个人简介
Thai grew up in the state of Tamil Nadu in India, where he spent early childhood near the city of Tirunelveli and his college years in the beautiful temple city of Madurai. He obtained his Bachelors and Masters degrees in Chemistry from The American College in Madurai. Following this, he obtained his Ph.D. degree working in organolithium chemistry, under the guidance of Professor Peter Beak at the University of Illinois at Urbana-Champaign. After a postdoctoral stint with Professor Seth R. Marder at the California Institute of Technology, working on developing optoelectronic materials, he started his independent career as an Assistant Professor at Tulane University. After four years at Tulane, he moved the lab to the University of Massachusetts Amherst in 2003.
研究领域
Supramolecular Disassembly
Supramolecular assemblies, especially those that can be achieved in aqueous media, have been attractive as these should be capable of non-covalently encapsulating guest molecules in one environment and releasing them in another. If this change in environment is relevant to the differences encountered in health vs. disease tissues, then the implications are even higher. Considering these, there have been great advances in designing stimuli-sensitive supramolecular assemblies. However, these have mainly focused on secondary imbalances in biology (e.g. pH, temperature, redox conditions, etc.). Since primary imbalances in biology involve a change in protein activity, generating supramolecular assemblies that respond to proteins is exciting. Our goal is to obtain a better understanding of the structural factors that control the assembly/disassembly events in response to the concentration of a specific protein or the activity of an enzyme. The structural requirements for achieving control over these assembly/disassembly events are quite stringent. Using our custom-designed small molecule amphiphiles, facially amphiphilic dendrimers and amphiphilic homopolymers, we take a concerted approach to achieve controlled disassembly of well-defined amphiphilic assemblies in response to a specific protein stimulus, providing insight into the structural underpinnings of supramolecular disassembly.
Responsive Nanomaterials
Nanomaterials that predictably respond to an external stimulus or a combination of stimuli are of great interest, because of their implications in a rather broad range of applications. The primary design challenge concerns two factors: input (stimulus or stimuli) and output (response). For example, one could design materials that are responsive to pH changes, yielding a response in the form of a molecular release. The ability to tailor the molecular design to achieve materials that respond to a broad range of inputs, yielding a broad range of outputs has significant implications in a variety of areas. When focusing on an application, although our primary design will provide the fundamental structure-property relationship handles, secondary design challenges emerge. In drug delivery, for example, the molecular design needs to account for factors such as encapsulation stability, drug loading capacity, and biocompatibility. Within drug delivery, there are tertiary design challenges, dictated by the specific disease targeted. In our group, we are focused on developing generalized principles that underlie responsive molecular assemblies and the resultant materials. By addressing the primary design challenge, we have developed and are developing capabilities to tackle a broad range of challenges including drug delivery, diagnostics, and sensing. Prominent examples of materials developed in our group for this purpose include a novel self-crosslinking polymeric nanogel for drug delivery and kinetically-trapped amphiphilic homopolymers for sensing in complex milieu
Molecule and Materials for Harnessing Solar Energy
Organic photovoltaics undergo four fundamental processes to convert sunlight to electrical energy: exciton generation (light absorption), exciton dissociation resulting in free charges (charge separation), charge migration (charge transport), and charge collection. The area of organic photovoltaics has been a challenging prospect for the chemical community, because well-defined molecular design algorithms do not exist to concurrently optimize all the four processes mentioned above. In our group, we take a systematic approach to make in-roads into this problem. For example, systematic structure-property relationship studies with polymers are inherently complicated, because of the heterogeneity of the samples that one obtains during syntheses. On the other hand, designing molecules that preserve supramolecular organization for charge separation and charge transport, while also exhibiting broad light absorption is also a challenge. We are beginning to address these issues by starting with building blocks that are inherently low energy absorbers (e.g. BODIPY). Our earlier contributions in this have revolved around optimizing the early events (light absorption and charge separation) in macromolecules such as dendrimers and polymers. Our current work combines our earlier findings (as well as others’) to develop a unified set of molecular design guidelines for organic photovoltaics.
近期论文
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Gao, J.*; Prachyathipsakul, T.*; Thayumanavan, S. “Multichannel Dual Protein Sensing Using Amphiphilic Supramolecular Assemblies” Chem. Commun., 2021, Accepted Manuscript. (DOI:10.1039/D1CC05407D)
Lionello, C.; Gardin, A.; Cardellini, A.; Bochicchio, D.; Shivrayan, M.; Fernandez, A.; Thayumanavan, S.; and Pavan, G.M. “Toward Chemotactic Supramolecular Nanoparticles: From Autonomous Surface Motion Following Specific Chemical Gradients to Multivalency-Controlled Disassembly” ACS Nano, 2021, 15, 10, 16149-16161 . (DOI:10.1021/acsnano.1c05000)
Nandi, D.; Shivrayan, M.; Gao, J.; Krishna, J.; Das, R.; Liu, B.; Thayumanavan, S.; and Kulkarni, A. “Core Hydrophobicity of Supramolecular Nanoparticles Induces NLRP3 Inflammasome Activation” ACS Appl. Mater. Interfaces, 2021, 13, 38, 45300-45314. (DOI:10.1021/acsami.1c14082)
Liu, H.; Prachyathipsakul, T.; Koyasseril-Yehiya, T.M.; Le, S.P.; Thayumanavan, S. “Molecular bases for temperature sensitivity in supramolecular assemblies and their applications as thermoresponsive soft materials” Mater. Horiz., 2021, Advance Article. (DOI:10.1039/D1MH01091C)
Gao, J.; Le, S.; Thayumanavan, S. “Enzyme Catalysis in Non-Native Environment with Unnatural Selectivity using Polymeric Nanoreactors” Angew. Chem. Int. Ed., 2021, Accepted Article. (DOI:10.1002/anie.202109477)
Liu, H.; Westley, J.; Thayumanavan, S. “Excimer-monomer fluorescence changes by supramolecular disassembly for protein sensing and quantification” Chem. Commun., 2021, Advanced Article. (DOI:10.1039/D1CC03944J)
Cao, R.; Gao, J.; Thayumanavan, S.; Dinsmore, A.D. “Triggered interactions between nanoparticles and lipid membranes: design principles for gel formation or disruption-and-release” Soft Matter, 2021, Advance Article. (DOI:10.1039/D1SM00864A)
Anson, F.; Thayumanavan, S.; Hardy, J.A. “Exogenous Introduction of Initiator and Executioner Caspases Results in Different Apoptotic Outcomes” JACS Au, 2021 . (DOI:10.1021/jacsau.1c00261)
Dutta, K.; Das, R.; Medeiros, J.; Kanjilal, K.; Thayumanavan, S.“Charge-Conversion Strategies for Nucleic Acid Delivery” Adv. Funct. Mater., 2021, 31, 2011103. (DOI:10.1002/adfm.202011103)
Liu, H.; Lionello, C.; Westley, J.; Cardellini, A.; Huynh, U.; Pavan, G.M.; Thayumanavan, S. “Understanding functional group and assembly dynamics in temperature responsive systems leads to design principles for enzyme responsive assemblies” Nanoscale, 2021 , Advance Article . (DOI:10.1039/D1NR02000E)
Liu, B.; Singh, K.; Gong, S.; Canakci, M.; Osborne, B.A.; Thayumanavan, S. “Protein-Antibody Conjugates (PACs): A Plug-and-Play Strategy for Covalent Conjugation and Targeted Intracellular Delivery of Pristine Proteins” Angew. Chemie. Int. Ed., 2021 , 60, 12813-12818 . (DOI:10.1002/anie.202103106)
Anson, F.; Liu, B.; Kanjilal, P.; Wu, P.; Hardy, J. A.; Thayumanavan, S. “Evaluating Endosomal Escape of Caspase-3-Containing Nanomaterials Using Split GFP” Biomacromolecules, 2021 , In Press. . (DOI:10.1021/acs.biomac.0c01767)
Dutta, K.; Das, R.; Medeiros, J. M.; Thayumanavan, S. “”Disulfide Bridging Strategies in Viral and Non-viral Platforms for Nucleic Acid Delivery” Biochemistry, 2021, In Press. . (DOI:10.1021/acs.biochem.0c00860)
Gopalakrishnan, S.; Pan, S.; Fernandez, A.; Lee, J.; Bai, Y.; Wang, L-S.; Thayumanavan, S.; Duan, X.; Rotello, V. M. “Hypersound-Assisted Size Sorting of Microparticles on Inkjet-Patterned Protein Films” Langmuir, 2021, 37 , In Press. . (DOI:10.1002/pro.3992)
Anson, F.; Kanjilal, P.; Thayumanavan, S.; Hardy, J. “Tracking Exogenous Intracellular Casp-3 Using Split GFP” Prot. Sci., 2020, 30 , 366-380 . (DOI:10.1002/pro.3992)
Liu, B.; Thayumanavan, S. “Mechanistic Investigations on the Oxidative Degradation of ROS Responsive Thio-Acetal/-Ketal Moieties and Their Implications” Cell Rep. Phys. Sci., 2020,1, 100271. (DOI:10.1016/j.xcrp.2020.100271)
Dutta, K.; Kanjilal, P.; Das, R.; Thayumanavan, S. “Synergistic Interplay of Covalent and Non-Covalent Interactions in Reactive Polymer Nanoassembly Facilitates Intracellular Delivery of Antibodies” Angew. Chem. Int. Ed., 2020, 59, 2-12 . (DOI: 10.1002/anie.202010412)
Koyasseril-Yehiya, T. M.; García-Heredia, A.; Anson, F.; Rangadurai, P.; Siegrist, M. S.; Thayumanavan, S. “Supramolecular Antibiotics: A Strategy for Conversion of Broad-Spectrum to Narrow-Spectrum Antibiotics for Staphylococcus aureus” Nanoscale, 2020, 12, 20693-20698 . (DOI: 10.1039/D0NR04886K)
Jiang, Z.; He, H.; Liu, H.; Thayumanavan, S. “Azide-terminated RAFT Polymers for Biological Applications” Curr. Protocols Chem. Biol., 2020, 12, e85 . (DOI: 10.1002/cpch.85)
Gao, J.; Dutta, K.; Zhuang, J.; Thayumanavan, S. “Cellular and subcellular targeted delivery using a simple all-in-one polymeric nanoassembly” Angew. Chem. Int. Ed., 2020, 59, 23466-23470 . (DOI: 10.1002/anie.202008272)
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