Sub-wavelength modulation of Ï ‡ (2) optical nonlinearity in organic thin films

Yixin Yan, Yakun Yuan, Baomin Wang, Venkatraman Gopalan, Noel C. Giebink

Research output: Contribution to journalArticlepeer-review

11 Scopus citations


Modulating the second-order nonlinear optical susceptibility (ξ(2)) of materials at the nanoscale represents an ongoing technological challenge for a variety of integrated frequency conversion and nonlinear nanophotonic applications. Here we exploit the large hyperpolarizability of intermolecular charge transfer states, naturally aligned at an organic semiconductor donor-acceptor (DA) interface, as a means to control the magnitude and sign of ξ(2) at the nanoscale. Focusing initially on a single pentacene-C60 DA interface, we confirm that the charge transfer transition is strongly aligned orthogonal to the heterojunction and find that it is responsible for a large interfacial nonlinearity probed via second harmonic generation that is sufficient to achieve d33 >10 pmV-1, when incorporated in a non-centrosymmetric DA multilayer stack. Using grating-shadowed oblique-angle deposition to laterally structure the DA interface distribution in such multilayers subsequently enables the demonstration of a ξ(2) grating with 280 nm periodicity, which is the shortest reported to date.

Original languageEnglish (US)
Article number14269
JournalNature communications
StatePublished - Jan 27 2017

All Science Journal Classification (ASJC) codes

  • General Chemistry
  • General Biochemistry, Genetics and Molecular Biology
  • General Physics and Astronomy


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