Controlling rotational quenching rates in cold molecular collisions

Croft, James; Balakrishnan, N.

doi:10.1063/1.5091576

Cited by 31 publications

(46 citation statements)

References 46 publications

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“…Previous studies of Croft et al 24,25 and Morita et al 26,27 have shown that collision-induced resonances are more sensitive to the relative orientation of the colliding partners. Therefore, we have first scanned collision energies for the various entrance channels mentioned above to survey for any resonances.…”

Section: Resultsmentioning

confidence: 93%

“…The methodology used herein is, in many aspects, very similar to that utilized in the previous works of Croft et al 24,25 and Morita et al 26,27 except that reactive channels are also taken into consideration as a collision-induced outcome. Thus, upon a H + D 2 (υ, j) reactive collision (or likewise D + HD), the probability of detecting a scattered HD(υ , j ) product (or D 2 ) by a detector placed at Ω = (θ, φ), at a given collision en-ergy E coll , is governed by the state-to-state scattering amplitude 33 f J nn (θ, E coll ), i.e.…”

Section: Theoretical Approachmentioning

confidence: 99%

“…The experiments of Perreault et al have been accompanied by the theoretical works of Croft et al 24,25 on HD + H 2 and Morita et al 26,27 on He + HD collisions. Further, Jambrina et al 28 and Morita et al 29 have explored the control of isolated partial wave resonances through stereodynamic preparations of HD + H 2 and HCl + H 2 collisions, respectively, as in the experiments of Perreault et al In a recent work, Jambrina et al examined stereodynamic control of CO + HD collisions in which the HD molecule is prepared in a stereodynamic state but both molecules undergo a change in rotational angular momentum 30 .…”

Section: Introductionmentioning

confidence: 98%

See 2 more Smart Citations

On the use of stereodynamical effects to control cold chemical reactions: the H + D$_{2}\longleftrightarrow$ D + HD case study

Silva,

Kendrick,

Balakrishnan

2021

Preprint

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Quantum calculations are reported for the stereodynamic control of the H + D 2 ←→ D + HD chemical reaction in the energy range of 1-50 K. Stereodynamic control is achieved by a formalism similar to that reported by Perreault et al. [Nature Chem. 10, 561 (2018)] in recent experimental works in which the alignment of the molecular bond axis relative to the incident relative velocity is controlled by selective preparations of the molecule in a specific or superposition of magnetic projection quantum numbers of the initial molecular rotational level. The approach presented here generalizes the experimental scheme of Perreault et al. and offers additional degree of control through various experimental preparation of the molecular alignment angle. Illustrative results presented for the H + D 2 and D + HD reactions show significant control with the possibility of turning the reaction completely on or off with appropriate stereodynamic preparation of the molecular state. Various scenarios for maximizing and minimizing the reaction outcomes are identified with selective preparation of molecular rotational states.

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Section: Resultsmentioning

confidence: 93%

Section: Theoretical Approachmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 98%

See 1 more Smart Citation

On the use of stereodynamical effects to control cold chemical reactions: the H + D$_{2}\longleftrightarrow$ D + HD case study

Silva,

Kendrick,

Balakrishnan

2021

Preprint

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“…18 A large number of theoretical studies have illustrated in great detail the importance of the relative alignment of the colliding pair on the dynamics of cold diatom-diatom scattering. [18][19][20][21][22][23][24][25][26] Unfortunately, the vast majority of experimental work thus far has not explored the effect of the spatial alignment of the collision partners on the scattering process, and so there is very little data available for comparison with theory. Defining the initial state with this level of precision is equivalent to setting the boundary conditions for experimentally solving the dynamical equations.…”

Section: Introductionmentioning

confidence: 99%

Highly anisotropic resonant dynamics in the aligned-aligned scattering of cold diatoms

Zhou

Perreault

Mukherjee

et al. 2021

Preprint

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The dynamics of a resonant oriented scattering process dominated by a single partial wave provide the most sensitive probe of the long-range anisotropic forces important to chemical reactions. Here, we control the collision temperature and geometry to probe the dynamics of the cold (<2 K) rotationally inelastic scattering of a pair of optically state-prepared D2 molecules. The collision temperature is manipulated by combining the strobing action of laser state preparation and detection with the velocity dispersion of the molecular beam. When the bond axes are aligned parallel to the collision velocity, the scattering rate drops by nearly an order of magnitude when collision energies >1 K are removed, demonstrating a clear geometry-dependent resonance. Using partial wave analysis of the measured scattering angular distribution, we determine that an l = 2 shape resonance originates from the collisions between a pair of aligned D2 molecules. Our experiment illustrates the strong anisotropy of the long-range quadrupole-quadrupole interaction that controls the dynamic resonance for diatom-diatom collisions.

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“…Currently there is much interest in studying inelastic and reactive molecular collisions near 1 K as well as in the mK (cold) and µK (ultracold) regimes [18][19][20][21][22][23][24][25][26][27][28][29][30][31][32]. Quantum effects are amplified in these regimes and quantum control of molecular collisions using external electric and magnetic fields becomes feasible [1][2][3][4][5][6][7].…”

Section: Introductionmentioning

confidence: 99%

Stereodynamic control of cold rotationally inelastic CO + HD collisions

Jambrina,

Croft,

Balakrishnan

et al. 2021

Preprint

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Quantum control of molecular collision dynamics is an exciting emerging area of cold collisions. Co-expansion of collision partners in a supersonic molecular beam combined with precise control of their quantum states and alignment/orientation using Stark-induced Adiabatic Raman Passage allows exquisite stereodynamic control of the collision outcome. This approach has recently been demonstrated for rotational quenching of HD in collisions with H2, D2, and He and D2 by He. Here we illustrate this approach for HD(v = 0, j = 2)+CO(v = 0, j = 0)→HD(v = 0, j )+CO(v = 0, j ) collisions through full-dimensional quantum scattering calculations at collision energies near 1 K. It is shown that the collision dynamics at energies between 0.01-1 K are controlled by an interplay of L = 1 and L = 2 partial wave resonances depending on the final rotational levels of the two molecules. Polarized cross sections resolved into magnetic sub-levels of the initial and final rotational quantum numbers of the two molecules also reveal significant stereodynamic effect in the cold energy regime. Overall, the stereodynamic effect is controlled by both geometric and dynamical factors, with parity conservation playing an important role in modulating these contributions depending on the particular final state.

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Controlling rotational quenching rates in cold molecular collisions

Cited by 31 publications

References 46 publications

On the use of stereodynamical effects to control cold chemical reactions: the H + D$_{2}\longleftrightarrow$ D + HD case study

On the use of stereodynamical effects to control cold chemical reactions: the H + D$_{2}\longleftrightarrow$ D + HD case study

Highly anisotropic resonant dynamics in the aligned-aligned scattering of cold diatoms

Stereodynamic control of cold rotationally inelastic CO + HD collisions

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