Quantum control via chirped coherent anti-Stokes Raman spectroscopy

Jabir Chathanathil, Dmitry Budker, Svetlana A. Malinovskaya

Research output: Contribution to journalArticlepeer-review

Abstract

A chirped-pulse quantum control scheme applicable to coherent anti-Stokes Raman scattering spectroscopy, named as C-CARS, is presented aimed at maximizing the vibrational coherence in molecules. It implies chirping of three incoming pulses in the four-wave mixing process of CARS, the pump, the Stokes and the probe, to fulfill the conditions of adiabatic passage. The scheme is derived in the framework of rotating wave approximation and adiabatic elimination of excited state manifold simplifying the four-level model system into a ‘super-effective’ two level system. We demonstrate that the selectivity of excitation of vibrational degrees of freedom can be controlled by carefully choosing the spectral chirp rate of the pulses. The robustness, spectral selectivity and adiabatic nature of this method are advantageous for improving the existing methods of CARS spectroscopy for sensing, imaging and detection.

Original languageEnglish
Article number045005
JournalQuantum Science and Technology
Volume8
Issue number4
DOIs
StatePublished - Oct 2023

Keywords

  • adiabatic passage
  • coherent anti-Stokes Raman scattering
  • four-wave mixing
  • linearly chirped pulse
  • remote detection
  • ultrafast quantum control

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