Computing thermal effects on nonlinear optical properties of small atoms
Research output: Other conference contribution › Paper, poster or abstract › Scientific
|Publication status||Published - 23 Mar 2017|
|Event||51st Annual Meeting of the Finnish Physical Society: Physics Days 2017 - Aalto University Töölö Campus, Helsinki, Finland|
Duration: 22 Mar 2017 → 24 Mar 2017
|Conference||51st Annual Meeting of the Finnish Physical Society|
|Period||22/03/17 → 24/03/17|
The path-integral Monte Carlo method (PIMC) provides a tangible interface between the tensorial and the thermally averaged character of molecular (hyper)polarizabilities. In a recent study , we have derived field-free estimators that make the computation even more straightforward than our previous finite-field approach . With the adiabatic, i.e. Born–Oppenheimer, approximation we obtain accurate tensorial ground state (hyper)polarizabilities, while the non-adiabatic simulation adds in considerable rovibrational effects and thermal coupling. In case of several two-electron systems, our results at the 0 K limit are either novel or in excellent agreement with the literature (e.g., see Fig. 1). Besides these results, we are presenting the derivation and demonstration of yet unpublished estimators for dipole-quadrupole polarizabilities of small molecules.