Dear Marcos,
I am not sure if I understood you correctly, but I checked my calculation
with graphene (with options that you indicated) and I did not get any
changes. The convergence is still reached very fast and the final Pressure
is 0.4 GPa. Just to be on save side, I would like you to glance at my
input file that I used, perhaps, there is something wrong with that how I
handled with these options.
But anyway, granting that you are correct (and I missed again something
important), what does all this prove? The fact that I have to include
relaxation as conditio sine qua non? And without relaxation all previous
results are not reliable? But I am quite surprised why this relaxation is
so important if I started from (more or less) the equilibrium geometry (I
know about it beforehand). Moreover, my questions about the role of
k-point sampling in case of GNribbons are still open.
Here is my input file:

NumberOfAtoms       2
NumberOfSpecies     1

%block ChemicalSpeciesLabel
 1  6  C      # Species index, atomic number, species label
%endblock ChemicalSpeciesLabel
Meshcutoff     800.00 Ry
LongOutput T
WriteDenchar T
AtomicCoordinatesFormat  Ang
%block AtomicCoordinatesAndAtomicSpecies
  0.000   0.000         0.000   1
  1.42    0.00          0.000   1

%endblock AtomicCoordinatesAndAtomicSpecies

%block PAO.BasisSizes
   C     DZP
%endblock PAO.BasisSizes

LatticeConstant  2.459512147  Ang
%block LatticeVectors
  0.866025403  0.5 0.0
  0.866025403 -0.5 0.0
  0.0          0.0 60.0

%endblock LatticeVectors

%block BandLines
1    0.0  -1.33333333   0.0
30   0.0   0.0  0.0
30   0.577350269   1.0  0.0
20   0.0   1.33333333   0.0
%endblock BandLines

MD.VariableCell .true.
MD.TypeOfRun CG
MD.NumCGsteps 50
MD.TargetStressTol 0.01 GPa
MD.TargetPressure  0.01 GPa

Yours respectfully,
Artem Baskin
PhD student,
University of Illinois at Chicago


On Thu, April 29, 2010 6:05 pm, Marcos Veríssimo Alves wrote:
> Artem,
>
> For a moment I thought I was completely hallucinating about my previous
> experience with graphene :) but then I remembered that if you don't set a
> variable explicitly in the input, the default values are used. I have just
> run a variable-cell calculation for graphene using your input and, indeed,
> if you don't set the target pressure, Siesta's default - 1 GPa, which is
> huge!!! - is too high, since the final pressure is 0.4 GPa, which is still
> too high. I set MD.TargetPressure and MD.TargetStressTol to 0.01 GPa and
> the
> lattice parameter comes out extremely bad - check it out. Actually, what I
> see is that, at some point, the c-axis length starts to diminish
> enormously
> (surely a spurious effect) and I didn't even bother letting the
> calculation
> finish. I think now this should prove my points.
>
> Marcos
>
> On Thu, Apr 29, 2010 at 11:49 PM, Artem Baskin <[email protected]> wrote:
>
>> Dear Marcos,
>>
>> Thank you once again.
>> I recalculated the same jobs (systems) with MD relaxation parameters:
>> MD.TypeOfRun CG
>> MD.NumCGsteps 50
>> to compare the results. The results are the same no matter with or
>> without
>> relaxation steps (no changing in structural parameters at the end of
>> calculations compared to the initial ones). As to forces and stresses,
>> they were (and are) much below their respective tolerances. So the
>> convergence is reached very fast (within 17 - 22 SCF iterations).
>>
>> I was looking for answers to my questions in the SIESTA archive but
>> still
>> I am stuck at the same. I still need some help. Could you push me to the
>> right direction?
>>
>> Thanks a lot,
>>
>> Artem Baskin,
>> PhD student,
>> University of Illinois at Chicago
>>
>>
>> On Wed, April 28, 2010 2:25 am, Marcos Veríssimo Alves wrote:
>> > Artem,
>> >
>> > Before proceeding to any other discussion: if this is indeed the
>> complete
>> > input, then the results will be the same, since you don't specify the
>> > number
>> > of relaxation steps; Siesta uses the default value, which is zero. So
>> > nothing is moved, and all results are identical in what regards the
>> > positions of the atoms and that of the Fermi level. However, how do
>> the
>> > forces and cell stresses look in each of the cases? Can you confirm
>> that
>> > Siesta is indeed performing a non-zero number of CG steps and that, by
>> the
>> > end of your calculation, all forces and stresses are below their
>> > respective
>> > tolerances?
>> >
>> > Marcos
>> >
>> > On Wed, Apr 28, 2010 at 3:46 AM, Artem Baskin <[email protected]> wrote:
>> >
>> >> Dear Marcos,
>> >>
>> >> Thank you for your elucidative response. I learned a lot. I also
>> >> apologize
>> >> for my not well defined questions and for that I did not provide my
>> >> input
>> >> file for graphene.
>> >> Here it is. (that one that used initially)
>> >>
>> >> NumberOfAtoms       2
>> >> NumberOfSpecies     1
>> >>
>> >> %block ChemicalSpeciesLabel
>> >>  1  6  C      # Species index, atomic number, species label
>> >> %endblock ChemicalSpeciesLabel
>> >> Meshcutoff     800.00 Ry
>> >> LongOutput T
>> >> WriteDenchar T
>> >> AtomicCoordinatesFormat  Ang
>> >> %block AtomicCoordinatesAndAtomicSpecies
>> >>  0.000   0.000         0.000   1
>> >>  1.42    0.00          0.000   1
>> >>
>> >> %endblock AtomicCoordinatesAndAtomicSpecies
>> >>
>> >> %block PAO.BasisSizes
>> >>   C     DZP
>> >> %endblock PAO.BasisSizes
>> >>
>> >> LatticeConstant  2.459512147  Ang
>> >> %block LatticeVectors
>> >>  0.866025403  0.5 0.0
>> >>  0.866025403 -0.5 0.0
>> >>  0.0          0.0 60.0
>> >>
>> >> %endblock LatticeVectors
>> >>
>> >> %block BandLines
>> >> 1    0.0  -1.33333333   0.0
>> >> 30   0.0   0.0          0.0
>> >> 30   0.577350269   1.0  0.0
>> >> 20   0.0   1.33333333   0.0
>> >> %endblock BandLines
>> >>
>> >> I did what you suggested. I used the the content of STRUCT_NEXT_ITER
>> >> files
>> >>  to see the difference in structural parameters and here they are :
>> >> ----------------------------------------------------------------
>> >> 1) MD.VariableCell   .false.; no k-point sampling; Meshcutoff=800 Ry
>> >>
>> >>         2.129999998       1.229756074       0.000000000
>> >>         2.129999998      -1.229756074       0.000000000
>> >>         0.000000000       0.000000000     147.570728820
>> >>           2
>> >>  1     6       0.000000000      -0.000000001       0.000000000
>> >>  1     6       0.333333333       0.333333334       0.000000000
>> >>
>> >> FE=2.916573
>> >> -----------------------------------------------------------------
>> >> 2) MD.VariableCell   .true.; no k-point sampling; Meshcutoff=800 Ry
>> >>
>> >>          2.129999998       1.229756074       0.000000000
>> >>          2.129999998      -1.229756074       0.000000000
>> >>          0.000000000       0.000000000     147.570728820
>> >>           2
>> >>  1     6       0.000000000      -0.000000001       0.000000000
>> >>  1     6       0.333333333       0.333333334       0.000000000
>> >> FE=2.916573
>> >> -------------------------------------------------------------------
>> >> 3) MD.VariableCell   .true.;k-point sampling:
>> >> %block kgrid_Monkhorst_Pack
>> >> 21   0   0    0.0
>> >>  0  21   0    0.0
>> >>  0   0   1    0.0
>> >> %endblock kgrid_Monkhorst_Pack ; Meshcutoff=800 Ry
>> >>          2.129999998       1.229756074       0.000000000
>> >>          2.129999998      -1.229756074       0.000000000
>> >>          0.000000000       0.000000000     147.570728820
>> >>           2
>> >>  1     6       0.000000001      -0.000000001       0.000000000
>> >>  1     6       0.333333334       0.333333335       0.000000000
>> >>  FE=-3.788733
>> >> -------------------------------------------------------------------
>> >> 4) MD.VariableCell   .true.;k-point sampling:
>> >> %block kgrid_Monkhorst_Pack
>> >>  6   0   0    0.0
>> >>  0   6   0    0.0
>> >>  0   0   1    0.0
>> >> %endblock kgrid_Monkhorst_Pack ; Meshcutoff=800 Ry
>> >>          2.129999998       1.229756074       0.000000000
>> >>          2.129999998      -1.229756074       0.000000000
>> >>          0.000000000       0.000000000     147.570728820
>> >>           2
>> >>  1     6       0.000000001       0.000000000       0.000000000
>> >>  1     6       0.333333334       0.333333335       0.000000000
>> >> FE=-3.785969
>> >>
>> >> Is it that info that you asked for? So, if it is that, you may easily
>> >> see
>> >> that there is no difference in cell vectors and atomic positions
>> >> regardless of the presence of the options you indicated. The only
>> >> significant difference is the Fermi Level (as it is expected). It is
>> >> also
>> >> interesting that the band structure looks very similarly in all these
>> >> cases but the crossing points (at the K-points) are shifted and do
>> not
>> >> tally with the calculated level of FE (in case without k-point
>> >> sampling).
>> >> The fact that there is no difference in structure parameters may be
>> the
>> >> simple consequence of that I used the initial geometry very closed to
>> >> equilibrium one. Is it so?
>> >>
>> >> Now I have more questions.
>> >> 1) Why do you want to compare these results? Are they indicative for
>> >> what?
>> >> 2) How to specify (what reasons or ideas to follow) the k-point
>> sampling
>> >> in case of GNRs?
>> >> 3) Why I got the more or less correct band structure (merely shifted
>> >> with
>> >> respect to correct FE) for Zigzag NR without sampling and can not get
>> >> the
>> >> same WITH k-point sampling along that ribbon?
>> >> 4) Why I could not get the more or less reasoning BS for Armchair NR
>> >> until
>> >> I used
>> >> %block kgrid_Monkhorst_Pack
>> >>  45  0   0    0.0
>> >>  0   1   0    0.0
>> >>  0   0   1    0.0
>> >> %endblock kgrid_Monkhorst_Pack ?
>> >> 5) How does k-point sampling influence the convergence of SCF loop?
>> >> 6) Why the doubling of unit cell for Armchair NR (with the same or
>> >> larger
>> >> k-point sampling along the ribbon) does not lead to convergence and
>> any
>> >> reasonable results?
>> >> 7) What should I do now to circumvent all these hurdles?
>> >>
>> >> I'm looking forward for you instructive (enlightening) advice.
>> >>
>> >> Artem Baskin,
>> >> PhD student,
>> >> University of Illinois at Chicago
>> >>
>> >>
>> >>
>> >>
>> >>
>> >>
>> >>
>> >>
>> >> On Thu, April 22, 2010 7:35 pm, Marcos Veríssimo Alves wrote:
>> >> > Artem,
>> >> >
>> >> > Let's go step by step. The fact that you get "good" results with
>> >> graphene
>> >> > only at the Gamma point seems extremely strange (weird might not
>> sound
>> >> so
>> >> > good, I acknowledge that) for the following.
>> >> >
>> >> > Graphene has an extremely small Fermi surface - actually, a
>> *single*
>> >> > k-point,
>> >> > which is located at the high-symmetry point K of the Brillouin
>> zone.
>> >> To
>> >> > accurately sum over the bands of graphene, you need a specific
>> k-point
>> >> > sampling, which includes the coordinates of K in reciprocal space,
>> as
>> >> well
>> >> > as a pretty dense k-point mesh in order to get the (linear, in the
>> >> > vicinity
>> >> > of K) dispersion of the bands in this region.
>> >> >
>> >> > Why is this important? Well, due to symmetry reasons, the Fermi
>> level
>> >> lies
>> >> > *
>> >> > exactly* at this point. Thus, it is important to accurately sample
>> the
>> >> > region of the BZ close to K, both including this particular point
>> in
>> >> your
>> >> > sampling, *and* including enough k-points in order to accurately
>> sum
>> >> over
>> >> > the occupied states and get a good total energy, which is the
>> >> variational
>> >> > quantity in DFT. Andf, as you may easily realize, Gamma-only
>> sampling
>> >> is
>> >> > not
>> >> > enough for that.
>> >> >
>> >> > You do not provide enough details on your graphene calculation,
>> >> therefore
>> >> > I
>> >> > cannot know what you have done (this is the reason we always ask
>> for
>> >> the
>> >> > input files. Repetitive? Yes, but... an image is worth a thousand
>> >> words,
>> >> > if
>> >> > you catch my drift). So, I propose the following test for you, in
>> your
>> >> > graphene unit cell with two atoms. Start from ideal positions
>> ((0,0,0)
>> >> ;
>> >> > (0.3333333333,0.3333333333,0.3333333333) in fractional coordinates)
>> >> for
>> >> > the
>> >> > C atoms, and the following cell:
>> >> >
>> >> > LatticeConstant     2.44  Ang
>> >> > %block LatticeParameters
>> >> > 1.00  1.00   10.0   90.0  90.0   60.0
>> >> > %endblock LatticeParameters
>> >> >
>> >> > (check the convention for the angles between the lattice vectors in
>> >> > crystallographic format in the manual, but I think this would be
>> the
>> >> > correct
>> >> > setting). Now, do two calculations:
>> >> >
>> >> > 1) one with fixed cell, and only atomic coordinate relaxation
>> >> > (MD.VariableCell   .false.), and
>> >> > 2) one with MD.VariableCell   .true. .
>> >> >
>> >> > For those, check the cell parameters and angle between the cell
>> >> vectors
>> >> at
>> >> > the end of the second calculation.
>> >> >
>> >> > After this, do a third calculation, starting from the same ideal
>> >> > coordinates
>> >> > and with MD. VariableCell set to .true., but now using
>> >> >
>> >> > %block kgrid_Monkhorst_Pack
>> >> > 21   0   0    0.0
>> >> >  0  21   0    0.0
>> >> >  0   0    1    0.0
>> >> > %endblock kgrid_Monkhorst_Pack
>> >> >
>> >> > This is a sampling that, for the graphene cell described, includes
>> the
>> >> > high-symmetry point K in the sampling, and has a rather dense
>> k-point
>> >> > grid.
>> >> > As a final calculation, lower the Monkhorst-Pack grid to
>> >> >
>> >> > %block kgrid_Monkhorst_Pack
>> >> >  6   0   0    0.0
>> >> >  0   6   0    0.0
>> >> >  0   0   1    0.0
>> >> > %endblock kgrid_Monkhorst_Pack
>> >> >
>> >> > which still includes the high-symmetry point K, but has a much less
>> >> dense
>> >> > grid. Do it still with MD.VariableCell     .true., and look at the
>> >> > structural parameters. Use a 800 Ry cutoff in all of them, since
>> this
>> >> will
>> >> > help avoid the infamous egg-box effect. Please tell me if you see
>> any
>> >> > difference in the structural parameters from each of the
>> calculations.
>> >> You
>> >> > can use, if you wish, an automatically generated DZP basis set with
>> an
>> >> > EnergyShift  0.2 eV. An anticipation on the results: if there is no
>> >> > difference between these results, there is something wrong :)
>> >> >
>> >> > The fact that you use Stephan Roche's results as a benchmark is
>> good -
>> >> his
>> >> > calculations are very reliable. Nevertheless, I would say that you
>> are
>> >> > somehow inadvertently forcing symmetry in your system, which is the
>> >> cause
>> >> > of
>> >> > the - much likely fortuitous - agreement of whatever result you are
>> >> > obtaining in your calculations, with those of S. Roche.
>> >> >
>> >> > Some years ago, there were several posts on graphene on the list,
>> with
>> >> > some
>> >> > very enlightening paricipations by Stephanie Reich. Search the list
>> >> > archives
>> >> > for these posts - you will learn a lot from them. I did, when I was
>> >> still
>> >> > working with graphene.
>> >> >
>> >> > Later on we can deal with different beasts like GNRs.
>> >> >
>> >> > Cheers,
>> >> >
>> >> > Marcos
>> >> >
>> >> > On Thu, Apr 22, 2010 at 11:32 PM, Artem Baskin <[email protected]>
>> >> wrote:
>> >> >
>> >> >> Dear Marcos,
>> >> >> Thanks for your help, but the situation looks really WEIRD or I
>> don't
>> >> >> understand anything at all (that may be also true).
>> >> >> When I was calculating the BS for graphene and zigzag NR I did not
>> >> use
>> >> >> any
>> >> >> specific supercell (I did not use the supercell block, the naive
>> >> >> supercell
>> >> >> factors were 6*6*1 for graphene (initially my elementary unit cell
>> >> >> consisted of 2 atoms) and 6*1*1 for Zigzag NR (with 22 atoms - 5
>> >> rings
>> >> >> width)). Of course, the SCF procedure converged in these two
>> cases.
>> >> >> As to criterion to determine whether my calculations are good or
>> not,
>> >> I
>> >> >> used the comparison both with tight-bonding method results and the
>> >> DFT
>> >> >> calculations that were already done (using Siesta) by Pr. Stephan
>> >> Roche
>> >> >> and co-workers. My results tallied with the those ones perfectly.
>> >> >>
>> >> >> As to convergence in case with the zigzag NR (with k-point grid),
>> >> double
>> >> >> unit cell of armchair NR and its flakes, the procedure did not
>> >> >> converged,
>> >> >> and I don't know how to have it converged.  Moreover, form one
>> step
>> >> of
>> >> >> the
>> >> >> iteration to another one the charges on the edge H-atoms are
>> >> fluctuating
>> >> >> getting more and more asymmetrical. This is another manifestation
>> of
>> >> the
>> >> >> non-zero dipole moment.
>> >> >>
>> >> >> Best,
>> >> >> Artem Baskin,
>> >> >> PhD student,
>> >> >> University of Illinois at Chicago
>> >> >>
>> >> >>
>> >> >> On Thu, April 22, 2010 1:16 pm, Marcos Veríssimo Alves wrote:
>> >> >> > Artem,
>> >> >> >
>> >> >> > Good results for graphene without any k-point sampling (only
>> Gamma
>> >> >> point)?
>> >> >> > And also for a zigzag NR? Now THAT's weird... unless you are
>> using
>> >> a
>> >> >> huge
>> >> >> > supercell for each of them. What is your criterion for saying
>> that
>> >> >> your
>> >> >> > calculation is good? For a zigzag NR you might get away with a
>> >> smaller
>> >> >> > supercell, if it's a semiconductor (I guess it is, I don't
>> remember
>> >> it
>> >> >> > right
>> >> >> > now).
>> >> >> >
>> >> >> > What is your procedure for calculating the band structure? Are
>> you
>> >> >> making
>> >> >> > sure you re-use the converged DM file?
>> >> >> >
>> >> >> > Marcos
>> >> >> >
>> >> >> >
>> >> >> > On Thu, Apr 22, 2010 at 8:06 PM, Artem Baskin <[email protected]>
>> >> wrote:
>> >> >> >
>> >> >> >> Dear all users,
>> >> >> >> I am involved in band structure calculations for armchair and
>> >> zigzag
>> >> >> >> nanoribbons and I have problems with the appropriate k-point
>> >> >> sampling.
>> >> >> >> My
>> >> >> >> problem is like this:
>> >> >> >> Initially, I calculated the band structure for graphene and
>> zigzag
>> >> NR
>> >> >> >> without specifying any k-points. The results (with Meshcutoff
>> >> level
>> >> >> 800
>> >> >> >> Ry
>> >> >> >> and 400 Ry respectively) were quite good. But when I tried to
>> >> >> calculate
>> >> >> >> the band structure for armchair (5 rings width) NR I got
>> >> absolutely
>> >> >> >> wrong
>> >> >> >> results, moreover, in spite of symmetrical configuration I
>> >> obtained
>> >> >> the
>> >> >> >> non-zero significant dipole moment perpendicular to the ribbon
>> >> (even
>> >> >> >> with 400 Ry MCutoff).
>> >> >> >> Then I generated a k-point grid using
>> >> >> >> %block kgrid_Monkhorst_Pack
>> >> >> >> 45 0 0 0.5
>> >> >> >> 0  1 0 0.5
>> >> >> >> 0  0 1 0.5
>> >> >> >> %endblock kgrid_Monkhorst_Pack
>> >> >> >>  and I got correct results (no dipole moment and reasonable FE
>> and
>> >> >> band
>> >> >> >> structure).
>> >> >> >>
>> >> >> >> FIRST problem that I encountered was that when I tried to
>> >> recalculate
>> >> >> BS
>> >> >> >> for zigzag NR with the SAME k-point grid I got an enormous
>> dipole
>> >> >> moment
>> >> >> >> (perpendicular to the ribbon) and wrong BS and FE level. Why is
>> it
>> >> >> so?
>> >> >> >>
>> >> >> >> SECOND problem is that when I doubled the elementary cell for
>> >> 5-rings
>> >> >> >> width armchair ribbon (using the SAME k-point grid and 400 Ry
>> >> MCoff
>> >> >> >> level)
>> >> >> >> just to make sure that I will get the same good results I got
>> >> again
>> >> >> an
>> >> >> >> enormous Dip moment and incorrect Band Structure.
>> >> >> >>
>> >> >> >> And THIRD (mysterious) problem is that when I tried to
>> calculate
>> >> Band
>> >> >> >> Structure for an isolated flake of armchair NR (3*5 rings size)
>> I
>> >> got
>> >> >> >> non
>> >> >> >> zero Dip moment (in this case for x- and y- directions) that is
>> >> >> >> nonsense.
>> >> >> >>
>> >> >> >> I guess, the problem is how to define correctly k-grid in these
>> >> three
>> >> >> >> cases, but I don't know how. I performed the convergence test
>> >> >> increasing
>> >> >> >> the number of k-points but neither dipole moment nor FE level
>> >> >> >> demonstrate
>> >> >> >> the monotonic behaviour, so I could not reach the correct
>> results.
>> >> >> >>
>> >> >> >> Any help will be appreciated.
>> >> >> >>
>> >> >> >> Artem Baskin,
>> >> >> >> PhD student,
>> >> >> >> University of Illinois at Chicago
>> >> >> >>
>> >> >> >>
>> >> >> >>
>> >> >> >>
>> >> >> >
>> >> >> >
>> >> >>
>> >> >>
>> >> >>
>> >> >
>> >>
>> >>
>> >>
>> >
>>
>>
>>
>


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