Vanishing and Revival of Resonance Raman Scattering

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-$\mathrm{\ensuremath{\Lambda}}$ 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.