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Charles H. Camp Jr.

Publications and source records attributed to Charles H. Camp Jr..

5 recordsLinked to original sources

A Liquid-Core Fiber Platform for Classical and Entangled Two-Photon Absorption Measurements

We introduce a toluene-filled fiber platform for two-photon absorption measurements. By confining both the light and molecular sample inside the 5 $μ$m hollow core of the fiber, we increase the distance over which the nonlinear light-matter interaction occurs. With only a 7.3 nL excitation volume, we measure classical two-photon absorption (C2PA) at an average laser power as low as 1.75 nW, which is a 45-fold improvement over a conventional free-space technique. We use this platform to attempt to measure entangled two-photon absorption (E2PA), a process with a limited regime where the quantum advantage is large. This regime arises due to a crossover from linear to quadratic scaling with photon flux as photon flux is increased. Recently, several teams of researchers have reported that E2PA cross-sections are much smaller than previously claimed. As a result, the linear scaling dominates at photon fluxes so low that it is extremely difficult or impossible to measure using conventional free-space techniques. In this report, we implement the first E2PA measurement using a waveguide. We see no evidence of E2PA, and we set an upper bound on the cross-section consistent with these recent reports.

quant-ph↗

Setting bounds on two-photon absorption cross-sections in common fluorophores with entangled photon pair excitation

Excitation with entangled photon pairs may lead to an increase in the efficiency of two-photon absorption at low photon flux. The corresponding process, entangled two-photon absorption (E2PA), has been investigated in numerous theoretical and experimental studies. However, significant ambiguity and inconsistency remain in the literature about the absolute values of E2PA cross-sections. Here, we use a fluorescence-based registration scheme to experimentally determine upper bounds on the cross-sections for six fluorophores. These bounds are up to four orders of magnitude lower than the smallest published cross-section. 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.

quant-ph↗

Real-time and high-throughput Raman signal extraction and processing in CARS hyperspectral imaging

We present a new collection of processing techniques, collectively "factorized Kramers--Kronig and error correction" (fKK-EC), for (a) Raman signal extraction, (b) denoising, and (c) phase- and scale-error correction in coherent anti-Stokes Raman scattering (CARS) hyperspectral imaging and spectroscopy. These new methods are orders-of-magnitude faster than conventional methods and are capable of real-time performance, owing to the unique core concept: performing all processing on a small basis vector set and using matrix/vector multiplication afterwards for direct and fast transformation of the entire dataset. Experimentally, we demonstrate that a 703026 spectra image of chicken cartilage can be processed in 70 s (approximately 0.1 ms / spectrum), which is approximately 70 times faster than with the conventional workflow (approximately 7.0 ms / spectrum). Additionally, we discuss how this method may be used for machine learning (ML) by re-using the transformed basis vector sets with new data. Using this ML paradigm, the same tissue image was processed (post-training) in approximately 33 s, which is a speed-up of approximately 150 times when compared with the conventional workflow.

eess.SP↗

Quantitative, Comparable Coherent Anti-Stokes Raman Scattering (CARS) Spectroscopy: Correcting Errors in Phase Retrieval

Coherent anti-Stokes Raman scattering (CARS) microspectroscopy has demonstrated significant potential for biological and materials imaging. To date, however, the primary mechanism of disseminating CARS spectroscopic information is through pseudocolor imagery, which explicitly neglects a vast majority of the hyperspectral data. Furthermore, current paradigms in CARS spectral processing do not lend themselves to quantitative sample-to-sample comparability. The primary limitation stems from the need to accurately measure the so-called nonresonant background (NRB) that is used to extract the chemically-sensitive Raman information from the raw spectra. Measurement of the NRB on a pixel-by-pixel basis is a nontrivial task; thus, reference NRB from glass or water are typically utilized, resulting in error between the actual and estimated amplitude and phase. In this manuscript, we present a new methodology for extracting the Raman spectral features that significantly suppresses these errors through phase detrending and scaling. Classic methods of error-correction, such as baseline detrending, are demonstrated to be inaccurate and to simply mask the underlying errors. The theoretical justification is presented by re-developing the theory of phase retrieval via the Kramers-Kronig relation, and we demonstrate that these results are also applicable to maximum entropy method-based phase retrieval. This new error-correction approach is experimentally applied to glycerol spectra and tissue images, demonstrating marked consistency between spectra obtained using different NRB estimates, and between spectra obtained on different instruments. Additionally, in order to facilitate implementation of these approaches, we have made many of the tools described herein available free for download.

physics.optics↗

High-Speed Coherent Raman Fingerprint Imaging of Biological Tissues

We have developed a coherent Raman imaging platform using broadband coherent anti-Stokes Raman scattering (BCARS) that provides an unprecedented combination of speed, sensitivity, and spectral breadth. The system utilizes a unique configuration of laser sources that probes the Raman spectrum over 3,000 cm$^{-1}$ and generates an especially strong response in the typically weak Raman "fingerprint" region through heterodyne amplification of the anti-Stokes photons with a large nonresonant background (NRB) while maintaining high spectral resolution of $<$ 13 cm$^{-1}$. For histology and pathology, this system shows promise in highlighting major tissue components in a non-destructive, label-free manner. We demonstrate high-speed chemical imaging in two- and three-dimensional views of healthy murine liver and pancreas tissues and interfaces between xenograft brain tumors and the surrounding healthy brain matter.

physics.optics↗