diff --git a/BSE-PES.tex b/BSE-PES.tex index 4f04f0f..c07d626 100644 --- a/BSE-PES.tex +++ b/BSE-PES.tex @@ -534,7 +534,7 @@ The error (in \%) compared to the reference CC3 values are reported in square br CC2 & 1.391[$-0.78\%$] & 2.989[$-0.99\%$] & 2.982[$+0.64\%$] & 2.396[$-0.29\%$] & 2.106[$+1.49\%$] & 2.156[$+0.94\%$] & 2.393[$+0.13\%$] & 2.665[$+0.08\%$] \\ MP2 & 1.391[$-0.78\%$] & 3.008[$-0.36\%$] & 2.970[$+0.24\%$] & 2.395[$-0.33\%$] & 2.091[$+0.77\%$] & 2.137[$+0.05\%$] & 2.382[$-0.33\%$] & 2.634[$-1.09\%$] \\ BSE@{\GOWO}@HF & 1.399[$-0.21\%$] & 3.017[$-0.07\%$] & (2.974)[$+0.37\%$] & \gb{(2.408)} & 2.065[$-0.48\%$] & 2.134[$-0.09\%$] & \gb{(2.383)} & (2.640)[$-0.86\%$] \\ - RPA@{\GOWO}@HF & 1.382[$-1.43\%$] & 2.997[$-0.73\%$] & (2.965)[$+0.07\%$] & \gb{(2.389)} & 2.043[$-1.54\%$] & 2.132[$-0.19\%$] & \gb{(2.367)} & (2.571)[$-3.45\%$] \\ + RPA@{\GOWO}@HF & 1.382[$-1.43\%$] & 2.997[$-0.73\%$] & (2.965)[$+0.07\%$] & \gb{(2.389)} & 2.043[$-1.54\%$] & 2.132[$-0.19\%$] & 2.367[$-0.96\%$] & (2.571)[$-3.45\%$] \\ RPAx@HF & 1.394[$-0.57\%$] & 3.011[$-0.26\%$] & 2.944[$-0.64\%$] & 2.391[$-0.50\%$] & 2.041[$-1.64\%$] & 2.104[$-1.50\%$] & 2.366[$-1.00\%$] & 2.565[$-3.68\%$] \\ RPA@HF & 1.386[$-1.14\%$] & 2.994[$-0.83\%$] & 2.946[$-0.57\%$] & 2.382[$-0.87\%$] & 2.042[$-1.59\%$] & 2.103[$-1.54\%$] & 2.364[$-1.09\%$] & 2.573[$-3.38\%$] \\ \\ @@ -548,7 +548,7 @@ The error (in \%) compared to the reference CC3 values are reported in square br CC2 & 33.259[$-17.64\%$] & 57.289[$-18.13\%$] & 376.712[$-1.82\%$] & 356.909[$-6.61\%$] & 488.017[$-1.29\%$] & 465.492[$-2.53\%$] & 427.285[$-4.51\%$] & 654.878[$-2.09\%$] \\ MP2 & 33.164[$-17.87\%$] & 57.930[$-17.21\%$] & 372.997[$-2.79\%$] & 355.652[$-6.94\%$] & 477.951[$-3.33\%$] & 455.020[$-4.72\%$] & 421.600[$-5.78\%$] & 644.349[$-3.67\%$] \\ BSE@{\GOWO}@HF & 46.498[$+15.15\%$] & 78.075[$+11.58\%$] & 388.907[$+1.36\%$] & xxx.xxx[$+0.00\%$] & 499.145[$+0.96\%$] & 481.151[$+0.75\%$] & xxx.xxx[$+0.00\%$] & 675.701[$+1.02\%$] \\ - RPA@{\GOWO}@HF & 57.567[$+42.56\%$] & 101.092[$+44.47\%$] & 473.053[$+23.29\%$] & xxx.xxx[$+0.00\%$] & 580.318[$+17.38\%$] & 566.536[$+18.63\%$] & xxx.xxx[$+0.00\%$] & 794.324[$+18.76\%$] \\ + RPA@{\GOWO}@HF & 57.567[$+42.56\%$] & 101.092[$+44.47\%$] & 473.053[$+23.29\%$] & xxx.xxx[$+0.00\%$] & 580.318[$+17.38\%$] & 566.536[$+18.63\%$] & 545.543[$+21.92\%$] & 794.324[$+18.76\%$] \\ RPAx@HF & 37.886[$-6.18\%$] & 65.203[$-6.82\%$] & 343.604[$-10.45\%$] & 344.249[$-9.93\%$] & 427.170[$-13.60\%$] & 416.315[$-12.83\%$] & 399.060[$-10.82\%$] & 586.090[$-12.38\%$] \\ RPA@HF & 57.332[$+41.98\%$] & 100.164[$+43.15\%$] & 465.905[$+21.43\%$] & 442.675[$+15.83\%$] & 569.384[$+15.17\%$] & 555.857[$+16.39\%$] & 537.685[$+20.16\%$] & 781.323[$+16.81\%$] \\ \end{tabular} diff --git a/Cover_Letter/CNRS_logo.pdf b/Cover_Letter/CNRS_logo.pdf new file mode 100644 index 0000000..954b3f7 Binary files /dev/null and b/Cover_Letter/CNRS_logo.pdf differ diff --git a/Cover_Letter/CoverLetter.tex b/Cover_Letter/CoverLetter.tex new file mode 100644 index 0000000..a58d192 --- /dev/null +++ b/Cover_Letter/CoverLetter.tex @@ -0,0 +1,49 @@ +\documentclass[10pt]{letter} +\usepackage{UPS_letterhead,xcolor,mhchem,mathpazo,ragged2e} +\newcommand{\alert}[1]{\textcolor{red}{#1}} +\definecolor{darkgreen}{HTML}{009900} + + +\begin{document} + +\begin{letter}% +{To the Editors of the Journal of Physical Chemistry Letters} + +\opening{Dear Editors,} + +\justifying +Please find enclosed our manuscript entitled +\begin{quote} +\textit{``Pros and Cons of the Bethe-Salpeter Formalism for Ground-State Energies''}, +\end{quote} +which we would like you to consider as a Letter in the \textit{Journal of Physical Chemistry Letters}. +This contribution fits nicely in the section \textit{``Spectroscopy and Photochemistry; General theory''}. +This contribution has never been submitted in total nor in parts to any other journal, and has been seen and approved by all authors. + +In the past few years, the Bethe-Salpeter formalism has demonstrated to be a valuable and cost-effective alternative to TD-DFT to compute excitation energies. +It has gained significant momentum, not only in Physics, but also within the Chemistry community, and is now available in several popular quantum chemistry software packages. +It is now a genuine multidisciplinary methodology that can be applied to materials as well as molecular systems. +Although less popular to date, the Bethe-Salpeter formalism can also be applied to compute ground-state energies via the adiabatic-connection fluctuation dissipation formalism. + +The present Letter provides, what we believe, are two important messages. +On the one hand, we show that Bethe-Salpeter can provide extremely accurate total energies and equilibrium bond distances. +We have illustrated this for 8 diatomic molecules for which we have also computed reference ground-state data using increasingly accurate coupled cluster methods. +For the larger systems considered here, we observe that Bethe-Salpeter recovers 99\% of the CC3 correlation energy and yields outstanding equilibrium bond lengths. +It should be stressed that such a success cannot be not reached with popular quantum chemistry methods such as MP2, CC2 or CCSD, and was never shown before. +On the other hand, we have also observed that, in some cases, unphysical irregularities on the ground-state potential energy surfaces due to the appearance of a satellite resonance with a weight similar to that of the GW quasiparticle peak. + +Because of the large impact of our work, we expect it to be of interest to a wide audience within the chemistry community and beyond. +We suggest Julien Toulouse, Patrick Rinke, Michael van Setten, Timothy Berkelbach, Fabien Bruneval, Wim Klopper, Trygve Helgaker, Pina Romaniello, and Lucia Reining as potential referees. +We look forward to hearing from you soon. + +\closing{Sincerely, the authors.} + + +\end{letter} +\end{document} + + + + + + diff --git a/Cover_Letter/UPS_letterhead.sty b/Cover_Letter/UPS_letterhead.sty new file mode 100644 index 0000000..2e5f5bb --- /dev/null +++ b/Cover_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} + \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 + } + +%I do not know what does the macro below + +%\long\def\closing#1{\par\nobreak\vspace{\parskip} + %\stopbreaks + %\noindent + %\ifx\@empty\fromaddress\else + %\hspace*{\longindentation}\fi + %\parbox{\indentedwidth}{\raggedright + %\ignorespaces #1\vskip .65in + %\ifx\@empty\fromsig + %\else \fromsig \fi\strut} + %\vspace*{\fill} +% \par} diff --git a/Cover_Letter/UPS_logo.pdf b/Cover_Letter/UPS_logo.pdf new file mode 100644 index 0000000..ca9ecee Binary files /dev/null and b/Cover_Letter/UPS_logo.pdf differ diff --git a/SI/BSE-PES-SI.tex b/SI/BSE-PES-SI.tex index 0a1f2e3..ea10837 100644 --- a/SI/BSE-PES-SI.tex +++ b/SI/BSE-PES-SI.tex @@ -211,7 +211,7 @@ When irregularities appear in the PES, the values are reported in parenthesis an & cc-pVQZ &\rb{1.399} &\rb{3.017} &\rb{(2.974)} &\gb{2.408} &\rb{2.065} &\rb{2.134} &\gb{2.383} &\rb{(2.640)}\\ RPA@{\GOWO}@HF & cc-pVDZ & 1.426 & 3.019 & 2.994 & 2.436 & 2.083 & 2.144 & 2.403 & (2.629) \\ & cc-pVTZ & 1.388 & 2.988 & (2.965) & 2.408 & 2.055 & 2.114 & (2.370) & (2.584) \\ - & cc-pVQZ & 1.382 & 2.997 & (2.965) &\gb{2.389} & 2.043 & 2.132 &\gb{2.367} & (2.571) \\ + & cc-pVQZ & 1.382 & 2.997 & (2.965) &\gb{2.389} & 2.043 & 2.132 & 2.367 & (2.571) \\ RPAx@HF & cc-pVDZ & 1.428 & 3.040 & 2.998 & 2.424 & 2.077 & 2.130 & 2.417 & 2.611 \\ & cc-pVTZ & 1.395 & 3.003 & 2.943 & 2.400 & 2.046 & 2.110 & 2.368 & 2.568 \\ & cc-pVQZ & 1.394 & 3.011 & 2.944 & 2.391 & 2.041 & 2.104 & 2.366 & 2.565 \\