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.

We demonstrate the creation, characterization, and manipulation of frequency-entangled qudits by shaping the energy spectrum of entangled photons. The generation of maximally entangled qudit states is verified up to dimension $d=4$ through tomographic quantum-state reconstruction. Subsequently, we measure Bell parameters for qubits and qutrits as a function of their degree of entanglement. In agreement with theoretical predictions, we observe that for qutrits the Bell parameter is less sensitive to a varying degree of entanglement than for qubits. For frequency-entangled photons, the dimensionality of a qudit is ultimately limited by the bandwidth of the pump laser and can be on the order of a few millions.

The Abbe–Rayleigh diffraction limit constrains spatial resolution for classical imaging methods. Quantum imaging exploits correlations between photons to reproduce structures with higher resolution. Quantum-correlated $N$-photon states were shown to potentially surpass the classical limit by a factor of $1/N$, corresponding to the Heisenberg limit, using a method known as optical centroid measurement (OCM). In this work, the theory of OCM is reformulated for its application in imaging. Using entangled photon pairs and a recently developed integrated time-resolving detector array, OCM is implemented in a proof-of-principle experiment that demonstrates the expected enhancement. Those results show the relevance of entanglement for imaging at the Heisenberg limit.

Multisimultaneity is a causal model of relativistic quantum physics which assigns a real time ordering to any set of events, much in the spirit of the pilot-wave picture. Contrary to standard quantum mechanics, it predicts a disappearance of the correlations in a Bell-type experiment when both analyzers are in relative motion such that each one, in its own inertial reference frame, is first to select the output of the photons. We tested this prediction using acousto-optic modulators as moving beam splitters and interferometers separated by 55 m. We did not observe any disappearance of the correlations, in agreement with quantum mechanics.