[Wien] regarding exciton binding energies and dielectric constant [updated]

Peter Blaha pblaha at theochem.tuwien.ac.at
Thu Nov 10 18:05:57 CET 2016


Why would you do a runsp_lapw for a non-magnetic system ???

Spin-orbit is also active for a non-magnetic material.

Don't mix up  spin-polarization with spin-orbit ....

PS: I'm also not sure why you want to include the Pb-5p state as valence 
?? I don't think you have to use so small Pb spheres that you get core 
leakage ?? And with Pb-5p as core you have the full SO-splitting 
inluded, ....



> D.
>
> 1. initso_lapw
> 2. runsp_lapw -so -p -i 40 -ec 0.0001 -cc 0.0001'   Fine ????
>
> I am using both step C and D differently because Dr. Tran suggested for
> the same
> (http://www.mail-archive.com/wien@zeus.theochem.tuwien.ac.at/msg03843.html)
>
>
> One more question:
> how iqtlsave will change the calculation if I coose it as "0"?
>
> Kind regards
>
>
>
> ------------------------------------------------
> Dr. K. C. Bhamu
> (UGC-Dr. D. S. Kothari Postdoc Fellow)
> Department of Physics
> Goa University, Goa-403 206
> India
> Mob. No.  +91-9975238952
>
> On Thu, Nov 10, 2016 at 8:00 PM, Peter Blaha
> <pblaha at theochem.tuwien.ac.at <mailto:pblaha at theochem.tuwien.ac.at>> wrote:
>
>     Very good explanation.
>
>     So you should probably use SO + mBJ and see what comes out then ....
>     (you should get again a good band gap, although effective masses are
>     not necessarily improved by mBJ ...)
>
>     Am 10.11.2016 um 15:24 schrieb John McLeod:
>
>         I have some experience using WIEN2k for metal organic halide
>         perovskites.
>
>         PBE without SOC gets the correct band gap for CH3NH3PbI3 (which
>         I assume
>         is the compound Dr. Bhamu is studying) because of a "fortuitous"
>         error
>         cancellation between using PBE and ignoring SOC. This is
>         reasonably well
>         known and has been studied in detail in several manuscripts. SOC+PBE
>         results in a significantly underestimated band gap, as one might
>         expect.
>
>         I assume Dr. Bhamu is using the calculated low frequency dielectric
>         constant (e*), and the calculated effective mass (m*) to
>         estimate the
>         binding energy using the simple Mott-Wannier model: E_ex =
>         m*/e^2 (13.6)
>         eV .
>
>         SOC does modify the shape of the bands near the gamma-point (I
>         believe
>         it reduces the effective mass), and SOC also influences the
>         dielectric
>         constant. So I think perhaps including SOC and using a scissors
>         operation with OPTIC to get the correct band gap may be the most
>         straight-forward (if not completely ab initio) method.
>
>         Have you looked at F. Brivio, et al., Phys. Rev. B 89 155204 (DOI:
>         10.1103/PhysRevB.89.155204)?
>         They go into some detail about different approaches, it may be
>         helpful
>         for your present situation.
>
>         Regards,
>         -John McLeod
>
>         So I do not think SOC can be
>         On 2016-11-10 10:02 PM, Peter Blaha wrote:
>
>             I'm not the expert on that topic, but I think you mix up the two
>             dielectric constants, which could be a semantic problem. To
>             compare
>             with a classic experiment, you may need to obtain the ionic
>             contribution to the dielectric constant, which as far as I
>             know can be
>             done using BERRYPI.
>
>             Other comments:
>             To obtain the "correct" band gap using PBE is very
>             "unusual". For most
>             materials (but of course there could be exemptions) the PBE
>             band gaps
>             should be ~50%  smaller than experiment.
>
>             Pb ??? this is very "relativistic" ! Did you consider spin-orbit
>             coupling ?
>
>             And last but not least, I have no idea how you calculate exciton
>             binding energies from a single particle spectrum. We would
>             do this
>             using BSE calculations, but your system is probably too
>             complicated
>             for this.
>
>             Am 10.11.2016 um 14:26 schrieb Dr. K. C. Bhamu:
>
>                 Dear Prof. Peter and Experts
>                 This is with some more information:
>
>                 To put a joint paper on complex Metal-organic halide
>                 perovskites, I am
>                 trying to reproduce some experimental results measured by my
>                 collaborator.
>
>                 For my complex system, I got low frequency dielectric
>                 constant value of
>                 ~5.6 (at 0.013 eV) and the calculated the exciton
>                 binding energy  ~0.087
>                 - 0.095 eV  (85 -97 meV). This is too high because the
>                 measurements here
>                 get about 13 meV and a 1-2 transition of ~9.9 meV
>                 (measured).
>
>                 In literature the reported static and optical dielectric
>                 constants for
>                 the system are in the range of 17-24 and 4.5-6.5
>                 respectively using DFT.
>
>                 In my case the zero frequency dielectric constant (~
>                 5.6) is in tune
>                 with the optical dielectric constants (4.5-6.5).
>
>                 I think my value ~5.6 should be in the range of 17-24.
>                 *Is it so?*
>                 Please help me to understand it.
>
>                 I used PBE functional with 4x4x4 k mesh. I reduced rmt
>                 by 5% and then
>                 rmt for Pb and I were reduced by a factor of 0.3. I have
>                 doubt here??
>
>                  My band gap is in reasonable agreement with the
>                 experimentally observed
>                 band gap (1.57eV) +/- 0.1.
>
>                 The problem may be that my epsilon value (~5.6) is too
>                 low and I looked
>                 up our local measured value of ~18 for the low frequency
>                 part. If I use
>                 this value (18) then much better exciton binding
>                 energies come out.
>
>                 What can be an mistake that I may did in calculation? or
>                 may it be a
>                 reason of the device fabrication because for
>                 experimental part some
>                 p-i-n and n-i-p type device has been framed?
>
>
>                 Kind regards
>
>                 Bhamu
>
>
>
>
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