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Register a new userMultidimensional spectroscopy with entangled light; loop vs ladder delay scanning protocols
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Multidimensional optical signals are commonly recorded by varying the delays between time ordered pulses. These control the evolution of the density matrix and are described by ladder diagrams. We propose a new non-time-ordered protocol based on following the time evolution of the wavefunction and described by loop diagrams. The time variables in this protocol allow to observe different types of resonances and reveal information about intraband dephasing not readily available by time ordered techniques. The time variables involved in this protocol become coupled when using entangled light, which provides high selectivity and background free measurement of the various resonances. Entangled light can resolve certain states even when strong background due to fast dephasing suppresses the resonant features when probed by classical light.
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We propose a novel femtosecond stimulated Raman spectroscopy (FSRS) technique that combines entangled photons with interference detection to select matter pathways and enhance the resolution. Following photo excitation by an actinic pump, the measurement uses a pair of broadband entangled photons, one (signal) interacts with the molecule together with a third narrowband pulse induces the Raman process. The other (idler) photon provides a reference for the coincidence measurement. This interferometric photon-coincidence counting detection allows to separately measure Raman gain and loss signals, which is not possible with conventional probe transmission detection. Entangled photons further provide a unique temporal and spectral detection window that can better resolve fast excited state dynamics compared to classical and correlated disentangled states of light.
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.
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.
Correlated photons inspire abundance of metrology-related platforms, which benefit from quantum (anti-) correlations and outperform their classical-light counterparts. While such demonstrations mainly focus on entanglement, the role of photon exchange-phase and degree of distinguishability have not been widely utilized in quantum-enhanced applications. Using an interferometric setup we show that even at low degree entanglement, when a two-photon wave-function is coupled to matter, it is encoded with a reliable which pathway? information. An interferometric exchange-phase-cycling protocol is developed, which enables phase-sensitive discrimination between microscopic interaction histories (pathways). We find that quantum-light interferometry facilitates utterly different set of time-delay variables, which are unbound by uncertainty to the inverse bandwidth of the wave-packet. We illustrate our findings on an exciton model-system, and demonstrate how to probe intraband dephasing in time-domain without temporal resolution at the detection. The exotic scaling of multiphoton coincidence with respect to the applied intensity is discussed.
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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