Nonlinear optical effects in a three-nanolayer metal sandwich assembly

Abstract

We report spectral properties and frequency summing that induce superemission (SE) in sandwich structures built of Co nanolayers. We found that separate Co films with a layer thickness of 8.1, 9.2, and 11.3 nm have discrete absorption spectra, originating in transverse quantum confinement in such thin metal films. The surface plasmon resonance in this system should appear at energies over 50 000 cm−1, with its longer-wavelength tail easily observable. All of the nanolayers studied also presented discrete emission spectra, with the emission bands strongly overlapping due to large bandwidths (1500–2300 cm−1). The emission decay is described by a single-exponential function with the lifetime of 103±5 ns. Similarly, the sandwich assembly with three Co nanolayers separated by two BN nanolayers also has discrete lines in its absorption spectrum. The spectrum of the assembly is a superposition of the respective spectra of the individual Co layers. We report that the assembly can sum the pumping radiation photons, producing photons with a higher energy. This excitation summing/exciton joining effect, discovered in sandwich film systems, is reported for the first time. Exiting the two outside Co nanolayers at specific frequencies, the Co nanolayer in the middle produces the sum frequency. We identified this emission as SE, with a bandwidth of only 179±5 cm−1. This superemission band appeared with the rise time of 36±3 ns and disappeared with 73±5 ns decay time, with the estimated SE quantum yield of 0.063. We analyzed the energy transfer by the exchange mechanism in detail, although a contribution of the electric dipole-dipole mechanism could not be excluded.