journal article·2023-09-20Open access

Time-Dependent, Two-Photon Rabi Frequency Shift Observed in Multi-Frequency Raman Spectra

Zujun Xu, Zhiyu Jin, Donna Strickland

Applied Sciences· Volume 13· Issue 18

Abstract

It has been observed that when the multi-frequency Raman scattering process is pumped by two frequency chirped pulses in the transient regime, the anti-Stokes orders are spectrally broadened on the lower-frequency side, causing each of the orders to have a broader spectrum with double-peak pattern. In this article, we employ frequency-resolved optical gating to study the spectral shift of the first anti-Stokes Raman order. A double-pulse model is introduced to determine the electric field of the anti-Stokes orders from the experimental FROG spectrogram. With the help from the double-pulse model, we demonstrate that the double-peaked spectrum comes from linear Raman scattering between manifolds in the two-photon dressed states.
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Research context

OpenAlex topics: Laser-Matter Interactions and Applications · Spectroscopy and Quantum Chemical Studies · Spectroscopy Techniques in Biomedical and Chemical Research

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Affiliations

Department of Physics and Astronomy, University of Waterloo, Waterloo, ON N2L 3G1, Canada

Funding

Natural Sciences and Engineering Research Council of Canada

References (18)

Show source-provided references
1. Generation of More than 40 Laser Emission Lines from the Ultraviolet to the Visible Regions by Two-Color Stimulated Raman Effect10.1007/BF00324191 ↗
2. A New Approach for the Generation of Ultrashort Optical Pulses10.1016/0030-4018(93)90530-I ↗
3. Raman Generation by Phased and Antiphased Molecular States10.1103/PhysRevLett.85.562 ↗
4. Generation of a Single-Cycle Optical Pulse10.1103/PhysRevLett.94.033904 ↗
5. Yoshii, K., Nakamura, Y., Hagihara, K., and Katsuragawa, M. (2014, January 8–13). Generation of a Train of Ultrashort Pulses by Simply Inserting Transparent Plates on the Optical Path. Proceedings of the Conference on Lasers and Electro-Optics (CLEO)—Laser Science to Photonic Applications, San Jose, CA, USA.10.1364/CLEO_QELS.2014.FTh1D.5 ↗
6. The Simplest Route to Generating a Train of Attosecond Pulses10.1038/lsa.2013.14 ↗
7. Transient Multi-Frequency Raman Generation in SF610.1016/j.optcom.2006.09.021 ↗
8. High-Order Stimulated Raman Scattering in a Highly Transient Regime Driven by a Pair of Ultrashort Pulses10.1364/OL.29.000495 ↗
9. Simplified Setup for High-Resolution Spectroscopy That Uses Ultrashort Pulses10.1364/OL.28.000361 ↗
10. Effect of Two-Photon Stark Shift on the Multi-Frequency Raman Spectra10.3390/app4030390 ↗
11. Zhdanova, A.A., Bahari, A., Shutova, M., and Sokolov, A.V. (2019). Synthesis of Ultrafast Waveforms Using Coherent Raman Sidebands. arXiv.
12. Coherent Broadband Light Generation with a Double-Path Configuration10.1364/AO.53.002866 ↗
13. Synthesis of Ultrafast Waveforms Using Coherent Raman Sidebands10.1103/PhysRevA.102.013520 ↗
14. Frequency-Resolved Optical-Gating Measurements of Ultrashort Pulses Using Surface Third-Harmonic Generation10.1364/OL.21.001381 ↗
15. Dual-Wavelength Chirped-Pulse Amplification System10.1364/OL.25.000581 ↗
16. Theory of Multiwave Propagation and Frequency Conversion in a Raman Medium10.1103/PhysRevA.33.1788 ↗
17. Efficient Adiabatic Population Transfer by Two-Photon Excitation Assisted by a Laser-Induced Stark Shift10.1063/1.481829 ↗
18. Van der Veen, J. (2023). Analytic Spectrum of Multi-Frequency Raman Generation with Chirped Pulses. arXiv.10.1364/FIO.2022.JTu5A.26 ↗