[Wien] why artificial lowering of symmetry changes the total energy?

katrusiat katrusiat at yandex.ru
Wed Apr 16 15:24:14 CEST 2008


Dear Stefaan,

To be exact, I have never calculated the high-symmetry case, but only the cases with a symmetry reduced in different ways, that is, picking up Cu pairs in a different way. 

For example, the high-symmetry (62_Pnma) unit cell can be reduced into:

{1} - (26 Pmc21)
or
{2} - (11 P21/m).

The total FM energy of {1} is -152655.214439 Ry
           and that of {2} is -152655.214842 Ry

The precision of both calculations was 0.000001 Ry since all the figures after the point are important for me.

I am including the case.dmatdn files of both cases. There are differences between the density matrices of {1} and {2}, but I do not know what they mean physically.

{1}.dmatdn:
 5 atom density matrix
    2  0.000000  0.000000  0.000000 L, Lx,Ly,Lz in global orthogonal system
  0.88397491E+00  0.45772788E-17   -0.30112862E-16  0.33756139E-17
 -0.56905374E-01 -0.15502970E+00   -0.43813795E-16 -0.73875955E-17
  0.52324299E-01 -0.44662464E-01
 -0.30185041E-16 -0.14924055E-16    0.95408779E+00  0.18112910E-21
  0.47708400E-16 -0.13402175E-15    0.28855650E-03  0.50914101E-03
  0.43087170E-16  0.15093138E-16
 -0.56905374E-01  0.15502970E+00    0.45714984E-16  0.17002143E-15
  0.52349246E+00 -0.27031453E-32   -0.48102197E-16  0.16346734E-15
 -0.56905374E-01 -0.15502970E+00
 -0.41193459E-16  0.59607913E-17    0.28855650E-03 -0.50914101E-03
 -0.47367892E-16 -0.13707573E-15    0.95408779E+00 -0.18112910E-21
  0.26808369E-16 -0.10963618E-16
  0.52324299E-01  0.44662464E-01    0.43516606E-16  0.90640477E-18
 -0.56905374E-01  0.15502970E+00    0.29642355E-16  0.51200139E-17
  0.88397491E+00 -0.65160781E-17
   12 atom density matrix
    2  0.000000  0.000000  0.000000 L, Lx,Ly,Lz in global orthogonal system
  0.88397855E+00  0.59494382E-17   -0.29332059E-16  0.15369247E-17
 -0.56903686E-01 -0.15502442E+00   -0.43751283E-16 -0.44684061E-17
  0.52322421E-01 -0.44661108E-01
 -0.29778323E-16 -0.21703198E-16    0.95408899E+00  0.18112910E-21
  0.48457200E-16 -0.14148853E-15    0.28854483E-03  0.50909782E-03
  0.45130372E-16  0.44197062E-17
 -0.56903686E-01  0.15502442E+00    0.45677459E-16  0.17463781E-15
  0.52350765E+00 -0.18439027E-32   -0.48146709E-16  0.17406951E-15
 -0.56903686E-01 -0.15502442E+00
 -0.41648997E-16  0.98869904E-17    0.28854483E-03 -0.50909782E-03
 -0.51275854E-16 -0.14339813E-15    0.95408899E+00 -0.18112910E-21
  0.29503689E-16 -0.20466146E-16
  0.52322421E-01  0.44661108E-01    0.44185682E-16  0.13095126E-17
 -0.56903686E-01  0.15502442E+00    0.30179069E-16 -0.14347071E-16
  0.88397855E+00 -0.56814652E-17

and 

{2}.dmatdn:
   5 atom density matrix
    2  0.000000  0.000000  0.000000 L, Lx,Ly,Lz in global orthogonal system
  0.88622892E+00  0.00000000E+00   -0.14182705E-12 -0.19969227E-12
 -0.56403834E-01  0.15378237E+00    0.63378789E-12 -0.24981983E-12
  0.50668787E-01  0.43222111E-01
 -0.14182705E-12  0.19969227E-12    0.95421135E+00  0.00000000E+00
 -0.33383734E-12 -0.44952174E-12    0.27467590E-03 -0.48623493E-03
 -0.63378789E-12  0.24981983E-12
 -0.56403834E-01 -0.15378237E+00   -0.33383734E-12  0.44952174E-12
  0.51579922E+00  0.00000000E+00    0.33383734E-12  0.44952174E-12
 -0.56403834E-01  0.15378237E+00
  0.63378789E-12  0.24981983E-12    0.27467590E-03  0.48623493E-03
  0.33383734E-12 -0.44952174E-12    0.95421135E+00  0.00000000E+00
  0.14182705E-12  0.19969227E-12
  0.50668787E-01 -0.43222111E-01   -0.63378789E-12 -0.24981983E-12
 -0.56403834E-01 -0.15378237E+00    0.14182705E-12 -0.19969227E-12
  0.88622892E+00  0.00000000E+00
   12 atom density matrix
    2  0.000000  0.000000  0.000000 L, Lx,Ly,Lz in global orthogonal system
  0.88622701E+00  0.00000000E+00    0.54373017E-13 -0.18285763E-13
 -0.56343328E-01 -0.15380725E+00   -0.14830471E-12  0.10198634E-12
  0.50701253E-01 -0.43187447E-01
  0.54373017E-13  0.18285763E-13    0.95421141E+00  0.00000000E+00
 -0.97651269E-14 -0.18678439E-12    0.27045235E-03  0.48783445E-03
  0.14830471E-12 -0.10198634E-12
 -0.56343328E-01  0.15380725E+00   -0.97651269E-14  0.18678439E-12
  0.51580042E+00  0.00000000E+00    0.97651269E-14  0.18678439E-12
 -0.56343328E-01 -0.15380725E+00
 -0.14830471E-12 -0.10198634E-12    0.27045235E-03 -0.48783445E-03
  0.97651269E-14 -0.18678439E-12    0.95421141E+00  0.00000000E+00
 -0.54373017E-13  0.18285763E-13
  0.50701253E-01  0.43187447E-01    0.14830471E-12  0.10198634E-12
 -0.56343328E-01  0.15380725E+00   -0.54373017E-13 -0.18285763E-13
  0.88622701E+00  0.00000000E+00

Thanks for help,
Kateryna



_______________________________________________________


1) How large is your energy change? Perhaps it is just numerical noise?

2) If the change is large enough, and if it is a lowering of the  
energy upon symmetry reduction, you might have an onset of orbital  
ordering. Inspect the density matrices of the two inequivalent  
Cu-sites (dmat files), and see whether they are different from each  
other and/or different from the density matrix for the high-symmetry  
case. If there are differences, then this material apparently can  
lower its total energy by occupying the Cu-d orbitals in different  
ways in the two Cu-sites.

Stefaan


Quoting katrusiat <katrusiat at yandex.ru>:

> Dear all,
>
> I perform ferromagnetic (FM) (I make it FM by modifying the   
> case.inst file accordingly) GGA+U calculations of the total energy   
> of Cs2CuCl4, the compound with 4 equivalent magnetic Cu's in a unit   
> cell. When I create an artificial unit cell of a lower symmetry with  
>  2 inequivalent pairs of Cu's: Cu1 and Cu2, and again perform a FM   
> GGA+U calculation, the total energy of the system is slightly   
> different.
>
> By lowering the symmetry I only add labels to Cu's making them   
> inequivalent, and also the crystallographic axes are interchanged in  
>  the new unit cell. So, why after these seemingly harmless actions   
> the total energy should change?
>
> Thank you,
> Kateryna Foyevtsova





--
Яндекс.Почта. Чище не бывает http://mail.yandex.ru/nospam   Я





_______________________________________________________


1) How large is your energy change? Perhaps it is just numerical noise?

2) If the change is large enough, and if it is a lowering of the  
energy upon symmetry reduction, you might have an onset of orbital  
ordering. Inspect the density matrices of the two inequivalent  
Cu-sites (dmat files), and see whether they are different from each  
other and/or different from the density matrix for the high-symmetry  
case. If there are differences, then this material apparently can  
lower its total energy by occupying the Cu-d orbitals in different  
ways in the two Cu-sites.

Stefaan


Quoting katrusiat <katrusiat at yandex.ru>:

> Dear all,
>
> I perform ferromagnetic (FM) (I make it FM by modifying the   
> case.inst file accordingly) GGA+U calculations of the total energy   
> of Cs2CuCl4, the compound with 4 equivalent magnetic Cu's in a unit   
> cell. When I create an artificial unit cell of a lower symmetry with  
>  2 inequivalent pairs of Cu's: Cu1 and Cu2, and again perform a FM   
> GGA+U calculation, the total energy of the system is slightly   
> different.
>
> By lowering the symmetry I only add labels to Cu's making them   
> inequivalent, and also the crystallographic axes are interchanged in  
>  the new unit cell. So, why after these seemingly harmless actions   
> the total energy should change?
>
> Thank you,
> Kateryna Foyevtsova





--
Яндекс.Почта. Чище не бывает http://mail.yandex.ru/nospam   Я





_______________________________________________________


1) How large is your energy change? Perhaps it is just numerical noise?

2) If the change is large enough, and if it is a lowering of the  
energy upon symmetry reduction, you might have an onset of orbital  
ordering. Inspect the density matrices of the two inequivalent  
Cu-sites (dmat files), and see whether they are different from each  
other and/or different from the density matrix for the high-symmetry  
case. If there are differences, then this material apparently can  
lower its total energy by occupying the Cu-d orbitals in different  
ways in the two Cu-sites.

Stefaan


Quoting katrusiat <katrusiat at yandex.ru>:

> Dear all,
>
> I perform ferromagnetic (FM) (I make it FM by modifying the   
> case.inst file accordingly) GGA+U calculations of the total energy   
> of Cs2CuCl4, the compound with 4 equivalent magnetic Cu's in a unit   
> cell. When I create an artificial unit cell of a lower symmetry with  
>  2 inequivalent pairs of Cu's: Cu1 and Cu2, and again perform a FM   
> GGA+U calculation, the total energy of the system is slightly   
> different.
>
> By lowering the symmetry I only add labels to Cu's making them   
> inequivalent, and also the crystallographic axes are interchanged in  
>  the new unit cell. So, why after these seemingly harmless actions   
> the total energy should change?
>
> Thank you,
> Kateryna Foyevtsova






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