We propose a scheme to entangle two magnon modes via the Kerr nonlinear effect when driving the systems far from equilibrium. We consider two macroscopic yttrium iron garnets interacting with a single-mode microcavity through the magnetic dipole coupling. The Kittel mode describing the collective excitations of a large number of spins is excited through the driving cavity with a strong microwave field. We demonstrate how Kerr nonlinearity creates the entangled quantum states between the two macroscopic ferromagnetic samples, when the microcavity is strongly driven by a blue-detuned microwave field. Such quantum entanglement survives at the steady state. Our work offers insights and guidance in designing experiments for observing entanglement in massive ferromagnetic materials. It can also find broad applications in macroscopic quantum effects and magnetic spintronics.

Conventional spectroscopy uses classical light to detect matter properties through the variation of its response with frequencies or time delays. Quantum light opens up new avenues for spectroscopy by utilizing parameters of the quantum state of light as novel control knobs and through the variation of photon statistics by coupling to matter. This Roadmap article focuses on using quantum light as a powerful sensing and spectroscopic tool to reveal novel information about complex molecules that is not accessible by classical light. It aims at bridging the quantum optics and spectroscopy communities which normally have opposite goals: manipulating complex light states with simple matter e.g. qubits versus studying complex molecules with simple classical light, respectively. Articles cover advances in the generation and manipulation of state-of-the-art quantum light sources along with applications to sensing, spectroscopy, imaging and interferometry.

Quantum entanglement has emerged as a great resource for spectroscopy and its importance in two-photon spectrum and microscopy has been demonstrated. Current studies focus on the two-photon absorption, whereas the Raman spectroscopy with quantum entanglement still remains elusive, with outstanding issues of temporal and spectral resolutions. Here we study the new capabilities provided by entangled photons in coherent Raman spectroscopy. An ultrafast frequency-resolved Raman spectroscopy with entangled photons is developed for condensed-phase molecules, to probe the electronic and vibrational coherences. Using quantum correlation between the photons, the signal shows the capability of both temporal and spectral resolutions not accessible by either classical pulses or the fields without entanglement. We develop a microscopic theory for this Raman spectroscopy, revealing the electronic coherence dynamics even at timescale of 50fs. This suggests new paradigms of optical signals and spectroscopy, with potential to push detection below standard quantum limit.

Fröhlich discovered the remarkable condensation of polar vibrations into the lowest frequency mode when the system is pumped externally. For a full understanding of the Fröhlich condensate one needs to go beyond the mean field level to describe critical behavior as well as quantum fluctuations. The energy redistribution among vibrational modes with nonlinearity included is shown to be essential for realizing the condensate and the phonon-number distribution, revealing the transition from quasithermal to super-Poissonian statistics with the pump. We further study the spectroscopic properties of the Fröhlich condensate, which are especially revealed by the narrow linewidth. This gives the long-lived coherence and the collective motion of the condensate. Finally, we show that the proteins such as bovine serum albumin and lysozyme are most likely the candidates for observing such collective modes in THz regime by means of Raman or infrared spectroscopy.

Quantum entanglement has emerged as a great resource for studying the interactions between molecules and radiation. We propose a new scheme of stimulated Raman scattering with entangled photons. A quantum ultrafast Raman spectroscopy is developed for condensed-phase molecules, to monitor the exciton populations and coherences. Analytic results are obtained, showing an entanglement-enabled time-frequency scale not attainable by classical light. The Raman signal presents an unprecedented selectivity of molecular correlation functions, as a result of the Hong-Ou-Mandel interference. Our work suggests a new paradigm of using an unconventional interferometer as part of spectroscopy, with the potential to unveil advanced information about complex materials.

The cavity-mediated spin current between two ferrite samples has been reported by Bai et al., [ Phys. Rev. Lett. 118, 217201 (2017)]. This experiment was done in the linear regime of the interaction in the presence of external drive. In the current paper, we develop a theory for the spin current in the nonlinear domain where the external drive is strong so that one needs to include the Kerr nonlinearity of the ferrite materials. In this manner, the nonlinear polaritons are created and one can reach both bistable and multistable behavior of the spin current. The system is driven into a far-from-equilibrium steady state that is determined by the details of the driving field and various interactions. We present a variety of steady-state results for the spin current. A spectroscopic detection of the nonlinear spin current is developed, revealing the key properties of the nonlinear polaritons. The transmission of a weak probe is used to obtain quantitative information on the multistable behavior of the spin current. The results and methods that we present are quite generic and can be used in many other contexts where cavities are used to transfer information from one system to another, e.g., two different molecular systems.