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Register a new userCorrelations of cascaded photons: An analytical study in the two-photon Mollow regime
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Mollow physics in the two-photon regime shows interesting features such as path-controlled time-reordering of photon pairs without the need to delay them. Here, we calculate analytically the two-photon correlations $ g^{(2)}(tau)$, essential to discuss and study such phenomena in the resonant-driven dressed-state regime. It is shown that there exists upper and lower bounds of the $ g^{(2)}(tau)-$ function for certain spectrally-selected photon pairs. Recent reported experiments agree with the presented theory and thereby it is shown that the resonant-driven four-level system is an interesting source for steerable quantum light in quantum cascade setups. We furthermore discuss the unlikeliness to observe antibunching for the delay time $ tau=0 $ in the exciton-biexciton correlation functions in such experiments, since antibunching stems from a coherent and in-phase superposition of different photon emission events. Due to the occuring laser photon scattering, this coherent superposition state is easily disturbed and leads to correlation functions of $ g^{(2)}(0)=1$.
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Entangled two-photon absorption (ETPA) has recently become a topic of lively debate, mainly due to the apparent inconsistencies in the experimentally-reported ETPA cross sections of organic molecules. In this work, we provide a thorough experimental study of ETPA in the organic molecules Rhodamine B (RhB) and Zinc Tetraphenylporphirin (ZnTPP). The goal of this contribution is twofold: on one hand, it seeks to reproduce the results of previous experimental reports and, on the other, it aims to determine the effects of different temporal correlations -- introduced as a controllable time-delay between the photons to be absorbed -- on the strength of the ETPA signal. In our experiment, the samples are excited by entangled pairs produced by type-I SPDC, with a spectral distribution centered at 810 nm. Surprisingly, and contrary to what was expected, the time delay did not produce in our experiments any systematic change in the cross-sections when monitoring the ETPA signal using a transmission measurement scheme. As a plausible cause of this unexpected result, we argue that the photon-pair flux, typically-used in these experiments, is not sufficient to promote the two-photon absorption process in these molecules. This suggests that the actual absorption cross-section values are lower than those previously reported, and therefore do not lead to a measurable ETPA effect for the transmission method.
In this work we study the scattering of pairs of photons by a two-level system ultrastrongly coupled to a one-dimensional waveguide. We describe this problem using a spin-boson model with an Ohmic environment $J(omega)=pialphaomega^1.$ We show that when coupling strength lays is about $alphaleq 1,$ the dynamics is well approximated by a polaron Hamiltonian, under the approximation of a conserved number of excitations. In this regime, we develop analytical predictions for the single- and two-photon scattering matrix computed with a Greens function method.
We analyse the output quantum tripartite correlations from an intracavity nonlinear optical system which uses cascaded nonlinearities to produce both second and fourth harmonic outputs from an input field at the fundamental frequency. Using fully quantum equations of motion, we investigate two parameter regimes and show that the system produces tripartite inseparability, entanglement and EPR steering, with the detection of these depending on the correlations being considered.
While two-photon absorption (TPA) and other forms of nonlinear interactions of molecules with isolated time-frequency-entangled photon pairs (EPP) have been predicted to display a variety of fascinating effects, their potential use in practical quantum-enhanced molecular spectroscopy requires close examination. This paper presents a detailed theoretical study of quantum-enhanced TPA by both photon-number correlations and spectral correlations, including an account of the deleterious effects of dispersion. While such correlations in EPP created by spontaneous parametric down conversion can increase the TPA rate significantly in the regime of extremely low optical flux, we find that for typical molecules in solution this regime corresponds to such low TPA event rates as to be unobservable in practice. Our results support the usefulness of EPP spectroscopy in atomic or other narrow-linewidth systems, while questioning the efficacy of such approaches for broadband systems including molecules in solution.
The controllability of current quantum technologies allows to implement spin-boson models where two-photon couplings are the dominating terms of light-matter interaction. In this case, when the coupling strength becomes comparable with the characteristic frequencies, a spectral collapse can take place, i.e. the discrete system spectrum can collapse into a continuous band. Here, we analyze the thermodynamic limit of the two-photon Dicke model, which describes the interaction of an ensemble of qubits with a single bosonic mode. We find that there exists a parameter regime where two-photon interactions induce a superradiant phase transition, before the spectral collapse occurs. Furthermore, we extend the mean-field analysis by considering second-order quantum fluctuations terms, in order to analyze the low-energy spectrum and compare the critical behavior with the one-photon case.
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