Abstract
This paper describes a new class of techniques, called time-delayed laser saturation spectroscopy, which combine frequency and time-domain methods of laser spectroscopy to provide a way of studying a molecular system as it evolves from an initially-prepared stationary state to a second, final state. The specific example analyzed here is three-level free induction decay, in which the time dependent gain of a Doppler-broadened molecular transition is probed after the sudden termination of an intense field resonating with a coupled transition. The calculated lineshape features expected under different experimental conditions are described, and some of these are demonstrated in NH3. The experiments clearly separate the contributions of population saturation and Raman-type processes in the time evolution of the lineshapes, and yield the first measurement of the alignment relaxation rate in the ground electronic state of a molecule.
Supported in part by NSF and ARO (Durham).
This work was performed while the author was a Visiting Scientist at MIT.
Alfred P. Sloan Research Fellow.
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References
See e.g. V.S. Letokhov and V.P. Chebotayev, Nonlinear Laser Spectroscopy, Springer Series in Optical Sciences, Vol. 4, (Springer-Verlag, 1977 ).
See the contribution by R.G. Brewer in this volume.
A time-delayed Lamb dip experiment has been performed using a pulsed dye laser to produce counter-propagating beams: T.W. Hänsch, I.S. Shahin and A.L. Shcawlow, Phys. Rev. Lett. 27, 707 (1971). It should be noted that pulsed lasers are not ideal for such studies. The present approach has the advantage that the system can be prepared in a well defined steady state, and the weak c.w. field can precisely probe its decay. The importance of studying both co- and counter-propagating change signals is also emphasized.
M. Ducloy and M.S. Feld, J. de Phys.-Lettres (Paris) 37, L173 (1976);
M. Ducloy, J. Leite, R. Sheffield and M.S. Feld, Bull. Am. Phys. Soc. 21, 599 (1976).
M. Ducloy, J.R.R. Leite and M.S. Feld, to be published.
Both single and double-quantum Raman-type processes can occur in coupled systems of this type having a resonant intermediate state. See, for example, M.S. Feld in Fundamental and Applied Laser Physics, edited by M.S. Feld, N.A. Kurnit and A. Javan ( Wiley, New York, 1973 ), pp. 369–420.
J.R.R. Leite, M. Ducloy, A. Sanchez, D. Seligson and M.S. Feld, to be published.
For a general review of tensorial formalism and multipole moments see A. Omont in Progress in Quantum Electronics, Vol. 5, p. 69 (Pergamon Press, Oxford, 1977). For their application in laser spectroscopy see B. Decomps, M. Dumont and M. Ducloy in Laser Spectroscopy of Atoms and Molecules p. 283 (Topics in Applied Physics, Vcl. 2, Springer-Verlag, 1976 ).
M. Gorlicki and M. Ducloy, to be published.
G.M. Dobbs, R.H. Micheels, J. Steinfeld, J.H.S. Wang and J.M. Levy, J. Chem. Phys. 63, 1904 (1975).
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© 1977 Springer-Verlag Berlin Heidelberg
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Ducloy, M., Feld, M.S. (1977). Laser Saturation Spectroscopy in the Time-Delayed Mode. In: Hall, J.L., Carlsten, J.L. (eds) Laser Spectroscopy III. Springer Series in Optical Sciences, vol 7. Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-540-35968-5_28
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DOI: https://doi.org/10.1007/978-3-540-35968-5_28
Publisher Name: Springer, Berlin, Heidelberg
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