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

arXiv:2212.08258

Quantum control via chirped coherent anti-Stokes Raman spectroscopy

Jabir Chathanathil, Dmitry Budker, Svetlana Malinovskaya

Published Dec 16, 2022• 0 citations
arXivHTMLPDF

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 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.

DOI
10.48550/arxiv.2212.08258

Related papers

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

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

Effects of phase and coupling between the vibrational modes on selective excitation in coherent anti-Stokes Raman scattering microscopy

Vishesha Patel, Vladimir S. Malinovsky, Svetlana Malinovskaya

Coherent anti-Stokes Raman scattering (CARS) microscopy has been a major tool of investigation of biological structures as it contains the vibrational signature of molecules. A quantum control method based on chirped pulse adiabatic passage was recently proposed for selective excitation of a predetermined vibrational mode in CARS microscopy [Malinovskaya and Malinovsky, Opt. Lett. 32, 707 (2007)]. The method utilizes the chirp sign variation at the peak pulse amplitude and gives a robust adiabatic excitation of the desired vibrational mode. Using this method, we investigate the impact of coupling between vibrational modes in molecules on controllability of excitation of the CARS signal. We analyze two models of two coupled two-level systems (TLSs) having slightly different transitional frequencies. The first model, featuring degenerate ground states of the TLSs, gives robust adiabatic excitation and maximum coherence in the resonant TLS for positive value of the chirp. In the second model, implying nondegenerate ground states in the TLSs, a population distribution is observed in both TLSs, resulting in a lack of selectivity of excitation and low coherence. It is shown that the relative phase and coupling between the TLSs play an important role in optimizing coherence in the desired vibrational mode and suppressing unwanted transitions in CARS microscopy.

Physical Review A•Jun 8, 2010•13 citations

Robust control by two chirped pulse trains in the presence of decoherence

Svetlana Malinovskaya

We discuss a novel method to create maximum coherence in a two-level system that is selectively excited among many having similar frequencies by making use of two specifically chirped pulses in the Raman configuration. The feasibility of the method is analyzed in the presence of decoherence caused by vibrational energy relaxation and collisional dephasing. It has been demonstrated that a high value of coherence may be sustained by the implementation of two chirped pulse trains prepared in accordance with the proposed method and having the same period as the vibrational energy relaxation time. Maximum coherence between predetermined states in atoms and molecules is an important aspect of many problems in quantum optics. One possible example is the generation of optimal CARS signal in the CARS microscopy aiming to reveal structures constituted of particular molecular groups. Presently, in experiments on biological imaging, the CARS signal is generated with implementation of picosecond laser pulses (1), a narrow spectral bandwidth of which allows one to address a particular molecular group with a good accuracy. Aiming to improve chemical sensitivity and to get optimal CARS signal for given pulse intensity we propose to use the quantum control methods for selective excitation of required vibrations in complex molecular systems. We developed a novel method that allows one to achieve maximum coherence in a predetermined vibrational mode in a multimode mole- cular system via the Raman transitions induced by the pump and Stokes chirped pulses. According to the Maxwell-Bloch equations, maximum coherence is the condition for the CARS signal to acquire the highest intensity upon propagation through a molecular medium (2). The mechanism of creation of maximum coherence underlying the proposed method is based on the adiabatic passage. An important aspect in the investigations asso- ciated with a condense phase is decoherence. Two main sources of decoherence, the vibrational energy relaxa- tion and collisional dephasing, may significantly affect the CARS signal intensity. The phase control of molecular processes in the presence of collisions was

Bulletin of the American Physical Society•May 30, 2008•0 citations

Semiclassical control theory of coherent anti-Stokes Raman scattering maximizing vibrational coherence for remote detection

Jabir Chathanathil, G. Liu, Svetlana Malinovskaya

A semiclassical theory that describes the generation of a coherent anti-Stokes Raman scattering (CARS) signal is presented that maximizes vibrational coherence in a mode predetermined by the pump, the Stokes, and the probe chirped pulse trains and takes into account the field propagation effects in a cloud of molecules. The buildup of the anti-Stokes signal, which may be used as a molecular signature in the backward CARS signal, is demonstrated numerically. The theory is based on the solution of the coupled Maxwell's and Liouville--von Neumann equations and focuses on the quantum effects induced in the target molecules by the control pulse trains. A deep convolutional neural network technique is implemented to evaluate time-dependent phase characteristics of the control fields. The effect of decoherence induced by spontaneous decay and collisional dephasing is examined.

Physical Review A•Oct 5, 2021•7 citations

Remote sensing with quantum-enhanced Raman spectroscopy

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).

Optical and Quantum Sensing and Precision Metrology II•Mar 19, 2025•0 citations
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.
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 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.
Coherent anti-Stokes Raman scattering (CARS) microscopy has been a major tool of investigation of biological structures as it contains the vibrational signature of molecules. A quantum control method based on chirped pulse adiabatic passage was recently proposed for selective excitation of a predetermined vibrational mode in CARS microscopy [Malinovskaya and Malinovsky, Opt. Lett. 32, 707 (2007)]. The method utilizes the chirp sign variation at the peak pulse amplitude and gives a robust adiabatic excitation of the desired vibrational mode. Using this method, we investigate the impact of coupling between vibrational modes in molecules on controllability of excitation of the CARS signal. We analyze two models of two coupled two-level systems (TLSs) having slightly different transitional frequencies. The first model, featuring degenerate ground states of the TLSs, gives robust adiabatic excitation and maximum coherence in the resonant TLS for positive value of the chirp. In the second model, implying nondegenerate ground states in the TLSs, a population distribution is observed in both TLSs, resulting in a lack of selectivity of excitation and low coherence. It is shown that the relative phase and coupling between the TLSs play an important role in optimizing coherence in the desired vibrational mode and suppressing unwanted transitions in CARS microscopy.
We discuss a novel method to create maximum coherence in a two-level system that is selectively excited among many having similar frequencies by making use of two specifically chirped pulses in the Raman configuration. The feasibility of the method is analyzed in the presence of decoherence caused by vibrational energy relaxation and collisional dephasing. It has been demonstrated that a high value of coherence may be sustained by the implementation of two chirped pulse trains prepared in accordance with the proposed method and having the same period as the vibrational energy relaxation time. Maximum coherence between predetermined states in atoms and molecules is an important aspect of many problems in quantum optics. One possible example is the generation of optimal CARS signal in the CARS microscopy aiming to reveal structures constituted of particular molecular groups. Presently, in experiments on biological imaging, the CARS signal is generated with implementation of picosecond laser pulses (1), a narrow spectral bandwidth of which allows one to address a particular molecular group with a good accuracy. Aiming to improve chemical sensitivity and to get optimal CARS signal for given pulse intensity we propose to use the quantum control methods for selective excitation of required vibrations in complex molecular systems. We developed a novel method that allows one to achieve maximum coherence in a predetermined vibrational mode in a multimode mole- cular system via the Raman transitions induced by the pump and Stokes chirped pulses. According to the Maxwell-Bloch equations, maximum coherence is the condition for the CARS signal to acquire the highest intensity upon propagation through a molecular medium (2). The mechanism of creation of maximum coherence underlying the proposed method is based on the adiabatic passage. An important aspect in the investigations asso- ciated with a condense phase is decoherence. Two main sources of decoherence, the vibrational energy relaxa- tion and collisional dephasing, may significantly affect the CARS signal intensity. The phase control of molecular processes in the presence of collisions was
A semiclassical theory that describes the generation of a coherent anti-Stokes Raman scattering (CARS) signal is presented that maximizes vibrational coherence in a mode predetermined by the pump, the Stokes, and the probe chirped pulse trains and takes into account the field propagation effects in a cloud of molecules. The buildup of the anti-Stokes signal, which may be used as a molecular signature in the backward CARS signal, is demonstrated numerically. The theory is based on the solution of the coupled Maxwell's and Liouville--von Neumann equations and focuses on the quantum effects induced in the target molecules by the control pulse trains. A deep convolutional neural network technique is implemented to evaluate time-dependent phase characteristics of the control fields. The effect of decoherence induced by spontaneous decay and collisional dephasing is examined.
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).