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arXiv:2305.18652 · Physical Review A

Chirped fractional stimulated Raman adiabatic passage

Jabir Chathanathil, Aneesh Ramaswamy, Vladimir S. Malinovsky, Dmitry Budker, Svetlana Malinovskaya

Published Oct 13, 2023• 12 citations
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Abstract

In this work we develop a theory of fractional stimulated Raman adiabatic passage (FSTIRAP) using frequency-chirped pulses (CFSTIRAP). We analyze the CFSTIRAP as a method to create a coherent superposition state maximizing coherence between the initial and the target state in the presence of the two-photon detuning. We demonstrate that the pulse chirping permits relaxation of the condition of the two-photon resonance required for adiabatic passage in STIRAP and FSTIRAP. The choice of the chirp rate $|\ensuremath{\alpha}|=|\ensuremath{\delta}|/({t}_{p}\ensuremath{-}{t}_{s})$ enables adiabatic passage to a predetermined state between two nearly degenerate final states within a broad range of values of the two-photon detuning and the chirp rate. The proposed schemes will expand the scope of quantum control methods and contribute to the further improvement of quantum imaging, sensing, and metrology.

DOI
10.1103/physreva.108.043710

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In this work we develop a theory of fractional stimulated Raman adiabatic passage (FSTIRAP) using frequency-chirped pulses (CFSTIRAP). We analyze the CFSTIRAP as a method to create a coherent superposition state maximizing coherence between the initial and the target state in the presence of the two-photon detuning. We demonstrate that the pulse chirping permits relaxation of the condition of the two-photon resonance required for adiabatic passage in STIRAP and FSTIRAP. The choice of the chirp rate ∣\ensuremathα∣=∣\ensuremathδ∣/(tp\ensuremath−ts)|\ensuremath{\alpha}|=|\ensuremath{\delta}|/({t}_{p}\ensuremath{-}{t}_{s})∣\ensuremathα∣=∣\ensuremathδ∣/(tp​\ensuremath−ts​) enables adiabatic passage to a predetermined state between two nearly degenerate final states within a broad range of values of the two-photon detuning and the chirp rate. The proposed schemes will expand the scope of quantum control methods and contribute to the further improvement of quantum imaging, sensing, and metrology.
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.
We discuss the properties of a simple and robust scheme for preparing atoms and molecules in an arbitrary preselected coherent superposition of quantum states - fractional stimulated Raman adiabatic passage (fractional STIRAP) - first proposed by Marte et al (1991 Phys. Rev. A 44 R4118). As in STIRAP, the Stokes pulse arrives before the pump pulse, but unlike STIRAP, here the two pulses terminate simultaneously, while maintaining a constant ratio of amplitudes. We extend earlier research and suggest a realization of this scheme with two smoothly varying delayed laser pulses (which can be derived from a single laser), the parameters of the created superposition being controlled by the polarization of the delayed pulse. Furthermore, we provide simple analytic estimates of the robustness of this process against variations in the laser intensity, laser frequency and pulse delay. Finally, we discuss an extension to multistate systems which provides a possibility for creating coherent superpositions of more than two states.
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.
We discuss a simple scheme for preparing atoms and molecules in an arbitrary preselected coherent superposition of quantum states. The technique, which we call fractional stimulated Raman adiabatic passage ({\it f-STIRAP}), is based upon (incomplete) adiabatic population transfer between an initial state ψ1ψ_1ψ1​ and state ψ3ψ_3ψ3​ through an intermediate state ψ2ψ_2ψ2​. As in STIRAP, the Stokes pulse arrives before the pump pulse, but unlike STIRAP, the two pulses terminate simultaneously while maintaining a constant ratio of amplitudes. The independence of f-STIRAP from details of pulse shape and pulse area makes it the analog of conventional STIRAP in the creation of coherent superpositions of states. We suggest a smooth realization of f-STIRAP which requires only two laser pulses (which can be derived from a single laser) and at the same time ensures the automatic fulfillment of the asymptotic conditions at early and late times. Furthermore, we provide simple analytic estimates of the robustness of f-STIRAP against variations in the pulse intensity, the pulse delay, and the intermediate-state detuning, and discuss its possible extension to multistate systems.