دورية أكاديمية
Water interactions with hydrophobic groups: Assessment and recalibration of semiempirical molecular orbital methods
| العنوان: | Water interactions with hydrophobic groups: Assessment and recalibration of semiempirical molecular orbital methods |
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| المؤلفون: | Marıon, Antoıne, Monard, Gerald, Ruiz-Lopez, Manuel F., Ingrosso, Francesca |
| بيانات النشر: | JOURNAL OF CHEMICAL PHYSICS |
| سنة النشر: | 2014 |
| مصطلحات موضوعية: | Am1, Complexes, Parameters, Hydrogen-Bonds, Bonding correction, Nddo approximations, Interaction energies, Dispersion corrections, Ab-initio, Density-functional theory |
| الوصف: | In this work, we present a study of the ability of different semiempirical methods to describe intermolecular interactions in water solution. In particular, we focus on methods based on the Neglect of Diatomic Differential Overlap approximation. Significant improvements of these methods have been reported in the literature in the past years regarding the description of non-covalent interactions. In particular, a broad range of methodologies has been developed to deal with the properties of hydrogen-bonded systems, with varying degrees of success. In contrast, the interactions between water and a molecule containing hydrophobic groups have been little analyzed. Indeed, by considering the potential energy surfaces obtained using different semiempirical Hamiltonians for the intermolecular interactions of model systems, we found that none of the available methods provides an entirely satisfactory description of both hydrophobic and hydrophilic interactions in water. In addition, a vibrational analysis carried out in a model system for these interactions, a methane clathrate cluster, showed that some recent methods cannot be used to carry out studies of vibrational properties. Following a procedure established in our group [M. I. Bernal-Uruchurtu, M. T. C. Martins-Costa, C. Millot, and M. F. Ruiz-Lopez, J. Comput. Chem. 21, 572 (2000); W. Harb, M. I. Bernal-Uruchurtu, and M. F. Ruiz-Lopez, Theor. Chem. Acc. 112, 204 (2004)], we developed new parameters for the core-core interaction terms based on fitting potential energy curves obtained at the MP2 level for our model system. We investigated the transferability of the new parameters to describe a system, having both hydrophilic and hydrophobic groups, interacting with water. We found that only by introducing two different sets of parameters for hydrophilic and hydrophobic hydrogen atom types we are able to match the features of the ab initio calculated properties. Once this assumption is made, a good agreement with the MP2 reference is achieved. The results reported ... |
| نوع الوثيقة: | article in journal/newspaper |
| اللغة: | unknown |
| تدمد: | 0021-9606 |
| العلاقة: | Marion A., Monard G., Ruiz-Lopez M. F. , Ingrosso F., "Water interactions with hydrophobic groups: Assessment and recalibration of semiempirical molecular orbital methods", JOURNAL OF CHEMICAL PHYSICS, cilt.141, 2014; 84904645115; https://hdl.handle.net/11511/47007Test; 141; WOS:000340711300007 |
| DOI: | 10.1063/1.4886655 |
| الإتاحة: | https://doi.org/10.1063/1.4886655Test https://hdl.handle.net/11511/47007Test |
| حقوق: | Attribution-NonCommercial-NoDerivatives 4.0 International ; http://creativecommons.org/licenses/by-nc-nd/4.0Test/ |
| رقم الانضمام: | edsbas.232E7215 |
| قاعدة البيانات: | BASE |
| تدمد: | 00219606 |
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| DOI: | 10.1063/1.4886655 |