diff --git a/Revision/cnrs.png b/Revision/cnrs.png new file mode 100644 index 0000000..f568727 Binary files /dev/null and b/Revision/cnrs.png differ diff --git a/Revision/cnrslet.cls b/Revision/cnrslet.cls new file mode 100644 index 0000000..191de89 --- /dev/null +++ b/Revision/cnrslet.cls @@ -0,0 +1,240 @@ +% chulet.cls -- A Cambridge University Letterhead class for LaTeX +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% +% Simon's Lab Letter Class for 2001 +% Modified by Robert Whittaker for use in DAMTP +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% +% Simon Moore, University of Cambridge, Computer Laboratory +% Please use freely (it's just a hack!) +% Source from: http://www.cl.cam.ac.uk/~swm11/letters/index.html +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% +% +% Class Options: +% usebwarms - uses a black and white version of the Univ. arms +% usecmfont - uses computer modern font rather than Sabon (works +% better with xdvi +% usetimesfont - uses times font rather than Sabon +% +% e.g.: +% \documentclass[usecmfont,usebwarms,usetimesfont]{/homes/swm11/texmacros/letters/lablet2001} +% +% Compulsory commands: +% \fromwhome{title}{your name}{qualifications}{job-title}{email}{phone}{fax} +% \towhom{to name}{to address} +% \begin{letter}[salutation name] +% \end{letter} +% +% The 'to name' is used in address, the optional 'salutation name' is +% used in 'Dear ... ,'. In its absence, 'to name' is used there instead. +% +% Extra commands: +% \lettertitle{title of letter} +% \setdate{date string} +% \setsigned{greeting}{signature} +% \setsalutation{salutation} +% \cclist{list of people\\to cc the\\message to} +% \enclosures{list of enclosures} +% \reference{reference string} + +\ProvidesClass{cnrslet}[2013/07/14] + +\typeout{Univeristy of Cambridge Dept of Chemistry letter class by Alex Thom} +\typeout{Adapted from Churchill College Letter class by Alex Thom} +\typeout{Adapted from DAMTP Letter class by Robert Whittaker} +\typeout{Adapted from Simon Moore's Computer Lab Letter Class} +%\usepackage{showframe} +%\usepackage{layout} +%\usepackage{sabon} % Univ. font is Sabon! +\renewcommand{\ttdefault}{cmtt} % but don't use courier for typewriter +%I'm not sure this has any effect with the sabon package we have in DAMTP + +\usepackage{color} +\usepackage{graphicx} +\usepackage{fancyhdr} +\usepackage{marvosym} +\usepackage{scrextend} +%\usepackage{tweaklist} + +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% +% A few new options (rest are passed through to article class). + + + +\DeclareOption{usebwarms}{\AtBeginDocument{\bwarms}} +\DeclareOption{usetimesfont}{\typeout{Replacing Sabon with Times} + \AtEndOfClass{\usepackage{times}}} +\DeclareOption*{\PassOptionsToClass{\CurrentOption}{article}} + +\ProcessOptions\relax + +\LoadClass[10.75pt,a4paper]{article} + +% page layout +%\pagestyle{plain} +\setlength{\oddsidemargin}{0mm} +\setlength{\evensidemargin}{0mm} +\setlength{\topmargin}{-16mm} +\setlength{\textwidth}{16cm} +\setlength{\textheight}{220mm} +\setlength{\headheight}{25mm} +\setlength{\footskip}{20mm} + +\parskip 10pt +\parindent 0.0pt + +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% +% main content commands +\newcommand{\fromtitle}{your title?} +\newcommand{\fromnamedetails}{Use $\backslash$from to speficfy your name, +position, email, phone, fax} +\newcommand{\fromquoldetails}{your qualifications?} +\newcommand{\fromjobdetails}{your position?} +\newcommand{\fromemaildetails}{email?} +\newcommand{\fromphonedetails}{phone?} +\newcommand{\fromfaxdetails}{fax?} +\newcommand{\fromwhom}[7]{ + \renewcommand{\fromtitle}{#1} + \renewcommand{\fromnamedetails}{#2} + \renewcommand{\fromquoldetails}{#3} + \renewcommand{\fromjobdetails}{#4} + \renewcommand{\fromemaildetails}{#5} + \renewcommand{\fromphonedetails}{#6} + \renewcommand{\fromfaxdetails}{#7} + } + +\newcommand{\towhomaddress}{Use $\backslash$towhom to set the name +and address} +\newcommand{\towhomname}{Name?} +\newcommand{\towhom}[2]{ + \renewcommand{\towhomname}{#1} + \renewcommand{\towhomaddress}{#2} +} + +\newcommand{\salutationname}{Name of recipient} + +\newcommand{\referencedetails}{\null} +\newcommand{\reference}[1]{\renewcommand{\referencedetails}{#1}} + +\newcommand{\datedetails}{\today} +\newcommand{\setdate}[1]{\renewcommand{\datedetails}{#1}} + +\newcommand{\salutation}{Dear} +\newcommand{\setsalutation}[1]{\renewcommand{\salutation}{#1}} + +\newcommand{\yoursdetails}{Yours sincerely,} +\newcommand{\signeddetails}{\fromnamedetails} + +\newcommand{\setsigned}[2]{\renewcommand{\yoursdetails}{#1}\renewcommand{\signeddetails}{#2}} + +\newcommand{\encldetails}{} +\newcommand{\enclosures}[1]{\renewcommand{\encldetails}{\vspace*{10em}\textbf{Encl}:~~\begin{minipage}[t]{100mm}#1\end{minipage}}} + +\newcommand{\cclistdetails}{} +\newcommand{\cclist}[1]{\renewcommand{\cclistdetails}{\vspace*{1em}cc:~~\begin{minipage}[t]{100mm}#1\end{minipage}}} + +\newcommand{\cuarms}{\includegraphics[width=30mm]{cnrs}} %65mm from UC style guidelines v5 +%\newcommand{\bwarms}{\typeout{Using B&W version of the arms}\renewcommand{\cuarms}{\includegraphics{BWUni3}}} +%\newcommand{\cuarms}{\includegraphics{CUni3}} +%\newcommand{\bwarms}{\typeout{Using B&W version of the arms}\renewcommand{\cuarms}{\includegraphics{BWUni3}}} + +\newcommand{\dostamp}{} +\newcommand{\stamp}[1]{\renewcommand{\dostamp}{#1}} + +\newcommand{\DeptHead}{\fontsize{14pt}{14pt}} + +\renewcommand{\headrulewidth}{0pt} +\newcommand{\lettertitle}[1]{\begin{center}\bf#1\end{center}} +\fancypagestyle{firststyle} +{ +\fancyhf[HL]{% +\setlength{\unitlength}{1mm}% +\begin{picture}(70,0)(0,0) +\put(-13,-1){\makebox(66,20)[tl]{\cuarms}}%14mm from top and 12mm from left +\put(1,-1){\makebox(52,5)[tl]{\DeptHead}} +\end{picture}} +\fancyhf[HR]{% +\begin{flushright}{\bf\fromtitle~\fromnamedetails~\fromquoldetails}\\{\it\fromjobdetails}\end{flushright}} +%\fancyhf[FR]{\vspace{-35mm}\swmfoot} +} +\pagestyle{fancyplain} + + + +\newcommand{\dolettertop}{% +\thispagestyle{firststyle}% +\begin{flushright} +\swmfoot +\end{flushright} +\makeatletter +\ifx\towhomname\@empty +\setlength{\unitlength}{1mm} +%\begin{picture}(160,80)(0,0) +\begin{picture}(190,35)(0,0) +%\put(95,60){\makebox(75,25)[tl]{\parbox{75mm}{\begin{flushright}{\bf\fromtitle~\fromnamedetails~\fromquoldetails}\\{\it\fromjobdetails}\\\fromphonedetails\\\fromemaildetails\end{flushright}} +%}} +\put(0,10){\makebox(100,25)[tl]{\begin{tabular}{@{}p{90mm}@{}}\towhomname\\\towhomaddress\end{tabular}}} +\put(0,40){\makebox(160,00)[tr]{\dostamp}} +\end{picture} +\else +\fi +\hfill\referencedetails \\ +\datedetails + +\salutation\ \salutationname,\\ +%\enlargethispage{-25mm}% +%\begin{figure}[b!]\swmfoot\end{figure} +\makeatother +} + + +\renewcommand{\footnoterule}{} +\renewcommand{\thefootnote}{} + +\newcommand{\swmfoot}{\fontsize{9pt}{10pt}\rm\hfill\begin{tabular}{@{}r@{~~}r@{ }r@{}} + & & \\ +\multicolumn{2}{@{}r@{}}{Centre National de la Recherche Scientifique}\\ +\multicolumn{2}{@{}r@{}}{Universit\'e Toulouse III, Paul Sabatier}\\ +\multicolumn{2}{@{}r@{}}{Bat.~3R1b4, 118 route de Narbonne}\\ +\multicolumn{2}{@{}r@{}}{31062 Toulouse Cedex 09}\\ +\multicolumn{2}{@{}r@{}}{France}\\ + & \\ + & \fromphonedetails\\ + & \fromemaildetails\\ +\end{tabular} +} + + +\newcommand{\doletterbottom}{ +{ +%\centering +\begin{addmargin}[3em]{0em} +\yoursdetails + +%\hspace{-2.5em}\includegraphics[scale=0.3, trim={0cm 1cm 0cm 0cm}, clip]{HGAB} + + +\signeddetails + +\encldetails + +\cclistdetails +\end{addmargin} + +} +\cleardoublepage} + +\newenvironment{letter}[1] + {\renewcommand{\salutationname}{#1}% + \dolettertop} + {\doletterbottom} + +\def\opening#1{\ifx\@empty\fromaddress + \thispagestyle{firstpage} + \hspace*{\longindendation}\today\par + \else \thispagestyle{empty} + {\centering\fromaddress \vspace{5\parskip} \\ +\today\hspace*{\fill}\par} + \fi + \vspace{3\parskip} + {\raggedright \toname \\ \toaddress \par}\vspace{3\parskip} + \noindent #1\par\raggedright\parindent 5ex\par + } diff --git a/Revision/response_letter.tex b/Revision/response_letter.tex new file mode 100644 index 0000000..8e49012 --- /dev/null +++ b/Revision/response_letter.tex @@ -0,0 +1,178 @@ +\documentclass[10pt]{cnrslet} +\usepackage{xcolor,mhchem,mathpazo,ragged2e} +\usepackage[utf8]{inputenc} +\usepackage[T1]{fontenc} +\usepackage{txfonts} +\usepackage{url} +\newcommand{\alert}[1]{\textcolor{red}{#1}} +\usepackage[UKenglish]{datetime} + +% Formal environment +\usepackage[strict]{changepage} +\definecolor{darkblue}{rgb}{0.0, 0.0, 0.55} +\definecolor{formalshade}{rgb}{0.95,0.95,1} +\usepackage{framed} +\newcommand{\ajwt}[1]{{\color{red}{#1}}} +\newenvironment{formal}{% + \def\FrameCommand{% + {\color{darkblue}\vrule width 2pt}% + {\color{formalshade}\vrule width 4pt}% + \colorbox{formalshade}% + }% + \MakeFramed{\advance\hsize-\width\FrameRestore}% + \noindent\hspace{-4.55pt}% disable indenting first paragraph + \begin{adjustwidth}{}{7pt}% + \vspace{-4pt}% +} +{% + \vspace{4pt}\end{adjustwidth}\endMakeFramed% + \vspace{-8pt} +} + + + +% Paper specifics +\newcommand{\journal}{the Journal of Chemical Physics} +\newcommand{\papertitle}{Stochastically accelerated perturbative triples correction in coupled cluster calculations} + +\begin{document} + +\newdateformat{UKvardate}{% +\THEDAY\ \monthname[\THEMONTH], \THEYEAR} +\UKvardate\renewcommand{\headrulewidth}{0pt} + +\fromwhom{}{Anthony Scemama}{}{Laboratoire de Chimie et Physique Quantiques (UMR5626)}{scemama@irsamc.ups-tlse.fr}{+33 5 6155 7339}{} +\setsalutation{To} +\renewcommand{\yoursdetails}{Yours sincerely, the authors} + +\begin{letter}% +{the Editors of \textit{\journal}} + +%\opening{Dear Editors,} + +\vspace{-1em} +\justifying +Please find attached a manuscript entitled +\vspace{-1.25em} +\begin{center} +\textbf{\papertitle{}} +\end{center} +\vspace{-1.25em} +that we recently submitted as an \underline{Invited Article} to the \textit{\journal}. +We thank the reviewers for their constructive comments and for supporting 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. + +\end{letter} + +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% +\clearpage +{\large \bf Response to Reviewer 1:} +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% + + +In this paper, calculation of the perturbative triples correction, usually +abbreviated as (T), is considered. It is well-known that the cost of CCSD(T) +calculations for large systems is frequently dominated by the (T) component. +This is due to the $N^7$ scaling of the computational costs, higher than the $N^6$ +of the preceding CCSD iterations. Taking into account that the use of CCSD(T) +is widespread nowadays, new approaches to evaluation of the (T) corrections are +welcomed. The authors propose a novel method based on the stochastic sampling +of the triplets of virtual orbitals. The samples are drawn according to a +probability distribution (importance sampling) suggested in the manuscript +which approximately describes the importance of each triplet for the final +result. While the same triplet can be randomized several times during the Monte +Carlo procedure, a memorization algorithm is introduced to avoid unnecessary +recalculation. As a result, the stochastic algorithm has a small overhead +compared with the conventional implementation and converges to the exact result +in the limit of infinite number of samples. + +The paper is well-written, the numerical results are comprehensive and convincing and hence I recommend the paper to be published. However, I have a few minor suggestions which the authors may consider and revise their paper -- they are listed below. + +\begin{formal} +We thank the reviewer for his/her support and remarks. His/her comments are addressed below. +\end{formal} + + +1. The authors focus primarily on the calculations of the total (T) correction +rather than the energy differences. However, the latter are of main importance +in most applications. The example of CuCl can be seen as involving energy +differences (along the potential energy curve), but the they are quite large in +comparison with, e.g. hydrogen bond strengths, dispersion forces, etc. It is +clear that when errors in the total energies do not exceed, say, $\sigma$, +relative energies must be accurate to within $2\sigma$ (in the worst-case +scenario). However, most quantum-chemical methods benefit from significant +error cancellation when energy differences are evaluated. Are there any +prospects of carrying out the sampling in a way that would be, in some sense, +systematic for, e.g. a water dimer and water molecule in the basis set of the +dimer (the same number of basis set functions)? + +\begin{formal} +This is indeed a very interesting suggestion! It is sure that modifying the +algorithm to compute directly energy differences would be a major improvement +of the presented algorithm. But it is not straightforward for the general case +as it necessitates finding an efficient importance sampling function. +As the reviewer suggests, computing the energy difference between two systems +with the same number of orbitals, and where the orbitals can be identified as +equivalent seems like a relatively simple first test to see the potential benefits +of the method. +\end{formal} + +2. The probability distribution in Eq. (7) is defined with a "threshold" for small energy differences. Alternatively, one can view this threshold a continuous parameter that "interpolates" between the uniform sampling ($e_{min} \rightarrow \infty$) and sampling based on the pure denominator (which may be unphysically small). This threshold is set to 0.2 au. Is there a justification of adopting this particular value? Are the results sensitive to this parameter (when changed within reasonable bounds)? + +\begin{formal} +Along the dissociation curve of CuCl we have observed, with +$\epsilon_\text{min}=0$, a slow convergence of the points at the largest +distances. This was due to the quasi-degeneracies of the orbital energies that made +$1/\Delta \epsilon$ diverge. We have empirically taken a value for +$\epsilon_\text{min}$ that did not change the speed of convergence of the +points with short distances, and that also enabled a similar convergence on the +problematic ones. +A sentence was added: +\begin{quote} +The algorithm is not very sensitive to the value of $\epsilon_{\min}$ as long as it is taken within reasonable bounds, in the range of the level-shift parameter in SCF calculations. +\end{quote} +\end{formal} + +3. Several typos/omissions: +- the CCSD method should probably be cited along with (T); +\begin{formal} +Thank you.We have now added the citation for the CCSD method. +\end{formal} + +- first paragraph on page 3: typo in "memorization"; +\begin{formal} +This is not a typo. It is really \emph{memoization}: \url{https://en.wikipedia.org/wiki/Memoization}. +\end{formal} + +- below Eq. (5): Coulomb (capital letter); +\begin{formal} +Thank you, this typo was fixed. +\end{formal} + + +%%% + + +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% +{\large \bf Response to Reviewer 2:} +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% + +This is an excellent manuscript on combining explicit coupled cluster (CCSD) and stochastic perturbational triples to speed-up CC correlated wave function calculations. Very straightforward and "obvious" idea (in fact, a number of such techniques is used in purely stochastic codes). It should be effective since sampling and corresponding weights takes care of triples contribution with known error bars. + +Indeed, the results are solid, for example, an order of magnitude speed-up that is benchmarked against fully explicit calculations. The resource analysis shows for which situations this can be effective. + +I did not catch any obvious mistakes or shortcomings. The work is very well described and the narrative has the right level of important details. + +In fact, the results suggest that there might be other explicit-and-stochastic algorithms possible with further reduction in run times. This implies that there is a potential for a solid impact in future. + +I recommend publishing in JCP. + + +\begin{formal} +We thank the reviewer for his/her support! +\end{formal} + + + +\end{document}