title: Amplification of the linear and nonlinear optical response of a chiral molecular crystal.
abstract: We have observed large second-order nonlinear optical and vibrational circular dichroism (VCD) responses in a charge-transfer-type L-Histidinium salt. Using X-ray Diffraction, VCD spectroscopy, and time-dependent density functional theory to characterize the compound, we employ a two-level model to explain and quantify the strongly enhanced optical signals. We find that both linear and nonlinear optical responses are greatly enhanced by a single low-lying charge-transfer state.
authors.affiliation: Van't Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH Amsterdam, The Netherlands. s.m.rosadomingos@uva.nl
authors.forename: Sérgio R
authors.initials: SR
authors.lastname: Domingos
authors.forename: Pedro S Pereira
authors.initials: PS
authors.lastname: Silva
authors.forename: Wybren Jan
authors.initials: WJ
authors.lastname: Buma
authors.forename: M Helena
authors.initials: MH
authors.lastname: Garcia
authors.forename: Nelson C
authors.initials: NC
authors.lastname: Lopes
authors.forename: José António
authors.initials: JA
authors.lastname: Paixão
authors.forename: Manuela Ramos
authors.initials: MR
authors.lastname: Silva
authors.forename: Sander
authors.initials: S
authors.lastname: Woutersen