[gmx-users] Wrong bond and Lennard-Jones potentials in cyclohexane

Henri Ervasti h.k.ervasti at tudelft.nl
Fri Dec 11 14:43:07 CET 2009


Dear all,

I have tried to simulate cyclohexane to produce vaporization enthalpy
for it. I have tried it with two approaches: 

1) using geometry, torsion potentials (harmonic) + charges obtained from
B3LYP/6-311++G** (DFT) calculations and OPLS-AA Lennard-Jones, bond and
angle potentials. 

2) Using only OPLS-AA force field values (slightly modified for
torsions). 

In both cases I do achieve a reasonable accuracy for density, but the
energetics go totally wrong and even the sign of the result is the
opposite than it should be. I have noticed that this results from very
large bond potentials and L-J potentials in the averaged results. From a
512 molecules NPT MD simulation (minimization using steep, 400ps
relaxation, 2ns run, 2fs time-step) using OPLS-AA parameters only, I get
an average energy (the total divided by 512) for a bond to be 115.9
kJ/mol, while for a single cyclohexane in vacuum this is 24.4 kJ/mol.
The L-J results into an average (the total divided by 512) 14.03 kJ/mol,
which suggests that the L-J part would be repulsive! If I approximate
that the intramolecular energies would be the same (thus ignore bond,
angle, torsion terms) I get vaporization enthalpy of about -20.6 kJ/mol,
while the experimental result is around +33 kJ/mol. Thus, a wrong sign
indicating that the system should be in the gas phase, enlarging (which
it does not do). The results are even slightly worse using the DFT
geometries, torsions, charges. Also, the creators of OPLS-AA have
simulated cyclohexane and obtained DvapH very close to the experimental
results [Jorgensen et al, JACS 1996, 118, 11225-11236 + the supporting
info].

I have tried using different time-step, different L-J for hydrogen and
carbon, different torsion potentials, but the results are always the
same: very large potentials for bonds and L-J.

This discrepancy baffles me, especially that this problem does not
appear when I have modelled f.ex. methanol, ethanol, hexane, acetone...
Even N-formyl morpholine did not show this problem, although it also has
a six-membered ring. Could this be some kind of problem in the code for
(more) symmetric (non-aromatic) ring/cyclic molecules?

See the topology file and a pdb file for the OPLS-AA cyclohexane
simulation at the end of the message.

Thank you for your help!

Kind regards,
Henri Ervasti

PDB:

HEADER
HETATM    1  CAA CHE     1       0.140   2.640   0.160  1.00 20.00
C
HETATM    2  CAB CHE     1      -0.030   1.160  -0.190  1.00 20.00
C
HETATM    3  CAC CHE     1       1.450   3.180  -0.410  1.00 20.00
C
HETATM    4  HAA CHE     1       0.148   2.753   1.244  1.00 20.00
H
HETATM    5  CAD CHE     1       1.160   0.360   0.350  1.00 20.00
C
HETATM    6  HAC CHE     1      -0.080   1.048  -1.273  1.00 20.00
H
HETATM    7  HAD CHE     1      -0.916   0.808   0.338  1.00 20.00
H
HETATM    8  CAF CHE     1       2.470   0.890  -0.220  1.00 20.00
C
HETATM    9  HAG CHE     1       1.045  -0.687   0.068  1.00 20.00
H
HETATM   10  HAH CHE     1       1.191   0.528   1.426  1.00 20.00
H
HETATM   11  CAE CHE     1       2.630   2.380   0.130  1.00 20.00
C
HETATM   12  HAK CHE     1       2.466   0.772  -1.304  1.00 20.00
H
HETATM   13  HAL CHE     1       3.277   0.358   0.285  1.00 20.00
H
HETATM   14  HAI CHE     1       2.595   2.455   1.217  1.00 20.00
H
HETATM   15  HAJ CHE     1       3.552   2.756  -0.313  1.00 20.00
H
HETATM   16  HAB CHE     1      -0.668   3.178  -0.337  1.00 20.00
H
HETATM   17  HAF CHE     1       1.420   3.015  -1.487  1.00 20.00
H
HETATM   18  HAE CHE     1       1.563   4.226  -0.123  1.00 20.00
H

TOPOLOGY:

[ defaults ]
; nbfunc        comb-rule       gen-pairs          fudgeLJ fudgeQQ
  1             2               yes                0.5     0.5

[ atomtypes ]
; name  at.num      mass     charge   ptype     sigma        epsilon    
  CH1     6     12.01100     0.000      A   3.50000e-01  2.76144e-01
  HC      1      1.00790     0.000      A   2.50000e-01  1.25000e-01

[ nonbond_params ]
   ; i    j func          c6           c12

[ pairtypes ]
   ; i    j func         cs6          cs12

[ moleculetype ]
; Name nrexcl
   CHE    5

[ atoms ]
;   nr      type  resnr resid  atom  cgnr      charge  mass  
     1       CH1     1  CHE     CAA    1    -0.120  12.0110   
     2       CH1     1  CHE     CAB    2    -0.120  12.0110   
     3       CH1     1  CHE     CAC    3    -0.120  12.0110   
     4        HC     1  CHE     HAA    1     0.060   1.0079
     5       CH1     1  CHE     CAD    4    -0.120  12.0110   
     6        HC     1  CHE     HAC    2     0.060   1.0079
     7        HC     1  CHE     HAD    2     0.060   1.0079
     8       CH1     1  CHE     CAF    5    -0.120  12.0110   
     9        HC     1  CHE     HAG    4     0.060   1.0079
    10        HC     1  CHE     HAH    4     0.060   1.0079
    11       CH1     1  CHE     CAE    6    -0.120  12.0110   
    12        HC     1  CHE     HAK    5     0.060   1.0079
    13        HC     1  CHE     HAL    5     0.060   1.0079
    14        HC     1  CHE     HAI    6     0.060   1.0079
    15        HC     1  CHE     HAJ    6     0.060   1.0079
    16        HC     1  CHE     HAB    1     0.060   1.0079
    17        HC     1  CHE     HAF    3     0.060   1.0079
    18        HC     1  CHE     HAE    3     0.060   1.0079

[ bonds ]
; ai  aj  fu    c0, c1, ...  CHARMM/22 ; B3LYP/CBSB7
   1   2   1    0.1529  224262.4  ; 0.154 
   1   3   1    0.1529  224262.4  ; 0.154 
   1   4   1    0.1090  284512.0  ; 0.110 
   1  16   1    0.1090  284512.0  ; 0.110 
   2   5   1    0.1529  224262.4  ; 0.154 
   2   6   1    0.1090  284512.0  ; 0.110 
   2   7   1    0.1090  284512.0  ; 0.110 
   3  11   1    0.1529  224262.4  ; 0.154 
   3  17   1    0.1090  284512.0  ; 0.110 
   3  18   1    0.1090  284512.0  ; 0.110 
   5   8   1    0.1529  224262.4  ; 0.154 
   5   9   1    0.1090  284512.0  ; 0.110 
   5  10   1    0.1090  284512.0  ; 0.110 
   8  11   1    0.1529  224262.4  ; 0.154 
   8  12   1    0.1090  284512.0  ; 0.110 
   8  13   1    0.1090  284512.0  ; 0.110 
  11  14   1    0.1090  284512.0  ; 0.110 
  11  15   1    0.1090  284512.0  ; 0.110 

[ pairs ]
; ai  aj  fu    c0, c1, ...

[ exclusions ]
; ai  aj  ak  ...

[ angles ]
; ai  aj  ak  fu    c0, c1, ... CHARMM/22 ; B3LYP/CBSB7
   1   2   6   1   110.7  313.800  ; 110.2 
   1   2   7   1   110.7  313.800  ; 109.1 
   1   3  11   1   112.7  488.273  ; 111.6 
   1   3  17   1   110.7  313.800  ; 110.2 
   1   3  18   1   110.7  313.800  ; 109.1 
   2   1   3   1   112.7  488.273  ; 111.5 
   2   1   4   1   110.7  313.800  ; 109.1 
   2   1  16   1   110.7  313.800  ; 110.2 
   2   5   8   1   112.7  488.273  ; 111.6 
   2   5   9   1   110.7  313.800  ; 109.1 
   2   5  10   1   110.7  313.800  ; 110.2 
   3   1   4   1   110.7  313.800  ; 109.1 
   3   1  16   1   110.7  313.800  ; 110.2 
   3  11   8   1   112.7  488.273  ; 111.6 
   3  11  14   1   110.7  313.800  ; 109.1 
   3  11  15   1   110.7  313.800  ; 110.2 
   4   1  16   1   107.8  276.144  ; 106.4 
   5   2   6   1   110.7  313.800  ; 110.2 
   5   2   7   1   110.7  313.800  ; 109.1 
   5   8  11   1   112.7  488.273  ; 111.5 
   5   8  12   1   110.7  313.800  ; 110.2 
   5   8  13   1   110.7  313.800  ; 109.2 
   6   2   7   1   107.8  276.144  ; 106.5 
   8   5   9   1   110.7  313.800  ; 109.1 
   8   5  10   1   110.7  313.800  ; 110.2 
   8  11  14   1   110.7  313.800  ; 109.1 
   8  11  15   1   110.7  313.800  ; 110.2 
   9   5  10   1   107.8  276.144  ; 106.5 
  11   3  17   1   110.7  313.800  ; 110.2 
  11   3  18   1   110.7  313.800  ; 109.1 
  11   8  12   1   110.7  313.800  ; 110.2 
  11   8  13   1   110.7  313.800  ; 109.2 
  12   8  13   1   107.8  276.144  ; 106.4 
  14  11  15   1   107.8  276.144  ; 106.5 

[ dihedrals ]
; ai  aj  ak  al  fu    c0, c1, m, ...
   1   2   5   8   5   0.0000  0.0000 40.0000  0.0000 
   1   2   5   9   5   0.0000  0.0000  1.2552  0.0000
   1   2   5  10   5   0.0000  0.0000  1.2552  0.0000
   1   3  11   8   5   0.0000  0.0000 40.0000  0.0000 
   1   3  11  14   5   0.0000  0.0000  1.2552  0.0000
   1   3  11  15   5   0.0000  0.0000  1.2552  0.0000
   2   1   3  11   5   0.0000  0.0000 40.0000  0.0000 
   2   1   3  17   5   0.0000  0.0000  1.2552  0.0000
   2   1   3  18   5   0.0000  0.0000  1.2552  0.0000
   2   5   8  11   5   0.0000  0.0000 40.0000  0.0000 
   2   5   8  12   5   0.0000  0.0000  1.2552  0.0000
   2   5   8  13   5   0.0000  0.0000  1.2552  0.0000
   3   1   2   5   5   0.0000  0.0000 40.0000  0.0000 
   3   1   2   6   5   0.0000  0.0000  1.2552  0.0000
   3   1   2   7   5   0.0000  0.0000  1.2552  0.0000
   3  11   8   5   5   0.0000  0.0000 40.0000  0.0000 
   3  11   8  12   5   0.0000  0.0000  1.2552  0.0000
   3  11   8  13   5   0.0000  0.0000  1.2552  0.0000
   4   1   2   5   5   0.0000  0.0000  1.2552  0.0000
   4   1   2   6   5   0.0000  0.0000  1.2552  0.0000
   4   1   2   7   5   0.0000  0.0000  1.2552  0.0000
   4   1   3  11   5   0.0000  0.0000  1.2552  0.0000
   4   1   3  17   5   0.0000  0.0000  1.2552  0.0000
   4   1   3  18   5   0.0000  0.0000  1.2552  0.0000
   5   2   1  16   5   0.0000  0.0000  1.2552  0.0000
   5   8  11  14   5   0.0000  0.0000  1.2552  0.0000
   5   8  11  15   5   0.0000  0.0000  1.2552  0.0000
   6   2   1  16   5   0.0000  0.0000  1.2552  0.0000
   6   2   5   8   5   0.0000  0.0000  1.2552  0.0000
   6   2   5   9   5   0.0000  0.0000  1.2552  0.0000
   6   2   5  10   5   0.0000  0.0000  1.2552  0.0000
   7   2   1  16   5   0.0000  0.0000  1.2552  0.0000
   7   2   5   8   5   0.0000  0.0000  1.2552  0.0000
   7   2   5   9   5   0.0000  0.0000  1.2552  0.0000
   7   2   5  10   5   0.0000  0.0000  1.2552  0.0000
   8  11   3  17   5   0.0000  0.0000  1.2552  0.0000
   8  11   3  18   5   0.0000  0.0000  1.2552  0.0000
   9   5   8  11   5   0.0000  0.0000  1.2552  0.0000
   9   5   8  12   5   0.0000  0.0000  1.2552  0.0000
   9   5   8  13   5   0.0000  0.0000  1.2552  0.0000
  10   5   8  11   5   0.0000  0.0000  1.2552  0.0000
  10   5   8  12   5   0.0000  0.0000  1.2552  0.0000
  10   5   8  13   5   0.0000  0.0000  1.2552  0.0000
  11   3   1  16   5   0.0000  0.0000  1.2552  0.0000
  12   8  11  14   5   0.0000  0.0000  1.2552  0.0000
  12   8  11  15   5   0.0000  0.0000  1.2552  0.0000
  13   8  11  14   5   0.0000  0.0000  1.2552  0.0000
  13   8  11  15   5   0.0000  0.0000  1.2552  0.0000
  14  11   3  17   5   0.0000  0.0000  1.2552  0.0000
  14  11   3  18   5   0.0000  0.0000  1.2552  0.0000
  15  11   3  17   5   0.0000  0.0000  1.2552  0.0000
  15  11   3  18   5   0.0000  0.0000  1.2552  0.0000

[ system ]
cyclohexane

[ molecules ]
CHE     512



-- 
----------------------------------- 
Dr. Henri K. Ervasti 
Delft University of Technology 
Process & Energy Laboratory 
Leeghwaterstraat 44 k. 0.30 
2628CA Delft 
Netherlands 

e-mail: h.k.ervasti at tudelft.nl 
phone: +31 (0)15 27 86662 
fax:   +31 (0)15 27 82460




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