ROHF energy discrepancy between Q-Chem and CFOUR

Hello,

I am running a simple ROHF calculation on the W20 dianion using the 6-311++G**+H(s) basis set to follow with a EOM-EE-MP2 job
Using the attached input file, Q-Chem gives the following results:

Nuclear Repulsion Energy = 2353.0399823917 hartrees
E(SCF) =  -1521.10032860

However, using the same basis set and coordinates in CFOUR, I obtain:

NUCLEAR REPULSION ENERGY: 2353.0394897083 a.u.
E(ROHF) = -1521.10034092542673

I am a bit confused, since both calculations were run in the correct Ci symmetry, and in Q-Chem I set unrestricted = false to enforce ROHF. I initially thought the discrepancy might be due to using a contracted basis set in Q-Chem, but using the uncontracted version leads to the same discrepancy.
I also don’t believe the issue is how I massage the SCF procedure in CFOUR, since the discrepancy appears even in the nuclear repulsion energy.

Thank you for your help!

  • Q-chem input
$molecule                                                                                                                                                                                                                                                                                                                  
   -2 1
O                  0.81970390    3.76180188    1.46198421
H                  1.25733314    3.57623864    0.60662586
H                  1.28053058    3.15236640    2.08985186
O                  3.23531149    0.32384416    0.82599793
H                  2.28704679    0.24534129    0.54501863
H                  3.49730856   -0.60763578    1.01618688
O                  2.12038214    1.83018807    3.06713251
H                  2.71678728    1.43075505    2.40256623
H                  1.39368615    1.16573414    3.09435004
O                  1.67889978    2.66759777   -1.09845507
H                  1.31345759    1.81126453   -0.75488271
H                  0.97978370    2.95012344   -1.72374558
O                  4.03170854    1.18133322   -1.78319056
H                  3.32970052    1.86297519   -1.75980377
H                  3.97661340    0.83597026   -0.86530409
O                 -0.95148381    2.86761049   -2.33075086
H                 -1.07366672    2.76925194   -1.36379456
H                 -0.72502626    1.94837269   -2.61441428
O                  2.44423083   -0.83761865   -3.02570310
H                  3.05470385   -0.16291434   -2.64493233
H                  2.25681964   -1.43877987   -2.27814630
O                 -0.16320877    0.18675191   -2.66773044
H                  0.75486481   -0.07288729   -2.93729087
H                 -0.14033978    0.07651131   -1.66791290
O                 -1.40160789    2.29458293    0.60787206
H                 -0.93199048    1.42618076    0.40724019
H                 -0.68720703    2.86686792    1.00101251
O                  3.69931899   -2.47696211    1.11052040
H                  3.13116201   -2.68488228    1.87264116
H                  3.07256270   -2.57733255    0.36267269
O                 -2.44423083    0.83761865    3.02570310
H                 -3.05470385    0.16291434    2.64493233
H                 -2.25681964    1.43877987    2.27814630
O                  0.95148381   -2.86761049    2.33075086
H                  1.07366672   -2.76925194    1.36379456
H                  0.72502626   -1.94837269    2.61441428
O                  0.16320877   -0.18675191    2.66773044
H                 -0.75486481    0.07288729    2.93729087
H                  0.14033978   -0.07651131    1.66791290
O                 -3.69931899    2.47696211   -1.11052040
H                 -3.13116201    2.68488228   -1.87264116
H                 -3.07256270    2.57733255   -0.36267269
O                  1.40160789   -2.29458293   -0.60787206
H                  0.93199048   -1.42618076   -0.40724019
H                  0.68720703   -2.86686792   -1.00101251
O                 -4.03170854   -1.18133322    1.78319056
H                 -3.32970052   -1.86297519    1.75980377
H                 -3.97661340   -0.83597026    0.86530409
O                 -1.67889978   -2.66759777    1.09845507
H                 -1.31345759   -1.81126453    0.75488271
H                 -0.97978370   -2.95012344    1.72374558
O                 -3.23531149   -0.32384416   -0.82599793
H                 -2.28704679   -0.24534129   -0.54501863
H                 -3.49730856    0.60763578   -1.01618688
O                 -0.81970390   -3.76180188   -1.46198421
H                 -1.25733314   -3.57623864   -0.60662586
H                 -1.28053058   -3.15236640   -2.08985186
O                 -2.12038214   -1.83018807   -3.06713251
H                 -2.71678728   -1.43075505   -2.40256623
H                 -1.39368615   -1.16573414   -3.09435004
$end

$rem
   UNRESTRICTED    FALSE
   METHOD          eom-mp2
   BASIS           gen
   EE_SINGLETS     [6,6]
   EE_TRIPLETS     [6,6]
   SYMMETRY        true
   PURECART        1
  SCF_ALGORROTH    DIIS
  THRESH           14
  S2THRESH         16
$end

$basis
H     0   
S   3   1.00
     33.86500                0.0254938
      5.094790               0.190373
      1.158790               0.852161
S   1   1.00
      0.325840               1.000000
S   1   1.00
      0.102741               1.000000
S   1   1.00
      0.0360000              1.0000000
S   1   1.00
      0.0090000              1.0000000
P   1   1.00
      0.750                  1.000000
****
O     0   
S   6   1.00
   8588.500                  0.00189515
   1297.230                  0.0143859
    299.2960                 0.0707320
     87.37710                0.2400010
     25.67890                0.5947970
      3.740040               0.2808020
SP   3   1.00
     42.11750                0.113889               0.0365114
      9.628370               0.920811               0.237153
      2.853320              -0.00327447             0.819702
SP   1   1.00
      0.905661               1.000000               1.000000
SP   1   1.00
      0.255611               1.000000               1.000000
SP   1   1.00
      0.0845000              1.0000000              1.0000000
D   1   1.00
      1.292                  1.000000
****
$end
  • CFOUR input (ZMAT)
*CFOUR(CALC=MP2
EXCITE=EOMEE
ESTATE_CONV=7
ABCDTYPE=AOBASIS
ESTATE_SYM=3/3
BASIS=SPECIAL
REF=ROHF
COORD=CARTESIAN
SCF_MAXCYC=1050
FROZEN_CORE=ON
MEMORY=100000, MEM_UNIT=MB
SUBGROUP=4
UNITS=ANGSTROM
OCCUPATION=51-50/51-50
SCF_DAMPING=500
SCF_EXPORDER=25
CHARGE=-2
MULTIPLICITY=1)
  • CFOUR input (GENBAS)
H:6-311++G**                                                                                                                                                                                 
VTZ Valence Triple Zeta: 3 Funct.'s/Valence AO with diffuse+polarization on all atoms

  2
    0    1   
    5    1   
    7    1   

33.86500 5.094790 1.158790 0.325840 0.102741 0.0360000 0.009

0.0254938 0.00000000 0.00000000 0.00000000  0.00000 
0.190373 0.00000000 0.00000000 0.00000000   0.00000
0.852161 0.00000000 0.00000000 0.00000000   0.00000 
0.00000000 1.000000 0.00000000 0.00000000   0.00000 
0.00000000 0.00000000 1.000000 0.00000000   0.00000 
0.00000000 0.00000000 0.00000000 1.0000000  0.00000 
0.00000000 0.00000000 0.00000000 0.0000000  1.00000 

0.750

1.000000 

O:6-311++G**
VTZ Valence Triple Zeta: 3 Funct.'s/Valence AO with diffuse+polarization on all atoms

  3
    0    1    2   
    5    4    1   
   12    6    1   

8588.500 1297.230 299.2960 87.37710 42.11750 
25.67890 9.628370 3.740040 2.853320 0.905661 
0.255611 0.0845000 

0.00189515 0.00000000 0.00000000 0.00000000 0.00000000
0.0143859 0.00000000 0.00000000 0.00000000 0.00000000
0.0707320 0.00000000 0.00000000 0.00000000 0.00000000
0.2400010 0.00000000 0.00000000 0.00000000 0.00000000
0.00000000 0.113889 0.00000000 0.00000000 0.00000000
0.5947970 0.00000000 0.00000000 0.00000000 0.00000000
0.00000000 0.920811 0.00000000 0.00000000 0.00000000
0.2808020 0.00000000 0.00000000 0.00000000 0.00000000
0.00000000 -0.00327447 0.00000000 0.00000000 0.00000000
0.00000000 0.00000000 1.000000 0.00000000 0.00000000
0.00000000 0.00000000 0.00000000 1.000000 0.00000000
0.00000000 0.00000000 0.00000000 0.00000000 1.0000000

42.11750 9.628370 2.853320 0.905661 0.255611 
0.0845000 

0.0365114 0.00000000 0.00000000 0.00000000 
0.237153 0.00000000 0.00000000 0.00000000 
0.819702 0.00000000 0.00000000 0.00000000 
0.00000000 1.000000 0.00000000 0.00000000 
0.00000000 0.00000000 1.000000 0.00000000 
0.00000000 0.00000000 0.00000000 1.0000000 

1.292

1.000000

A discrepancy in the nuclear repulsion energy suggests the geometries aren’t the same.

Hello,

I agree. However, if one look to the full ZMAT (CFOUR) input,
the geometries are the same

PES of W20 DIANION
O                  0.81970390    3.76180188    1.46198421
H                  1.25733314    3.57623864    0.60662586
H                  1.28053058    3.15236640    2.08985186
O                  3.23531149    0.32384416    0.82599793
H                  2.28704679    0.24534129    0.54501863
H                  3.49730856   -0.60763578    1.01618688
O                  2.12038214    1.83018807    3.06713251
H                  2.71678728    1.43075505    2.40256623
H                  1.39368615    1.16573414    3.09435004
O                  1.67889978    2.66759777   -1.09845507
H                  1.31345759    1.81126453   -0.75488271
H                  0.97978370    2.95012344   -1.72374558
O                  4.03170854    1.18133322   -1.78319056
H                  3.32970052    1.86297519   -1.75980377
H                  3.97661340    0.83597026   -0.86530409
O                 -0.95148381    2.86761049   -2.33075086
H                 -1.07366672    2.76925194   -1.36379456
H                 -0.72502626    1.94837269   -2.61441428
O                  2.44423083   -0.83761865   -3.02570310
H                  3.05470385   -0.16291434   -2.64493233
H                  2.25681964   -1.43877987   -2.27814630
O                 -0.16320877    0.18675191   -2.66773044
H                  0.75486481   -0.07288729   -2.93729087
H                 -0.14033978    0.07651131   -1.66791290
O                 -1.40160789    2.29458293    0.60787206
H                 -0.93199048    1.42618076    0.40724019
H                 -0.68720703    2.86686792    1.00101251
O                  3.69931899   -2.47696211    1.11052040
H                  3.13116201   -2.68488228    1.87264116
H                  3.07256270   -2.57733255    0.36267269
O                 -2.44423083    0.83761865    3.02570310
H                 -3.05470385    0.16291434    2.64493233
H                 -2.25681964    1.43877987    2.27814630
O                  0.95148381   -2.86761049    2.33075086
H                  1.07366672   -2.76925194    1.36379456
H                  0.72502626   -1.94837269    2.61441428
O                  0.16320877   -0.18675191    2.66773044
H                 -0.75486481    0.07288729    2.93729087
H                  0.14033978   -0.07651131    1.66791290
O                 -3.69931899    2.47696211   -1.11052040
H                 -3.13116201    2.68488228   -1.87264116
H                 -3.07256270    2.57733255   -0.36267269
O                  1.40160789   -2.29458293   -0.60787206
H                  0.93199048   -1.42618076   -0.40724019
H                  0.68720703   -2.86686792   -1.00101251
O                 -4.03170854   -1.18133322    1.78319056
H                 -3.32970052   -1.86297519    1.75980377
H                 -3.97661340   -0.83597026    0.86530409
O                 -1.67889978   -2.66759777    1.09845507
H                 -1.31345759   -1.81126453    0.75488271
H                 -0.97978370   -2.95012344    1.72374558
O                 -3.23531149   -0.32384416   -0.82599793
H                 -2.28704679   -0.24534129   -0.54501863                                                                                                                                                                                                                                                                  
H                 -3.49730856    0.60763578   -1.01618688
O                 -0.81970390   -3.76180188   -1.46198421
H                 -1.25733314   -3.57623864   -0.60662586
H                 -1.28053058   -3.15236640   -2.08985186
O                 -2.12038214   -1.83018807   -3.06713251
H                 -2.71678728   -1.43075505   -2.40256623
H                 -1.39368615   -1.16573414   -3.09435004

*CFOUR(CALC=MP2
EXCITE=EOMEE
ESTATE_CONV=7
ABCDTYPE=AOBASIS
ESTATE_SYM=3/3
BASIS=SPECIAL
REF=ROHF
COORD=CARTESIAN
SCF_MAXCYC=1050
GUESS=MOREAD
FROZEN_CORE=ON
MEMORY=100000, MEM_UNIT=MB
SUBGROUP=4
UNITS=ANGSTROM
OCCUPATION=51-50/51-50
SCF_DAMPING=500
SCF_EXPORDER=25
CHARGE=-2
MULTIPLICITY=1)

I ran into this issue some time ago… If you input geometries in Bohr with INPUT = BOHR in QChem and the corresponding keyword in CFour they’ll both give you much closer nuclear repulsion energies (but still not exactly the same). So, when one of the programs converts the coordinates to one unit system to the other there is a discrepancy somewhere.