Remote multi-color excitation using femtosecond propagating surface plasmon polaritons in gold films.

We demonstrate dual-color nonlinear excitation of quantum dots positioned onto a gold film at distances up to 40 µm away from a micrometer sized focused laser spot. We attribute the observed remote nonlinear signal to the excitation of two independent surface plasmon polariton (SPP) modes excited at the laser spot in the gold film, which subsequently propagate in a collinear fashion to a distant site and provide the surface field required for nonlinear excitation of the target. This scheme decouples the illuminating photon flux from surface plasmon mediated nonlinear excitation of the target, which provides more control of unwanted heating effects at the target site and represents an attractive approach for surface-mediated femtosecond nonlinear examinations of molecules.

Nanoscale chemical imaging by photoinduced force microscopy.

Correlating spatial chemical information with the morphology of closely packed nanostructures remains a challenge for the scientific community. For example, supramolecular self-assembly, which provides a powerful and low-cost way to create nanoscale patterns and engineered nanostructures, is not easily interrogated in real space via existing nondestructive techniques based on optics or electrons. A novel scanning probe technique called infrared photoinduced force microscopy (IR PiFM) directly measures the photoinduced polarizability of the sample in the near field by detecting the time-integrated force between the tip and the sample. By imaging at multiple IR wavelengths corresponding to absorption peaks of different chemical species, PiFM has demonstrated the ability to spatially map nm-scale patterns of the individual chemical components of two different types of self-assembled block copolymer films. With chemical-specific nanometer-scale imaging, PiFM provides a powerful new analytical method for deepening our understanding of nanomaterials.

Molecular orientation in dry and hydrated cellulose fibers: a coherent anti-Stokes Raman scattering microscopy study.

Coherent anti-Stokes Raman scattering (CARS) microscopy is combined with spontaneous Raman scattering microspectroscopy and second harmonic generation (SHG) microscopy to interrogate the molecular alignment in dry and hydrated cellulose fibers. Two types of cellulose were investigated: natural cellulose I in cotton fibers and regenerated cellulose II in rayon fibers. On the basis of the orientation of the methylene symmetric stretching vibration, the molecular alignment of cellulose microfibrils is found to be conserved on the micrometer scale. Whereas the molecular orientation in cotton shows modest variability along the fiber, the alignment of the cellulose units in rayon is highly consistent throughout the fiber. The ordered alignment is retained upon fiber hydration. Upon hydration of the cellulose fibers, an anisotropic electronic contribution is observed, which indicates an ordered incorporation of water molecules into the fiber structure. The third-order and second-order electronic polarizability of cellulose I are directed along the axis of the polyglucan chain. No second-order optical response is observed in cellulose II, supporting the antiparallel arrangement of the polyglucan chains in regenerated cellulose.