Abstract
Abstract Third harmonic generation (THG) measurements on cis- and trans -polyacetylene over the pump frequency range from 0.55 eV though 1.25 eV show that Ξ (3) (-3ω; ω,ω,ω) for trans- (CH) x 1 is an order of magnitude larger than that for the cis -isomer over the entire spectral range, even comparing the respective 3ω resonance maxima. The THG data demonstrate a symmetry specific mechanism favoring the degenerate ground state system, consistent with the existence of an important contribution from virtual soliton pairs enabled by nonlinear zero-point fluctuations. Because the soliton pair creation energy at finite separation is less than the energy gap, X (3) can be simultaneously resonant at 3ω and at 2ω, and, therefore, significantly enhanced in polymers with a degenerate ground state.
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