With our dual-species Li and Rb magneto-optical trap apparatus, we detect PA resonances with binding energies up to ∼62 cm(-1) below the (7)Li 2s (2)S1/2 + (85)Rb 5p (2)P1/2 asymptote. In addition, we use REMPI spectroscopy to probe the a(3)Σ(+) state and excited electronic 3(3)Π and 4(3)Σ(+) states and identify a(3)Σ(+) (v″ = 7-13), 3(3)Π (vΠ' = 0-10), and 4(3)Σ(+) (vΣ' = 0-5) vibrational levels. Our line assignments agree well with ab initio calculations. These preliminary spectroscopic studies on previously unobserved electronic states are crucial to discovering transition pathways for transferring ultracold LiRb molecules created via PA to deeply bound rovibrational levels of the electronic ground state.
We present spectroscopic studies of ultracold LiRb molecules using ionization detection. The molecules are created by cooling and trapping Li and Rb atoms in overlapping magneto-optical traps (MOTs) and using light resonant with a free-bound transition to create weakly bound excited state molecules in a process known as photoassociation (PA). We explore weakly bound vibrational levels of LiRb with PA spectroscopy using ionization detection and, where possible, compare our results with earlier measurements performed in our lab using trap-loss spectroscopy. In addition, we also probe vibrational levels of the ground triplet electronic state and excited electronic states using resonantly enhanced multiphoton ionization (REMPI) spectroscopy. We identify several vibrational levels of the α3Σ+, (3)3ΠΩ and (4)3Σ + states and compare our observations with theoretical calculations. As LiRb is one of the least studied heteronuclear diatomic molecules, these studies are aimed towards exploring the molecular structure. The spectroscopic work is also in line with the long-term project goals of transferring ultracold LiRb molecules into the lowest rotational and vibrational levels of the ground singlet electronic state. Molecules in this rovibronic ground state possess a large electric dipole moment, which is essential for application of ultracold molecules in various quantum computation schemes. The rovibronic ground state will also be an ideal starting point for investigating molecular entangled states.
We present spectra of ultracold 7Li85Rb^{7}\mathrm{Li}^{85}\mathrm{Rb}7Li85Rb molecules in their electronic ground state formed by spontaneous decay of weakly bound photoassociated molecules. Beginning with atoms in a dual-species magneto-optical trap, weakly bound molecules are formed in the 4(1) electronic state, which corresponds to the ${B}^{1}\ensuremath{\Pi}$ state at short range. These molecules spontaneously decay to the electronic ground state and we use resonantly enhanced multiphoton ionization to determine the vibrational population distribution in the electronic ground states after spontaneous emission. Many of the observed lines from the spectra are consistent with transitions from the ${X}^{1}{\ensuremath{\Sigma}}^{+}$ ground electronic state to either the ${B}^{1}\ensuremath{\Pi}$ or the ${D}^{1}\ensuremath{\Pi}$ electronic state that has been previously observed, with levels possibly as low as ${X}^{1}{\ensuremath{\Sigma}}^{+}({v}^{\ensuremath{'}\ensuremath{'}}=2)$ being populated. We do not observe decay to weakly bound vibrational levels of the ${X}^{1}{\ensuremath{\Sigma}}^{+}$ or ${a}^{3}{\ensuremath{\Sigma}}^{+}$ electronic state in the spectra. We also deduce a lower bound of $3900 \mathrm{cm}{}^{\ensuremath{-}1}$ for the dissociation energy of the LiRb+\mathrm{LiRb}{}^{+}LiRb+ molecular ion.
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.
We have observed short-range photoassociation of 7Li85Rb^{7}\mathrm{Li}^{85}\mathrm{Rb}7Li85Rb to the two lowest vibrational states of the $d{\phantom{\rule{0.16em}{0ex}}}^{3}\mathrm{\ensuremath{\Pi}}$ potential. We have also observed several ${a}^{3}\phantom{\rule{0.16em}{0ex}}{\mathrm{\ensuremath{\Sigma}}}^{+}$ vibrational levels with generation rates between $\ensuremath{\sim}{10}^{2}$ and $\ensuremath{\sim}{10}^{3}$ molecules per second, resulting from the spontaneous decay of these $d{\phantom{\rule{0.16em}{0ex}}}^{3}\mathrm{\ensuremath{\Pi}}$ molecules. We observe an alternation of the peak heights in the rotational photoassociation spectrum that depends on the parity of the excited molecular state. Franck-Condon overlap calculations predict that photoassociation to higher vibrational levels of the $d{\phantom{\rule{0.16em}{0ex}}}^{3}\mathrm{\ensuremath{\Pi}}$ potential, in particular, the sixth vibrational level, should populate the lowest vibrational level of the $a{\phantom{\rule{0.16em}{0ex}}}^{3}{\mathrm{\ensuremath{\Sigma}}}^{+}$ state at a rate as high as 104{10}^{4}104 molecules per second. This work also motivates an experimental search for short-range photoassociation to other bound molecular states, such as $c{\phantom{\rule{0.16em}{0ex}}}^{3}{\mathrm{\ensuremath{\Sigma}}}^{+}$ or $b{\phantom{\rule{0.16em}{0ex}}}^{3}\mathrm{\ensuremath{\Pi}}$, as prospects for preparing ground-state molecules.