Interferometric two-photon-absorption spectroscopy with three entangled photons

Ye, Lyuzhou; Mukamel, Shaul

doi:10.1063/5.0004617

Cited by 10 publications

(11 citation statements)

References 24 publications

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“…Furthermore, we demonstrated that the transmission measurement could provide the same information contents as in heterodyned four-wave mixing signals, such as 2D Fourier-transformed photon echo, although a simple optical system and simple light source are employed. This correspondence inspires us to anticipate that the usage of more elaborately engineered quantum states of light [46][47][48] would broaden the availability of quantum light spectroscopy [49] or molecular quantum metrology. The extensions of the present work in these directions are to be explored in future studies.…”

Section: Discussionmentioning

confidence: 98%

Probing excited-state dynamics with quantum entangled photons: Correspondence to coherent multidimensional spectroscopy

Ishizaki

2020

Preprint

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Quantum light is a key resource for promoting quantum technology. One such class of technology aims to improve the precision of optical measurements using engineered quantum states of light. In this study, we investigate transmission measurement of frequency-entangled broadband photon pairs generated via parametric down-conversion with a monochromatic laser. It is observed that state-to-state dynamics in the system under study are temporally resolved by adjusting the path difference between the entangled twin beams when the entanglement time is sufficiently short. The non-classical photon correlation enables time-resolved spectroscopy with monochromatic pumping. It is further demonstrated that the signal corresponds to the spectral information along anti-diagonal lines of, for example, two-dimensional Fourier-transformed photon echo spectra. This correspondence inspires us to anticipate that more elaborately engineered photon states would broaden the availability of quantum light spectroscopy.

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Section: Discussionmentioning

confidence: 98%

Probing excited-state dynamics with quantum entangled photons: Correspondence to coherent multidimensional spectroscopy

Ishizaki

2020

Preprint

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“…For simplicity, we consider the electric fields inside the one-dimensional nonlinear crystals. In the weak down-conversion regime, the state vector of the generated three photons is written as 65,71,75…”

Section: Theorymentioning

confidence: 99%

“…The momentum mismatch between the input and output photons in the n-th nonlinear crystal is expressed by ∆k n (ω, ω ′ ), and the length of the n-th crystal is given by L n . The momentum mismatches may be linearly approximated around the central frequencies of the generated beams, ωσ , as in 71,75 1. Schematic of frequency-dispersed two-photon coincidence counting measurement using entangled three photons generated via cascaded PDC pumped with a monochromatic laser of frequency ωp.…”

Section: Theorymentioning

confidence: 99%

“…In this study, we investigate a spectroscopic method to overcome the difficulties associated with implementing timeresolved entangled photon spectroscopy. The central idea is to use entangled three photons [60][61][62][63][64][65][66][67][68][69][70][71][72][73][74][75] and frequency-dispersed two-photon coincidence counting measurements. In this scheme, two of the three photons are irradiated into the molecular sample to induce a nonlinear optical process, while the remaining photon is detected in coincidence with the probe field transmitted through the sample.…”

Section: Introductionmentioning

confidence: 99%

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Achieving two-dimensional optical spectroscopy with temporal and spectral resolution using quantum entangled three photons

Fujihashi,

Ishizaki

2021

Preprint

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Recent advances in techniques for generating quantum light have stimulated research on novel spectroscopic measurements using quantum entangled photons. One such spectroscopy technique utilizes non-classical correlations among entangled photons to enable measurements with enhanced sensitivity and selectivity. Here, we investigate spectroscopic measurement utilizing entangled three photons generated through cascaded parametric down-conversion. In this measurement, time-resolved entangled photon spectroscopy with monochromatic pumping [J. Chem. Phys. 153, 051102 (2020).] is integrated with the frequency-dispersed two-photon counting technique, which suppresses undesired accidental photon counts in the detector and thus allows one to separate the weak desired signal. This time-resolved frequency-dispersed two-photon counting signal, which is a function of two frequencies, is shown to provide the same information as that of coherent two-dimensional optical spectra. The spectral distribution of the phase-matching function works as a frequency filter to selectively resolve a specific region of the two-dimensional spectra, whereas the excited-state dynamics under investigation are temporally resolved in the time region longer than the entanglement time. The signal is not subject to Fourier limitations on the joint temporal and spectral resolution, and therefore, it is expected to be useful for investigating complex molecular systems in which multiple electronic states are present within a narrow energy range.

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“…[1][2][3][4][5] Such studies can also be extended to the domain of the characterization of unknown matter properties, where the non-classical correlation features of the optical modes induce controlled dynamical evolution of the matter modes, thereby emphasizing their scope as spectroscopic probes. [6][7][8][9][10] In such studies, the resultant spectral features of the matter modes crucially depend on the windowed dynamics in the joint time-frequency space, which were controllably induced. Depending on their generation processes, the photonic modes can be entangled in temporal-spectral, polarization, or the orbital angular momentum degrees of freedom.…”

Section: Introductionmentioning

confidence: 99%

Entangled photon assisted multidimensional nonlinear optics of exciton–polaritons

Debnath

Rubio

2020

Journal of Applied Physics

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We present a theoretical formulation of the frequency domain multidimensional pump-probe analog spectroscopy, which utilizes the spectral-temporal entanglement features of the biphoton sources. It has been shown, via a compact multi-time, convolutional Green's function expression and the accompanying numerical simulations, that utilizing the correlation properties of non-classical sources offers a viable scheme for the exploration of dissipative kinetics of the cavity confined quantum aggregates. The cooperative and competitive modifications brought in by the photonic cavity mode and the auxiliary vibrational modes into the scattering and dephasing properties of the excitonpolaritons have been explored via their signatures in the multidimensional correlation maps. The study offers a new parameter window for the investigation of the dynamical polariton characteristics and warrants the usage of multi-mode entanglement properties of the external photonic sources in future studies.

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Interferometric two-photon-absorption spectroscopy with three entangled photons

Cited by 10 publications

References 24 publications

Probing excited-state dynamics with quantum entangled photons: Correspondence to coherent multidimensional spectroscopy

Probing excited-state dynamics with quantum entangled photons: Correspondence to coherent multidimensional spectroscopy

Achieving two-dimensional optical spectroscopy with temporal and spectral resolution using quantum entangled three photons

Entangled photon assisted multidimensional nonlinear optics of exciton–polaritons

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