个人简介

Education: B.S., 1989, Calvin College; Ph.D., 1994, University of California at Los Angeles Awards: President's Postdoctoral Fellow, 1994; Fulbright Junior Researcher, 1995; NSF CAREER Award, 1998; Research Corporation Innovation Award, 1998; Alfred P. Sloan Research Fellow, 1999; Beckman Young Investigator, 1999; Packard Fellowship in Science and Engineering, 1999; Dreyfus Foundation Teacher-Scholar, 2000; Helen Corley Petit Professor, 2002; UIUC University Scholar, 2004; John D. and Catherine T. MacArthur Foundation Fellow, 2005; American Physical Society Fellow, 2005; American Association for the Advancement of Science Fellow, 2006; Gutgsell Chair in Chemistry, 2006

研究领域

Physical/Theoretical

Quantum chemistry traditionally solves the time-independent, zero temperature electronic Schrödinger equation, assuming separability of the electronic and nuclear degrees of freedom. This provides potential energy surfaces for use in molecular dyna-mics simulations to understand finite temperature and time-dependent effects. We take a different approach-extending quantum chemistry into the time domain, bridging the gap between traditional molecular dynamics (what are the atoms doing?) and quantum chemistry (what are the electrons doing?). We include quantum mechanical effects on the behavior of the electrons and the atoms by simultaneously solving the electronic and nuclear Schrödinger equations. This "ab initio multiple spawning" (AIMS) method opens exciting possibilities in modeling chemistry. Rearrangement of chemical bonds, tunneling, and dynamics on multiple electronic states are all treated correctly without ad hoc assumptions. We are especially interested in electronic excited states, where the assumption of electron-nuclear separability breaks down. Using AIMS, we investigated fundamental photochemical reactions-quenching of excited metal atoms, cis-trans isomerization in ethylene and butadiene, and ring-opening of cyclobutene. In each case we found that conventional explanations required modification. This research furthers the understanding of complex molecular dynamics on multiple electronic states during photochemical reactions. Our goal is AIMS for reactions in complex environments, whether they be normal solvents (e.g., water), solid cages (e.g.,zeolites), or portions of a protein. We are developing methods to address solvent effects on photochemistry and spectroscopy, with ultimate application to biologically relevant molecules such as visual pigments. Because of tunneling effects, proton transfer reactions require quantum treatment of the nuclei. We recently performed the first ab initio molecular dynamics simulation of real-time tunneling dynamics, simulating intramolecular proton transfer in malonaldehyde. Future directions include AIMS studies of coupled electron and proton transfer reactions, which are important in biological systems and possibly for designing molecular electronic devices. Finally, we use novel quantum chemistry methods to elucidate the function of biologically relevant metallo-proteins-currently, the reaction mechanism of cytochrome c oxidase. This final enzyme in the respiratory cycle reduces oxygen. We investigate the nature of spin coupling between transition metal centers, the role of tyrosyl radicals in the mechanism, and the coupling of electron transfer and proton transfer in the enzyme active site.

近期论文

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Diesendruck, Charles E. and Peterson, Gregory I. and Kulik, Heather J. and Kaitz, Joshua A. and Mar, Brendan D. and May, Preston A. and White, Scott R. and Martinez, Todd J. and Boydston, Andrew J. and Moore, Jeffrey S. , Mechanically triggered heterolytic unzipping of a low-ceiling-temperature polymer , Nature Chemistry , 6, (7), 624-629, 2014. [link] Gaenko, Alexander and DeFusco, Albert and Varganov, Sergey A. and Martinez, Todd J. and Gordon, Mark S. , Interfacing the Ab Initio Multiple Spawning Method with Electronic Structure Methods in GAMESS: Photodecay of trans-Azonnethane , Journal of Physical Chemistry A , 118, (46), 10902-10908, 2014. [link] Joalland, Baptiste and Mori, Toshifumi and Martinez, Todd J. and Suits, Arthur G. , Photochemical Dynamics of Ethylene Cation C2H4+ , Journal of Physical Chemistry Letters , 5, (8), 1467-1471, 2014. [link] Luehr, Nathan and Markland, Thomas E. and Martinez, Todd J. , Multiple time step integrators in ab initio molecular dynamics , Journal of Chemical Physics , 140, (8), 2014. [link] Makhov, Dmitry V. and Glover, William J. and Martinez, Todd J. and Shalashilin, Dmitrii V. , Ab initio multiple cloning algorithm for quantum nonadiabatic molecular dynamics , Journal of Chemical Physics , 141, (5), 2014. [link] McFarland, B. K. and Berrah, N. and Bostedt, C. and Bozek, J. and Bucksbaum, P. H. and Castagna, J. C. and Coffee, R. N. and Cryan, J. P. and Fang, L. and Farrell, J. P. and Feifel, R. and Gaffney, K. J. and Glownia, J. M. and Martinez, T. J. and Miyabe, S. and Mucke, M. and Murphy, B. and Natan, A, Experimental strategies for optical pump - soft x-ray probe experiments at the LCLS , Xxviii International Conference on Photonic, Electronic and Atomic Collisions (Icpeac) , 488, 2014. [link] Parrish, Robert M. and Sherrill, C. David and Hohenstein, Edward G. and Kokkila, Sara I. L. and Martinez, Todd J. , Communication: Acceleration of coupled cluster singles and doubles via orbital-weighted least-squares tensor hypercontraction , Journal of Chemical Physics , 140, (18), 2014. [link] Presselt, Martin and Wojdyr, Michal and Beenken, Wichard J. D. and Kruk, Mikalai and Martinez, Todd J. , Steric and electronic contributions to the core reactivity of monoprotonated 5-phenylporphyrin: A DFT study , Chemical Physics Letters , 603, 21-27, 2014. [link] Punwong, C. and Martinez, T. J. and Hannongbua, S. , Direct QM/MM simulation of photoexcitation dynamics in bacteriorhodopsin and halorhodopsin , Chemical Physics Letters , 610, 213-218, 2014. [link] Silberstein, Meredith N. and Cremar, Lee D. and Beiermann, Brett A. and Kramer, Sharlotte B. and Martinez, Todd J. and White, Scott R. and Sottos, Nancy R. , Modeling mechanophore activation within a viscous rubbery network , Journal of the Mechanics and Physics of Solids , 63, 141-153, 2014. [link] Sisto, Aaron and Glowacki, David R. and Martinez, Todd J. , Ab Initio Nonadiabatic Dynamics of Multichromophore Complexes: A Scalable Graphical-Processing-Unit-Accelerated Exciton Framework , Accounts of Chemical Research , 47, (9), 2857-2866, 2014. [link] Virshup, Aaron M. and Levine, Benjamin G. and Martinez, Todd J. , Steric and electrostatic effects on photoisomerization dynamics using QM/MM ab initio multiple spawning , Theoretical Chemistry Accounts , 133, (7), 2014. [link] Wang, Junpeng and Kouznetsova, Tatiana B. and Kean, Zachary S. and Fan, Lin and Mar, Brendan D. and Martinez, Todd J. and Craig, Stephen L. , A Remote Stereochemical Lever Arm Effect in Polymer Mechanochemistry , Journal of the American Chemical Society , 136, (43), 15162-15165, 2014. [link] Wang, Lee-Ping and Martinez, Todd J. and Pande, Vijay S. , Building Force Fields: An Automatic, Systematic, and Reproducible Approach , Journal of Physical Chemistry Letters , 5, (11), 1885-1891, 2014. [link] Wang, Lee-Ping and Titov, Alexey and McGibbon, Robert and Liu, Fang and Pande, Vijay S. and Martinez, Todd J. , Discovering chemistry with an ab initio nanoreactor , Nature Chemistry , 6, (12), 1044-1048, 2014. [link] Wolf, T. J. A. and Kuhlman, T. S. and Schalk, O. and Martinez, T. J. and Moller, K. B. and Stolow, A. and Unterreiner, A. N. , Hexamethylcyclopentadiene: time-resolved photoelectron spectroscopy and ab initio multiple spawning simulations , Physical Chemistry Chemical Physics , 16, (23), 11770-11779, 2014. [link] Hohenstein, Edward G. and Kokkila, Sara I. L. and Parrish, Robert M. and Martinez, Todd J. , Quartic scaling second-order approximate coupled cluster singles and doubles via tensor hypercontraction: THC-CC2 , Journal of Chemical Physics , 138, (12), 2013. [link] Hohenstein, Edward G. and Kokkila, Sara I. L. and Parrish, Robert M. and Martinez, Todd J. , Tensor Hypercontraction Equation-of-Motion Second-Order Approximate Coupled Cluster: Electronic Excitation Energies in O(N-4) Time , Journal of Physical Chemistry B , 117, (42), 12972-12978, 2013. [link] Isborn, Christine M. and Mar, Brendan D. and Curchod, Basile F. E. and Tavernelli, Ivan and Martinez, Todd J. , The Charge Transfer Problem in Density Functional Theory Calculations of Aqueously Solvated Molecules , Journal of Physical Chemistry B , 117, (40), 12189-12201, 2013. [link] Parrish, Robert M. and Hohenstein, Edward G. and Martinez, Todd J. and Sherrill, C. David , Discrete variable representation in electronic structure theory: Quadrature grids for least-squares tensor hypercontraction , Journal of Chemical Physics , 138, (19), 2013. [link]