Many challenging problems in the modern science and technology are related to preparation, properties, and utilization of novel functional materials. The polymer chemistry and the chemical microelectronics programs represent parts of the multidisciplinary effort in this field. The many-pronged approach includes: synthesis and molecular characterization of well-defined block and graft copolymers; preparation of new engineering thermoplastics and liquid crystalline materials; synthesis, modification and processing of polymers in super-critical carbon dioxide; chemical design of hybrid polymers for catalysis and photoredox activity, polymers for microelectronics applications including 193 nm and 157 nm photoresists and low-k dielectrics, and defined microstructures.
Chemical microelectronics is focused on preparation of organic and inorganic electronic materials; microscopic patterning of thin films using novel techniques, plasma, ion beam, laser beam, etc.; kinetics of etching and film formation; characterization of mechanical, electronic, and optical properties; spatially resolved chemical analysis of surfaces, interfaces, and thin films and microstructures. A broad variety of expertise includes visualization and probing of submicrometer surface structures by scanning probe microscopy, characterization of polymer dynamics by NMR techniques and light scattering, measurement of molecular conductivity, and analytical as well as computational and numerical methods in polymers.
Nanoparticle (NP) drug loading is one of the key defining characteristics of an NP formulation. However, the effect of NP drug loading on therapeutic efficacy and pharmacokinetics has not been thoroughly evaluated. Published in Biomaterials, researchers in the DeSimone Group, characterize the efficacy, toxicity and pharmacokinetic properties of NP docetaxel formulations that have differential drug loading but are otherwise identical.
Particle Replication in Non-wetting Templates, PRINT®, a soft-lithography fabrication technique, was used to formulate NPs with identical size, shape and surface chemistry, but with variable docetaxel loading. The lower weight loading (9%-NP) of docetaxel was found to have a superior pharmacokinetic profile and enhanced efficacy in a murine cancer model when compared to that of a higher docetaxel loading (20%-NP). The 9%-NP docetaxel increased plasma and tumor docetaxel exposure and reduced liver, spleen and lung exposure when compared to that of 20%-NP docetaxel.
Published in Molecular Pharmaceutics, scientists in the DeSimone Group report on the development of a nonviral lipid-complexed PRINT, Particle Replication in Nonwetting Templates, protein particle system, LPP particle, for RNA replicon delivery with a view toward RNA replicon-based vaccination. Cylindrical bovine serum albumin, BSA, particles with a diameter, d, of 1 μm, height, h, 1 μm, loaded with RNA replicon and stabilized with a fully reversible disulfide cross-linker were fabricated using PRINT technology.
Highly efficient delivery of the particles to Vero cells was achieved by complexing particles with a mixture of 1,2-dioleoyl-3-trimethylammonium-propane (DOTAP) and 1,2-dioleoyl-sn-glycero-3-phosphoethanolamine (DOPE) lipids. Our data suggest that (1) this lipid-complexed protein particle is a promising system for delivery of RNA replicon-based vaccines and (2) it is necessary to use a degradable cross-linker for successful delivery of RNA replicon via protein-based particles.
Self-Healing of Unentangled Polymer Networks with Reversible Bonds. Evgeny B. Stukalin, Li-Heng Cai, N. Arun Kumar, Ludwik Leibler, and Michael Rubinstein. Macromolecules, 2013, 46 (18), pp 7525–7541.
Nonflammable Perfluoropolyether-Based Electrolytes for Lithium Batteries. Dominica H. C. Wong, Jacob L. Thelen, Yanbao Fu, Didier Devaux, Ashish A. Pandya, Vincent S. Battaglia, Nitash P. Balsara, and Joseph M. DeSimone. PNAS, Online: DOI10.1073/pnas.1314615111.
Synthetically Encoding 10 nm Morphology in Silicon Nanowires. Joseph D. Christesen, Christopher W. Pinion, Erik M. Grumstrup, John M. Papanikolas, and James F. Cahoon. Nano Lett., 2013, 13 (12), pp 6281–6286.
Nanoparticle Drug Loading as a Design Parameter to Improve Docetaxel Pharmacokinetics and Efficacy. Kevin S. Chu, Allison N. Schorzman, Mathew C. Finniss, Charles J. Bowerman, Lei Peng, James C. Luft, Andrew J. Madden, Andrew Z. Wang, William C. Zamboni, Joseph M. DeSimone. Biomaterials, Volume 34, Issue 33, November 2013, Pages 8424–8429.
RNA Replicon Delivery via Lipid-Complexed PRINT Protein Particles. Jing Xu, J. Christopher Luft, Xianwen Yi, Shaomin Tian, Gary Owens, Jin Wang, Ashley Johnson, Peter Berglund, Jonathan Smith, Mary E. Napier, and Joseph M. DeSimone. Mol. Pharmaceutics, 2013, 10 (9), pp 3366–3374.
Real Function of Semiconducting Polymer in GaAs/Polymer Planar Heterojunction Solar Cells. Liang Yan and Wei You. ACS Nano, 2013, 7 (8), pp 6619–6626.
Near-Infrared Activation of Semi-Crystalline Shape Memory Polymer Nanocomposites. Duy M. Le, Michael A. Tycon, Christopher J. Fecko, Valerie S. Ashby. JAPS, Online, 27 JUL, 2013, DOI: 10.1002/app.39604.
Identifying Champion Nanostructures for Solar Water-Splitting. Scott C. Warren, Kislon Voïtchovsky, Hen Dotan, Celine M. Leroy, Maurin Cornuz, Francesco Stellacci, Cécile Hébert, Avner Rothschild & Michael Grätzel. Nature Materials (2013) doi:10.1038/nmat3684.
Scalable Manufacture of Built-to-Order Nanomedicine: Spray-Assisted Layer-by-Layer Functionalization of PRINT Nanoparticles. Stephen W. Morton, Kevin P. Herlihy, Kevin E. Shopsowitz, Zhou J. Deng, Kevin S. Chu, Charles J. Bowerman, Joseph M. DeSimone, Paula T. Hammond. Advanced Materials, online, July 1, 2013. DOI: 10.1002/adma.201302025.
Perfect Mixing of Immiscible Macromolecules at Fluid Interfaces. Sergei S. Sheiko, Jing Zhou, Jamie Arnold, Dorota Neugebauer, Krzysztof Matyjaszewski, Constantinos Tsitsilianis, Vladimir V. Tsukruk, Jan-Michael Y. Carrillo, Andrey V. Dobrynin & Michael Rubinstein . Nature Materials (2013) doi:10.1038/nmat3651.