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.     

Backscatter reduction using combined spatial, temporal, and polarization beam smoothing in a long-scale-length laser plasma

Spatial, temporal, and polarization smoothing schemes are combined for the first time to reduce to a few percent the total stimulated backscatter of a NIF-like probe laser beam (2x10(15) W/cm (2), 351 nm, f/8) in a long-scale-length laser plasma. Combining temporal and polarization smoothing reduces simulated Brillouin scattering and simulated Raman scattering (SRS) up to an order of magnitude although neither smoothing scheme by itself is uniformly effective. The results agree with trends observed in simulations performed with the laser-plasma interaction code F3D simulations [R. L. Berger et al., Phys. Plasma 6, 1043 (1999)].     

超短超强激光与气体靶相互作用中的背向受激Raman散射

 实验诊断测量了超短超强激光与气体靶相互作用产生的背向受激Raman散射,在实验条件下呈现强耦合模式,背向受激Raman散射出现非线性Stokes多峰伴线结构,峰值的频率间隔小于等离子体波的频率,可以大致地推断出激光打靶过程中产生的等离子体密度偏低,其结果与等离子体强耦合理论计算结果一致。     

驱动激光束间相干性以及对背向散射影响的研究

早期的研究表明, 束匀滑技术能够有效地抑制高功率激光与等离子体相互作用中产生的各种参量不稳定性, 大大减少受激布里渊散射和受激拉曼散射. 但在NIF最近的实验研究中发现, 受激布里渊散射和受激拉曼散射份额远远高于预期, 原因可能与驱动激光束间的相干性有关. 本文利用"神光II"装置两路倍频纳秒激光辐照金平面靶, 研究了小口径取样情况下两者背向散射的能量和光谱在不同驱动激光相干条件下的变化情况. 初步结果表明, 激光束间存在着较强的相干性, 并且随着束间相干程度的增加, 背向散射也逐渐增强.     

Phase conjugated wavefronts by stimulated brillouin and Raman scattering

Experimental investigations were made of wavefront reproduction (WFR) by backward stimulated Raman scattering (SRS) and backward stimulated Brillouin scattering (SBS) in CS₂ with a linearly polarized ruby pump beam. The experimental studies were carried out as a function of the optical waveguide diameter and photographic records comparing the pump beam with the backscattered SBS and SRS beams are presented. In all of the cases studied there was a high degree of replication between the SBS and pump beams; however, a deterioration in the quality of the replicated SRS beam was observed, and it increased as the cross-sectional area of the waveguide increased.     

Raman Microscopy and Associated Techniques for Label-Free Imaging of Cancer Tissue

Abstract

Raman spectroscopy can identify cancerous from healthy tissue, with a chemical analysis from the measurement of vibrational bond frequencies. However, to detect small tumors a form of Raman imaging is required. Such imaging—by acquiring a Raman spectrum at each imaging pixel—can detect tumors but is rather slow. Multiphoton versions of Raman—anti-Stokes Raman scattering (CARS) microscopy and stimulated Raman scattering (SRS) microscopy—offer similar accuracies in identifying cancerous tissue and tumor margins but with a far higher speed, which is beneficial for diagnosis of small tumors in tissue. SRS microscopy can also be used to image extrinsic molecules in living cells, such as anti-cancer drugs at typical concentrations.     

Pump spectral linewidth influence on stimulated Brillouin scattering (SBS) and stimulated Raman scattering (SRS) and self‐termination behavior of SRS in liquids

The threshold, temporal behavior, and conversion efficiency of stimulated Brillouin scattering (SBS) and stimulated Raman scattering (SBS) in three liquids (benzene, hexane, and dimethyl sulfoxide) and two crystals (calcite and barium nitrate) have been investigated under three largely different spectral linewidth conditions. Pumped with 532‐nm and nanosecond duration laser pulses of ≤ 0.01 cm^?1 linewidth, only SBS can be generated in all tested liquids with a high nonlinear reflectivity. However when the pump spectral linewidth is ～0.07 cm^?1 or ～0.8 cm^?1, both SBS and SRS can be observed in benzene while only SRS can be generated in dimethyl sulfoxide; in all these cases SRS is the dominant contribution to the stimulated scattering but the efficiency values are drastically decreased due to the self‐termination behavior of SRS in liquids, which arises from the thermal self‐defocusing of both pump beam and SRS beam owing to Stokes‐shift related opto‐heating effect. In contrast, for SRS process in the two crystals, the thermal self‐defocusing influence is negligible benefitting from their much greater thermal conductivity, and a higher conversion efficiency of SRS generation can be retained under all three pump conditions.

     

Disturbing interference patterns in femtosecond stimulated Raman microscopy

Femtosecond stimulated Raman microscopy (FSRM) is an upcoming technique in nonlinear microscopy which facilitates rapid chemical mapping. It employs femtosecond white‐light pulses as probe pulses and intense picosecond pulses as pump pulses. Stimulated Raman scattering (SRS) occurs at the focus of a scanning microscope. Chemical constituents in the sample are identified via their Raman signatures. In this article, disturbing interference patterns in FSRM are reported. They are caused by a broadening of the pump pulse due to nonlinear interactions in the focal region of the microscope and reduce the signal‐to‐noise ratio. The properties of these modulations are explored, and the methods to suppress them are presented. Copyright © 2009 John Wiley & Sons, Ltd.     

Subwavelength-resolution near-field Raman spectroscopy

The resolution capabilities of near-field Raman spectroscopy based on a giant enhancement of the electric field near a nanosized metal probe are studied. As a test sample, bundles of single-walled carbon nanotubes deposited on glass substrates are used. It is shown that this method ensures a subwavelength spatial resolution of about 50 nm and demonstrates a Raman scattering enhancement of the order of 10⁴.     

神光Ⅲ原型装置的黑腔靶背向散射光测量技术

在惯性约束聚变研究中,为研究激光等离子体互作用产生的受激布里渊与受激拉曼散射光(SRS),基于神光Ⅲ原型装置利用新的背向散射诊断系统对真空黑腔靶与充气黑腔靶以及有无束匀滑效果情况下的散射光光谱进行了测量。实验发现,在相同条件下,充气黑腔靶SRS散射光比真空黑腔靶大,在终端光学组件中使用束匀滑效果后也能降低散射光。诊断系统记录的散射光强度及光谱的时间变化过程对研究激光等离子体相互作用提供了重要的数据支撑。     

Continuous wave stimulated Raman scattering of benzene by fluorescence enhancement in hollow fused silica fiber

We present continuous wave stimulated Raman scattering (SRS) of benzene (C₆H₆) influenced by the fluorescent dye m‐cresol purple in a hollow fused silica fiber (HFSF). Because of the transmission loss of the HFSF filled with C₆H₆, the SRS occurs when the Stokes gain equals the transmission loss, with the loss taken at the Stokes wavelength. The 992 cm⁻¹ stimulated Stokes line has been obtained at the pump wavelength 658 nm, which cannot be obtained at 532 nm because the Stokes wavelength (562 nm) does not locate in the transmission loss. Also, the pump power is 35 mW with m‐cresol purple which is much lower than 800 mW without the dye. The profile of the 992 cm⁻¹ stimulated Stokes is changed, and the weak shoulders of the profile are amplified by fluorescence. These results are expected to be of relevance in applications on the tunable Raman laser at new wavelengths. Copyright © 2011 John Wiley & Sons, Ltd.     

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.     

Detection of a new SRS‐promoting phonon mode and cross‐cascaded χ(3)‐nonlinear lasing in single crystals of calcite (trigonal CaCO3)

For calcite (CaCO₃), one of the pioneer crystals in nonlinear optics, new results of stimulated Raman scattering (SRS) spectroscopy are presented. Among them are the discovery of a new SRS‐promoting vibration mode with ω_SRS2 ≈︁ 282 cm^‐1 and its participation, together with the main SRS mode ω_SRS1 ≈︁ 1086.5 cm^‐1, in cross‐cascaded (χ⁽³⁾ ↔ χ⁽³⁾) nonlinear‐lasing generation, as well as the observation of efficient self‐upconversion via cascaded parametric four‐wave processes of one‐micron Stokes and anti‐Stokes χ⁽³⁾‐lasing into the UV‐region of third harmonic generation. The investigations show that calcite is able to generate a χ⁽³⁾‐lasing comb of more than two octaves bandwidth. The article also gives a brief review on the discovery and study of the SRS‐effect in natural crystals (minerals), which have expanded our ability to study the photon‐phonon nonlinear‐laser interactions in crystalline materials. A short summary of information about χ⁽³⁾‐lasing properties of the triangular planar structure units in SRS‐active crystals is included.     

Applying the method of Coherent Anti‐stokes Raman microscopy for imaging of carotenoids in microalgae and cyanobacteria

Coherent anti‐stokes Raman scattering microscopy (CARS) was applied to visualize carotenoids in microalgae and cyanobacteria. Nonlinear light–matter interaction utilized in CARS microscopy inevitably induces a number of competing nonlinear processes, such as multiphoton excitation fluorescence. Microalgae and cyanobacteria being an intrinsically well‐fluorescent object generates a strong two‐photon‐excitation fluorescence (TPEF) signal which should be effectively suppressed during the CARS experiment. Using an energetically balanced duel‐wavelength excitation scheme and spectral purification of detecting signal, the TPEF was completely blocked providing a possibility to probe microalgae and cyanobacteria in a fingerprint region of the CARS spectrum. Microspectroscopy experiments were carried out with three species ‐ cyanobacteria Nostoc Commune, Nostoc sp. and Chlorella sp. Distinct bands obtained in CARS spectra of such species were assigned to carotenoids and were taken as spectral markers in the imaging experiment. CARS imaging known as a chemical selective and label‐free technique allows non‐invasion monitoring of accumulation and movement of chemical compound at the subcellular level. Obtained high‐resolution images of carotenoid distribution in algae and cyanobacteria clearly demonstrate the potential of CARS microscopy for spatially resolved analysis of the natural products stored in the microalgae and cyanobacteria cell. Copyright © 2013 John Wiley & Sons, Ltd.     

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.     

有孔探针近场拉曼光谱和成像技术进展

基于有孔探针SNOM的近场拉曼光谱和成像技术的出现使得拉曼光谱的分辨率突破了光学衍射极限,从而提供了一个有力的工具对样品亚波长尺度之下的化学信息进行表征。文章讨论了探针性质对实现近场拉曼光谱的影响,并全面地介绍了有孔探针近场拉曼光谱发展十余年来在纳米尺度化学分辨成像、液-液界面性质研究、微观层面解释SERS增强机理、图像化反映SERS热点分布等诸多领域的研究进展。     

Investigation of the spatial profile of stimulated Raman scattering beams in D<Subscript>2</Subscript> and H<Subscript>2</Subscript> gases using a pulsed Nd:YAG laser at 266 nm

The stimulated Raman scattering (SRS) beam spatial mode structure is studied in H₂ and D₂ gases, in a 60 cm-long high-pressure Raman cell, using a pulsed Nd:YAG laser at 266 nm. The conversion efficiencies of the first and second Stokes in H₂, D₂ and H₂/D₂ mixtures have been measured precisely in the 1–14 atm range. The SRS beam profiles were recorded for different gas pressures in the high-pressure Raman cell and interesting behaviour is revealed. Homogeneous SRS spatial profiles were obtained only for pressures higher than 7 atm. For lower pressures the profiles are either in the form of a ring or of a more complicated shape. The results are explained in terms of nonlinear self-focusing processes during the pump beam propagation in the Raman cell. Also, from our measurements, a more precise value of the nonlinear index of refraction for the H₂ and D₂ at 266 nm is proposed. PACS 42.65.Dr; 42.60.Jf; 42.60.Lh; 42.65.Jx     

神光Ⅱ激光装置的全口径背向散射测量系统

报道了基于神光Ⅱ激光装置的全口径背向散射测量系统。系统通过激光聚焦透镜收集激光等离子体相互作用产生的散射光;两个热能量卡计分别测量波长348~354 nm范围的受激布里渊散射和波长400~700 nm范围的受激拉曼散射产生的散射光。该系统可以测量散射光的能量、功率和光谱图像,提供优于0.5 nm光谱分辨和10 ps时间分辨的光谱物理信息。同时采用PIN二极管阵列对聚焦透镜外侧附近的近背向散射光信息进行测量。     

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.     

Beryllium Silicate,Be2SiO4 (phenakite) – a Novel Trigonal SRS‐Active Crystal

In single crystals of the beryllium silicate Be₂SiO₄ with trigonal symmetry , known also as the mineral phenakite, χ⁽³⁾‐nonlinear lasing by stimulated Raman scattering (SRS) is investigated. All observed Stokes and anti‐Stokes lasing components are identified and ascribed to a single SRS‐promoting vibration mode with ω_SRS ≈876 cm⁻¹. With picosecond single‐wavelength pumping at one micrometer the generation of an octave‐spanning Stokes and anti‐Stokes comb is observed.