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, 12, 5381-5394
RETURN TO ISSUEPREVArticleNEXT

Incremental CCSD(T)(F12*)|MP2: A Black Box Method To Obtain Highly Accurate Reaction Energies

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, 12, 5381–5394
Publication Date (Web):November 18, 2013
https://doi.org/10.1021/ct4008074
Copyright © 2013 American Chemical Society
RIGHTS & PERMISSIONS
Article Views
704
Altmetric
-
Citations
59
LEARN ABOUT THESE METRICS
Read OnlinePDF (1 MB)
Get e-Alerts
Supporting Info (1)»
SUBJECTS:

Abstract

Abstract Image

In this work we present a new partitioning scheme for the incremental approach in combination with the efficient (F12*) approximation for explicitly correlated coupled cluster (J. Chem. Phys.2010, 132, 231102). Furthermore we establish a black-box truncation scheme which provides chemical accuracy for the absolute energies of 81 molecules and 51 reaction energies. The errors in the absolute CCSD(T)/cc-pVTZ-F12 energies due to the local approximations are characterized by mean = −0.24 kJ/mol, σ = 0.49 kJ/mol, mae = 0.37 kJ/mol, rmsd = 0.54 kJ/mol, and range = 3.63 kJ/mol. For the reaction energies we find mean = 0.07 kJ/mol, σ = 0.49 kJ/mol, mae = 0.33 kJ/mol, rmsd = 0.49 kJ/mol, and range = 2.40 kJ/mol. On the basis of these findings it is evident that the incremental scheme provides highly accurate CCSD(T) energies of benchmark quality.

Supporting Information

ARTICLE SECTIONS
Jump To

Reaction energies and the corresponding errors for all methods discussed in the text. Furthermore, the absolute energies of the incremental CCSD(T)(F12*) expansions. Finally, all coordinates of the molecular structures are included in atomic units. This material 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 59 publications.

  1. Qianli Ma, Hans-Joachim Werner. Scalable Electron Correlation Methods. 8. Explicitly Correlated Open-Shell Coupled-Cluster with Pair Natural Orbitals PNO-RCCSD(T)-F12 and PNO-UCCSD(T)-F12. Journal of Chemical Theory and Computation 2021, 17 (2) , 902-926. https://doi.org/10.1021/acs.jctc.0c01129
  2. Zack M. Williams, Timothy C. Wiles, Frederick R. Manby. Accurate Hybrid Density Functionals with UW12 Correlation. Journal of Chemical Theory and Computation 2020, 16 (10) , 6176-6194. https://doi.org/10.1021/acs.jctc.0c00442
  3. Qianli Ma, Hans-Joachim Werner. Scalable Electron Correlation Methods. 7. Local Open-Shell Coupled-Cluster Methods Using Pair Natural Orbitals: PNO-RCCSD and PNO-UCCSD. Journal of Chemical Theory and Computation 2020, 16 (5) , 3135-3151. https://doi.org/10.1021/acs.jctc.0c00192
  4. Dominique A. Wappett, Lars Goerigk. Toward a Quantum-Chemical Benchmark Set for Enzymatically Catalyzed Reactions: Important Steps and Insights. The Journal of Physical Chemistry A 2019, 123 (32) , 7057-7074. https://doi.org/10.1021/acs.jpca.9b05088
  5. Asim Najibi, Lars Goerigk. The Nonlocal Kernel in van der Waals Density Functionals as an Additive Correction: An Extensive Analysis with Special Emphasis on the B97M-V and ωB97M-V Approaches. Journal of Chemical Theory and Computation 2018, 14 (11) , 5725-5738. https://doi.org/10.1021/acs.jctc.8b00842
  6. 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
  7. Qianli Ma and Hans-Joachim Werner . Scalable Electron Correlation Methods. 5. Parallel Perturbative Triples Correction for Explicitly Correlated Local Coupled Cluster with Pair Natural Orbitals. Journal of Chemical Theory and Computation 2018, 14 (1) , 198-215. https://doi.org/10.1021/acs.jctc.7b01141
  8. 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
  9. Qianli Ma, Max Schwilk, Christoph Köppl, and Hans-Joachim Werner . Scalable Electron Correlation Methods. 4. Parallel Explicitly Correlated Local Coupled Cluster with Pair Natural Orbitals (PNO-LCCSD-F12). Journal of Chemical Theory and Computation 2017, 13 (10) , 4871-4896. https://doi.org/10.1021/acs.jctc.7b00799
  10. Max Schwilk, Qianli Ma, Christoph Köppl, and Hans-Joachim Werner . Scalable Electron Correlation Methods. 3. Efficient and Accurate Parallel Local Coupled Cluster with Pair Natural Orbitals (PNO-LCCSD). Journal of Chemical Theory and Computation 2017, 13 (8) , 3650-3675. https://doi.org/10.1021/acs.jctc.7b00554
  11. Gunnar Schmitz and Christof Hättig . Accuracy of Explicitly Correlated Local PNO-CCSD(T). Journal of Chemical Theory and Computation 2017, 13 (6) , 2623-2633. https://doi.org/10.1021/acs.jctc.7b00180
  12. Mateusz Marianski, Adriana Supady, Teresa Ingram, Markus Schneider, and Carsten Baldauf . Assessing the Accuracy of Across-the-Scale Methods for Predicting Carbohydrate Conformational Energies for the Examples of Glucose and α-Maltose. Journal of Chemical Theory and Computation 2016, 12 (12) , 6157-6168. https://doi.org/10.1021/acs.jctc.6b00876
  13. 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
  14. 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
  15. 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
  16. 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
  17. Qianli Ma and Hans-Joachim Werner . Scalable Electron Correlation Methods. 2. Parallel PNO-LMP2-F12 with Near Linear Scaling in the Molecular Size. Journal of Chemical Theory and Computation 2015, 11 (11) , 5291-5304. https://doi.org/10.1021/acs.jctc.5b00843
  18. Yury Minenkov, Edrisse Chermak, and Luigi Cavallo . Accuracy of DLPNO–CCSD(T) Method for Noncovalent Bond Dissociation Enthalpies from Coinage Metal Cation Complexes. Journal of Chemical Theory and Computation 2015, 11 (10) , 4664-4676. https://doi.org/10.1021/acs.jctc.5b00584
  19. 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
  20. 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
  21. 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
  22. 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
  23. 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
  24. 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
  25. Joachim Friedrich , Haoyu Yu, Hannah R. Leverentz, Peng Bai, J. Ilja Siepmann, and Donald G. Truhlar . Water 26-mers Drawn from Bulk Simulations: Benchmark Binding Energies for Unprecedentedly Large Water Clusters and Assessment of the Electrostatically Embedded Three-Body and Pairwise Additive Approximations. The Journal of Physical Chemistry Letters 2014, 5 (4) , 666-670. https://doi.org/10.1021/jz500079e
  26. 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
  27. Alexander Lipp, Shorouk O. Badir, Ryan Dykstra, Osvaldo Gutierrez, Gary A. Molander. Catalyst‐Free Decarbonylative Trifluoromethylthiolation Enabled by Electron Donor‐Acceptor Complex Photoactivation. Advanced Synthesis & Catalysis 2021, 363 (14) , 3507-3520. https://doi.org/10.1002/adsc.202100469
  28. 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
  29. Arno Förster, Lucas Visscher. Double hybrid DFT calculations with Slater type orbitals. Journal of Computational Chemistry 2020, 41 (18) , 1660-1684. https://doi.org/10.1002/jcc.26209
  30. Sree Ganesh Balasubramani, Guo P. Chen, Sonia Coriani, Michael Diedenhofen, Marius S. Frank, Yannick J. Franzke, Filipp Furche, Robin Grotjahn, Michael E. Harding, Christof Hättig, Arnim Hellweg, Benjamin Helmich-Paris, Christof Holzer, Uwe Huniar, Martin Kaupp, Alireza Marefat Khah, Sarah Karbalaei Khani, Thomas Müller, Fabian Mack, Brian D. Nguyen, Shane M. Parker, Eva Perlt, Dmitrij Rappoport, Kevin Reiter, Saswata Roy, Matthias Rückert, Gunnar Schmitz, Marek Sierka, Enrico Tapavicza, David P. Tew, Christoph van Wüllen, Vamsee K. Voora, Florian Weigend, Artur Wodyński, Jason M. Yu. TURBOMOLE: Modular program suite for ab initio quantum-chemical and condensed-matter simulations. The Journal of Chemical Physics 2020, 152 (18) , 184107. https://doi.org/10.1063/5.0004635
  31. Hans-Joachim Werner, Peter J. Knowles, Frederick R. Manby, Joshua A. Black, Klaus Doll, Andreas Heßelmann, Daniel Kats, Andreas Köhn, Tatiana Korona, David A. Kreplin, Qianli Ma, Thomas F. Miller, Alexander Mitrushchenkov, Kirk A. Peterson, Iakov Polyak, Guntram Rauhut, Marat Sibaev. The Molpro quantum chemistry package. The Journal of Chemical Physics 2020, 152 (14) , 144107. https://doi.org/10.1063/5.0005081
  32. Jitnapa Sirirak, Narin Lawan, Marc W. Van der Kamp, Jeremy N. Harvey, Adrian J. Mulholland. Benchmarking quantum mechanical methods for calculating reaction energies of reactions catalyzed by enzymes. PeerJ Physical Chemistry 2020, 2 , e8. https://doi.org/10.7717/peerj-pchem.8
  33. Mark Dornbach, Hans-Joachim Werner. Analytical energy gradients for local second-order Møller-Plesset perturbation theory using intrinsic bond orbitals. Molecular Physics 2019, 117 (9-12) , 1252-1263. https://doi.org/10.1080/00268976.2018.1537529
  34. Tina N. Mihm, Alexandra R. McIsaac, James J. Shepherd. An optimized twist angle to find the twist-averaged correlation energy applied to the uniform electron gas. The Journal of Chemical Physics 2019, 150 (19) , 191101. https://doi.org/10.1063/1.5091445
  35. Peter Pinski, Frank Neese. Analytical gradient for the domain-based local pair natural orbital second order Møller-Plesset perturbation theory method (DLPNO-MP2). The Journal of Chemical Physics 2019, 150 (16) , 164102. https://doi.org/10.1063/1.5086544
  36. Pierpaolo Morgante, Roberto Peverati. ACCDB: A collection of chemistry databases for broad computational purposes. Journal of Computational Chemistry 2019, 40 (6) , 839-848. https://doi.org/10.1002/jcc.25761
  37. Justyna Kozłowska, Max Schwilk, Agnieszka Roztoczyńska, Wojciech Bartkowiak. Assessment of DFT for endohedral complexes' dipole moment: PNO-LCCSD-F12 as a reference method. Physical Chemistry Chemical Physics 2018, 20 (46) , 29374-29388. https://doi.org/10.1039/C8CP05928D
  38. Tim Gould. ‘Diet GMTKN55’ offers accelerated benchmarking through a representative subset approach. Physical Chemistry Chemical Physics 2018, 20 (44) , 27735-27739. https://doi.org/10.1039/C8CP05554H
  39. Qianli Ma, Hans‐Joachim Werner. Explicitly correlated local coupled‐cluster methods using pair natural orbitals. WIREs Computational Molecular Science 2018, 8 (6) https://doi.org/10.1002/wcms.1371
  40. Karl Karu, Maksim Mišin, Heigo Ers, Jianwei Sun, Vladislav Ivaništšev. Performance of SCAN density functional for a set of ionic liquid ion pairs. International Journal of Quantum Chemistry 2018, 118 (13) https://doi.org/10.1002/qua.25582
  41. Nisha Mehta, Marcos Casanova-Páez, Lars Goerigk. Semi-empirical or non-empirical double-hybrid density functionals: which are more robust?. Physical Chemistry Chemical Physics 2018, 20 (36) , 23175-23194. https://doi.org/10.1039/C8CP03852J
  42. Thomas Kjærgaard, Pablo Baudin, Dmytro Bykov, Kasper Kristensen, Poul Jørgensen. The divide–expand–consolidate coupled cluster scheme. WIREs Computational Molecular Science 2017, 7 (6) https://doi.org/10.1002/wcms.1319
  43. Hans-Joachim Werner, Christoph Köppl, Qianli Ma, Max Schwilk. Explicitly Correlated Local Electron Correlation Methods. 2017,,, 1-79. https://doi.org/10.1002/9781119129271.ch1
  44. Joaquín Calbo, Juan C. Sancho-García, Enrique Ortí, Juan Aragó. DLPNO-CCSD(T) scaled methods for the accurate treatment of large supramolecular complexes. Journal of Computational Chemistry 2017, 38 (21) , 1869-1878. https://doi.org/10.1002/jcc.24835
  45. Lars Goerigk, Andreas Hansen, Christoph Bauer, Stephan Ehrlich, Asim Najibi, Stefan Grimme. A look at the density functional theory zoo with the advanced GMTKN55 database for general main group thermochemistry, kinetics and noncovalent interactions. Physical Chemistry Chemical Physics 2017, 19 (48) , 32184-32215. https://doi.org/10.1039/C7CP04913G
  46. James J. Shepherd. Communication: Convergence of many-body wave-function expansions using a plane-wave basis in the thermodynamic limit. The Journal of Chemical Physics 2016, 145 (3) , 031104. https://doi.org/10.1063/1.4958461
  47. 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
  48. Yang Min Wang, Christof Hättig, Simen Reine, Edward Valeev, Thomas Kjærgaard, Kasper Kristensen. Explicitly correlated second-order Møller-Plesset perturbation theory in a Divide-Expand-Consolidate (DEC) context. The Journal of Chemical Physics 2016, 144 (20) , 204112. https://doi.org/10.1063/1.4951696
  49. Wei Li, Zhigang Ni, Shuhua Li. Cluster-in-molecule local correlation method for post-Hartree–Fock calculations of large systems. Molecular Physics 2016, 114 (9) , 1447-1460. https://doi.org/10.1080/00268976.2016.1139755
  50. Fabijan Pavošević, Peter Pinski, Christoph Riplinger, Frank Neese, Edward F. Valeev. SparseMaps—A systematic infrastructure for reduced-scaling electronic structure methods. IV. Linear-scaling second-order explicitly correlated energy with pair natural orbitals. The Journal of Chemical Physics 2016, 144 (14) , 144109. https://doi.org/10.1063/1.4945444
  51. 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
  52. Jiří Chmela, Michael E. Harding, Dimitri Matioszek, Christopher E. Anson, Frank Breher, Wim Klopper. Differential Many-Body Cooperativity in Electronic Spectra of Oligonuclear Transition-Metal Complexes. ChemPhysChem 2016, 17 (1) , 37-45. https://doi.org/10.1002/cphc.201500626
  53. 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
  54. Peter Pinski, Christoph Riplinger, Edward F. Valeev, Frank Neese. Sparse maps—A systematic infrastructure for reduced-scaling electronic structure methods. I. An efficient and simple linear scaling local MP2 method that uses an intermediate basis of pair natural orbitals. The Journal of Chemical Physics 2015, 143 (3) , 034108. https://doi.org/10.1063/1.4926879
  55. 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
  56. 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
  57. 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
  58. Aleksandr V. Marenich, Junming Ho, Michelle L. Coote, Christopher J. Cramer, Donald G. Truhlar. Computational electrochemistry: prediction of liquid-phase reduction potentials. Phys. Chem. Chem. Phys. 2014, 16 (29) , 15068-15106. https://doi.org/10.1039/C4CP01572J
  59. 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

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