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ChemPhysChem

Production of RbCs Molecules in the Rovibronic Ground State via Short‐Range Photoassociation to the 2 1Π1, 2 3Π1, and 3 3Σ States

Toshihiko Shimasaki, Jin‐Tae Kim, David P. DeMille

Published Oct 20, 2016• 11 citations
Publisher

Abstract

Abstract We report the production of ultracold 85Rb133Cs molecules in their rovibronic ground state X 1Σ+ (v=0; J=0), by short‐range photoassociation (PA) to the 2 1Π1, 2 3Π1, and 3 3Σ states. In the PA frequency range from 11650 to 12150 cm−1 (corresponding to energy levels 15500–16000 cm−1 above the bottom of the X potential), we have observed 40 sets of new PA lines. For selected PA states, we investigate vibrational branching, rotational branching, and saturation behavior. Among these 40 new PA lines, the 3 3Σ (v=3) state has the highest molecule production rate of 2 x 103 molecules s−1 into the rovibronic ground state.

DOI
10.1002/cphc.201600933

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Abstract We report the production of ultracold 85Rb133Cs molecules in their rovibronic ground state X 1Σ+ (v=0; J=0), by short‐range photoassociation (PA) to the 2 1Π1, 2 3Π1, and 3 3Σ states. In the PA frequency range from 11650 to 12150 cm−1 (corresponding to energy levels 15500–16000 cm−1 above the bottom of the X potential), we have observed 40 sets of new PA lines. For selected PA states, we investigate vibrational branching, rotational branching, and saturation behavior. Among these 40 new PA lines, the 3 3Σ (v=3) state has the highest molecule production rate of 2 x 103 molecules s−1 into the rovibronic ground state.
We investigate the production of cold 85Rb133Cs molecules in the lowest vibronic level of the ground electronic state via the B1Π1 short-range state. The photoassociation (PA) spectra of the B1Π1 state, including newly observed transition to 2 vibronic levels, are obtained by high sensitivity time-of-flight mass spectrometry. Based on these PA spectra, the harmonic and anharmonic constants of vibronic states are obtained, resulting in predicted vibronic energies with an uncertainty of 1–2 cm−1. The B1Π1 (v = 3) state is found to have the maximum production rate for ground-state molecules with a value of 3(1) × 104 s−1, which is 3 times larger than the value via the previously studied 23Π0+ (v = 10, J = 0) state with two-photon cascade decay. The populations of J = 0, 1, and 2 rotational levels of X1Σ+ (v = 0) state molecules formed via the B1Π1 (v = 3, J = 1) state are measured to be around 20%, 40%, and 20%. To quantify the coupling strength between the B1Π1 (v = 3) state and X1Σ+ (v = 0) state, the transition dipole moment between them is measured to be 7.2(2) × 10−3ea0, which is also 3 times larger than the value between the 23Π0+(v=10) state and X1Σ+ (v = 0) state, meaning the B1Π1 (v = 3) state has a stronger coupling with the X1Σ+ (v = 0) state. Our detailed measurements provide relevant parameters for investigation on direct stimulated Raman adiabatic passage transfer between the atomic scattering state and molecular bound state for 85Rb133Cs molecules.
We demonstrate the direct formation of vibronic ground state RbCs molecules by photoassociation of ultracold atoms followed by radiative stabilization. The photoassociation proceeds through deeply bound levels of the (2)3Π0+ state. From analysis of the relevant free-to-bound and bound-to-bound Franck–Condon factors, we have predicted and experimentally verified a set of photoassociation resonances that lead to efficient creation of molecules in the v = 0 vibrational level of the X1Σ+ electronic ground state. We also compare the observed and calculated laser intensity required to saturate the photoassociation rate. We discuss the prospects for using short-range photoassociation to create and accumulate samples of ultracold polar molecules in their rovibronic ground state.
Rovibronic levels of the mixed ${b}^{3}\phantom{\rule{0}{0ex}}{\mathrm{\ensuremath{\Pi}}}_{1}$-${c}^{3}\phantom{\rule{0}{0ex}}{\mathrm{\ensuremath{\Sigma}}}_{1}^{+}$-${B}^{1}\phantom{\rule{0}{0ex}}{\mathrm{\ensuremath{\Pi}}}_{1}$ states of RbCs molecules are experimentally investigated with photoassociation, where the strong singlet-triplet mixing in the states facilitates a rate of 104{10}^{4}104 s${}^{\ensuremath{-}1}$ for producing rovibronic-ground-state molecules.
We investigate the production of ultracold ground state X 1 σ + (v = 0) RbCs molecules in the lowest vibrational level via short-range photoassociation followed by spontaneous emission. The starting point is the laser cooled 85 Rb and 133 Cs atoms in a dual species, forced dark magneto-optical trap. The special intermediate level (5)0 + (v = 10) correlated to the (2) 3 π electric state is achieved by the photoassociation process. The formed ground state X 1 σ + (v = 0) molecule is resonantly excited to the 2 1 π intermediate state by a 651 nm pulse laser and is ionized by a 532 nm pulse laser and then detected by the time-of-flight mass spectrum. Saturation of the photoionization spectroscopy at large ionization laser energy is observed and the ionization efficiency is obtained from the fitting. The production of ultracold ground state 85 Rb 133 Cs molecules is facilitative for the further research about the manipulation of ultracold molecules in the rovibrational ground state.
We demonstrate the direct formation of vibronic ground state RbCs molecules by photoassociation of ultracold atoms followed by radiative stabilization.The photoassociation proceeds through deeply bound levels of the (2) 3 0 + state.From analysis of the relevant free-to-bound and bound-to-bound Franck-Condon factors, we have predicted and experimentally verified a set of photoassociation resonances that lead to efficient creation of molecules in the v = 0 vibrational level of the X 1 + electronic ground state.We also compare the observed and calculated laser intensity required to saturate the photoassociation rate.We discuss the prospects for using short-range photoassociation to create and accumulate samples of ultracold polar molecules in their rovibronic ground state.
We report the production of ultracold RbCs molecules in the rovibronic ground state, i.e., $X{\phantom{\rule{0.16em}{0ex}}}^{1}{\ensuremath{\Sigma}}^{+}(v=0,J=0)$, by short-range photoassociation to the $2{\phantom{\rule{0.16em}{0ex}}}^{3}{\ensuremath{\Pi}}_{0}$ state followed by spontaneous emission. We use narrow-band depletion spectroscopy to probe the distribution of rotational levels formed in the $X{\phantom{\rule{0.16em}{0ex}}}^{1}{\ensuremath{\Sigma}}^{+}(v=0)$ state. We conclude, based on selection rules, that the primary decay route to $X{\phantom{\rule{0.16em}{0ex}}}^{1}{\ensuremath{\Sigma}}^{+}(v=0)$ is a two-step cascade decay that leads to as much as 3333%33 branching into the J=0J=0J=0 rotational level. The experimental simplicity of our scheme opens up the possibility of easier access to the study and manipulation of ultracold heteronuclear molecules in the rovibronic ground state.