Image formation in CARS and SRS: effect of an inhomogeneous nonresonant background medium

We investigate the role of a spatially inhomogenous nonresonant background medium on several Raman-based imaging modalities. In particular, we consider a small resonant bead submerged in a spatially heterogeneous nonresonant χ(3) background. Using detailed 3D electrodynamic simulations, we compare coherent anti-Stokes Raman scattering (CARS), frequency-modulated CARS, amplitude-modulated stimulated Raman scattering (SRS), and frequency-modulated SRS. We find that only FM-SRS is background-free.     

Polarization coherent anti-Stokes Raman scattering microscopy

We report polarization coherent anti-Stokes Raman scattering (P-CARS) microscopy that allows vibrational imaging with high sensitivity and spectral selectivity. The nonresonant background signals from both Raman scatterers and the solvent are efficiently suppressed in P-CARS microscopy. We demonstrate P-CARS imaging of unstained cells based on the contrast of the protein amide I band.     

Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy

Phase-and-polarization coherent control is applied to control the nonlinear response of a quantum system. We use it to obtain high-resolution background-free single-pulse coherent anti-Stokes Raman spectra. The ability to control both the spectral phase and the spectral polarization enables measurement of a specific off-diagonal susceptibility tensor element while exploiting the different spectral response of the resonant Raman signal and the nonresonant background to achieve maximal background suppression.     

Heterodyne coherent anti-Stokes Raman scattering (CARS) imaging

We have achieved rapid nonlinear vibrational imaging free of nonresonant background with heterodyne coherent anti-Stokes Raman scattering (CARS) interferometric microscopy. This technique completely separates the real and imaginary responses of nonlinear susceptibility chi(3) and yields a signal that is linear in the concentration of vibrational modes. We show that heterodyne CARS microscopy permits the detection of weak vibrational resonances that are otherwise overshadowed by the strong interference of the nonresonant background.     

Binary phase shaping for selective single‐beam CARS spectroscopy and imaging of gas‐phase molecules

We report on mode‐selective single‐beam coherent anti‐Stokes Raman scattering spectroscopy of gas‐phase molecules. Binary phase shaping (BPS) is used to produce single‐mode excitation of O₂, N₂, and CO₂ vibrational modes in ambient air and gas‐phase mixtures, with high‐contrast rejection of off‐resonant Raman modes and efficient nonresonant‐background suppression. In particular, we demonstrate independent excitation of CO₂ Fermi dyads at ∼1280 and ∼1380 cm⁻¹ and apply BPS for high‐contrast imaging of CO₂ jet in ambient air. Copyright © 2010 John Wiley & Sons, Ltd.     

Ultrabroadband background-free coherent anti-Stokes Raman scattering microscopy based on a compact Er:fiber laser system

We demonstrate a scheme for efficient coherent anti-Stokes Raman scattering (CARS) microscopy free of nonresonant background. Our method is based on a compact Er:fiber laser source. Impulsive excitation of molecular resonances is achieved by an 11 fs pulse at 1210 nm. Broadband excitation gives access to molecular resonances from 0 cm(-1) up to 4000 cm(-1). Time-delayed narrowband probing at 775 nm enables sensitive and high-speed spectral detection of the CARS signal free of nonresonant background with a resolution of 10 cm(-1).     

Coherent anti-stokes raman scattering spectral interferometry: determination of the real and imaginary components of nonlinear susceptibility chi(3) for vibrational microscopy

We demonstrate coherent anti-Stokes Raman scattering (CARS) heterodyne spectral interferometry for retrieval of the real and imaginary components of the third-order nonlinear susceptibility (chi(3)) of molecular vibrations. Extraction of the imaginary component of chi(3) allows a straightforward reconstruction of the vibrationally resonant signal that is completely free of the electronic nonresonant background and resembles the spontaneous Raman spectrum. Heterodyne detection offers potential for signal amplification and enhanced sensitivity for CARS microscopy.     

Time-resolved coherent anti-Stokes Raman scattering with a femtosecond soliton output of a photonic-crystal fiber

We demonstrate time-resolved coherent anti-Stokes Raman scattering (CARS) by using a frequency-tunable femtosecond soliton output of a silica photonic-crystal fiber (PCF) as a Stokes field. This approach allows quantum beats originating from two close Raman modes to be resolved in the time-domain CARS response. The nonresonant CARS background is efficiently suppressed by introducing a delay time between the probe pulse and the pump-Stokes pulse dyad, suggesting a convenient fiber-optic format for the Stokes source in time-resolved CARS and allowing sensitivity improvement in PCF-based CARS spectroscopes and microscopes.     

Femtosecond pulse-shape modulation at kilohertz rates

We demonstrate a new scanning femtosecond pulse-shaping technique that allows pulse shapes to be modulated at kilohertz rates. This technique is particularly useful for lock-in measurements in which the signal is synchronized with the alternating pulse shapes. The pulse-shape lock-in technique is demonstrated in resonant coherent anti-Stokes Raman scattering, where it is shown to significantly improve the ratio of the resonant signal to both the nonresonant background and to noise.     

Fourier-transform coherent anti-Stokes Raman scattering microscopy

We report a novel Fourier-transform-based implementation of coherent anti-Stokes Raman scattering (CARS) microscopy. The method employs a single femtosecond laser source and a Michelson interferometer to create two pulse replicas that are fed into a scanning multiphoton microscope. By varying the time delay between the pulses, we time-resolve the CARS signal, permitting easy removal of the nonresonant background while providing high resolution, spectrally resolved images of CARS modes over the laser bandwidth (approximately 1500 cm(-1)). We demonstrate the method by imaging polystyrene beads in solvent.     

CARS-Background suppression by phase-controlled nonlinear interferometry

We have developed a new technique for efficient suppression of the nonresonant background in coherent anti-Stokes Raman scattering (CARS). The advantage of this technique, which is based upon phase-controlled superposition of an appropriately selected reference signal, is presented in theory and demonstrated experimentally by the example of the S(3) (pure rotational) transition of molecular hydrogen.     

Interferometric polarization coherent anti-Stokes Raman scattering (IP-CARS) microscopy

We report a novel interferometry-based polarization coherent anti-Stokes Raman scattering (IP-CARS) implementation for effectively suppressing the nonresonant background while significantly amplifying the resonant signal for vibrational imaging. By modulating the phase difference between the two interference CARS signals generated from the same sample and measuring the peak-to-peak intensity of the periodically modulated interference CARS signal, the IP-CARS technique yields a sixfold improvement in the signal-to-background ratio compared with conventional CARS while providing an approximately 20-fold amplification of the resonant CARS signal compared with conventional polarization CARS. We demonstrate this method by imaging 4.69 microm polystyrene beads and unstained human epithelial cells immersed in water.     

Single-pulse phase-contrast nonlinear Raman spectroscopy

High spectral resolution nonlinear vibrational spectroscopy with a single ultrashort pulse is demonstrated on a variety of samples. The spectral data are obtained by shaping the excitation pulse in order to control the relative phase between the weak resonant signal and the strong nonresonant background, in analogy with phase-contrast microscopy techniques. This is unlike the more conventional approach to nonlinear spectroscopy, in which the nonresonant background is reduced to a minimum. By measuring the spectrum of the coherent anti-Stokes Raman signal, it is possible to infer the vibrational energy levels in a band spanning almost an entire octave.     

High-sensitivity vibrational imaging with frequency modulation coherent anti-Stokes Raman scattering (FM CARS) microscopy

We demonstrate a new approach to coherent anti-Stokes Raman scattering (CARS) microscopy that significantly increases the detection sensitivity. CARS signals are generated by collinearly overlapped, tightly focused, and raster scanned pump and Stokes laser beams, whose difference frequency is rapidly modulated. The resulting amplitude modulation of the CARS signal is detected through a lock-in amplifier. This scheme efficiently suppresses the nonresonant background and allows for the detection of far fewer vibrational oscillators than possible through existing CARS microscopy methods.     

Fourier transform spectral interferometric coherent anti-Stokes Raman scattering (FTSI-CARS) spectroscopy

A novel Fourier transform spectral interferometric (FTSI) multiplex coherent anti-Stokes Raman scattering (CARS) technique is developed to extract the vibrational spectrum equivalent to the spontaneous Raman scattering. The conventional FTSI method is modified to use the internal nonresonant CARS signal as a local oscillator to perform spectral interferometry. Utilizing the causality of the coherent vibration (i.e., there should be no signal before the laser excitation), this new FTSI method recovers the entire complex vibrational spectral parameters. We demonstrate this technique with a previously reported single-pulse multiplex CARS method that uses a single phase-controlled broadband ultrafast laser pulse.     

High-spectral-resolution coherent anti-Stokes Raman scattering with interferometrically detected broadband chirped pulses

To achieve high-spectral-resolution multiplex coherent anti-Stokes Raman scattering (CARS), one typically uses a narrowband pump pulse and a broadband Stokes pulse. This is to ensure a correspondence between anti-Stokes and vibrational frequencies. We obtain high-resolution CARS spectra of isopropanol, using a broadband chirped pump pulse and a broadband Stokes pulse, by detecting the anti-Stokes pulse with spectral interferometry. With the temporally resolved anti-Stokes signal, we can remove the chirp of the anti-Stokes pulse and restore high spectral resolution while also rejecting nonresonant scattering.     

Coherent raman spectroscopy

A review of the salient features of five coherent Raman techniques is given, including typical spectra produced by each technique. The resonant and nonresonant signal contributions in the monochromatic plane wave limit are calculated for: (1) Coherent AntiStokes Raman Spectroscopy(CARS); (2) a polarization technique referred to as ASTERISK; (3) Raman-induced Kerr-effect Spectroscopy(RIKES); (4) Optically Heterodyned RIKES (OHD-RIKES); (5) Stimulated Raman Spectroscopy (SRS). The relevant noise contribution to each of these techniques is developed within the framework of a comparative signal-to-noise analysis, and realistic detection limits are discussed. The OHD-RIKES technique is selected as the most viable of the coherent Raman techniques which satisfies the following criteria: (A) suppression of nonresonant background signals and enhanced signal-to-noise ratio; (b) simplicity of operation and interpretation of results. This is the first known application of optical heterodyne detection and optimization to coherent Raman spectroscopy, and the principles developed are generally applicable to all forms of third-order nonlinear spectroscopu.     

基于光强传输方程相位成像的宽场相干反斯托克斯拉曼散射显微背景抑制

相干反斯托克斯拉曼散射(CARS)显微能够对样品的特殊化学组分进行选择性成像,无需荧光标记,在生物医学领域被广泛应用.然而,传统的CARS图像往往存在非共振背景信号.本文将基于光强传输方程的单光束相位成像技术用于CARS显微成像,来抑制CARS的非共振背景信号.该方法通过记录样品在三个相邻平面上的CARS图像,然后利用光强传输方程获取CARS光场的相位分布,最后利用共振CARS信号和非共振背景信号在相位上的差异,实现了对背景噪声的抑制.该方法无需参考光,通过三次测量可完成CARS的背景噪声抑制,具有良好的应用前景.     

Diode-pumped nonresonant continuous-wave Raman laser in H2 with resonant optical feedback stabilization

We demonstrate a nonresonant cw Raman laser pumped by an optically locked diode laser at 790 nm that produces cw Stokes (1178-nm) and coherent anti-Stokes (595-nm) emission. Considering the modest pump powers, relative low cost, and predicted spectral purity, we expect that frequency downconversion of tunable diode lasers through stimulated Raman scattering will provide an attractive source for remote sensing, spectroscopic, and atomic physics applications. The Stokes laser threshold is 240+/-19muW pump power, and emission is observed over a roughly 10-nm range by adjustment of the optical locking feedback phase. Photon-conversion efficiency rises throughout the pump-power region, with a peak value of 15+/-2% .     

Dual-pump coherent anti-Stokes-Raman scattering microscopy

We introduce dual-pump coherent anti-Stokes-Raman scattering (dual-CARS) microscopy. This new technique permits simultaneous imaging of two species characterized by different molecular vibrations, as well as the removal of nonresonant background. This is achieved by using three synchronized laser pulses probing two different vibrations. We demonstrate the virtues of the method by imaging a mixture of nondeuterated and deuterated lipids, clearly distinguishing the individual components and their organization in the mixed arrangement. Further, dual-CARS images of lipid stores in living Caenorhabditis elegans nematodes show that the suppression of the nonresonant background results in significantly enhanced image contrast.