Performance of Localized-Orbital Coupled-Cluster Approaches for the Conformational Energies of Longer n ‑Alkane Chains
We report an update and enhancement of the ACONFL (conformer energies of large alkanes [ J. Phys. Chem. A 2022, 126 , 3521–3535]) dataset. For the ACONF12 ( n -dodecane) subset, we report basis set limit canonical coupled-cluster with singles, doubles, and perturbative triples [i.e., CCSD(T)] refere...
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ftunivfreestate:oai:figshare.com:article/21714101 2023-05-15T17:54:04+02:00 Performance of Localized-Orbital Coupled-Cluster Approaches for the Conformational Energies of Longer n ‑Alkane Chains Golokesh Santra (6824864) Jan M.L. Martin (537232) 2022-12-12T00:00:00Z https://doi.org/10.1021/acs.jpca.2c06407.s002 unknown https://figshare.com/articles/dataset/Performance_of_Localized-Orbital_Coupled-Cluster_Approaches_for_the_Conformational_Energies_of_Longer_i_n_i_Alkane_Chains/21714101 doi:10.1021/acs.jpca.2c06407.s002 CC BY-NC 4.0 CC-BY-NC Biophysics Biochemistry Physiology Evolutionary Biology Cancer Space Science Biological Sciences not elsewhere classified Chemical Sciences not elsewhere classified s66x8 noncovalent interactions related truncation errors may upend orderings given accuracy threshold gets slightly better best pick among >‑ alkane chains )]- based post based methods tested revised reference data less accurate methods vtight – tight statistically similar accuracy large alkanes [< explicitly correlated dlpno e . ccsd f12 ]/ aug revised aconfl set f12 *)- mp2 cutpno </ sub accurate methods reference datasets )/ aug f12 extrapolation basis set aconfl set aconf12 set ultimately finding perturbative triples n </ n -</ improves things gradually tightening error statistics dodecane conformers cutoffs improves conventional ccsd conformer energies conformational energies composite scheme canonical mp2 Dataset 2022 ftunivfreestate https://doi.org/10.1021/acs.jpca.2c06407.s002 2022-12-16T00:31:32Z We report an update and enhancement of the ACONFL (conformer energies of large alkanes [ J. Phys. Chem. A 2022, 126 , 3521–3535]) dataset. For the ACONF12 ( n -dodecane) subset, we report basis set limit canonical coupled-cluster with singles, doubles, and perturbative triples [i.e., CCSD(T)] reference data obtained from the MP2-F12/cc-pV{T,Q}Z-F12 extrapolation, [CCSD(F12*)-MP2-F12]/aug-cc-pVTZ-F12, and a (T) correction from conventional CCSD(T)/aug-cc-pV{D,T}Z calculations. Then, we explored the performance of a variety of single and composite localized-orbital CCSD(T) approximations, ultimately finding an affordable localized natural orbital CCSD(T) [LNO-CCSD(T)]-based post-MP2 correction that agrees to 0.006 kcal/mol mean absolute deviation with the revised canonical reference data. In tandem with canonical MP2-F12 complete basis set extrapolation, this was then used to re-evaluate the ACONF16 and ACONF20 subsets for n- hexadecane and n- icosane, respectively. Combining those with the revised canonical reference data for the dodecane conformers (i.e., ACONF12 subset), a revised ACONFL set was obtained. It was then used to assess the performance of different localized-orbital coupled-cluster approaches, such as pair natural orbital localized CCSD(T) [PNO-LCCSD(T)] as implemented in MOLPRO, DLPNO-CCSD(T 0 ) and DLPNO-CCSD(T 1 ) as implemented in ORCA, and LNO-CCSD(T) as implemented in MRCC, at their respective “Normal”, “Tight”, “vTight”, and “vvTight” accuracy settings. For a given accuracy threshold and basis set, DLPNO-CCSD(T 1 ) and DLPNO-CCSD(T 0 ) perform comparably. With “VeryTightPNO” cutoffs, explicitly correlated DLPNO-CCSD(T 1 )-F12/VDZ-F12 is the best pick among all the DLPNO-based methods tested. To isolate basis set incompleteness from localized-orbital-related truncation errors (domain, LNOs), we have also compared the localized coupled-cluster approaches with canonical DF-CCSD(T)/aug-cc-pVTZ for the ACONF12 set. We found that gradually tightening the cutoffs improves the performance of ... Dataset Orca KovsieScholar Repository (University of the Free State - UFS UV) |
institution |
Open Polar |
collection |
KovsieScholar Repository (University of the Free State - UFS UV) |
op_collection_id |
ftunivfreestate |
language |
unknown |
topic |
Biophysics Biochemistry Physiology Evolutionary Biology Cancer Space Science Biological Sciences not elsewhere classified Chemical Sciences not elsewhere classified s66x8 noncovalent interactions related truncation errors may upend orderings given accuracy threshold gets slightly better best pick among >‑ alkane chains )]- based post based methods tested revised reference data less accurate methods vtight – tight statistically similar accuracy large alkanes [< explicitly correlated dlpno e . ccsd f12 ]/ aug revised aconfl set f12 *)- mp2 cutpno </ sub accurate methods reference datasets )/ aug f12 extrapolation basis set aconfl set aconf12 set ultimately finding perturbative triples n </ n -</ improves things gradually tightening error statistics dodecane conformers cutoffs improves conventional ccsd conformer energies conformational energies composite scheme canonical mp2 |
spellingShingle |
Biophysics Biochemistry Physiology Evolutionary Biology Cancer Space Science Biological Sciences not elsewhere classified Chemical Sciences not elsewhere classified s66x8 noncovalent interactions related truncation errors may upend orderings given accuracy threshold gets slightly better best pick among >‑ alkane chains )]- based post based methods tested revised reference data less accurate methods vtight – tight statistically similar accuracy large alkanes [< explicitly correlated dlpno e . ccsd f12 ]/ aug revised aconfl set f12 *)- mp2 cutpno </ sub accurate methods reference datasets )/ aug f12 extrapolation basis set aconfl set aconf12 set ultimately finding perturbative triples n </ n -</ improves things gradually tightening error statistics dodecane conformers cutoffs improves conventional ccsd conformer energies conformational energies composite scheme canonical mp2 Golokesh Santra (6824864) Jan M.L. Martin (537232) Performance of Localized-Orbital Coupled-Cluster Approaches for the Conformational Energies of Longer n ‑Alkane Chains |
topic_facet |
Biophysics Biochemistry Physiology Evolutionary Biology Cancer Space Science Biological Sciences not elsewhere classified Chemical Sciences not elsewhere classified s66x8 noncovalent interactions related truncation errors may upend orderings given accuracy threshold gets slightly better best pick among >‑ alkane chains )]- based post based methods tested revised reference data less accurate methods vtight – tight statistically similar accuracy large alkanes [< explicitly correlated dlpno e . ccsd f12 ]/ aug revised aconfl set f12 *)- mp2 cutpno </ sub accurate methods reference datasets )/ aug f12 extrapolation basis set aconfl set aconf12 set ultimately finding perturbative triples n </ n -</ improves things gradually tightening error statistics dodecane conformers cutoffs improves conventional ccsd conformer energies conformational energies composite scheme canonical mp2 |
description |
We report an update and enhancement of the ACONFL (conformer energies of large alkanes [ J. Phys. Chem. A 2022, 126 , 3521–3535]) dataset. For the ACONF12 ( n -dodecane) subset, we report basis set limit canonical coupled-cluster with singles, doubles, and perturbative triples [i.e., CCSD(T)] reference data obtained from the MP2-F12/cc-pV{T,Q}Z-F12 extrapolation, [CCSD(F12*)-MP2-F12]/aug-cc-pVTZ-F12, and a (T) correction from conventional CCSD(T)/aug-cc-pV{D,T}Z calculations. Then, we explored the performance of a variety of single and composite localized-orbital CCSD(T) approximations, ultimately finding an affordable localized natural orbital CCSD(T) [LNO-CCSD(T)]-based post-MP2 correction that agrees to 0.006 kcal/mol mean absolute deviation with the revised canonical reference data. In tandem with canonical MP2-F12 complete basis set extrapolation, this was then used to re-evaluate the ACONF16 and ACONF20 subsets for n- hexadecane and n- icosane, respectively. Combining those with the revised canonical reference data for the dodecane conformers (i.e., ACONF12 subset), a revised ACONFL set was obtained. It was then used to assess the performance of different localized-orbital coupled-cluster approaches, such as pair natural orbital localized CCSD(T) [PNO-LCCSD(T)] as implemented in MOLPRO, DLPNO-CCSD(T 0 ) and DLPNO-CCSD(T 1 ) as implemented in ORCA, and LNO-CCSD(T) as implemented in MRCC, at their respective “Normal”, “Tight”, “vTight”, and “vvTight” accuracy settings. For a given accuracy threshold and basis set, DLPNO-CCSD(T 1 ) and DLPNO-CCSD(T 0 ) perform comparably. With “VeryTightPNO” cutoffs, explicitly correlated DLPNO-CCSD(T 1 )-F12/VDZ-F12 is the best pick among all the DLPNO-based methods tested. To isolate basis set incompleteness from localized-orbital-related truncation errors (domain, LNOs), we have also compared the localized coupled-cluster approaches with canonical DF-CCSD(T)/aug-cc-pVTZ for the ACONF12 set. We found that gradually tightening the cutoffs improves the performance of ... |
format |
Dataset |
author |
Golokesh Santra (6824864) Jan M.L. Martin (537232) |
author_facet |
Golokesh Santra (6824864) Jan M.L. Martin (537232) |
author_sort |
Golokesh Santra (6824864) |
title |
Performance of Localized-Orbital Coupled-Cluster Approaches for the Conformational Energies of Longer n ‑Alkane Chains |
title_short |
Performance of Localized-Orbital Coupled-Cluster Approaches for the Conformational Energies of Longer n ‑Alkane Chains |
title_full |
Performance of Localized-Orbital Coupled-Cluster Approaches for the Conformational Energies of Longer n ‑Alkane Chains |
title_fullStr |
Performance of Localized-Orbital Coupled-Cluster Approaches for the Conformational Energies of Longer n ‑Alkane Chains |
title_full_unstemmed |
Performance of Localized-Orbital Coupled-Cluster Approaches for the Conformational Energies of Longer n ‑Alkane Chains |
title_sort |
performance of localized-orbital coupled-cluster approaches for the conformational energies of longer n ‑alkane chains |
publishDate |
2022 |
url |
https://doi.org/10.1021/acs.jpca.2c06407.s002 |
genre |
Orca |
genre_facet |
Orca |
op_relation |
https://figshare.com/articles/dataset/Performance_of_Localized-Orbital_Coupled-Cluster_Approaches_for_the_Conformational_Energies_of_Longer_i_n_i_Alkane_Chains/21714101 doi:10.1021/acs.jpca.2c06407.s002 |
op_rights |
CC BY-NC 4.0 |
op_rightsnorm |
CC-BY-NC |
op_doi |
https://doi.org/10.1021/acs.jpca.2c06407.s002 |
_version_ |
1766161777319477248 |