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 vs. 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.

Few-layer transition-metal dichalcogenide WSe2/MoSe2 nanosheets are fabricated by a liquid exfoliation technique using sodium deoxycholate bile salt as surfactant, and their nonlinear optical properties are investigated based on a balanced twin-detector measurement scheme. It is demonstrated that both types of nanosheets exhibit nonlinear saturable absorption properties at the wavelength of 1.55 μm. By depositing the nanosheets on side polished fiber (SPF) or mixing the nanosheets with polyvinyl alcohol (PVA) solution, SPF-WSe2 saturable absorber (SA), SPF-MoSe2 SA, PVA-WSe2 SA, and PVA-MoSe2 SA are successfully fabricated and further tested in erbium-doped fiber lasers. The SPF-based SA is capable of operating at the high pump regime without damage, and a train of 3252.65 MHz harmonically mode-locked pulses are obtained based on the SPF-WSe2 SA. Soliton mode locking operations are also achieved in the fiber laser separately with other three types of SAs, confirming that the WSe2 and MoSe2 nanosheets could act as cost-effective high-power SAs for ultrafast optics.

We report a random delayed-choice quantum eraser experiment. In a Young's double-slit interferometer, the which-slit information is learned from the photon-number fluctuation correlation of thermal light. The reappeared interference indicates that the which-slit information of a photon, or wave packet, can be "erased" by a second photon or wave packet, even after the annihilation of the first. Different from an entangled photon pair, the jointly measured two photons, or wave packets, are just two randomly distributed and randomly created photons of a thermal source that fall into the coincidence time window. The experimental observation can be explained as a nonlocal interference phenomenon in which a random photon or wave packet pair, interferes with the pair itself at distance.

We present a flexible approach to generate arbitrary vector beams with a trapezoid Sagnac interferometer. With the interferometer, the different orders of two orthogonally polarized beams from computer-generated holograms coincide with each other in Fourier spectrum domain, and coaxially combine into the vector beams. This approach provides convenient way to experimentally study the properties of vector beams with complex polarization.

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.