Nonlinear plasmonics at planar metal surfaces

Philos Trans A Math Phys Eng Sci. 2011 Sep 13;369(1950):3497-509. doi: 10.1098/rsta.2011.0100.

Abstract

We investigate the nonlinear optical response of a noble metal surface. We derive the components of the third-order nonlinear susceptibility and determine an absolute value of χ((3))≈0.2 nm(2) V(-2), a value that is more than two orders of magnitude larger than the values found for typical nonlinear laser crystals. Using nonlinear four-wave mixing (4WM) with incident laser pulses of frequencies ω(1) and ω(2), we generate fields oscillating at the nonlinear frequency ω(4WM)=2ω(1)-ω(2). We identify and discuss three distinct regimes: (i) a regime where the 4WM field is propagating, (ii) a regime where it is evanescent, and (iii) a regime where the nonlinear response couples to surface plasmon polaritons.