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arXiv:2403.09291 · Nature Communications

Parametric tuning of quantum phase transitions in ultracold reactions

Vijay Ganesh Sadhasivam, Fumika Suzuki, Bin Yan, Nikolai A. Sinitsyn

Published Nov 26, 2024• 10 citations
arXivHTMLPDF

Abstract

Advances in atomic physics have led to the possibility of a coherent transformation between ultracold atoms and molecules including between completely bosonic condensates. Such transformations are enabled by the magneto-association of atoms at a Feshbach resonance which results in a passage through a quantum critical point. In this study, we show that the presence of generic interaction between the constituent atoms and molecules can fundamentally alter the nature of the critical point, change the yield of the reaction and the order of the consequent phase transition. We find that the correlations introduced by this interaction induce nontrivial many-body physics such as coherent oscillations between atoms and molecules, and a selective formation of squeezed molecular quantum states and quantum cat states. We provide analytical and numerical descriptions of these effects, along with scaling laws for the reaction yield in non-adiabatic regimes.

DOI
10.1038/s41467-024-54489-3

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Advances in atomic physics have led to the possibility of a coherent transformation between ultracold atoms and molecules including between completely bosonic condensates. Such transformations are enabled by the magneto-association of atoms at a Feshbach resonance which results in a passage through a quantum critical point. In this study, we show that the presence of generic interaction between the constituent atoms and molecules can fundamentally alter the nature of the critical point, change the yield of the reaction and the order of the consequent phase transition. We find that the correlations introduced by this interaction induce nontrivial many-body physics such as coherent oscillations between atoms and molecules, and a selective formation of squeezed molecular quantum states and quantum cat states. We provide analytical and numerical descriptions of these effects, along with scaling laws for the reaction yield in non-adiabatic regimes.
We map the phase diagram of a two-mode atom-molecule Bose-Einstein condensate with Fano-Feshbach and coherent three-body recombination (cTBR) terms. The standard second order phase transition observed as the molecular energy is tuned through the Feshbach resonance, is replaced by a first order transition when cTBR becomes prominent, due to a double-well structure in the free energy landscape. This transition is associated with atom-molecule entanglement, bistability, and molecular metastability. Our results establish cTBR as a powerful knob for quantum state engineering and control of reaction dynamics in ultracold chemistry.
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.
Abstract We adopt a modified spin-boson model to investigate the quantum phase transition in an ultracold atom-molecule conversion system involving molecule–molecule interaction. We explore the properties of ground state, entanglement entropy, and many-body dynamics, which confirm that the system exhibits a second-order phase transition from a pure atom phase to a mixed atom-molecule phase when the energy detuning is below a critical value. We obtain three scaling laws and the corresponding two critical exponents to characterize the phase transition. In particular, we discuss the effects of both the speed of ground-state dynamical evolution and the strength of molecular interaction on the phase transition. The adiabatic evolution condition is obtained as well. Our results show that the molecular interaction can greatly reduce the upper bound of the adiabatic condition, which provides a theoretical basis for easier observation of the phase transition in experiments.
We solve a model that describes a stimulated conversion between ultracold bosonic atoms and molecules. The reaction is triggered by a linearly time-dependent transition throughout the Feshbach resonance. Our solution predicts a dependence, with a dynamic phase transition, of the reaction efficiency on the transition rate for both atoms-to-molecule pairing and molecular dissociation processes. We find that for the latter process with a linear energy dispersion of atomic modes, the emerging phase can have a thermalized energy distribution of noninteracting bosons with the temperature defined by the rate of the transition. This provides a simple interpretation of the phase transition in terms of the creation of equilibrium Bose-Einstein condensate.
Trapped cold atoms at very low temperatures, now readily accessible experimentally, can be controlled and serve as a testing ground for many theoretical physical properties which are paralleled in condensed matter systems. Ultracold trapped atom experiments show promise to recreate analogous condensed matter systems in a controlled environment and to create novel many-body quantum states of matter. The tunability of trapping laser intensities and magnetically controlled Feshbach interactions are the main tools for varying lattice hopping strengths and inter-particle interactions. In this thesis, we search for the phase of a many-body system of cold fermion atoms that can convert to boson molecules and vice versa. We then look at the microscopic details of two atoms that interact to form a quasibound molecule. Our two-atom model explains the mechanism behind the magnetically tunable interparticle interaction known as the Feshbach resonance. We find a dependence of the bound pair formation on the two-particle energy. Our results show that if a magnetic field can be fine tuned to sufficient precision, of order 10 mG, a narrow resonance can be achieved where longer lived bound states can be created. This narrow resonance reconciliates the two-body physics with the effective Hamiltonian that describes the many-body system.
The recent observations of a stable molecular condensate emerging from a condensate of bosonic atoms and related ``super-chemical'' dynamics have raised an intriguing set of questions. Here we provide a microscopic understanding of this unexpected stability and dynamics in atom-molecule superfluids; we show one essential element behind these phenomena is an extremely narrow Feshbach resonance in 133Cs^{133}\mathrm{Cs}133Cs at 19.849G. Comparing theory and experiment, we demonstrate how this narrow resonance enables the dynamical creation of a large closed-channel molecular fraction superfluid, appearing in the vicinity of unitarity. Theoretically, the observed superchemistry (i.e., Bose-enhanced reactions of atoms and molecules) is found to be assisted by the formation of Cooper-like pairs of bosonic atoms that have opposite momenta. Importantly, this narrow resonance opens the possibility to explore the quantum critical point of a molecular Bose superfluid and related phenomena which would not be possible near a more typically broad Feshbach resonance.