The revolution that has taken place in atomic, molecular, and optical (AMO) physics and physical chemistry since the early 2000s has been made possible by a variety of techniques allowing experiments to reach ultracold temperatures, and to control the interactions between particles. One of the most important tools in the modern ultracold toolkit is the ability to modify and control the behavior of ultracold samples by using resonances. Those resonances can take a variety of forms, such as shape resonances, tunable Feshbach resonances, or lasers resonant with specific states. In this chapter, we review some of the concepts relevant to the study of resonances in ultracold chemical systems, and give a few examples of their applications.
The revolution that has taken place in atomic, molecular, and optical (AMO) physics and physical chemistry since the early 2000s has been made possible by a variety of techniques allowing experiments to reach ultracold temperatures, and to control the interactions between particles. One of the most important tools in the modern ultracold toolkit is the ability to modify and control the behavior of ultracold samples by using resonances. Those resonances can take a variety of forms, such as shape resonances, tunable Feshbach resonances, or lasers resonant with specific states. In this chapter, we review some of the concepts relevant to the study of resonances in ultracold chemical systems, and give a few examples of their applications.
Ultracold chemistry operates in a regime where thermal motion is suppressed to the microkelvin scale, allowing quantum mechanics to dictate every aspect of molecular interaction. This paper reviews the theoretical foundations and experimental breakthroughs that now make coherent control of ultracold reactions possible. It first outlines the separation of short- and long-range physics through quantum defect theory, emphasizing why short-range dynamics remain intractable and why universal loss emerges naturally. It then examines how long-range potentials, resonances, and quantum interference enable tunable scattering behavior. Two major milestones anchor this discussion: phase-coherent atom–atom–molecule coupling, which confirms the transfer and control of reaction phase, and the experimental resolution of long-range atom–molecule Feshbach resonances using a Fabry–P´erot interferometer model. Finally, it highlights the recent observation of a magnetically tunable molecule–molecule Feshbach resonance in NaLi, overturning long-held assumptions about the impossibility of resonance control in complex molecular systems. Together, these results demonstrate that ultracold molecules can be engineered to undergo fully coherent, interference-driven reactions, establishing a framework for quantum-controlled chemistry and laying the groundwork for applications in quantum simulation and computation.
The susceptibility of ultracold gases to precise manipulation via external fields makes them ideal systems to study fundamental quantum mechanical phenomena. Various regimes, which are not possible to reach in condensed matter or nuclear physics, can be probed with these quantum gases. Especially the tunability of the interactions and confining potentials make that these ultracold gases offer unique possibilities to explore and study universal behavior. The tunability of the dominant two-body interactions in dilute ultracold atomic gases stems from the presence of Feshbach resonances. Via these resonances pairs of ultracold atoms can be associated to form ultracold molecules. In fact, measurements of Feshbach resonance positions can be used to reveal part of the underlying molecular structure. Vica versa, accurate molecular Born-Oppenheimer potentials can be used as input for full numerical coupled-channels calculations to reliably predict Feshbach resonances. For most of the heteronuclear mixtures currently studied however, the relevant molecular potentials are not accurate enough. As the coupled-channels method is often too elaborate and too time consuming to be used to fit the measured data to enable the construction of more accurate potentials, a need for accurate models which complement this established method is created. In this thesis we have developed a simplified model for resonant scattering of two ultracold atoms which fulfills this need. The asymptotic bound-state model (ABM) is a hierarchical model which can be systematically increased in complexity and accuracy. In its most simple form, the ABM only needs two parameters to predict the position and strength of Feshbach resonances: Two binding energies corresponding to the least bound state of the two molecular potentials involved. We demonstrate that this model, although it is solely based on bound states, can incorporate threshold effects. Additionally, the model can be extended to include: Multiple vibrational levels, overlapping resonances, and magnetic dipole-dipole interactions. This versatile model allows for a description of Feshbach resonances in a large variety of systems without accurate knowledge of the relevant molecular Born-Oppenheimer potentials. Being computationally light, the ABM can be used to analyze measurements of Feshbach resonances and hereby expose the basic underlying molecular structure. Additionally, the ABM is well suited to map out all available Feshbach resonances in a system. This ability is particularly useful when an optimal resonance is required for a certain experiment. For the 6Li-40K mixture we have utilized this ability to experimentally observe a strong Feshbach resonance which offers promising perspectives to reach the strongly interacting universal regime in a mass-imbalanced Fermi gas. By analyzing the various inelastic decay processes and the accuracy of the ab initio Born-Oppenheimer potentials, we predict a strong resonance in a mixture of metastable bosonic and fermionic helium atoms. For the homonuclear (bosonic as well as fermionic) helium gas we do not find strong resonances. For an ultracold gas of 40K atoms, an elaborate combined theoretical and experimental effort is presented to map out the Feshbach resonance structure. On the experimental side we observed 36 Feshbach resonances, 31 of which where observed for the first time. These observations are in excellent agreement with coupled-channels calculations which use unmodified Born-Oppenheimer potentials as input. On the theoretical side, we present a comparison between different simplified models of resonance scattering and the full numerical coupled-channels calculations. We have developed the resonant state model (RSM) to describe the resonant scattering of two ultracold atoms. This model is founded on resonant states, the natural (eigen) frequencies of the two-body system, and their non-trivial properties. Threshold effects are implicitly build into the RSM. The RSM can describe the effect of the continuum of scattering states, states which are neglected in the ABM, on the position and strength of a Feshbach resonance by only a few resonant states. Especially when a low-energy resonance is embedded in the continuum of scattering states, the effect of these states on the Feshbach resonance cannot be neglected. The RSM can be viewed as the natural generalization of the ABM. As the RSM can be based on just a few resonant states, it retains the computational simplicity of the ABM. Using the tunability of two-body interactions induced by a Feshbach resonance, we describe a crossover for a rotating Fermi gas between two strongly-correlated many-body states. We demonstrate that the correlation induced long-range interaction will shift the crossover with respect to the non-rotating case.
The study of ultracold atomic Fermi gases is a rapidly exploding subject which is defining new directions in condensed matter and atomic physics. Quite generally what makes these gases so important is their remarkable tunability and controllability. Using a Feshbach resonance one can tune the attractive two-body interactions from weak to strong and thereby make a smooth crossover from a BCS superfluid of Cooper pairs to a Bose-Einstein condensed superfluid. Furthermore, one can tune the population of the two spin states, allowing observation of exotic spin-polarized superfluids, such as the Fulde Ferrell Larkin Ovchinnikov (FFLO) phase. A wide array of powerful characterization tools, which often have direct condensed matter analogues, are available to the experimenter. In this Chapter, we present a general review of the status of these Fermi gases with the aim of communicating the excitement and great potential of the field.
In this habilitation-thesis a collection of 14 experiments is presented. In these experiments we have developed and used novel techniques to control ultracold gases on the quantum level. In brief, Bose-Einstein condensates (BEC) and degenerate Fermi gases of laser-cooled alkali atoms are subjected to specially designed optical and magnetic fields. The fields influence in a coherent way the behavior, properties and dynamics of the gases. On this basis we developed tools to prepare, coherently manipulate, and analyze pre-defined quantum states. With this high level of control, it was possible to investigate interesting physics phenomena, and we were able to achieve several breakthroughs in the field of ultracold atoms. Highlights of our experimental results include the demonstration of phase engineering of a BEC wavefunction where we created solitons in a BEC and studied their propagation. In another experiment we constructed a spatially resolved matter wave interferometer with which we mapped out the phase distribution on a condensate. Illuminating the BEC with a periodic pattern, i.e. an optical lattice, allowed us to study solid states physics phenomena. In a second set of experiments we demonstrated optically tuning of the interaction between atoms with optical Feshbach resonances. Employing either magnetically tunable Feshbach resonances or laser radiation, we were able to produce ground state molecules in well defined quantum states. This led to the production of the first molecular BEC. By tuning the coupling of atom pairs in a Fermi gas of atoms, we could for the first time investigate the so-called BEC-BCS crossover which describes the continuous change from a BEC superfluid to a Bardeen-Cooper Schrieffer (BCS) superfluid. Due to the excellent control on the quantum level, the developed cold atom techniques open up intriguing prospects for future applications and experiments. They represent a general tool box to investigate fundamental physical phenomena in a pure and undisturbed environment. In the future, cold atoms might serve as a testing ground for fundamental theories or as quantum simulators for complex systems.
Photoassociation is the process in which two colliding atoms absorb a photon to form an excited molecule. The development of laser-cooling techniques for producing gases at ultracold (<1mK) temperatures allows photoassociation spectroscopy to be performed with very high spectral resolution. Of particular interest is the investigation of molecular states whose properties can be related, with high precision, to the properties of their constituent atoms with the ``complications'' of chemical binding accounted for by a few parameters. These include bound long-range or purely long-range vibrational states in which two atoms spend most or all of their time at large internuclear separations. Low-energy atomic scattering states also share this characteristic. Photoassociation techniques have made important contributions to the study of all of these. This review describes what is special about photoassociation spectroscopy at ultracold temperatures, how it is performed, and a sampling of results including the determination of scattering lengths, their control via optical Feshbach resonances, precision determinations of atomic lifetimes from molecular spectra, limits on photoassociation rates in a Bose-Einstein condensate, and briefly, production of cold molecules. Discussions are illustrated with examples on alkali-metal atoms as well as other species. Progress in the field is already past the point where this review can be exhaustive, but an introduction is provided on the capabilities of photoassociation spectroscopy and the techniques presently in use.
Feshbach resonances are the essential tool to control the interaction between atoms in ultracold quantum gases. They have found numerous experimental applications, opening up the way to important breakthroughs. This review broadly covers the phenomenon of Feshbach resonances in ultracold gases and their main applications. This includes the theoretical background and models for the description of Feshbach resonances, the experimental methods to find and characterize the resonances, a discussion of the main properties of resonances in various atomic species and mixed atomic species systems, and an overview of key experiments with atomic Bose-Einstein condensates, degenerate Fermi gases, and ultracold molecules.