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Chemistry near absolute zero: optical control of ultracold atomic collisions

Vanderlei Salvador Bagnato, J. Weiner

Published Jan 1, 1996• 0 citations
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Molecules near absolute zero and external field control of atomic and molecular dynamics

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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.

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Photodissociation of a diatomic molecule in the quantum regime reveals ultracold chemistry

Mickey McDonald, B. H. McGuyer, Fabian A. C. Apfelbeck +4 more

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.

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Quantum control of reactions and collisions at ultralow temperatures

Bo Zhao, Jian-Wei Pan

At temperatures close to absolute zero, the molecular reactions and collisions are dominantly governed by quantum mechanics. Remarkable quantum phenomena such as quantum tunneling, quantum threshold behavior, quantum resonances, quantum interference, and quantum statistics are expected to be the main features in ultracold reactions and collisions. Ultracold molecules offer great opportunities and challenges in the study of these intriguing quantum phenomena in molecular processes. In this article, we review the recent progress in the preparation of ultracold molecules and the study of ultracold reactions and collisions using ultracold molecules. We focus on the controlled ultracold chemistry and the scattering resonances at ultralow temperatures. The challenges in understanding the complex ultracold reactions and collisions are also discussed.

Chemical Society Reviews•Jan 1, 2022•23 citations
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.
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^{88}88Sr2_22​ 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.
At temperatures close to absolute zero, the molecular reactions and collisions are dominantly governed by quantum mechanics. Remarkable quantum phenomena such as quantum tunneling, quantum threshold behavior, quantum resonances, quantum interference, and quantum statistics are expected to be the main features in ultracold reactions and collisions. Ultracold molecules offer great opportunities and challenges in the study of these intriguing quantum phenomena in molecular processes. In this article, we review the recent progress in the preparation of ultracold molecules and the study of ultracold reactions and collisions using ultracold molecules. We focus on the controlled ultracold chemistry and the scattering resonances at ultralow temperatures. The challenges in understanding the complex ultracold reactions and collisions are also discussed.