Calculating TPSE using DFT quadratic response single residue
Hello !
I'm new to Dalton and want to use it to calculate two-photon spontaneous emission (TPSE) instead of two-photon absorption (TPA). Using the quadratic response with a single residue (with DFT), it's possible to get the second-order transition moment directly, without calculating the transitions between excited states (with the double residue). In particular, for the molecule I'm interested in, the error with a single residue is smaller than with a double residue.
The second-order transition moment of TPSE is very similar to that of TPA. In the denominator of TPA, we have something like this (it seems that the energy of the two photons is limited to \omega_{eg}/2 in Dalton): (\omega_{gm} - \omega_{eg}/2) for the two terms of the sum of the states, with \hbar \omega_{gm} the energy difference between the ground state (\ket{g}) and the intermediate state (\ket{m}), and with \hbar \omega_{eg} the energy difference between the excited state (\ket{e}) and the ground state (\ket{g}). For TPSE, the denominator is (\omega_{em} - \omega) and (\omega_{em} - (\omega_{eg}-\omega)) with \hbar \omega_{em} the energy difference between the excited state (\ket{e}) and the intermediate state (\ket{m}).
My question is, is it possible for me to implement these modifications quite easily? i.e., replace \omega_{gm} with \omega_{em} and add the possibility of having two photons of different energies).
Thank you very much,