Dipole‐like backscatter stimulated Raman scattering for in vivo imaging

Stimulated Raman scattering (SRS) scanning microscopy has the potential to enable label‐free in vivo imaging for research and clinical medicine. Volume SRS from focus occurs in the forward scattered direction. Therefore, multiple scattering events are required to direct the light out of the tissue, reducing imaging depth and resolution. Here, a method called Stokes interference SRS (SISRS) is introduced that operates by the addition to the standard pump and stimulated emission probe beams a third beam called the donut beam. The donut is close in wavelength to the probe beam and, after passage through a π phase plate, forms an annular beam in the focal plane with bright nodes above and below focus. The donut beats with the probe beam, and when they destructively interfere with each other, the microscope's 3‐D stimulated emission focal spot is reduced to subwavelength dimensions. A subwavelength focal volume emits a dipole pattern of SRS with forward and backscatter lobes, enabling high‐resolution single‐backscatter imaging from deep within tissues. The reduction of the focal volume also increases the resolution of the scanning image creating imaging beyond the diffraction limit. SISRS imaging may provide in vivo label‐free Raman images comparable with that achieved in stained in vitro tissues in all planes of section. Copyright © 2014 John Wiley & Sons, Ltd.     

Stimulated Raman hyperspectral imaging based on spectral filtering of broadband fiber laser pulses

We demonstrate a technique of hyperspectral imaging in stimulated Raman scattering (SRS) microscopy using a tunable optical filter, whose transmission wavelength can be varied quickly by a galvanometer mirror. Experimentally, broadband Yb fiber laser pulses are synchronized with picosecond Ti:sapphire pulses, and then spectrally filtered out by the filter. After amplification by fiber amplifiers, we obtain narrowband pulses with a spectral width of <3.3 cm(-1) and a wavelength tunability of >225 cm(-1). By using these pulses, we accomplish SRS imaging of polymer beads with spectral information.     

Influencing factors of external fluorescence seeding enhancing stimulated Raman scattering in liquid‐core optical fiber

This paper reports an external fluorescence seeding technology enhancing the stimulated Raman scattering (SRS) in liquid‐core optical fiber (LCOF). By surrounding a small section of LCOF with a glass capillary and a solution of Rhodamine 6G filled between them to separate fluorescent dye and Raman medium, the initial intensity of SRS is linearly amplified by external fluorescence seeding, and then the SRS of LCOF can be enhanced effectively. Experimental results show that both the concentration of fluorescent dye and the seeding position have an influence on enhancement of SRS. The maximum enhancement of Stokes lines is obtained when the concentration of dye solution is optimized at ~10⁻⁶ mol/l and seeding position is located at the input end. Copyright © 2013 John Wiley & Sons, Ltd.     

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.     

Power limitations in fiber-optic frequency-division multiplexed systems

Abstract

Launch power is limited to the milliwatt level by stimulated Brillouin scattering (SBS) in a single-channel, coherent fiber-optic network. Increasing the number of frequency-division multiplexed channels causes the power limit to decrease quickly to submilliwatt levels due to three-wave intermodulation to keep the signal-to-noise ratio from deteriorating significantly. As the number of channels increases, stimulated Raman scattering (SRS) begins to dominate. If a maximum of 0.5–dB depletion in the highest-frequency channel is allowed, SRS dominates when the number of multiplexed channels reaches about 300. Generally, the launch-power-limiting phenomenon is dependent on the number of channels being multiplexed.     

Control of radiation spatial coherence under synchronous amplification in crystalline LiF:F 2 − amplifier

A technique of spatial coherence control, based on the synchronous amplification of a radiation in LiF crystals with F ₂ ^? color centers, is demonstrated. Spatial radiation distributions of stimulated Raman scattering (SRS) in oxide crystals were investigated under picosecond laser excitation. Low spatial radiation coherence was revealed for both the transient and quasi-stationary SRS. Spatially incoherent SRS was transformed to spatially coherent radiation as a result of phase—locked picosecond synchronous laser pumping of nonlinear Raman and LiF: F ₂ ^? crystals and the Stokes radiation amplification in the color center crystal.     

Higher-Order Effects Induced Optical Solitons in Fiber

In this paper, we study the existence conditions of the soliton solutions induced by considering the higher-order effects such as the third-order dispersion (TOD), self-steepening (SS), and self-frequency shift arising from stimulated Raman scattering (SRS) simultaneously in optical soliton communication. Based on the Jacobian expansion method, we successfully obtain bright and dark solitons. The results shows that the resultant inclusion is in agreement with Mollenauer et al. [Physical Review Letters 45 (1980) 1095] when the SRS is not considered; while when the SRS is considered, the existence conditions of the higher-order effects induced bright and dark solitons are not only quite different from those of the group velocity dispersion (GVD)-induced and self-phase modulation (SPM)-induced solitons, but also different from those of the TOD- and SS-induced solitons discussed by Mollenauer et al. [Physical Review Letters 45 (1980) 1095].     

Low‐noise,vibrational phase‐sensitive chemical imaging by balanced detection RIKE

We perform a back‐to‐back comparison between two nonlinear vibrational imaging techniques: stimulated Raman scattering (SRS) and balanced detection Raman‐induced Kerr effect (BD‐RIKE). Using a compact fiber‐based laser system for generation of pump and Stokes signals, we image polymer beads as well as human hepatocytes under the same experimental conditions. We show that BD‐RIKE, despite the slightly lower signal levels, consistently offers an improved signal‐to‐noise ratio with respect to SRS, resulting in significantly higher image quality. Importantly, we observe that such quality is not affected by the static birefringence of the sample, which makes BD‐RIKE a robust and attractive alternative to SRS. We also highlight a unique advantage of the technique, which is its capability to easily access both the real and imaginary parts of the nonlinear susceptibility, thus allowing for vibrational phase imaging. The phase information can be readily obtained from BD‐RIKE with minimal experimental effort and provides an additional chemical selectivity channel for coherent Raman microscopy. Copyright © 2014 John Wiley & Sons, Ltd.     

Enhanced stimulated Raman scattering in H<Subscript>2</Subscript> by seeding an SRS line into an H-ɛ Balmer line: Amplification-coupled laser wavelength shifter

The stimulated Raman scattering (SRS) in H₂ gas above the dissociation energy limit was recorded using a 266-nm UV laser. All of the observed Stokes and anti-Stokes SRS lines showed a normal behavior except the third Stokes SRS lines at 397.8 nm, which showed a substantial intensity enhancement of about a 36%-conversion efficiency of the pump energy. This enhancement in the SRS line is attributed to the seeding of the SRS line into the Balmer H-? line at 397 nm in molecular hydrogen. To the best of our knowledge, there is no report of any work on enhanced stimulated Raman scattering in H₂ by the seeding of the H-? Balmer line into the SRS line and attaining a very high intensity at the third Stokes SRS lines at 397.8 nm. The cell pressure and the laser pulse energy dependence of these SRS lines substantiate our explanation.     

Nonlinearity in Intensity versus Concentration Dependence for the Deep UV Resonance Raman Spectra of Toluene and Heptane

Abstract: The relation between Raman scattering, resonance Raman scattering, and absorption is reviewed to determine to what extent quantitative analysis can be applied in resonance Raman spectroscopy. In addition, it is demonstrated experimentally that normal Raman spectra can be dramatically inhibited by absorption and resonance Raman effects. Raman spectra of toluene and heptane mixtures—with progressively increasing concentrations of heptane—were measured using 229-nm laser excitation. The results show that the characteristic band intensities are not directly proportional to the relative concentrations of the compounds and deviate due to absorption resonance effects. An approximated mathematical model is developed to demonstrate that the intensities of the normal Raman scattering bands are suppressed. An inhibition coefficient K_i is introduced to describe the situation and determine the penetration depth. Most remarkably, it is shown that the intensity of the resonance Raman scattering bands can be constant even when the concentration ratios differ substantially in the sampled mixtures.     

Effect of crystal orientation on picosecond-laser bulk microstructuring and Raman lasing in diamond

In the paper we report on picosecond-laser bulk microstructuring and stimulated Raman scattering (SRS) in type IIa single-crystal diamond in the course of multipulse irradiation at λ=532 nm wavelength using an advanced ps-laser system equipped with additional setups for on-line video imaging and photoluminescence spectra measurements. The effect of crystal orientation (relative to the incident laser beam) on (i) optical breakdown thresholds, (ii) character of bulk modifications, and (iii) generation of stimulated Raman scattering in diamond during irradiation with picosecond pulses of different durations (τ ₁=10 ps and τ ₂=44 ps) is studied. It is shown that the processes of laser-induced breakdown in the bulk of diamond (at the backside of the crystals) and bulk microstructure growth are governed by the dielectric breakdown mechanism. It is found that generation of high-order stimulated Raman scattering in diamond crystals has a considerable effect on the threshold of laser-induced breakdown and bulk microstructuring. Conditions of the efficient SRS lasing are determined, depending on the pulse duration and the direction ([100] and [110]) of the laser beam incidence. A method of local temperature measurements in the bulk of diamond based on the Stokes-to-anti-Stokes intensity ratio in the recorded SRS spectra is proposed, its applicability to determine a “pre-breakdown” temperature of diamond during multipulse ps-laser irradiation is discussed.     

用激光增益获取弱增益拉曼模式的受激拉曼散射光谱

当酒精的弱增益拉曼模式处于罗丹明640染料分子的激光增益范围时，在由悬垂液滴构成的圆形谐振腔中，观察到乙醇分子C—H伸缩系列模中多个弱增益拉曼模式的受激拉曼散射（SRS）光谱.随着抽运光的增强，迅速增长的强增益拉曼模式的受激辐射抑制了其他弱增益模式的SRS，并导致染料激光的完全淬灭.通过分析圆形腔腔模的光子速率方程和激光染料分子的三能级粒子数速率方程，解释了观察到的实验现象. 关键词： 受激拉曼散射 悬垂液滴 弱拉曼增益模式 激光增益     

Continuous-wave stimulated Raman scattering (cwSRS) microscopy

Stimulated Raman scattering (SRS) microscopy is a powerful tool for chemically sensitive non-invasive optical imaging. However, ultrafast laser sources, which are currently employed, are still expensive and require substantial maintenance to provide temporal overlap and spectral tuning. SRS imaging, which utilizes continuous-wave laser sources, has a major advantage, as it eliminates the cell damage due to exposure to the high-intensity light radiation, while substantially reducing the cost and complexity of the setup. As a proof-of-principle, we demonstrate microscopic imaging of dimethyl sulfoxide using two independent, commonly used lasers, a diode-pumped, intracavity doubled 532-nm laser and a He–Ne laser operating at 632.8-nm.     

Nonlinear optical microscopy: Endogenous signals and exogenous probes

Nonlinear optical microscopy (NLOM) relies on nonlinear light–matter interactions to provide images from larger depths within biological structures compared to conventional confocal fluorescence microscopy. These nonlinear light–matter interactions include multiphoton excitation fluorescence (MPEF), second‐harmonic generation (SHG), coherent anti‐Stokes Raman scattering (CARS), and stimulated Raman scattering (SRS). This review discusses the theories of and instrumentation for various NLOM techniques, with a particular focus on endogenous signals and exogenous probes. These signals and probes expand the breadth of information that optical imaging can provide. We also discuss the application of NLOM in biomedical research, including tissue engineering, drug delivery and clinical diagnostics. Current technological limitations are also discussed.

     

Stimulated supercontinuum-radiation generation of carbon disulfide by all-trans-β-carotene fluorescence enhancement effect in liquid core optical fibre

We demonstrate stimulated supercontinuum-radiation of carbon disulfide (CS₂) influenced by biological molecules all-trans-β -carotene in liquid core optical fibre (LCOF). By virtue of the broad fluorescence characteristics and large third-order optical nonlinearities of all-{trans}-β-carotene,the high-order Stokes lines of stimulated Raman scattering (SRS) and the multi-order Stokes lines of stimulated Brillouin scattering (SBS) excitated by SRS are observed at low input-laser energies. The results indicate that the fluorescence not only enhances the SRS, but also the SBS. These Stokes lines generate the SRS--SBS supercontinuum radiation (RBSR). A flat-amplitude bandwidth of 110 nm from 515nm to 625nm is observed when a frequency-doubled Nd:YAG laser at 532nm with an energy of 0.86mJ is used. This result is expected to be useful for the multi-wavelength fibre laser.     

Polarization resolved stimulated raman scattering: probing depolarization ratios of liquids

Polarization resolved stimulated Raman scattering (SRS) signal is described in the case of isotropic media and linearly polarized incident fields. The model gives simple expressions for the two perpendicularly polarized SRS signals I_X and I_Y, detected along the X and Y directions, respectively, as a function of the incident pump and Stokes polarization angles. We find that Raman depolarization ratio can be simply obtained from the ratio of the SRS intensities detected along the X and Y axis. These theoretical findings are supported by polarization resolved SRS measurements performed on polarized and depolarized bands of cyclohexane. Copyright © 2011 John Wiley & Sons, Ltd.     

Stimulated Raman scattering microscopy for live-cell imaging with high contrast and high sensitivity

We describe the principle and experiment of stimulated Raman scattering (SRS) microscopy, which has various advantages such as high-contrast and high sensitivity. To discuss how these advantages are realized in SRS microscopy, we introduce an intuitive picture of SRS, where the SRS process is viewed as homodyne detection of a nonlinear-optical signal by the excitation pulse.     

Transient stimulated Raman scattering in binary mixed liquids

Stimulated Raman scattering (SRS) spectra in several mixed liquids with a large optical Kerr constant are studied with nanosecond and picosecond light pulses. These spectra show a dependence of the SRS intensity on the relaxation times T₂ of Raman active modes.     

Stimulated Raman scattering and spontaneous Raman solitons in ammonia

In this study we report the first observation of spontaneous Raman solitons in stimulated Raman scattering (SRS) by the gas NH₃. The scattered radiation is called Stokes radiation. Raman solitons are of considerable interest, because their existence can be explained by quantum-mechanical fluctuations of the electromagnetic field in vacuum. We have observed spontaneous Raman solitons in a forward SRS configuration for two different molecular transitions of NH₃, the laser emissions at 58 μm and 72.6 μm wavelength. These are optically pumped by 10 μm CO₂-laser pulses with a duration of 100 ns and an energy of 150 mJ. Spontaneous Raman solitons are short spikes in the pump pulse which occur during its depletion. Their origin is the rapid π phase change of the Stokes seed. In contrast to other laboratories we have used single-pass cells. Thus, we have succeeded in observing multiple spontaneous Raman solitons during one pump pulse. Previous experiments with multi-pass cells never showed multiple solitons. Since multiple spontaneous Raman solitons have already been reported in an earlier experiment with a single-pass cell filled with hydrogen at high pressure, we conclude that such multiple Raman solitons can be observed mainly in this type of gas cell. Subsequently, we have performed statistical measurements on the delay time and the height of the spontaneous Raman solitons in the depleted pump pulse for the 58 μm-NH₃ emission. We have compared these statistics with theory and equivalent experimental results of other laboratories. They are in good agreement with the assumption that quantum-mechanical fluctuations are the origin of spontaneous Raman solitons. The most recent theories postulate that the origin of the formation of spontaneous Raman solitons can be explained by the rapid π phase change of the Stokes seed as well as that of the laser or polarization wave. Therefore, we have determined the phase of the spontaneous Raman solitons relative to the depleted pump pulse. Although, such changes of sign of the relative phase have already been observed in an earlier SRS experiment with hydrogen at high pressure, we did not detect any in our experiment. Therefore, we conclude that in this experiment the π phase change occurs in the Stokes or polarization wave.     

Frequency comb expansion in a monolithic self‐mode‐locked laser concurrent with stimulated Raman scattering

The discovery of a novel phase‐locked frequency comb generated from a monolithic laser with the concurrent processes of self‐mode locking (SML) and stimulated Raman scattering (SRS) is reported. It is experimentally shown that the width of the Raman gain can be exploited to considerably expand the frequency comb of a monolithic SML crystal laser via the SRS process. At a pump power of 6.5 W, an output power of 140 mW in the Stokes wave with a pulse width as narrow as 2.9 ps at a pulse repetition rate of 6.615 GHz is obtained. The present finding not only provides useful insights into the monolithic intracavity SRS process but also paves the way for generating mode‐locked pulses based on monolithic self‐Raman crystals.