arXiv subjects

Manni He

Publications and source records attributed to Manni He.

5 recordsLinked to original sources

arXiv2023

Experimental Upper Bounds for Resonance-Enhanced Entangled Two-Photon Absorption Cross Section of Indocyanine Green

Resonant intermediate states have been proposed to increase the efficiency of entangled two-photon absorption (ETPA). Although resonance-enhanced ETPA (r-ETPA) has been demonstrated in atomic systems using bright squeezed vacuum, it has not been studied in organic molecules. We investigate for the first time r-ETPA in an organic molecular dye, indocyanine green (ICG), when excited by broadband entangled photons in near-IR. Similar to many reported virtual state mediated ETPA (v-ETPA) measurements, no r-ETPA signals are measured, with an experimental upper bound for the cross section placed at $6 \times 10^{-23}$ cm$^2$/molecule. In addition, the classical resonance-enhanced two-photon absorption (r-TPA) cross section of ICG at 800 nm is measured for the first time to be $20(\pm13)$ GM, suggesting that having a resonant intermediate state does not significantly enhance two-photon processes in ICG. The spectrotemporally resolved emission signatures of ICG excited by entangled photons are also presented to support this conclusion.

quant-ph↗

arXiv2023

Entangled Photon Correlations Allow a Continuous-Wave Laser Diode to Measure Single Photon, Time-Resolved Fluorescence

Fluorescence lifetime experiments are a standard approach for measuring excited state dynamics and local environment effects. Here, we show that entangled photon pairs produced from a continuous-wave (CW) laser diode can replicate pulsed laser experiments without phase modulation. As a proof of principle, picosecond fluorescence lifetimes of indocyanine green are measured in multiple environments. The use of entangled photons has three unique advantages. First, low power CW laser diodes and entangled photon source design lead to straightforward on-chip integration for a direct path to distributable fluorescence lifetime measurements. Second, the entangled pair wavelength is easily tuned by temperature or electric field, allowing a single source to cover octave bandwidths. Third, femtosecond temporal resolutions can be reached without requiring major advances in source technology or external phase modulation. Entangled photons could therefore provide increased accessibility to time-resolved fluorescence while also opening new scientific avenues in photosensitive and inherently quantum systems.

quant-ph↗

arXiv2022

Single Photon Scattering Can Account for the Discrepancies Between Entangled Two-Photon Measurement Techniques

Entangled photon pairs are predicted to linearize and increase the efficiency of two-photon absorption, allowing continuous wave laser diodes to drive ultrafast time-resolved spectroscopy and nonlinear processes. Despite a range of theoretical studies and experimental measurements, inconsistencies persist about the value of the entanglement enhanced interaction cross section. A spectrometer is constructed that can temporally and spectrally characterize the entangled photon state before, during, and after any potential two-photon excitation event. For the molecule Rhodamine 6G, which has a virtual state pathway, any entangled two-photon interaction is found to be equal to or lower than classical, single photon scattering events. This result can account for the discrepancies between the wide variety of entangled two-photon absorption cross sections reported from different measurement techniques. The reported instrumentation can unambiguously separate classical and entangled effects and therefore is of importance for the growing field of nonlinear and multiphoton entangled spectroscopy.

quant-ph↗

arXiv2021

Designing High-Power, Octave Spanning Entangled Photon Sources for Quantum Spectroscopy

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 $\mu$W-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.

physics.optics↗

arXiv2020

Entangled light-matter interactions and spectroscopy

Entangled photons exhibit non-classical light-matter interactions that create new opportunities in materials and molecular science. For example, in entangled two-photon absorption, the intensity-dependence scales linearly as if only one photon was present. The entangled two-photon absorption cross section approaches but does not match the one-photon absorption cross section. The entangled two photon cross section also does not follow classical two photon molecular design motifs. Questions such as these seed the rich but nascent field of entangled light-matter interactions. In this perspective, we use the experimental developments in entangled photon spectroscopy to outline the current status of the field. Now that the fundamental tools are outlined, it is time to start the exploration of how materials, molecules, and devices can control or utilize interactions with entangled photons.

physics.optics↗