D. S. Jin

Observation of dipolar spin-exchange interactions with lattice-confined polar molecules

With the recent production of polar molecules in the quantum regime [1, 2], long-range dipolar interactions are expected to facilitate the understanding of strongly interacting many-body quantum systems and to realize lattice spin models [3] for exploring quantum magnetism. In atomic systems, where interactions require wave function overlap, effective spin interactions on a lattice can be realized through superexchange; however, the coupling is relatively weak and limited to nearest-neighbor interactions [4–6]. In contrast, dipolar interactions exist even in the absence of tunneling and extend beyond nearest neighbors. This allows coherent spin dynamics to persist even for gases with relatively high entropy and low lattice filling. While measured effects of dipolar interactions in ultracold molecular gases have thus far been limited to the modification of inelastic collisions and chemical reactions [7, 8], we now report the first observation of dipolar interactions of polar molecules pinned in a three-dimensional optical lattice. We realize a lattice spin model where spin is encoded in rotational states of molecules that are prepared and probed by microwaves. This interaction arises from the resonant exchange of rotational angular momentum between two molecules and realizes a spin-exchange interaction. The dipolar interactions are apparent in the evolution of the spin coherence, where we observe clear oscillations in addition to an overall decay of the coherence. The frequency of these oscillations, the strong dependence of the spin coherence time on the lattice filling factor, and the effect of a multi-pulse sequence designed to reverse dynamics due to two-body exchange interactions all provide clear evidence of dipolar interactions. Furthermore, we demonstrate the suppression of loss in weak lattices due to a quantum Zeno mechanism [9]. Measurements of these tunneling-induced losses allow us to independently determine the lattice filling factor. The results reported here comprise an initial exploration of the behavior of many-body spin models with direct, long-range spin interactions and lay the groundwork for future studies of many-body dynamics in spin lattices.With the production of polar molecules in the quantum regime, long-range dipolar interactions are expected to facilitate understanding of strongly interacting many-body quantum systems and to realize lattice spin models for exploring quantum magnetism. In ordinary atomic systems, where contact interactions require wavefunction overlap, effective spin interactions on a lattice can be mediated by tunnelling, through a process referred to as superexchange; however, the coupling is relatively weak and is limited to nearest-neighbour interactions. In contrast, dipolar interactions exist even in the absence of tunnelling and extend beyond nearest neighbours. This allows coherent spin dynamics to persist even for gases with relatively high entropy and low lattice filling. Measured effects of dipolar interactions in ultracold molecular gases have been limited to the modification of inelastic collisions and chemical reactions. Here we use dipolar interactions of polar molecules pinned in a three-dimensional optical lattice to realize a lattice spin model. Spin is encoded in rotational states of molecules that are prepared and probed by microwaves. Resonant exchange of rotational angular momentum between two molecules realizes a spin-exchange interaction. The dipolar interactions are apparent in the evolution of the spin coherence, which shows oscillations in addition to an overall decay of the coherence. The frequency of these oscillations, the strong dependence of the spin coherence time on the lattice filling factor and the effect of a multipulse sequence designed to reverse dynamics due to two-body exchange interactions all provide evidence of dipolar interactions. Furthermore, we demonstrate the suppression of loss in weak lattices due to a continuous quantum Zeno mechanism. Measurements of these tunnelling-induced losses allow us to determine the lattice filling factor independently. Our work constitutes an initial exploration of the behaviour of many-body spin models with direct, long-range spin interactions and lays the groundwork for future studies of many-body dynamics in spin lattices.

Creation of a low-entropy quantum gas of polar molecules in an optical lattice

Filling a molecular lattice of light Cold atoms in optical lattices normally interact only when two of them occupy the same lattice site. More-complex interactions would expand the potential of the system for quantum simulation. A promising approach is to use polar molecules instead of atoms, which interact at much longer length scales. However, “packing” the lattice with molecules is tricky. Moses et al. introduced bosonic 87Rb atoms and fermionic 40K atoms into an optical lattice, combined them into molecules, and brought the molecules into their ground state, achieving a considerable lattice filling of 25%. Science, this issue p. 659 Bosonic rubidium-87 atoms and fermionic potassium-40 atoms combine into molecules in an optical lattice, achieving a lattice filling of 25%. Ultracold polar molecules, with their long-range electric dipolar interactions, offer a unique platform for studying correlated quantum many-body phenomena. However, realizing a highly degenerate quantum gas of molecules with a low entropy per particle is challenging. We report the synthesis of a low-entropy quantum gas of potassium-rubidium molecules (KRb) in a three-dimensional optical lattice. We simultaneously load into the optical lattice a Mott insulator of bosonic Rb atoms and a single-band insulator of fermionic K atoms. Then, using magnetoassociation and optical state transfer, we efficiently produce ground-state molecules in the lattice at those sites that contain one Rb and one K atom. The achieved filling fraction of 25% should enable future studies of transport and entanglement propagation in a many-body system with long-range dipolar interactions.

Observation of Resonance Condensation of Fermionic Atom Pairs

We have observed condensation of fermionic atom pairs in the BCS-BEC crossover regime. A trapped gas of fermionic 40K atoms is evaporatively cooled to quantum degeneracy and then a magnetic-field Feshbach resonance is used to control the atom-atom interactions. The location of this resonance is precisely determined from low-density measurements of molecule dissociation. In order to search for condensation on either side of the resonance, we introduce a technique that pairwise projects fermionic atoms onto molecules; this enables us to measure the momentum distribution of fermionic atom pairs. The transition to condensation of fermionic atom pairs is mapped out as a function of the initial atom gas temperature T compared to the Fermi temperature T(F) for magnetic-field detunings on both the BCS and BEC sides of the resonance.

A High Phase-Space-Density Gas of Polar Molecules

A quantum gas of ultracold polar molecules, with long-range and anisotropic interactions, not only would enable explorations of a large class of many-body physics phenomena but also could be used for quantum information processing. We report on the creation of an ultracold dense gas of potassium-rubidium (40K87Rb) polar molecules. Using a single step of STIRAP (stimulated Raman adiabatic passage) with two-frequency laser irradiation, we coherently transfer extremely weakly bound KRb molecules to the rovibrational ground state of either the triplet or the singlet electronic ground molecular potential. The polar molecular gas has a peak density of 1012 per cubic centimeter and an expansion-determined translational temperature of 350 nanokelvin. The polar molecules have a permanent electric dipole moment, which we measure with Stark spectroscopy to be 0.052(2) Debye (1 Debye = 3.336 × 10–30 coulomb-meters) for the triplet rovibrational ground state and 0.566(17) Debye for the singlet rovibrational ground state.

Emergence of a molecular Bose–Einstein condensate from a Fermi gas

The realization of superfluidity in a dilute gas of fermionic atoms, analogous to superconductivity in metals, represents a long-standing goal of ultracold gas research. In such a fermionic superfluid, it should be possible to adjust the interaction strength and tune the system continuously between two limits: a Bardeen–Cooper–Schrieffer (BCS)-type superfluid (involving correlated atom pairs in momentum space) and a Bose–Einstein condensate (BEC), in which spatially local pairs of atoms are bound together. This crossover between BCS-type superfluidity and the BEC limit has long been of theoretical interest, motivated in part by the discovery of high-temperature superconductors. In atomic Fermi gas experiments superfluidity has not yet been demonstrated; however, long-lived molecules consisting of locally paired fermions have been reversibly created. Here we report the direct observation of a molecular Bose–Einstein condensate created solely by adjusting the interaction strength in an ultracold Fermi gas of atoms. This state of matter represents one extreme of the predicted BCS–BEC continuum.

Creation of ultracold molecules from a Fermi gas of atoms

Following the realization of Bose–Einstein condensates in atomic gases, an experimental challenge is the production of molecular gases in the quantum regime. A promising approach is to create the molecular gas directly from an ultracold atomic gas; for example, bosonic atoms in a Bose-Einstein condensate have been coupled to electronic ground-state molecules through photoassociation or a magnetic field Feshbach resonance. The availability of atomic Fermi gases offers the prospect of coupling fermionic atoms to bosonic molecules, thus altering the quantum statistics of the system. Such a coupling would be closely related to the pairing mechanism in a fermionic superfluid, predicted to occur near a Feshbach resonance. Here we report the creation and quantitative characterization of ultracold 40K2 molecules. Starting with a quantum degenerate Fermi gas of atoms at a temperature of less than 150 nK, we scan the system over a Feshbach resonance to create adiabatically more than 250,000 trapped molecules; these can be converted back to atoms by reversing the scan. The small binding energy of the molecules is controlled by detuning the magnetic field away from the Feshbach resonance, and can be varied over a wide range. We directly detect these weakly bound molecules through their radio-frequency photodissociation spectra; these probe the molecular wavefunction, and yield binding energies that are consistent with theory.

Quantum-State Controlled Chemical Reactions of Ultracold Potassium-Rubidium Molecules

Colliding in the Cold Chemical reactions occur through molecular collisions, which, in turn, are governed by the distributions of energy in each colliding partner. What happens when molecules are cooled so that they no longer have sufficient energy to collide? Ospelkaus et al. (p. 853; see the Perspective by Hutson) explored this question by preparing a laser-cooled sample of potassium rubidium (KRb) diatomics with barely any residual energy in any form (translational, rotational, vibrational, or electronic). By monitoring heat release over time, evidence was gathered for exothermic atom exchange reactivity through quantum mechanical tunneling. As predicted by theory, these reactions were exquisitely sensitive to the molecular states, with rates changing by orders of magnitude on varying minor factors such as nuclear spin orientation. Reactions mediated by quantum mechanical tunneling are observed, even in a sample of molecules cooled almost to a standstill. How does a chemical reaction proceed at ultralow temperatures? Can simple quantum mechanical rules such as quantum statistics, single partial-wave scattering, and quantum threshold laws provide a clear understanding of the molecular reactivity under a vanishing collision energy? Starting with an optically trapped near–quantum-degenerate gas of polar 40K87Rb molecules prepared in their absolute ground state, we report experimental evidence for exothermic atom-exchange chemical reactions. When these fermionic molecules were prepared in a single quantum state at a temperature of a few hundred nanokelvin, we observed p-wave–dominated quantum threshold collisions arising from tunneling through an angular momentum barrier followed by a short-range chemical reaction with a probability near unity. When these molecules were prepared in two different internal states or when molecules and atoms were brought together, the reaction rates were enhanced by a factor of 10 to 100 as a result of s-wave scattering, which does not have a centrifugal barrier. The measured rates agree with predicted universal loss rates related to the two-body van der Waals length.

Dipolar collisions of polar molecules in the quantum regime

Ultracold polar molecules offer the possibility of exploring quantum gases with interparticle interactions that are strong, long-range and spatially anisotropic. This is in stark contrast to the much studied dilute gases of ultracold atoms, which have isotropic and extremely short-range (or ‘contact’) interactions. Furthermore, the large electric dipole moment of polar molecules can be tuned using an external electric field; this has a range of applications such as the control of ultracold chemical reactions, the design of a platform for quantum information processing and the realization of novel quantum many-body systems. Despite intense experimental efforts aimed at observing the influence of dipoles on ultracold molecules, only recently have sufficiently high densities been achieved. Here we report the experimental observation of dipolar collisions in an ultracold molecular gas prepared close to quantum degeneracy. For modest values of an applied electric field, we observe a pronounced increase in the loss rate of fermionic potassium–rubidium molecules due to ultracold chemical reactions. We find that the loss rate has a steep power-law dependence on the induced electric dipole moment, and we show that this dependence can be understood in a relatively simple model based on quantum threshold laws for the scattering of fermionic polar molecules. In addition, we directly observe the spatial anisotropy of the dipolar interaction through measurements of the thermodynamics of the dipolar gas. These results demonstrate how the long-range dipolar interaction can be used for electric-field control of chemical reaction rates in an ultracold gas of polar molecules. Furthermore, the large loss rates in an applied electric field suggest that creating a long-lived ensemble of ultracold polar molecules may require confinement in a two-dimensional trap geometry to suppress the influence of the attractive, ‘head-to-tail’, dipolar interactions.

Using photoemission spectroscopy to probe a strongly interacting Fermi gas

Ultracold atomic gases provide model systems in which to study many-body quantum physics. Recent experiments using Fermi gases have demonstrated a phase transition to a superfluid state with strong interparticle interactions. This system provides a realization of the ‘BCS–BEC crossover’ connecting the physics of Bardeen–Cooper–Schrieffer (BCS) superconductivity with that of Bose–Einstein condensates (BECs). Although many aspects of this system have been investigated, it has not yet been possible to measure the single-particle excitation spectrum (a fundamental property directly predicted by many-body theories). Here we use photoemission spectroscopy to directly probe the elementary excitations and energy dispersion in a strongly interacting Fermi gas of 40K atoms. In the experiments, a radio-frequency photon ejects an atom from the strongly interacting system by means of a spin-flip transition to a weakly interacting state. We measure the occupied density of single-particle states at the cusp of the BCS–BEC crossover and on the BEC side of the crossover, and compare these results to that for a nearly ideal Fermi gas. We show that, near the critical temperature, the single-particle spectral function is dramatically altered in a way that is consistent with a large pairing gap. Our results probe the many-body physics in a way that could be compared to data for the high-transition-temperature superconductors. As in photoemission spectroscopy for electronic materials, our measurement technique for ultracold atomic gases directly probes low-energy excitations and thus can reveal excitation gaps and/or pseudogaps. Furthermore, this technique can provide an analogue of angle-resolved photoemission spectroscopy for probing anisotropic systems, such as atoms in optical lattice potentials.

Measurement of positive and negative scattering lengths in a Fermi gas of atoms.

We report on progress toward realizing a predicted superfluid phase in a Fermi gas of atoms. We present measurements of both large positive and large negative scattering lengths in a quantum degenerate Fermi gas of atoms near a magnetic-field Feshbach resonance. We employ an rf spectroscopy technique to directly measure the mean-field interaction energy, which is proportional to the s-wave scattering length. Near the peak of the resonance we observe a saturation of the interaction energy; it is in this strongly interacting regime that superfluidity is predicted to occur. We have also observed anisotropic expansion of the gas, which has recently been suggested as a signature of superfluidity. However, we find that this can be attributed to a purely collisional effect.