Nucleation of molecular crystals driven by relative information entropy
Simulating nucleation of molecular crystals is extremely challenging for all but the simplest cases. The challenge lies in formulating effective order parameters that are capable of driving the transition process. In recent years, order parameters based on molecular pair-functions have been successf...
| Main Authors: | , , , , |
|---|---|
| Other Authors: | |
| Format: | Article |
| Language: | English |
| Published: |
American Chemical Society (ACS)
2020
|
| Online Access: | https://hdl.handle.net/1721.1/128717 |
| _version_ | 1811092960885866496 |
|---|---|
| author | Gobbo, Gianpaolo Bellucci, Michael A. Tribello, Gareth A. Ciccotti, Giovanni Trout, Bernhardt L. |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Gobbo, Gianpaolo Bellucci, Michael A. Tribello, Gareth A. Ciccotti, Giovanni Trout, Bernhardt L. |
| author_sort | Gobbo, Gianpaolo |
| collection | MIT |
| description | Simulating nucleation of molecular crystals is extremely challenging for all but the simplest cases. The challenge lies in formulating effective order parameters that are capable of driving the transition process. In recent years, order parameters based on molecular pair-functions have been successfully used in combination with enhanced sampling techniques to simulate nucleation of simple molecular crystals. However, despite the success of these approaches, we demonstrate that they can fail when applied to more complex cases. In fact, we show that order parameters based on molecular pair-functions, while successful at nucleating benzene, fail for paracetamol. Hence, we introduce a novel approach to formulate order parameters. In our approach, we construct reduced dimensional distributions of relevant quantities on the fly and then quantify the difference between these distributions and selected reference distributions. By computing the distribution of different quantities and by choosing different reference distributions, it is possible to systematically construct an effective set of order parameters. We then show that our new order parameters are capable of driving the nucleation of ordered states and, in particular, the form I crystal of paracetamol. ©2017 American Chemical Society. |
| first_indexed | 2024-09-23T15:37:20Z |
| format | Article |
| id | mit-1721.1/128717 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T15:37:20Z |
| publishDate | 2020 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1287172022-09-29T15:05:00Z Nucleation of molecular crystals driven by relative information entropy Gobbo, Gianpaolo Bellucci, Michael A. Tribello, Gareth A. Ciccotti, Giovanni Trout, Bernhardt L. Massachusetts Institute of Technology. Department of Chemical Engineering Simulating nucleation of molecular crystals is extremely challenging for all but the simplest cases. The challenge lies in formulating effective order parameters that are capable of driving the transition process. In recent years, order parameters based on molecular pair-functions have been successfully used in combination with enhanced sampling techniques to simulate nucleation of simple molecular crystals. However, despite the success of these approaches, we demonstrate that they can fail when applied to more complex cases. In fact, we show that order parameters based on molecular pair-functions, while successful at nucleating benzene, fail for paracetamol. Hence, we introduce a novel approach to formulate order parameters. In our approach, we construct reduced dimensional distributions of relevant quantities on the fly and then quantify the difference between these distributions and selected reference distributions. By computing the distribution of different quantities and by choosing different reference distributions, it is possible to systematically construct an effective set of order parameters. We then show that our new order parameters are capable of driving the nucleation of ordered states and, in particular, the form I crystal of paracetamol. ©2017 American Chemical Society. MIT-Novartis Center for Continuous Manufacturing 2020-12-03T00:14:16Z 2020-12-03T00:14:16Z 2017-12 2017-10 2019-09-13T16:57:21Z Article http://purl.org/eprint/type/JournalArticle 1549-9618 1549-9626 https://hdl.handle.net/1721.1/128717 Gobbo, Gianpaolo et al., "Nucleation of Molecular Crystals Driven by Relative Information Entropy." Journal of Chemical Theory and Computation 14, 2 (February 2018): 959–972 doi. 10.1021/acs.jctc.7b01027 ©2017 Authors en https://dx.doi.org/10.1021/ACS.JCTC.7B01027 Journal of Chemical Theory and Computation Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf American Chemical Society (ACS) Other repository |
| spellingShingle | Gobbo, Gianpaolo Bellucci, Michael A. Tribello, Gareth A. Ciccotti, Giovanni Trout, Bernhardt L. Nucleation of molecular crystals driven by relative information entropy |
| title | Nucleation of molecular crystals driven by relative information entropy |
| title_full | Nucleation of molecular crystals driven by relative information entropy |
| title_fullStr | Nucleation of molecular crystals driven by relative information entropy |
| title_full_unstemmed | Nucleation of molecular crystals driven by relative information entropy |
| title_short | Nucleation of molecular crystals driven by relative information entropy |
| title_sort | nucleation of molecular crystals driven by relative information entropy |
| url | https://hdl.handle.net/1721.1/128717 |
| work_keys_str_mv | AT gobbogianpaolo nucleationofmolecularcrystalsdrivenbyrelativeinformationentropy AT belluccimichaela nucleationofmolecularcrystalsdrivenbyrelativeinformationentropy AT tribellogaretha nucleationofmolecularcrystalsdrivenbyrelativeinformationentropy AT ciccottigiovanni nucleationofmolecularcrystalsdrivenbyrelativeinformationentropy AT troutbernhardtl nucleationofmolecularcrystalsdrivenbyrelativeinformationentropy |