D. Gachet, N. Sandeau, H. Rigneault
We propose a full-vectorial numerical study of far field radiation patterns in coherent anti-Stokes Raman scattering (CARS) microscopy. We emphasis the particular role of the Raman depolarisation ratio of the observed medium and show how it modifies the radiation pattern of thin objects.
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Far field radiation pattern under tight focusing condition is investigated in Coherent Anti-stokes Raman Scattering (CARS) microscopy both in the forward (F-CARS) and backward (E-CARS) directions. While we assume no refraction index mismatch between the sample and the environing medium, our rigorous numerical electromagnetic computation takes into account the exact polarizations of the excitation laser beams and of the induced nonlinear dipoles. F-CARS and E-CARS radiation patterns, as well as their divergence, are studied as a function of the size of the sample object and compared to the exci…
The noise figure and photon probability distribution are calculated for coherent anti-Stokes Raman scattering (CARS) where an anti-Stokes signal is converted to Stokes. We find that the minimum noise figure is ~ 3dB.
Coherent Anti Stokes Raman Scattering (CARS) offers many advantages for nonlinear bio-imaging, thanks to its sub-cellular spatial resolution and unique chemical specificity. Its working principle requires two incident pulsed laser beams with distinct frequencies to be focused in space and time, which focus quality however rapidly deteriorates when propagating at large depths in biological tissues. The depth limits of CARS and the capability of wavefront correction to overcome these limits are currently unknown. In this work we exploit the spectral correlation properties of the transmission mat…
We apply coherent anti-Stokes Raman Scattering (CARS) microscopy to characterize director structures in liquid crystals.
We theoretically investigate a scheme in which backward coherent anti-Stokes Raman scattering (CARS) is significantly enhanced by using slow light. Specifically, we reduce the group velocity of the Stokes excitation pulse by introducing a coupling laser that causes electromagnetically induced transparency (EIT). When the Stokes pulse has a spatial length shorter than the CARS wavelength, the backward CARS emission is significantly enhanced. We also investigated the possibility of applying this scheme as a CARS lidar with O2 or N2 as the EIT medium. We found that if nanosecond laser with large …
Coherent Raman scattering (CRS) spectroscopy techniques have been widely developed and optimized for different applications in biomedicine and fundamental science. The most utilized CRS technique has been coherent anti-Stokes Raman scattering (CARS), and more recently, stimulated Raman scattering (SRS). Coherent Stokes Raman scattering (CSRS) has been largely ignored mainly because it is often strongly affected by fluorescence, particularly for resonance enhanced measurements. However, in the cases of resonant excitation the information contained in the CSRS signal can be different and complem…
We show that the increasingly popular nonlinear optical technique of time-domain coherent anti-Stokes Raman scattering (CARS), which is usually understood in terms of the semiclassical time-dependent third-order polarization, can be equally explained in terms of the time-delayed version of the Yuratich equation so popular in traditional frequency-domain CARS. The method brings out the strong dependence of CARS time traces and time-delayed CARS lineshapes on the spectral envelope of the probe laser electric field. Examples are analytically shown for experimental results that are otherwise treat…
Micromolar chemical imaging by high-energy low-photodamage Coherent Anti-stokes Raman Scattering (HELP-CARS)
HELP-CARS通过高能低损伤技术实现微摩尔级生物化学成像，提升灵敏度和成像精度。
We propose an elegant scheme towards phase locking of two independent degenerate coherent anti-Stokes Raman scattering (CARS) processes. The optical implementation involves a modified Mach-Zehnder interferometer that is utilized to transfer phase coherence from three totally uncorrelated laser beams into two degenerate CARS beams which are independently produced in two distinct Raman active samples. Such a phase-transport interferometer allows for explicit measurement and control of phase differences between the two phase-locked degenerate CARS processes, hence may lead to applications in othe…
Removing distortions in coherent anti-Stokes Raman scattering (CARS) spectra due to interference with the nonresonant background (NRB) is vital for quantitative analysis. Popular computational approaches, the Kramers-Kronig relation and the maximum entropy method, have demonstrated success but may generate significant errors due to peaks that extend in any part beyond the recording window. In this work, we present a learned matrix approach to the discrete Hilbert transform that is easy to implement, fast, and dramatically improves accuracy of Raman retrieval using the Kramers-Kronig approach.
We report stimulated Raman spectroscopy of the G phonon in both single and multi-layer graphene, through Coherent anti-Stokes Raman Scattering (CARS). The signal generated by the third order nonlinearity is dominated by a vibrationally non-resonant background (NVRB), which obscures the Raman lineshape. We demonstrate that the vibrationally resonant CARS peak can be measured by reducing the temporal overlap of the laser excitation pulses, suppressing the NVRB. We model the observed spectra, taking into account the electronically resonant nature of both CARS and NVRB. We show that CARS can be us…
A new interferometric technique is demonstrated for measuring Coherent Anti-Stokes Raman Scattering (CARS) signals. Two forward-directed CARS signals are generated, one in each arm of an interferometer. The deterministic nature of the CARS process allows for these two signals, when spatially and temporally overlapped, to interfere with one another. Heterodyne detection can therefore be employed to increase the sensitivity in CARS signal detection. In addition, nonlinear CARS interferometry will facilitate the use of this spectroscopic technique for molecular contrast in Optical Coherence Tomog…
Surface-enhanced coherent anti-Stokes Raman scattering (SE-CARS) takes advantage of surface plasmon resonances supported on metallic nanostructures to amplify the coherent Raman response of target molecules. While these metallic antennas have found significant success in SE-CARS studies, photo-induced morphological changes to the nanoantenna under ultrafast excitation introduce significant hurdles in terms of stability and reproducilibty. These hurdles need to be overcome in order to establish SE-CARS as a reliable tool for rapid biomolecular sensing. Here we address this challenge by performi…
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 chemi…
We propose to use frequency-selective quasi parity-time symmetry to reduce the heat generated by coherent anti-Stokes Raman scattering (CARS) reversed cycles in active Raman media with phase mismatch. This is accomplished using a coupled-waveguide structure, which includes the active Raman waveguide (RW), where the Stokes signal undergoes amplification via stimulated Stokes Raman scattering (SSRS), and a dissipative waveguide (DW), which is tuned to the anti-Stokes wavelength so as to evacuate the corresponding anti-Stokes photons from the RW by coupling. The DW introduces optical loss that pa…
We propose an all-fiber-generated dual-soliton pulses based scheme for the background-free detection of coherent anti-Stokes Raman spectroscopy under the spectral focusing mechanism. Due to the strong birefringence and high nonlinearity of a polarization-maintaining photonic crystal fiber (PM-PCF), two redshifted soliton pulses can be simultaneously generated relying on high-order dispersion and nonlinear effects along two eigenpolarization axes in the anomalous dispersion regime, while allowing feasible tunability of the frequency distance and temporal interval between them. This proposed sch…
We demonstrate the use of hybrid rotational femtosecond/picosecond (fs/ps) coherent anti-Stokes Raman spectroscopy (HR-CARS) as a technique for temperature measurements in nitrogen gas at high pressures and temperatures. A broadband pulse shaper-adjusted 42 fs pulse interacts with a narrow-bandwidth, frequency-upconverted 5.5 ps pulse in a cell containing nitrogen at pressures of 1-70 atm and temperatures of 300-1000 K. A computational code is used to model spectra and fit experimental results to obtain best-fit temperatures. We demonstrate good qualitative fits as well as good accuracy and pr…
Airborne contaminants, e.g., bacterial spores, are usually analyzed by time consuming microscopic, chemical and biological assays. Current research into real time laser spectroscopic detectors of such contaminants is based on e.g. resonant Raman spectroscopy. The present approach derives from recent experiments in which atoms and molecules are prepared by one (or more) coherent laser(s) and probed by another set of lasers. The connection with previous studies based on "Coherent Anti-Stokes Raman Spectroscopy" (CARS) is to be noted. However generating and utilizing maximally coherent oscillatio…
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 th…
Single-shot time resolved Coherent Anti-Stokes Raman Scattering (CARS) is presented as a viable method for fast measurements of molecular spectra. The method is based on the short spatial extension of femtosecond pulses and maps time delays between pulses onto the region of intersection between broad beams. The image of the emitted CARS signal contains full temporal information on the field-free molecular dynamics, from which spectral information is extracted. The method is demonstrated on liquid samples of CHBr3 and CHCl3 and the Raman spectrum of the low-lying vibrational states of these mol…
Coherent anti-Stokes Raman scattering (CARS) and, in particular, femtosecond adaptive spectroscopic techniques (FAST CARS) have been successfully used for molecular spectroscopy and microscopic imaging. Recent progress in ultrafast nanooptics provides flexibility in generation and control of optical near fields, and holds promise to extend CARS techniques to the nanoscale. In this theoretical study, we demonstrate ultrafast subwavelentgh control of coherent Raman spectra of molecules in the vicinity of a plasmonic nanostructure excited by ultrashort laser pulses. The simulated nanostructure de…
Thousand foci coherent anti-Stokes Raman scattering microscopy
本文利用高重复频率放大振荡器和光学参量放大器实现了1089个焦点的CARS显微技术，通过相机多通道探测分离信号，实现了0.3Hz的百万像素成像，并有望通过更快的相机实现超过100Hz的帧率。
Phonon dephasing times determined with time-delayed, broadband CARS
本文提出基于时间延迟宽带CARS的方法，可同时测量全声子谱的退相时间，并在金刚石、KTP和KTA晶体上验证，测得金刚石sp3峰退相时间为7.81 ps。
Since its first demonstration in the sixties, coherent anti-Stokes Raman scattering (CARS) has become a powerful spectroscopic sensing tool with broad applications in biology and chemistry. However, it is a complex nonlinear optical process that often leads to the lacks of quantitative data outputs. In this letter, we observe how CARS signal builds up gradually and demonstrate how to control its deferral with laser-pulse shaping. A time-resolved three-color CARS that involves a pair of driving broadband femtosecond pulses and delayed shaped probe pulse is realized experimentally. Driving pulse…
Ultra-high-speed coherent anti-Stokes Raman spectroscopy with a hybrid dual-comb source
本文提出一种混合双光梳CARS系统，结合宽带光纤激光器与灵活电光频率梳，在1 MHz刷新率下实现2800–3200 cm⁻¹光谱测量，速度比现有系统高一个数量级，并演示了液体混合物的快速光谱成像。
We study coherent anti-Stokes Raman spectroscopy in air-filled anti-resonance hollow-core photonic crystal fiber, otherwise known as 'revolver' fiber. We compare the vibrational coherent anti-Stokes Raman signal of N$_2$, at 2331 cm$^{-1}$, generated in ambient air (no fiber present), with the one generated in a 2.96 cm of a revolver fiber. We show a 170 times enhancement for the signal produced in the fiber, due to an increased interaction path. Remarkably, the N$_2$ signal obtained in the revolver fiber shows near-zero non-resonant background, due to near-zero overlap between the laser field…
We demonstrate a single-beam, standoff (>10m) coherent anti-Stokes Raman scattering spectroscopy (CARS) of various materials, including trace amounts of explosives and nitrate samples, under ambient light conditions. The multiplex measurement of characteristic molecular vibrations with <20cm-1 spectral resolution is carried out using a single broadband (>550cm-1) phase-shaped femtosecond laser pulse. We exploit the strong nonresonant background signal for amplification of the weak backscattered resonant CARS signal by using a homodyne detection scheme. This facilitates a simple, highly sensiti…
Frequency modulation coherent anti-Stokes Raman scattering (FM CARS) is presented, using a compact as well as fast and widely tunable fiber-based light source. With this light source Raman resonances between 700 cm$^{-1}$ and 3200 cm$^{-1}$ can be addressed via wavelength tuning within only 5 ms, which allows for FM CARS measurements with frame-to-frame wavelength switching. Moreover, the functionality for high-sensitivity FM CARS measurements was integrated by means of fiber optics to keep a stable and reliable operation. The light source accomplished FM CARS measurements with a 40 times enha…
Investigating the effect of non-resonant background variation on the CARS data analysis and classification
本研究系统考察非共振背景变化对CARS拉曼信号提取的影响，利用真实数据模拟并对比MEM、KK、CNN和LSTM四种方法，发现高背景强度下MEM和KK更优，且归一化与背景去除对不同方法的表现和分类准确率有不同影响。
Phase-resolved wide-field CARS microscopy with speckle illumination
本文提出一种结合高功率OPA、散斑照明和QLSI的相位分辨宽场高光谱CARS显微镜，抑制非共振背景，实现大视场快速成像，并用于微塑料和肝脏脂肪变性成像。
Coherent Anti-Stokes Raman Scattering (CARS) processes are ``coherent,'' but the phase of the anti-Stokes radiation is usually lost by most incoherent spectroscopic CARS measurements. We propose a novel Raman microscopy imaging method called Nonlinear Interferometric Vibrational Imaging, which measures Raman spectra by obtaining the temporal anti-Stokes signal through nonlinear interferometry. With a more complete knowledge of the anti-Stokes signal, we show through simulations that a high-resolution Raman spectrum can be obtained of a molecule in a single pulse using broadband radiation. This…
Broadband coherent Raman spectroscopy based on single-pulse spectral-domain ghost imaging
本文提出将非线性光谱鬼成像与时间拉伸色散傅里叶变换光谱相结合，利用随机超连续谱和单像素探测器实现微秒级、13 cm⁻¹分辨率的宽带CARS光谱重建。
We present an improvement on the signal-to-background of single-beam coherent anti-Stokes Raman scattering (SB-CARS) spectroscopy measurements for systems employing ultrafast supercontinuum sources based on all-normal dispersion photonic crystal fibers. Improvements to the signal-to-background arise in the use of a new pulse-reconstruction algorithm based on temporal ptychography, I$^2$PIE. A simple SB-CARS strategy is used to measure the spectrum of para-xylene, where the supercontinuum pulses used are compressed using multiphoton intrapulse interference phase scan (MIIPS) and, for the first …
We introduce new lineshapes of coherent anti-Stokes Raman spectra of gases by considering realistic nanosecond laser pulses that deviate from the Gaussian representations of their time and spectral envelopes. The analysis suggests that the contribution to the linewidth caused by the interaction with such laser pulses could be erroneously attributed to the intrinsic Raman width if the customary CARS approach, based primarily on the Voigt lineshape, is assumed.
We demonstrate three-dimensional vibrational imaging of director structures in liquid crystals using coherent anti-Stokes Raman scattering (CARS) polarized microscopy. Spatial mapping of the structures is based on sensitivity of a polarized CARS signal to orientation of anisotropic molecules in liquid crystals. As an example, we study structures in a smectic material and demonstrate that single-scan CARS and two-photon fluorescence images of molecular orientation patterns are consistent with each other and with the structure model.
A major impediment of using Coherent Anti-Stokes Raman Scattering to identify biological molecules is that the illumination levels required to produce a measurable signal often also produce significant nonresonant background from the medium, especially from water, that is not specific to the resonance being investigated. We present a method of using nonlinear interferometry to measure the temporal shape of the anti-Stokes signal to differentiate which components are resonant and nonresonant. This method is easily adaptable to most existing pulsed CARS illumination methods and should allow for …
Raman spectroscopy is one of the key techniques in the study of vibrational modes and molecular structures. In Coherent Anti-Stokes Raman Scattering (CARS) spectroscopy, a molecular vibrational spectrum is resolved via the third-order nonlinear interaction of pump, Stokes and probe photons, typically using a complex experimental setup with multiple beams and laser sources. Although CARS has become a widespread technique for label-free chemical imaging and detection of contaminants, its multi-source, multi-beam experimental implementation is challenging. In this work we present a simple and eas…
We have developed an interferometric implementation of coherent anti-Stokes Raman scattering (CARS) which enables broadband coherent Raman spectroscopy free from non-resonant background (NRB), with a signal strength proportional to concentration. Spectra encode mode symmetry information into the amplitude response which can be directly compared to polarised spontaneous Raman spectra. The method requires only passive polarisation optics and is suitable for a wide range of laser linewidths and pulse durations
We present a theoretical investigation of coherent anti-Stokes Raman scattering (CARS) that is modulated by periodically depleting the ground state population through Rabi oscillations driven by an additional control laser. We find that such a process generates optical sidebands in the CARS spectrum and that the frequency of the sidebands depends on the intensity of the control laser light field. We show that analyzing the sideband frequency upon scanning the beams across the sample allows one to spatially resolve emitter positions where a spatial resolution of 65 nm, which is well below the d…
Super-resolved CARS by coherent image scanning
本文提出将相位分辨图像扫描显微与CARS结合，通过内联干涉测量解析复场，实现最高两倍分辨率提升，方法简单且兼容传统正向探测CARS装置。
We propose a new technique for comparing two Raman active samples. The method employs optical interference of the signals generated via coherent anti-Stokes Raman scattering (CARS) of broadband laser pulses with noisy spectra. It does not require spectrally resolved detection, and no prior knowledge about either the Raman spectrum of the samples, or the spectrum of the incident light is needed. We study the proposed method theoretically, and demonstrate it in a proof-of-principle experiment on Toluene and ortho-Xylene samples.
We present a simple method and its experimental implementation to completely determine the characteristics of the pump-and-probe pulse and the Stokes pulse in a coherent anti-Stokes Raman scattering microscope at sample level without additional autocorrelators. Our approach exploits the delay line, ubiquitous in such microscopes, to perform a convolution of the pump-and-probe and Stokes pulses as a function of their relative delay and it is based on the detection of the photons emitted from an appropriate non-linear sample. The analysis of the non-resonant four-wave-mixing and sum-frequency-ge…
We present a multimodal non-linear optical (NLO) laser-scanning microscope, based on a compact fiber-format excitation laser and integrating coherent anti-Stokes Raman scattering (CARS), stimulated Raman scattering (SRS) and two-photon-excitation fluorescence (TPEF) on a single platform. We demonstrate its capabilities in simultaneously acquiring CARS and SRS images of a blend of 6-μm poly(methyl methacrylate) beads and 3-μm polystyrene beads. We then apply it to visualize cell walls and chloroplast of an unprocessed fresh leaf of Elodea aquatic plant via SRS and TPEF modalities, respectively.…
Nonlinear optical methods, such as coherent anti-Stokes Raman scattering (CARS) and stimulated Raman scattering (SRS), are able to perform label free imaging, with chemical bonds specificity. Here, we demonstrate that the use of circularly polarized light allows to retrieve not only the chemical nature but also the symmetry of the probed sample, in a single shot measurement. Our symmetry-resolved scheme offers simple access to the local organization of vibrational bonds and as a result provides enhanced image contrast for anisotropic samples as well as an improved chemical selectivity. We quan…
Exploitation of the nonresonant background of Multiplex-Coherent anti-Stokes Raman Scattering for label-free discrimination of proteins
提出基于M-CARS评估共振与非共振贡献对比度的方法，在肌肉组织中无标记区分肌动蛋白与肌球蛋白丝，为生物显微学无标记成像提供新途径。
Doppler dual-comb coherent Raman spectromicroscopy
利用多普勒双梳技术实现相干拉曼光谱显微镜，通过非线性相位调制实现宽谱带宽和高分辨率成像，具有高灵敏度和快速成像能力。
We demonstrate single-beam coherent anti-Stokes Raman spectroscopy (CARS), for detecting and identifying traces of solids, including minute amounts of explosives, from a standoff distance (>50 m) using intense femtosecond pulses. Until now, single-beam CARS methods relied on pulse-shapers in order to obtain vibrational spectra. Here we present a simple and easy-to-implement detection scheme, using a commercially available notch filter, that does not require the use of a pulse-shaper.
Statistical estimation theory detection limits for label-free imaging
本文构建统计估计理论统一框架，利用 Fisher 信息与 CRLB 量化多种无标记显微模态的信号检测与参数估计极限。
Coherent Raman microscopy provide label-free imaging by interrogating the intrinsic vibration of biomolecules. Nevertheless, trade-off between high chemical-specificity and high imaging-speed currently exists in transition from spectroscopy to spectroscopic imaging when capturing dynamics in complex living systems. Here, we present a novel concept in dual-comb scheme to substantially beat this trade-off and facilitate high-resolution broadband coherent anti-Stokes Raman spectroscopic imaging based on down-converted, automatically varying delay-time in spectral focusing excitation. A rapid meas…
We present a new interferometric technique for measuring Coherent Anti-Stokes Raman Scattering (CARS) and Second Harmonic Generation (SHG) signals. Heterodyne detection is employed to increase the sensitivity in both CARS and SHG signal detection, which can also be extended to different coherent processes. The exploitation of the mentioned optical nonlinearities for molecular contrast enhancement in Optical Coherence Tomography (OCT) is presented. Numerical simulations for both coherent nonlinear processes are performed in order to determine the properties of the signal expected at the exit of…
Concatenation of Kerr solitary waves in Ceramic YAG: application to coherent Raman imaging
本文研究陶瓷 YAG 中多个 Townes 孤子相干级联形成宽带光丝的机制，并通过模拟与实验分析峰值功率对成丝位置和超连续谱的影响，以支持无延迟线、高灵敏度的自参考复用 CARS 成像。
We demonstrate coherent anti-Stokes Raman scattering (CARS) microscopy in a wide-field setup with nanosecond laser pulse excitation. In contrast to confocal setups, the image of a sample can be recorded with a single pair of excitation pulses. For this purpose the excitation geometry is specially designed in order to satisfy the phase matching condition over the whole sample area. The spectral, temporal and spatial sensitivity of the method is demonstrated by imaging test samples, i.e. oil vesicles in sunflower seeds, on a nanosecond timescale. The method provides snapshot imaging in 3 nanosec…
Optical spectroscopy and imaging of microscopic samples have opened up a wide range of applications throughout the physical, chemical, and biological sciences. High chemical specificity may be achieved by directly interrogating the fundamental or low-lying vibrational energy levels of the compound molecules. Amongst the available prevailing label-free techniques, coherent Raman scattering has the distinguishing features of high spatial resolution down to 200 nm and three-dimensional sectioning. However, combining fast imaging speed and identification of multiple - and possibly unexpected- comp…
Given the long subclinical stage of Alzheimer's disease (AD), the study of biomarkers is relevant both for early diagnosis and the fundamental understanding of the pathophysiology of AD. Biomarkers provided by amyloid-${\unicode[Times]{x3B2}}$ (A${\unicode[Times]{x3B2}}$) plaques have led to an increasing interest in characterizing this hallmark of AD due to its promising potential. In this work, we characterize A${\unicode[Times]{x3B2}}$ plaques by label-free multimodal imaging: we combine two-photon excitation autofluorescence (TPEA), second harmonic generation (SHG), spontaneous Raman scatt…
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