Cross-Molecular Coupling in Combined Photoassociation and Feshbach Resonances
Matt Mackie, Matthew Fenty, Danielle Savage, Jake Kesselman
备注：
4 pages, 2 figs, 22+ refs; v2 improved abstract, refined discussion of exptl motivation, improved word choice in discussion of future work; to appear in Phys. Rev. Lett
We model combined photoassociation and Feshbach resonances in a Bose-Einstein condensate. When the magnetic field is far-off resonance, cross coupling between the two target molecules--enabled by the shared dissociation continuum--leads to an anomalous dispersive shift in the position of laser resonance, as well as unprecedented elimination and enhancement of resonant photoassociation via quantum interference. For off-resonant lasers, a dispersive shift and quantum interference appear similarly in resonant three-body Feshbach losses, except that the Feshbach node is tunable with intensity.
Two-color photoassociation of ground state $^6$Li$^{87}$Rb molecules via the $\mathrm{B}^1Π$ electronic state using short pulses near a magnetic Feshbach resonance is studied theoretically. A near-resonant magnetic field is applied to mix the hyperfine singlet and triplet components of the initial wave function and enhance the photoassociation rate, before the population is transferred to the ground state by a second pulse. We show that an increase of up to three orders of magnitude in the absolute number of molecules produced is attainable for deeply bound vibrational levels. This technique c…
We consider photoassociation from a state of two free atoms when the continuum state is close to a magnetic field induced Feshbach resonance and analyze Fano interference in photoassociation. We show that the minimum in photoassociation profiles characterized by the Fano asymmetry parameter $q$ is independent of laser intensity, while the maximum explicitly depends on laser intensity. We further discuss the possibility of nonlinear Fano effect in photoassociation near a Feshbach resonance.
We demonstrate Feshbach optimized photoassociation (FOPA) into the $0_{g}^{-} (5$S$_{1/2}+5$P$_{1/2}$) state in $^{85}$Rb$_{2}$. FOPA uses the enhancement of the amplitude of the initial atomic scattering wave function due to a Feshbach resonance to increase the molecular formation rate from photoassociation. We observe three vibrational levels, $v=$127, 140, and 150, with previously unmeasured binding energies of 256, 154, and 96 cm$^{-1}$. We measure the frequency, central magnetic field position, and magnetic field width of each Feshbach resonance. Our findings experimentally confirm that t…
Ultracold molecules offer a broad variety of applications, ranging from metrology to quantum computing. However, forming "real" ultracold molecules, {\it i.e.} in deeply bound levels, is a very difficult proposition. Here, we show how photoassociation in the vicinity of a Feshbach resonance enhance molecular formation rates by several orders of magnitude. We illustrate this effect in heteronuclear systems, and find giant rate coefficients even in deeply bound levels. We also give a simple analytical expression for the photoassociation rates, and discuss future applications of the Feshbach Opti…
We reveal the existence of high-density Feshbach resonances in the collision between the ground and metastable states of $^{171}$Yb and coherently produce the associated Feshbach molecules by photoassociation. The extremely small transition rate is overcome by the enhanced Franck-Condon factor of the weakly bound Feshbach molecule, allowing us to observe Rabi oscillations with long decay time between an atom pair and a molecule in an optical lattice. We also perform the precision measurement of the binding energies, which characterizes the observed resonances. The ultra-narrow photoassociation…
Photoassociation (PA) spectrum in the presence of a magnetic Feshbach resonance is analyzed. Nonperturbative solution of the problem yields analytical expressions for PA linewidth and shift which are applicable for arbitrary PA laser intensity and magnetic field tuning of Feshbach Resonance. We show that by tuning magnetic field close to Fano minimum, it is possible to suppress power broadening at increased laser intensities. This occurs due to quantum interference of PA transitions from unperturbed and perturbed continuum. Line narrowing at high laser intensities is accompanied by large spect…
We analyse the formation of ultracold 7Li133Cs molecules in the rovibrational ground state through photoassociation into the B1Pi state, which has recently been reported [J. Deiglmayr et al., Phys. Rev. Lett. 101, 133004 (2008)]. Absolute rate constants for photoassociation at large detunings from the atomic asymptote are determined and are found to be surprisingly large. The photoassociation process is modeled using a full coupled-channel calculation for the continuum state, taking all relevant hyperfine states into account. The enhancement of the photoassociation rate is found to be caused b…
We model the formation of stable heteronuclear molecules via pulsed Raman photoassociation of a two-component Bose-Einstein condensate near a strong Feshbach resonance, for both counterintuitive and intuitive pulse sequencing. Compared to lasers alone, weak Raman photoassociation is enhanced by as much as a factor of ten (five) for a counterintuitive (intuitive) pulse sequence, whereas strong Raman photoassociation is barely enhanced at all--regardless of pulse sequence. Stronger intra-atom, molecule, or atom-molecule collisions lead to an expected decrease in conversion efficiency, but strong…
We show that the photoassociation (PA) rate of ultracold diatomic molecules in the vicinity of a Feshbach resonance could be used to probe variations of the electron-to-proton mass ratio $β= m_e/m_p$, a quantity related to other fundamental constants via the $Λ_{\mathrm{QCD}}$ scale. The PA rate exhibits two features near a Feshbach resonance, a minimum and a maximum, which are very sensitive to the details of the interactions and the exact mass of the system. The effect and detection threshold are illustrated in the formation rates of ultracold Li$_2$ and LiNa molecules by performing coupled-…
The electronic structure of the (LiYb)$^+$ molecular ion is investigated with two variants of the coupled cluster method restricted to single, double, and noniterative or linear triple excitations. Potential energy curves for the ground and excited states, permanent and transition electric dipole movements, and long-range interaction coefficients $C_4$ and $C_6$ are reported. The data is subsequently employed in scattering calculations and photoassociation studies. Feshbach resonances are shown to be measurable despite the ion's micromotion in the Paul trap. Molecular ions can be formed in the…
The multichannel quantum defect theory (MQDT) in combination with the frame transformation (FT) approach is applied to model the Fano-Feshbach resonances measured for $^{7}$Li$^{87}$Rb and $^{6}$Li$^{87}$Rb [Marzok {\it et al.} Phys. Rev. A {\bf 79} 012717 (2009)]. The MQDT results show a level of accuracy comparable to that of previous models based on direct, fully numerical solutions of the the coupled channel Schrödinger equations (CC). Here, energy levels deduced from 2-photon photoassociation spectra for $^{7}$Li$^{85}$Rb are assigned by applying the MQDT approach, obtaining the bound sta…
Optical Feshbach resonances [Phys. Rev. Lett. 94, 193001 (2005)] and pump-dump photoassociation with short laser pulses [Phys. Rev. A 73, 033408 (2006)] have been proposed as means to coherently form stable ultracold alkali dimer molecules. In an optical Feshbach resonance, the intensity and possibly frequency of a cw laser are ramped up linearly followed by a sudden switch-off of the laser. This is applicable to tightly trapped atom pairs. In short-pulse photoassociation, the pump pulse forms a wave-packet in an electronically excited state. The ensuing dynamics carry the wave-packet to short…
The properties of bosonic Ytterbium photoassociation spectra near the intercombination transition $^{1}S_{0}$--$^{3}P_{1}$ are studied theoretically at ultra low temperatures. We demonstrate how the shapes and intensities of rotational components of optical Feshbach resonances are affected by mass tuning of the scattering properties of the two colliding ground state atoms. Particular attention is given to the relationship between the magnitude of the scattering length and the occurrence of shape resonances in higher partial waves of the van der Waals system. We develop a mass scaled model of t…
Photoassociation and the Feshbach resonance are, in principle, feasible means for creating a molecular Bose-Einstein condensate from an already-quantum-degenerate gas of atoms; however, mean-field shifts and irreversible decay place practical constraints on the efficient delivery of stable molecules using either mechanism alone. We therefore propose Feshbach-stimulated Raman photoproduction, i.e., a combination of magnetic and optical methods, as a viable means to collectively convert degenerate atoms into a stable molecular condensate with near-unit efficiency.
We demonstrate a p$-wave optical Feshbach resonance (OFR) using purely long-range molecular states of a fermionic isotope of ytterbium ^{171}Yb, following the proposition made by K. Goyal et al. [Phys. Rev. A 82, 062704 (2010)]. The p-wave OFR is clearly observed as a modification of a photoassociation rate for atomic ensembles at about 5 micro-Kelvins. A scattering phase shift variation of δη=0.022 rad is observed with an atom loss rate coefficient K=28.0*10^{-12} cm^3/s.
We present precise measurements of the optical Feshbach resonances (OFRs) of $^{174}$Yb atoms for the intercombination transition. We measure the photoassociation (PA) spectra of a pure $^{174}$Yb Bose-Einstein condensate, and determine the dependence of OFRs to PA laser intensities and frequencies for four least bound vibrational levels near the intercombination transition. We confirm that our measurements are consistent with the temporal decay of a BEC subjected to a PA beam in the vicinity of the fourth vibrational level from the dissociation limit.
We investigate magnetically tunable Feshbach resonances in ultracold collisions between ground-state Yb and Cs atoms, using coupled-channel calculations based on an interaction potential recently determined from photoassociation spectroscopy. We predict resonance positions and widths for all stable isotopes of Yb, together with resonance decay parameters where appropriate. The resonance patterns are richer and more complicated for fermionic Yb than for spin-zero isotopes, because there are additional level splittings and couplings due to scalar and tensorial Yb hyperfine interactions. We exami…
Motivated by a recent experiment by Zelevinsky et al. [Phys. Rev. Lett. 96, 203201], we present the theory for photoassociation and optical Feshbach resonances of atoms confined in a tight one-dimensional (1D) or two-dimensional (2D) optical lattice. In the case of an alkaline-earth intercombination resonance, the narrow natural width of the line makes it possible to observe clear manifestations of the dimensionality, as well as some sensitivity to the scattering length of the atoms. Among possible applications, a 2D lattice may be used to increase the spectroscopic resolution by about one ord…
We develop the theory for the Adiabatic Raman Photoassociation (ARPA) of ultracold atoms to form ultracold molecules in the presence of scattering resonances. Based on a computational method in which we replace the continuum with a discrete set of "effective modes", we show that the existence of resonances greatly aids in the formation of deeply bound molecular states. We illustrate our general theory by computationally studying the formation of $^{85}$Rb$_2$ molecules from pairs of colliding ultracold $^{85}$Rb atoms. The single-event transfer yield is shown to have a near-unity value for wid…
We present the prospects for photoassociation, optical control of interspecies scattering lengths and finally, the production of ultracold absolute ground state molecules in the Rb+Hg system. We use the "gold standard" ab initio methods for the calculations of ground (CCSD(T)) and excited state (EOM-CCSD) potential curves. The RbHg system, thanks to the wide range of stable Hg bosonic isotopes, offers possibilities for mass-tuning of ground state interactions. The optical lengths describing the strengths of optical Feshbach resonances near the Rb transitions are favorable even at large laser d…
We present an analytical study of three-state Feshbach resonances induced by second-order couplings. Such resonances arise when the scattering amplitude is modified by the interaction with a bound state that is not directly coupled to the scattering state containing incoming flux. Coupling occurs indirectly through an intermediate state. We consider two problems: (i) the intermediate state is a scattering state in a distinct open channel; (ii) the intermediate state is an off-resonant bound state in a distinct closed channel. The first problem is a model of electric-field-induced resonances in…
We model two bosons in an optical lattice near a Feshbach or photoassociation resonance, focusing on the Bose-Hubbard model in one dimension. Whereas the usual atoms-only theory with a tunable scattering length yields one bound state for a molecular dimer for either attractive or repulsive atom-atom interaction, an atom-molecule theory gives two bound states that may represent attractively and repulsively bound dimers occurring simultaneously. Such unusual molecular physics should be observable for an atom-molecule coupling strength comparable to the width of the dissociation continuum of the …
We survey results on the creation of heteronuclear Fermi molecules by tuning a degenerate Bose-Fermi mixture into the neighborhood of an association resonance, either photoassociation or Feshbach, as well as the subsequent prospects for Cooper-like pairing between atoms and molecules. In the simplest case of only one molecular state, corresponding to either a Feshbach resonance or one-color photoassociation, the system displays Rabi oscillations and rapid adiabatic passage between a Bose-Fermi mixture of atoms and fermionic molecules. For two-color photoassociation, the system admits stimulate…
It is possible to tune the scattering length for the collision of ultra-cold 1S0 ground state alkaline-earth atoms using an optical Feshbach resonance. This is achieved with a laser far detuned from an excited molecular level near the frequency of the atomic intercombination 1S0--3P1 transition. Simple resonant scattering theory, illustrated by the example of 40Ca, allows an estimate of the magnitude of the effect. Unlike alkali metal species, large changes of the scattering length are possible while atom loss remains small, because of the very narrow line width of the molecular photoassociati…
We present a method for the creation and control of cold molecules that involves coherently combining Feshbach Resonances and STIRAP. We present analytical and numerical results showing how to optimize this process that can be implemented using techniques readily available in standard experimental setups. This will provide a link in the chain from atoms to ground state molecules and can serve as a building block towards more complex processes in coherent ultracold chemistry.
This chapter summarizes the properties of near-threshold molecular states that can be formed from ultracold atoms. The properties of the states for a single potential are characterized for different partial waves using the concepts of quantum defect theory for a van der Waals potential. Examples are given for various isotopes of the Yb_2 molecule. Magnetically tunable Feshbach resonances or photoassociation resonances are characterized by the multichannel version of the theory. Examples of the latter are given for the KRb molecule.
Using new experimental measurements of photoassociation resonances near the $^1\mathrm{S}_0 \rightarrow \phantom{ }^3\mathrm{P}_1$ intercombination transition in $^{84}$Sr and $^{86}$Sr, we present an updated study into the mass-scaling behavior of bosonic strontium dimers. A previous mass-scaling model [Borkowski et al., Phys. Rev. A 90, 032713 (2014)] was able to incorporate a large number of photoassociation resonances for $^{88}$Sr, but at the time only a handful of resonances close to the dissociation limit were known for $^{84}$Sr and $^{86}$Sr. In this work, we perform a more thorough m…
Ultracold molecules have experienced increasing attention in recent years. Compared to ultracold atoms, they possess several unique properties that make them perfect candidates for the implementation of new quantum-technological applications in several fields, from quantum simulation to quantum sensing and metrology. In particular, ultracold molecules of two-electron atoms (such as strontium or ytterbium) also inherit the peculiar properties of these atomic species, above all the possibility to access metastable electronic states via direct excitation on optical clock transitions with ultimate…
A rigorous quantum theory of atomic collisions in the presence of radio frequency (rf) magnetic fields is developed and applied to elucidate the effects of combined dc and rf magnetic fields on elastic scattering in ultracold collisions of Rb atoms. We show that rf fields can be used to induce Feshbach resonances, which can be tuned by varying the amplitude and frequency of the rf field. The rf-induced Feshbach resonances occur also in collisions of atoms in low-field-seeking states at moderate rf field strengths easily available in atom chip experiments, which opens up the world of tunable in…
We study collision of two atoms with formation of Feshbach resonance at combined interaction with the external magnetic field and laser radiation. In cases of one- and two-photon resonances of laser radiation with two discrete vibrational molecular levels, we show that Feshbach resonances appear at interaction of external magnetic field with dressed states formed via Autler-Townes effect. In addition, in case of one-photon resonance the lower vibrational molecular state is coupled by laser radiation with the continuum of the elastic channel and forms laser-induced Feshbach resonance via both A…
We theoretically evaluate the feasibility to form magnetically-tunable Feshbach molecules in collisions between fermionic $^6$Li atoms and bosonic metastable $^{174}$Yb($^3$P$_2$) atoms. In contrast to the well-studied alkali-metal atom collisions, collisions with meta-stable atoms are highly anisotropic. Our first-principle coupled-channel calculation of these collisions reveals the existence of broad Feshbach resonances due to the combined effect of anisotropic-molecular and atomic-hyperfine interactions. In order to fit our predictions to the specific positions of experimentally-observed br…
We show that recent high-precision measurements of relative on-site interaction energies $ΔU$ in a Mott insulator require a theoretical description beyond the standard Hubbard-model interpretation, when combined with an accurate coupled-channels calculation. In contrast to more sophisticated lattice models, which can be elaborate especially for parameter optimization searches, we introduce an easy to use effective description of $U$ valid over a wide range of interaction strengths modeling atomic pairs confined to single lattice sites. This concise model allows for a straightforward combinatio…
We have performed radio-frequency dissociation spectroscopy of weakly bound ^6Li_2 Feshbach molecules using low-density samples of about 30 molecules in an optical dipole trap. Combined with a high magnetic field stability this allows us to resolve the discrete trap levels in the RF dissociation spectra. This novel technique allows the binding energy of Feshbach molecules to be determined with unprecedented precision. We use these measurements as an input for a fit to the ^6Li scattering potential using coupled-channel calculations. From this new potential, we determine the pole positions of t…
It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a vast array of fields. Unfortunately laser cooling has not yet been extended to molecules because of their complex internal structure. However, this complexity makes molecules potentially useful for many applications. For example, heteronuclear molecules possess permanent electric dipole moments which lead to long-range, tunable, anisotropic dipole-dipole interactions. The combination of the dipole-dipole interaction and the precise control over molecular degrees of freedom …
Controlling physical systems and their dynamics on the level of individual quanta propels both fundamental science and quantum technologies. Trapped atomic and molecular systems, neutral and charged, are at the forefront of quantum science. Their extraordinary level of control is evidenced by numerous applications in quantum information processing and quantum metrology. Studying the long-range interactions between these systems when combined in a hybrid atom-ion trap has lead to landmark results. Reaching the ultracold regime, however, where quantum mechanics dominates the interaction, e.g., g…
Simultaneous sub-Doppler laser cooling and optical trapping of bosonic $^{39}$K-$^{133}$Cs and $^{41}$K-$^{133}$Cs mixtures
Institute of Experimental Physics, University of Warsaw（华沙大学实验物理研究所）；Durham University（杜伦大学）；Stockholm University（斯德哥尔摩大学）；eleQtron GmbH（eleQtron有限公司）；Warsaw University of Technology（华沙理工大学）
We demonstrate photoassociation (PA) of ultracold fermionic $^{87}$Sr atoms. The binding energies of a series of molecular states on the $^1Σ^+_u$ $5s^2\,^1$S$_0+5s5p\,^1$P$_1$ molecular potential are fit with the semiclassical LeRoy-Bernstein model, and PA resonance strengths are compared to predictions based on the known $^1$S$_0+^1$S$_0$ ground state potential. Similar measurements and analysis were performed for the bosonic isotopes $^{84}$Sr and $^{86}$Sr, allowing a combined analysis of the long-range portion of the excited-state potential and determination of the $5s5p\,^1$P$_1$ atomic …
