Pulse chirping in coherent control via stimulated Raman scattering

Jabir Chathanathil, Svetlana Malinovskaya

A. V. Chugreev, A. Nazarkin, A. Abdolvand +3 more

Transient stimulated Raman scattering is investigated in methane-filled hollow-core photonic crystal fiber. Using frequency-chirped ps-pulses at 1.06 microm as pump and tunable CW-radiation as Stokes seed, the vibrational excitation of the CH(4) molecules can be controlled on the sub T(2) time-scale. In this way the generated Stokes pulse can be phase-locked to the pump pulse and its spectrum manipulated.

B. Chatel, B. Girard

Svetlana Malinovskaya

We propose a method to control population transfer and coherence in a multimode system using a transform-limited pump and a linearly chirped Stokes pulse in stimulated Raman scattering. Simultaneously applied pump and Stokes pulse are shown to induce the ac Stark shifts that result in nonadiabatic coupling of the dressed states, through which the pulse chirp governs population distribution. The method may be applied to selectively excite Raman transitions having the frequency difference less than the bandwidth of a transform-limited pulse.

Jabir Chathanathil, Aneesh Ramaswamy, Dmitry Budker +2 more

The integration of quantum-enabled technology into remote sensing revolutionizes sensitivity and accuracy, enabling the detection of subtle environmental changes, biochemical markers, hazardous materials, and other critical targets beyond the reach of traditional sensors. We have developed advanced remote sensing methodologies by integrating linearly chirped pulses into Coherent Anti-Stokes Raman Scattering (C-CARS) [1-4] and Fractional Stimulated Raman Adiabatic Passage (CFSTIRAP) [5], thereby enhancing their performance. This integration facilitates the generation of highly directional, backward-propagating signals, significantly amplifies signal intensity, and reduces noise by optimizing coherence within the target species, which ensures superior detection accuracy. The proposed methodologies open new possibilities for precise and reliable sensing in complex and challenging environments, paving the way for groundbreaking applications in high-resolution climate monitoring, secure long-range communication, and precise material analysis over vast distances [6]. The work is partially supported the Office of Naval Research through award N00014-22-1-2374. [1] J. Chathanathil, S. A. Malinovskaya, Chirped pulse control of Raman coherence in atoms and molecules. Adv. Quant. Chem. 89, 225-289 (2024). [2] J. Chathanathil, D. Budker, S. A. Malinovskaya, Quantum control via chirped coherent anti-Stokes Raman spectroscopy, Quantum Sci. Tech. 8, 045005 (2023). [3] J. Chathanathil, G. Lui, S. A. Malinovskaya, A semi-classical control theory of Coherent Anti-Stokes Raman Scattering (CARS) maximizing vibrational coherence for remote detection, Phys. Rev. A 104, 043701 (2021). [4] N. Pandya, G. Lui, F. A. Narducci, J. Chathanathil, S. A. Malinovskaya, Creation of the maximum coherence via adiabatic passage in the four-wave mixing process of coherent anti-Stokes Raman scattering, Chem. Phys. Lett., 738, 136763 (2020). [5] J. Chathanathil, A. Ramaswamy, V. S. Malinovsky, D. Budker, S. A. Malinovskaya, Chirped fractional stimulated Raman adiabatic passage, Phys. Rev. A 108, 043710 (2023). [6] G. Liu, F. A. Narducci, S. A. Malinovskaya, Limits to remote molecular detection via coherent anti-Stokes Raman spectroscopy using a maximal coherence control technique, J. Mod. Opt. 67, 21-25 (2020).

Xiaohong Song, Shangqing Gong, Weifeng Yang +3 more