Theory for determination of the low-frequency time-dependent response function in liquids using time-resolved terahertz pulse spectroscopy
J. Chem. Phys. 110, 8589 (1999); doi:10.1063/1.478766
Issue Date: 1 May 1999
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With the current rapid improvement in techniques for generating and detecting femtosecond terahertz (fs-THz) pulses, it is now possible to detect time-dependent perturbations to low-frequency intermolecular far-infrared modes during solvation events. The interpretation of these time-resolved terahertz spectroscopy experiments has generally relied on a collapse of the information available in the fs-THz pulse to give a one-dimensional time-dependent function, whose physical significance is not well defined. We describe a method to exploit the full electric field profile of the pulse as a function of pump/probe delay time to obtain a two-dimensional function that describes the system's time-dependent dielectric response. We discuss the physical significance of this response function in terms of the time evolution of solute/solvent modes following photoexcitation, and give examples to show how its qualitative features relate to the measurable signal. ©1999 American Institute of Physics.
| History: | Received 8 December 1998; accepted 5 February 1999 |
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KEYWORDS and PACS
- 78.30.Cp
Optical properties, condensed-matter spectroscopy and other interactions of radiation and particles with condensed matter Infrared and Raman spectra Liquids - 78.47.+p
Optical properties, condensed-matter spectroscopy and other interactions of radiation and particles with condensed matter Time-resolved optical spectroscopies and other ultrafast optical measurements in condensed matter - 82.30.Nr
Physical chemistry Specific chemical reactions; reaction mechanisms Association, addition, insertion, cluster formation, hydrogen bonding - YEAR: 1999
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PUBLICATION DATA
0021-9606 (print)
1089-7690 (online)
REFERENCES (31)
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For access to fully linked references, you need to Log in.
- For recent broad reviews, see R. M. Stratt and M. Maroncelli,
J. Phys. Chem. 100, 12981 (1996) ; - G. R. Fleming and M. Cho,
Annu. Rev. Phys. Chem. 47, 109 (1996) . - For reviews of the application of time-dependent Stokes shift experiments to solvation dynamics, see M. Maroncelli,
J. Mol. Liq. 57, 1 (1993) ; - P. F. Barbara and W. Jarzeba,
Adv. Photochem. 15, 1 (1990) . - For a recent review, see W. P. de Boeij, M. S. Pshenichnikov, and D. A. Wiersma,
Annu. Rev. Phys. Chem. 49, 99 (1998) . - X.-C. Zhang, B. B. Hu, J. T. Darrow, and D. H. Auston, Appl. Phys. Lett. 56, 1011 (1990).
- N. Katzenellenbogen and D. Grischkowsky, Appl. Phys. Lett. 58, 222 (1991).
- Q. Wu, M. Litz, and X.-C. Zhang Appl. Phys. Lett. 68, 2924 (1996).
- M. C. Nuss, D. H. Auston, and F. Capasso, Phys. Rev. Lett. 58, 2355 (1987).
- B. I. Greene, J. F. Federici, D. R. Dykaar, A. F. J. Levi, and L. Pfeiffer,
Opt. Lett. 16, 48 (1991) . - P. N. Saeta, J. F. Federici, B. I. Greene, and D. R. Dykaar, Appl. Phys. Lett. 60, 1477 (1992).
- R. R. Jones, D. You, and P. H. Bucksbaum, Phys. Rev. Lett. 70, 1236 (1993).
- R. H. M. Groeneveld and D. Grischkowsky,
J. Opt. Soc. Am. B 11, 2502 (1994) . - J. Zielbauer and M. Wegener, Appl. Phys. Lett. 68, 1223 (1995).
- G. M. Lankhuijzen and L. D. Noordam, Phys. Rev. Lett. 76, 1784 (1996).
- C. Raman, C. W. S. Conover, C. I. Sukenik, and P. H. Bucksbaum, Phys. Rev. Lett. 76, 2436 (1996).
- R. R. Jones, Phys. Rev. Lett. 76, 3927 (1996).
- G. Haran, W.-D. Sun, K. Wynne, and R. M. Hochstrasser,
Chem. Phys. Lett. 274, 365 (1997) . - R. McElroy and K. Wynne, Phys. Rev. Lett. 79, 3078 (1997).
- D. S. Venables and C. A. Schmuttenmaer, in Ultrafast Phenomena XI, edited by T. Elsaesser, J. G. Fujimoto, D. Wiersma, and W. Zinth (Springer, Berlin, 1998).
- S. S. Prabhu, S. E. Ralph, M. R. Melloch, and E. S. Harmon, Appl. Phys. Lett. 70, 2419 (1997).
- B. N. Flanders, D. C. Arnett, and N. F. Scherer,
IEEE J. Sel. Top. Quantum Electron. 4, 353 (1998) . - D. S. Venables and C. A. Schmuttenmaer, J. Appl. Phys. (to be published).
- D. Chandler, Introduction to Modern Statistical Mechanics (Oxford, New York, 1987).
- J. R. Reitz, F. J. Milford, and R. W. Christy, Foundations of Electromagnetic Theory (AddisonWesley, Reading, MA, 1993).
- W. T. Scott, The Physics of Electricity and Magnetism, 2nd ed. (Wiley, New York, 1996).
- S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford, New York, 1995).
- K. Okumura and Y. Tanimura,
Chem. Phys. Lett. 295, 298 (1998) . - J. B. Marion and S. T. Thornton, Classical Dynamics of Particles and Systems (Harcourt Brace Jovanovich, San Diego, 1988).
- A possible experimental approach to isolate the solvent shell polarization response itself would use a strong dc electric field to achieve a time-independent equilibrium solute orientation. Electronic excitation would then lead to a THz pulse mapping the time derivative of both the solute dipole itself, and the change in dipole from the solvent response. This approach would eliminate any complication from the orientational dynamics of the solute response to an ultrafast THz pulse probe, which may not be well suited to achieve significant orientation of the typically very slowly rotating solute dye molecules.
- A. S. Vengurlekar and S. S. Jha, Phys. Rev. B 38, 2044 (1988);
- 41, 1286 (1990);
- H. Harde and D. Grischkowsky,
J. Opt. Soc. Am. B 8, 1642 (1991) ;
H. Harde, N. Katzenellenbogen, and D. Grischkowsky, - For an example, see G. J. Moro and A. Polimeno, J. Chem. Phys. 107, 7884 (1997);
H. Harde, R. A. Cheville, and D. Grischkowsky,








