2020/12/09 by Michael G. Raymer, Raymer, Michael G., Tiemo Landes +9
Computer Science · Physics and Astronomy · #FOS: Physical sciences #Mechanical and Optical Resonators #Quantum Information and Cryptography #Quantum Physics (quant-ph) #Quantum optics and atomic interactions #Spectroscopy and Quantum Chemical Studies
paper · pdf · doi:10.48550/arxiv.2012.05375
openalex publication_date 2020/12/09 · openalex created_date 2023/03/08 · openalex updated_date 2026/07/28
While two-photon absorption (TPA) and other forms of nonlinear interactions\nof molecules with isolated time-frequency-entangled photon pairs (EPP) have\nbeen predicted to display a variety of fascinating effects, their potential use\nin practical quantum-enhanced molecular spectroscopy requires close\nexamination. This paper presents a detailed theoretical study of\nquantum-enhanced TPA by both photon-number correlations and spectral\ncorrelations, including an account of the deleterious effects of dispersion.\nWhile such correlations in EPP created by spontaneous parametric down\nconversion can increase the TPA rate significantly in the regime of extremely\nlow optical flux, we find that for typical molecules in solution this regime\ncorresponds to such low TPA event rates as to be unobservable in practice. Our\nresults support the usefulness of EPP spectroscopy in atomic or other\nnarrow-linewidth systems, while questioning the efficacy of such approaches for\nbroadband systems including molecules in solution.\n