\documentclass[10pt]{letter}
\usepackage{UPS_letterhead,xcolor,mhchem,mathpazo,ragged2e,hyperref}
\newcommand{\alert}[1]{\textcolor{red}{#1}}
\definecolor{darkgreen}{HTML}{009900}


\begin{document}

\begin{letter}%
{To the Members of the Faraday Discussions Scientific Committee,}

\opening{Dear Members of the Faraday Discussions Scientific Committee,}

\justifying
Please find attached a revised version of the manuscript entitled 
\begin{quote}
\textit{``Weight Dependence of Local Exchange-Correlation Functionals in Ensemble Density-Functional Theory: Double Excitations in Two-Electron Systems''}.
\end{quote}
We thank the reviewer for his/her constructive comments.
Our detailed responses to his/her comments can be found below.

We look forward to hearing from you.

\closing{Sincerely, the authors.}

%%% REVIEWER 1 %%%
\noindent \textbf{\large Authors' answer to Reviewer \#1}

\begin{itemize}

	\item
	{The authors describe the ensemble formulation of DFT or the Gross-Oliveira-Kohn DFT (GOK-DFT) in its Kohn-Sham formulation as a viable method for excited state calculations. They provide a very clear summary of the theory, followed by the main work of the paper which is the investigation of weight-dependent LDA-type xc functionals for eDFT calculations. The provide important insights on small systems with 2 electrons and functionals that are tailored for double excitations in these systems. The manuscript makes an important contribution to the field of DFT and should be accepted for publication. However, I would be grateful if the authors modify the paper slightly to address the following minor points and corrections:}
	\\
	\alert{We thank the reviewer for his/her kind comments. 
	His/her comments are addressed below.}

	\item 
	{They should comment about what is needed (or even if it is possible) to develop a weight-dependent universal xc functional for eDFT calculations instead of application-specific functionals as presented in this paper.}
	\\
	\alert{This is a good point. For clarity, we complemented the
theory section as follows.\\
{\it 
``As shown in Sec. IV A 4, the weight dependence of the correlation
energy can be extracted from a FUEG model. In order to make the
resulting weight-dependent correlation functional truly universal, i.e.
independent on the number of electrons in the FUEG, one could use the
curvature of the Fermi hole [88] as an additional variable in the
density-functional approximation. The development of such a generalized
cor- relation eLDA is left for future work. Even though a similar
strategy could be applied to the weight-dependent exchange part, we
explore in the present work a different path where the
(system-dependent) exchange functional parameterization relies on the
ensemble energy linearity constraint (see Sec. IV A 2). Finally, let us
stress that, in order to further improve the description of the ensemble
correlation energy, a post-treatment of the recently revealed
density-driven correlations [62,92-94] (which, by construction, are absent from FUEGs) might be necessary. An orbital-dependent correction derived in Ref. 92 might be used for that purpose. Work is currently in progress in this direction.
''}}

	\item 
	{In the captions of Figures 1 and 2 replace "functional's" with "functionals'"}
	\\
	\alert{This has been fixed.}

	\item 
	{The density $n(r)$ used in equation 21, 9, 10 and more doesn't represent any specific density. 
	In the case of equation 21, we simply present the well-known Dirac-exchange density functional and, by definition of a density functional, we don't have to specify in its formulation to which density it is applied but only that it is a mathematical object applying to any density $n(r)$.
Of course, when we will use this functional or any other one in our work we will surely apply it to the ensemble Density $n^w(r)$ and the notation will be carefully modified accordingly. }
	
	\item 
	{Change "Third, we add up correlation effects" to "Third, we include correlation effects"}	
	\\
	\alert{ This has been fixed.}	

	
	\item 
	{Change "studied in excruciated details" to "studied extensively"}	
	\\
	\alert{ This has been fixed.}	
	
		
	\item 
	{They need to be a bit more consistent with their notation as in equation 9 and elsewhere "$n(r)$" should be the ensemble (weight-dependent) density "$n^w(r)$". 
	I don?t believe they defined "$n(r)$" in the paper so I don?t know which density it represents. }	
	\\
	\alert{See our response to 6.}	
		
	\item 
	{Even if it sounds trivial, they should explain why the exact xc functional should have linear dependence in the excitation energies as a function of the weight value.}	
	\\
	\alert{GOK variational principle states that the expectation value of the ensemble energy admits/possesses a lower bond which is linear with respect to each of the ensemble-weights $w_i$ and is the exact ensemble energy of the studied system (equation 1). 
	Moreover, by construction, one can easily see that the slope of the exact ensemble energy with respect to a specific weight $w_i$ corresponds to the excitation energy of the system defined between the ground state and the ith-excited state associated to this specific weight (equation 4). 
	It is important that the reader keeps in mind that the exact excitation energies are based on pure-state energies and, therefore, do not depend on the weights of the ensemble.
	In practice, the ensemble energy is rarely w-linear (linear in w ?) because of the use of approximate xc-functionals. 
	Indeed, by inserting the ensemble density in the Hartree interaction functional (equation 9), it introduces spurious quadratic curvature with respect to the weight in the ensemble energy. 
	Some of those terms are responsible of the unphysical phenomenon called ghost-interaction errors. 
	Therefore, the ensemble-Khon-Sham gap obtained at the end of the ensemble-HF-calculation is, somehow, "weight-contaminated" and doesn't possess the right weight-dependence. 
	(two first terms of the right-hand side of equation16)
	By taking its first derivative with regard to the weight, the xc-functional is expected to compensate those parasite-quadratic terms in order to retrieve the linear behavior of the exact ensemble energy and one can understand that only a weight-dependant xc-functional could do so.
	At the best of my knowledge, I cannot see any reason why the xc-functional should be w-linear. 
	The important idea is that the linearity must be in the ensemble energy but the main constraint on the xc-functional should be that it is weight-dependant.
	We emphasize that only the exact ensemble-xc-functional would have the ideal weight-dependency that would make the corresponding ensemble energy reproduce perfectly the linear behavior of the exact ensemble energy and lead to weight-independant excitation energies, that is exact excitation energies.
	The use of an approximate weight-dependant xc-functional could reduce the ensemble energy curvature and give less weight-dependant excitation energies but it is reasonable to admit that it also could make things worse it the weight-dependency of the functional is poorly chosen.
	That is why the construction of "good" weight-dependant xc-functionals is a really challenging matter in eDFT.}	
	
\end{itemize}

\end{letter}
\end{document}