scholarly journals Growth Kinetics of Single Polymer Particles in Solution via Active-Feedback 3D Tracking

2021 ◽  
Author(s):  
Donggeng Yu ◽  
Antonio Garcia IV ◽  
Suzanne A. Blum ◽  
Kevin D. Welsher
Keyword(s):  
Chemical Reactions ◽  
Chemical Reaction ◽  
Single Particle ◽  
Rational Design ◽  
Solution Phase ◽  
Three Dimensions ◽  
Polymer Particles ◽  
3D Tracking ◽  
Average Growth ◽  
Volumetric Images

The ability to directly observe chemical reactions at the single-molecule and single-particle level has enabled the discovery of behaviors otherwise obscured by the ensemble averaging in bulk measurements. However powerful, a common restriction of these studies to date has been the absolute requirement to surface tether or otherwise immobilize the chemical reagent/reaction of interest. This constraint arose from a fundamental limitation of conventional microscopy techniques, which could not track molecules or particles rapidly diffusing in three dimensions, as occurs in solution. However, much chemistry occurs in the solution phase, leaving single-particle/-molecule analysis of this critical area of science beyond the scope of available technology. Here we report the first solution-phase studies and measurements of any chemical reaction at single-particle/-molecule level in freely diffusing solution. During chemical reaction, freely diffusing polymer particles (D ~ 10-12 m2/s) yielded single-particle 3D trajectories and real-time volumetric images that were analyzed to extract the growth rates of individual particles. These volumetric images show that the average growth rate is a poor representation of the true underlying variability in polymer-particle growth behavior. These data revealed statistically significant populations of faster- and slower-growing particles at different depths in the sample, showing emergent heterogeneity while particles are still in the solution phase. These results go against the prevailing premise that chemical processes freely diffusing in solution will exhibit uniform kinetics. These new understandings of mechanisms behind polymer growth variations bring about an exciting opportunity to control particle-size and plausibly molecular weight polydispersity by the rational design of conditions to dictate spatial growth gradients. We anticipate that these studies will launch a new field of solution-phase, nonensemble-averaged measurements of chemical reactions.

QLB for Quantum Many-Body and Quantum Field Theory

2018 ◽  
Author(s):  
Sauro Succi
Keyword(s):  
Field Theory ◽  
Quantum Field Theory ◽  
Quantum Mechanics ◽  
Quantum Computing ◽  
Single Particle ◽  
Body Problem ◽  
Three Dimensions ◽  
Quantum Field ◽  
Many Body ◽  
Quantum Particles

Chapter 32 expounded the basic theory of quantum LB for the case of relativistic and non-relativistic wavefunctions, namely single-particle quantum mechanics. This chapter goes on to cover extensions of the quantum LB formalism to the overly challenging arena of quantum many-body problems and quantum field theory, along with an appraisal of prospective quantum computing implementations. Solving the single particle Schrodinger, or Dirac, equation in three dimensions is a computationally demanding task. This task, however, pales in front of the ordeal of solving the Schrodinger equation for the quantum many-body problem, namely a collection of many quantum particles, typically nuclei and electrons in a given atom or molecule.

Normal approximations for distributions arising in the stochastic approach to chemical reaction kinetics

1981 ◽  
Vol 18 (01) ◽  
pp. 263-267 ◽  
Author(s):  
F. D. J. Dunstan ◽  
J. F. Reynolds
Keyword(s):  
Reaction Kinetics ◽  
Chemical Reactions ◽  
Chemical Reaction ◽  
Stochastic Approach ◽  
Algebraic Functions ◽  
Chemical Reaction Kinetics ◽  
Normal Approximations ◽  
Formal Solutions

Earlier stochastic analyses of chemical reactions have provided formal solutions which are unsuitable for most purposes in that they are expressed in terms of complex algebraic functions. Normal approximations are derived here for solutions to a variety of reactions. Using these, it is possible to investigate the level at which the classical deterministic solutions become inadequate. This is important in fields such as radioimmunoassay.

scholarly journals Mapping the Space of Chemical Reactions using Attention-Based Neural Networks

2020 ◽  
Author(s):  
Philippe Schwaller ◽  
Daniel Probst ◽  
Alain C. Vaucher ◽  
Vishnu H Nair ◽  
David Kreutter ◽  
...  
Keyword(s):  
Neural Networks ◽  
Reaction Center ◽  
Chemical Reactions ◽  
Chemical Reaction ◽  
Classification Accuracy ◽  
Similarity Searching ◽  
Reaction Space ◽  
Fine Grained ◽  
Visual Clustering ◽  
Better Than

<div><div><div><p>Organic reactions are usually assigned to classes grouping reactions with similar reagents and mechanisms. Reaction classes facilitate communication of complex concepts and efficient navigation through chemical reaction space. However, the classification process is a tedious task, requiring the identification of the corresponding reaction class template via annotation of the number of molecules in the reactions, the reaction center and the distinction between reactants and reagents. In this work, we show that transformer-based models can infer reaction classes from non-annotated, simple text-based representations of chemical reactions. Our best model reaches a classification accuracy of 98.2%. We also show that the learned representations can be used as reaction fingerprints which capture fine-grained differences between reaction classes better than traditional reaction fingerprints. The unprecedented insights into chemical reaction space enabled by our learned fingerprints is illustrated by an interactive reaction atlas providing visual clustering and similarity searching. </p><p><br></p><p>Code: https://github.com/rxn4chemistry/rxnfp</p><p>Tutorials: https://rxn4chemistry.github.io/rxnfp/</p><p>Interactive reaction atlas: https://rxn4chemistry.github.io/rxnfp//tmaps/tmap_ft_10k.html</p></div></div></div>

scholarly journals Mass transfer with complex reversible chemical reactions—I. Single reversible chemical reaction

1989 ◽  
Vol 44 (10) ◽  
pp. 2295-2310 ◽  
Author(s):  
G.F. Versteeg ◽  
J.A.M. Kuipers ◽  
F.P.H. Van Beckum ◽  
W.P.M. Van Swaaij
Keyword(s):  
Mass Transfer ◽  
Chemical Reactions ◽  
Chemical Reaction ◽  
Reversible Chemical Reaction

Kinetic study of key species and reactions of atmospheric pressure pulsed corona discharge in humid air

2021 ◽  
Author(s):  
Yongkang Peng ◽  
Xiaoyue Chen ◽  
Yeqiang Deng ◽  
Lan Lei ◽  
Zhan Haoyu ◽  
...  
Keyword(s):  
Chemical Reactions ◽  
Chemical Reaction ◽  
Atmospheric Pressure ◽  
Discharge Plasma ◽  
Reaction Rates ◽  
Global Model ◽  
Discharge Process ◽  
Humid Air ◽  
Pressure Discharge ◽  
Atmospheric Pressure Discharge

Abstract The traditional corona discharge fluid model considers only electrons, positive and negative ions, and the discharge parameters are determined using the simplified weighting method involving the partial pressure ratio. Atmospheric pressure discharge plasma in humid air involves three main neutral gas molecule types: N2, O2, and H2O(g). However, in these conditions, the discharge process involves many types of particles and chemical reactions, and the charge and substance transfer processes are complex. At present, the databases of plasma chemical reaction equations are still expanding based on scholarly research. In this study, we examined the key particles and chemical reactions that substantially influence plasma characteristics. In summarizing the chemical reaction model for the discharge process of N2–O2–H2O(g) mixed gases, 65 particle types and 673 chemical reactions were investigated. On this basis, a global model of atmospheric pressure humid air discharge plasma was developed, with a focus on the variation of charged particles densities and chemical reaction rates with time under the excitation of a 0–200 Td pulsed electric field. Particles with a density greater than 1% of the electron density were classified as key particles. For such particles, the top ranking generation or consumption reactions (i.e., where the sum of their rates was greater than 95% of the total rate of the generation or consumption reactions) were classified as key chemical reactions On the basis of the key particles and reactions identified, a simplified global model was derived. A comparison of the global model with the simplified global model in terms of the model parameters, particle densities, reaction rates (with time), and calculation efficiencies demonstrated that both models can adequately identify the key particles and chemical reactions reflecting the chemical process of atmospheric pressure discharge plasma in humid air. Thus, by analyzing the key particles and chemical reaction pathways, the charge and substance transfer mechanism of atmospheric pressure pulse discharge plasma in humid air was revealed, and the mechanism underlying water vapor molecules’ influence on atmospheric pressure air discharge was elucidated.

Chemical Reaction Kinetics in Solution

2004 ◽  
Author(s):  
W. Ronald Fawcett
Keyword(s):  
Reaction Kinetics ◽  
Chemical Reactions ◽  
Chemical Reaction ◽  
Physical Property ◽  
Theoretical Description ◽  
Time Range ◽  
Chemical Changes ◽  
Elementary Reactions ◽  
Chemical Reaction Kinetics ◽  
Liquid Solutions

The kinetics of chemical reactions were first studied in liquid solutions. These experiments involved mixing two liquids and following the change in the concentration of a reactant or product with time. The concentration was monitored by removing a small sample of the solution and stopping the reaction, for example, by rapidly lowering the temperature, or by following a physical property of the system in situ, for example, its color. Although the experiments were initially limited to slow reactions, they established the basic laws governing the rate at which chemical changes occur. The variables considered included the concentrations of the reactants and of the products, the temperature, and the pressure. Thus, the reacting system was examined using the variables normally considered for a system at equilibrium. Most reactions were found to be complex, that is, to be made up of several elementary steps which involved one or two reactants. As the fundamental concepts of chemical kinetics developed, there was a strong interest in studying chemical reactions in the gas phase. At low pressures the reacting molecules in a gaseous solution are far from one another, and the theoretical description of equilibrium thermodynamic properties was well developed. Thus, the kinetic theory of gases and collision processes was applied first to construct a model for chemical reaction kinetics. This was followed by transition state theory and a more detailed understanding of elementary reactions on the basis of quantum mechanics. Eventually, these concepts were applied to reactions in liquid solutions with consideration of the role of the non-reacting medium, that is, the solvent. An important turning point in reaction kinetics was the development of experimental techniques for studying fast reactions in solution. The first of these was based on flow techniques and extended the time range over which chemical changes could be observed from a few seconds down to a few milliseconds. This was followed by the development of a variety of relaxation techniques, including the temperature jump, pressure jump, and electrical field jump methods. In this way, the time for experimental observation was extended below the nanosecond range.

scholarly journals Rational design of functional materials guided by single particle chemiluminescence imaging

2019 ◽  
Vol 10 (21) ◽  
pp. 5444-5451 ◽  
Author(s):  
Weijun Kong ◽  
Qi Li ◽  
Wei Wang ◽  
Xiaoning Zhao ◽  
Shenglong Jiang ◽  
...  
Keyword(s):  
Structural Characterization ◽  
Single Particle ◽  
Rational Design ◽  
Functional Materials ◽  
Single Particles ◽  
Improved Performance

Correlated chemiluminescence imaging and structural characterization of single particles helped the rational design of functional materials with significantly improved performance.

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