Limitations in Fluorescence-Detected Entangled Two-Photon-Absorption Experiments: Exploring the Low- to High-Gain Squeezing Regimes

• URL: http://arxiv.org/abs/2404.16342v1
• Date: Thu, 25 Apr 2024 05:36:47 GMT
• Title: Limitations in Fluorescence-Detected Entangled Two-Photon-Absorption Experiments: Exploring the Low- to High-Gain Squeezing Regimes
• Authors: Tiemo Landes, Brian J. Smith, Michael G. Raymer,
• Abstract summary: We study efforts to enable quantum-enhanced molecular spectroscopy and imaging at ultra-low optical flux. Time-frequency photon entanglement does not provide a practical means to enhance in-solution molecular two-photon fluorescence spectroscopy or imaging.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: We closely replicated and extended a recent experiment ("Spatial properties of entangled two-photon absorption," Phys. Rev. Lett. 129, 183601, 2022) that reportedly observed enhancement of two-photon absorption rates in molecular samples by using time-frequency-entangled photon pairs, and we found that in the low-flux regime, where such enhancement is theoretically predicted in-principle, the two-photon fluorescence signal is below detection threshold using current state-of-the-art methods. The results are important in the context of efforts to enable quantum-enhanced molecular spectroscopy and imaging at ultra-low optical flux. Using an optical parametric down-conversion photon-pair source that can be varied from the low-gain spontaneous regime to the high-gain squeezing regime, we observed two-photon-induced fluorescence in the high-gain regime but in the low-gain regime any fluorescence was below detection threshold. We supplemented the molecular fluorescence experiments with a study of nonlinear-optical sum-frequency generation, for which we are able to observe the low-to-high-gain crossover, thereby verifying our theoretical models and experimental techniques. The observed rates (or lack thereof) in both experiments are consistent with theoretical predictions and with our previous experiments, and indicate that time-frequency photon entanglement does not provide a practical means to enhance in-solution molecular two-photon fluorescence spectroscopy or imaging with current techniques.

Related papers

• Enhancing entangled two-photon absorption of Nile Red via temperature-controlled SPDC [0.0]
  Entangled two-photon absorption can enable a linear scaling of fluorescence emission with the excitation power. Existing theoretical models struggle to accurately predict the entangled-two-photon-absorption behavior of chemically complex dyes.
  arXiv  Detail & Related papers  (2024-06-03T07:49:37Z)
• Solution-phase single-particle spectroscopy for probing multi-polaronic dynamics in quantum emitters at femtosecond resolution [6.722815153728718]
  We develop a solution-phase single-particle pump-probe spectroscopy with photon correlation detection that captures sample-averaged dynamics in single molecules and/or defect states with unprecedented clarity at femtosecond resolution. Our work provides a framework for ultrafast spectroscopy in single emitters, molecules, or defects prone to photoluminescence intermittency and heterogeneity, opening new avenues of extreme-scale characterization and synthetic improvements for quantum information applications.
  arXiv  Detail & Related papers  (2023-04-03T06:14:14Z)
• On-chip quantum information processing with distinguishable photons [55.41644538483948]
  Multi-photon interference is at the heart of photonic quantum technologies. Here, we experimentally demonstrate that detection can be implemented with a temporal resolution sufficient to interfere photons detuned on the scales necessary for cavity-based integrated photon sources. We show how time-resolved detection of non-ideal photons can be used to improve the fidelity of an entangling operation and to mitigate the reduction of computational complexity in boson sampling experiments.
  arXiv  Detail & Related papers  (2022-10-14T18:16:49Z)
• Two-photon emission in detuned resonance fluorescence [0.0]
  We discuss two-photon correlations from the side peaks that are formed when a two-level system emitter is driven coherently. We show that their combination leads to a neat picture compatible with perturbative two-photon scattering. This should help to control, enhance and open new regimes of multiphoton emission.
  arXiv  Detail & Related papers  (2022-10-07T17:59:38Z)
• Quantum-Enhanced Stimulated Brillouin Scattering Spectroscopy and Imaging [15.435543573654524]
  Quantum-enhanced stimulated Brillouin scattering is demonstrated for the first time using low power continuous-wave lasers at 795nm. The proposed new way of utilizing squeezed light for enhanced stimulated Brillouin scattering can be easily adapted for both spectroscopic and imaging applications.
  arXiv  Detail & Related papers  (2021-12-06T04:17:26Z)
• Quantum interferometric two-photon excitation spectroscopy [7.708943730059219]
  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. Results may significantly facilitate the use of quantum interferometric spectroscopy for extracting the information about the electronic structure of the two-photon excited-state manifold of atoms or molecules.
  arXiv  Detail & Related papers  (2021-11-23T15:44:08Z)
• Two-photon resonance fluorescence of two interacting non-identical quantum emitters [77.34726150561087]
  We study a system of two interacting, non-indentical quantum emitters driven by a coherent field. We show that the features imprinted by the two-photon dynamics into the spectrum of resonance fluorescence are particularly sensitive to changes in the distance between emitters. This can be exploited for applications such as superresolution imaging of point-like sources.
  arXiv  Detail & Related papers  (2021-06-04T16:13:01Z)
• Experimental requirements for entangled two-photon spectroscopy [0.0]
  Entangled two-photon spectroscopy is expected to provide advantages compared with classical protocols. We present here an experimental setup that allows the spectral shaping of entangled photons with high resolution.
  arXiv  Detail & Related papers  (2021-03-18T08:28:06Z)
• Optical repumping of resonantly excited quantum emitters in hexagonal boron nitride [52.77024349608834]
  We present an optical co-excitation scheme which uses a weak non-resonant laser to reduce transitions to a dark state and amplify the photoluminescence from quantum emitters in hexagonal boron nitride (hBN) Our results are important for the deployment of atom-like defects in hBN as reliable building blocks for quantum photonic applications.
  arXiv  Detail & Related papers  (2020-09-11T10:15:22Z)
• Setting bounds on two-photon absorption cross-sections in common fluorophores with entangled photon pair excitation [48.7576911714538]
  We use a fluorescence-based registration scheme to experimentally determine upper bounds on the cross-sections for six fluorophores. For two samples that have been studied by others, Rhodamine 6G and 9R-S, we measure upper bounds four and five orders of magnitude lower than the previously reported cross-sections.
  arXiv  Detail & Related papers  (2020-08-06T13:53:16Z)
• Spectrally reconfigurable quantum emitters enabled by optimized fast modulation [42.39394379814941]
  Spectral control in solid state platforms such as color centers, rare earth ions, and quantum dots is attractive for realizing such applications on-chip. We propose the use of frequency-modulated optical transitions for spectral engineering of single photon emission. Our results suggest that frequency modulation is a powerful technique for the generation of new light states with unprecedented control over the spectral and temporal properties of single photons.
  arXiv  Detail & Related papers  (2020-03-27T18:24:35Z)

This list is automatically generated from the titles and abstracts of the papers in this site.

This site does not guarantee the quality of this site (including all information) and is not responsible for any consequences.