Chemical reactions at temperatures near absolute zero require a full quantum description of the reaction pathways and enable enhanced control of the products via quantum state selection. Ultracold molecule experiments have provided initial insight into the quantum nature of basic chemical processes involving diatomic molecules, for example from studies of bimolecular reactions, but complete control over the reactants and products has remained elusive. The half-collision process of photodissociation is an indispensable tool in molecular physics and offers significantly more control than the reverse process of photoassociation. Here we reach a fully quantum regime with photodissociation of ultracold $^{88}$ Sr $_2$ molecules where the initial bound state of the molecule and the target continuum state of the fragments are strictly controlled. Detection of the photodissociation products via optical absorption imaging reveals the hallmarks of ultracold chemistry: resonant and nonresonant barrier tunneling, importance of quantum statistics, presence of forbidden reaction pathways, and matter wave interference of reaction products. In particular, this interference yields fragment angular distributions with a strong breaking of cylindrical symmetry, so far unobserved in photodissociation. We definitively show that the quasiclassical description of photodissociation fails in the ultracold regime. Instead, a quantum model accurately reproduces our results and yields new intuition.Chemical reactions at temperatures near absolute zero require a full quantum description of the reaction pathways and enable enhanced control of the products via quantum state selection. Ultracold molecule experiments have provided initial insight into the quantum nature of basic chemical processes involving diatomic molecules, for example from studies of bimolecular reactions, but complete control over the reactants and products has remained elusive. The half-collision process of photodissociation is an indispensable tool in molecular physics and offers significantly more control than the reverse process of photoassociation. Here we reach a fully quantum regime with photodissociation of ultracold $^{88}$Sr$_2$ molecules where the initial bound state of the molecule and the target continuum state of the fragments are strictly controlled. Detection of the photodissociation products via optical absorption imaging reveals the hallmarks of ultracold chemistry: resonant and nonresonant barrier tunneling, importance of quantum statistics, presence of forbidden reaction pathways, and matter wave interference of reaction products. In particular, this interference yields fragment angular distributions with a strong breaking of cylindrical symmetry, so far unobserved in photodissociation. We definitively show that the quasiclassical description of photodissociation fails in the ultracold regime. Instead, a quantum model accurately reproduces our results and yields new intuition.

Dec 21, 20150 citations

A cryogenic circuit cools from afar

Johanna L. Miller

A cloud of ultracold ions can lower the temperature of a trapped proton 9 cm away.

Physics TodayNov 1, 20210 citations

Quantum dynamics and control of ultracold molecules in external fields

Michał Tomza

Jun 10, 20140 citations

Ultracold molecules in an optical tweezer array: From dipolar interaction to ground state cooling

Yicheng Bao

Ultracold molecules are attractive candidates for various applications including ultracold chemistry, quantum information processing, quantum simulation and searches for physics beyond the standard model. Combined with optical tweezer techniques, an optical tweezer array of ultracold polar molecules holds promise for versatile quantum applications. Their long-lived molecular rotational states form robust qubits, while the long-range dipolar interaction between molecules provides quantum entanglement. In this thesis, we build a new generation experiment of optical tweezer array of ultracold CaF molecules. We optically transport the laser cooled and optically trapped molecules into a science glass cell using a hybrid method, where high numerical aperture optical access allows for tighter optical tweezers. In an array of these tight optical tweezers, we demonstrate dipolar spin-exchange interactions between single CaF molecules for the first time. We realize the spin- $\frac{1}{2}$ quantum XY model by encoding an effective spin- $\frac{1}{2}$ system into the rotational states of the molecules, and use it to generate a Bell state through an iSWAP operation. Conditioned on the verified existence of molecules in both tweezers at the end of the measurement, we obtain a Bell state fidelity of 0.89(6). Employing interleaved tweezer arrays, we demonstrate single site molecular addressability. To further improve the platform, cooling of the molecules to near the motional ground state is crucial for reducing various dephasings. We demonstrate Raman sideband cooling (RSC) of CaF molecules in optical tweezers to near their 3-D motional ground state, with a 3-D motional ground state probability of $54\pm18\%$ of the molecules that survive the RSC. This paves the way to increase molecular coherence times in optical tweezers for robust quantum information processing and simulation applications in the near future.Ultracold molecules are attractive candidates for various applications including ultracold chemistry, quantum information processing, quantum simulation and searches for physics beyond the standard model. Combined with optical tweezer techniques, an optical tweezer array of ultracold polar molecules holds promise for versatile quantum applications. Their long-lived molecular rotational states form robust qubits, while the long-range dipolar interaction between molecules provides quantum entanglement. In this thesis, we build a new generation experiment of optical tweezer array of ultracold CaF molecules. We optically transport the laser cooled and optically trapped molecules into a science glass cell using a hybrid method, where high numerical aperture optical access allows for tighter optical tweezers. In an array of these tight optical tweezers, we demonstrate dipolar spin-exchange interactions between single CaF molecules for the first time. We realize the spin-$\frac{1}{2}$ quantum XY model by encoding an effective spin-$\frac{1}{2}$ system into the rotational states of the molecules, and use it to generate a Bell state through an iSWAP operation. Conditioned on the verified existence of molecules in both tweezers at the end of the measurement, we obtain a Bell state fidelity of 0.89(6). Employing interleaved tweezer arrays, we demonstrate single site molecular addressability. To further improve the platform, cooling of the molecules to near the motional ground state is crucial for reducing various dephasings. We demonstrate Raman sideband cooling (RSC) of CaF molecules in optical tweezers to near their 3-D motional ground state, with a 3-D motional ground state probability of $54\pm18\%$ of the molecules that survive the RSC. This paves the way to increase molecular coherence times in optical tweezers for robust quantum information processing and simulation applications in the near future.

Jan 1, 20240 citations

Quantum engineering and chemistry with ultracold molecules

Kang-Kuen Ni

Bulletin of the American Physical SocietyJun 1, 20200 citations

^{88}

_2

molecules where the initial bound state of the molecule and the target continuum state of the fragments are strictly controlled. Detection of the photodissociation products via optical absorption imaging reveals the hallmarks of ultracold chemistry: resonant and nonresonant barrier tunneling, importance of quantum statistics, presence of forbidden reaction pathways, and matter wave interference of reaction products. In particular, this interference yields fragment angular distributions with a strong breaking of cylindrical symmetry, so far unobserved in photodissociation. We definitively show that the quasiclassical description of photodissociation fails in the ultracold regime. Instead, a quantum model accurately reproduces our results and yields new intuition.

\frac{1}{2}

quantum XY model by encoding an effective spin-

\frac{1}{2}

system into the rotational states of the molecules, and use it to generate a Bell state through an iSWAP operation. Conditioned on the verified existence of molecules in both tweezers at the end of the measurement, we obtain a Bell state fidelity of 0.89(6). Employing interleaved tweezer arrays, we demonstrate single site molecular addressability. To further improve the platform, cooling of the molecules to near the motional ground state is crucial for reducing various dephasings. We demonstrate Raman sideband cooling (RSC) of CaF molecules in optical tweezers to near their 3-D motional ground state, with a 3-D motional ground state probability of

54\pm18\%

of the molecules that survive the RSC. This paves the way to increase molecular coherence times in optical tweezers for robust quantum information processing and simulation applications in the near future.