Nonlinear fluctuations and dissipation in matter revealed by quantum light

Quantum optical fields offer numerous control knobs which are not available with classical light and may be used for monitoring the properties of matter by novel types of spectroscopy. It has been recently argued that such quantum spectroscopy signals can be obtained by a simple averaging of their classical spectroscopy counterparts over the Glauber-Sudarshan quasiprobability distribution of the quantum field; the quantum light thus merely provides a novel gating window for the classical response functions. We show that this argument only applies to the linear response and breaks down in the nonlinear regime. The quantum response carries additional valuable information about response and spontaneous fluctuations of matter that may not be retrieved from the classical response by simple data processing. This is connected to the lack of a nonlinear fluctuation-dissipation relation.

Figure 1

Loop diagrams for the third-order nonlinear response. The time runs along the loop forward in left branch and backward in the right branch. Time translation invariance enforces $\omega -{\omega }_1-{\omega }_2-{\omega }_3=0$. For diagram rules, see [35]. Since we do not invoke rotating wave approximation, field-matter interactions depicted by blue lines do not have arrows indicating whether it is creation or annihilation operator. Interaction with $\omega$ has an arrow as it represents the signal in the form of Eq. (4), where having negative frequency component is necessary.