TDDFT calculations with DIRAC

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Here I would like to give a typical input for a TDDFT calculation of excitation energies with DIRAC and discuss the important keywords (colored).

This is a TDDFT calculation of the Zn atom with the PBE functional.

To obtain good TDDFT excitation energies it is essential to include the spin density contribution (spin magnetization contribution). This is done with the .SDFT keyword. Without spin density, triplet excitation energies correspond to KS orbital energy differences.

We suppress orbital rotations between positive and negative energy orbitals with .SKIPEP.

Also include the .TRIPLET keyword. This keyword is without effect (but also without harm) when spin-orbit coupling is turned on. However, without spin-orbit coupling (nonrelativistic or spin-free calculations) this keyword allows the spin density contribution in spin-forbidden transitions. Without spin-orbit coupling and without .TRIPLET, triplet energies again correspond to KS orbital energy differences. This keyword does not mean that only triplet states are solved for.

**DIRAC
.WAVE FUNCTION
.PROPERTIES
.ANALYZE
**HAMILTONIAN
.LVCORR
.DFT
 PBE
*DFT
.SDFT
**INTEGRALS
*READIN
.UNCONTRACT
**WAVE FUNCTION
.DHF
*DHFCAL
.EVCCNV
 1.0D-9 1.0D-6
.CLOSED
 18 12      !zinc atom
**PROPERTIES
*EXCITATION ENERGIES
.TRIPLET
.SKIPEP
.ANALYZE
.EXCITATION ENERGIES
 3 4
.EXCITATION ENERGIES
 5 4
.EXCITATION ENERGIES
 8 4
.OPERATOR
 XDIPLEN
.OPERATOR
 YDIPLEN
.OPERATOR
 ZDIPLEN
**ANALYZE
.MULPOP
*MULPOP
.VECPOP
 1..oo
 1..oo      !remove this line if there is only one Fermion irreducible corepresentation
*END OF

With

.EXCITATION ENERGIES
 3 4
.EXCITATION ENERGIES
 5 4
.EXCITATION ENERGIES
 8 4

we ask for the four lowest excitation energies in the irreps 3, 5, and 8.

In this example (Zn, D2h) these are the ungerade irreps B2u, B1u, and Au.

Finally, it is a good idea to always include

.OPERATOR
 XDIPLEN
.OPERATOR
 YDIPLEN
.OPERATOR
 ZDIPLEN

to get transition dipole moments and oscillator strengths (if symmetry allowed).

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