From 7ddfc221d1c8a98ae25f4145990a824f1d1fffcc Mon Sep 17 00:00:00 2001 From: Pierre-Francois Loos Date: Sat, 22 Aug 2020 09:46:07 +0200 Subject: [PATCH] almost done with note --- benzene.dat | 1 + benzene.nb | 489 +++++++++++++++++++++-------------------- benzene.tex | 56 ++--- benzene_noS2.dat | 1 + benzene_noS2_local.dat | 1 + fig1a.pdf | Bin 42500 -> 42613 bytes fig1b.pdf | Bin 33038 -> 33099 bytes 7 files changed, 282 insertions(+), 266 deletions(-) diff --git a/benzene.dat b/benzene.dat index 04763b1..fee72a9 100644 --- a/benzene.dat +++ b/benzene.dat @@ -21,3 +21,4 @@ 5892976 -231.43454648 -231.55441275 0.00059892 -231.55185712 0.00058615 11786019 -231.44370625 -231.55550485 0.00055109 -231.55332245 0.00054034 23572080 -231.45375768 -231.55855354 0.00051764 -231.55667052 0.00050834 + 47144174 -231.46449337 -231.56037965 0.00046967 -231.55882970 0.00046208 diff --git a/benzene.nb b/benzene.nb index b089868..61f7f89 100644 --- a/benzene.nb +++ b/benzene.nb @@ -10,10 +10,10 @@ 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\onlinecite{Eriksen_2020} \\ + iCIPT2 & $-861.1(5)$ & \onlinecite{Eriksen_2020} \\ + CCSDTQ & $-862.4$ & \onlinecite{Eriksen_2020} \\ + DMRG & $-862.8(7)$ & \onlinecite{Eriksen_2020} \\ + FCCR(2) & $-863.0$ & \onlinecite{Eriksen_2020} \\ + CAD-FCIQMC & $-863.4$ & \onlinecite{Eriksen_2020} \\ + AS-FCIQMC & $-863.7(3)$ & \onlinecite{Eriksen_2020} \\ + SHCI & $-864.2(2)$ & \onlinecite{Eriksen_2020} \\ \hline - ph-AFQMC & -864.3(4) & \onlinecite{Lee_2020} \\ + ph-AFQMC & $-864.3(4)$ & \onlinecite{Lee_2020} \\ \hline - CIPSI & -8xx.x(x) & This work \\ + CIPSI & \titou{$-86x.x(x)$} & This work \\ \end{tabular} \end{ruledtabular} \end{table} @@ -117,43 +117,48 @@ Being late to the party, we obviously cannot report blindly our CIPSI results. However, following the philosophy of Eriksen \textit{et al.}, \cite{Eriksen_2020} we will report our results with the most neutral tone, leaving the freedom to the reader to make up his/her mind. We then follow our usual ``protocol'' \cite{Scemama_2018,Scemama_2018b,Scemama_2019,Loos_2018a,Loos_2019,Loos_2020a,Loos_2020b,Loos_2020c} by performing a preliminary SCI calculation using Hartree-Fock orbitals in order to generate a SCI wave function with at least $10^7$ determinants. Natural orbitals (NOs) are then computed based on this wave function, and a new, larger SCI calculation is performed with this new set of orbitals. -This has the advantage to produce a smoother and faster convergence of the SCI energy toward the FCI limit +This has the advantage to produce a smoother and faster convergence of the SCI energy toward the FCI limit. The total SCI energy is defined as the sum of the variational energy $E_\text{var.}$ (computed via diagonalization of the CI matrix in the reference space) and a second-order perturbative correction $E_\text{PT2}$ which takes into account the external determinants, \ie, the determinants which do not belong to the variational space but are linked to the reference space via a nonzero matrix element. The magnitude of $E_\text{PT2}$ provides a qualitative idea of the ``distance'' to the FCI limit. As mentioned above, SCI+PT2 methods rely heavily on extrapolation, especially when one deals with medium-sized systems. We then linearly extrapolate the total SCI energy to $E_\text{PT2} = 0$ (which effectively corresponds to the FCI limit) using the two largest SCI wave functions. -Although it is not possible to provide a theoretically sound error bar, we estimate the extrapolation error by the difference in excitation energy between the largest SCI wave function and its corresponding extrapolated value. +Although it is not possible to provide a theoretically sound error bar, we estimate the extrapolation error by \titou{the difference in excitation energy between the largest SCI wave function and its corresponding extrapolated value.} We believe that it provides a very safe estimate of the extrapolation error. %Note that all the wave functions are eigenfunctions of the $\Hat{S}^2$ spin operator, as described in Ref.~\onlinecite{Applencourt_2018}. +The corresponding energies are reported in Table \ref{tab:NOvsLO} as functions of the number of determinants in the variational space $N_\text{det}$. A second run has been performed with localized orbitals. -A Pipek-Mezey localization procedure \cite{Pipek_1989} was performed in several orbital windows: i) core, ii) valence $\sigma$, iii) valence $\pi$, iv) valence $\pi^*$, v) valence $\sigma^*$, and vi) the rest. \titou{More information needed here.} -As one can see from the results of Table \ref{tab:NOvsLO}, the variational energy as well as the PT2 corrected energy is much lower with localized orbitals for a same number of determinants. +Starting from the Hartree-Fock orbitals, a Pipek-Mezey localization procedure \cite{Pipek_1989} was performed in several orbital windows: i) core, ii) valence $\sigma$, iii) valence $\pi$, iv) valence $\pi^*$, v) valence $\sigma^*$, and vi) the higher virtual orbitals. \titou{More information needed here.} +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 NOs. We, therefore, consider these energies more trustworthy, and we will based 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 $\Delta E_\text{var.}$, $\Delta E_\text{var.} + E_\text{PT2}$, and $\Delta E_\text{var.} + E_\text{rPT2}$ as a function of $N_\text{det}$ (left panel). +The right panel of Fig.~\ref{fig:CIPSI} shows $\Delta E_\text{var.} + E_\text{PT2}$ and $\Delta E_\text{var.} + E_\text{rPT2}$ (in m$E_h$) as functions of $E_\text{PT2}$ or $E_\text{rPT2}$, and their corresponding \titou{two}-point linear extrapolation curves that we have used to get our final estimate of the correlation energy. -% Results and discussion +% Results +Our final numbers 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 the ASCI, iCI, SHCI, CIPSI, and DMRG results. +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 methods yield correlation energies ranging from $-863.7$ to $-862.8$ m$E_h$. Our final CIPSI number is \titou{$-86x.xx$} m$E_h$. + +% 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. These nodes are connected via Infiniband HDR100. -The three flavours of SCI fall into an interval ranging from $-863.7$ to $-862.8$ m$E_h$. -The CIPSI number is ? - %%$ FIG. 1 %%% \begin{figure*} \includegraphics[width=0.4\linewidth]{fig1a} \hspace{0.08\linewidth} \includegraphics[width=0.4\linewidth]{fig1b} \caption{ - Convergence of the CIPSI correlation energy for benzene using localized orbitals. + Convergence of the CIPSI correlation energy 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. Right: $\Delta E_\text{var.} + E_\text{PT2}$ and $\Delta E_\text{var.} + E_\text{rPT2}$ (in m$E_h$) as functions of $E_\text{PT2}$ or $E_\text{rPT2}$. - The two-point linear extrapolation curves (dashed lines) are also reported. + The \titou{two}-point linear extrapolation curves (dashed lines) are also reported. The theoretical best estimate of $-863$ m$E_h$ from Ref.~\onlinecite{Eriksen_2020} is marked by a black line for comparison purposes. \label{fig:CIPSI} } \end{figure*} %%% TABLE II %%% -\begin{squeezetable} +%\begin{squeezetable} \begin{table*} \caption{Variational energy $E_\text{var.}$, second-order perturbative correction $E_\text{PT2}$ and its renormalized version $E_\text{rPT2}$ (in $E_h$) as a function of the number of determinants $N_\text{det}$ for the ground-state of the benzene molecule computed in the cc-pVDZ basis set. The statistical error on $E_\text{PT2}$, corresponding to one standard deviation, are reported in parenthesis.} @@ -187,10 +192,11 @@ The statistical error on $E_\text{PT2}$, corresponding to one standard deviation 2\,621\,440 & $-231.439\,324$ & $-231.553\,845(572)$ & $-231.551\,544(560)$ & $-231.473\,751$ & $-231.555\,261(403)$ & $-231.554\,159(397)$ \\ 5\,242\,880 & $-231.450\,156$ & $-231.557\,541(534)$ & $-231.555\,558(524)$ & $-231.485\,829$ & $-231.558\,303(362)$ & $-231.557\,451(358)$ \\ 10\,485\,760 & $-231.461\,927$ & $-231.559\,390(481)$ & $-231.557\,796(474)$ & $-231.497\,515$ & $-231.562\,568(322)$ & $-231.561\,901(319)$ \\ + 20\,971\,520 & $-231.474\,019$ & $-231.561\,315(430)$ & $-231.560\,063(424)$ & $-231.508\,714$ & $-231.564\,707(275)$ & $-231.564\,223(273)$ \\ \end{tabular} \end{ruledtabular} \end{table*} -\end{squeezetable} +%\end{squeezetable} %%% %%% %%% %%% %%% TABLE II %%% @@ -199,7 +205,7 @@ The statistical error on $E_\text{PT2}$, corresponding to one standard deviation The final variational energies $\Delta E_{\text{var.}}$ are also reported. See Ref.~\onlinecite{Eriksen_2020} for more details. All the energies are given in m$E_h$. - \label{extrap_dist_table} + \label{tab:extrap_dist_table} } \begin{ruledtabular} \begin{tabular}{lcccc} @@ -208,7 +214,7 @@ The statistical error on $E_\text{PT2}$, corresponding to one standard deviation ASCI & $-737.1$ & $-835.4$ & $-860.0$ & $-24.6$ \\ iCI & $-730.0$ & $-833.7$ & $-861.1$ & $-27.4$ \\ SHCI & $-827.2$ & $-852.8$ & $-864.2$ & $-11.4$ \\ - CIPSI & $-8xx.x$ & $-8xx.x$ & $-8xx.x$ & $-xx.x$ \\ + CIPSI & \titou{$-8xx.x$} & \titou{$-8xx.x$} & \titou{$-86x.x$} & \titou{$-xx.x$} \\ DMRG & $-859.2$ & $-859.2$ & $-862.8$ & $-3.6$ \\ \end{tabular} \end{ruledtabular} diff --git a/benzene_noS2.dat b/benzene_noS2.dat index 54e8099..41a74f0 100644 --- a/benzene_noS2.dat +++ b/benzene_noS2.dat @@ -20,3 +20,4 @@ 2621440 -231.43932438 -231.55384542 0.00057169 -231.55154435 0.00056021 5242880 -231.45015608 -231.55754133 0.00053356 -231.55555800 0.00052371 10485760 -231.46192749 -231.55939032 0.00048147 -231.55779568 0.00047359 + 20971520 -231.47401920 -231.56131493 0.00043027 -231.56006331 0.00042410 diff --git a/benzene_noS2_local.dat b/benzene_noS2_local.dat index 18a1e81..d9c523c 100644 --- a/benzene_noS2_local.dat +++ b/benzene_noS2_local.dat @@ -20,3 +20,4 @@ 2621440 -231.47375051 -231.55526062 0.00040253 -231.55415883 0.00039709 5242880 -231.48582938 -231.55830266 0.00036203 -231.55745147 0.00035778 10485760 -231.49751473 -231.56256801 0.00032228 -231.56190078 0.00031897 + 20971520 -231.50871375 -231.56470650 0.00027492 -231.56422301 0.00027255 diff --git a/fig1a.pdf b/fig1a.pdf index f24645e636e7d693c895ad66a8a355c08bfb1c3f..051c12f2299cac1791f68316cb2bd6bdd2206f49 100644 GIT binary patch delta 23396 zcmX_mV{{-*6K;%+Hnummla0MeHr6KD*tRjTZQHhO+qTV(Z{GXebALTk(}kz&^qH>e zY5#GshjFm#Y*1iOitAO%>dE}l^!4-NT}qwv`j;qWPmPfI)%^}ubSWn!u@ zUi;3o>;8_-G2Dsz;X&rYkdKucWG~w2Zpah=E=ujBC6l}?Vk!1AiIuPnd|~RyVpmh! zh`&SY&ND9V?2Kz{f2GU0r^&8Edu$`}Sy8`_{Oq!>#U8+jXYUe3ES&TZth{L8u#u#$ 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