DC Field | Value | Language |
---|---|---|
dc.contributor.author | DiStasio, RA | ko |
dc.contributor.author | Jung, Yousung | ko |
dc.contributor.author | Head-Gordon, M | ko |
dc.date.accessioned | 2013-03-07T16:09:45Z | - |
dc.date.available | 2013-03-07T16:09:45Z | - |
dc.date.created | 2012-02-06 | - |
dc.date.created | 2012-02-06 | - |
dc.date.issued | 2005 | - |
dc.identifier.citation | JOURNAL OF CHEMICAL THEORY AND COMPUTATION, v.1, no.5, pp.862 - 876 | - |
dc.identifier.issn | 1549-9618 | - |
dc.identifier.uri | http://hdl.handle.net/10203/90646 | - |
dc.description.abstract | In this work, we incorporate the resolution-of-the-identity (RI) approximation into the theoretical framework of the local triatomics-in-molecules (TRIM) second-order Moller-Plesset (MP2) perturbation theory model. The resultant model, RI-TRIM MP2, emerges as a robust fourth-order methodology that extends the regime of practical MP2 calculations. With RI-TRIM MP2, correlation energy corrections can easily be obtained for systems that contain more than 125 heavy atoms with a computational timing cost less than those of the prerequisite self-consistent field procedure and popular density functional theory (DFT) alternatives. In this work, the chemical performance of RI-TRIM MP2 is numerically assessed against untruncated RI-MP2 and DFT (B3LYP) in determining the relative energies of 27 different alanine tetrapeptide conformations at the cc-pVXZ (X = D, T, and 0) levels and the results are T -> Q extrapolated to the complete basis set limit. As the quality of the basis set employed increases, we report a significant reduction in the error introduced by the RI-TRIM approximation; at the cc-pVDZ level, the root mean-square (RMS) relative error was found as 0.192 kcal/mol and is decreased to an almost negligible 0.040 kcal/mol at the T -> Q extrapolated complete basis set limit. Basis set dependence was investigated by computing the RMS (max) deviations from the extrapolated RI-MP2/cc-pV(TQ)Z data set found as 0.377 (0.944) kcal/mol (MP2/cc-pVTZ) and 0.250 (0.591) kcal/mol (TRIM MP2/cc-pVTZ). These deviations are chemically significant when compared against the conformer energy differences, suggesting that to obtain reliably converged relative conformational energies, computations must be done using the cc-pVTZ and cc-pVQZ basis sets followed by extrapolation to the cc-pV(TQ)Z limit. The findings reported herein also provide the first computational evidence demonstrating that the TRIM model approaches exactness as the one-particle basis approaches completeness. | - |
dc.language | English | - |
dc.publisher | AMER CHEMICAL SOC | - |
dc.subject | DENSITY FITTING APPROXIMATIONS | - |
dc.subject | ELECTRON CORRELATION METHODS | - |
dc.subject | LINEAR SCALING COMPUTATION | - |
dc.subject | CONSISTENT BASIS-SETS | - |
dc.subject | ACCURATE AB-INITIO | - |
dc.subject | FUNCTIONAL THEORY | - |
dc.subject | FOCK MATRIX | - |
dc.subject | MP2 | - |
dc.subject | SYSTEMS | - |
dc.subject | CONVERGENCE | - |
dc.title | A resolution-of-the-identity implementation of the local triatomics-in-molecules model for second-order Moller-Plesset perturbation theory with application to alanine tetrapeptide conformational energies | - |
dc.type | Article | - |
dc.identifier.wosid | 000231871500012 | - |
dc.identifier.scopusid | 2-s2.0-33746541851 | - |
dc.type.rims | ART | - |
dc.citation.volume | 1 | - |
dc.citation.issue | 5 | - |
dc.citation.beginningpage | 862 | - |
dc.citation.endingpage | 876 | - |
dc.citation.publicationname | JOURNAL OF CHEMICAL THEORY AND COMPUTATION | - |
dc.identifier.doi | 10.1021/ct050126s | - |
dc.contributor.localauthor | Jung, Yousung | - |
dc.contributor.nonIdAuthor | DiStasio, RA | - |
dc.contributor.nonIdAuthor | Head-Gordon, M | - |
dc.type.journalArticle | Article | - |
dc.subject.keywordPlus | DENSITY FITTING APPROXIMATIONS | - |
dc.subject.keywordPlus | ELECTRON CORRELATION METHODS | - |
dc.subject.keywordPlus | LINEAR SCALING COMPUTATION | - |
dc.subject.keywordPlus | CONSISTENT BASIS-SETS | - |
dc.subject.keywordPlus | ACCURATE AB-INITIO | - |
dc.subject.keywordPlus | FUNCTIONAL THEORY | - |
dc.subject.keywordPlus | FOCK MATRIX | - |
dc.subject.keywordPlus | MP2 | - |
dc.subject.keywordPlus | SYSTEMS | - |
dc.subject.keywordPlus | CONVERGENCE | - |
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