Hostname: page-component-586b7cd67f-l7hp2 Total loading time: 0 Render date: 2024-11-25T16:52:20.394Z Has data issue: false hasContentIssue false

Femtosecond Spectroscopy of Chemically Reactive Solids: a Methodology

Published online by Cambridge University Press:  15 February 2011

Weining Wang
Affiliation:
Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA 02139
Marc M. Wefers
Affiliation:
Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA 02139
Keith A. Nelson
Affiliation:
Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA 02139
Get access

Abstract

An experimental methodology for recording femtosecond time-resolved observations of irreversible change in solids is described. The central problem posed is that the trime-dependent evolution must be observed on a single-shot (i.e. real-time) basis since the sample may be permanently altered after each excitation event. Preliminary demonstrations of real-time femtosecond spectroscopic observations are presented. In addition, one-shot data acquisition techniques open up the possibility of excitation intensities that greatly exceed optical damage threshholds of most samples. Since only one excitation pulse is used, cumulative damage mechanisms may be circumvented. Even if the sample is damaged in a single shot, in some cases the events of interest may be observed before damage occurs. The use of timed sequences of high-intensity excitation pulses to drive large-amplitude, coherent lattice vibrations is discussed. If successful, such large-amplitude lattice vibrations could assist crystalline chemical reactions or structural phase transitions.

Type
Research Article
Copyright
Copyright © Materials Research Society 1993

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

1. See for example The Chemical Bond, Zewail, A.H., ed. (Academic Press, 1992).Google Scholar
2. Many examples are presented in Fleming, G.R., Chemical Applications of Ultrafast Spectrosop (Oxford, 1986).Google Scholar
3. Desiraju, G.R., ed., Organic Solid State Chemistry, (Elsevier, 1987).Google Scholar
4. Williams, L.R. and Nelson, K.A., J. Chem. Phys. 87, 7346 (1987).Google Scholar
5. Tokizaki, T. et al. , Proc. of Eighth Int'l Conf. on Ultrafast Phenomena, Martin, J.L., Migus, A., Mourou, G.A., and Zewail, A.H. (Springer-Verlag), in press.Google Scholar
6. Kosloff, R, and Dell Hammerich, A., and Tannor, D, Phys. Rev. Lett., submitted.Google Scholar
7. Yan, Y.-X., Gamble, E.B. Jr., and Nelson, K.A., J. Chem. Phys. J 8, 3591 (1985).Google Scholar
8. DeSilvestri, S., Fujimoto, J.G., Ippen, E.P., Gamble, E.B. Jr., Williams, L.R., and Nelson, K.A., Chem. Phys. Lett. 116., 146 (1985).Google Scholar
9. Weiner, A.M., Leaird, D.E., Wiederrecht, G.P., and Nelson, K.A., Science 247, 1317 (1990).CrossRefGoogle Scholar
10. Dougherty, T.P. et al. , Science 258,770 (1992).Google Scholar
11. Wiederrecht, G.P., Dougherty, T.P., Dhar, L., Nelson, K.A., Weiner, A.M., and Leaird, D.E., in preparation.Google Scholar
12. Weiner, A.M., Leaird, D.E., Patel, J.S., and Wullert, J.R., IEEE J. Quan. Elec. 28 908 (1992).Google Scholar
Weiner, A. M., Heritage, J. P., and Kirschner, E. M., J. Opt. Soc. Amer. B, 5. 1563 (1988).Google Scholar
13. Dougherty, T.P. et al. , Phys. Rev. B, submitted.Google Scholar
14. Fourkas, J.T., Wang, W., Nelson, K.A., and Trebino, R., in preparation.Google Scholar