Proceedings of nanoGe September Meeting 2015 (NFM15)
Publication date: 8th June 2015
Materials with large two-photon absorption (TPA) are of current interest and highly desirable for many photonic applications. In the wavelength range of 650-1350 nm they can combine deep tissue penetration with the high spacial resolution of two-photon confocal imaging for in-vivo microscopy. We investigate the spectral dependence of the linear and two-photon absorption of wurtzite CdS nanoparticles (dots and rods) by means of quantitative one- and two-photon photoluminescence excitation spectroscopy and effective mass theory modeling. For both geometries we observe a sizable spectral shift between the first one- and two-photon absorption maxima, which we conclude is inherent to the small rates of near-bandgap two-photon transitions rather than to geometry of the absorber. The two-photon spectrum features of rods strongly differ from those of dots, due to the distinct energy structure of quasi-one-dimensional systems. The transversal confinement is found to dominate the energy of the absorption maxima, the longitudinal one dominates their absorption intensity. This suggests two-photon transition energy and intensity can be controlled independently in nanorods. The absolute TPA cross sections are obtained free from spectrally varying beam related uncertainties by means of a new reference dye based method which proves a powerful characterization tool for wavelength dependent measurements of TPA properties of semiconductor nanoparticles, also beyond zero and one-dimensional geometries.
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