Two-photon absorption cross sections of pulsed entangled beams.

Entangled two-photon absorption (ETPA) could form the basis of nonlinear quantum spectroscopy at very low photon fluxes, since, at sufficiently low photon fluxes, ETPA scales linearly with the photon flux. When different pairs start to overlap temporally, accidental coincidences are thought to give rise to a "classical" quadratic scaling that dominates the signal at large photon fluxes and, thus, recovers a supposedly classical regime, where any quantum advantage is thought to be lost. Here, we scrutinize this assumption and demonstrate that quantum-enhanced absorption cross sections can persist even for very large photon numbers.

Nonlinear Interferometry for Quantum-Enhanced Measurements of Multiphoton Absorption.

Multiphoton absorption is of vital importance in many spectroscopic, microscopic, or lithographic applications. However, given that it is an inherently weak process, the detection of multiphoton absorption signals typically requires large field intensities, hindering its applicability in many practical situations. In this Letter, we show that placing a multiphoton absorbent inside an imbalanced nonlinear interferometer can enhance the precision of multiphoton cross section estimation with respect to strategies based on photon-number measurements using coherent or even squeezed light directly transmitted through the medium.

Multidimensional four-wave mixing signals detected by quantum squeezed light.

Four-wave mixing (FWM) of optical fields has been extensively used in quantum information processing, sensing, and memories. It also forms a basis for nonlinear spectroscopies such as transient grating, stimulated Raman, and photon echo where phase matching is used to select desired components of the third-order response of matter. Here we report an experimental study of the two-dimensional quantum noise intensity difference spectra of a pair of squeezed beams generated by FWM in hot Rb vapor.

Optimization of selective two-photon absorption in cavity polaritons.

We investigate optimal states of photon pairs to excite a target transition in a multilevel quantum system. With the help of coherent control theory for two-photon absorption with quantum light, we infer the maximal population achievable by optimal entangled vs separable states of light. Interference between excitation pathways as well as the presence of nearby states may hamper the selective excitation of a particular target state, but we show that quantum correlations can help to overcome this problem and enhance the achievable "selectivity" between two energy levels, i.

Detection of photon statistics and multimode field correlations by Raman processes.

Glauber's g-function provides a common measure of quantum field statistics through two-photon coincidence counting in Hanbury Brown-Twiss measurements. Here, we propose to use nonlinear optical signals as a tool for the characterization of quantum light. In particular, we show that Raman measurements provide an alternative direct probe for a different component of the four-point correlation function underlying the g-function.

Photoinduced Electron Pairing in a Driven Cavity.

We demonstrate how virtual scattering of laser photons inside a cavity via two-photon processes can induce controllable long-range electron interactions in two-dimensional materials. We show that laser light that is red (blue) detuned from the cavity yields attractive (repulsive) interactions whose strength is proportional to the laser intensity. Furthermore, we find that the interactions are not screened effectively except at very low frequencies.

Photon Correlation Spectroscopy as a Witness for Quantum Coherence.

The development of spectroscopic techniques able to detect and verify quantum coherence is a goal of increasing importance given the rapid progress of new quantum technologies, the advances in the field of quantum thermodynamics, and the emergence of new questions in chemistry and biology regarding the possible relevance of quantum coherence in biochemical processes. Ideally, these tools should be able to detect and verify the presence of quantum coherence in both the transient dynamics and the steady state of driven-dissipative systems, such as light-harvesting complexes driven by thermal photons in natural conditions. This requirement poses a challenge for standard laser spectroscopy methods.

Cavity-Mediated Unconventional Pairing in Ultracold Fermionic Atoms.

We investigate long-range pairing interactions between ultracold fermionic atoms confined in an optical lattice which are mediated by the coupling to a cavity. In the absence of other perturbations, we find three degenerate pairing symmetries for a two-dimensional square lattice. By tuning a weak local atomic interaction via a Feshbach resonance or by tuning a weak magnetic field, the superfluid system can be driven from a topologically trivial s wave to topologically ordered, chiral superfluids containing Majorana edge states.

Cavity-Mediated Electron-Photon Superconductivity.

We investigate electron paring in a two-dimensional electron system mediated by vacuum fluctuations inside a nanoplasmonic terahertz cavity. We show that the structured cavity vacuum can induce long-range attractive interactions between current fluctuations which lead to pairing in generic materials with critical temperatures in the low-kelvin regime for realistic parameters. The induced state is a pair-density wave superconductor which can show a transition from a fully gapped to a partially gapped phase-akin to the pseudogap phase in high-T_{c} superconductors.

Entangled Two-Photon Absorption Spectroscopy.

The application of quantum states of light such as entangled photons, for example, created by parametric down conversion, has experienced tremendous progress in the almost 40 years since their first experimental realization. Initially, they were employed in the investigation of the foundations of quantum physics, such as the violation of Bell's inequalities and studies of quantum entanglement. They later emerged as basic platforms for quantum communication protocols and, in the recent experiments on single-photon interactions, in photonic quantum computation.

Probing polariton dynamics in trapped ions with phase-coherent two-dimensional spectroscopy.

We devise a phase-coherent three-pulse protocol to probe the polariton dynamics in a trapped-ion quantum simulation. In contrast to conventional nonlinear signals, the presented scheme does not change the number of excitations in the system, allowing for the investigation of the dynamics within an N-excitation manifold. In the particular case of a filling factor one (N excitations in an N-ion chain), the proposed interaction induces coherent transitions between a delocalized phonon superfluid and a localized atomic insulator phase.

Two-photon spectroscopy of excitons with entangled photons.

The utility of quantum light as a spectroscopic tool is demonstrated for frequency-dispersed pump-probe, integrated pump-probe, and two-photon fluorescence signals which show Ramsey fringes. Simulations of the frequency-dispersed transmission of a broadband pulse of entangled photons interacting with a three-level model of matter reveal how the non-classical time-bandwidth properties of entangled photons can be used to disentangle congested spectra, and reveal otherwise unresolved features. Quantum light effects are most pronounced at weak intensities when entangled photon pairs are well separated, and are gradually diminished at higher intensities when different photon pairs overlap.

Suppression of population transport and control of exciton distributions by entangled photons.

Entangled photons provide an important tool for secure quantum communication, computing and lithography. Low intensity requirements for multi-photon processes make them idealy suited for minimizing damage in imaging applications. Here we show how their unique temporal and spectral features may be used in nonlinear spectroscopy to reveal properties of multiexcitons in chromophore aggregates.