From a04354ac1f93543e250653c405a6b4a0d78eef66 Mon Sep 17 00:00:00 2001 From: Pierre-Francois Loos Date: Tue, 25 Aug 2020 17:09:45 +0200 Subject: [PATCH] ready to submit --- benzene.nb | 844 ++++++++++++++++++++++++++++++++++++---------------- benzene.tex | 31 +- fig1a.pdf | Bin 43536 -> 43532 bytes fig1b.pdf | Bin 33415 -> 32984 bytes 4 files changed, 606 insertions(+), 269 deletions(-) diff --git a/benzene.nb b/benzene.nb index 177ef26..daf204c 100644 --- a/benzene.nb +++ b/benzene.nb @@ -10,10 +10,10 @@ NotebookFileLineBreakTest NotebookFileLineBreakTest NotebookDataPosition[ 158, 7] -NotebookDataLength[ 955487, 17961] -NotebookOptionsPosition[ 952722, 17906] -NotebookOutlinePosition[ 953115, 17922] -CellTagsIndexPosition[ 953072, 17919] +NotebookDataLength[ 967358, 18303] +NotebookOptionsPosition[ 962105, 18206] +NotebookOutlinePosition[ 962498, 18222] +CellTagsIndexPosition[ 962455, 18219] WindowFrame->Normal*) (* Beginning of Notebook Content *) @@ -81,8 +81,7 @@ Cell[BoxData[{ 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Open ]], +Cell[CellGroupData[{ +Cell[961531, 18188, 225, 4, 30, "Input",ExpressionUUID->"b22ca888-a8e8-4120-b6e9-9321f209da71"], +Cell[961759, 18194, 306, 7, 34, "Output",ExpressionUUID->"f93e1c9b-3d6f-4087-bd6f-29699c9090c6"] }, Open ]] }, Open ]] }, Open ]] diff --git a/benzene.tex b/benzene.tex index 1830785..34375f7 100644 --- a/benzene.tex +++ b/benzene.tex @@ -43,7 +43,7 @@ % Abstract \begin{abstract} -Following the recent work of Eriksen \textit{et al.}~[\href{https://arxiv.org/abs/2008.02678}{arXiv:2008.02678 [physics.chem-ph]}], we report the performance of the \textit{Configuration Interaction using a Perturbative Selection made Iteratively} (CIPSI) method on the non-relativistic frozen-core correlation energy of the benzene molecule in the cc-pVDZ basis. Following our usual protocol, we obtain a correlation energy of \titou{$-86x.x(x)$} m$E_h$ which agrees with the theoretical estimate of $-863$ m$E_h$ proposed by Eriksen \textit{et al.}~using an extensive array of highly-accurate new electronic structure methods. +Following the recent work of Eriksen \textit{et al.}~[\href{https://arxiv.org/abs/2008.02678}{arXiv:2008.02678 [physics.chem-ph]}], we report the performance of the \textit{Configuration Interaction using a Perturbative Selection made Iteratively} (CIPSI) method on the non-relativistic frozen-core correlation energy of the benzene molecule in the cc-pVDZ basis. Following our usual protocol, we obtain a correlation energy of $-863.4(5)$ m$E_h$ which agrees with the theoretical estimate of $-863$ m$E_h$ proposed by Eriksen \textit{et al.}~using an extensive array of highly-accurate new electronic structure methods. \end{abstract} % Title @@ -97,7 +97,7 @@ The outcome of this work is nicely summarized in the abstract of Ref.~\onlinecit \hline ph-AFQMC & $-864.3(4)$ & \onlinecite{Lee_2020} \\ \hline - CIPSI & \titou{$-86x.x(x)$} & This work \\ + CIPSI & $-863.4(5)$ & This work \\ \end{tabular} \end{ruledtabular} \end{table} @@ -142,25 +142,14 @@ higher-lying $\sigma$ [37,38,40,44,45,47,48,51,52,58--70,75--81,86,88--91,94--97 Like Pipek-Mezey, \cite{Pipek_1989} this choice of orbital windows allows to preserve a strict $\sigma$-$\pi$ separation in planar systems like benzene. As one can see from the energies of Table \ref{tab:NOvsLO}, for a given value of $N_\text{det}$, the variational energy as well as the PT2-corrected energies are much lower with localized orbitals than with natural orbitals. We, therefore, consider these energies more trustworthy, and we will base our best estimate of the correlation energy of benzene on these calculations. The convergence of the CIPSI correlation energy using localized orbitals is illustrated in Fig.~\ref{fig:CIPSI}, where one can see the behavior of the correlation energy, $\Delta E_\text{var.}$ and $\Delta E_\text{var.} + E_\text{(r)PT2}$, as a function of $N_\text{det}$ (left panel). -The right panel of Fig.~\ref{fig:CIPSI} is more instructive as it shows $\Delta E_\text{var.}$ as a function of $E_\text{(r)PT2}$, and their corresponding \titou{five}-point linear extrapolation curves that we have used to get our final estimate of the correlation energy. +The right panel of Fig.~\ref{fig:CIPSI} is more instructive as it shows $\Delta E_\text{var.}$ as a function of $E_\text{(r)PT2}$, and their corresponding four-point linear extrapolation curves that we have used to get our final estimate of the correlation energy. From this figure, one clearly sees that the rPT2-based correction behaves more linearly than its corresponding PT2 version, and is thus systematically employed in the following. % Results Our final number are gathered in Table \ref{tab:extrap_dist_table}, where, following the notations of Ref.~\onlinecite{Eriksen_2020}, we report, in addition to the final variational energies $\Delta E_{\text{var.}}$, the extrapolation distances, $\Delta E_{\text{dist}}$, defined as the difference between the final computed energy, $\Delta E_{\text{final}}$, and the extrapolated energy, $\Delta E_{\text{extrap.}}$ associated with ASCI, iCI, SHCI, DMRS, and CIPSI. -The three flavours of SCI fall into an interval ranging from $-860.0$ m$E_h$ (ASCI) to $-864.2$ m$E_h$ (SHCI), while the other non-SCI methods yield correlation energies ranging from $-863.7$ to $-862.8$ m$E_h$ (see Table \ref{tab:energy}). Our final CIPSI number (obtained with localized orbitals and rPT2 correction via a \titou{five}-point linear extrapolation) is \titou{$-86x.x(x)$} m$E_h$. +The three flavours of SCI fall into an interval ranging from $-860.0$ m$E_h$ (ASCI) to $-864.2$ m$E_h$ (SHCI), while the other non-SCI methods yield correlation energies ranging from $-863.7$ to $-862.8$ m$E_h$ (see Table \ref{tab:energy}). Our final CIPSI number (obtained with localized orbitals and rPT2 correction via a four-point linear extrapolation) is $-863.4(5)$ m$E_h$, where the error reported in parenthesis represents the fitting error (not the extrapolation error for which it is much harder to provide a theoretically sound estimate). For comparison, the best post blind test SHCI estimate is $-863.3$ m$E_h$, which agrees almost perfectly with our best CIPSI estimate. -\titou{Although it is not possible to provide a theoretically sound error bar, we estimate the extrapolation error by ... -We believe that it provides a very safe estimate of the extrapolation error.} - -% Timings -The present calculations have been performed on the AMD partition of GENCI's Irene supercomputer. -Each Irene's AMD node is a dual-socket AMD Rome (Epyc) CPU@2.60 GHz with 256GiB of RAM, with a total of 64 physical CPU cores per socket. -These nodes are connected via Infiniband HDR100. -The first step of the calculation, \ie, performing a CIPSI calculation up to $N_\text{det} \sim 10^7$ with Hartree-Fock orbitals in order to produce natural orbitals, takes roughly 24 hours on a single node, and reaching the same number of determinants with natural orbitals or localized orbitals takes roughly the same amount of time. -A second 24-hour run on 10 distributed nodes was performed to push the selection to $8 \times 10^7$ determinants, and a third distributed run using 40 nodes was used to reach $16 \times 10^7$ determinants. -A last 24-hour run on 60 distributed nodes was performed to obtain the largest wave function of $25 \times 10^7$ determinants and its PT2 correction. -In total, the present calculation has required \titou{340k} core hours, almost half of it being spent in the last stage of the computation. %%$ FIG. 1 %%% \begin{figure*} @@ -171,7 +160,7 @@ In total, the present calculation has required \titou{340k} core hours, almost h Convergence of the CIPSI correlation energy of benzene using localized orbitals. Left: $\Delta E_\text{var.}$, $\Delta E_\text{var.} + E_\text{PT2}$, and $\Delta E_\text{var.} + E_\text{rPT2}$ (in m$E_h$) as functions of the number of determinants in the variational space $N_\text{det}$. Right: $\Delta E_\text{var.}$ (in m$E_h$) as a function of $E_\text{PT2}$ or $E_\text{rPT2}$. - The \titou{five}-point linear extrapolation curves (dashed lines) are also reported. + The four-point linear extrapolation curves (dashed lines) are also reported. The theoretical estimate of $-863$ m$E_h$ from Ref.~\onlinecite{Eriksen_2020} is marked by a black line for comparison purposes. \label{fig:CIPSI} } @@ -216,7 +205,6 @@ The statistical error on $E_\text{(r)PT2}$, corresponding to one standard deviat 41\,943\,040 & $-231.487\,978$ & $-231.564\,529(382)$ & $-231.563\,593(377)$ & $-231.519\,122$ & $-231.567\,419(240)$ & $-231.567\,069(238)$ \\ 83\,886\,080 & $-231.501\,334$ & $-231.566\,994(317)$ & $-231.566\,325(314)$ & $-231.528\,568$ & $-231.570\,084(199)$ & $-231.569\,832(198)$ \\ 167\,772\,160 & $-231.514\,009$ & $-231.569\,939(273)$ & $-231.569\,467(271)$ & $-231.536\,655$ & $-231.571\,981(175)$ & $-231.571\,804(174)$ \\ - 251\,658\,240 & \\ \end{tabular} \end{ruledtabular} \end{table*} @@ -240,11 +228,18 @@ The statistical error on $E_\text{(r)PT2}$, corresponding to one standard deviat SHCI & $-827.2$ & $-852.8$ & $-864.2$ & $-11.4$ \\ DMRG & $-859.2$ & $-859.2$ & $-862.8$ & $-3.6$ \\ \hline - CIPSI & \titou{$-8xx.x$} & \titou{$-8xx.x$} & \titou{$-86x.x$} & \titou{$-xx.x$} \\ + CIPSI & $-814.8$ & $-850.2$ & $-863.4$ & $-13.2$ \\ \end{tabular} \end{ruledtabular} \end{table} +% Timings +The present calculations have been performed on the AMD partition of GENCI's Irene supercomputer. +Each Irene's AMD node is a dual-socket AMD Rome (Epyc) CPU@2.60 GHz with 256GiB of RAM, with a total of 64 physical CPU cores per socket. +These nodes are connected via Infiniband HDR100. +The first step of the calculation, \ie, performing a CIPSI calculation up to $N_\text{det} \sim 10^7$ with Hartree-Fock orbitals in order to produce natural orbitals, takes roughly 24 hours on a single node, and reaching the same number of determinants with natural orbitals or localized orbitals takes roughly the same amount of time. +A second 24-hour run on 10 distributed nodes was performed to push the selection to $8 \times 10^7$ determinants, and a third distributed run using 40 nodes was used to reach $16 \times 10^7$ determinants. 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