Manu: done with my revisions. T2, you neeed to check some of my responses.

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Emmanuel Fromager 2020-05-07 18:37:37 +02:00
parent 49d6804b8a
commit fd862e166d

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@ -82,10 +82,10 @@ relevance of these
expansions by considering weak deviations from the uniform density
regime. Indeed, in this case, eLDA is a reasonable approximation and the
difference in density between the ensemble and the individual states is
weak. Let us finally stress that our embedding strategy does not rely on these
small. Let us finally stress that our embedding strategy does not rely on these
Taylor expansions. They are exclusively used for analysis purposes in
this work. As written explicitly in the revised manuscript, it just
gives more insight into eLDA.}
this work. As written explicitly in the revised manuscript, they just
give more insight into eLDA.}
\item
{Page 5: Though the ringium model is developed elsewhere in the literature in great detail, a diagram for readers not as familiar with it would be a kindness. }
@ -138,7 +138,16 @@ gives more insight into eLDA.}
{Page 7: Does strong correlation always result in non-linear ghosts uncorrected by the GIC-eLDA, or is it particularly difficult or changed by the embedding scheme somehow?
Is this result influenced by the state mixing shown by FCI in Figure 3's discussion? }
\\
\alert{According to our observation, yes.}
\alert{As now discussed in more detail in the revised manuscript,
the remaining non-linear ghosts originate from the weight dependence
(i.e. the dependence on the state mixing) of
the individual correlation energies, which is itself connected to the eLDA correlation
functional. This can be understood from the general ensemble correlation
energy per particle expression in Eq. (41) and the above-mentioned
Taylor expansions, without referring to our
embedding approach. In summary, the deviation from linearity of the
ensemble GIC-eLDA energy is a
general feature of ensemble LDA-type functionals.}
\item
{Page 7: In the penultimate paragraph on this page, the discussion of Eqns 47 and 49 and the variation in the ensemble weights touches on one of the more subtle results of the GIC-eLDA, in my opinion, so it would be best to more explicitly describe this and its tie to the aforementioned equations.}
@ -190,13 +199,24 @@ you agree?}
\item
{Page 8: If the authors have evidence of behavior between $w=(0,0)$ and the equiensemble, instead of just these endpoints, that would be interesting to mention for the eDFT crowd. }
\\
\alert{Nothing to mention here.}
\alert{Actually, we were probably not clear enough about what we
plotted in Figs. 1 and 2 of the original manuscript, but it was exactly
the continuous variation of (individual or ensemble) energies from
$w=(0,0)$ up to the equiensemble case $w=(1/3,1/3)$. For convenience,
the path was just split in two parts: a first one where $w_2=0$ and
$0\leq w_1\leq 1/3$, and a second one where $w_1=1/3$ and $0\leq w_2\leq
1/3$. For clarity, this is now mentioned explicitly in the revised
manuscrit before commenting on the plots.}\manu{OK?}
\item
{Are there similar issues with combining HF exchange with LDA C as seen in the ground-state?
If not, why not? }
\\
\alert{Yes, similar issues appear for excited states.}
\alert{Yes, as readily seen from the data provided in the
supplemental material, similar issues appear for excited states.
Interestingly, increasing the ensemble weights (which of course cannot
be done in conventional ground-state DFT) seems to reduce
errors}\manu{We need to check the tables in the SI}
\item
{Figure 3 discussion: Will eLDA always overestimate double excitations?
@ -218,7 +238,12 @@ you agree?}
\alert{As mentioned in the original manuscript (see Results and Discussion section), we believe that it might be a consequence of how we constructed the eLDA functional, as the weight dependence of the eLDA functional is based on a two-electron uniform electron gas.
We do not think this is due to the uniformity of its density, though.
Incorporating a $N$-dependence in the functional through the curvature of the Fermi hole might be valuable in this respect.
This is left for future work.}
This is left for future work.}\manu{Could we argue that the
difference in density between the ground and the excited states is
not that substantial? Or the deviations cancel out after integration? The
question does not seem to be focused on the functional itself but more
on the evaluation of this term for a system (boxium) that is not
uniform. What do you think?}
\item
{Figure 6: Do the ground-state and equiensemble results for doubles converge as $N$ goes to infinity?}