Example: FDE NMR shielding: Acetonitrile in water¶
This examples demonstrates both the calculation of NMR shieldings using FDE, and how the approximate environment density can be improved by partial relaxation of individual solvent molecules. The test system is a cluster of acetonitrile and 12 solvent water molecules, of which for two the densities are relaxed, while for the remaining 10 the frozen density of the isolated water is used. For details, see Refs. C. R. Jacob, J. Neugebauer, and L. Visscher, A flexible implementation of frozendensity embedding for use in multilevel simulation, submitted, 2007. R. E. Bulo, Ch. R. Jacob, and L. Visscher, NMR Solvent Shifts of Acetonitrile from Frozen-Density Embedding Calculation, to be submitted, 2007
First, the isolated solvent water molecule is prepared. Again, because this will be rotated and translated afterwards, the option NOSYMFIT has to be included.
$ADFBIN/adf << eor
UNITS
Length Angstrom
Angle Degree
END
ATOMS
O -1.46800 2.60500 1.37700
H -0.95200 3.29800 0.96500
H -1.16100 1.79900 0.96100
END
FRAGMENTS
H t21.H.DZP
O t21.O.DZP
END
XC
LDA
END
NUMERICALQUALITY GOOD
end input
eor
mv TAPE21 t21.h2o
Afterwards, the FDE calculation is performed. In addition to the nonfrozen acetonitrile molecule, three different fragments are used for the solvent water molecules. The first two fragments frag1 and frag2 are relaxed (in up to two freeze-and-thaw cycles), while the third fragment is used for the remaining 10 solvent molecules. Since a calculation of the shielding is performed afterwards, the option has to be included.
...
$ADFBIN/adf << eor
Title Input generated by PyADF
UNITS
Length Angstrom
Angle Degree
END
ATOMS
C 0.83000 0.66100 -0.44400
N 0.00000 0.00000 0.00000
C 1.87800 1.55900 -0.81900
H 1.78500 2.40300 -0.13500
H 1.76200 1.94900 -1.83000
H 2.82900 1.12200 -0.51300
O -1.46800 2.60500 1.37700 f=frag1/1
H -0.95200 3.29800 0.96500 f=frag1/1
H -1.16100 1.79900 0.96100 f=frag1/1
O 2.40400 -2.51000 -0.36200 f=frag2/1
H 2.70000 -3.41900 -0.40900 f=frag2/1
H 1.77500 -2.50000 0.35900 f=frag2/1
O -3.44400 2.36700 3.13700 f=frag3/10
H -2.70200 2.29200 2.53700 f=frag3/10
H -3.47300 3.29500 3.36800 f=frag3/10
END
FRAGMENTS
H t21.H.DZP
C t21.C.DZP
N t21.N.DZP
frag1 t21.h2o type=FDE &
fdeoptions RELAX
RELAXCYCLES 2
SubEnd
frag2 t21.h2o type=FDE &
fdeoptions RELAX
RELAXCYCLES 2
SubEnd
frag3 t21.h2o type=FDE &
FDEDENSTYPE SCFexact
SubEnd
END
XC
GGA BP86
END
NUMERICALQUALITY GOOD
SAVE TAPE10
FDE
PW91k
END
End Input
eor
Finally, the calculation of the NMR shielding of the nitrogen atom is performed using the NMR program.
$ADFBIN/adf << eor
NMR
out tens iso
nuc 3
END
eor