Jeffrey G. Winiarz

Photogeneration, charge transport, and photoconductivity of a novel PVK/CdS-nanocrystal polymer composite

Abstract We report on the photoconductive characteristics of an inorganic:organic hybrid composite in which PVK serves as a polymeric charge-transporting matrix and quantum dots composed of surface passivated cadmium sulfide serve as a charge-generating sensitizer. The PVK:CdS nanocomposites prepared are directly compared with a similar composite composed of PVK and C60, an extensively studied system due to its promising characteristics. We demonstrate the possibility of tuning the band-gap of these sensitizing nanocrystals through careful discretion in the method of synthesis such that their spectral response can be adjusted to suit a particular wave-length of operation. In this way materials can be fabricated which posses photoconductive characteristics exceeding those observed in the PVK:C60 system. In this paper results concerning photosensitivity will be presented and the Onsager formalism developed for organic systems will be employed in order to extract the parameters r0 and Φ0 from the photocharge generation efficiency data.

Charge carrier mobility in an organic-inorganic hybrid nanocomposite

This study was supported by a NSF, DMR Solid State and Polymer Chemistry Grant No. DMR0075867. Partial support by a Defense Research Initiative on Nanotechnology (DURINT), Contract No. F496200110358, through the Directorate of Chemistry and Life Sciences of the Air Force Office of Scientific Research is also acknowledged.

Temperature-dependence studies of photorefractive effect in a low glass-transition-temperature polymer composite

The temperature dependence of the photorefractive effect in a polymer composite containing poly(9-vinycarbazole), tricresyl phosphate, buckminsterfullerene, and 4-(N,N- diethylamino)-β-nitrostyrene is presented. The photoconductive, electro-optic and photorefractive properties of the material have been studied in the temperature range of 22–61 °C. An apparent increase of electro-optic modulation with temperature and its eventual saturation is observed. This behavior is attributed to the temperature activated orientational mobility of the second-order nonlinear chromophores. The polarization anisotropy between the p- and s-polarized readouts is consistent with what would be expected on the basis of directly measured effective electro-optic coefficients. By correlating the electro-optic value with the diffraction efficiency, the temperature dependence of the space-charge field is obtained and explained by temperature dependencies of the dark conductivity and the photoconductivity of the material.

Second-harmonic and sum-frequency imaging of organic nanocrystals with photon scanning tunneling microscope

Second-harmonic generation and sum-frequency generation with photon scanning tunneling microscopy and shear-force detection are used to map the nonlinear optical response and the surface topograph of N-(4-nitrophenyl)-(L)-prolinol crystals with a subdiffraction-limited resolution. The domain-size dependence of the spatial feature is obtained, which shows the local orientational distribution of the optical near field radiated by nonlinear nanocrystals and reveals the difference between nanoscopic and macroscopic second-order optical nonlinearities of molecular crystals.

Photorefractive inorganic–organic polymer-dispersed liquid-crystal nanocomposite photosensitized with cadmium sulfide quantum dots

We report on a new photorefractive medium consisting of a hole-transporting polymer composite matrix, electro-optically active nanodroplets of liquid crystals, and cadmium sulfide quantum dots as photosensitizers. This medium exhibits greater than 90% internal diffraction efficiency and a net two-beam coupling gain of 22.5 cm(-1) with a response time of <1 min . Data on optical transmission are also presented.

Nanoscopic study of second-harmonic generation in organic crystals with collection-mode near-field scanning optical microscopy

Collection-mode near-field scanning optical microscopy (NSOM) is used to map nanoscopic second-harmonic generation (SHG) in N -(4-nitrophenyl)- (L) -prolinol crystals. A spatial resolution of 98 nm is achieved. Near-field polarization-dependent SHG measurement is performed, and a local effective SHG susceptibility of 224+/-18 pm/V is obtained.

Dynamic correction of a distorted image using a photorefractive polymeric composite

We demonstrate, for the first time, the dynamic correction of aberrated images in real-time using a polymeric composite with fast response times. The current novel experimental design is capable of restoring a phase aberrated, image carrying laser beam, to nearly its original quality. The ability to reconstruct images in real-time is demonstrated through the changing of the aberrating medium at various speeds. In addition, this technique allows for the correction of images in motion, demonstrated through the oscillatory movement of the resolution target. We also have demonstrated that important parameters of the materials in the study such as response times, diffraction efficiencies and optical gains all retain high figures of merit values under the current experimental conditions.

Beam Cleanup and Image Restoration with a Photorefractive Polymeric Composite

We demonstrate, for the first time to our knowledge, the use of a photorefractive polymeric composite to clean a phase-distorted laser beam and reconstruct a badly distorted image. Advantageous qualities including relatively high figures of merit, ease of processability, and low cost make this class of materials attractive when compared with their inorganic crystalline counterparts. In addition, we used four-wave-mixing and holographic techniques to obtain an internal diffraction efficiency of approximately 31% at 54.5 V/micron and a two-beam-coupling gain coefficient of gamma = 17 cm-1 at 54.5 V/micron under our experimental conditions.

Nanophotonics: Nanoscale Optical Science and Technology

Nanophotonics defined as nanoscale optical science and technology is a new frontier, which includes nanoscale confinement of radiation, nanoscale confinement of matter, and nanoscale photophysical or photochemical transformation. Selected examples of our research work in each of these areas are presented here. Nonlinear optical interactions involving nanoscale confinement of radiation is both theoretically and experimentally studied using a near-field geometry. The effort in nanoscale confinement of optical domains is focused to control excitation dynamics and energy transfer as well as to produce photon localization using nanostructured rare-earth doped glasses and novel inorganic-organic photorefractive nanocomposites. Spatially localized photochemistry using a near-field two-photon excitation is being developed for nanofabrication and nanoscale memory.