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My research group is exploring a variety of topics, that range from the basic understanding of chemical reaction dynamics to the nature of the chemical contents of single cells.
Under thermal conditions nature seems to hide the details of how elementary reactions occur through a series of averages -- averages over reagent velocity, internal energy, impact parameter, and orientation. To discover the effects of these variables on reactivity, it is necessary to carry out studies of chemical reactions far from equilibrium in which the states of the reactants are more sharply restricted and can be varied in a controlled manner. This poses a tough experimental challenge that we are trying to meet through a number of laser techniques -- techniques that prepare reactants in specific quantum states and probe the quantum state distributions of the resulting products. It is our belief that such state-to-state information gives the deepest insight into the forces that operate in the breaking of old bonds and the making of new ones.
Space does not permit a full description of these projects, and I earnestly invite correspondence. The following examples are representative:
The simplest of all neutral bimolecular reactions is the exchange reaction H + H2 ---> H2 + H. We are studying this system and various isotopic cousins using a tunable UV laser pulse to photodissociate HI (DI) and hence create "fast" H ( D) atoms of known translational energy in the presence of H2 and/or D2 and using a laser multiphoton ionization time-of-flight mass spectrometer to detect the nascent molecular products in a quantum-state-specific manner. It is expect ed that these product state distributions will provide a key test of the adequacy of various advanced theoretical schemes for modeling this reaction.
Another experiment involves preparing molecular ions with a known degree of internal excitation through resonant-enhanced multiphoton ionization and then studying selected ion-molecule reactions as a function of the ion's translational and internal energy. We are also investigating photoionization dynamics by measuring the angular distributions of rotationally resolved photoelectrons. Analytical efforts involve the use of capillary zone electrophoresis and two-step laser desorption laser multiphoton ionization mass spectrometry. We believe these two methods can revolutionize trace analysis, particularly of biomolecules. Particular attention is being focused on the organic species found in meteorites and on the neuropeptides found in large snail neurons.
1. "Probing Individual Molecules with Confocal Fluorescence Microscopy," S. Nie, D.T. Chiu, and R.N. Zare, Science 266, 1018-1021 (1994).
2. "Photoionization Dynamics of the NO A2sigma+ State Deduced from Energy- and Angle-Resolved Photoelectron Spectroscopy," H. Park and R.N. Zare, J. Chem. Phys., 99, 6537-6544 (1993).
3. "Picturing the transition-state region and understanding vibrational enhancement for the Cl+CH4 ---> HCl+CH3 reaction," W.R. Simpson, T.P. Rakitsis, S.A. Kandel, T. Lev-On, and R.N. Zare, J. Phys. Chem, 100, 7938-7947 (1996).
4. "Single Cells as Biosensors for Chemical Separations," J.B. Shear, H.A. Fishman, H.L. Allbritton, D. Garigan, R.N. Zare, and R.H. Scheller, Science 267, 74-77 (1995).
5. "Identification of Complex Aromatic Molecules in Individual Interplanetary Dust Particles," S.J. Clemett, C.R. Maechling, R.N. Zare, P.D. Swan, and R.M. Walker, Science, 262, 721-725 (1993).
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