<div dir="ltr"><p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">Dear
Wien2k developers and users,</span></p>

<p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">I
would like to calculate Bader charges in BaTiO3. The input and output files are
uploaded to</span> <span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black"><a href="https://www.mediafire.com/file/o6ceodngk93mh72/aim.rar/file" style="color:blue">https://www.mediafire.com/file/o6ceodngk93mh72/aim.rar/file</a>
for your kind consideration.</span></p>

<p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">I
have run a PBE-GGA calculation using 1000 k-points, RMTKmax =7, Gmax = 12
(Bohr)-1 employing WIIEN2k_21.1 and then executed “x aim” by the third part of
case.inaim from SRC_templates. The calculated charges are:</span></p>

<p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">Ba:
2.91, Ti: 2.68, O: 0.299</span></p>

<p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">The
results cannot satisfy the stoichiometry of the compound because of the
positive charge wrongly calculated for O, i.e., 2.91+2.68+3*0.299=6.487 != 0 </span></p>

<p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">Then,
to improve the results, I increased the LM in the original calculation with no
optimistic effect. </span></p>

<p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">Accidently,
I found that the Bader charges of BaTiO3 can be perfectly improved using “x
aim” of WIIEN2k_18.2 as follows:</span></p>

<p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">Ba:
1.52, Ti: 2.23, O: -1.25</span></p>

<p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">The
above results, as calculated by the older version 18.2, not only give a
negative value for the charge of oxygen but also perfectly lead to zero taking
the stoichiometry of the compound into account, i.e., 1.52+2.23+3*(-1.25) =
0.  </span></p>

<p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">For
sure, I checked the 14 and 16.1 versions of the WIEN2k code and found correct
results the same as WIIEN2k_18.2. This shows that most likely something is
different in the older versions WIIEN2k_18.2, WIIEN2k_16.1, and WIIEN2k_14
compared to the latest version WIIEN2k_21.1?</span></p>

<p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">I
also checked LaCrO3, and found the same dissonancy. The Bader charges were
calculated for LaCrO3 to be La: 2.08, Cr: 1.65, O:  -1.24  in Ref. [Energy Environ. Sci.,
2011, 4, 4933]. These results also correctly lead to zero approximately:
2.08+1.65+3*(-1.24) ~ 0.01. </span></p>

<p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">Would
you, please, have a look at this issue and let us know the source of the above
discrepancy?    </span></p>

<p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">Sincerely
yours,</span></p>

<p class="MsoNormal" style="margin:0cm 0cm 10pt;line-height:115%;font-size:11pt;font-family:Calibri,"sans-serif""><span style="font-size:12pt;line-height:115%;font-family:"Times New Roman","serif";color:black">Leila
Mollabashi</span></p></div>