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arXiv:1605.08557 · Physical Review A

Measurement of the binding energy of ultracold Rb87Cs133 molecules using an offset-free optical frequency comb

Peter K. Molony, Avinash Kumar, Philip D. Gregory, Russell Kliese, Thomas Puppe, C. Ruth Le Sueur, J. Aldegunde, Jeremy M. Hutson, Simon L. Cornish

Published Aug 15, 2016• 19 citations
arXivHTMLPDF

Abstract

We report the binding energy of $^{87}\mathrm{Rb}^{133}\mathrm{Cs}$ molecules in their rovibrational ground state measured using an offset-free optical frequency comb based on difference frequency generation technology. We create molecules in the absolute ground state using stimulated Raman adiabatic passage (STIRAP) with a transfer efficiency of 88%. By measuring the absolute frequencies of our STIRAP lasers, we find the energy-level difference from an initial weakly bound Feshbach state to the rovibrational ground state with a resolution of $\ensuremath{\sim}5$ kHz over an energy-level difference of more than $114\phantom{\rule{0.28em}{0ex}}\mathrm{T}\mathrm{Hz}$; this lets us discern the hyperfine splitting of the ground state. Combined with theoretical models of the Feshbach-state binding energies and ground-state hyperfine structure, we determine a zero-field binding energy of $h\ifmmode\times\else\texttimes\fi{}114\phantom{\rule{0.16em}{0ex}}268\phantom{\rule{0.16em}{0ex}}135.24(4)(3)\phantom{\rule{0.28em}{0ex}}\mathrm{M}\mathrm{Hz}$. To our knowledge, this is the most accurate determination to date of the dissociation energy of a molecule.

DOI
10.1103/physreva.94.022507

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One possibility for the creation of ultracold, high phase space density quantum gases of molecules in the rovibronic ground state relies on first associating weakly-bound molecules from quantum-degenerate atomic gases on a Feshbach resonance and then transferring the molecules via several steps of coherent two-photon stimulated Raman adiabatic passage (STIRAP) into the rovibronic ground state. Here, in ultracold samples of Cs2 Feshbach molecules produced out of ultracold samples of Cs atoms, we observe several optical transitions to deeply-bound rovibrational levels of the excited 0(u)+ molecular potentials with high resolution. At least one of these transitions, although rather weak, allows efficient STIRAP transfer into the deeply-bound vibrational level (see text for symbols)v = 73 > of the singlet X1 sigma(g)+ ground state potential, as recently demonstrated (J. G. Danzl, E. Haller, M. Gustavsson, M. J. Mark, R. Hart, N. Bouloufa, O. Dulieu, H. Ritsch, and H.-C. Nägerl, Science, 2008, 321, 1062). From this level, the rovibrational ground state (see text for symbols)v = 0, J = 0 > can be reached with one more transfer step. In total, our results show that coherent ground state transfer for Cs2 is possible using a maximum of two successive two-photon STIRAP processes or one single four-photon STIRAP process.

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We report the binding energy of 87Rb133Cs^{87}\mathrm{Rb}^{133}\mathrm{Cs}87Rb133Cs molecules in their rovibrational ground state measured using an offset-free optical frequency comb based on difference frequency generation technology. We create molecules in the absolute ground state using stimulated Raman adiabatic passage (STIRAP) with a transfer efficiency of 88%. By measuring the absolute frequencies of our STIRAP lasers, we find the energy-level difference from an initial weakly bound Feshbach state to the rovibrational ground state with a resolution of \ensuremath∼5\ensuremath{\sim}5\ensuremath∼5 kHz over an energy-level difference of more than 114THz114\phantom{\rule{0.28em}{0ex}}\mathrm{T}\mathrm{Hz}114THz; this lets us discern the hyperfine splitting of the ground state. Combined with theoretical models of the Feshbach-state binding energies and ground-state hyperfine structure, we determine a zero-field binding energy of h\ifmmode×\else\texttimes\fi114268135.24(4)(3)MHzh\ifmmode\times\else\texttimes\fi{}114\phantom{\rule{0.16em}{0ex}}268\phantom{\rule{0.16em}{0ex}}135.24(4)(3)\phantom{\rule{0.28em}{0ex}}\mathrm{M}\mathrm{Hz}h\ifmmode×\else\texttimes\fi114268135.24(4)(3)MHz. To our knowledge, this is the most accurate determination to date of the dissociation energy of a molecule.
This thesis reports the creation and trapping of 87RbCs molecules in the absolute ground state with a temperature of 1 uK. We build a tunable narrow-linewidth laser system at 1550 nm and 980 nm, using a single high-finesse optical cavity as a reference for both colours. We use fibre-coupled electro-optic modulators to continuously tune both lasers. These allow a novel measurement of the free spectral range of the cavity to better than 1 part in 10^6. We perform one- and two-photon spectroscopy on 87RbCs Feshbach molecules and identify a suitable intermediate state for transfer to the molecular ground state. We measure the electric dipole moment of the molecular ground state as 1.225(3)(8) D, and demonstrate the highest lab-frame dipole moment of any ultracold molecular system at the time of measurement. We transfer the molecules to the electronic, rovibrational and hyperfine ground state using stimulated Raman adiabatic passage, with 88% efficiency. We measure the transition strengths and excited state linewidth for this transfer route. We develop a model for the transfer which includes the effect of laser linewidth, and find excellent agreement with experimental data. The molecular sample is trapped in an optical dipole potential, and has a lifetime of 0.89(6) s. We reference the STIRAP lasers to a novel design of frequency comb which uses difference frequency generation to cancel the carrier-envelope offset. We use this to measure the binding energy of the molecules as h x 114 268 135.24(4)(3) MHz. To our knowledge, this is the most precise determination of the dissociation energy of a molecule to date. Finally, we report progress toward loading the molecules into a 1D optical lattice at 1064 nm. We develop the tools and methods to characterise a lattice, and demonstrate trapping of Feshbach molecules in both a 1D optical lattice and a harmonic optical potential at 1064 nm.
RbCs molecules in the electronic, rovibrational and hyperfine ground state, using stimulated Raman adiabatic passage to transfer the molecules from a weakly bound Feshbach state. We measure one-way transfer efficiencies of 92(1)% and fully characterise the strengths and linewidths of the transitions used. We model the transfer, including a Monte Carlo simulation of the laser noise, and find this matches well with both the transfer efficiency and our previous measurements of the laser linewidth and frequency stability.
We report the creation of a sample of over 1000 ultracold 87Rb133Cs^{87}\mathrm{Rb}^{133}\mathrm{Cs}87Rb133Cs molecules in the lowest rovibrational ground state, from an atomic mixture of 87Rb^{87}\mathrm{Rb}87Rb and 133Cs^{133}\mathrm{Cs}133Cs, by magnetoassociation on an interspecies Feshbach resonance followed by stimulated Raman adiabatic passage (STIRAP). We measure the binding energy of the RbCs molecule to be $hc\ifmmode\times\else\texttimes\fi{}3811.576(1)\text{ }\text{ }{\mathrm{cm}}^{\ensuremath{-}1}$ and the $|{v}^{\ensuremath{'}\ensuremath{'}}=0,{J}^{\ensuremath{'}\ensuremath{'}}=0⟩$ to $|{v}^{\ensuremath{'}\ensuremath{'}}=0,{J}^{\ensuremath{'}\ensuremath{'}}=2⟩$ splitting to be $h\ifmmode\times\else\texttimes\fi{}2940.09(6)\text{ }\text{ }\mathrm{MHz}$. Stark spectroscopy of the rovibrational ground state yields an electric dipole moment of 1.225(3)(8) D, where the values in parentheses are the statistical and systematic uncertainties, respectively. We can access a space-fixed dipole moment of 0.355(2)(4) D, which is substantially higher than in previous work.
We report a detailed molecular spectroscopy study of the lowest excited electronic states of 23Na87Rb^{23}\mathrm{Na}\phantom{\rule{0.16em}{0ex}}^{87}\mathrm{Rb}23Na87Rb for producing ultracold 23Na87Rb^{23}\mathrm{Na}\phantom{\rule{0.16em}{0ex}}^{87}\mathrm{Rb}23Na87Rb molecules in the electronic, rovibrational, and hyperfine ground state. Starting from weakly bound Feshbach molecules, a series of vibrational levels of the $A{\phantom{\rule{0.16em}{0ex}}}^{1}{\mathrm{\ensuremath{\Sigma}}}^{+}\text{\ensuremath{-}}b{\phantom{\rule{0.16em}{0ex}}}^{3}\mathrm{\ensuremath{\Pi}}$ coupled excited states is investigated. After resolving, modeling, and interpreting the hyperfine structure of several lines, we successfully identify a long-lived level resulting from the accidental hyperfine coupling between the 0+{0}^{+}0+ and ${0}^{\ensuremath{-}}$ components of the $b{\phantom{\rule{0.16em}{0ex}}}^{3}\mathrm{\ensuremath{\Pi}}$ state, satisfying all the requirements for the population transfer toward the lowest rovibrational level of the $X{\phantom{\rule{0.16em}{0ex}}}^{1}{\mathrm{\ensuremath{\Sigma}}}^{+}$ state. Using two-photon spectroscopy, its binding energy is measured to be 4977.308(3) ${\mathrm{cm}}^{\ensuremath{-}1}$. We calibrate all the transition strengths carefully and also demonstrate Raman transfer of Feshbach molecules to the absolute ground state.
A narrow-linewidth, dual-wavelength laser system is vital for the creation of ultracold ground state molecules via stimulated Raman adiabatic passage (STIRAP) from a weakly bound Feshbach state. Here we describe how a relatively simple apparatus consisting of a single fixed-length optical cavity can be used to narrow the linewidth of the two different wavelength lasers required for STIRAP simultaneously. The frequency of each of these lasers is referenced to the cavity and is continuously tunable away from the cavity modes through the use of non-resonant electro-optic modulators. Self-heterodyne measurements suggest the laser linewidths are reduced to several hundred Hz. In the context of 87Rb133Cs molecules produced via magnetoassociation on a Feshbach resonance, we demonstrate the performance of the laser system through one- and two-photon molecular spectroscopy. Finally, we demonstrate transfer of the molecules to the rovibrational ground state using STIRAP. ar X iv
One possibility for the creation of ultracold, high phase space density quantum gases of molecules in the rovibronic ground state relies on first associating weakly-bound molecules from quantum-degenerate atomic gases on a Feshbach resonance and then transferring the molecules via several steps of coherent two-photon stimulated Raman adiabatic passage (STIRAP) into the rovibronic ground state. Here, in ultracold samples of Cs2 Feshbach molecules produced out of ultracold samples of Cs atoms, we observe several optical transitions to deeply-bound rovibrational levels of the excited 0(u)+ molecular potentials with high resolution. At least one of these transitions, although rather weak, allows efficient STIRAP transfer into the deeply-bound vibrational level (see text for symbols)v = 73 > of the singlet X1 sigma(g)+ ground state potential, as recently demonstrated (J. G. Danzl, E. Haller, M. Gustavsson, M. J. Mark, R. Hart, N. Bouloufa, O. Dulieu, H. Ritsch, and H.-C. Nägerl, Science, 2008, 321, 1062). From this level, the rovibrational ground state (see text for symbols)v = 0, J = 0 > can be reached with one more transfer step. In total, our results show that coherent ground state transfer for Cs2 is possible using a maximum of two successive two-photon STIRAP processes or one single four-photon STIRAP process.