Precision of Radiation Chemistry Networks: Playing Jenga with Kinetic Models for Liquid-Phase Electron Microscopy  

作　　者：Birk Fritsch Paolo Malgaretti Jens Harting Karl J.J.Mayrhofer Andreas Hutzler 

机构地区：[1]Helmholtz Institute Erlangen-Nürnberg for Renewable Energy(IEK-11),Forschungszentrum Jülich GmbH,91058 Erlangen,Germany [2]Department of Chemical and Biological Engineering and Department of Physics,Friedrich-Alexander-Universität Erlangen-Nürnberg,91058 Erlangen,Germany

出　　处：《Precision Chemistry》2023年第10期592-601,共10页精准化学（英文）

基　　金：A.H.and B.F.acknowledge the financial support by the Federal Ministry of Education and Research(BMBF)of Germany in the programme H2Giga−StacIE(Project Identification Number:03HY103H);.P.M.,J.H.,and K.J.J.M.acknowledge funding by the Deutsche Forschungsgemeinschaft(DFG,German Re-search Foundation)Project-ID 431791331SFB 1452.

摘　　要：Liquid-phase transmission electron microscopy(LP-TEM)is a powerful tool to gain unique insights into dynamics at the nanoscale.The electron probe,however,can induce significant beam effects that often alter observed phenomena such as radiolysis of the aqueous phase.The magnitude of beam-induced radiolysis can be assessed by means of radiation chemistry simulations potentially enabling quantitative application of LP-TEM.Unfortunately,the computational cost of these simulations scales with the amount of reactants regarded.To minimize the computational cost,while maintaining accurate predictions,we optimize the parameter space for the solution chemistry of aqueous systems in general and for diluted HAuCl4 solutions in particular.Our results indicate that sparsened kinetic models can accurately describe steady-state formation during LP-TEM and provide a handy prerequisite for efficient multidimensional modeling.We emphasize that the demonstrated workflow can be easily generalized to any kinetic model involving multiple reaction pathways.

关 键 词：Electron beam effects GOLD RADIOLYSIS kinetic modeling simulation efficiency liquid cell transmission electron microscopy 

分 类 号：O64[理学—物理化学]