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Physical Review Letters

Vanishing and Revival of Resonance Raman Scattering

Yu Guo, Chuan‐Cun Shu, Daoyi Dong, Franco Nori

Published Nov 26, 2019• 48 citations
Publisher

Abstract

The possibility to manipulate quantum coherence and interference, apart from its fundamental interest in quantum mechanics, is essential for controlling nonlinear optical processes such as high harmonic generation, multiphoton absorption, and stimulated Raman scattering. We show, analytically and numerically, how a nonlinear optical process via resonance Raman scattering (RRS) can be manipulated in a four-level double-Λ system by using pulsed laser fields. We find that two simultaneously excited RRS paths involved in the system can generate an ultimately destructive interference in the broad-bandwidth-limit regime. This, in turn, reduces the four-level system to an equivalent three-level system in a V configuration capable of naturally vanishing RRS effects. We further show that this counterintuitive phenomenon, i.e., the RRS vanishing, can be prevented by transferring a modulated phase of the laser pulse to the system at resonance frequencies. This work demonstrates a clear signature of both quantum destructive and constructive interference by actively controlling resonant multiphoton processes in multilevel quantum systems, and it therefore has potential applications in nonlinear optics, quantum control, and quantum information science.

DOI
10.1103/physrevlett.123.223202

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The possibility to manipulate quantum coherence and interference, apart from its fundamental interest in quantum mechanics, is essential for controlling nonlinear optical processes such as high harmonic generation, multiphoton absorption, and stimulated Raman scattering. We show, analytically and numerically, how a nonlinear optical process via resonance Raman scattering (RRS) can be manipulated in a four-level double-Λ system by using pulsed laser fields. We find that two simultaneously excited RRS paths involved in the system can generate an ultimately destructive interference in the broad-bandwidth-limit regime. This, in turn, reduces the four-level system to an equivalent three-level system in a V configuration capable of naturally vanishing RRS effects. We further show that this counterintuitive phenomenon, i.e., the RRS vanishing, can be prevented by transferring a modulated phase of the laser pulse to the system at resonance frequencies. This work demonstrates a clear signature of both quantum destructive and constructive interference by actively controlling resonant multiphoton processes in multilevel quantum systems, and it therefore has potential applications in nonlinear optics, quantum control, and quantum information science.
In this thesis, quantum coherent control of dynamic properties of double-dark-resonance atomic systems is pursued in detail. First we show our scheme for creating atomic coherent superposition states via the technique of stimulated Raman adiabatic passage in a Lambda-type four-level system. With the application of a control field, it is found that the presence of double dark states leads to two arbitrary coherent superposition states with equal amplitude but inverse relative phases, even though the condition of multiphoton resonance is not met. The suitable manipulation of the control field and detunings enables the proposed scheme to create any coherent superposition states one desired. Then, in the above mentioned double-dark-resonant system, a scheme for giant enhancement of the Kerr nonlinearity is put forward. Compared with that generated in a single-dark-resonance system, the Kerr nonlinearity can be enhanced by several orders of magnitude with vanishing linear absorption. We attribute this dramatic enhancement to the interaction of dark resonances. As another possible means for enhancement of Kerr nonlinearity, spontaneously generated coherence is proposed. Meanwhile, a theoretical investigation is carried out in a five-level tripod system for obtaining a high efficiency double-channel four-wave-mixing process. By manipulating the intensity of the two coupling fields, the conversion efficiency of four-wave-mixing can be controlled.
Atomic coherence and interference manifested by electromagentically induced transparency (EIT) and coherent population trapping (CPT) plays an important role in the current studies of atom-photon interactions and has found numerous applications in optical physics. EIT is created in a three-level atomic system by a coupling field and results in destructive interference between two excitation paths of a weak probe laser interacting with the atomic medium. This leads to suppressed linear absorption and rapidly varying atomic dispersion for the probe laser near the atomic resonance, which provides the platform for a variety of applications such as nonlinear optics at low light levels, slow light manipulation, and quantum state engineering for photons and atoms. Here we extend the simple three-level EIT system to more complicated and versatile configurations in a multi-level atomic system coupled by multiple laser fields. We show that with multiple excitation paths provided by different laser fields, phase-dependent quantum interference is induced: either constructive or destructive interference can be realized by varying the relative phases among the laser fields. Two specific examples are discussed. One is a three-level system coupled by bichromatic coupling and probe fields, in which the phase dependent interference between the resonant two-photon Raman transitions can be initiated and controlled. Another is a four-level system coupled by two coupling fields and two probe fields, in which a double-EIT configuration is created by the phase-dependent interference between three-photon and one-photon excitation processes. We analyze the coherently coupled multi-level atomic system and discuss the control parameters for the onset of constructive or destructive quantum interference. We describe two experiments performed with cold Rb atoms that can be approximately treated as the coherently coupled three-level and four-level atomic systems respectively. The experimental results show the phase-dependent quantum coherence and interference in the multi-level Rb atomic system, and agree with the theoretical calculations based on the coherently coupled three-level or four-level model system.
A new scheme is suggested to manipulate the probe transitions (and hence the optical properties of atomic vapors) via double-control destructive and constructive quantum interferences. The influence of phase coherence between the two control transitions on the probe transition is also studied. The most remarkable feature of the present scheme is that the optical properties (absorption, transparency and dispersion) of an atomic system can be manipulated using this double-control multi-pathway interferences (multiple routes to excitation). It is also shown that a four-level system will exhibit a two-level resonant absorption because the two control levels (driven by the two control fields) form a dark state (and hence a destructive quantum interference occurs between the two control transitions). However, the present four-level system will exhibit electromagnetically induced transparency to the probe field when the three lower levels (including the probe level and the two control levels) form a three-level dark state. The present scenario has potential applications in new devices (e.g. logic gates and sensitive optical switches) and new techniques (e.g. quantum coherent information storage).
A model of two-level weakly interacting quantum systems is used to demonstrate that the phase of molecular vibrations excited through stimulated Raman scattering can be controlled by the relative phase of time-separated laser pulses, allowing synchronization and amplitude control of coherence excitation in a medium. For transients with a phase relaxation time less than the field cycle, the field half-cycle can serve as a subfemtosecond probe of coherent vibrations. In this regime, the high-frequency field-induced modulation of molecular dipole moments gives rise to a detectable modulation of the optical response of a medium at the frequency $2\ensuremath{\omega}$, $\ensuremath{\omega}$ being the frequency of the laser field.
Summary form only given.A less well understood regime of quantum optical systems is the case when they are far from equilibrium and highly nonlinear. One device that inherently operates in this regime is the two-photon laser that is based on the two-photon-stimulated emission process, whereby two photons stimulate the emission of four photons. Such lasers are predicted to have highly unusual nonlinear dynamic and quantum statistical behaviors. Recently, our group demonstrated large continuous-wave two-photon amplification in a laser-driven potassium vapor based on a multiphoton Raman scattering process. Subsequent studies have revealed that destructive interference between multiple quantum pathways significantly reduces the two-photon-stimulated emission rate for this process. To overcome this problem, we have devised a new mechanism for two-photon amplification that suppresses the quantum interference using electromagnetically induced transparency in conjunction with a novel geometry.
The work is aimed at modeling coherence effects in a dissipative quantum system under the semi-classical density matrix formalism. A number of multiphoton coherence effects have been shown to be feasible by controlling the incoherent pumping mechanism in a generic four-level model. The specialty of the model is in finding inversionless gain without any restrictions being imposed on the decay rates of the driven transitions. Many of the coherence effects, such as absorption cancellation, inversionless gain at the line center, and sidebands of an absorptive line shape accompanied by dispersive switching, are explained using the same model under different parametric conditions. Further, it is shown that modulation in the coherence effects can effectively be controlled by the two- and three-photon excitation mechanisms with the proper choice of the rates of incoherent pumping under a stimulated Raman process. Different conditions of population inversion are found for both coherent and incoherent control of stimulated Raman resonance. In addition to Raman gain, gain without inversion in any standard state basis is found to be achieved in our present model. The proposed scheme can have potential application in controlling the properties of an optical field on propagation through rare earth ion-doped fiber material or other solid-state, as well as atomic, media.