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Register a new userExperimental study on the effects of photon-pair temporal correlations in entangled two-photon absorption
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Added by
Roberto Le\\'on-Montiel
Publication date
2021
fields
Physics
and research's language is
English
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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.
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Entangled photon pairs have been promised to deliver a substantial quantum advantage for two-photon absorption spectroscopy. However, recent work has challenged the previously reported magnitude of quantum enhancement in two-photon absorption. Here, we present an experimental comparison of sum-frequency generation and molecular absorption, each driven by isolated photon pairs. We establish an upper bound on the enhancement for entangled-two-photon absorption in Rhodamine-6G, which lies well below previously reported values.
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.
Entangled two-photon absorption spectroscopy (TPA) has been widely recognized as a powerful tool for revealing relevant information about the structure of complex molecular systems. However, to date, the experimental implementation of this technique has remained elusive, mainly because of two major difficulties. First, the need to perform multiple experiments with two-photon states bearing different temporal correlations, which translates in the necessity to have at the experimenters disposal tens, if not hundreds, of sources of entangled photons. Second, the need to have emph{a priori} knowledge of the absorbing mediums lowest-lying intermediate energy level. In this work, we put forward a simple experimental scheme that successfully overcomes these two limitations. By making use of a temperature-controlled entangled-photon source, which allows the tuning of the central frequencies of the absorbed photons, we show that the TPA signal, measured as a function of the temperature of the nonlinear crystal that generates the paired photons, and a controllable delay between them, carries all information about the electronic level structure of the absorbing medium, which can be revealed by a simple Fourier transformation.
Multiplexed quantum memories capable of storing and processing entangled photons are essential for the development of quantum networks. In this context, we demonstrate the simultaneous storage and retrieval of two entangled photons inside a solid-state quantum memory and measure a temporal multimode capacity of ten modes. This is achieved by producing two polarization entangled pairs from parametric down conversion and mapping one photon of each pair onto a rare-earth-ion doped (REID) crystal using the atomic frequency comb (AFC) protocol. We develop a concept of indirect entanglement witnesses, which can be used as Schmidt number witness, and we use it to experimentally certify the presence of more than one entangled pair retrieved from the quantum memory. Our work puts forward REID-AFC as a platform compatible with temporal multiplexing of several entangled photon pairs along with a new entanglement certification method useful for the characterisation of multiplexed quantum memories.
We show that temporal two-photon interference effects involving the signal and idler photons created by parametric down-conversion can be fully characterized in terms of the variations of two length parameters--called the biphoton path-length difference and the biphoton path-asymmetry- length difference--which we construct using the six different length parameters that a general two-photon interference experiment involves. We perform an experiment in which the effects of the variations of these two parameters can be independently controlled and studied. In our experimental setup, which does not involve mixing of signal and idler photons at a beam splitter, we further report observations of Hong-Ou-Mandel- (HOM-)like effects both in coincidence and in one-photon count rates. As an important consequence, we argue that the HOM and the HOM-like effects are best described as observations of how two-photon coherence changes as a function of the biphoton path- asymmetry-length difference.
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