Quantum-state-specific reaction rate measurements for the photo-induced reaction Ca+ + O2 → CaO+ + O

Schmid, Philipp C.; Miller, Mikhail; Greenberg, J. M.; Nguyen, Thanh Lam; Stanton, John F.; Lewandowski, H. J.

doi:10.1080/00268976.2019.1622811

Cited by 17 publications

(16 citation statements)

References 51 publications

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“…Systematic uncertainties in pressure gauge readings are difficult to quantify and are not included in our reported uncertainties. 21,22 Note that this systematic uncertainty does not affect the relative reaction rate coefficients recorded for each reaction system, as we are using the same methodology and ion gauge for each set of experimental measurements (see the ESI † for more details). The progress of the reaction is monitored in two ways, as set out in detail in the ESI.…”

Section: Methodsmentioning

confidence: 99%

Inverse kinetic isotope effects in the charge transfer reactions of ammonia with rare gas ions

et al. 2021

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Section: Methodsmentioning

confidence: 99%

Inverse kinetic isotope effects in the charge transfer reactions of ammonia with rare gas ions

et al. 2021

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“…1) 108 . A number of ion-molecule reactions have now been precisely studied in Coulomb crystals at collision energies from a few K up to a few hundred K 31,98,[109][110][111][112][113][114][115][116][117][118][119][120] .…”

Section: Reactions In the Astrophysical Temperature Regimementioning

confidence: 99%

Towards chemistry at absolute zero

Heazlewood¹,

Softley

2021

Nat Rev Chem

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The prospect of cooling matter down to temperatures that are close to the absolute zero raises intriguing questions about how chemical reactivity changes under these extreme conditions. Although some types of chemical reaction still occur at 1 µK, they can no longer adhere to the conventional picture of reactants passing over an activation energy barrier to become products. Indeed at ultracold temperatures, the system enters a fully quantum regime, and quantum mechanics replaces the classical picture of colliding particles. In this Review, we discuss recent experimental and theoretical developments that allow us to explore chemical reactions at temperatures that range from 10 K to 500 nK. Although the field is still in its infancy, exceptional control has already been demonstrated over reactivity at low temperatures.ultracold temperatures, the classical description of the collision of particles needs to be replaced with a quantum description and the picture of a ball rolling over a hill needs to be replaced by that of a wave propagating across a barrier.The quantum regime is a physical regime in which our basic understanding of how chemical processes happen, in terms of molecules bumping into each other and breaking and remaking bonds, needs to be challenged. Strictly speaking, the dynamical system of moving and colliding molecules needs to be described as a superposition of partial waves, the components of which represent the different angular momentum states associated with the relative motion of the colliding particles. As the temperature is lowered, the system moves towards a regime in which it can be described by just a few quantised collisional angular momentum states (and, ultimately, just a single state). We denote the collisions as 's-wave' or 'p-wave' collisions (known as the partial-wave description) to represent those with zero or one unit of collisional angular momentum, respectively. Furthermore, in the quantum regime the population of molecular quantum states is distributed over just a few rovibrational states and ultimately collapses to a single quantum state at the lowest temperatures (under conditions of thermal equilibrium). At low temperatures, quantum effects on the rate coefficient and other properties of the reaction, such as collision energy resonances, quantum reflection and geometric phase (described in detail in the 'Reactions in the ultracold regime' section), are most likely to be observable. This is in contrast to what we observe at room temperature, where we understand the overall rate of a process to be an average of the behaviours of individual collisions of molecules with vastly varying sets of quantum numbers and a distribution of energies.When the temperature reaches sub-µK, the translational wavelength typically exceeds the average separation of molecules in the sample, even for a low density gas, and ultimately the system may enter the regime of quantum degeneracy (for example, bosonic particles that form a Bose-Einstein condensate, in which all particles are in the same quan...

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“…Sev- eral experiments in precision measurement 9,37 and cold chemistry 6,38 require molecular ions in a single quantum state, but typical methods of ion production (e.g., discharge, laser ablation) are violent and produce ions in numerous quantum states. In contrast, autoionization of Rydberg states has been used in a few previous experiments 8,9 to generate molecular ions in only a few quantum states, greatly increasing the yield of the desired state and reducing the complexity of subsequent state preparation steps.…”

Section: Rotational State Distributions From Autoionization Of G Rydb...mentioning

confidence: 99%

Long-range model of vibrational autoionization in core-nonpenetrating Rydberg states of NO

Barnum,

Clausen,

Jiang

et al. 2021

Preprint

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Quantum-state-specific reaction rate measurements for the photo-induced reaction Ca⁺ + O₂ → CaO⁺ + O

Cited by 17 publications

References 51 publications

Inverse kinetic isotope effects in the charge transfer reactions of ammonia with rare gas ions

Inverse kinetic isotope effects in the charge transfer reactions of ammonia with rare gas ions

Towards chemistry at absolute zero

Long-range model of vibrational autoionization in core-nonpenetrating Rydberg states of NO

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