Theory for determination of the low-frequency time-dependent response function in liquids using time-resolved terahertz pulse spectroscopy
Abstract
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.
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The straightforward interpretation of THz-TDS as a snapshot of the optical conductivity spectrum breaks down when characteristic relaxation times are comparable to the photoexcitation delay, because the Fourier transform involves times that precede photoexcitation.
“However, the straightforward interpretation of THz-TDS as a snapshot of the optical conductivity spectrum breaks down when the characteristic relaxation times are comparable to the photoexcitation delay, because the Fourier transform involves times that precede photoexcitation. 1,9-16”
From Terahertz time-domain spectroscopy of transient metallic and superconducting states (2015) · cites this paper as [16]
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Hendry, E., Koeberg, M., Schins, J. M., Nienhuys, H. K., Sundström, V., Siebbeles, L. D. A., & Bonn, M. (2005) · Physical Review B · doi:10.1103/physrevb.71.125201 · Cited by 206 · see citing works
Nicoletti, D., Casandruc, E., Laplace, Y., Khanna, V., Hunt, C. R., Kaiser, S., Dhesi, S. S., Gu, G. D., Hill, J. P., & Cavalleri, A. (2014) · Physical Review B · doi:10.1103/physrevb.90.100503 · Cited by 141 · see citing works
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Němec, H., Kadlec, F., & Kužel, P. (2002) · The Journal of Chemical Physics · doi:10.1063/1.1512648 · Cited by 79 · see citing works
Terahertz time-domain spectroscopy of transient metallic and superconducting states
Orenstein, J., & Dodge, J. S. (2015) · Physical Review B · doi:10.1103/physrevb.92.134507 · Cited by 50 · see citing works
Němec, H., Kadlec, F., Surendran, S., Kužel, P., & Jungwirth, P. (2005) · The Journal of Chemical Physics · doi:10.1063/1.1857851 · Cited by 31 · see citing works
The effect of the Gouy phase in optical-pump-THz-probe spectroscopy
Ahmed, S., Savolainen, J., & Hamm, P. (2014) · Optics Express · doi:10.1364/oe.22.004256 · Cited by 16 · see citing works
- Authors
- Kindt, J. T., & Schmuttenmaer, C. A.
- Affiliations
- Yale University (US)
- Venue
- The Journal of Chemical Physics
- Publisher
- AIP Publishing
- Published
- 1999-05-01
- Volume
- 110
- Issue
- 17
- Pages
- 8589-8596
- ISSN
- 0021-9606 (ISSN-L)
- 1089-7690
- OpenAlex
- W2091809372
- Cited by
- 102
- References
- 0
- Citations by year
- 2026: 2 · 2025: 4 · 2024: 2 · 2023: 6 · 2022: 3 · 2021: 4 · 2020: 6 · 2019: 5 · 2018: 3 · 2017: 6 · 2016: 2 · 2015: 4 · 2014: 5 · 2013: 1 · 2012: 4
- FWCI
- 5.33
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- The Journal of Chemical Physics (publishedVersion)
- Funders
- National Science Foundation
- Division of Chemistry
- Topics
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Terahertz technology and applications
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
- Keywords
- time-resolved terahertz spectroscopy, solvation dynamics, photoexcitation, liquids
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