We show that the lifetime of ultracold ground-state $^{87}$Rb$^{133}$Cs molecules in an optical trap is limited by fast optical excitation of long-lived two-body collision complexes. We partially suppress this loss mechanism by applying square-wave modulation to the trap intensity, such that the molecules spend 75% of each modulation cycle in the dark. By varying the modulation frequency, we show that the lifetime of the collision complex is $0.53\pm0.06$ ms in the dark. We find that the rate of optical excitation of the collision complex is $3^{+4}_{-2}\times10^{3}$ W$^{-1}$ cm$^2$ s$^{-1}$ for $λ= 1550$ nm, leading to a lifetime of <100 ns for typical trap intensities. These results explain the two-body loss observed in experiments on nonreactive bialkali molecules.
We investigate the effect of far-off-resonant trapping light on ultracold bosonic RbCs molecules. We use kHz-precision microwave spectroscopy to measure the differential AC Stark shifts between the ground and first excited rotational levels of the molecule with hyperfine-state resolution. We demonstrate through both experiment and theory that coupling between neighboring hyperfine states manifests in rich structure with many avoided crossings. This coupling may be tuned by rotating the polarization of the linearly polarized trapping light. A combination of spectroscopic and parametric heating …
Understanding ultracold collisions involving molecules is of fundamental importance for current experiments, where inelastic collisions typically limit the lifetime of molecular ensembles in optical traps. Here we present a broad study of optically trapped ultracold RbCs molecules in collisions with one another, in reactive collisions with Rb atoms, and in nonreactive collisions with Cs atoms. For experiments with RbCs alone, we show that by modulating the intensity of the optical trap, such that the molecules spend 75% of each modulation cycle in the dark, we partially suppress collisional lo…
We have produced ultracold, polar RbCs* molecules via photoassociation in a laser-cooled mixture of Rb and Cs atoms. Using a model of the RbCs* molecular interaction which reproduces the observed rovibrational structure, we infer decay rates in our experiments into deeply bound singlet ground state RbCs vibrational levels as high as 5 x 10^5 s^-1 per level. Population in such deeply bound levels could be efficiently transferred to the vibrational ground state using a single stimulated Raman transition, opening the possibility to create large samples of stable, ultracold polar molecules.
We produce ultracold dense trapped samples of 87Rb133Cs molecules in their rovibrational ground state, with full nuclear hyperfine state control, by stimulated Raman adiabatic passage (STIRAP) with efficiencies of 90%. We observe the onset of hyperfine-changing collisions when the magnetic field is ramped so that the molecules are no longer in the hyperfine ground state. A strong quadratic shift of the transition frequencies as a function of applied electric field shows the strongly dipolar character of the RbCs ground-state molecule. Our results open up the prospect of realizing stable bosoni…
Using resonance-enhanced two-photon ionization, we detect ultracold, ground-state RbCs molecules formed via photoassociation in a laser-cooled mixture of 85Rb and 133Cs atoms. We obtain extensive bound-bound excitation spectra of these molecules, which provide detailed information about their vibrational distribution, as well as spectroscopic data on the RbCs ground a^3Σ^+ and excited (2)^3Σ^+, (1)^1Πstates. Analysis of this data allows us to predict strong transitions from observed excited levels to the absolute vibronic ground state of RbCs, potentially allowing the production of stable, ult…
We perform one- and two-photon high resolution spectroscopy on ultracold samples of RbCs Feshbach molecules with the aim to identify a suitable route for efficient ground-state transfer in the quantum-gas regime to produce quantum gases of dipolar RbCs ground-state molecules. One-photon loss spectroscopy allows us to probe deeply bound rovibrational levels of the mixed excited (A1Σ+ - b3Π0) 0+ molecular states. Two-photon dark state spectroscopy connects the initial Feshbach state to the rovibronic ground state. We determine the binding energy of the lowest rovibrational level |v"=0,J"=0> of t…
We report the creation of a sample of over 1000 ultracold $^{87}$RbCs molecules in the lowest rovibrational ground state, from an atomic mixture of $^{87}$Rb and Cs, 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 $h c \times 3811.576(1)$ cm$^{-1}$ and the $|v''=0, J''=0>$ to $|v''=0, J''=2>$ splitting to be $h \times 2940.09(6)$ MHz. Stark spectroscopy of the rovibrational ground state yields an electric dipole moment of 1.225(3)(8) D, where the values in parentheses a…
Ultracold metastable RbCs molecules are observed in a double species MOT through photoassociation near the Rb(5S$_{1/2}$)+Cs(6P$_{3/2}$) dissociation limit followed by radiative stabilization. The molecules are formed in their lowest triplet electronic state and are detected by resonant enhanced two-photon ionization through the previously unobserved $(3)^{3}Π\leftarrow a^{3}Σ^{+}$ band. The large rotational structure of the observed photoassociation lines is assigned to the lowest vibrational levels of the $0^+,0^-$ excited states correlated to the Rb(5P$_{1/2}$)+Cs(6S$_{1/2}$) dissociation l…
We explore the uses of ultracold molecules as a platform for future experiments in the field of quantum simulation, focusing on two molecular species, $^{40}$Ca$^{19}$F and $^{87}$Rb$^{133}$Cs. We report the development of coherent quantum state control using microwave fields in both molecular species; this is a crucial ingredient for many quantum simulation applications. We demonstrate proof-of-principle Ramsey interferometry measurements with fringe spacings of $\sim 1~\rm kHz$ and investigate the dephasing time of a superposition of $N=0$ and $N=1$ rotational states when the molecules are c…
Understanding and controlling collisions is crucial to the burgeoning field of ultracold molecules. All experiments so far have observed fast loss of molecules from the trap. However, the dominant mechanism for collisional loss is not well understood when there are no allowed 2-body loss processes. Here we experimentally investigate collisional losses of nonreactive ultracold RbCs molecules, and compare our findings with the sticky collision hypothesis that pairs of molecules form long-lived collision complexes. We demonstrate that loss of molecules occupying their rotational and hyperfine gro…
The formation of ultracold metastable RbCs molecules is observed in a double species magneto-optical trap through photoassociation below the ^85Rb(5S_1/2)+^133Cs(6P_3/2) dissociation limit followed by spontaneous emission. The molecules are detected by resonance enhanced two-photon ionization. Using accurate quantum chemistry calculations of the potential energy curves and transition dipole moment, we interpret the observed photoassociation process as occurring at short internuclear distance, in contrast with most previous cold atom photoassociation studies. The vibrational levels excited by p…
We investigate the use of microwave radiation to produce a repulsive shield between pairs of ultracold polar molecules and prevent collisional losses that occur when molecular pairs reach short range. We carry out coupled-channels calculations on RbCs+RbCs and CaF+CaF collisions in microwave fields. We show that effective shielding requires predominantly circular polarization, but can still be achieved with elliptical polarization that is around 90% circular.
We investigate the possibility of forming deeply bound ultracold RbCs molecules by a two-color photoassociation experiment. We compare the results with those for Rb_2 in order to understand the characteristic differences between heteronuclear and homonuclear molecules. The major differences arise from the different long-range potential for excited states. Ultracold 85Rb and 133Cs atoms colliding on the X^1Sigma+ potential curve are initially photoassociated to form excited RbCs molecules in the region below the Rb(5S) + Cs(6P_1/2) asymptote. We explore the nature of the Omega=0^+ levels in thi…
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 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}Π_{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}Σ^{+} electronic ground state. We also compare the observed and calculated laser intensity required to s…
We report the production of ultracold RbCs molecules in the rovibronic ground state, i.e., $X^1Σ^+ (v=0, J=0)$, by short-range photoassociation to the $2^3Π_{0}$ state followed by spontaneous emission. We use narrowband depletion spectroscopy to probe the distribution of rotational levels formed in the $X ^1Σ^+(v=0)$ state. We conclude, based on selection rules, that the primary decay route to $X ^1Σ^+(v=0)$ is a two-step cascade decay that leads to as much as $33\%$ branching into the $J=0$ rotational level. The experimental simplicity of our scheme opens up the possibility of easier access t…
We explore the feasibility of optically forming long-range tetratomic and larger polyatomic molecules in their ground electronic state from ultracold pairs of polar molecules aligned by external fields. Depending on the relative orientation of the interacting diatomic molecules, we find that a tetratomic can be formed either as a weakly bound complex in a very extended halo state or as a pure long-range molecule composed of collinear or nearly-collinear diatomic molecules. The latter is a novel type of tetratomic molecule comprised of two diatomic molecules bound at long intermolecular range a…
We report the production of a high phase-space density mixture of $^{87}$Rb and $^{133}$Cs atoms in a levitated crossed optical dipole trap as the first step towards the creation of ultracold RbCs molecules via magneto-association. We present a simple and robust experimental setup designed for the sympathetic cooling of $^{133}$Cs via interspecies elastic collisions with $^{87}$Rb. Working with the $|F=1, m_F=+1 >$ and the $|3, +3 >$ states of $^{87}$Rb and $^{133}$Cs respectively, we measure a high interspecies three-body inelastic collision rate $\sim 10^{-25}-10^{-26} \rm{cm}^{6}\rm{s}^{-1}…
We demonstrate the production of ultracold polar RbCs molecules in their vibronic ground state, via photoassociation of laser-cooled atoms followed by a laser-stimulated state transfer process. The resulting sample of $X ^1Σ^+ (v=0)$ molecules has a translational temperature of $\sim100 μ$K and a narrow distribution of rotational states. With the method described here it should be possible to produce samples even colder in all degrees of freedom, as well as other bi-alkali species.
We associate Sr atom pairs on sites of a Mott insulator optically and coherently into weakly-bound ground-state molecules, achieving an efficiency above 80\%. This efficiency is 2.5 times higher than in our previous work [S. Stellmer, B. Pasquiou, R. Grimm, and F. Schreck, Phys. Rev. Lett. 109, 115302 (2012)] and obtained through two improvements. First, the lifetime of the molecules is increased beyond one minute by using an optical lattice wavelength that is further detuned from molecular transitions. Second, we compensate undesired dynamic light shifts that occur during the stimulated Raman…
Compared to purely atomic collisions, ultracold molecular collisions potentially support a much larger number of Fano-Feshbach resonances due to the enormous number of ro-vibrational states available. In fact, for alkali-metal dimers we find that the resulting density of resonances cannot be resolved at all, even on the sub-$μ$K temperature scale of ultracold experiments. As a result, all observables become averaged over many resonances and can effectively be described by simpler, non-resonant scattering calculations. Two particular examples are discussed: non-chemically reactive RbCs and chem…
We create fermionic dipolar $^{23}$Na$^6$Li molecules in their triplet ground state from an ultracold mixture of $^{23}$Na and $^6$Li. Using magneto-association across a narrow Feshbach resonance followed by a two-photon STIRAP transfer to the triplet ground state, we produce $3\,{\times}\,10^4$ ground state molecules in a spin-polarized state. We observe a lifetime of $4.6\,\text{s}$ in an isolated molecular sample, approaching the $p$-wave universal rate limit. Electron spin resonance spectroscopy of the triplet state was used to determine the hyperfine structure of this previously unobserve…
Controlling the pathways and outcomes of reactions is a broadly pursued goal in chemistry. In gas phase reactions, this is typically achieved by manipulating the properties of the reactants, including their translational energy, orientation, and internal quantum state. In contrast, here we influence the pathway of a reaction via its intermediate complex, which is generally too short-lived to be affected by external processes. In particular, the ultracold preparation of potassium-rubidium (KRb) reactants leads to a long-lived intermediate complex (K$_2$Rb$_2^*$), which allows us to steer the re…
We argue that the quenched ultracold plasma presents an experimental platform for studying quantum many-body physics of disordered systems in the long-time and finite energy-density limits. We consider an experiment that quenches a plasma of nitric oxide to an ultracold system of Rydberg molecules, ions and electrons that exhibits a long-lived state of arrested relaxation. The qualitative features of this state fail to conform with classical models. Here, we develop a microscopic quantum description for the arrested phase based on an effective many-body spin Hamiltonian that includes both dipo…
We investigate collisional loss in an ultracold mixture of $^{40}$K$^{87}$Rb molecules and $^{87}$Rb atoms, where chemical reactions between the two species are energetically forbidden. Through direct detection of the KRb$_{2}^{*}$ intermediate complexes formed from atom-molecule collisions, we show that a $1064$ nm laser source used for optical trapping of the sample can efficiently deplete the complex population via photo-excitation, an effect which can explain the universal two-body loss observed in the mixture. By monitoring the time-evolution of the KRb$_{2}^{*}$ population after a sudden…
We observed the $A^1Σ^+\sim b^3Π\to a^3Σ^+/X^1Σ^+$ laser-induced fluorescence (LIF) spectra of the RbCs molecule excited from the ground $X^1Σ^+$ state by the Ti:Sapphire laser. The LIF radiation from the common perturbed levels of the singlet-triplet $A\sim b$ complex was recorded by the Fourier-transform (FT) spectrometer with the instrumental resolution of 0.03~cm$^{-1}$. The relative intensity distribution in the rotationally resolved $A\sim b\to a^3Σ^+(v_a)/X^1Σ^+(v_X)$ progressions was measured, and their branching ratio was found to be about of 1$÷$5$ \times$10$^{-4}$ in the bound regio…
We investigate the energy levels of heteronuclear alkali metal dimers in levels correlating with the lowest rotational level of the ground electronic state, which are important in efforts to produce ground-state ultracold molecules. We use density-functional theory to calculate nuclear quadrupole and magnetic coupling constants for RbK and RbCs and explore the hyperfine structure in the presence of electric and magnetic fields. For nonrotating states, the zero-field splittings are dominated by the electron-mediated part of the nuclear spin-spin coupling. They are a few kHz for RbK isotopologs …
Promising pathways for photoassociative formation of ultracold heteronuclear alkali metal dimers in their lowest rovibronic levels (denoted X(0,0)) are examined using high quality ab initio calculations of potential energy curves currently available. A promising pathway for KRb, involving the resonant coupling of the $2 ^1Π$ and $1 ^1Π$ states just below the lowest excited asymptote (K($4s$)+Rb($5p_{1/2}$)), is found to occur also for RbCs and less promisingly for KCs as well. The resonant coupling of the $3 ^1 Σ^+ $ and $1 ^1Π$ states, also just below the lowest excited asymptote, is found to…
We investigate the dynamics of molecular photoexcitation by unchirped femtosecond laser pulses using RbCs as a model system. This study is motivated by a goal of optimizing a two-color scheme of transferring vibrationally-excited ultracold molecules to their absolute ground state. In this scheme the molecules are initially produced by photoassociation or magnetoassociation in bound vibrational levels close to the first dissociation threshold. We analyze here the first step of the two-color path as a function of pulse intensity from the low-field to the high-field regime. We use two different a…
Quantum states with long-lived coherence are essential for quantum computation, simulation and metrology. The nuclear spin states of ultracold molecules prepared in the singlet rovibrational ground state are an excellent candidate for encoding and storing quantum information. However, it is important to understand all sources of decoherence for these qubits, and then eliminate them, in order to reach the longest possible coherence times. Here, we fully characterise the dominant mechanisms for decoherence of a storage qubit in an optically trapped ultracold gas of RbCs molecules using high-reso…
Harnessing the potential wide-ranging quantum science applications of molecules will require control of their interactions. Here, we use microwave radiation to directly engineer and tune the interaction potentials between ultracold calcium monofluoride (CaF) molecules. By merging two optical tweezers, each containing a single molecule, we probe collisions in three dimensions. The correct combination of microwave frequency and power creates an effective repulsive shield, which suppresses the inelastic loss rate by a factor of six, in agreement with theoretical calculations. The demonstrated mic…
We show that radiofrequency (RF) radiation may be used to create Feshbach resonances in ultracold gases of alkali-metal atoms at desired magnetic fields that are convenient for atomic cooling and degeneracy. For the case of $^{39}$K+$^{133}$Cs, where there are no RF-free resonances in regions where Cs may be cooled to degeneracy, we show that a resonance may be created near 21~G with 69.2~MHz RF radiation. This resonance is almost lossless with circularly polarized RF, and the molecules created are long-lived even with plane-polarized RF.
A barrier to realizing the potential of molecules for quantum information science applications is a lack of high-fidelity, single-molecule imaging techniques. Here, we present and theoretically analyze a general scheme for dispersive imaging of electronic ground-state molecules. Our technique relies on the intrinsic anisotropy of excited molecular rotational states to generate optical birefringence, which can be detected through polarization rotation of an off-resonant probe laser beam. Using \narb and \rbcs as examples, we construct a formalism for choosing the molecular state to be imaged an…
This review describes recent experimental and theoretical advances in forming molecules in ultracold gases of trapped alkali metal atoms, both by magnetic tuning through Feshbach resonances and by photoassociation. Molecular Bose-Einstein condensation of long-range states of both boson dimers and fermion dimers was achieved in 2002-3. Condensates of boson dimers were found to be short-lived, but long-lived condensates of fermion dimers have been produced. Signatures of triatomic and tetraatomic molecules have recently been observed. Both homonuclear and heteronuclear molecules have been formed…
Progress in ultracold experiments with polar molecules requires a clear understanding of their interactions and reactivity at ultra-low collisional energies. Two important theoretical steps in this process are the characterization of interaction potentials between molecules and the modeling of reactive scattering mechanism. Here, we report on the {\it abinitio} calculation of isotropic and anisotropic van der Waals interaction potentials for polar KRb and RbCs colliding with each other or with ultracold atoms. Based on these potentials and two short-range scattering parameters we then develop …
We demonstrate a generally applicable technique for mixing two-species quantum degenerate bosonic samples in the presence of an optical lattice, and we employ it to produce low-entropy samples of ultracold 87Rb133Cs Feshbach molecules with a lattice filling fraction exceeding 30%. Starting from two spatially separated Bose-Einstein condensates of Rb and Cs atoms, Rb-Cs atom pairs are efficiently produced by using the superfluid-to-Mott insulator quantum phase transition twice, first for the Cs sample, then for the Rb sample, after nulling the Rb-Cs interaction at a Feshbach resonance's zero cr…
We propose a method to suppress the chemical reactions between ultracold bosonic ground-state $^{23}$Na$^{87}$Rb molecules based on optical shielding. By applying a laser with a frequency blue-detuned from the transition between the lowest rovibrational level of the electronic ground state $X^1Σ^+ (v_X=0, j_X=0)$, and the long-lived excited level $b^3Π_0 (v_b=0, j_b=1)$, the long-range dipole-dipole interaction between the colliding molecules can be engineered, leading to a dramatic suppression of reactive and photoinduced inelastic collisions, for both linear and circular laser polarizations.…
We report a detailed molecular spectroscopy study on the lowest excited electronic states of $^{23}\rm{Na}^{87}\rm{Rb}$ for producing ultracold $^{23}\rm{Na}^{87}\rm{Rb}$ molecules in the electronic, rovibrational and hyperfine ground state. Starting from weakly-bound Feshbach molecules, a series of vibrational levels of the $A^{1}Σ^{+}-b^{3}Π$ coupled excited states were investigated. After resolving, modeling and interpreting the hyperfine structure of several lines, we successfully identified a long-lived level resulting from the accidental hyperfine coupling between the $0^+$ and $0^-$ com…
We investigate the electric field shielding of ultracold collisions of dipolar rotors, initially in their first rotational excited state, using an adimensional approach. We establish a map of good and bad candidates for efficient evaporative cooling based on this shielding mechanism, by presenting the ratio of elastic over quenching processes as a function of a rescaled rotational constant $\tilde{B} = B/s_{E_3}$ and a rescaled electric field $\tilde{F} = dF/B$. $B, d, F, s_{E_3}$ are respectively the rotational constant, the full electric dipole moment of the molecules, the applied electric f…
We present an experimental scheme which combines the well established method of velocity-mapimaging, with a cold trapped metastable neon target. The device is used for obtaining the branching ratios and recoil-ion energy distributions for the penning ionization process in optical collisions of ultracold metastable neon. The potential depth of the highly excited dimer potential is extracted and compared with theoretical calculations. The simplicity to construct, characterize and apply such a device, makes it a unique tool for the low-energy nuclear physics community, enabling opportunities for …
We demonstrate coherent microwave control of rotational and hyperfine states of trapped, ultracold, and chemically stable $^{23}$Na$^{40}$K molecules. Starting with all molecules in the absolute rovibrational and hyperfine ground state, we study rotational transitions in combined magnetic and electric fields and explain the rich hyperfine structure. Following the transfer of the entire molecular ensemble into a single hyperfine level of the first rotationally excited state, $J{=}1$, we observe collisional lifetimes of more than $3\, \rm s$, comparable to those in the rovibrational ground state…
It has long been expected that quantum degenerate gases of molecules would open access to a wide range of phenomena in molecular and quantum sciences. However, the very complexity that makes ultracold molecules so enticing has made reaching degeneracy an outstanding experimental challenge over the past decade. We now report the production of a Fermi degenerate gas of ultracold polar molecules of potassium--rubidium (KRb). Through coherent adiabatic association in a deeply degenerate mixture of a rubidium Bose-Einstein condensate and a potassium Fermi gas, we produce molecules at temperatures b…
We present a combined experimental and theoretical study of the effects of Rydberg interactions on Autler-Townes spectra of ultracold gases of atomic strontium. Realizing two-photon Rydberg excitation via a long-lived triplet state allows us to probe the thus far unexplored regime where Rydberg state decay presents the dominant decoherence mechanism. The effects of Rydberg interactions are observed in shifts, asymmetries, and broadening of the measured atom-loss spectra. The experiment is analyzed within a one-body density matrix approach, accounting for interaction-induced level shifts and de…
We investigate Cs+Cs scattering in excited Zeeman and hyperfine states. We calculate the real and imaginary parts of the s-wave scattering length; the imaginary part directly provides the rate coefficient for 2-body inelastic loss, while the real part allows us to identify regions of magnetic field where 3-body recombination will be slow. We identify field regions where Cs in its $(f,m_f)=(3,+2)$ and $(3,+1)$ states may be stable enough to allow Bose-Einstein condensation, and additional regions for these and the $(3,0)$ and $(3,-3)$ states where high-density clouds should be long-lived.
Femtochemistry techniques have been instrumental in accessing the short time scales necessary to probe transient intermediates in chemical reactions. Here we take the contrasting approach of prolonging the lifetime of an intermediate by preparing reactant molecules in their lowest ro-vibronic quantum state at ultralow temperatures, thereby drastically reducing the number of exit channels accessible upon their mutual collision. Using ionization spectroscopy and velocity-map imaging of a trapped gas of potassium-rubidium molecules at a temperature of 500~nK, we directly observe reactants, interm…
We report an apparatus and method capable of producing Bose-Einstein condensates (BECs) of ~1x10^6 87Rb atoms, and ultimately designed for sympathetic cooling of 133Cs and the creation of ultracold RbCs molecules. The method combines several elements: i) the large recapture of a magnetic quadrupole trap from a magneto-optical trap, ii) efficient forced RF evaporation in such a magnetic trap, iii) the gain in phase-space density obtained when loading the magnetically trapped atoms into a far red-detuned optical dipole trap and iv) efficient evaporation to BEC within the dipole trap. We demonstr…
Collisional resonances are an important tool which has been used to modify interactions in ultracold gases, for realizing novel Hamiltonians in quantum simulations, for creating molecules from atomic gases and for controlling chemical reactions. So far, such resonances have been observed for atom-atom collisions, atom-molecule collisions and collisions between Feshbach molecules which are very weakly bound. Whether such resonances exist for ultracold ground state molecules has been debated due to the possibly high density of states and/or rapid decay of the resonant complex. Here we report a v…
Advances in atomic, molecular, and optical (AMO) physics techniques allowed the cooling of simple molecules down to the ultracold regime ($\lesssim$ 1 mK), and opened the opportunities to study chemical reactions with unprecedented levels of control. This review covers recent developments in studying bimolecular chemistry at ultralow temperatures. We begin with a brief overview of methods for producing, manipulating, and detecting ultracold molecules. We then survey experimental works that exploit the controllability of ultracold molecules to probe and modify their long-range interactions. Fur…