A Bi-Axial Quantum State That Controls Molecular Collisions Like a Double-Slit Interferometer

Perreault, William E.; Zhou, Haowen; Mukherjee, Nandini; Zare, Richard N.

doi:10.3389/fphy.2021.671997

Cited by 6 publications

(6 citation statements)

References 37 publications

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“…As such, scattering from the coupled orientations of the biaxial state mimics the way that a photon or particle simultaneously experiences the two mechanical slits in a traditional double-slit scattering experiment. Our earlier theoretical study ( 37 ) showed that the biaxial state is capable of producing an interference pattern in the scattering intensity in the plane perpendicular to the collision velocity. In this study, we experimentally demonstrate the double-slit action and show that the interference is evident in the scattering distribution projected parallel to the collision velocity.…”

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confidence: 99%

Quantum mechanical double slit for molecular scattering

Zhou

Perreault

Mukherjee

et al. 2021

Science

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Double slits with molecular states Despite decades of research, the role of quantum mechanical effects in molecular scattering has not yet been fully investigated and can still demonstrate fascinating results, even for simple triatomic systems. Zhou et al . show that the entangled bond axis orientations in the biaxial state of a deuterium molecule can act as the two slits of a double-slit interferometer for rotationally inelastic collision with a helium atom, giving rise to quantum interference between two indistinguishable pathways (see the Perspective by Wang and Yang). The present work presents an elegant example of quantum interference in molecular scattering that is conceptually similar to the famous Young’s optical double-slit experiment. The proposed molecular interferometer could be used to coherently control the phases in various molecular processes in future experiments. —YS

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confidence: 99%

Quantum mechanical double slit for molecular scattering

Zhou

Perreault

Mukherjee

et al. 2021

Science

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“…For inelastic collisions of NO(A 2 Σ) with He, Chandler and co-workers determined how the orientation of the product’s angular momentum ( j ′) depends on the initial orientation of the NO molecule . In Brouard’s group, differences in the differential cross-sections (DCSs) for collisions between rare gases (Rg) and NO(X 2 Π) molecules were observed depending on the NO orientation: whether the collision was head-on or side-on and whether the Rg hits the molecule close to the O or N atom. − Zare and co-workers exploited the combination of copropagating molecular beams with the Stark-induced adiabatic Raman passage (SARP) method for state preparation and alignment of the molecules. − ,− In these experiments, the colliding molecules are copropagated in the same molecular beam, allowing relative collision energies near 1 K although the molecular velocities in the laboratory frame are much higher (about 2000 m/s). This is a particularly interesting regime which, when combined with the SARP method, allows for the study of sterodynamical preferences where only a few partial-waves contribute.…”

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Role of Low Energy Resonances in the Stereodynamics of Cold He + D₂ Collisions

Jambrina

Morita

Croft

et al. 2022

J. Phys. Chem. Lett.

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In recent experiments using the Stark-induced adiabatic Raman passage technique, Zhou et al. (J. Chem. Phys. 2021, 154, 104309; Science 2021, 374, 960−964) measured the product's angular distribution for the collisions between He and aligned D 2 molecules at cold collision energies. The signatures of the angular distributions were attributed to an = 2 resonance that governs scattering at low energies. A first-principles quantum mechanical treatment of this problem is presented here using a highly accurate interaction potential for the He−H 2 system. Our results predict a very intense = 1 resonance at low energies, leading to angular distributions that differ from those measured in the experiment. A good agreement with the experiment is achieved only when the = 1 resonance is artificially removed, for example, by excluding the lowest energies present in the experimental velocity distribution. Our analysis revealed that neither the position nor the intensity of the = 1 resonance significantly changes when the interaction potential is modified within its predicted uncertainties. Energy-resolved measurements may help to resolve the discrepancy.

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“…Moreover, because the coherent superposition of the degenerate m states is stationary in time, it can be used to coherently control a bimolecular reaction. Some of these controls have already been demonstrated in the cold scattering experiments and also have been discussed theoretically. − ,,, …”

Section: Sarp Control Of Internal States and Collision Geometrymentioning

confidence: 92%

Quantum-Controlled Collisions of H₂ Molecules

Mukherjee

2023

J. Phys. Chem. A

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The amount of information that can be obtained from a scattering experiment depends upon the precision with which the quantum states are defined in the incoming channel. By precisely defining the incoming states and measuring the outgoing states in a scattering experiment, we set up the boundary condition for experimentally solving the Schrodinger equation. In this Perspective we discuss cold inelastic scattering experiments using the most theoretically tractable H 2 and its isotopologues as the target. We prepare the target in a precisely defined rovibrational (v, j, m) quantum state using a special coherent optical technique called the Stark-induced adiabatic Raman passage (SARP). v and j represent the quantum numbers of the vibrational and rotational energy levels, and m refers to the projection of the rotational angular momentum vector j on a suitable quantization axis in the laboratory frame. Selection of the m quantum numbers defines the alignment of the molecular frame, which is necessary to probe the anisotropic interactions. For us to achieve the collision temperature in the range of a few degrees Kelvin, we co-expand the colliding partners in a mixed supersonic beam that is collimated to define a direction for the collision velocity. When the bond axis is aligned with respect to a well-defined collision velocity, SARP achieves stereodynamic control at the quantum scale. Through various examples of rotationally inelastic cold scattering experiments, we show how SARP coherently controls the dynamics of anisotropic interactions by preparing quantum superpositions of the orientational m states within a single rovibrational (v, j) energy state. A partial wave analysis, which has been developed for the cold scattering experiments, shows dominance of a resonant orbital that leaves its mark in the scattering angular distribution. These highly controlled cold collision experiments at the single partial wave limit allow the most direct comparison with the results of theoretical computations, necessary for accurate modeling of the molecular interaction potential.

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A Bi-Axial Quantum State That Controls Molecular Collisions Like a Double-Slit Interferometer

Cited by 6 publications

References 37 publications

Quantum mechanical double slit for molecular scattering

Quantum mechanical double slit for molecular scattering

Role of Low Energy Resonances in the Stereodynamics of Cold He + D₂ Collisions

Quantum-Controlled Collisions of H₂ Molecules

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A Bi-Axial Quantum State That Controls Molecular Collisions Like a Double-Slit Interferometer

Cited by 6 publications

References 37 publications

Quantum mechanical double slit for molecular scattering

Quantum mechanical double slit for molecular scattering

Role of Low Energy Resonances in the Stereodynamics of Cold He + D2 Collisions

Quantum-Controlled Collisions of H2 Molecules

Contact Info

Product

Resources

About

Role of Low Energy Resonances in the Stereodynamics of Cold He + D₂ Collisions

Quantum-Controlled Collisions of H₂ Molecules