Motivated by the interest in zinc oxide nanostructures and their properties, we calculate in this work molecular polarizabilities and hyperpolarizabilities of a series of zinc oxide nanoclusters using modern response theory in the form of damped and pulsed response for both Hartree-Fock and DFT reference states. We show that as the size of the cluster grows, both real and imaginary parts of polarizability, computed with these two distinct approaches, asymptotically converge. We also show the importance of eliminating the dangling bonds in small clusters for predicting the correct trend in the values of the HOMO/LUMO gap. Finally, we calculate the hyperpolarizability tensors, associated with the second order nonlinear optical effects, in the hexagonal (wurtzite) phase of ZnO nanoclusters and demonstrate a highly nonlinear growth of this quantity with the cluster size.
|Original language||English (US)|
|Journal||Chemical Physics Letters|
|State||Published - May 17 2021|
Bibliographical noteKAUST Repository Item: Exported on 2021-06-08
Acknowledgements: This work was supported by Defense Advanced Research Projects Agency (DARPA), grant D19AC00017. The authors are thankful to Patrick Norman (KTH) for fruitful discussion and instrumental advice on VeloxChem calculations.
ASJC Scopus subject areas
- Physics and Astronomy(all)
- Physical and Theoretical Chemistry