Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userExperimental feasibility of molecular two-photon absorption with isolated time-frequency-entangled photon pairs
99
0
0.0
(
0
)
Ask ChatGPT about the research
No Arabic abstract
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.
rate research
Read More
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.
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.
Photonic time-frequency entanglement is a promising resource for quantum information processing technologies. We investigate swapping of continuous-variable entanglement in the time-frequency degree of freedom using three-wave mixing in the low-gain regime with the aim of producing heralded biphoton states with high purity and low multi-pair probability. Heralding is achieved by combining one photon from each of two biphoton sources via sum-frequency generation to create a herald photon. We present a realistic model with pulsed pumps, investigate the effects of resolving the frequency of the herald photon, and find that frequency-resolving measurement of the herald photon is necessary to produce high-purity biphotons. We also find a trade-off between the rate of successful entanglement swapping and both the purity and quantified entanglement resource (negativity) of the heralded biphoton state.
The authors demonstrate a form of two-photon-counting interferometry by measuring the coincidence counts between single-photon-counting detectors at an output port of a Mach-Zehnder Interferometer (MZI) following injection of broad-band time-frequency-entangled photon pairs (EPP) generated from collinear spontaneous parametric down conversion into a single input port. Spectroscopy and refractometry are performed on a sample inserted in one internal path of the MZI by scanning the other path in length, which acquires phase and amplitude information about the samples linear response. Phase modulation and lock-in detection are introduced to increase detection signal-to-noise ratio and implement a down-sampling technique for scanning the interferometer delay, which reduces the sampling requirements needed to reproduce fully the temporal interference pattern. The phase-modulation technique also allows the contributions of various quantum-state pathways leading to the final detection outcomes to be extracted individually. Feynman diagrams frequently used in the context of molecular spectroscopy are used to describe the interferences resulting from the coherence properties of time-frequency EPPs passing through the MZI. These results are an important step toward implementation of a proposed method for molecular spectroscopy, i.e. quantum-light-enhanced two-dimensional spectroscopy.
Energy-time entangled photons are critical in many quantum optical phenomena and have emerged as important elements in quantum information protocols. Entanglement in this degree of freedom often manifests itself on ultrafast timescales making it very difficult to detect, whether one employs direct or interferometric techniques, as photon-counting detectors have insufficient time resolution. Here, we implement ultrafast photon counters based on nonlinear interactions and strong femtosecond laser pulses to probe energy-time entanglement in this important regime. Using this technique and single-photon spectrometers, we characterize all the spectral and temporal correlations of two entangled photons with femtosecond resolution. This enables the witnessing of energy-time entanglement using uncertainty relations and the direct observation of nonlocal dispersion cancellation on ultrafast timescales. These techniques are essential to understand and control the energy-time degree of freedom of light for ultrafast quantum optics.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
