We present and analyze a toolbox for the controlled manipulation of ultracold polar molecules, consisting of detection of molecules, atom-molecule entanglement, and engineering of dissipative dynamics. Our setup is based on fast chemical reactions between molecules and atoms leading to a quantum Zeno-based collisional blockade in the system. We demonstrate that the experimental parameters for achieving high fidelities can be found using a straightforward numerical optimization. We exemplify our approach for a system composed of NaK molecules and Na atoms and we discuss the consequences of residual imperfections such as a finite strength of the quantum Zeno blockade.
We present and analyze a toolbox for the controlled manipulation of ultracold polar molecules, consisting of detection of molecules, atom-molecule entanglement, and engineering of dissipative dynamics. Our setup is based on fast chemical reactions between molecules and atoms leading to a quantum Zeno-based collisional blockade in the system. We demonstrate that the experimental parameters for achieving high fidelities can be found using a straightforward numerical optimization. We exemplify our approach for a system composed of NaK molecules and Na atoms and we discuss the consequences of residual imperfections such as a finite strength of the quantum Zeno blockade.
Polar molecules, with their rich internal structure, offer immense potential for fundamental physics, quantum technology, and controlled chemistry. However, their utilization is currently limited because of slow and imperfect state detection and weak dipolar interaction, limiting fast and large-scale entanglement generation. We propose and analyze a scheme for quantum logic control and measurement-based state preparation in a hybrid platform of polar molecules and neutral atoms. The method leverages fast, high-fidelity atom-molecule gates and high-fidelity atomic ancilla measurements to overcome the common challenges in molecule-only platforms, while preserving their diverse structural advantages. The proposed atom-molecule controlled-phase gate is based on resonant dipole-dipole exchange between a molecular rotational transition and an atomic Rydberg transition, rendering it three orders of magnitude faster than any direct molecule-molecule entangling gate. We further study several applications of our scheme including the preparation of molecular GHZ states for quantum enhanced precision measurements, the preparation of exotic molecular qudit states with topological order, and measurement-altered criticality. Our scheme is applicable to any polar molecule. It expands the paradigm of quantum logic control and paves the way to large-scale molecular entangled states. More generally, it highlights a concrete hybrid quantum system in which each qubit is utilized in an optimal way and where the measurement-based approach can yield a significant advantage in near-term devices.
Ultracold polar molecular quantum gases promise to open new research directions ranging from the study of ultra-cold chemistry, precision measurements to novel quantum phase transitions. Based on the preparation of high-phase space density gases of polar KRb molecules [1–3], I will discuss the control of dipolar collisions and chemical reactions of polar molecules in a regime where quantum statistics, single scattering partial waves, and quantum threshold laws play a dominant role [4]. In particular, I will point out the crucial role of electric dipole-dipole interactions [5] and external confinement [6] in determining the chemical reaction rate. Finally, I will discuss prospects of reaching quantum degeneracy in bialkali samples of polar molecules and prospects for these systems as novel dipolar quantum many-body systems.
Ultracold polar molecular gases promise new directions and exciting appli-cations in precision measurements, ultracold chemistry, electric-field controlled collisions, dipolar quantum gases, and quantum information sciences. This the-sis presents experimental realization of a near quantum degenerate gas of polar molecules, where the phase-space density of the gas achieved is more than 10 or-ders of magnitude higher than previous results. The near quantum degenerate gas of polar molecules is created using two coherent steps. First, atoms in an ul-tracold gas mixture are converted into extremely weakly bound molecules near a Fano-Feshbach resonance. Second, the weakly bound molecules are transferred to the ro-vibronic ground state using a coherent two-photon Raman technique. The fact that these ground-state molecules are polar is confirmed with a spectroscopic measurement of the permanent electric dipole moment. Finally, manipulation of the molecular hyperfine state is demonstrated; this allows molecules to be pop-ulated in a single quantum state, in particular, the lowest energy state. With an ultracold gas of molecules, full control of molecular internal state, and electric field as a new handle, ultracold molecular collisions, including ultracold chemical reactions and dipolar collisions, are studied.
Studying ultracold chemical reactions with quantum state resolution reveals details of the reaction processes, especially with single quantum state preparation of the reactants and state-selective detection of reaction products. In this thesis, we investigate two main processes: KRb + KRb → K2 + Rb2 reactions, and Rb and KRb atom-molecule collisions. In the KRb bimolecular reaction, we demonstrate the preservation of quantum coherence in bimolecular reactions for the first time, which is surprising in a reaction considered to be largely chaotic. Additionally, we proposed a coherent control scheme to manipulate product yields across different product channels. These results represent a critical step toward probing quantum coherence and entanglement in the chemical reaction. In atom-molecule collisions between Rb and KRb, we discovered an exceptionally long-lived intermediate complex, KRb2, which can be photo-excited by trapping light. The observed complex lifetime was orders of magnitude longer than theoretical predictions, underscoring the limitations of the current theory. We further explored the dependence of complex lifetimes on the initial quantum states and external electric and magnetic fields, providing additional experimental benchmarks to guide future theoretical work. Separately, we found that inelastic collisions between hyperfine-excited Rb atoms and KRb molecules can lead to rotation excitation of KRb post-collision. By probing the product state distribution, the result suggests that mechanical angular momentum is coupled to the spins. Such couplings are too weak in the current theory models to explain the result. Moreover, our result contradicts state-of-the-art coupled-channel calculations. These suggest that some subtle effects, such as molecular vibration and conical intersections, play a critical role in the reaction dynamics. The final piece of the thesis describes the observation of resonant interaction between a Rydberg atom and an ensemble of polar molecules. Such hybrid quantum systems have been proposed for a wide range of applications. Our work provides an experimental demonstration of resonant dipolar interactions between Rydberg atoms and ultracold polar molecules, paving the way for the realization of hybrid systems for quantum computation and simulation.
Advances in atomic, molecular, and optical physics techniques allowed the cooling of simple molecules down to the ultracold regime ([Formula: see text]1 mK) and opened 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. Further combining the use of physical chemistry techniques such as mass spectrometry and ion imaging significantly improved the detection of ultracold reactions and enabled explorations of their dynamics in the short range. We discuss a series of studies on the reaction KRb + KRb → K 2 + Rb 2 initiated below 1 μK, including the direct observation of a long-lived complex, the demonstration of product rotational state control via conserved nuclear spins, and a test of the statistical model using the complete quantum state distribution of the products.
This article reviews the current state of the art in the field of cold and ultracold molecules and demonstrates that chemical reactions, inelastic collisions and dissociation of molecules at subkelvin temperatures can be manipulated with external electric or magnetic fields. The creation of ultracold molecules may allow for spectroscopy measurements with extremely high precision and tests of fundamental symmetries of nature, quantum computation with molecules as qubits, and controlled chemistry. The probability of chemical reactions and collisional energy transfer can be very large at temperatures near zero kelvin. The collision energy of ultracold atoms and molecules is much smaller than perturbations due to interactions with external electric or magnetic fields available in the laboratory. External fields may therefore be used to induce dissociation of weakly bound molecules, stimulate forbidden electronic transitions, suppress the effect of centrifugal barriers in outgoing reaction channels or tune Feshbach resonances that enhance chemical reactivity.