Unveiling the interplay of Mollow physics and perturbed free induction decay by nonlinear optical signals of a dynamically driven two-level system

Abstract

Nonlinear optical signals in optically driven quantum systems can reveal coherences and thereby open up the possibility for manipulation of quantum states. While the limiting cases of ultrafast and continuous-wave excitation have been extensively studied, the time dynamics of finite pulses bear interesting phenomena. In this paper, we explore the nonlinear optical probe signals of a two-level system excited with a laser pulse of finite duration. In addition to the prominent Mollow peaks, the probe spectra feature several smaller peaks for certain time delays. Similar features have been recently observed for resonance fluorescence signals [K. Boos et al., Phys. Rev. Lett. 132, 053602 (2024)]. We discuss that the emergent phenomena can be explained by a combination of Mollow triplet physics and perturbed free induction decay effects, providing an insightful understanding of the underlying physics.