scholarly journals Comment on ‘‘Non‐Rice–Ramsperger–Kassel–Marcus dynamics and the statistics of reaction rates in chaotic systems’’ [J. Chem. Phys.98, 7898 (1993)]

1994 ◽  
Vol 100 (2) ◽  
pp. 1773-1774
Author(s):  
Joshua Wilkie ◽  
Paul Brumer
Keyword(s):  
Chaotic Systems ◽  
Reaction Rates ◽  
Chem Phys

scholarly journals Minimizing irreversible losses in quantum systems by local counterdiabatic driving

2017 ◽  
Vol 114 (20) ◽  
pp. E3909-E3916 ◽  
Author(s):  
Dries Sels ◽  
Anatoli Polkovnikov
Keyword(s):  
Variational Approach ◽  
Chaotic Systems ◽  
Chem Phys ◽  
Quantum Systems ◽  
Particle Systems ◽  
Coupling Constant ◽  
Quantum Annealing ◽  
Physical Constraints ◽  
Adiabatic Dynamics

Counterdiabatic driving protocols have been proposed [Demirplak M, Rice SA (2003) J Chem Phys A 107:9937–9945; Berry M (2009) J Phys A Math Theor 42:365303] as a means to make fast changes in the Hamiltonian without exciting transitions. Such driving in principle allows one to realize arbitrarily fast annealing protocols or implement fast dissipationless driving, circumventing standard adiabatic limitations requiring infinitesimally slow rates. These ideas were tested and used both experimentally and theoretically in small systems, but in larger chaotic systems, it is known that exact counterdiabatic protocols do not exist. In this work, we develop a simple variational approach allowing one to find the best possible counterdiabatic protocols given physical constraints, like locality. These protocols are easy to derive and implement both experimentally and numerically. We show that, using these approximate protocols, one can drastically suppress heating and increase fidelity of quantum annealing protocols in complex many-particle systems. In the fast limit, these protocols provide an effective dual description of adiabatic dynamics, where the coupling constant plays the role of time and the counterdiabatic term plays the role of the Hamiltonian.

Non‐Rice–Ramsperger–Kassel–Marcus dynamics and the statistics of reaction rates in chaotic systems

1993 ◽  
Vol 98 (10) ◽  
pp. 7898-7902 ◽  
Author(s):  
Ann C. Gentile ◽  
Sarah A. Schofield ◽  
Peter G. Wolynes
Keyword(s):  
Chaotic Systems ◽  
Reaction Rates

Investigation of the behavior of tropospheric relevant compounds at the interface gas/organic acid aerosols: An ONIOM QM/MM study

2021 ◽  
Author(s):  
Antoine Roose ◽  
Denis Duflot ◽  
Césaire Fotsing Kwetche ◽  
Céline Toubin
Keyword(s):  
Oleic Acid ◽  
Bulk Diffusion ◽  
Reaction Rates ◽  
Oxidative Capacity ◽  
Chem Phys ◽  
Computational Method ◽  
Strong Impact ◽  
Development Fund ◽  
Wide Range ◽  
Uptake Coefficients

<p>The uptake of atmospheric gaseous oxidant such as O<sub>3</sub> or the ROx (OH, HO<sub>2</sub>, RO<sub>2</sub>) family, have a strong impact on the oxidative capacity of the atmosphere. [1], [2] Last decade, few studies have been carried out on the uptake of such compounds on atmospheric aerosol. However, the large variety of organic compounds provides uptake coefficients with a wide range of order of magnitude. [3], [4] Furthermore, the uptake resulting from the combination of different processes (mass accommodation, bulk diffusion, reactivity), the detailed understanding of such a process is not always accessible through experiments. Theoretical tools such as quantum mechanics (QM) combined with Molecular Mechanics (MM) is one way to investigate separately the different processes.</p><p>The ONIOM hybrid QM/MM method [5] allows to study the reactivity of few molecules in a large system. In our group, a methodology using this computational method have been developed in order to estimate the reactive uptake of gaseous compounds onto organic aerosol particles. In this presentation, reactive uptake of HO<sub>2</sub> and O<sub>3</sub> onto glutaric acid and oleic acid aerosols respectively will be discussed. Comparisons will be addressed with gas phase theoretical reaction rates and with experimental data.</p><p><em>We acknowledge support by the French government through the Program “Investissement d'avenir” through the Labex CaPPA (contract ANR-11-LABX-0005-01) and I-SITE ULNE project OVERSEE (contract ANR-16-IDEX-0004), CPER CLIMIBIO (European Regional Development Fund, Hauts de France council, French Ministry of Higher Education and Research) and French national supercomputing facilities (grants DARI x2016081859 and A0050801859).</em></p><p> </p><p>References</p><p>[1]          H. L. Macintyre and M. J. Evans, “Parameterisation and impact of aerosol uptake of HO2 on a global tropospheric model,” Atmos. Chem. Phys., vol. 11, no. 21, pp. 10965–10974, Nov. 2011, doi: 10.5194/acp-11-10965-2011.</p><p>[2]          M. Zeng and K. R. Wilson, “Efficient Coupling of Reaction Pathways of Criegee Intermediates and Free Radicals in the Heterogeneous Ozonolysis of Alkenes,” The Journal of Physical Chemistry Letters, Jul. 2020, doi: 10.1021/acs.jpclett.0c01823.</p><p>[3]          P. S. J. Lakey, I. J. George, L. K. Whalley, M. T. Baeza-Romero, and D. E. Heard, “Measurements of the HO2 Uptake Coefficients onto Single Component Organic Aerosols,” Environ. Sci. Technol., vol. 49, no. 8, pp. 4878–4885, Apr. 2015, doi: 10.1021/acs.est.5b00948.</p><p>[4]          M. Mendez, N. Visez, S. Gosselin, V. Crenn, V. Riffault, and D. Petitprez, “Reactive and Nonreactive Ozone Uptake during Aging of Oleic Acid Particles,” J. Phys. Chem. A, vol. 118, no. 40, pp. 9471–9481, Oct. 2014, doi: 10.1021/jp503572c.</p><p>[5]          L. W. Chung et al., “The ONIOM Method and Its Applications,” Chem. Rev., vol. 115, no. 12, pp. 5678–5796, Jun. 2015, doi: 10.1021/cr5004419.</p>

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