Understanding and Controlling High Harmonic Generation Processes in Hybrid Materials at the Nanoscale

Understanding and Controlling High Harmonic Generation Processes in Hybrid Materials at the Nanoscale Understanding and controlling high harmonic generation processes in hybrid materials at the nanoscale publically releasable. Abstract The goal of the proposed research program is to develop and apply rigorous theoretical/ computational models to quantitatively describe high harmonic generation (HHG) processes at the nanoscale. The intent is to surpass the conventional approaches frequently used in nanophotonics and to incorporate the nonlinear optical response of metal interfaces into the state-of-the-art numerical solvers. The microscopic model describing quantum dynamics of molecules will be combined with the nonlinear dispersive model for metal. The developed model will be used to investigate a wide variety of optical phenomena ranging from fundamental properties of HHG fields through their coherent control at the nanoscale to understanding dynamics of high intense femtosecond laser pulses interacting with hybrid (exciton-plasmon) nanomaterials. Furthermore, the model will be extended beyond the mean field approximation in order to scrutinize the influence of entangled states on HHG processes. Three subprograms are proposed: (1) High harmonic generation in hybrid nanomaterials The goal of this part is to develop computational models describing nonlinear responses of hybrid nanomaterials in time domain. To achieve this rigorous quantum mechanical models of molecular excitons will be combined with the nonlinear hydrodynamic model for metal interfaces. (2) Applications of the nonlinear microscopic model The nonlinear microscopic model developed and tested during the first stage of the program will be applied to describe chiral hybrid nanomaterials and the optical bistability at the nanoscale. For the first time chiral plasmonic materials of various topologies will be considered in the nonlinear regime. HHG processes will be simulated in such systems. The optical bistability phenomenon in hybrid nanosystems will be considered at high molecular concentrations. (3) Beyond mean field approximation Further extension of the microscopic model will include quantum correlations between molecules currently missing in the standard semiclassical models to understand how entangled molecular states may influence HHG processes.