个人简介

B.S. 1969, Southwestern University Ph.D. 1974, Cornell University John E. Willard and Hilldale Professor Currently on leave to National Science Foundation as Assistant Director, Directorate for Mathematical & Physical Sciences .

研究领域

Physical

Our group studies the dynamics of reaction and photodissociation with the goal of understanding the essential features of chemistry in both gases and liquids. The unifying theme of our research is connecting chemical reaction dynamics occurring in gases to those in liquids. We use both high resolution lasers and ultrafast lasers, and the key to all of our experiments is preparing molecules in vibrationally excited states and spectroscopically monitoring their subsequent behavior. Vibrational excitation is crucial in many chemical reactions because motion of the atoms relative to each other carries the system through the transition state that lies atop the barrier to reaction. Because laser excitation is a particularly attractive means of preparing molecules in specific internal states, our strategy is to excite molecules with a laser pulse and use time-resolved spectroscopy to follow their subsequent behavior. We use high resolution lasers in some experiments and ultrafast lasers, which produce pulses of less than 100 fs duration, in others. The two approaches often provide complementary information and allow us to study some of the same reactions in isolated molecules and in liquids. In the former case, laser excitation prepares a molecular eigenstate that does not evolve in time and whose properties we exploit to control the course of a chemical reaction. In the later case, the short laser pulse prepares a state that does evolve in time and that we intercept at different points in its evolution. This good time resolution allows us to observe processes that occur during a time that is comparable to the interval between the interactions in solution. We use a variety of excitation and detection techniques, such as resonant multiphoton ionization with ion imaging in molecular beams and time-resolved transient absorption or non-linear spectroscopy in liquids. The molecular beam experiments provide an extremely detailed view of the chemical dynamics of isolated, well-characterized molecules. We have exploited our understanding of the behavior of vibrationally excited molecules to control the course of a chemical reaction, and we have used laser excitation to cleave a particular bond selectively in both photodissociation and bimolecular reaction. The ultrafast laser techniques now allow us to follow the flow of energy within a molecule directly and to study vibrationally driven reactions in liquids. Discovering the controlling aspects of chemical reactions at a fundamental level is the focus of our research. The attached list gives a few representative publications

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Probing the Photoisomerization of CHBr3 and CHI3 in Solution with Transient Vibrational and Electronic Spectroscopy. Thomas J. Preston, Michael A. Shaloski, and F. Fleming Crim, J. Phys. Chem. A,, 117 (14), 2899 (2013) Molecular Reaction Dynamics Across the Phases: Similarities and Differences. F. Fleming Crim, Faraday Discussions 157, 1 (2012). The Photoisomerization and Relaxation Dynamics of a Structurally Modified Biomimetic Photoswitch. Adam D. Dunkelberger, Ryan D. Kieda, Jae Yoon Shin, Riccardo Rossi Paccani, Stefania Fusi, Massimo Olivucci, and F. Fleming Crim J. Phys. Chem. A, 116, 3527 (2012) Determining the Dissociation Threshold of Ammonia Trimers from Action Spectroscopy of Small Clusters. Amanda S. Case, Cornelia G. Heid, Colin M. Western, and F. Fleming Crim J. Chem. Phys. 136, 124310 (2012) Formation and Relaxation Dynamics of iso-CH2Cl-I in Cryogenic Matrices. Thomas J. Preston, Maitreya Dutta, Brian J. Esselman, Aimable Kalume, Lisa George, Robert J. McMahon, Scott A. Reid, and F. Fleming Crim J. Chem. Phys. 135, 114503 (2011) Dissociation Energy and Vibrational Predissociation Dynamics of the Ammonia Dimer. Amanda S. Case, Cornelia G. Heid, Scott H. Kable, and F. Fleming Crim J. Chem. Phys. 135, 084312 (2011) Surrounded by Complications. F. Fleming Crim Nature Chem. 3, 344 (2011) Reactive Scattering: Quantum-State-Resolved Chemistry. F. Fleming Crim in Tutorials in Molecular Reaction Dynamics Eds. Mark Brouard and Claire Vallance (Royal Society of Chemistry, London, 2010). The Influence of Vibrational Excitation on the Photoisomerization trans-Stilbene in Solution. Kristin A. Briney, Leslie Herman, David S. Boucher, Adam D. Dunkelberger, and F. Fleming Crim J. Phys. Chem. A, 144, 9788 (2010). Ultrafast Observation of Isomerization and Complexation in the Photolysis of Bromoform in Solution. Stacey L. Carrier, Thomas J. Preston, Maitreya Dutta, Andrew C. Crowther, and F. Fleming Crim J. Phys. Chem. A, 144, 1548 (2010). Time-Resolved Studies of the Reactions of CN Radical Complexes with Alkanes, Alcohols, and Chloroalkanes. Andrew C. Crowther, Stacey L. Carrier, Thomas J. Preston and F. Fleming Crim J. Phys. Chem. A 113, 3758 (2009) Time-Resolved Studies of CN Radical Reactions and the Role of Complexes in Solution. Andrew C. Crowther, Stacey L. Carrier, Thomas J. Preston and F. Fleming Crim J. Phys. Chem. A 112, 12081 (2008) Reaction Dynamics and Vibrational Spectroscopy of CH3D Molecules with Both C-H and C-D Stretches Excited. Christopher J. Annesley, Andrew E. Berke and F. Fleming Crim J. Phys. Chem. A 112, 9448 (2008) The Chemical Dynamics of Vibrationally Excited Methane: Controlling Reactions in Gases and on Surfaces. F. Fleming Crim PNAS 105, 12654 (2008) Vibrationally Mediated Photodissociation of Ammonia: Product Angular Distributions from Adiabatic and Nonadiabatic Dissociation. Michael L. Hause, Y. Heidi Yoon, and F. Fleming Crim Mol. Phys. 106, 1127 (2008) Dynamics at Conical Intersections: The Influence of O-H Stretching Vibrations on the Photodissociation of Phenol. Michael L. Hause, Y. Heidi Yoon, Amanda S. Case and F. Fleming Crim J. Chem. Phys. 128, 104307 (2008) Vibrational Action Spectroscopy of the C-H and C-D Stretches in Partially Deuterated Formic Acid Dimer. Y. Heidi Yoon, Michael L. Hause, Amanda S. Case and F. Fleming Crim J. Chem. Phys. 128, 084305 (2008) Making Energy Count. F. Fleming Crim Science 316, 1707 (2007) Vibrationally Mediated Photodissociation of Ammonia: The Influence of N-H Stretching Vibrations on Passage through Conical Intersections. Michael L. Hause, Y. Heidi Yoon and F. Fleming Crim J. Chem. Phys. 125, 174309 (2006) Mode- and Bond-Selective Reaction of Cl(2P3/2) with CH3D: C-H Stretch Overtone Excitation near 6000 cm-1. Robert J. Holiday, Chan Ho Kwon, Christopher J. Annesley and F. Fleming Crim J. Chem. Phys. 125, 133101 (2006)