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Optical and Quantum Sensing and Precision Metrology II

Remote sensing with quantum-enhanced Raman spectroscopy

Jabir Chathanathil, Aneesh Ramaswamy, Dmitry Budker, Frank A. Narducci, Svetlana Malinovskaya

Published Mar 19, 2025• 0 citations
Publisher

Abstract

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).

DOI
10.1117/12.3057034

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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).
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.
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 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.
Quantum correlations offer the possibility of surpassing classical limits in optical measurements, but their integration into nonlinear vibrational spectroscopy has remained largely unexplored. Here, we introduce a quantum-enhanced implementation of coherent Raman spectroscopy that employs broadband squeezed-light detection to interrogate relative intensity correlations between Stokes and anti-Stokes fields generated in an ultrafast four-wave-mixing process. By exploiting nonclassical correlations between these fields, we suppress the nonresonant background and enhance the signal-to-noise performance in both temporal and spectral domains, enabling detection sensitivities beyond the classical shot-noise limit. Importantly, the quantum advantage demonstrated here does not arise solely from improved detection statistics. Rather, it originates from microscopic intermolecular correlations mediated by cascaded exchange of a virtual photon between molecular pairs. This mechanism establishes a fundamentally distinct and significant pathway for information extraction in vibrational spectroscopy, providing access to structural and dynamical observables that are intrinsically inaccessible by conventional classical Raman techniques. Numerical simulations illustrate the power of the technique by resolving intradimer [Formula: see text] bond splitting in cyclobutane thymine dimers following ultraviolet excitation, highlighting its potential for probing ultrafast photochemical processes with quantum-limited sensitivity and for label-free biomedical optical sensing and imaging.