From 222fb53f14e4e99147aafcd614232f018173e4c6 Mon Sep 17 00:00:00 2001 From: Pierre-Francois Loos Date: Thu, 10 Sep 2020 15:37:48 +0200 Subject: [PATCH] subsets --- config.toml | 15 ++++++++---- content/_index.md | 1 + content/subsets.md | 48 +++++++++++++++++++++++++++++++++++++++ static/img/molecules.pdf | Bin 0 -> 59439 bytes static/img/subsets.pdf | Bin 0 -> 35598 bytes 5 files changed, 59 insertions(+), 5 deletions(-) create mode 100644 content/subsets.md create mode 100644 static/img/molecules.pdf create mode 100644 static/img/subsets.pdf diff --git a/config.toml b/config.toml index 99d437e6..3d9b5ef8 100644 --- a/config.toml +++ b/config.toml @@ -37,30 +37,35 @@ theme = "beautifulhugo" url = "" weight = 1 +[[menu.main]] + name = "Subsets" + url = "subsets" + weight = 3 + [[menu.main]] name = "Dataset" url = "dataset" - weight = 2 + weight = 4 [[menu.main]] name = "Publications" url = "publications" - weight = 3 + weight = 5 [[menu.main]] name = "About" url = "about" - weight = 4 + weight = 6 [[menu.main]] name = "Funding" url = "funding" - weight = 5 + weight = 7 [[menu.main]] identifier = "external" name = "External links" - weight = 6 + weight = 8 [[menu.main]] parent="external" diff --git a/content/_index.md b/content/_index.md index 66e62cfb..02d6dece 100644 --- a/content/_index.md +++ b/content/_index.md @@ -7,6 +7,7 @@ draft: false ## The QUEST database of excitation energies The purpose of the [QUEST](about) project is to provide reference (i.e. highly accurate) vertical excitation energies for small- and medium-sized molecules in order to compare the precision of computational quantum chemistry methods thanks to reliable and fair statistical analyses. One of the key aspect of the QUEST dataset is that it does not rely on any experimental values, avoiding potential biases inherently linked to experiments and facilitating in the process theoretical cross comparisons. +The QUEST dataset of vertical excitations is composed by 5 subsets which are described in the [SUBSETS section](subsets). This website is an integral part of this project and makes it possible to dynamically compare the accuracy of a given method with respect to various variables such as the molecule size or its family, the nature of the excited states, the size of the basis set, and many others. See the [DATASET section](dataset). diff --git a/content/subsets.md b/content/subsets.md new file mode 100644 index 00000000..c7a06c54 --- /dev/null +++ b/content/subsets.md @@ -0,0 +1,48 @@ +--- +title: "Subsets" +date: 2020-09-10 15:00 +draft: false +--- + +The QUEST database provides theoretical best estimates (TBEs) for more than 470 highly-accurate excitation energies of various natures (valence, Rydberg, $n \ra \pis$, $\pi \ra \pis$, singlet, doublet, triplet, and double excitations) for molecules ranging from diatomics to molecules as large as naphthalene. +The molecules included in the QUEST dataset have been systematically optimized at the CC3/aug-cc-pVTZ level of theory, except for a very few cases. +The QUEST dataset of vertical excitations is composed by 5 subsets: + +{{< figure src="/img/subsets.pdf" title="Composition of each of the five subsets making up the present QUEST dataset of highly-accurate vertical excitation energies" >}} + +{{< figure src="/img/molecules.pdf" title="Molecules each of the five subsets making up the present QUEST dataset of highly-accurate vertical excitation energies: QUEST#1 (red), QUEST#2 (magenta and/or underlined), QUEST#3 (black), QUEST#4 (green), and QUEST#5 (blue)." >}} + +### [QUEST#1](https://pubs.acs.org/doi/10.1021/acs.jctc.8b00406) +The QUEST#1 benchmark set consists of 110 vertical excitation energies (as well as oscillator strengths) from 18 molecules with sizes ranging from one to three non-hydrogen atoms (water, hydrogen sulfide, ammonia, hydrogen chloride, dinitrogen, carbon monoxide, acetylene, ethylene, formaldehyde, methanimine, thioformaldehyde, acetaldehyde, cyclopropene, diazomethane, formamide, ketene, nitrosomethane, and the smallest +streptocyanine). For this set, we provided two sets of TBEs: i) one obtained within the frozen-core approximation and the aug-cc-pVTZ basis set, and ii) another one including further corrections for basis set incompleteness and "all electron" effects. +For the former set, we systematically selected FCI/aug-cc-pVTZ values to define our TBEs except in very few cases. +For the latter set, both the "all electron" correlation and the basis set corrections were systematically obtained at the CC3 level of theory and with the d-aug-cc-pV5Z basis for the nine smallest molecules, and slightly more compact basis sets for the larger compounds. + +### [QUEST#2](https://pubs.acs.org/doi/10.1021/acs.jctc.8b01205) +The QUEST#2 benchmark set reports reference energies for double excitations. +This set gathers 20 vertical transitions from 14 small- and medium-size molecules (acrolein, benzene, beryllium atom, butadiene, carbon dimer and trimer, ethylene, formaldehyde, glyoxal, hexatriene, nitrosomethane, nitroxyl, pyrazine, and tetrazine). +The TBEs of the QUEST#2 set are obtained with SCI and/or multiconfigurational [CASSCF, CASPT2, (X)MS-CASPT2, and NEVPT2] calculations depending on the size of the molecules and the level of theory that we could afford. +An important addition to this second study was the inclusion of various flavors of multiconfigurational methods (CASSCF, CASPT2, and NEVPT2) in addition to high-order CC methods including, at least, perturbative triples (CC3, CCSDT, CCSDTQ, etc). + +### [QUEST#3](https://pubs.acs.org/doi/10.1021/acs.jctc.9b01216) +The QUEST#3 benchmark set is, by far, our largest set, and consists of highly accurate vertical transition energies and oscillator strengths obtained for 27 molecules encompassing 4, 5, and 6 non-hydrogen atoms (acetone, acrolein, benzene, butadiene, cyanoacetylene, cyanoformaldehyde, cyanogen, cyclopentadiene, cyclopropenone, cyclopropenethione, diacetylene, furan, glyoxal, imidazole, isobutene, methylenecyclopropene, propynal, pyrazine, pyridazine, pyridine, pyrimidine, pyrrole, tetrazine, thioacetone, thiophene, thiopropynal, and triazine) for a total of 238 vertical transition energies and 90 oscillator strengths with a reasonably good balance between singlet, triplet, valence, and Rydberg excited states. +For these 238 transitions, we have estimated that 224 are chemically accurate for the considered geometry. +To define the TBEs of the QUEST#3 set, we employed CC methods up to the highest technically possible order (CC3, CCSDT, and CCSDTQ), and, when affordable SCI calculations with very large reference spaces (up to hundred million determinants in certain cases), as well as the most reliable multiconfigurational method, NEVPT2, for double excitations. +Most of our TBEs are based on CCSDTQ (4 non-hydrogen atoms) or CCSDT (5 and 6 non-hydrogen atoms) excitation energies. +For all the transitions of the QUEST#3 set, we reported at least CCSDT/aug-cc-pVTZ (sometimes with basis set extrapolation) and CC3/aug-cc-pVQZ transition energies as well as CC3/aug-cc-pVTZ oscillator strengths for each dipole-allowed transition. + +### [QUEST#4](https://pubs.acs.org/doi/10.1021/acs.jctc.0c00227) +The QUEST#4 benchmark set consists of two subsets of excitations and oscillator strengths. +An "exotic" subset of 30 excited states for closed-shell molecules containing F, Cl, P, and Si atoms (carbonyl fluoride, \ce{CCl2}, \ce{CClF}, \ce{CF2}, difluorodiazirine, formyl fluoride, \ce{HCCl}, \ce{HCF}, \ce{HCP}, \ce{HPO}, \ce{HPS}, \ce{HSiF}, \ce{SiCl2}, and silylidene) and a "radical" subset of 51 doublet-doublet transitions in small radicals (allyl, \ce{BeF}, \ce{BeH}, \ce{BH2}, \ce{CH}, \ce{CH3}, \ce{CN}, \ce{CNO}, \ce{CON}, \ce{CO+}, \ce{F2BO}, \ce{F2BS}, \ce{H2BO}, \ce{HCO}, \ce{HOC}, \ce{H2PO}, \ce{H2PS}, \ce{NCO}, \ce{NH2}, nitromethyl, \ce{NO}, \ce{OH}, \ce{PH2}, and vinyl) characterized by open-shell electronic configurations and an unpaired electron. +This represents a total of 81 high-quality TBEs, the vast majority being obtained at the FCI level with at least the aug-cc-pVTZ basis set. +We further performed high-order CC calculations to ascertain these estimates. + +### [QUEST#5]() + +The QUEST#5 subset is composed by additional accurate excitation energies that we have produced for the present website. +This new set gathers small molecules as well as larger molecules (aza-naphthalene, benzoquinone, cyclopentadienone, cyclopentadienethione, hexatriene, maleimide, naphthalene, nitroxyl, streptocyanine-C3, streptocyanine-C5, and thioacrolein). +QUEST#5 does also provide additional FCI/6-31+G* estimates of the lowest singlet and triplet transitions for the five- and six-membered rings considered in QUEST#3. + + + + diff --git a/static/img/molecules.pdf b/static/img/molecules.pdf new file mode 100644 index 0000000000000000000000000000000000000000..f5be1ae91d6481ff350e576e1792bfa4138b528a GIT binary patch literal 59439 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