122 lines
6.9 KiB
TeX
122 lines
6.9 KiB
TeX
\documentclass[11pt]{letter}
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\usepackage{UPS_letterhead,color,mhchem,mathpazo,ragged2e,bm}
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\newcommand{\alert}[1]{\textcolor{red}{#1}}
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\begin{document}
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\begin{letter}%
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{To the Editors of the Journal of Physical Chemistry Letters}
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\justifying
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\opening{Dear Editors,}
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Please find attached a revised version of the manuscript entitled
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{\it "A Density-Based Basis-Set Correction For Wave Function Theory"}.
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We would to thank the reviewers for their constructive comments.
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Our detailed responses to their comments can be found below.
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For convenience, all modifications and changes are highlighted in red in the revised version of the manuscript.
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We hope that you will agree that our manuscript is now suitable for publication in JPCL.
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We look forward to hearing from you.
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\closing{Sincerely, the authors.}
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\newpage
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%%% REVIEWER 1 %%%
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\noindent \textbf{\large Authors' answer to Reviewer \#1}
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\begin{itemize}
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\item
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\textit{This manuscript reports a major advance in electronic structure theory, by providing a cheap and mathematically motivated correction for finite basis size effects in high-level theories.
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I expect it to have immediate applications among users, certainly once user friendly code is released.
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The work is definitely worthy of being published in JPCL, after changes.
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That said, for the reasons explained below, I think the current manuscript requires changes somewhere between major and minor.}
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\\
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\alert{We thank the reviewer for his/her support.
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We also believe that the present contribution is a major advance in electronic structure theory.}
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\item
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\textit{My main issue with the manuscript is that it is not sufficiently well self-contained or explained.
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Being familiar with previous work on the topic, I was mostly able to follow the manuscript without hassle.
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Someone without familiarity would struggle.
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For example, the authors refer several times to work in the Appendix of a previous paper.
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The gist of such results should (IMO) be summarised here.}
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\\
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\alert{The main results of the previous paper (Ref.~[41]) has already been summarized in the present manuscript.
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We strongly believe that adding more technical details would not improve the readability of the present paper, especially for the wide audience of a journal like JPCL.
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In the present manuscript, we point out clearly the key equations of Ref.~[41] and we refer the reader to this reference for further details.
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Note that this is the only point where we disagree with the reviewer.}
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\item
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\textit{This readability issue is not made easier by the authors' commendable focus on generality, which leaves the reader carrying a lot of variables and ideas in their head.
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Fine for a long paper, not so much for a Letter.
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My first suggestion to the authors would be to change from describing things in terms of a generic method "Y" to using a specific case [e.g. CCSD(T)] and then generalizing only at the end, e.g., "Of course, the above holds true for any method that provides a good approximation to the energy, not just CCSD(T).".
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Other changes along these lines would probably also be useful.
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This would help the reader cement the key concept (basis correction) without worrying about quite so many variables.}
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\\
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\alert{Thank you for pointing that out.
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We have made the manuscript more explicit.
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In particular, as proposed by the reviewer, we have explicitly specified the methods "Y" and "Z" that we have employed throughout the manuscript.
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We believe that it has significantly improved the readability of the present manuscript.
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We thank the reviewer for this advice.}
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\item
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\textit{On a related note, I do not see the benefit of reporting the LDA correction in the main text, although for sure it belongs in the SI.
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There seems to be no practical reason to do LDA when it just as expensive (??) as GGA, but gives worse results.
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This would have the added advantage of reducing discussion on outcomes.
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I kind of understand why the authors report LDA, but think it is a distraction since they have PBE.}
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\\
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\alert{It is true that the LDA and PBE corrections have similar computational cost.
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Therefore, as proposed by the reviewer, we have moved the description, discussion and results associated with the LDA functional to the SI.
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The manuscript is now more compact and space has been freed to include the new figure requested by the reviewer (see below).}
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\item
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\textit{What I think would be very useful is to show $\mu(\bm{r})$ for an example, e.g. along the bond in an interesting diatom.
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This would illustrate the range of values taken by $\mu$, and the advantage of doing things point-by-point.
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If values for multiple basis sets were reported it might also help in understanding how and where larger basis sets help, which might point to how to improve basis sets in a more systematic fashion.
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Removing the discussion on LDA would probably free enough space to show this, especially if Figure 2 was condensed into a single figure (which should be feasible sans LDA).}
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\\
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\alert{This is an excellent suggestion.
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We have reported a figure showing $\mu(\bm{r})$ and the associated energetic correction for \ce{N2} in various basis sets.
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A short discussion has also been included.}
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\item
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\textit{One final (minor) key point is that the proposed use of density fitting or related time-saving steps seems rather ambitious, given that it necessarily introduces a further basis set dependence.
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I would suggest the authors do not mention the last sentence in the relevant paragraph, or give more detail if it is included.}
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\\
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\alert{Following the reviewer's advice, we have removed our comment on density-fitting and related methods.}
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\item
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\textit{Regardless of my issues with presentation, this is important work which should definitely be published in JPCL.
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It just first needs to be made a bit easier to follow.}
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\\
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\alert{We would like to thank the reviewer for these supportive comments.}
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\end{itemize}
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\newpage
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%%% REVIEWER 2 %%%
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\noindent \textbf{\large Authors' answer to Reviewer \#2}
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\textit{This is an excellent paper on density-based basis-set corrections for accelerating the basis-set convergence of an arbitrary wavefunction method.
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The corrections are examined for the atomization and correlation energies of the G2 set of molecules.
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In wavefunction theory, F12 methods have been developed in the 2000s.
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The approach described in this paper provides a fast alternative to F12 that requires relatively large auxiliary basis functions for computing three- and four-electron integrals.
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As a small notice, I suggest the the following for an update of reviews on F12, Grueneis et al., J. Chem. Phys., 146, 080901 (2017), Ma and Werner, WIREs Comput. Mol. Sci., 8:e1371 (2018).
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To summarize, I think this is an excellent paper that should be published in JPCL basically in the present form.}
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\alert{We would like to thank the reviewer for his/her kind comments.
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We have added the two references suggested by the reviewer in due place.}
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\end{letter}
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\end{document}
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