Enhanced vibrational-mode-selective two-step excitation using ultrabroadband frequency-entangled photons

Oka, Hisaki

doi:10.1103/physreva.97.063859

Cited by 23 publications

(12 citation statements)

References 30 publications

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“…The specific QI effect considered in this paper reveals itself as a fast, nonmonotonic modulation of the ETPA profile as a function of the delay between two components of the entangled pair within a delay time window shorter than entanglement time T e . , The modulation is the result of the interference between different pathways through which two photon excitation of the medium can occur. − While this specific interference effect theoretically suggests very promising applications of the nonclassical states of light such as virtual state spectroscopy − and highly selective excitation of the specific states, − the experimental information on it is very limited and related physical mechanisms are not well understood. ,,, …”

Section: Introductionmentioning

confidence: 89%

Two-Photon Fluorescence Microscopy at Extremely Low Excitation Intensity: The Power of Quantum Correlations

2020

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Quantum entanglement has been shown to imply correlations stronger than those allowed by classical models. The possibility of performing tasks that are classically impossible has made quantum entanglement a powerful resource for the development of novel methods and applications in various fields of research such as quantum computing, quantum cryptography, and quantum metrology. There is a great need for the development of next generation instrumentation and technologies utilizing entangled quantum light. Among the many applications of nonclassical states of light, nonlinear microscopy has the potential to make an impact in broad areas of science from physics to biology. Here, the microscopic image created by the fluorescence selectively excited by the process of the entangled two-photon absorption is reported. Entangled two-photon microscopy offers nonlinear imaging capabilities at an unprecedented low excitation intensity 107, which is 6 orders of magnitude lower than the excitation level for the classical two-photon image. The nonmonotonic dependence of the image on the femtosecond delay between the components of the entangled photon pair is demonstrated. This delay dependence is a result of specific quantum interference effects associated with the entanglement and this is not observable with classical excitation light. In combination with novel spectroscopic capabilities provided by a nonclassical light excitation, this is of critical importance for sensing and biological applications.

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Section: Introductionmentioning

confidence: 89%

Two-Photon Fluorescence Microscopy at Extremely Low Excitation Intensity: The Power of Quantum Correlations

2020

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“…Entangled photon pairs also linearize multiphoton and nonlinear spectroscopy, as has been well-studied in two photon absorption and fluorescence [7][8][9][10][11][12][13] . Entangled photons also have non-Fourier reciprocal spectral-temporal resolutions and are able to yield spatial resolutions which scale inversely with the number of correlated entangled photons N [14][15][16][17][18] .…”

Section: Introductionmentioning

confidence: 99%

Designing high-power, octave spanning entangled photon sources for quantum spectroscopy

Szoke

Hickam

et al. 2021

The Journal of Chemical Physics

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Entangled photon spectroscopy is a nascent field that has important implications for measurement and imaging across chemical, biology, and materials fields. Entangled photon spectroscopy potentially offers improved spatial and temporal-frequency resolutions, increased cross sections for multiphoton and nonlinear measurements, and new abilities in inducing or measuring quantum correlations. A critical step in enabling entangled photon spectroscopies is the creation of high-flux entangled sources that can use conventional detectors, as well as provide redundancy for the losses in realistic samples. Here, we report a periodically poled, chirped, lithium tantalate platform that generates entangled photon pairs with a ∼ 10 −7 efficiency. For a near watt level diode laser, this results in a near µW-level flux. The single photon per mode limit that is necessary to maintain non-classical photon behavior is still satisfied by distributing this power over up to an octave-spanning bandwidth. The spectral-temporal photon correlations are observed via a Michelson-type interferometer that measures the broadband Hong-Ou-Mandel two-photon interference. A coherence time of 245 fs for a 10 nm bandwidth in the collinear case and a 62 fs for a 125 nm bandwidth in the non-collinear case is measured using a CW pump laser, and, essentially, collecting the full photon cone. We outline in detail the numerical methods used for designing and tailoring the entangled photons source, such as changing center wavelength or bandwidth, with the ultimate aim of increasing the availability of high-flux UV-Vis entangled photon sources in the optical spectroscopy community.

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“…Among different quantum-enabled techniques, entangled two-photon absorption spectroscopy [14][15][16][17][18][19][20][21][22][23][24][25][26][27][28][29][30] has long been recognized as a promising spectroscopic tool for extracting the information about the electronic levels that participate in the two-photon excitation of a molecular samples. Although there is a current debate on the true quantum enhancement that such a technique might offer to spectroscopy [31][32][33], the experimental demonstration of its working principle, the socalled entangled two-photon absorption (eTPA), has become a topic of lively interest [34][35][36][37].…”

Section: Introductionmentioning

confidence: 99%

Quantum interferometric two-photon excitation spectroscopy

Chen

León‐Montiel

Chen

2021

Preprint

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Two-photon excitation spectroscopy is a nonlinear technique that has gained rapidly in interest and significance for studying the complex energy-level structure and transition probabilities of materials. While the conventional spectroscopy based on tunable classical light has been long established, quantum light provides an alternative way towards excitation spectroscopy with potential advantages in temporal and spectral resolution, as well as reduced photon fluxes. By using a quantum Fourier transform that connects the sum-frequency intensity and N00N-state temporal interference, we present an approach for quantum interferometric two-photon excitation spectroscopy. Our proposed protocol overcomes the difficulties of engineering two-photon joint spectral intensities and fine-tuned absorption-frequency selection. These results may significantly facilitate the use of quantum interferometric spectroscopy for extracting the information about the electronic structure of the twophoton excited-state manifold of atoms or molecules, in a "single-shot" measurement. This may be particularly relevant for photon-sensitive biological and chemical samples.

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Enhanced vibrational-mode-selective two-step excitation using ultrabroadband frequency-entangled photons

Cited by 23 publications

References 30 publications

Two-Photon Fluorescence Microscopy at Extremely Low Excitation Intensity: The Power of Quantum Correlations

Two-Photon Fluorescence Microscopy at Extremely Low Excitation Intensity: The Power of Quantum Correlations

Designing high-power, octave spanning entangled photon sources for quantum spectroscopy

Quantum interferometric two-photon excitation spectroscopy

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