<div dir="ltr">Hi<div><br></div><div>Looks like you may changed your input from the initial one slightly: the PDOS analysis shows you are running spin polarised calculations (at least for CP2K, as the sum equals to 1; you didn't include UKS or LSD in your initial input). For the analysis on VASP calculation, are these numbers correspond to all the atoms in the cell or just part of it? The sum of the numbers doesn't equal to 1 or 2, so we cannot see what are the real differences.</div><div><br></div><div><br></div><div><span style="font-size:12.8px">"I will also try to do a ternary system like CsPbBr3."</span><br></div><div><span style="font-size:12.8px"><br></span></div><div><span style="font-size:12.8px">From your benchmark data, I would be more worried about In and Ag. I cannot find any ternary halide involving Ag and In, but you can find AgInS2 from ICSD database. I think this may be a better system to test. You may also try CsAgX and CsInX.</span></div><div><span style="font-size:12.8px"><br></span></div><div><span style="font-size:12.8px"><br></span></div><div><span style="font-size:12.8px">"</span><span style="font-size:12.8px">I have another question for Cs2InAgCl6. You are saying that Ag is optimized for +1. What I am going to study is the hole state of Cs2InAgCl6, so one electron will be removed from the system. In that case, Ag will tend to be in 2+ state. Can you comment on the reliability of the PBE0 calculation if I focus on the structure instead of the band gap?"</span></div><div><span style="font-size:12.8px"><br></span></div><div><span style="font-size:12.8px">I think the uncontracted ADMM basis sets (FIT??, not cFIT??) should be flexible enough to describe Ag2+. From your CP2K/PDOS analysis, it looks like there may be a competition in terms of hole localisation, as the HOMO features mixed Ag+ and Cl- states. I am not sure how the smaller band gap in CP2K (compared with your reference) will affect hole localisation in </span><span style="font-size:12.8px">Cs2InAgCl6. Again, I would start from a simpler binary system as a testbed, e.g. AgCl, which I am sure has been studied before, I would use the same PBE0-TC functional, and I would then compare the hole localisation properties (e.g. self-trapping energy, etc) of AgCl with previous literatures. Once I am happy with the results on binary system, I would then feel more comfortable to move to the more complicated ternary and </span><span style="font-size:12.8px">quaternary</span><span style="font-size:12.8px"> systems.</span></div><div><span style="font-size:12.8px"><br></span></div><div><span style="font-size:12.8px">An additional test you can try is to relax the cell paramters and atomic positions of </span><span style="font-size:12.8px">Cs2InAgCl6</span><span style="font-size:12.8px"> in CP2K at PBE0-TC level, and see if that improves the agreement with the experimental value on band gap. I was looking at a JPCL paper (DOI: 10.1021/acs.jpclett.6b02682) on </span><span style="font-size:12.8px">Cs2InAgCl6</span><span style="font-size:12.8px">, and it looks like the authors reported a range (2.9~3.3 eV) of band gap values at PBE0 level for </span><span style="font-size:12.8px">Cs2InAgCl6 with different geometry relaxations. This actually shows the band gap is quite sensitive to small differences in geometries.</span></div><div><span style="font-size:12.8px"><br></span></div><div><span style="font-size:12.8px">It looks like this discussion has become quite technical now. I am happy to continue the discussion offline if you are interested.</span></div><div><span style="font-size:12.8px"><br></span></div><div><span style="font-size:12.8px">SL</span></div><div><span style="font-size:12.8px"><br></span></div><div><br></div></div><div class="gmail_extra"><br><div class="gmail_quote">On 21 September 2017 at 18:48, Xiaoming Wang <span dir="ltr"><<a href="mailto:wxia...@gmail.com" target="_blank">wxia...@gmail.com</a>></span> wrote:<br><blockquote class="gmail_quote" style="margin:0 0 0 .8ex;border-left:1px #ccc solid;padding-left:1ex"><div dir="ltr">Hi,<div><br></div><div>Here is PBE0 PDOS of HOMO and LUMO of Cs2InAgCl6.</div><div><br></div><div><table border="0" cellpadding="0" cellspacing="0" width="448" style="border-collapse:collapse;width:336pt"> <colgroup><col width="56" span="8" style="width:42pt"> </colgroup><tbody><tr height="20" style="height:15.0pt"> <td colspan="2" rowspan="2" height="40" class="m_-832108695443472909oa1" width="112" style="height:30.0pt;width:84pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"></p> </td> <td colspan="3" class="m_-832108695443472909oa1" width="168" style="width:126pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11pt;font-family:Calibri;color:black">CP2K</span></p> </td> <td colspan="3" class="m_-832108695443472909oa1" width="168" style="width:126pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11pt;font-family:Calibri;color:black">VASP</span></p> </td> </tr> <tr height="20" style="height:15.0pt"> <td height="20" class="m_-832108695443472909oa1" width="56" style="height:15.0pt;width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">s</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">p</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">d</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">s</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">p</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">d</span></p> </td> </tr> <tr height="20" style="height:15.0pt"> <td rowspan="4" height="80" class="m_-832108695443472909oa4" width="56" style="height:60.0pt;width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11pt;font-family:Calibri;color:black">HOMO</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">Cs</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> </tr> <tr height="20" style="height:15.0pt"> <td height="20" class="m_-832108695443472909oa1" width="56" style="height:15.0pt;width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">In</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.050</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.030</span></p> </td> </tr> <tr height="20" style="height:15.0pt"> <td height="20" class="m_-832108695443472909oa1" width="56" style="height:15.0pt;width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">Ag</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.454</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.368</span></p> </td> </tr> <tr height="20" style="height:15.0pt"> <td height="20" class="m_-832108695443472909oa1" width="56" style="height:15.0pt;width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">Cl</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.003</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.488</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.004</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.456</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> </tr> <tr height="20" style="height:15.0pt"> <td rowspan="4" height="80" class="m_-832108695443472909oa4" width="56" style="height:60.0pt;width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11pt;font-family:Calibri;color:black">LUMO</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">Cs</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.085</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> </tr> <tr height="20" style="height:15.0pt"> <td height="20" class="m_-832108695443472909oa1" width="56" style="height:15.0pt;width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">In</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.300</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.332</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> </tr> <tr height="20" style="height:15.0pt"> <td height="20" class="m_-832108695443472909oa1" width="56" style="height:15.0pt;width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">Ag</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.241</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.212</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.000</span></p> </td> </tr> <tr height="20" style="height:15.0pt"> <td height="20" class="m_-832108695443472909oa1" width="56" style="height:15.0pt;width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">Cl</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.194</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.074</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.107</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.096</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.048</span></p> </td> <td class="m_-832108695443472909oa1" width="56" style="width:42pt"> <p style="margin-top:0pt;margin-bottom:0pt;margin-left:0in;text-align:center;direction:ltr;unicode-bidi:embed;vertical-align:bottom;word-break:normal"><span style="font-size:11.0pt;font-family:Calibri;color:black">0.024</span></p> </td> </tr> </tbody></table><br></div><div>I will also try to do a ternary system like CsPbBr3.</div><div><br></div><div>I have another question for Cs2InAgCl6. You are saying that Ag is optimized for +1. What I am going to study is the hole state of Cs2InAgCl6, so one electron will be removed from the system. In that case, Ag will tend to be in 2+ state. Can you comment on the reliability of the PBE0 calculation if I focus on the structure instead of the band gap? </div><div><br></div><div>Best,</div><div><span class=""><br><br>On Thursday, September 21, 2017 at 11:10:15 AM UTC-4, S Ling wrote:</span><blockquote class="gmail_quote" style="margin:0;margin-left:0.8ex;border-left:1px #ccc solid;padding-left:1ex"><div dir="ltr">Hi<div><br></div><span class=""><div>I am not sure how you ran the PBE0 calculation without ADMM using the MOLOPT basis sets, which were not designed for hybrid DFT calculations. Hybrid DFT calculations without ADMM for your Cs2InAgCl6 system will use a lot of memory, and as Prof Hutter suggested earlier, it will also be 100~1000 times slower.</div><div><br></div><div>"<span style="font-size:12.8px">without ADMM basis sets I have SCF convergence issue if I don't use the Coulomb truncation method, both for OT and diagonalization, the SCF didn't tend to converge. Why is that?"</span></div><div><span style="font-size:12.8px"><br></span></div><div><span style="font-size:12.8px">Please have a look at the two papers below, which answer your question:</span></div><div><span style="font-size:12.8px"><br></span></div><div><span style="font-size:12.8px"><a href="http://pubs.acs.org/doi/abs/10.1021/ct900494g" rel="nofollow" target="_blank">http://pubs.acs.org/doi/abs/10<wbr>.1021/ct900494g</a></span></div><div><span style="font-size:12.8px"><a href="http://aip.scitation.org/doi/10.1063/1.2931945" rel="nofollow" target="_blank">http://aip.scitation.org/doi/1<wbr>0.1063/1.2931945</a></span><br></div><div><br></div><div>For the PBE0 band gaps calculated using different codes, I can see for binary systems, the differences are at the order of 0.2 eV or smaller, which I think is not something totally unexpected, because of the different HFX implementation strategies, different basis sets and different pseudopotentials used by the two codes. If you try a third code based on atomic orbital basis sets, you may also get different answers. In addition, similar results at PBE level doesn't necessarily mean the numbers at PBE0 level will or should be similar as well. From computational point of view, compounds involving d block elements are usually more difficult to deal with than compounds involving only s and p block elements. As you mentioned earlier, it could simply be the case that the differences in binary systems added up in your quaternary system. It may be useful to check what numbers the two codes will give for the ternary system, before we look at the more complicated quaternary system. The <span style="color:rgb(80,0,80);font-size:12.8px">VASP/PROCAR and CP2K/PDOS analysis will tell us what are the nature of the states at the top of the valence band and at the bottom of the conduction band, which will help us to understand the difference between the two codes.</span></div><div><br></div><div><span style="color:rgb(80,0,80);font-size:12.8px">SL</span></div><div><span style="color:rgb(80,0,80);font-size:12.8px"><br></span></div></span></div><div><div class="h5"><div><br><div class="gmail_quote">On 21 September 2017 at 14:57, Xiaoming Wang <span dir="ltr"><<a rel="nofollow">wxi...@gmail.com</a>></span> wrote:<br><blockquote class="gmail_quote" style="margin:0 0 0 .8ex;border-left:1px #ccc solid;padding-left:1ex"><div dir="ltr">I'd like to add that my PBE0 calculation without ADMM basis sets has been done. I tested 10*10*10 Cs2InAgCl6, which is the system of my original post. The band gap is 2.52 and 2.50 eV for with and without ADMM. So it seems not the ADMM basis problem? <div>I have another question that without ADMM basis sets I have SCF convergence issue if I don't use the Coulomb truncation method, both for OT and diagonalization, the SCF didn't tend to converge. Why is that? (The calculation is fine with TC.)</div><div><br></div><div>Best,<div><div><br><br>On Thursday, September 21, 2017 at 8:54:49 AM UTC-4, Xiaoming Wang wrote:<blockquote class="gmail_quote" style="margin:0;margin-left:0.8ex;border-left:1px #ccc solid;padding-left:1ex"><div dir="ltr">Hi,<div><br></div><div>I am sorry for the confusing formula. It is actually Cs2InAgCl6, in which Ag is +1. When you are fitting the ADMM basis sets, what's the reference system for Ag? Is it in solid environment? Is it possible for me to fit the ADMM basis myself based on my vasp calculations? Well, maybe it is too difficult for me, since I am new to cp2k. Btw, do the ADMM basis sets depend on the oxidation states of the elements involved? If that's the case, there would be problems dealing with different systems with the same basis sets. Moreover, the oxidation state is an arbitrary quantity depending on the charge partition scheme. The oxidation state may be slight different even for the systems which are assumed to be +1 for a particular element, for example.</div><div><br></div><div>Best,</div><div><br></div><div>Xiaoming <br><br>On Thursday, September 21, 2017 at 6:17:45 AM UTC-4, S Ling wrote:<blockquote class="gmail_quote" style="margin:0;margin-left:0.8ex;border-left:1px #ccc solid;padding-left:1ex"><div dir="ltr">Hi<div><br></div><div>Can you confirm the chemical formula of your CsInAgCl system? I looked through the ICSD database, and the only related compound which I can find is CsAgInF6, in which Ag is in an uncommon +2 oxidation state (in your benchmark test, you looked at AgCl, in which Ag is in the common +1 oxidation state). If this is the case for CsInAgCl6, there is a possibility that your CP2K/PBE0 and VASP/PBE0 calculations may have converged to slightly different SCF solutions. You can check this by comparing the orbital occupation numbers from your VASP/PROCAR and from the CP2K/PDOS analysis. Another possibility is that the ADMM basis sets are indeed not good enough to describe Ag2+ (I have only considered Ag+ when I was fitting the ADMM basis sets of Ag).</div><div><br></div><div>SL</div><div><br></div><div> </div></div><div><br><div class="gmail_quote">On 21 September 2017 at 03:52, Xiaoming Wang <span dir="ltr"><<a rel="nofollow">wxi...@gmail.com</a>></span> wrote:<br><blockquote class="gmail_quote" style="margin:0 0 0 .8ex;border-left:1px #ccc solid;padding-left:1ex"><div dir="ltr"><p style="text-align:left;clear:both">Hi, Can you see it this time?</p><p style="text-align:center;clear:both"><a href="https://lh3.googleusercontent.com/-f1GOmo2FRic/WcMpJhTURnI/AAAAAAAAGcU/MqO1xDMjsmQIV1PsgFDq5Aq_IqaPdz-CQCLcBGAs/s1600/benchmark.PNG" style="margin-left:1em;margin-right:1em" rel="nofollow" target="_blank"><img src="https://lh3.googleusercontent.com/-f1GOmo2FRic/WcMpJhTURnI/AAAAAAAAGcU/MqO1xDMjsmQIV1PsgFDq5Aq_IqaPdz-CQCLcBGAs/s320/benchmark.PNG" border="0" width="320" height="186"></a></p><div><div><br><br>On Wednesday, September 20, 2017 at 10:45:10 PM UTC-4, Matt W wrote:<blockquote class="gmail_quote" style="margin:0;margin-left:0.8ex;border-left:1px #ccc solid;padding-left:1ex"><div dir="ltr">Hi,<div><br></div><div>I only see the check for InCl3, not the main system?</div><div><br></div><div>Matt</div><div><br>On Thursday, September 21, 2017 at 10:36:15 AM UTC+8, Xiaoming Wang wrote:<blockquote class="gmail_quote" style="margin:0;margin-left:0.8ex;border-left:1px #ccc solid;padding-left:1ex"><div dir="ltr">Hi Matt,<div><br></div><div>Actually I also did the calculation for a supercell of 21*21*21 with 320 atoms. PBE0 without TC are also tested, please see my benchmark tests in previous post (attachment in reply to Ling).</div><div><br></div><div>Best,</div><div>Xiaoming<br><br><br>On Wednesday, September 20, 2017 at 10:27:48 PM UTC-4, Matt W wrote:<blockquote class="gmail_quote" style="margin:0;margin-left:0.8ex;border-left:1px #ccc solid;padding-left:1ex"><div dir="ltr">That ADMM basis is already pretty large, so whilst it might be the problem, first I'd check the cell size.<div><br></div><div>Can you build a cell about 15 x 15 x 15 A or larger to allow you to extend the range of the hybrid out to 6 or 7 A?</div><div><br></div><div>You are truncating at about 5.25 A, which might not be enough to be fully converged (note VASP won't be doing this as it works in K space). </div><div><br></div><div>Matt </div><br>On Thursday, September 21, 2017 at 8:36:29 AM UTC+8, Xiaoming Wang wrote:<blockquote class="gmail_quote" style="margin:0;margin-left:0.8ex;border-left:1px #ccc solid;padding-left:1ex"><div dir="ltr">Hi Ling,<div><br></div><div>Thanks for your comments. I have attached my benchmark results here. Based on my tests, it seems that the ADMM basis set size is not so important for ionic crystals. One can get reasonable results even with smallest basis sets. Btw, the cutoff and rel_cutoff used are well converged values for my target property. So I think there is still room to improve the ADMM basis for Ag and In (with semicore d states in the valence). To check whether it is the problem of Ag and In ADMM basis, the simplest way is to do the PBE0 calculations without ADMM. But the calculation takes me too long time, as also pointed out by Juerg. I suspect if it is possible to do HFX without ADMM using MOLOPT basis sets.</div><div><br></div><div><br></div><div><br></div><div><br></div><div><br></div><div>Best,</div><div>Xiaoming<br><br>On Wednesday, September 20, 2017 at 6:20:09 AM UTC-4, S Ling wrote:<blockquote class="gmail_quote" style="margin:0;margin-left:0.8ex;border-left:1px #ccc solid;padding-left:1ex"><div dir="ltr">Hi<div><br></div><div>I am not sure whether you are using the same ADMM basis sets (see your initial input) for these new test calculations. One thing which I can see is that you are not using the largest available ADMM basis sets for some of the elements, e.g. the largest available ADMM basis sets for Cl, Ag and In are pFIT3, FIT12 and FIT13, respectively. Taking In as an example, the FIT13 ADMM basis set of In contains more p and d functions than FIT11, which may be important for your system. </div><div><br></div><div>You mentioned a few different functionals, including PBE, PBE0 and HSE06, and you have run quite a lot of benchmark tests. It would help if you can tabulate all the numbers you have got (including the reference), so we can understand your problem better.</div><div><br></div><div>In addition, I can see you're using a CUTOFF of 250 Ry. Please also check whether your calculation is converged with respect to this parameter.</div><div><br></div><div>Please also keep in mind that CP2K and VASP use different pseudopotentials and basis sets. I wouldn't expect the two codes to give the same numbers for your target properties. If you look into literatures, you will also find people reporting different numbers for the same property using the same method and code.</div><div><br></div><div>SL</div><div> </div><div><br></div></div> </blockquote></div></div></blockquote></div></blockquote></div></div></blockquote></div></div></blockquote></div></div></div><div><div> <p></p> -- <br> You received this message because you are subscribed to the Google Groups "cp2k" group.<br> To unsubscribe from this group and stop receiving emails from it, send an email to <a rel="nofollow">cp2k+...@googlegroups.com</a>.<br> To post to this group, send email to <a rel="nofollow">cp...@googlegroups.com</a>.<br> Visit this group at <a href="https://groups.google.com/group/cp2k" rel="nofollow" target="_blank">https://groups.google.com/grou<wbr>p/cp2k</a>.<br> For more options, visit <a href="https://groups.google.com/d/optout" rel="nofollow" target="_blank">https://groups.google.com/d/op<wbr>tout</a>.<br> </div></div></blockquote></div><br></div> </blockquote></div></div></blockquote></div></div></div></div><div><div> <p></p> -- <br> You received this message because you are subscribed to the Google Groups "cp2k" group.<br> To unsubscribe from this group and stop receiving emails from it, send an email to <a rel="nofollow">cp2k+...@googlegroups.com</a>.<br> To post to this group, send email to <a rel="nofollow">cp...@googlegroups.com</a>.<br> Visit this group at <a href="https://groups.google.com/group/cp2k" rel="nofollow" target="_blank">https://groups.google.com/grou<wbr>p/cp2k</a>.<br> For more options, visit <a href="https://groups.google.com/d/optout" rel="nofollow" target="_blank">https://groups.google.com/d/op<wbr>tout</a>.<br> </div></div></blockquote></div><br></div> </div></div></blockquote></div></div><div class="HOEnZb"><div class="h5"> <p></p> -- <br> You received this message because you are subscribed to the Google Groups "cp2k" group.<br> To unsubscribe from this group and stop receiving emails from it, send an email to <a href="mailto:cp2k+uns...@googlegroups.com" target="_blank">cp2k+unsubscribe@googlegroups.<wbr>com</a>.<br> To post to this group, send email to <a href="mailto:cp...@googlegroups.com" target="_blank">cp...@googlegroups.com</a>.<br> Visit this group at <a href="https://groups.google.com/group/cp2k" target="_blank">https://groups.google.com/<wbr>group/cp2k</a>.<br> For more options, visit <a href="https://groups.google.com/d/optout" target="_blank">https://groups.google.com/d/<wbr>optout</a>.<br> </div></div></blockquote></div><br></div>