Our theoretical examination of second and third harmonic generation from metal-based nanostructures predicts that nonlocal and quantum tunneling phenomena can significantly exceed expectations based solely on local, classical electromagnetism. Mindfu
l that the diameter of typical transition metal atoms is approximately 3{AA}, we adopt a theoretical model that treats nanometer-size features and/or sub-nanometer size gaps or spacers by taking into account: (i) the limits imposed by atomic size to fulfill the requirements of continuum electrodynamics; (ii) spillage of the nearly-free electron cloud into the surrounding vacuum; and (iii) the increased probability of quantum tunneling as objects are placed in close proximity. Our approach also includes the treatment of bound charges, which add crucial, dynamical components to the dielectric constant that are neglected in the conventional hydrodynamic model, especially in the visible and UV ranges, where interband transitions are important. The model attempts to inject into the classical electrodynamic picture a simple, perhaps more realistic description of the metal surface by incorporating a thin patina of free-electrons that screens an internal, polarizable medium.
We simulate and discuss novel spatio-temporal propagation effects that relate specifically to pulsed, phase-mismatched second harmonic generation in a negative index material having finite length. Using a generic Drude model for the dielectric permit
tivity and magnetic permeability, the fundamental and second harmonic frequencies are tuned so that the respective indices of refraction are negative for the pump and positive for the second harmonic signal. A phase-locking mechanism causes part of the second harmonic signal generated at the entry surface to become trapped and dragged along by the pump and to refract negatively, even though the index of refraction at the second harmonic frequency is positive. These circumstances culminate in the creation of an anomalous state consisting of a forward-moving second harmonic wave packet that has negative wave vector and momentum density, which in turn leads to non-specular reflections at intervening material interfaces. The forward-generated second harmonic signal trapped under the pump pulse propagates forward, but has all the attributes of a reflected pulse, similar to its twin counterpart generated at the surface and freely propagating backward away from the interface. This describes a new state of negative refraction, associated with nonlinear frequency conversion and parametric processes, whereby a beam generated at the interface can refract negatively even though the index of refraction at that wavelength is positive.
