We predict plasmonic mediated nucleation of pancake shaped resonant nano-cavities in metallic layers that are penetrable to laser irradiation. The underlying physics is that the cavity provides a narrow plasmonic resonance that maximizes its polarizability in an external field. The resonance yields a significant energy gain making the formation of such cavities highly favorable. Possible implications include nano-optics and generation of the dielectric bits in conductive films that underlie the existing optical recording phase change technology.
PACS numbers:Non-photochemical acceleration of nucleation under laser irradiation or static electric fields has been observed in a number of systems. [1][2][3][4] The effect was attributed to electric field induced polarization and lowering of the nucleation barrier. For ac fields, the frequency dependence of the material polarization, especially near plasmonic resonances, has not yet been considered and may completely modify that effect; it is of particular importance for metallic phases.In this letter we predict a phenomenon of plasmonic mediated nucleation of nano-cavities in metallic layers that are penetrable to laser fields. The underlying idea is that the nucleated cavity provides a narrow plasmonic resonance that maximizes its polarizability in an external field. The ability to adjust resonance oscillations frequency and phase makes such cavities highly energetically favorable.Our consideration is based on the classical nucleation theory 5,6 , which accounts for the bulk µV and surface σA contributions to the free energy. With the addition of the term F E to describe the electric polarization gain, the free energy is F = F E + µV + σA, where µ is the difference in chemical potential (per volume) due to cavity nucleation, σ is the surface tension, and V and A are the cavity volume and surface area, respectively. Our analysis below starts with the case of µ < 0, corresponding to a metastable metallic system wherein nucleation is naturally expected. We then consider the case of a stable metal layer, µ > 0, where cavities are energetically unfavorable in zero field.For a static field, the polarization induced energy gain of a particle that nucleates in a dielectric material, with permittivity ǫ, can be represented as, 6where α is the particle polarizability, and E is the field strength. A subtle point here is that ǫ makes Eq. (1) different from the energy of a dipole in an external field; ǫ reflects the contributions from all charges in the system, including those responsible for the field. That factor was confirmed by several authors. [6][7][8] Eq.(1) was originally obtained by integrating, over the entire space, the energy density difference caused by introduction of the particle. It must be modified for the case of dispersive media (metals), in which( 2) where ω is the field frequency, τ is the relaxation time, and ω p = 4πN e 2 /m is the plasma frequency with N being the electron concentration, m the electron mass, and e the electron charge. We assume, as usual, τ...