Accurate and Scalable Quantum Hydrodynamic Simulations of Plasmonic Nanostructures Within OFDFT

Quantum hydrodynamic theory (QHT) provides a computationally efficient alternative to time-dependent density functional theory for simulating plasmonic nanostructures, but its predictive power depends critically on the choice of ground-state electron density and energy functional. To construct ground-state densities, we adopt orbital-free density functional theory and numerically evaluate the effect of different exchange–correlation functionals and kinetic energy functionals. A suitable energy functional to reproduce both the DFT-calculated work function and charge density is identified. In the excited-state part, we adopt this obital-free ground-state density and investigate how variations in the von Weizsäcker kinetic energy fraction within the Laplacian-level functional affect the resonance energy and oscillator strengths. The appropriate functional form is identified, achieving an accuracy comparable to that reported in previous studies. Applied to sodium nanodimers, our approach captures nonlinear density responses at sub-nanometer gaps. This work extends QHT beyond idealized geometries and offers a robust path toward efficient quantum plasmonic modeling.