Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Journal of Raman Spectroscopy

Creating maximum coherence using chirped pulses without adiabatic elimination of excited states

Vladimir S. Malinovsky

Published May 26, 2009• 5 citations
Publisher

Abstract

Abstract We demonstrate the adiabatic passage based method to maximize coherent anti‐Stokes Raman scattering coherence. We present numerical results of the roof scheme implementation without making an assumption of adiabatic elimination of detuned excited electronic states. Copyright © 2009 John Wiley & Sons, Ltd.
DOI
10.1002/jrs.2324

Related papers

Optimizing CARS signal using coherent control methods

Vladimir S. Malinovsky

We demonstrate the adiabatic passage based method to maximize CARS coherence and present numerical results of the roof scheme implementation without making an assumption of adiabatic elimination of detuned excited electronic states. Also we analyze influence of fast decoherence in the molecular samples on the results of proposed scheme. It is shown that the adiabatic method allows achieving chemical sensitivity with high resolution and can be used to obtain CARS signal with efficiently suppressed background in molecular systems with coherence times of several hundred of femtoseconds.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Feb 12, 2009•2 citations

Quantum control via chirped coherent anti-Stokes Raman spectroscopy

Jabir Chathanathil, Dmitry Budker, Svetlana Malinovskaya

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.

Quantum Science and Technology•Jul 4, 2023•1 citation

Quantum control via chirped coherent anti-Stokes Raman spectroscopy

Jabir Chathanathil, Dmitry Budker, Svetlana Malinovskaya

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 fulfil 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. The robustness, spectral selectivity and adiabatic nature of this method are helpful in improving the existing methods of CARS spectroscopy for sensing, imaging and detection. We also show that the selectivity of excitation of vibrational degrees of freedom can be controlled by carefully choosing the spectral chirp rate of the pulses.

arXiv:2212.08258•Dec 16, 2022•0 citations

Optimal coherence via chirped pulse adiabatic passage in the presence of dephasing

Svetlana Malinovskaya, Vladimir S. Malinovsky

We propose the adiabatic passage control scheme to maximize coherence in a predetermined molecular vibrational mode via two-photon Raman transitions. We investigate vibrational energy relaxation and collisional dephasing as factors of coherence loss, and demonstrate the possibility for sustaining high value of coherence in the presence of dephasing by two chirped pulse trains. The proposed method may be used to advance imaging techniques currently applied in the coherent anti-stokes Raman scattering (CARS) microscopy.

Journal of Modern Optics•Nov 10, 2008•4 citations

Chirped Pulse Control of Raman Coherence in Atoms and Molecules

Jabir Chathanathil, Svetlana Malinovskaya

A novel chirped pulse control scheme is presented based on Coherent Anti-Stokes Raman Spectroscopy (C-CARS) aiming at maximizing the vibrational coherence in atoms and molecules. The scheme utilizes chirping of the three incoming pulses, the pump, the Stokes and the probe, in the four-wave mixing process of C-CARS to fulfill the adiabatic passage conditions. The derivation of the scheme is based on simplifying the four-level system into a 'super-effective' two level system via rotating wave approximation and adiabatic elimination of the excited state manifold. The robustness, spectral selectivity and adiabatic nature of C-CARS method may prove useful for sensing, imaging, and detection. It is demonstrated that the selectivity in excitation of vibrational degrees of freedom can be controlled by carefully choosing the spectral chirp rate of the pulses. The C-CARS control scheme is applied to a surrogate methanol molecule to generate an optimal anti-Stokes signal backscattered from a cloud of molecules a kilometer away. The theory is based on the solution of the coupled Maxwell-Liouville von Neumann equations and focuses on the quantum effects induced in the target molecules by the control pulse trains. The propagation effects of pulses through the medium are evaluated and the buildup of the molecular-specific anti-Stokes signal is demonstrated numerically. A deep learning technique, using Convolutional Neural Networks (CNN), is implemented to characterize the control pulses and evaluate time-dependent phase characteristics from them. The effects of decoherence induced by spontaneous decay and collisional dephasing are also examined. Additionally, we present the technique of Fractional Stimulated Raman Adiabatic Passage (F-STIRAP) and demonstrate that it can be utilized for remote detection in a multi-level system by creation of a maximally coherent superposition state.

arXiv:2309.01232•Sep 3, 2023•0 citations

Laser pulse control of Raman processes by chirped non-adiabatic passage

François Légaré, Szczepan Chelkowski, André D. Bandrauk

Chirped pulses allow for non-adiabatic passage between dressed states of Raman processes. It is shown that using an appropriately chirped pulse, one can control the interference between resonant and non-resonant pathways in stimulated Raman processes. A three-level system is studied in detail and application to complete ro-vibrational level inversion to high vibration quantum numbers (v > 10) in H2 via RCNAP (Raman chirped non-adiabatic passage) is presented. Copyright © 2000 John Wiley & Sons, Ltd.

Journal of Raman Spectroscopy•Jan 1, 2000•26 citations
We demonstrate the adiabatic passage based method to maximize CARS coherence and present numerical results of the roof scheme implementation without making an assumption of adiabatic elimination of detuned excited electronic states. Also we analyze influence of fast decoherence in the molecular samples on the results of proposed scheme. It is shown that the adiabatic method allows achieving chemical sensitivity with high resolution and can be used to obtain CARS signal with efficiently suppressed background in molecular systems with coherence times of several hundred of femtoseconds.
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.
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 fulfil 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. The robustness, spectral selectivity and adiabatic nature of this method are helpful in improving the existing methods of CARS spectroscopy for sensing, imaging and detection. We also show that the selectivity of excitation of vibrational degrees of freedom can be controlled by carefully choosing the spectral chirp rate of the pulses.
We propose the adiabatic passage control scheme to maximize coherence in a predetermined molecular vibrational mode via two-photon Raman transitions. We investigate vibrational energy relaxation and collisional dephasing as factors of coherence loss, and demonstrate the possibility for sustaining high value of coherence in the presence of dephasing by two chirped pulse trains. The proposed method may be used to advance imaging techniques currently applied in the coherent anti-stokes Raman scattering (CARS) microscopy.
A novel chirped pulse control scheme is presented based on Coherent Anti-Stokes Raman Spectroscopy (C-CARS) aiming at maximizing the vibrational coherence in atoms and molecules. The scheme utilizes chirping of the three incoming pulses, the pump, the Stokes and the probe, in the four-wave mixing process of C-CARS to fulfill the adiabatic passage conditions. The derivation of the scheme is based on simplifying the four-level system into a 'super-effective' two level system via rotating wave approximation and adiabatic elimination of the excited state manifold. The robustness, spectral selectivity and adiabatic nature of C-CARS method may prove useful for sensing, imaging, and detection. It is demonstrated that the selectivity in excitation of vibrational degrees of freedom can be controlled by carefully choosing the spectral chirp rate of the pulses. The C-CARS control scheme is applied to a surrogate methanol molecule to generate an optimal anti-Stokes signal backscattered from a cloud of molecules a kilometer away. The theory is based on the solution of the coupled Maxwell-Liouville von Neumann equations and focuses on the quantum effects induced in the target molecules by the control pulse trains. The propagation effects of pulses through the medium are evaluated and the buildup of the molecular-specific anti-Stokes signal is demonstrated numerically. A deep learning technique, using Convolutional Neural Networks (CNN), is implemented to characterize the control pulses and evaluate time-dependent phase characteristics from them. The effects of decoherence induced by spontaneous decay and collisional dephasing are also examined. Additionally, we present the technique of Fractional Stimulated Raman Adiabatic Passage (F-STIRAP) and demonstrate that it can be utilized for remote detection in a multi-level system by creation of a maximally coherent superposition state.
Chirped pulses allow for non-adiabatic passage between dressed states of Raman processes. It is shown that using an appropriately chirped pulse, one can control the interference between resonant and non-resonant pathways in stimulated Raman processes. A three-level system is studied in detail and application to complete ro-vibrational level inversion to high vibration quantum numbers (v > 10) in H2 via RCNAP (Raman chirped non-adiabatic passage) is presented. Copyright © 2000 John Wiley & Sons, Ltd.