Machine-Learned Free Energy Surfaces for Capillary Condensation and Evaporation in Mesopores
Using molecular simulations, we study the processes of capillary condensation and capillary evaporation in model mesopores. To determine the phase transition pathway, as well as the corresponding free energy profile, we carry out enhanced sampling molecular simulations using entropy as a reaction co...
| Main Authors: | , |
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| Format: | Article |
| Language: | English |
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MDPI AG
2022-01-01
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| Series: | Entropy |
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| Online Access: | https://www.mdpi.com/1099-4300/24/1/97 |
| _version_ | 1797494164807483392 |
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| author | Caroline Desgranges Jerome Delhommelle |
| author_facet | Caroline Desgranges Jerome Delhommelle |
| author_sort | Caroline Desgranges |
| collection | DOAJ |
| description | Using molecular simulations, we study the processes of capillary condensation and capillary evaporation in model mesopores. To determine the phase transition pathway, as well as the corresponding free energy profile, we carry out enhanced sampling molecular simulations using entropy as a reaction coordinate to map the onset of order during the condensation process and of disorder during the evaporation process. The structural analysis shows the role played by intermediate states, characterized by the onset of capillary liquid bridges and bubbles. We also analyze the dependence of the free energy barrier on the pore width. Furthermore, we propose a method to build a machine learning model for the prediction of the free energy surfaces underlying capillary phase transition processes in mesopores. |
| first_indexed | 2024-03-10T01:30:25Z |
| format | Article |
| id | doaj.art-29149976cc704f36989ef00c0fb7d37b |
| institution | Directory Open Access Journal |
| issn | 1099-4300 |
| language | English |
| last_indexed | 2024-03-10T01:30:25Z |
| publishDate | 2022-01-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Entropy |
| spelling | doaj.art-29149976cc704f36989ef00c0fb7d37b2023-11-23T13:41:51ZengMDPI AGEntropy1099-43002022-01-012419710.3390/e24010097Machine-Learned Free Energy Surfaces for Capillary Condensation and Evaporation in MesoporesCaroline Desgranges0Jerome Delhommelle1MetaSimulation of Nonequilibrium Processes (MSNEP) Group, Tech Accelerator, University of North Dakota, Grand Forks, ND 58202, USAMetaSimulation of Nonequilibrium Processes (MSNEP) Group, Tech Accelerator, University of North Dakota, Grand Forks, ND 58202, USAUsing molecular simulations, we study the processes of capillary condensation and capillary evaporation in model mesopores. To determine the phase transition pathway, as well as the corresponding free energy profile, we carry out enhanced sampling molecular simulations using entropy as a reaction coordinate to map the onset of order during the condensation process and of disorder during the evaporation process. The structural analysis shows the role played by intermediate states, characterized by the onset of capillary liquid bridges and bubbles. We also analyze the dependence of the free energy barrier on the pore width. Furthermore, we propose a method to build a machine learning model for the prediction of the free energy surfaces underlying capillary phase transition processes in mesopores.https://www.mdpi.com/1099-4300/24/1/97capillaryphase transitionfree energyactivated processliquid bridgesbubbles |
| spellingShingle | Caroline Desgranges Jerome Delhommelle Machine-Learned Free Energy Surfaces for Capillary Condensation and Evaporation in Mesopores Entropy capillary phase transition free energy activated process liquid bridges bubbles |
| title | Machine-Learned Free Energy Surfaces for Capillary Condensation and Evaporation in Mesopores |
| title_full | Machine-Learned Free Energy Surfaces for Capillary Condensation and Evaporation in Mesopores |
| title_fullStr | Machine-Learned Free Energy Surfaces for Capillary Condensation and Evaporation in Mesopores |
| title_full_unstemmed | Machine-Learned Free Energy Surfaces for Capillary Condensation and Evaporation in Mesopores |
| title_short | Machine-Learned Free Energy Surfaces for Capillary Condensation and Evaporation in Mesopores |
| title_sort | machine learned free energy surfaces for capillary condensation and evaporation in mesopores |
| topic | capillary phase transition free energy activated process liquid bridges bubbles |
| url | https://www.mdpi.com/1099-4300/24/1/97 |
| work_keys_str_mv | AT carolinedesgranges machinelearnedfreeenergysurfacesforcapillarycondensationandevaporationinmesopores AT jeromedelhommelle machinelearnedfreeenergysurfacesforcapillarycondensationandevaporationinmesopores |