In weakly bound diatomic molecules, energy levels are closely spaced and thus more susceptible to mixing by magnetic fields than in the constituent atoms. We use this effect to control the strengths of forbidden optical transitions in $^{88}$Sr$_2$ over 5 orders of magnitude with modest fields by taking advantage of the intercombination-line threshold. The physics behind this remarkable tunability is accurately explained with both a simple model and quantum chemistry calculations, and suggests new possibilities for molecular clocks. We show how mixed quantization in an optical lattice can simplify molecular spectroscopy. Furthermore, our observation of formerly inaccessible $f$-parity excited states offers an avenue for improving theoretical models of divalent-atom dimers.
We observe "trilobite-like" states of ultracold 85Rb2 molecules, in which a ground-state atom is bound by the electronic wavefunction of its Rydberg-atom partner. We populate these states through the ultraviolet excitation of weakly-bound molecules, and access a regime of trilobite-like states at low principal quantum numbers and with vibrational turning points around 35 Bohr radii. This demonstrates that, unlike previous studies that used free-to-bound transitions, trilobite-like states can also be excited through bound-to-bound transitions. This approach provides high excitation probabilitie…
In a recent work [T. C. H. Liew and V. Savona, Phys. Rev. Lett. {\bf104}, 183601 (2010)] it was numerically shown that in a photonic 'molecule' consisting of two coupled cavities, near-resonant coherent excitation could give rise to strong photon antibunching with a surprisingly weak nonlinearity. Here, we show that a subtle quantum interference effect is responsible for the predicted efficient photon blockade effect. We analytically determine the optimal on-site nonlinearity and frequency detuning between the pump field and the cavity mode. We also highlight the limitations of the proposal an…
By making use of the quantization rule of Raab and Friedrich [P. Raab and H. Friedrich, Phys. Rev. A 78, 022707 (2008)], we derive simple and accurate formulae for the number of rotational states supported by a weakly-bound vibrational level of a diatomic molecule and the rotational constants of any such levels up to the threshold, and provide a criterion for determining whether a given weakly-bound vibrational level is rotationless. The results depend solely on the long-range part of the molecular potential and are applicable to halo molecules.
Using the multipolar expansion of electrostatic and magnetostatic potential energies, we characterize the long-range interactions between two weakly-bound diatomic molecules, taking as an example the paramagnetic Er$_2$ Feshbach molecules which were produced recently. Since inside each molecule, individual atoms conserve their identity, the intermolecular potential energy can be expanded as the sum of pairwise atomic potential energies. In the case of Er$_2$ Feshbach molecules, we show that the interaction between atomic magnetic dipoles gives rise to the usual $R^{-3}$ term of the multipolar …
We show that weakly-bound molecules can be probed by "shaking" in a pulsed nonresonant laser field. The field introduces a centrifugal term which expels the highest vibrational level from the potential that binds it. Our numerical simulations applied to the Rb$_2$ and KRb Feshbach molecules indicate that shaking by feasible laser pulses can be used to accurately recover the square of the vibrational wavefunction and, by inversion, also the long-range part of the molecular potential.
We investigated transition strengths from ultracold weakly bound 41K87Rb molecules produced via the photoassociation of laser-cooled atoms. An accurate potential energy curve of the excited state (3)1Sigma+ was constructed by carrying out direct potential fit analysis of rotational spectra obtained via depletion spectroscopy. Vibrational energies and rotational constants extracted from the depletion spectra of v'=41-50 levels were combined with the results of the previous spectroscopic study, and they were used for modifying an ab initio potential. An accuracy of 0.14% in vibrational level spa…
Several extensions to the Standard Model of particle physics, including light dark matter candidates and unification theories, predict deviations from Newton's law of gravitation. For macroscopic distances, the inverse-square law of gravitation is well confirmed by astrophysical observations and laboratory experiments. At micrometer and shorter length scales, however, even the state-of-the-art constraints on deviations from gravitational interaction, whether provided by neutron scattering or precise measurements of forces between macroscopic bodies, are currently many orders of magnitude large…
In response to arXiv:1506.07423v1 we discuss the authors work, and our own, on proposed schemes aiming to achieve a discriminatory optical force for chiral molecules.
Fully internal and motional state controlled and individually manipulable polar molecules are desirable for many quantum science applications leveraging the rich state space and intrinsic interactions of molecules. While prior efforts at assembling molecules from their constituent atoms individually trapped in optical tweezers achieved such a goal for exactly one molecule, here we extend the technique to an array of five molecules, unlocking the ability to study molecular interactions. We detail the technical challenges and solutions inherent in scaling this system up. With parallel preparatio…
The present paper aims at finding optimal parameters for trapping of Cs$_2$ molecules in optical lattices, with the perspective of creating a quantum degenerate gas of ground-state molecules. We have calculated dynamic polarizabilities of Cs$_2$ molecules subject to an oscillating electric field, using accurate potential curves and electronic transition dipole moments. We show that for some particular wavelengths of the optical lattice, called "magic wavelengths", the polarizability of the ground-state molecules is equal to the one of a Feshbach molecule. As the creation of the sample of groun…
Due to their intrinsic electric dipole moments and rich internal structure, ultracold polar molecules are promising candidate qubits for quantum computing and for a wide range of quantum simulations. Their long-lived molecular rotational states form robust qubits while the long-range dipolar interaction between molecules provides quantum entanglement. Using a molecular optical tweezer array, single molecules can be moved and separately addressed for qubit operations using optical and microwave fields, creating a scalable quantum platform. Here, we demonstrate long-range dipolar spin-exchange i…
We have produced large samples of ultracold $^{88}$Sr$_2$ molecules in the electronic ground state in an optical lattice. The molecules are bound by 0.05 cm$^{-1}$ and are stable for several milliseconds. The fast, all-optical method of molecule creation via intercombination line photoassociation relies on a near-unity Franck-Condon factor. The detection uses a weakly bound vibrational level corresponding to a very large dimer. This is the first of two steps needed to create Sr$_2$ in the absolute ground quantum state. Lattice-trapped Sr$_2$ is of interest to frequency metrology and ultracold …
We study the rotational predissociation of atom - molecule complexes with very small binding energy. Such complexes can be produced by Feshbach resonance association of ultracold molecules with ultracold atoms. Numerical calculations of the predissociation lifetimes based on the computation of the energy dependence of the scattering matrix elements become inaccurate when the binding energy is smaller than the energy width of the predissociating state. We derive expressions that represent accurately the predissociation lifetimes in terms of the real and imaginary parts of the scattering length …
When the scattering length is proportional to the distance from the center of the system, two particles are shown to be trapped about the center. Furthermore, their spectrum exhibits discrete scale invariance, whose scale factor is controlled by the slope of the scattering length. While this resembles the Efimov effect, our system has a number of advantages when realized with ultracold atoms. We also elucidate how the emergent discrete scaling symmetry is violated for more than two bosons, which may shed new light on Efimov physics. Our system thus serves as a tunable model system to investiga…
Optical molecular clocks promise unparalleled sensitivity to the temporal variation of the electron-to-proton mass ratio and insight into possible new physics beyond the Standard Model. We propose to realize a molecular clock with bosonic $^{174}$Yb$_2$ molecules, where the forbidden $^1$S$_0$$\rightarrow$$^3$P$_0$ clock transition would be induced magnetically. The use of a bosonic species avoids possible complications due to hyperfine structure present in fermionic species. While direct clock line photoassociation would be challenging, weakly bound ground state molecules could be produced by…
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…
We create weakly bound bosonic $^{23}\textrm{Na}^{39}\textrm{K}$ molecules in a mixture of ultracold $^{23}\textrm{Na}$ and $^{39}\textrm{K}$. The creation is done in the vicinity of a so far undetected Feshbach resonance at about $196\,\text{G}$ which we identify in this work by atom-loss spectroscopy. We investigate the involved molecular state by performing destructive radio frequency binding energy measurements. For the constructive molecule creation we use radio frequency pulses with which we assemble up to $6000$ molecules. We analyze the molecule creation efficiency as a function of the…
Cold inelastic collisions between confined cesium (Cs) atoms and Cs$\_2$ molecules are investigated inside a CO$\_2$ laser dipole trap. Inelastic atom-molecule collisions can be observed and measured with a rate coefficient of $\sim 2.5 \times 10^{-11} $cm$^3$ s$^{-1}$, mainly independent of the molecular ro-vibrational state populated. Lifetimes of purely atomic and molecular samples are essentially limited by rest gas collisions. The pure molecular trap lifetime ranges 0,3-1 s, four times smaller than the atomic one, as is also observed in a pure magnetic trap. We give an estimation of the i…
We have studied interspecies scattering in an ultracold mixture of $^{87}$Rb and $^{133}$Cs atoms, both in their lowest-energy spin states. The three-body loss signatures of 30 incoming s- and p-wave magnetic Feshbach resonances over the range 0 to 667 G have been catalogued. Magnetic field modulation spectroscopy was used to observe molecular states bound by up to 2.5 MHz$\times h$. Magnetic moment spectroscopy along the magneto-association pathway from 197 to 182 G gives results consistent with the observed and calculated dependence of the binding energy on magnetic field strength. We have c…
We theoretically study non-destructive detection of ultracold molecules, using a Fabry-Perot cavity. Specifically, we consider vacuum Rabi splitting where we demonstrate the use of collective strong coupling for detection of molecules with many participating energy levels. We also consider electromagnetically induced transparency and transient response of light for the molecules interacting with a Fabry-Perot cavity mode, as a mean for non-destructive detection. We identify the parameters that are required for the detection of molecules in the cavity electromagnetically induced transparency co…
Optical trapping of molecules with long coherence times is crucial for many protocols in quantum information and metrology. However, the factors that limit the lifetimes of the trapped molecules remain elusive and require improved understanding of the underlying molecular structure. Here we show that measurements of vibronic line strengths in weakly and deeply bound $^{88}$Sr$_2$ molecules, combined with \textit{ab initio} calculations, allow for unambiguous identification of vibrational quantum numbers. This, in turn, enables the construction of refined excited potential energy curves that in…
Arrays of single ultracold molecules promise to be a powerful platform for many applications ranging from quantum simulation to precision measurement. Here we report on the creation of an optical tweezer array of single ultracold CaF molecules. By utilizing light-induced collisions during the laser cooling process, we trap single molecules. The high densities attained inside the tweezer traps have also enabled us to observe in the absence of light molecule-molecule collisions of laser cooled molecules for the first time.
The mean-square radii of the molecules $^4$He$_3$, $^4$He$_2-^6$Li, $^4$He$_2-^7$Li and $^4$He$_2-^{23}$Na are calculated using a three-body model with contact interactions. They are obtained from a universal scaling function calculated within a renormalized scheme for three particles interacting through pairwise Dirac-delta interaction. The root-mean-square distance between two atoms of mass $m_A$ in a triatomic molecule are estimated to be of de order of ${\cal C}\sqrt{\hbar^2/[m_A(E_3-E_2)]}$, where $E_2$ is the dimer and $E_3$ the trimer binding energies, and ${\cal C}$ is a constant (vary…
We study the dynamics of a supersonic molecular beam in a low-finesse optical cavity and demonstrate that most molecules in the beam can be decelerated to zero central velocity by the intracavity optical field in a process analogous to electrostatic Stark deceleration. We show that the rapid switching of the optical field for slowing the molecules is automatically generated by the cavity-induced dynamics. We further show that $\sim1\%$ of the molecules can be optically trapped at a few millikelvin in the same cavity.
We demonstrate rotational and vibrational cooling of cesium dimers by optical pumping techniques. We use two laser sources exciting all the populated rovibrational states, except a target state that thus behaves like a dark state where molecules pile up thanks to absorption-spontaneous emission cycles. We are able to accumulate photoassociated cold Cs2 molecules in their absolute ground state (v = 0, J = 0) with up to 40% efficiency. Given its simplicity, the method could be extended to other molecules and molecular beams. It also opens up general perspectives in laser cooling the external deg…
A detailed treatment of an electro-optical trap for polar molecules, realized by embedding an optical trap within a uniform electrostatic field, is presented and the trap's properties analyzed and discussed. The electro-optical trap offers significant advantages over an optical trap that include an increased trap depth and conversion of alignment of the trapped molecules to marked orientation. Tilting the polarization plane of the optical field with respect to the electrostatic field diminishes both the trap depth and orientation and lifts the degeneracy of the $\pm M$ states of the trapped mo…
We respond to recent works by Bradshaw and Andrews on the discriminatory optical force for chiral molecules, in particular to the erroneous claims made by them concerning our earlier work.
We present spectra of ultracold $^7$Li$^{85}$Rb 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 (MOT), weakly bound molecules are formed in the 4(1) electronic state, which corresponds to the B$^1Π$ state at short range. These molecules spontaneously decay to the electronic ground state and we use resonantly enhanced multiphoton ionization (REMPI) to determine the vibrational population distribution in the electronic ground states after spontaneous emission. Many of the…
Ultracold paramagnetic and polar diatomic molecules are among the promising systems for quantum simulation of lattice-spin models. Unfortunately, their experimental observation is still challenging. Based on our recent \textit{ab-initio} calculations, we analyze the feasibility of all-optical schemes for the formation of ultracold $^{87}$Rb$^{84}$Sr bosonic molecules. First, we have studied the formation by photoassociation followed by spontaneous emission. The photoassociation rates to levels belonging to electronic states converging to the $^{87}$Rb$(5s\,^2S)$+$^{84}$Sr($5s5p\,^3P_{0,1,2}$) …
Heteronuclear alkali-metal dimers represent the class of molecules of choice for creating samples of ultracold molecules exhibiting an intrinsic large permanent electric dipole moment. Among them, the KCs molecule, with a permanent dipole moment of 1.92~Debye still remains to be observed in ultracold conditions. Based on spectroscopic studies available in the literature completed by accurate quantum chemistry calculations, we propose several optical coherent schemes to create ultracold bosonic and fermionic KCs molecules in their absolute rovibrational ground level, starting from a weakly boun…
We report magneto-optical trapping (MOT) of a polyatomic molecule, calcium monohydroxide (CaOH). The MOT contains $2.0(5)\times 10^4$ CaOH molecules at a peak density of $3.0(8)\times10^{6}$ cm$^{-3}$. CaOH molecules are further sub-Doppler laser cooled in an optical molasses, to a temperature of 110(4) $μ$K. The temperatures and densities achieved here make CaOH a viable candidate for a wide variety of quantum science applications, including the creation of optical tweezer arrays of CaOH molecules. This work also suggests that laser cooling and magneto-optical trapping of many other polyatomi…
The study of ultracold molecules tightly trapped in an optical lattice can expand the frontier of precision measurement and spectroscopy, and provide a deeper insight into molecular and fundamental physics. Here we create, probe, and image microkelvin $^{88}$Sr$_2$ molecules in a lattice, and demonstrate precise measurements of molecular parameters as well as coherent control of molecular quantum states using optical fields. We discuss the sensitivity of the system to dimensional effects, a new bound-to-continuum spectroscopy technique for highly accurate binding energy measurements, and prosp…
We demonstrate an all-optical method for magnetic sensing of individual molecules in ambient conditions at room temperature. Our approach is based on shallow nitrogen-vacancy (NV) centers near the surface of a diamond crystal, which we use to detect single paramagnetic molecules covalently attached to the diamond surface. The manipulation and readout of the NV centers is all-optical and provides a sensitive probe of the magnetic field fluctuations stemming from the dynamics of the electronic spins of the attached molecules. As a specific example, we demonstrate detection of a single paramagnet…
Optically trapped laser-cooled polar molecules hold promise for new science and technology in quantum information and quantum simulation. Large numerical aperture optical access and long trap lifetimes are needed for many studies, but these requirements are challenging to achieve in a magneto-optical trap (MOT) vacuum chamber that is connected to a cryogenic buffer gas beam source, as is the case for all molecule laser cooling experiments so far. Long distance transport of molecules greatly eases fulfilling these requirements as molecules are placed into a region separate from the MOT chamber.…
We report laser cooling and trapping of yttrium monoxide (YO) molecules in an optical lattice. We show that gray molasses cooling remains exceptionally efficient for YO molecules inside the lattice with a molecule temperature as low as 6.1(6) $μ$K. This approach has produced a trapped sample of 1200 molecules, with a peak spatial density of $\sim1.2\times10^{10}$ cm$^{-3}$, and a peak phase-space density of $\sim3.1\times10^{-6}$. By adiabatically ramping down the lattice depth, we cool the molecules further to 1.0(2) $μ$K, twenty times colder than previously reported for laser-cooled molecule…
State-dependent optical tweezers can be used to trap a pair of molecules with a separation much smaller than the wavelength of the trapping light, greatly enhancing the dipole-dipole interaction between them. Here we describe a general approach to producing these state-dependent potentials using the tensor part of the ac Stark shift and show how it can be used to carry out two-qubit gates between pairs of molecules. The method is applicable to broad classes of molecules including bialkali molecules produced by atom association and those amenable to direct laser cooling.
We propose and demonstrate a novel technique that combines Raman scattering and optical cycling in molecules with diagonal Franck-Condon factors. This resonance Raman optical cycling manipulates molecules to behave like efficient fluorophores with discrete absorption and emission profiles that are readily separated for sensitive fluorescence detection in high background light environments. Using a molecular beam of our test species, SrF, we realize up to an average of $\approx20$ spontaneously emitted photons per molecule, limited by the interaction time, while using a bandpass filter to suppr…
We have realized long-lived ground-state polar molecules in a 3D optical lattice, with a lifetime of up to 25 s, which is limited only by off-resonant scattering of the trapping light. Starting from a 2D optical lattice, we observe that the lifetime increases dramatically as a small lattice potential is added along the tube-shaped lattice traps. The 3D optical lattice also dramatically increases the lifetime for weakly bound Feshbach molecules. For a pure gas of Feshbach molecules, we observe a lifetime of >20 s in a 3D optical lattice; this represents a 100-fold improvement over previous resu…
We predict $s-$wave elastic cross-sections $σ$ for low-energy atom-molecule collisions with kinetic energies up to 40 mK, for the $^4$He collision with weakly bound diatomic molecules formed by $^4$He with $^7$Li, $^6$Li and $^{23}$Na. Our scattering calculations are performed by using diatomic and triatomic molecular binding energies obtained from several available realistic models as input in a renormalized zero-range model, as well as a finite-range one-term separable potential in order to quantify the relevance of range corrections to our predictions. Of particular relevance for possible e…
Optical pumping by blackbody radiation is a feature shared by all polar molecules and fundamentally limits the time that these molecules can be kept in a single quantum state in a trap. To demonstrate and quantify this, we have monitored the optical pumping of electrostatically trapped OH and OD radicals by room-temperature blackbody radiation. Transfer of these molecules to rotationally excited states by blackbody radiation at 295 K limits the $1/e$ trapping time for OH and OD in the $X^{2}Π_{3/2},v''=0,J''=3/2(f)$ state to 2.8 s and 7.1 s, respectively.
It is demonstrated that weakly bound van der Waals complexes can dissociate in a magnetic field through coupling between the Zeeman levels. The Zeeman predissociation process is shown to be efficient and it can be controlled by external magnetic fields.
We demonstrate a scheme for magneto-optically trapping strontium monofluoride (SrF) molecules at temperatures one order of magnitude lower and phase space densities three orders of magnitude higher than obtained previously with laser-cooled molecules. In our trap, optical dark states are destabilized by rapidly and synchronously reversing the trapping laser polarizations and the applied magnetic field gradient. The number of molecules and trap lifetime are also significantly improved from previous work by loading the trap with high laser power and then reducing the power for long-term trapping…
We report the high resolution photoassociation (PA) spectroscopy of a $^{87}Rb$ Bose-Einstein condensate (BEC) to excited molecular states near the dissociation limit of $5P_{1/2} +5S_{1/2}$ by optical Bragg scattering. Since the detection of optical Bragg scattering in BEC has a high signal-noise ratio, we obtain the high resolution PA spectrum of excited molecular states in the range of $\pm1$ GHz near the dissociation limit of $5P_{1/2} +5S_{1/2}$. We compare the results with the conventional method of trap loss and show that the results agree each other very well. Many interesting phenomen…
We demonstrate a 1D magneto-optical trap of the polar free radical calcium monohydroxide (CaOH). A quasi-closed cycling transition is established to scatter $\sim 10^3$ photons per molecule, predominantly limited by interaction time. This enables radiative laser cooling of CaOH while compressing the molecular beam, leading to a significant increase in on-axis beam brightness and reduction in temperature from 8.4 mK to 1.4 mK.
We investigate the dynamical process of optically trapped X$^{1}$$Σ$$^{+}$ (v" = 0) state $^{85}$Rb$^{133}$Cs molecules distributing in J" = 1 and J" = 3 rotational states. The considered molecules, formed from short-range photoassociation of mixed cold atoms, are subsequently confined in a crossed optical dipole trap. Based on a phenomenological rate equation, we provide a detailed study of the dynamics of $^{85}$Rb$^{133}$Cs molecules during the loading and holding processes. The inelastic collisions of $^{85}$Rb$^{133}$Cs molecules in the X$^{1}$$Σ$$^{+}$ (v" = 0, J" = 1 and J" = 3) states …
We consider the use of pulse-shaped broadband femtosecond lasers to optically cool rotational and vibrational degrees of freedom of molecules. Since this approach relies on cooling rotational and vibrational quanta by exciting an electronic transition, it is most easily applicable to molecules with similar ground and excited potential energy surfaces, such that the vibrational state is usually unchanged during electronic relaxation. Compared with schemes that cool rotations by exciting vibrations, this approach achieves internal cooling on the orders-of- magnitude faster electronic decay times…
Calcium monofluoride (CaF) is magnetically slowed and trapped using optical pumping. Starting from a collisionally cooled slow beam, CaF with an initial velocity of ~ 30 m/s is slowed via magnetic forces as it enters a 800 mK deep magnetic trap. Employing two-stage optical pumping, CaF is irreversibly loaded into the trap via two scattered photons. We observe a trap lifetime exceeding 500 ms, limited by background collisions. This method paves the way for cooling and magnetic trapping of chemically diverse molecules without closed cycling transitions.
