Measurements of Entangled Two-Photon Absorption in Organic Molecules with CW-Pumped Type-I Spontaneous Parametric Down-Conversion

Villabona-Monsalve, Juan P.; Burdick, Ryan K.; Goodson, Theodore

doi:10.1021/acs.jpcc.0c08678

Cited by 41 publications

(46 citation statements)

References 35 publications

(80 reference statements)

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“…Various experiments on ETPA in transmission [7,16,29] and in fluorescence [10,19] configurations have been implemented, these works have reported different values of σ e for different materials, however not considering the linear losses could have produced underestimated values of σ e . In our case, when the linear losses are not taken into account a value of σ e = (1.6978 × 10 −21 ) ± 1.32%[cm 2 /molecule] is obtained while a larger value of σ e = (5.6874 × 10 −21 ) ± 1.37%[cm 2 /molecule] is calculated by eliminating the linear losses, which is in good agreement with reported values [16,18].…”

Section: Variable Pump-power Measurementsmentioning

confidence: 99%

Entangled two-photon absorption detection through a Hong-Ou-Mandel interferometer

Triana-Arango¹,

Ramos‐Ortíz²,

Alarcón³

2022

Preprint

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Recently, different experimental methods to investigate the entangled two-photon absorption (ETPA) process in a variety of materials have been reported. The present work reports on a different approach on which the ETPA process is detected based on the changes induced on the Hong-Ou-Mandel (HOM) interferogram of two photons produced by a spontaneous parametric down conversion (SPDC) Type-II process. Using an organic solution of the laser dye Rhodamine B as a model, it is demonstrated that ETPA at 800nm can be monitored by the changes in the temporalwidth and visibility of the HOM interferogram produced by the photons at a beam splitter after interacting with the sample. Additionally, we present a detail model in which the sample is modeled as a filtering function which fullfills the energy conservation conditions required by ETPA, allowing to explain the experimental observations with excellent agreement. We believe that this work represents a new perspective to study the ETPA process, by using an ultra-sensitive quantum interference technique and a detailed mathematical model of the process.

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Section: Variable Pump-power Measurementsmentioning

confidence: 99%

Entangled two-photon absorption detection through a Hong-Ou-Mandel interferometer

Triana-Arango¹,

Ramos‐Ortíz²,

Alarcón³

2022

Preprint

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“…Comparison of the reported ETPA cross-sections for the same molecular species by different laboratories or even by the same laboratory is difficult, if not impossible, due to several reasons. First, the ETPA cross-section depends on not only the specific electronic transition of a given molecular species but also the properties of the SPDC source. , Accurate characterization of these properties for a given experiment setup is nontrivial and therefore has been left out in most of the reports so far. Second, such a quantification necessitates unambiguous determination of the exclusive contribution from the ETPA process to the observed linear rate dependence with negligible involvement of one-photon losses, precise measurement of the excitation volume, and fluorescence quantum yield for the chosen sample concentration in the case that fluorescence detection is used.…”

Section: Entangled Two-photon Absorption Cross-sectionmentioning

confidence: 99%

Nonlinear Optical Microscopy with Ultralow Quantum Light

Doughty

2021

J. Phys. Chem. A

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Nonlinear optical (NLO) microscopy relies on multiple light−matter interactions to provide unique contrast mechanisms and imaging capabilities that are inaccessible to traditional linear optical imaging approaches, making them versatile tools to understand a wide range of complex systems. However, the strong excitation fields that are necessary to drive higher-order optical processes efficiently are often responsible for photobleaching, photodegradation, and interruption in many systems of interest. This is especially true for imaging living biological samples over prolonged periods of time or in accessing intrinsic dynamics of electronic excited-state processes in spatially heterogeneous materials. This perspective outlines some of the key limitations of two NLO imaging modalities implemented in our lab and highlights the unique potential afforded by the quantum properties of light, especially entangled two-photon absorption based NLO spectroscopy and microscopy. We further review some of the recent exciting advances in this emerging filed and highlight some major challenges facing the realization of quantum-light-enabled NLO imaging modalities.

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“…As a result, two entangled photons leave the same side of a beamsplitter 3 and diffract from a grating at the wavelength of the pump photon [4][5][6] . 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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Measurements of Entangled Two-Photon Absorption in Organic Molecules with CW-Pumped Type-I Spontaneous Parametric Down-Conversion

Cited by 41 publications

References 35 publications

Entangled two-photon absorption detection through a Hong-Ou-Mandel interferometer

Entangled two-photon absorption detection through a Hong-Ou-Mandel interferometer

Nonlinear Optical Microscopy with Ultralow Quantum Light

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

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