From c3a47a403b6e6f4ced1d77ca19406eeddd2904dc Mon Sep 17 00:00:00 2001 From: pfloos Date: Fri, 27 May 2022 12:32:50 +0200 Subject: [PATCH] creating response letter --- Manuscript/CASPT3.tex | 2 +- Response_Letter/CNRS_logo.pdf | Bin 0 -> 180517 bytes Response_Letter/Response_Letter.tex | 117 ++++++++++++++++++++++++++++ Response_Letter/UPS_letterhead.sty | 70 +++++++++++++++++ Response_Letter/UPS_logo.pdf | Bin 0 -> 235750 bytes 5 files changed, 188 insertions(+), 1 deletion(-) create mode 100644 Response_Letter/CNRS_logo.pdf create mode 100644 Response_Letter/Response_Letter.tex create mode 100644 Response_Letter/UPS_letterhead.sty create mode 100644 Response_Letter/UPS_logo.pdf diff --git a/Manuscript/CASPT3.tex b/Manuscript/CASPT3.tex index 9ed45cd..e7d8b0e 100644 --- a/Manuscript/CASPT3.tex +++ b/Manuscript/CASPT3.tex @@ -585,7 +585,7 @@ This state was computed using a reference CASSCF wave function averaged over fou (The $3p_x$ orbitals were included to recover part of the radial correlation.) However, this strategy leads to a valence-Rydberg mixing due to the fact that the dynamic correlation is not sufficiently described at the CASSCF level. The ionic $B_{1u}(\pi,\pis)$ state lies \SI{9.65}{\eV} vertically above the ground state, while the Rydberg $B_{1u}(\pi,3p_x)$ state is \SI{0.2}{\eV} below at the CASSCF level. -For this reason, the two states are mixed and both CASPT2 and CASPT3 fails to predict accurate transition energies for the ionic state. +For this reason, the two states are mixed and both CASPT2 and CASPT3 fail to predict accurate transition energies for the ionic state. The Rydberg character of the ionic $B_{1u}(\pi,\pis)$ state is evident from the inspection of the CASSCF wave function and also from its value of $\expval*{x^2}$, which measures the spatial extent of the wave function out of the molecular plane (hence characteristic of the size of the $\pi$ orbitals in the considered state). The $\expval*{x^2}$ value is \SI{31.9}{\bohr^2} for the ionic $B_{1u}(\pi,\pis)$ state and \SI{51.1}{\bohr^2} for the $B_{1u}(\pi,3p_x)$ Rydberg state, while it is only \SI{26.6}{\bohr^2} for the ground state. diff --git a/Response_Letter/CNRS_logo.pdf b/Response_Letter/CNRS_logo.pdf new file mode 100644 index 0000000000000000000000000000000000000000..954b3f7efed5390fb7fe42a914adf6dccfdf6642 GIT binary patch literal 180517 zcmZs?dpy(s`#-+TWDyb}(iS11Dd)r}ht8BDktt^qA&Ts|5jrS}k{qTIot;U=CY7_v zAtXi#)nts>?78RjH@yy@*ZX_>{j=xx-1azJ*Y&ur`*pvrr>2vwz5bTXhLW1^zR!OD zRm92feD^`p2xou`JsBjqeLD`n&-b){WB|@sbn6ffZy$In(l=amJ#`||*VflN)W;WR zWhEIA8SZ-`MDiR`_b}%0#>1VmyY%-Q(BG)DzwO}07PO?YigMOQWyJcN8#zz&r?Y|| zjog&&k;5Qfe302M>3iDe@4t)QEzP<#)t~FurSF#BZT-)B4xbP6#o?V!`2Tqg_dOkn zGyH39hkPSK&xU*ZM&L~Ty0J6#bfoC}2;9l1ilN9Z}6yMgG&7K5!ue_oDD z;tvO$4LON3|MN4^cK)7rX_$Y+;1nL}?d%(ga~I8RYmdY44iT+j$KThTe_wawj^pr0 z9Zv@NdPm}xgtt3n3(oZKQJ3WO_rOcH{u%gh`I`Ot75=Z?{WApK`RvKaKl}YN9S-jr 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Physics,} + +\opening{Dear Editors,} + +\justifying +Please find attached a revised version of the manuscript entitled +\begin{quote} + \textit{``Benchmarking CASPT3 Vertical Excitation Energies ''}. +\end{quote} +We thank the reviewers for their constructive comments and to support publication of the present manuscript. +Our detailed responses to their comments can be found below. +For convenience, changes are highlighted in red in the revised version of the manuscript. + +We look forward to hearing from you. + +\closing{Sincerely, the authors.} + +\newpage + +%%% REVIEWER 1 %%% +\noindent \textbf{\large Authors' answer to Reviewer \#1} + +{Finally, some benchmarking on the CASPT3 method. +This should have been done long ago -- the authors are kicking in an open door. +A few things need to be modified -- minor -- for the paper to be accepted. +} +\\ +\alert{ +} + +\begin{enumerate} + +\item +{Table I should be moved to the SI. Key entries could be kept if explicitly discussed in the manuscript.} +\\ +\alert{ +} + +\item +{It should be stressed that the conclusions are only valid for medium-sized organic molecules. +The very important classes of transition metal complexes are not covered.} +\\ +\alert{ +} + +\item +{Make it VERY clear that the excitation energies are Single-State CASPTX excitation energies.} +\\ +\alert{ +} + +\item +{The authors should point out the difference between dynamic sigma polarization and so-called left-right polarization (https://doi.org/10.1021/jp9528020).} +\\ +\alert{ +} + +\end{enumerate} + +%%% REVIEWER 2 %%% +\noindent \textbf{\large Authors' answer to Reviewer \#2} + +{This is an interesting paper that shows a benchmark of CASPT3 energies using small organic molecules. +Such studies are important and suitable for JCP, so in principle I am in favor of it. +I have however some comments that I would like the authors consider. +} +\\ +\alert{ +} + +\begin{enumerate} + +\item +{One straightforward request is that I would have liked to see also a histogram in fig 2 of the CASSCF values of Table 1. +CASSCF has largest errors, sure, but it would be interesting to see how broad is the distribution in comparison to caspt3, represented in the same way.} +\\ +\alert{ +} + +\item +{My other, not so straightforward, comment refers to the IPEA correction. +It is a valuable and welcome conclusion that the authors found that CASTP3 is less sensitive to IPEA. +Still, in saying that CASPT3 is like CASPT2(NOIPEA) the paper seems to advocate that one should use IPEA in CASPT2. +The first thing that authors should do is to point out that the IPEA shift is differently implemented in MOLPRO (used in this paper) than in MOLCAS (used in ref 56 which recommends not to use IPEA for the same type of organic molecules) and therefore, this apparent conclusion should be taken with caution. +Second, this conclusion relies on the chosen theoretical best estimates (TBE). +The TBEs (for molecules of the Thiel set, \url{https://lcpq.github.io/QUESTDB_website/subsets/}, QUEST3 subset) seems to be largely CC3, CCSDT, CCSDTQ, and NEVPT2 with aug-TZ/QZ basis sets. +From a theoretical point of view, this should give an impressive accuracy, as they are high-order wave function based methods and large basis sets. +And indeed, CASPT2/IPEA performs similar to CCSD/CC3/NEVPT2 excitation energies for the Thiel set. +However, all these methods (CCSD/CC3/NEVPT2/IPEA) using the TZVP basis set overestimate experimental excitation energies, while NOIPEA underestimates excitation energies of the Thiel set, and this underestimation with the TZVP basis set was smaller in magnitude than the overestimation of the other methods, making NOIPEA with TZVP basis set preferable. +The question is, does one want to be as good as CASPT2 or as good as the experimental value? +I would say the latter, so while the TBEs are useful, a comparison with the experimental values should be provided and the results also discussed in this light.} +\\ +\alert{ +} + +\item +{Can the authors also discuss if there is any basis set effect? Are the TBEs obtained with the same basis set as their calculations? +Probably not. +The authors could be more a bit more specific about the method/basis set of each of the TBEs in the SI, so that everyone can compare for a specific molecule (if desired) the setups in which the values where obtained. +Again, this should be discussed against the experimental value in order to convey a clear recommendation to the readers.} +\\ +\alert{ +} + +\end{enumerate} + +\end{letter} +\end{document} diff --git a/Response_Letter/UPS_letterhead.sty b/Response_Letter/UPS_letterhead.sty new file mode 100644 index 0000000..2e5f5bb --- /dev/null +++ b/Response_Letter/UPS_letterhead.sty @@ -0,0 +1,70 @@ +%ANU etterhead Yves +%version 1.0 12/06/08 +%need to be improved + + +\RequirePackage{graphicx} + +%%%%%%%%%%%%%%%%%%%%% DEFINE USER-SPECIFIC MACROS BELOW %%%%%%%%%%%%%%%%%%%%% +\def\Who {Pierre-Fran\c{c}ois Loos} +\def\What {Dr} +\def\Where {Universit\'e Paul Sabatier} +\def\Address {Laboratoire de Chimie et Physique Quantiques} +\def\CityZip {Toulouse, France} +\def\Email {loos@irsamc.ups-tlse.fr} +\def\TEL {+33 5 61 55 73 39} +\def\URL {} % NOTE: use $\sim$ for tilde + +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% MARGINS %%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% +\textwidth 6in +\textheight 9.25in +\oddsidemargin 0.25in +\evensidemargin 0.25in +\topmargin -1.50in +\longindentation 0.50\textwidth +\parindent 5ex + +%%%%%%%%%%%%%%%%%%%%%%%%%%% ADDRESS MACRO BELOW %%%%%%%%%%%%%%%%%%%%%%%%%%%%% + +\address{ + \includegraphics[height=0.7in]{CNRS_logo.pdf} \hspace*{\fill}\includegraphics[height=0.7in]{UPS_logo.pdf} + \\ + \hrulefill + \\ + {\small \What~\Who\hspace*{\fill} Telephone:\ \TEL + \\ + \Where\hspace*{\fill} Email:\ \Email + \\ + \Address\hspace*{\fill} + \\ + \CityZip\hspace*{\fill} \URL} + } + +%%%%%%%%%%%%%%%%%%%%%%%%%%%% OTHER MACROS BELOW %%%%%%%%%%%%%%%%%%%%%%%%%%%%% +%\signature{\What~\Who} + +\def\opening#1{\ifx\@empty\fromaddress + \thispagestyle{firstpage} + 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