ACS Publications. Most Trusted. Most Cited. Most Read

OR SEARCH CITATIONS

My Activity
Publications
CONTENT TYPES

Figure 1Loading Img
Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Chem. Theory Comput. 2013, 9, 1, 408-417
RETURN TO ISSUEPREVArticleNEXT

Incremental CCSD(T)(F12)|MP2-F12—A Method to Obtain Highly Accurate CCSD(T) Energies for Large Molecules

View Author Information
Institute for Chemistry, Chemnitz University of Technology, Strasse der Nationen 62, 09111 Chemnitz, Germany
*E-mail: [email protected]
Cite this: J. Chem. Theory Comput. 2013, 9, 1, 408–417
Publication Date (Web):November 20, 2012
https://doi.org/10.1021/ct300938w
Copyright © 2012 American Chemical Society
RIGHTS & PERMISSIONS
Article Views
886
Altmetric
-
Citations
48
LEARN ABOUT THESE METRICS
Read OnlinePDF (2 MB)
Get e-Alerts
Supporting Info (1)»
SUBJECTS:

Abstract

Abstract Image

In this work, we apply the recently proposed MP2 correction to incremental energies within the domain-specific basis set approach to incrementally expanded CCSD(T)(F12) energies. The approach is tested for a set of 27 molecules with different electronic structures including water clusters, aqua complexes, aliphatic hydrocarbons, alkenes, alkynes, aromatic systems, and amino acids. The root mean squared deviation of the absolute energies with respect to the standard calculation is 1.7 kJ/mol, the mean absolute deviation is 1.2 kJ/mol, and the range is 4.7 kJ/mol. The wall time of the computations is reduced due to the application of a doubly parallel strategy—the independent coupled cluster calculations are performed on up to 70 nodes in parallel, and in addition the computations on one node are performed with the SMP-parallelized coupled cluster code in TURBOMOLE. Using this strategy, we can perform computations in minutes or hours, instead of days or months. Applying the proposed scheme enables us to routinely treat systems with 50 atoms at the CCSD(T)(F12) level in combination with appropriate basis sets to obtain nearly CBS accuracy. Also, larger systems are still feasible on a standard cluster as demonstrated for H3O+(H2O)25Cl– with 80 atoms.

Supporting Information

ARTICLE SECTIONS
Jump To

The Supporting Information includes the optimized geometries in xyz format and the tables monitoring the convergence of the incremental series for CCSD(F12), the fixed-RI-MP2-F12/2B contribution, CCSD(T)(F12), MP2, MP2-F12, and CCSD(T)(F12)|MP2-F12. This information is available free of charge via the Internet at http://pubs.acs.org/.

Terms & Conditions

Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

Cited By

This article is cited by 48 publications.

  1. Ashleigh L. Barnes, Dmytro Bykov, Dmitry I. Lyakh, Tjerk P. Straatsma. Multilayer Divide-Expand-Consolidate Coupled-Cluster Method: Demonstrative Calculations of the Adsorption Energy of Carbon Dioxide in the Mg-MOF-74 Metal–Organic Framework. The Journal of Physical Chemistry A 2019, 123 (40) , 8734-8743. https://doi.org/10.1021/acs.jpca.9b08077
  2. Péter R. Nagy, Mihály Kállay. Approaching the Basis Set Limit of CCSD(T) Energies for Large Molecules with Local Natural Orbital Coupled-Cluster Methods. Journal of Chemical Theory and Computation 2019, 15 (10) , 5275-5298. https://doi.org/10.1021/acs.jctc.9b00511
  3. Soumen Ghosh, Pragya Verma, Christopher J. Cramer, Laura Gagliardi, Donald G. Truhlar. Combining Wave Function Methods with Density Functional Theory for Excited States. Chemical Reviews 2018, 118 (15) , 7249-7292. https://doi.org/10.1021/acs.chemrev.8b00193
  4. Benjamin Fiedler, Daniel Himmel, Ingo Krossing, and Joachim Friedrich . More Stable Template Localization for an Incremental Focal-Point Approach—Implementation and Application to the Intramolecular Decomposition of Tris-perfluoro-tert-butoxyalane. Journal of Chemical Theory and Computation 2018, 14 (2) , 557-571. https://doi.org/10.1021/acs.jctc.7b00707
  5. Benjamin Fiedler, Gunnar Schmitz, Christof Hättig, and Joachim Friedrich . Combining Accuracy and Efficiency: An Incremental Focal-Point Method Based on Pair Natural Orbitals. Journal of Chemical Theory and Computation 2017, 13 (12) , 6023-6042. https://doi.org/10.1021/acs.jctc.7b00654
  6. Manuel Sparta, Marius Retegan, Peter Pinski, Christoph Riplinger, Ute Becker, and Frank Neese . Multilevel Approaches within the Local Pair Natural Orbital Framework. Journal of Chemical Theory and Computation 2017, 13 (7) , 3198-3207. https://doi.org/10.1021/acs.jctc.7b00260
  7. Benjamin Fiedler, Sonia Coriani, and Joachim Friedrich . Molecular Dipole Moments within the Incremental Scheme Using the Domain-Specific Basis-Set Approach. Journal of Chemical Theory and Computation 2016, 12 (7) , 3040-3052. https://doi.org/10.1021/acs.jctc.6b00076
  8. Jann A. Frey, Christof Holzer, Wim Klopper, and Samuel Leutwyler . Experimental and Theoretical Determination of Dissociation Energies of Dispersion-Dominated Aromatic Molecular Complexes. Chemical Reviews 2016, 116 (9) , 5614-5641. https://doi.org/10.1021/acs.chemrev.5b00652
  9. Tony Anacker, J. Grant Hill, and Joachim Friedrich . Optimized Basis Sets for the Environment in the Domain-Specific Basis Set Approach of the Incremental Scheme. The Journal of Physical Chemistry A 2016, 120 (15) , 2443-2458. https://doi.org/10.1021/acs.jpca.6b01097
  10. Tony Anacker, David P. Tew, and Joachim Friedrich . First UHF Implementation of the Incremental Scheme for Open-Shell Systems. Journal of Chemical Theory and Computation 2016, 12 (1) , 65-78. https://doi.org/10.1021/acs.jctc.5b00933
  11. Dimitrios G. Liakos and Frank Neese . Is It Possible To Obtain Coupled Cluster Quality Energies at near Density Functional Theory Cost? Domain-Based Local Pair Natural Orbital Coupled Cluster vs Modern Density Functional Theory. Journal of Chemical Theory and Computation 2015, 11 (9) , 4054-4063. https://doi.org/10.1021/acs.jctc.5b00359
  12. Joachim Friedrich . Efficient Calculation of Accurate Reaction Energies—Assessment of Different Models in Electronic Structure Theory. Journal of Chemical Theory and Computation 2015, 11 (8) , 3596-3609. https://doi.org/10.1021/acs.jctc.5b00087
  13. Dimitrios G. Liakos, Manuel Sparta, Manoj K. Kesharwani, Jan M. L. Martin, and Frank Neese . Exploring the Accuracy Limits of Local Pair Natural Orbital Coupled-Cluster Theory. Journal of Chemical Theory and Computation 2015, 11 (4) , 1525-1539. https://doi.org/10.1021/ct501129s
  14. Konstantinos D. Vogiatzis, Wim Klopper, and Joachim Friedrich . Non-covalent Interactions of CO2 with Functional Groups of Metal–Organic Frameworks from a CCSD(T) Scheme Applicable to Large Systems. Journal of Chemical Theory and Computation 2015, 11 (4) , 1574-1584. https://doi.org/10.1021/ct5011888
  15. Jun Zhang and Michael Dolg . Third-Order Incremental Dual-Basis Set Zero-Buffer Approach for Large High-Spin Open-Shell Systems. Journal of Chemical Theory and Computation 2015, 11 (3) , 962-968. https://doi.org/10.1021/ct501052e
  16. María Pilar de Lara-Castells, Hermann Stoll, and Alexander O. Mitrushchenkov . Assessing the Performance of Dispersionless and Dispersion-Accounting Methods: Helium Interaction with Cluster Models of the TiO2(110) Surface. The Journal of Physical Chemistry A 2014, 118 (33) , 6367-6384. https://doi.org/10.1021/jp412765t
  17. Luke Fiedler, Hannah R. Leverentz, Santhanamoorthi Nachimuthu, Joachim Friedrich, and Donald G. Truhlar . Nitrogen and Sulfur Compounds in Atmospheric Aerosols: A New Parametrization of Polarized Molecular Orbital Model Chemistry and Its Validation against Converged CCSD(T) Calculations for Large Clusters. Journal of Chemical Theory and Computation 2014, 10 (8) , 3129-3139. https://doi.org/10.1021/ct5003169
  18. Elena Voloshina and Beate Paulus . First Multireference Correlation Treatment of Bulk Metals. Journal of Chemical Theory and Computation 2014, 10 (4) , 1698-1706. https://doi.org/10.1021/ct401040t
  19. Joachim Friedrich and Julia Hänchen . Incremental CCSD(T)(F12*)|MP2: A Black Box Method To Obtain Highly Accurate Reaction Energies. Journal of Chemical Theory and Computation 2013, 9 (12) , 5381-5394. https://doi.org/10.1021/ct4008074
  20. Jun Zhang and Michael Dolg . Third-Order Incremental Dual-Basis Set Zero-Buffer Approach: An Accurate and Efficient Way To Obtain CCSD and CCSD(T) Energies. Journal of Chemical Theory and Computation 2013, 9 (7) , 2992-3003. https://doi.org/10.1021/ct400284d
  21. Vibin Abraham, Nicholas J. Mayhall. Cluster many-body expansion: A many-body expansion of the electron correlation energy about a cluster mean field reference. The Journal of Chemical Physics 2021, 155 (5) , 054101. https://doi.org/10.1063/5.0057752
  22. Prakash Verma, Lee Huntington, Marc P. Coons, Yukio Kawashima, Takeshi Yamazaki, Arman Zaribafiyan. Scaling up electronic structure calculations on quantum computers: The frozen natural orbital based method of increments. The Journal of Chemical Physics 2021, 155 (3) , 034110. https://doi.org/10.1063/5.0054647
  23. John Rogers, Tsung-Han Lee, Sahar Pakdel, Wenhu Xu, Vladimir Dobrosavljević, Yong-Xin Yao, Ove Christiansen, Nicola Lanatà. Bypassing the computational bottleneck of quantum-embedding theories for strong electron correlations with machine learning. Physical Review Research 2021, 3 (1) https://doi.org/10.1103/PhysRevResearch.3.013101
  24. Marius S. Frank, Gunnar Schmitz, Christof Hättig. Implementation of the iterative triples model CC3 for excitation energies using pair natural orbitals and Laplace transformation techniques. The Journal of Chemical Physics 2020, 153 (3) , 034109. https://doi.org/10.1063/5.0012597
  25. John M. Herbert. Fantasy versus reality in fragment-based quantum chemistry. The Journal of Chemical Physics 2019, 151 (17) , 170901. https://doi.org/10.1063/1.5126216
  26. Hermann Stoll. Toward a wavefunction-based treatment of strong electron correlation in extended systems by means of incremental methods. The Journal of Chemical Physics 2019, 151 (4) , 044104. https://doi.org/10.1063/1.5109860
  27. Yang Guo, Kantharuban Sivalingam, Edward F. Valeev, Frank Neese. Explicitly correlated N-electron valence state perturbation theory (NEVPT2-F12). The Journal of Chemical Physics 2017, 147 (6) , 064110. https://doi.org/10.1063/1.4996560
  28. Péter R. Nagy, Mihály Kállay. Optimization of the linear-scaling local natural orbital CCSD(T) method: Redundancy-free triples correction using Laplace transform. The Journal of Chemical Physics 2017, 146 (21) , 214106. https://doi.org/10.1063/1.4984322
  29. Andreas Grüneis, So Hirata, Yu-ya Ohnishi, Seiichiro Ten-no. Perspective: Explicitly correlated electronic structure theory for complex systems. The Journal of Chemical Physics 2017, 146 (8) , 080901. https://doi.org/10.1063/1.4976974
  30. Haoyu S. Yu, Shaohong L. Li, Donald G. Truhlar. Perspective: Kohn-Sham density functional theory descending a staircase. The Journal of Chemical Physics 2016, 145 (13) , 130901. https://doi.org/10.1063/1.4963168
  31. David P. Tew. Explicitly correlated coupled-cluster theory with Brueckner orbitals. The Journal of Chemical Physics 2016, 145 (7) , 074103. https://doi.org/10.1063/1.4960655
  32. Bence Hégely, Péter R. Nagy, György G. Ferenczy, Mihály Kállay. Exact density functional and wave function embedding schemes based on orbital localization. The Journal of Chemical Physics 2016, 145 (6) , 064107. https://doi.org/10.1063/1.4960177
  33. Joachim Friedrich, Benjamin Fiedler. Accurate calculation of binding energies for molecular clusters – Assessment of different models. Chemical Physics 2016, 472 , 72-80. https://doi.org/10.1016/j.chemphys.2016.02.022
  34. Michael von Domaros, Sascha Jähnigen, Joachim Friedrich, Barbara Kirchner. Quantum cluster equilibrium model of N -methylformamide–water binary mixtures. The Journal of Chemical Physics 2016, 144 (6) , 064305. https://doi.org/10.1063/1.4941278
  35. Christoph Riplinger, Peter Pinski, Ute Becker, Edward F. Valeev, Frank Neese. Sparse maps—A systematic infrastructure for reduced-scaling electronic structure methods. II. Linear scaling domain based pair natural orbital coupled cluster theory. The Journal of Chemical Physics 2016, 144 (2) , 024109. https://doi.org/10.1063/1.4939030
  36. Klaus Banert, Manfred Hagedorn, Tom Pester, Nicole Siebert, Cornelius Staude, Ivan Tchernook, Katharina Rathmann, Oldamur Hollóczki, Joachim Friedrich. Rearrangement Reactions of Tritylcarbenes: Surprising Ring Expansion and Computational Investigation. Chemistry - A European Journal 2015, 21 (42) , 14911-14923. https://doi.org/10.1002/chem.201501352
  37. María Pilar de Lara-Castells, Alexander O. Mitrushchenkov, Hermann Stoll. Combining density functional and incremental post-Hartree-Fock approaches for van der Waals dominated adsorbate-surface interactions: Ag 2 /graphene. The Journal of Chemical Physics 2015, 143 (10) , 102804. https://doi.org/10.1063/1.4919397
  38. Mihály Kállay. Linear-scaling implementation of the direct random-phase approximation. The Journal of Chemical Physics 2015, 142 (20) , 204105. https://doi.org/10.1063/1.4921542
  39. Joachim Friedrich, Harley R. McAlexander, Ashutosh Kumar, T. Daniel Crawford. Incremental evaluation of coupled cluster dipole polarizabilities. Physical Chemistry Chemical Physics 2015, 17 (22) , 14284-14296. https://doi.org/10.1039/C4CP05076B
  40. Tony Anacker, Joachim Friedrich. New accurate benchmark energies for large water clusters: DFT is better than expected. Journal of Computational Chemistry 2014, 35 (8) , 634-643. https://doi.org/10.1002/jcc.23539
  41. . Theoretische Chemie 2013. Nachrichten aus der Chemie 2014,,, 322-329. https://doi.org/10.1002/nadc.201490089
  42. Michael Dolg. Approaching the complete basis set limit of CCSD(T) for large systems by the third-order incremental dual-basis set zero-buffer F12 method. The Journal of Chemical Physics 2014, 140 (4) , 044114. https://doi.org/10.1063/1.4862826
  43. Barbara Kirchner, Frank Weinhold, Joachim Friedrich, Eva Perlt, Sebastian B. C. Lehmann. Quantum Cluster Equilibrium. 2014,,, 77-96. https://doi.org/10.1007/978-3-319-06379-9_4
  44. Manuel Sparta, Frank Neese. Chemical applications carried out by local pair natural orbital based coupled-cluster methods. Chem. Soc. Rev. 2014, 43 (14) , 5032-5041. https://doi.org/10.1039/C4CS00050A
  45. Christoph Riplinger, Barbara Sandhoefer, Andreas Hansen, Frank Neese. Natural triple excitations in local coupled cluster calculations with pair natural orbitals. The Journal of Chemical Physics 2013, 139 (13) , 134101. https://doi.org/10.1063/1.4821834
  46. Ingmar Polenz, Friedrich Georg Schmidt, Joachim Friedrich, Ivan Tchernook, Stefan Spange. Radical Polymerization of MMA Co-initiated by 2-Phenyloxazoline. Macromolecular Chemistry and Physics 2013, 214 (13) , 1473-1483. https://doi.org/10.1002/macp.201300200
  47. Tony Anacker, Joachim Friedrich. Highly accurate incremental CCSD(T) calculations on aqua- and amine-complexes. Molecular Physics 2013, 111 (9-11) , 1161-1172. https://doi.org/10.1080/00268976.2013.781693
  48. A. Roztoczyńska, A. Kaczmarek-Kędziera, R.W. Góra, W. Bartkowiak. How does the Boys and Bernardi counterpoise correction scheme affects the calculated interaction-induced electric properties? Model hydrogen-bonded systems as a case study. Chemical Physics Letters 2013, 571 , 28-33. https://doi.org/10.1016/j.cplett.2013.03.081

Pair your accounts.

Export articles to Mendeley

Get article recommendations from ACS based on references in your Mendeley library.

Pair your accounts.

Export articles to Mendeley

Get article recommendations from ACS based on references in your Mendeley library.

You’ve supercharged your research process with ACS and Mendeley!

STEP 1:
Click to create an ACS ID

Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

MENDELEY PAIRING EXPIRED
Your Mendeley pairing has expired. Please reconnect

This website uses cookies to improve your user experience. By continuing to use the site, you are accepting our use of cookies. Read the ACS privacy policy.

CONTINUE