研究领域

Biophysical Chemistry Energy Science Materials Chemistry Optics and Imaging Physical Chemistry Sensor Science Ultrafast Dynamics

Our research group utilizes a number of spectroscopic techniques towards investigating the optical properties and applications of novel organic macromolecular materials. A major emphasis is placed on the new properties observed in organic macromolecules with branching repeat structures as well as organic macromolecules encapsulated with small metal particles. These materials have been suggested to be candidates for variety of applications involving light emitting devices, artificial light harvesting, strong optical limiters, enhanced nonlinear optical effects, quantum optical effects and as sensors in certain organic and biological devices. Utilizing steady-state spectroscopy as well as ultra-fast time-resolved fluorescence (Upconversion) and absorption (pump-probe) measurements our research is focused on probing the kinetics of the fast energy redistribution processes that occur in branched (and related) macromolecular structures. With the additional use of fluorescence anisotropy decay measurements, we have characterized the fundamental limits of interaction in different molecular architectures. Investigations of novel larger branched structures (obtained through collaboration) as well as more fundamental investigations (were the synthesis of model compounds is carried in our lab) are used to probe the important structure-function relationships in these systems. These investigators are coupled with measurements of interactions and electronic dephasing in the branched (aggregate) systems with 3-pulse photon echo spectroscopy (3PEPS). This combined approach allows for the analysis of the energy transfer, interaction strength, dephasing, as well as other important physical properties of particular macromolecular systems. The research in the group is also directed at the use of organic branched structures for applications in nonlinear optics as well as quantum optical and quantum interference effects. The investigations of strong interactions in particular multi-chromophore systems suggest that there is a possibility of enhanced transition dipole moments. This has been observed in organic branched structures in our laboratory. New methods, both synthetically and optically to enhance the nonlinear response of organic branched macromolecules are developed in this research effort. These measurements are combined with two-photon-emission and degenerate-four-wave mixing experiments to fully characterize the complete response of novel materials. The initial investigations utilizing organic materials in quantum optical phenomena were carried out in our laboratory. This included measurements of photon number squeezed states of light in an organic polymeric material. The ability to reduce the photon fluctuation below the shot-wave limit is of significant use to those interested in an all optical telecommunication system. The striking result was that the organic material gave rise to the same magnitude of " squeezed light" as was observed for inorganic systems with interactions lengths that was orders of magnitude longer. Our recent investigations in this area include measurements of entangled photon and their use in the spectroscopy of organic materials at low photon-number as well as other novel quantum interference effects with organic materials.

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Clark, T. B.; Schatz, G.; Goodson, III. T.“Two-Photon Spectroscopy as a New Sensitive Probe for Secondary Structure Determination in Amyloid-b Peptides and Aggregates”, Proc. Nat. Acad. Sci., 2013, (submitted) Orr, M.; Goodson, III. T.“The Photophysical Explanation of the High Efficency: PTB-7 Polymer”, J. Phys. Chem. C, 2013, (submitted) Raymond, J.; Ogawa, S.; Kubuke, Y.; Baskar, A.; Goodson, III. T.“Ultrafast Spectroscopic Investigations of Porphyrin Macrosysles”, J. Phys. Chem. C, 2013, (submitted) McLean, A. M.; Socher, E.; Varnavski, O.; Cleark, T. B.; Imperiali, B.; Goodson, III. T.“Two-Photon Fluorescence Spectroscopy and Imaging of 4-Dimethylaminonaphthalimide Peptide and Protein Conjugates”, J. Phys. Chem. B.2013, Asap Adegoke, O. O.; Ince, M.; Mishra, A.; Green, A.; Varnavski, O.; Martinez-Diaz, M. V.; Bauerle, P.; Torres, T.; Goodson, III. T.“Synthesis and Ultrafast Time Reseolved Spectroscopy of Peripherally Functionalized Zine Phthalocyanine Bearing Oligothienylene-ethynylene Subunits”, J. Phy. Chem. C, 2013, 117, 20912-20918 Furgal, J. C .; Jung, J. H.; Clark, S.; Goodson, III. T.“Beads on a Chain (BoC) Phenylsilsesquioxane (SQ) Polymers via F- Catalyzed Rearrangements and ADMET or Resverse Heck Cross-couping REactions: Through Chain, Extended Conjugation in 3-D with Potential for Dendronization”, MACROMOLECULES, 2013, 46, 7591-7604 Furgal, J. C .; Jung, J. H.; Goodson, III. T.; Laine, R. M. “Analyzing Structure-Photophysical Property Relationships for Isolated T-8, T-10, and T-12 Stilbenevinylsilsesquioxanes”, J. of Am. Chem. Soc., 2013, 135, 12259-12269 Goodson, III. T.“Recent Advances in Designing Molecuar Assemblies”, J. Phys Chem. Letts., 2013, 4, 2705-2706 Upton, L.; Goodson, III. T.“Optically Excited Entangled States in Organic Molecules Illuminate the Dark”, J.Phys. Chem. Letts, 2013, 12, 2046-2052 Yau, S. H.; Varnavski, O.; Goodson, III. T.“An Ultrafast Look at Au Nanoclusters”, Accts. of Chem. Res 2013, 46, 1506-1516 Oliva, M.M.; Juarez, R.;Segura, J.; Van Cleuvenbergen, s.; Clays, K.; Goodson, T. "Linear and Nonliner Optical Properties of Ramified Hexaazatriphenylenes: Charge Tranfer Contributions to the Octupolar REsponse"" J. Phy. Chem. C. 2013, 117, 626-632 Zhang, J.; Fischer, M.K.R.; Bauerle, P.; Goodson, III. T.“Energy Migration in Dendritic Oligothiophene-perylene Bisimides”, J. Phys. Chem. B. 2013, 16, 4204-4215 Special Issue Furgal, J.C.; Jung, J.H.; Mizmuo, T.; Chou, K.; Schwartz, M.; Goodson, III. T.; Laine, R. M.“The Chemistry and Photophysical Properties of Conjugated Organic Functionalized T10/12 Silsesquioxanes”, ACS, Division of Polymer Chemistry, 2012, 53(1)1, 15-16 Jung, J. H.; Furgal, J.C.; Goodson, III. T.; Mizumo, T.; Schwartz, M.; Chous, K.; Vonet, J-F.; Laine, R. M.“3-D Molecular Mixtures of Catalytically Functionalized [vinylSiO1.2]10/[vinylSio1.5]12. Photophysical Characterization of Second Generation Derivatives”, Chem. of Materials, 2012, 24, 1883-1895 Phillips, H.; Zheng, S. H.; Hyla, A.; Laine, R. M.; Goodson, III. T.; Geva, E.; Dunietz, B. D. “Ab Initio Calculation of the Electronic Absorption of Funcationalized Octahedral Silsesquioxanes via Time-Dependent Density Functional Theory with Range-Seperated Hybrid Functionals”, J. of Phy. Chem. A, 2012, 116, 1137-1145 Yau, S.H.; Goodson, III. T.“Bright Two-Photon Emission and Ultrafast Relazation Dynamics in a DNA-Templated Nanocluster Investigated by Ultra-fast Spectroscopy”, Nanoscale2012, 4, 4247-4254 Philips, H.; Zheng, S.; Hyla, A.; Laine, R.; Goodson, III. T.; Geva, E.; Dunietz, B.“Ab Initio Calculations of the Electronics Absorption of Functionalized Octahedral Silsequioxanes via Time-Dependent Density Functional Theory with Range-Separated Hybird Functions”, J. Phy. Chem. A., 2012, 116, 1137-1145 Guo, M.; Hayakawa, T.; Kakimoto, N.; Goodson, III. T. “Organic Macromoecular high dielectric Constant Materials”, J. Phy. Chem. B., 2011, 115, 13419-13432 Goodson, III. T. “Understanding the Inricacies of Organic Photovoltaics”, J. Phy. Chem. Lett., 2011, 24, 3146 Raymond, J. E; Casado, J; Lopez, N; Juan, T; Takimiya, K; Goodson, III, T; “Two-Photon Mediated Three-Photon Flourscence: Lessons from a Quinoidal oligothiophene Dimer”, J. Phy. Chem. Lett., 2011, 17, 2179-2183