Ultrafast far-infrared dynamics probed by terahertz pulses: A frequency domain approach. I. Model systems
Abstract
Time-resolved terahertz spectroscopy has become a widely used experimental tool for the investigation of ultrafast dynamics of polar systems in the far infrared. We have recently proposed an analytical method for the extraction of a transient two-dimensional susceptibility from the experimental data [Němec, Kadlec, and Kužel, J. Chem. Phys. 117, 8454 (2002)]. In the present paper the methodology of optical pump-terahertz probe experiments is further developed for direct application in realistic experimental situations. The expected two-dimensional transient response function is calculated for a number of model cases (including Drude dynamics of free carriers, harmonic and anharmonic oscillator modes); these results serve as a basis for the interpretation of experimental results. We discuss also the cases where only partial (one-dimensional) information about the system dynamics can be experimentally obtained.
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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 [11]
The two-dimensional response function Σ(τ,t) has an implicit dependence on the pump intensity I(t) and lacks time invariance.
“which has the usual linear response form-except, crucially, that the two-dimensional response function Σ ( τ , t ) has an implicit dependence on I ( t ) and lacks time invarance. 9-11”
From Terahertz time-domain spectroscopy of transient metallic and superconducting states (2015) · cites this paper as [11]
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- Authors
- Němec, H., Kadlec, F., Surendran, S., Kužel, P., & Jungwirth, P.
- Affiliations
- Czech Academy of Sciences (CZ)
- Venue
- The Journal of Chemical Physics
- Publisher
- AIP Publishing
- Published
- 2005-03-08
- Volume
- 122
- Issue
- 10
- Pages
- 104503-104503
- ISSN
- 0021-9606 (ISSN-L)
- 1089-7690
- OpenAlex
- W2092432734
- Cited by
- 31
- References
- 31
- Citations by year
- 2026: 1 · 2025: 2 · 2024: 2 · 2023: 3 · 2021: 3 · 2020: 2 · 2015: 2 · 2012: 1
- FWCI
- 1.90
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- The Journal of Chemical Physics (publishedVersion)
- PubMed (publishedVersion)
- 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 › Chemistry › Spectroscopy › Spectroscopy and Laser Applications
- Keywords
- time-resolved terahertz spectroscopy, optical pump-terahertz probe, free carrier dynamics, polar systems, model systems
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