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Manuscript/QUESTDB.bib
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%% This BibTeX bibliography file was created using BibDesk.
%% http://bibdesk.sourceforge.net/
%% Created for Pierre-Francois Loos at 2020-09-07 09:29:50 +0200
%% Created for Pierre-Francois Loos at 2020-09-07 10:18:57 +0200
%% Saved with string encoding Unicode (UTF-8)
@article{Kucharski_1992,
Author = {Kucharski, S. A. and Bartlett, R. J.},
Date-Added = {2020-09-07 10:18:47 +0200},
Date-Modified = {2020-09-07 10:18:47 +0200},
Doi = {10.1063/1.463930},
Journal = {J. Chem. Phys.},
Pages = {4282},
Title = {The Coupled-Cluster Single, Double, Triple, and Quadruple Excitation Method},
Volume = {97},
Year = {1992},
Bdsk-Url-1 = {https://doi.org/10.1063/1.463930}}
@article{Oliphant_1991,
Author = {Oliphant, N. and Adamowicz, L.},
Date-Added = {2020-09-07 10:18:32 +0200},
Date-Modified = {2020-09-07 10:18:32 +0200},
Doi = {10.1063/1.461534},
Journal = {J. Chem. Phys.},
Pages = {6645},
Title = {Coupled-Cluster Method Truncated at Quadruples},
Volume = {95},
Year = {1991},
Bdsk-Url-1 = {https://doi.org/10.1063/1.461534}}
@article{Shi11,
Abstract = {The potential energy curves (PECs) of eight low-lying electronic states (X2Σ+, A2Π, B2Σ+, a4Σ+, D2Π, E2Σ+, 12Σ− and F2Δ) of the CN radical have been studied using the ab initio quantum chemical method. The calculations have been performed using the complete active space self-consistent field (CASSCF) method followed by the valence internally contracted multireference configuration interaction (MRCI) approach in combination with the correlation-consistent basis sets of Dunning and co-workers. The effects on the PECs by the core--valence correlation and relativistic corrections are taken into account. The way to consider the relativistic correction is to use the second-order Douglas--Kroll Hamiltonian approximation. The core--valence correlation correction calculations are performed with the cc-pCVQZ basis set. The relativistic correction is carried out at the level of cc-pV5Z basis set. In order to obtain more reliable results, the PECs determined by the MRCI calculations are also corrected for size-extensivity errors by means of the Davidson modification (MRCI+Q). The PECs are extrapolated to the complete basis set (CBS) limit by the total-energy extrapolation scheme. With these PECs, the spectroscopic parameters (Te, Re, ωe, ωexe, ωeуe, Be, αe and γe) are determined and compared with those reported in the literature. Finally, with the PECs obtained by the MRCI+Q/CV+DK+Q5 calculations, the complete vibrational states are computed for the eight electronic states by solving the ro-vibrational Schr{\"o}dinger equation for the non-rotating radical, and the vibrational levels and inertial rotation and centrifugal distortion constants of the first 11 vibrational states are reported, which agree favorably with the available experimental data. The spectroscopic parameters of 12Σ− and F2Δ electronic states obtained by the MRCI+Q/CV+DK+Q5 calculations should be good predictions for future laboratory experiments.},
Author = {De-heng Shi and Wen-tao Li and Jin-feng Sun and Zun-lue Zhu},
Date-Added = {2020-09-07 10:11:41 +0200},
Date-Modified = {2020-09-07 10:11:41 +0200},
Doi = {https://doi.org/10.1016/j.jqsrt.2011.06.002},
Issn = {0022-4073},
Journal = {J. Quant. Spectrosc. Radiat. Transf.},
Keywords = {Core--valence correlation correction, Relativistic correction, Molecular constant, Basis set extrapolation, Spectroscopic parameter},
Number = {14},
Pages = {2335--2346},
Title = {MRCI Study on Spectroscopic and Molecular Properties of Several Low-Lying Electronic States of the CN Radical},
Url = {http://www.sciencedirect.com/science/article/pii/S0022407311002147},
Volume = {112},
Year = {2011},
Bdsk-Url-1 = {http://www.sciencedirect.com/science/article/pii/S0022407311002147},
Bdsk-Url-2 = {https://doi.org/10.1016/j.jqsrt.2011.06.002}}
@article{Finley_1998,
Abstract = {An extension of the multiconfigurational second-order perturbation approach \{CASPT2\} is suggested, where several electronic states are coupled at second order via an effective-Hamiltonian approach. The method has been implemented into the MOLCAS-4 program system, where it will replace the single-state \{CASPT2\} program. The accuracy of the method is illustrated through calculations of the ionic-neutral avoided crossing in the potential curves for LiF and of the valence-Rydberg mixing in the V-state of the ethylene molecule. },
Author = {James Finley and Per-{\AA}ke Malmqvist and Bj{\"o}rn O. Roos and Luis Serrano-Andr{\'e}s},
Date-Added = {2020-09-07 10:11:08 +0200},
Date-Modified = {2020-09-07 10:11:14 +0200},
Doi = {https://doi.org/10.1016/S0009-2614(98)00252-8},
Issn = {0009-2614},
Journal = {Chem. Phys. Lett.},
Number = {2--4},
Pages = {299--306},
Title = {The Multi-State CASPT2 Method},
Url = {http://www.sciencedirect.com/science/article/pii/S0009261498002528},
Volume = {288},
Year = {1998},
Bdsk-Url-1 = {http://www.sciencedirect.com/science/article/pii/S0009261498002528},
Bdsk-Url-2 = {https://doi.org/10.1016/S0009-2614(98)00252-8}}
@article{molpro,
Abstract = {Abstract Molpro (available at http://www.molpro.net) is a general-purpose quantum chemical program. The original focus was on high-accuracy wave function calculations for small molecules, but using local approximations combined with explicit correlation treatments, highly accurate coupled-cluster calculations are now possible for molecules with up to approximately 100 atoms. Recently, multireference correlation treatments were also made applicable to larger molecules. Furthermore, an efficient implementation of density functional theory is available. {\copyright} 2011 John Wiley \& Sons, Ltd. This article is categorized under: Software > Quantum Chemistry},
Author = {Werner, Hans-Joachim and Knowles, Peter J. and Knizia, Gerald and Manby, Frederick R. and Sch{\"u}tz, Martin},
Date-Added = {2020-09-07 10:09:43 +0200},
Date-Modified = {2020-09-07 10:09:43 +0200},
Doi = {10.1002/wcms.82},
Eprint = {https://onlinelibrary.wiley.com/doi/pdf/10.1002/wcms.82},
Journal = {Wiley Interdisciplinary Reviews: Computational Molecular Science},
Number = {2},
Pages = {242-253},
Title = {Molpro: a general-purpose quantum chemistry program package},
Url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/wcms.82},
Volume = {2},
Year = {2011},
Bdsk-Url-1 = {https://onlinelibrary.wiley.com/doi/abs/10.1002/wcms.82},
Bdsk-Url-2 = {https://doi.org/10.1002/wcms.82}}
@article{Goerigk_2010a,
Author = {Goerigk, L. and Grimme, S.},
Date-Added = {2020-09-07 09:29:41 +0200},

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Manuscript/QUEST_WIREs.tex
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@ -74,13 +74,13 @@
\maketitle
\begin{abstract}
We describe our efforts of the last few years to create a mega set of more than \alert{470} highly-accurate vertical excitation energies of various natures ($\pi \to \pis$, $n \to \pis$, double excitation, Rydberg, singlet, doublet, triplet, etc) for small- and medium-sized molecules.
We describe our efforts of the past few years to create a mega set of more than \alert{470} highly-accurate vertical excitation energies of various natures ($\pi \to \pis$, $n \to \pis$, double excitation, Rydberg, singlet, doublet, triplet, etc) for small- and medium-sized molecules.
These values have been obtained using a combination of high-order coupled cluster and selected configuration interaction calculations using increasingly large diffuse basis sets.
One of the key aspect of the so-called QUEST dataset of vertical excitations is that it does not rely on any experimental values, avoiding potential biases inherently linked to experiments and facilitating in the process theoretical comparisons for a given basis set.
Following this composite protocol, we have been able to produce theoretical best estimate (TBEs) at the aug-cc-pVTZ level and near the complete basis set limit for each of these transitions.
These TBEs have been employed to benchmark a large number of wave function methods such as CIS(D), ADC(2), STEOM-CCSD, EOM-CCSD, CCSDR(3), CCSDT-3, ADC(3), CC3, CASPT2, NEVPT2, and others.
In order to gather the huge number of data produced during the QUEST project, we have created a website where one can easily test and 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 state, the size of the basis set, and many others.
We hope that the present review will provide a useful summary of our work so far.
One of the key aspect of the so-called QUEST dataset of vertical excitations 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.
Following this composite protocol, we have been able to produce theoretical best estimate (TBEs) with the aug-cc-pVTZ basis set, as well as basis set corrected TBEs (i.e., near the complete basis set limit) for each of these transitions.
These TBEs have been employed to benchmark a large number of (lower-order) wave function methods such as CIS(D), ADC(2), STEOM-CCSD, EOM-CCSD, CCSDR(3), CCSDT-3, ADC(3), CC3, CASPT2, NEVPT2, and others.
In order to gather the huge number of data produced during the QUEST project, we have created a website where one can easily test and 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.
We hope that the present review will provide a useful summary of our work so far and foster new developments around excited-state methods.
% Please include a maximum of seven keywords
\keywords{Excited states, full configuration interaction, excitation energies}
\end{abstract}
@ -93,57 +93,58 @@ We hope that the present review will provide a useful summary of our work so far
Nowadays, there exists a very large number of electronic structure computational approaches, more or less expensive depending on their overall accuracy, able to quantitatively predict the absolute and/or relative energies of electronic states in molecular systems \cite{JensenBook}.
One important aspect of some of these theoretical methods is their ability to access the energies of electronic excited states, i.e., states that have higher total energies than the so-called ground state (that is, the lowest-energy state).
The faithful description of excited states is particularly challenging from a theoretical point of view \cite{Gonzales_2012,Ghosh_2018,Loos_2020a} and is key to a deeper understanding of photochemical and photophysical processes like absorption, fluorescence, or even chemoluminescence \cite{Bernardi_1996,Olivucci_2010,Robb_2007,Navizet_2011}.
For a given level of theory, ground-state methods are usually more accurate than their excited-state analog.
For a given level of theory, ground-state methods are usually more accurate than their excited-state analogs.
The reasons behind this are (at least) twofold: i) one might lack a proper variational principle for excited-state energies, and ii) excited states are often very close in energy from each other but they can have very different natures ($\pi \to \pis$, $n \to \pis$, charge transfer, double excitation, valence, Rydberg, singlet, doublet, triplet, etc).
Designing excited-state methods which can tackle on the same footing all these types of excited states at an affordable cost remain an open challenge in theoretical computational chemistry \cite{Gonzales_2012,Ghosh_2018,Loos_2020a}.
When one designs a new theoretical model, the first feature that one might want to test is its overall accuracy, i.e., its ability to reproduce reference (or benchmark) values for a given system in a well-defined setup (same geometry, same basis set, etc).
These values can be absolute or relative energies, geometrical parameters, physical or chemical properties, etc, extracted from experiments, high-level theoretical calculations, or a combination of both.
To do so, the electronic structure community has designed along the years benchmark sets, i.e., sets of molecules for which one could (very) accurately computed theoretical estimates and/or access solid experimental data for given properties.
When one designs a new theoretical model, the first feature that one might want to test is its overall accuracy, i.e., its ability to reproduce reference (or benchmark) values for a given system with well-defined setup (same geometry, basis set, etc).
These values can be absolute or relative energies, geometrical parameters, physical or chemical properties, extracted from experiments, high-level theoretical calculations, or a combination of both.
To do so, the electronic structure community has designed along the years benchmark sets, i.e., sets of molecules for which one could (very) accurately compute theoretical estimates and/or access solid experimental data for given properties.
Regarding ground-states properties, two of the oldest and most employed sets are probably the Gaussian-1 and Gaussian-2 benchmark sets \cite{Pople_1989,Curtiss_1991,Curtiss_1997} developed by the group of Pople in the 1990's which gathers atomization energies, ionization energies, electron affinities, proton affinities, bond dissociation energies, and reaction barriers.
Another very useful set for the design of methods able to catch dispersion effects is the S22 benchmark set \cite{Jureka_2006} (and its extended S66 version \cite{Rezac_2011}) of Hobza and collaborators which provides benchmark interaction energies for weakly-interacting (non covalent) systems.
One could also mentioned the $GW$100 set \cite{vanSetten_2015,Krause_2015,Maggio_2016} (and its $GW$5000 extension \cite{Stuke_2020}) of ionization energies which has helped enormously the community to settle on the implementation of $GW$-type methods for molecular systems \cite{vanSetten_2013,Bruneval_2016,Caruso_2016,Govoni_2018}.
The extrapolated ab initio thermochemistry (HEAT) designed to achieve high accuracy for enthalpies of formation of atoms and small molecules (without experimental data) is another successful example of benchmak set \cite{Tajti_2004,Bomble_2006,Harding_2008}.
The extrapolated ab initio thermochemistry (HEAT) set designed to achieve high accuracy for enthalpies of formation of atoms and small molecules (without experimental data) is yet another successful example of benchmark set \cite{Tajti_2004,Bomble_2006,Harding_2008}.
More recently, the benchmark datasets provided by the \textit{Simons Collaboration on the Many-Electron Problem} have been extremely valuable to the community by providing, for example, highly-accurate ground state energies for hydrogen chains \cite{Motta_2017} and transition metal atoms and their ions and monoxides \cite{Williams_2020}.
Let us also mention the set of Zhao and Truhlar for small transition metal complexes \cite{Zhao_2006}, and the Gagliardi-Truhlar set \cite{Hoyer_2016} employed to compare the accuracy of multiconfiguration pair-density functional theory against the well-established CASPT2 method \cite{Andersson_1990,Andersson_1992,Roos,Roos_1996}.
Let us also mention the set of Zhao and Truhlar for small transition metal complexes employed to compare the accuracy density-functional methods for $3d$ transition-metal chemistry \cite{Zhao_2006}.
The examples presented above are all designed for ground-state properties, and there exists now specific protocols designed to accurately model excited-state energies and properties.
Benchmark datasets of excited-state energies and/or properties are less numerous than their ground-state counterparts but their number have been growing at a consistent pace in the last few years.
Benchmark datasets of excited-state energies and/or properties are less numerous than their ground-state counterparts but their number have been growing at a consistent pace in the past few years.
Below, we provide a short description of some of these.
One the most characteristic example is the benchmark set of vertical excitations proposed by Thiel and coworkers \cite{Schreiber_2008,Silva-Junior_2008,Silva-Junior_2010,Silva-Junior_2010b,Silva-Junior_2010c}.
The so-called Thiel (or M\"ulheim) set of excitation energies gathers a large number of excitation energies determined in 28 medium-size organic molecules with a total of 223 valence excited states (152 singlet and 71 triplet states) for which theoretical best estimates (TBEs) were defined.
In their first study, Thiel and collaborators performed CC2, CCSD, CC3, and CASPT2 calculations (with the TZVP basis) on MP2/6-31G(d) geometries in order to provide (based on additional high-quality literature data) TBEs for these transitions \cite{Silva-Junior_2010b}.
In their first study, Thiel and collaborators performed CC2 \cite{Christiansen_1995a,Hattig_2000}, CCSD \cite{Purvis_1982}, CC3 \cite{Christiansen_1995b,Koch_1997}, and CASPT2 \cite{Andersson_1990,Andersson_1992,Roos,Roos_1996} calculations (with the TZVP basis) on MP2/6-31G(d) geometries in order to provide (based on additional high-quality literature data) TBEs for these transitions \cite{Silva-Junior_2010b}.
These TBEs were quickly refined with the larger aug-cc-pVTZ basis set, highlighting the importance of diffuse functions in the faithful description of excited states (especially for Rydberg states).
In the same spirit, it is also worth mentioning Gordon's set of vertical transitions (based on experimental values) used to benchmark the performance of TD-DFT \cite{Leang_2012}, as well as its extended version by the Goerigk and coworkers \cite{Schwabe_2017,Casanova-Paez_2019,Casanova_Paes_2020} who decided to replace the experimental reference values by CC3 excitation energies instead.
A new benchmark set of charge-transfer excited states was recently introduced by Szalay and coworkers based on coupled cluster methods \cite{Kozma_2020}.
In the same spirit, it is also worth mentioning Gordon's set of vertical transitions (based on experimental values) used to benchmark the performance of time-dependent density-functional theory (TD-DFT) \cite{Leang_2012}, as well as its extended version by Goerigk and coworkers \cite{Schwabe_2017,Casanova-Paez_2019,Casanova_Paes_2020} who decided to replace the experimental reference values by CC3 excitation energies instead.
Let us also mention the new benchmark set of charge-transfer excited states recently introduced by Szalay and coworkers [based on coupled cluster (CC) methods] \cite{Kozma_2020} as well as the Gagliardi-Truhlar set \cite{Hoyer_2016} employed to compare the accuracy of multiconfiguration pair-density functional theory \cite{Ghosh_2018} against the well-established CASPT2 method.
Following a similar philosophy, we have recently reported in several studies highly-accurate vertical excitations for small- and medium-sized molecules \cite{Loos_2020a,Loos_2018a,Loos_2019,Loos_2020b,Loos_2020c}.
One of the key aspect of the so-called QUEST dataset of vertical excitations which we will describe in details in the present review article is that it does not rely on any experimental values, avoiding potential biases inherently linked to experiments and facilitating in the process theoretical comparisons.
Moreover, our protocol has been designed to be as uniform as possible, which means that we use a very systematic procedure for all excited states in order to make cross-comparison as straightforward as possible.
Importantly, it allowed us to benchmark a series of popular excited-state wave function methods partially or fully accounting for double and triple excitations as well as multiconfigurational methods such as CASPT2 and NEVPT2.
Importantly, it allowed us to benchmark, in a very systematic way, a series of popular excited-state wave function methods partially or fully accounting for double and triple excitations as well as multiconfigurational methods (see below).
In the same vein, we have also produced chemically-accurate theoretical 0-0 energies \cite{Loos_2018,Loos_2019a,Loos_2019b} which can be more straightforwardly compare to experimental data \cite{Kohn_2003,Dierksen_2004,Goerigk_2010a,Send_2011a,Winter_2013,Fang_2014}.
We refer the interested reader to Ref.~\cite{Loos_2019b} where we review the generic benchmark studies devoted to adiabatic and 0-0 energies performed in the last two decades.
The QUEST dataset has the particularity to be based in a large proportion on selected configuration interaction (SCI) reference excitation energies as well as high-order CC methods such as CCSDT and CCSDTQ.
The QUEST dataset has the particularity to be based in a large proportion on selected configuration interaction (SCI) reference excitation energies as well as high-order CC methods such as CCSDT and CCSDTQ \cite{Oliphant_1991,Kucharski_1992}.
Recently, SCI methods have been a force to reckon with for the computation of highly-accurate energies in small- and medium-sized molecules as they yield near-FCI quality energies for only a fraction of the computational cost of a genuine FCI calculation \cite{Holmes_2017,Chien_2018,Loos_2018a,Li_2018,Loos_2019,Loos_2020b,Loos_2020c,Loos_2020a,Li_2020,Eriksen_2020,Loos_2020e,Yao_2020}.
Due to the fairly natural idea underlying SCI methods, the SCI family is composed by numerous members \cite{Bender_1969,Whitten_1969,Huron_1973,Abrams_2005,Bunge_2006,Bytautas_2009,Giner_2013,Caffarel_2014,Giner_2015,Garniron_2017b,Caffarel_2016a,Caffarel_2016b,Holmes_2016,Sharma_2017,Holmes_2017,Chien_2018,Scemama_2018,Scemama_2018b,Garniron_2018,Evangelista_2014,Schriber_2016,Schriber_2017,Liu_2016,Per_2017,Ohtsuka_2017,Zimmerman_2017,Li_2018,Ohtsuka_2017,Coe_2018,Loos_2019}.
Their fundamental philosophy consists, roughly speaking, in retaining only the most energetically relevant determinants of the FCI space following a given criterion to avoid the exponential increase of the size of the CI expansion.
Originally developed in the late 1960's by Bender and Davidson \cite{Bender_1969} as well as Whitten and Hackmeyer, \cite{Whitten_1969} new efficient SCI algorithms have resurfaced recently.
Four examples are adaptive sampling CI (ASCI) \cite{Tubman_2016,Tubman_2018,Tubman_2020}, iCI \cite{Liu_2016}, semistochastic heat-bath CI (SHCI) \cite{Holmes_2016,Holmes_2017,Sharma_2017,Li_2018}), and \textit{Configuration Interaction using a Perturbative Selection made Iteratively} (CIPSI) \cite{Huron_1973}.
These four flavors of SCI include a second-order perturbative (PT2) correction which is key to estimate the ``distance'' to the FCI solution.
Four examples are adaptive sampling CI (ASCI) \cite{Tubman_2016,Tubman_2018,Tubman_2020}, iCI \cite{Liu_2016}, semistochastic heat-bath CI (SHCI) \cite{Holmes_2016,Holmes_2017,Sharma_2017,Li_2018}), and \textit{Configuration Interaction using a Perturbative Selection made Iteratively} (CIPSI) \cite{Huron_1973,Giner_2013,Giner_2015,Garniron_2019}.
These four flavors of SCI include a second-order perturbative (PT2) correction which is key to estimate the ``distance'' to the FCI solution (see below).
The QUEST set of excitation energies relies on the CIPSI algorithm, which is, from a historical point of view, one of the oldest SCI algorithm.
It was developed in 1973 by Huron, Rancurel, and Malrieu \cite{Huron_1973} (see also Refs.~\cite{Evangelisti_1983,Cimiraglia_1985,Cimiraglia_1987,Illas_1988,Povill_1992}).
Recently, the determinant-driven CIPSI algorithm has been efficiently implemented \cite{Giner_2013,Giner_2015} in the open-source programming environment {\QP} by our group enabling to perform massively parallel computations \cite{Garniron_2017,Garniron_2018,Garniron_2019,Loos_2020e}.
CIPSI is also frequently used to provide accurate trial wave function for QMC calculations in molecules \cite{Caffarel_2014,Caffarel_2016a,Caffarel_2016b,Giner_2013,Giner_2015,Scemama_2015,Scemama_2016,Scemama_2018,Scemama_2018b,Scemama_2019,Dash_2018,Dash_2019,Scemama_2020} and more recently for periodic solids \cite{Benali_2020}.
Recently, the determinant-driven CIPSI algorithm has been efficiently implemented \cite{Garniron_2019} in the open-source programming environment {\QP} by our group enabling to perform massively parallel computations \cite{Garniron_2017,Garniron_2018,Garniron_2019,Loos_2020e}.
CIPSI is also frequently used to provide accurate trial wave functions for QMC calculations in molecules \cite{Caffarel_2014,Caffarel_2016a,Caffarel_2016b,Giner_2013,Giner_2015,Scemama_2015,Scemama_2016,Scemama_2018,Scemama_2018b,Scemama_2019,Dash_2018,Dash_2019,Scemama_2020} and more recently for periodic solids \cite{Benali_2020}.
We refer the interested reader to Ref.~\cite{Garniron_2019} where one can find all the details regarding the implementation of the CIPSI algorithm.
The present article is organized as follows.
In Sec.~\ref{sec:tools}, we detail the specificities of our protocol by providing the computational details regarding geometries, basis sets, (reference and benchmarked) computational methods, the list of Electronic structure software we have employed, and a new way of estimating rigorously the extrapolation error in SCI calculations.
We then describe in Sec.~\ref{sec:QUEST} the content of our five QUEST sub-sets providing for each of them the number of reference excitation energies, the list of benchmarked methods as well as other specificities.
In Sec.~\ref{sec:tools}, we detail the specificities of our protocol by providing the computational details regarding geometries, basis sets, (reference and benchmarked) computational methods, and a new way of estimating rigorously the extrapolation error in SCI calculations.
We then describe in Sec.~\ref{sec:QUEST} the content of our five QUEST sub-sets providing for each of them the number of reference excitation energies, the nature and size of the molecules, the list of benchmarked methods, as well as other specificities.
A special emphasis is placed on our latest add-on, QUEST\#5, specifically designed for the present manuscript where we have considered, in particular but not only, larger molecules as well as additional FCI values for five- and six-membered rings.
Section \ref{sec:TBE} discusses the generation of the TBEs, while Sec.~\ref{sec:bench} proposes a comprehensive benchmark of various methods on the entire QUEST set which is composed by more than \alert{470} excitations with, in addition, a specific analysis for each type of excited states.
Section \ref{sec:website} describe the feature of the website of the specifically designed to gather the entire data generated during these last few years.
Thanks to this website, one can easily test and 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 state, the size of the basis set, and many others.
Section \ref{sec:website} describe the feature of the website that we have specifically designed to gather the entire data generated during these last few years.
Thanks to this website, one can easily test and 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, etc.
Finally, we draw our conclusions in Sec.~\ref{sec:ccl}.
%%%%%%%%%%%%%%%%%%%%%%%%%%%%%
@ -497,7 +498,7 @@ Triazine & $^1A_1''(n \ra \pis)$ & 4.85 & 4.84 & 4.769(132) \\
Because computing 450 excitation energies can be a costly exercise, we are planning on developing a ``diet set'' following the philosophy of the ``diet GMTKN55'' set \cite{Goerigk_2017} proposed recently by Gould \cite{Gould_2018b}.
Besides all the studies described above aiming at reaching chemically accurate vertical transition energies, it should be pointed out that an increasing amount of effort is currently devoted to the obtention of highly-trustable excited-state properties.
This includes, first, 0-0 energies, \cite{Die04b,Hat05c,Goerigk_2010a,Sen11b,Win13,Fan14b,Loo18b,Loo19a,Loo19b} which, as mentioned above, offer well-grounded comparisons with experiment.
This includes, first, 0-0 energies which, as mentioned above, offer well-grounded comparisons with experiment.
However, because 0-0 energies are fairly insensitive to the underlying molecular geometries, \cite{Sen11b,Win13,Loo19a} they are not a good indicator of their overall quality.
Consequently, one can find in the literature several sets of excited-state geometries obtained at various levels of theory, \cite{Pag03,Gua13,Bou13,Tun16,Bud17} some of them being determined using state-of-the-art models. \cite{Gua13,Bud17}
There are also investigations of the accuracy of the nuclear gradients at the Franck-Condon point. \cite{Taj18,Taj19}
@ -524,10 +525,11 @@ The authors have declared no conflicts of interest for this article.
\newpage
%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%
\begin{biography}[example-image-1x1]{M.~V\'eril}
Please check with the journal's author guidelines whether author biographies are required. They are usually only included for review-type articles, and typically require photos and brief biographies (up to 75 words) for each author.
\bigskip
\bigskip
\begin{biography}[MVeril]{M.~V\'eril}
was born in Toulouse in 1993.
He received his B.Sc.~in Molecular Chemistry from the Universit\'e Paul Sabatier (Toulouse, France) in 2015 and his M.Sc.~in Computational and Theoretical Chemistry and Modeling from the same university in 2018.
Since 2018, he is a Ph.D.~student in the group of Dr.~Pierre-Fran\c{c}ois Loos at the Laboratoire de Chimie et Physique Quantiques in Toulouse.
He is currently developing QUANTUM PACKAGE and the web application linked to the QUEST project.
\end{biography}
%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%
@ -565,7 +567,7 @@ Please check with the journal's author guidelines whether author biographies are
%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%
\begin{biography}[PFLoos]{P.-F.~Loos}
received his his Ph.D.~in Computational and Theoretical Chemistry from the Universit\'e Henri Poincar\'e (Nancy, France) in 2008.
received his Ph.D.~in Computational and Theoretical Chemistry from the Universit\'e Henri Poincar\'e (Nancy, France) in 2008.
From 2009 to 2013, He was undertaking postdoctoral research with Peter M.W.~Gill at the Australian National University (ANU).
From 2013 to 2017, he was a \textit{``Discovery Early Career Researcher Award''} recipient and, then, a senior lecturer at the ANU.
Since 2017, he holds a researcher position from the \textit{``Centre National de la Recherche Scientifique (CNRS)} at the \textit{Laboratoire de Chimie et Physique Quantiques} in Toulouse (France), and was awarded, in 2019, an ERC consolidator grant for the development of new excited-state methodologies.