Coherent Anti-Stokes Raman Scattering: Basics, Theoretical Background doi:10.1146/annurev.anchem.1.031207.112754, PubMed Abstract | CrossRef Full Text | Google Scholar. doi:10.1038/s41589-020-0565-2, 76 Choi DS, Jeoung SC, Chon BH. electrostriction and magnetostriction). The population follows the Boltzmann distribution: N exp ( E k B T) Therefore there are exponentially fewer molecules that start out in the higher energy vibrational state. Optic Express (2018) 26(11):1430714. doi:10.1002/jrs.2356, 49 Vartiainen EM, Rinia HA, Mller M, Bonn M. Direct extraction of Raman line-shapes from congested CARS spectra. Rev. . Laser-scanning coherent anti-Stokes Raman scattering microscopy and applications to cell biology. From the perspective of solid state physics, Brillouin scattering is an interaction between an electromagnetic wave and one of the three above-mentioned crystalline lattice waves (e.g. in 1964. CARS provides a signal that contains the Raman response of interest for performing label-free chemically sensitive microscopy. 595606. Frontiera, G.C. Rev. doi:10.1016/S0006-3495(02)75186-2, 17 Evans CL, Potma EO, Puoris'haag M, Ct D, Lin CP, Xie XS. doi:10.1364/josab.19.001363, 3 Evans CL, Xie XS. Biophys J (2010) 99(8):2695704. : The principles of nonlinear optics. V. Namboodiri, M. Namboodiri, G. I. C. Diaz, M. Oppermann, G. Flachenecker, A. Materny, Vibrational Spectroscopy; A Selection of the Papers Presented at the 3rd International Conference on Perspectives in Vibrational Spectroscopy 56, 912 (2011). Multiplex coherent anti-Stokes Raman scattering microspectroscopy and study of lipid vesicles. In this review, the history and early development of CARS are introduced, as well as the implementation of both single frequency and multiplex CARS. doi:10.1007/s00216-004-2942-1, 52 van Manen H-J, Kraan YM, Roos D, Otto C. Intracellular chemical imaging of heme-containing enzymes involved in innate immunity using resonance Raman microscopy. The intensity of anti-Stokes relative to Stokes Raman scattering decreases rapidly with increase in the wavenumber shift. Brillouin scattering - Wikipedia SL, LL and JQ wrote and edited the manuscript. Alignment-free, all-spliced fiber laser source for CARS microscopy based on four-wave-mixing. doi:10.1021/acs.analchem.9b01746, 92 Meyer T, Bae H, Hasse S, Winter J, Woedtke TV, Schmitt M, et al. Hill, C.W. Because the cost of the spontaneous Raman system is relatively low and the system is relatively simple, it will likely be chosen when imaging speed is not a priority or there are technical difficulties (such as sample environment) to apply the coherent method. The advantages of-fered over simple spontaneous Raman spectroscopy are the coherent signal blue-shifted away Opt Lett (2006) 31(3):3202. Official websites use .gov The full spectrum is essential when studying complex samples with many overlapping peaks and the quantitative nature of the spectrum makes multiplex CARS microscopy a particularly useful technique for probing such complex samples. CARS microscopy has been widely used for cell imaging [36, 4553]. Chem. doi:10.1002/anie.201001560, 37 Okuno M, Kano H, Leproux P, Couderc V, Hamaguchi HO. Rev. Micromachines (2019) 10(9). 11 Duncan MD, Reintjes J, Manuccia TJ. Initially, coherent anti-Stokes Raman scattering (CARS) microscopy was introduced as a means for the fast imaging of unlabeled samples. In another work, Di Napoli [59] fed different ratios of Palmitic acid and -linolenic acid to human adipose derived stem cells and the results showed good contrast between cellular components and the corresponding CARS spectra. Williams, Proc. Coherent Anti-Stokes Raman Scattering: Basics, Theoretical Background, and Applications. doi:10.1364/oe.15.004848, 91 Yarbakht M, Pradhan P, Kse-Vogel N, Bae H, Stengel S, Meyer T, et al. High-contrast, fast chemical imaging by coherent Raman scattering using a self-synchronized two-colour fibre laser. Spatial frequency modulated imaging in coherent anti-Stokes Raman microscopy. [1] Anal Chem (2019) 91(17):1111621. In addition, the laser excitation of the spectrum in the near infrared region can minimize the generation of the non-resonant background in CARS [12], providing less light-induced damage than visible light, and deeper penetration into the tissue. Frontiers | Coherent Anti-Stokes Raman Scattering Microscopy and Its Optic Express (2009) 17(4):298496. 7, 118119 (1961). doi:10.1364/ol.34.002051, 24 Cheng J-X, Volkmer A, Book LD, Xie XS. : Advances in Nonlinear Spectroscopy. The effects of the two phenomena provide very different information about the sample: Raman spectroscopy can be used to determine the transmitting medium's chemical composition and molecular structure, while Brillouin scattering can be used to measure the material's properties on a larger scale such as its elastic behavior. P.C. Although CARS has broad application prospects, it will not replace other imaging methods in all fields. Anal Bioanal Chem (2005) 381(1):2617. Science (2015) 350(6264):aaa8870. Ultrafast fiber lasers can potentially overcome these shortcomings but have not yet been fully exploited for CARS microscopy, as previous implementations have suffered from high intensity noise, a narrow tuning range, and low power, resulting in low image quality and slow imaging speed [23, 8390]. Opt Lett (2006) 31(12):18724. Appl Phys Lett (2008) 93(20):201103. doi:10.1063/1.3028346, 40 Langbein W, Rocha-Mendoza I, Borri P. Coherent anti-Stokes Raman micro-spectroscopy using spectral focusing: theory and experiment. 2021 The Author(s), under exclusive license to Springer Nature Singapore Pte Ltd. Mazaheri Tehrani, A., Mohaghegh, F., Materny, A. In CARS, a vibrational coherence is generated when a pair of photons (pump and Stokes) interact with the sample to excite a vibrationally resonant Raman mode at frequency vib = pump Stokes. Energy diagrams of the CARS process. J Raman Spectrosc (2007) 38(7):91626. doi:10.1063/1.1768312, 39 Rocha-Mendoza I, Langbein W, Borri P. Coherent anti-Stokes Raman microspectroscopy using spectral focusing with glass dispersion. For liquids and gases, the frequency shifts typically created are of the order of 110 GHz resulting in wavelength shifts of ~110 pm in the visible light. Nat Photon (2019) 14:11522. Photonics 8, 589591 (2014). School of Physics, Xian Jiaotong University, China, Huazhong University of Science and Technology, China. With this system we obtain 3000 cm-1 spectrum at each laser shot, allowing us to rapidly image chemically complex systems, such as the polymer blend shown in the figure below. Despite all of its advantages, however, the non-resonant background that limits the sensitivity of CARS is a major disadvantage. Arterioscler Thromb Vasc Biol (2009) 29(9):13428. The theory predicts anti-Stokes over Stokes scattering enhancement domination when both anti-Stokes and Stokes secondary photons energies correspond to the descending long-wave wing of extinction spectra of metal nanoparticles. doi:10.1038/s41566-019-0535-y, 81 Duarte AS, Schnedermann C, Kukura P. Wide-field detected fourier transform CARS microscopy. Raman scattering or the Raman effect ( / rmn /) is the inelastic scattering of photons by matter, meaning that there is both an exchange of energy and a change in the light's direction. Biophys J (2002) 83(1):5029. Van Duyne, J. These results clearly demonstrate the advantage and feasibility of anti-Stokes Raman scattering for the elimination of the thermal emission in comparison with Stokes scattering. Optic Express (2009) 17(5):36518. New York, NY: Springer Science & Business Media (2010). Bonghwan Chon Energy diagram of the (A) resonant condition and (B) non-resonant condition. Hyper-Raman microspectroscopy: a new approach to completing vibrational spectral and imaging information under a microscope. doi:10.1021/jp046955b, 53 McConnell G, Riis E. Photonic crystal fibre enables short-wavelength two-photon laser scanning fluorescence microscopy with fura-2. Paar et al. doi:10.1002/jbio.201200171, Keywords: Raman scattering, coherent anti-Stokes Raman scattering, nonlinear optical microscopy, label-free imaging, biomedical imaging, Citation: Li S, Li Y, Yi R, Liu L and Qu J (2020) Coherent Anti-Stokes Raman Scattering Microscopy and Its Applications. Measurements of nonlinear light scattering. 12, 327331 (1999). This is because the Raman stokes and anti-Stokes intensities are weaker than the Rayleigh scattering intensity in Raman distributed optical fiber sensors 81. Vibrational imaging of lipid droplets in live fibroblast cells with coherent anti-Stokes Raman scattering microscopy. Figure 2. The development of the femtosecond laser with high peak power has enabled the observation of many nonlinear processes, and promoted the study of coherent Raman scattering. Microsc Res Tech (2012) 75(4):4928. First, Raman scattered photons in the mid-infrared range carry information about molecular vibration. (B) CARS signal collection: forward-CARS (F-CARS) and backward (epi)-CARS (E-CARS). It is sensitive to the same vibrational signatures of molecules as seen in Raman spectroscopy, typically the nuclear vibrations of chemical bonds. Appl Spectrosc (2007) 61(9):197208. Dieringer, R.B. FIGURE 3. Several groups have reported that they employed 50200fs pulse widths rather than a 26picosecond pulse width [22, 2527]. Optic Express (2006) 14(8):362230. CARS has also been posited as a unique tool for label free tissue imaging. This lipid transfer is not a rapid spontaneous process but completed within a few hours. N. Lock Explain the difference between Stokes and anti-Stokes lines in a Raman spectrum. https://www.nist.gov/programs-projects/broadband-coherent-anti-stokes-raman-scattering-bcars-microscopy. Typically this effect involves vibrational energy being gained by a molecule as incident photons from a visible laser are shifted to lower energy. doi:10.1364/OE.20.021010, 87 Wang K, Freudiger CW, Lee JH, Saar BG, Xie XS, Xu C. All fiber, 1064-nm time-lens source for coherent anti-Stokes Raman scattering and stimulated Raman scattering microscopy. doi:10.1194/jlr.D300022-JLR200, 55 Paar M, Jngst C, Steiner NA, Magnes C, Sinner F, Kolb D, et al. van Schoot, T.J.A. Chemical imaging with frequency modulation coherent anti-Stokes Raman scattering microscopy at the vibrational fingerprint region. Begley and his co-workers used CARS to study the chemical reaction kinetics of combustion. A promising alternative to the SR-based investigation of LN structures is the application of coherent Raman techniques like broadband coherent anti-Stokes Raman scattering (B-CARS). Coherent anti-Stokes Raman spectroscopy (CARS) This technique involves the phenomenon of wave mixing, takes advantage of the high intensity of stimulated Raman scattering, and has the applicability of conventional Raman spectroscopy.In the CARS method two strong collinear laser beams at frequencies 1 and 2 ( 1 > 2) irradiate a sample.If the frequency difference, 1 2, is . J.A. doi:10.1364/OE.17.001282, 27 Ozeki Y, Dake F, Kajiyama S, Fukui K, Itoh K. Analysis and experimental assessment of the sensitivity of stimulated Raman scattering microscopy. Vibrational spectroscopic imaging of living systems: an emerging platform for biology and medicine. There is a need for label-free chemical microscopy in medicine, biology and materials science. doi:10.1021/jp104553s, 48 Brackmann C, Norbeck J, keson M, Bosch D, Larsson C, Gustafsson L, et al. Another recent trend has been focusing on label-free multimodal nonlinear microscopy based on CARS, two-photon excited fluorescence (TPEF), and SHG [9194]. The switch from infrared to visible light circumvents the strong optical absorption of water in the infrared region, which is of great significance in the field of biomedical science. Coherent anti-Stokes Raman Scattering (CARS)1 is an increasingly popular four-wave mix- ing optical technique for spectroscopy and chemically specic microscopy. Optic Laser Eng (2011) 49(1):6670. Label-free tetra-modal molecular imaging of living cells with CARS, SHG, THG and TSFG (coherent anti-Stokes Raman scattering, second harmonic generation, third harmonic generation and third-order sum frequency generation). Lett. Justify the difference in intensity between Stokes and anti-Stokes lines. 1 Raman CV, Krishnan KS. APL Photonics (2018) 3(9):090901. doi:10.1063/1.5040101, 7 Rigneault H, Berto P. Tutorial: coherent Raman light matter interaction processes. BMC Canc (2009) 9(1):42. doi:10.1186/1471-2407-9-42, 57 Mitra R, Chao O, Urasaki Y, Goodman OB, Le TT. I understand that from a Boltzmann distribution point of view, the ratio between Stokes and anti-Stokes scattering should be: $$\frac{I_S}{I_{aS}} . Wiley Interscience, New York (1984). Optic Express (2009) 17(23):207006. FIGURE 2. The process of stimulated Brillouin scattering (SBS) was first observed by Chiao et al. J Biophot (2010) 3(1011):72836. Christopher Hartshorn J Phys Chem B (2002) 106(34):84938. Appl Phys Lett (2005) 86(12):121113. doi:10.1063/1.1883714, 33 Kee TW, Cicerone MT. Interfacial Electrochem. Using photonic crystal fiber-based CARS microscopy, the capability of multimodal imaging was demonstrated by an alternative femtosecond system to study lesion development in myocardial infarction-prone, hyperlipidemic rabbits [70]. J Phys Chem B (2004) 108(3):82740. Appl Phys Lett (1974) 25(7):38790. Coherent anti-Stokes Raman scattering: Spectroscopy and - ScienceDirect Although it has many advantages, spontaneous Raman scattering is a very weak second-order radiative process. Images are pseudo-colored based on spectral content at each pixel (right). In addition, by adjusting the center wavelength of the Stokes pulse, other regions of the vibration spectrum can also be studied, although not simultaneously. Appl Phys Lett (2009) 95(8):081109. doi:10.1063/1.3216073, 42 Gu M, Satija A, Lucht RP. Spectra from regions of bone (bottom left), fat (top left) and cellular components (both) are shown. (C) Extremely broadband, 785cm1 (nuclei) to 1,665cm1 (protein), CARS imaging of a murine pancreatic duct and 3D reconstruction imaging [60]. Laser scanning CARS microscopy based on the picosecond pulsed laser was developed for high-speed imaging of biomedical samples [16], and the imaging speed of CARS reached the level of video-rate (20 frames/s) in 2005 [17]. M. D. doi:10.1111/j.1365-2818.2007.01729.x, 62 Jung Y, Ng JH, Keating CP, Senthil-Kumar P, Zhao J, Randolph MA, et al. Mater. Osterloh, Chem. They are called virtual because it does not correspond to any quantum state of the molecule. For example, Nan et al. High chemical specificity and classification accuracy without labeling is demonstrated by the differentiation of polymer beads and Euglena gracilis. Brillouin scattering can also be employed to sense mechanical strain and temperature in optical fibers. Tax calculation will be finalised at checkout, Copyright 2014 American Chemical Society, Copyright 2014 American Physical Society, Copyright 2011 American Chemical Society, L.A. Lyon, C.D. CARS is an ideal tool to study the interplay between catalyst architecture and reactivity and hence obtain previously inaccessible information about fundamental processes of catalysts. Since CARS microscopy suffers from a nonresonant background signal and a quadratic dependence on sample molecule concentration, soon afterward, stimulated Raman scattering (SRS) microscopy was introduced. Figures 3C shows multicolor CARS using a femtosecond pump and Stokes pulse with spectral focusing [30, 3844], and Figures 3D shows the principle of the spectral focusing method. We study the temperature dependence of car Multimodal imaging to study the morphochemistry of basal cell carcinoma. 86, 33913395 (1982), H. Hiramatsu, F.E. Therefore, the different components in the sample can be distinguished based on their vibrational information in an unlabeled manner, and the sensitivity of each component can be increased to the mMM level by using electronic resonance enhancement.
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