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might have to compete with other fluorescent processes. The CARS signal is detected on the blue side, which is free from fluorescence, but it comes with a non-resonant contribution. The differences between the signals from Raman and CARS (there are many variants of both techniques) stems largely from the fact that Raman relies on a spontaneous transition whereas CARS relies on a coherently driven transition. The total Raman signal collected from a sample is the incoherent addition of the signal from individual molecules. It is therefore linear in the concentration of those molecules and the signal is emitted in all directions. The total CARS signal comes from a coherent addition of the signal from individual molecules. For the coherent addition to be additive, phase-matching must be fulfilled. For tight focusing conditions this is generally not a restriction. Once phase-matching is fulfilled the signal amplitude grows linearly with distance so that the power grows quadratically. This signal forms a collimated beam that is therefore easily collected. The fact that the CARS signal is quadratic in the distance makes it quadratic with respect to the concentration and therefore especially sensitive to the majority constituent. The total CARS signal also contains an inherent non-resonant background. This non-resonant signal can be considered as the result of (several) far off-resonance transitions that also add coherently. The resonant amplitude contains a phase shift of π/2 radians over the resonance whereas the non-resonant part does not. The
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92.14×10 kg/mol. Therefore, the focal volume (~1 cubic micrometre) contains 6×10 molecules. Those molecules together generate a Raman signal in the order of 2×10 W (20 pW) or roughly one hundred million photons/sec (over 4π steradians). A CARS experiment with similar parameters (150 mW at 1064 nm, 200 mW at 803.5 nm, 15ps pulses at 80 MHz repetition frequency, same objective lens) yields roughly 17.5×10 W (on the 3000 cm line, which has 1/3 of the strength and roughly 3 times the width). This CARS power is roughly 10 higher than the Raman but since there are 6×10 molecules, the signal per molecule from CARS is only 4×10 W/molecule·s or 1.7×10 photons/molecule·s. If we allow two factors of three (line strength and line width) then the spontaneous Raman signal per molecule still exceeds the CARS per molecule by more than two orders of magnitude. The coherent addition of the CARS signal from the molecules however yields a total signal that is much higher than the Raman.
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situations (a factor of 10) using CARS. Imaging of known substances (known spectra) is therefore often done using CARS. Given the fact that CARS is a higher order nonlinear process, the CARS signal from a single molecule is larger than the Raman signal from a single molecule for a sufficiently high driving intensity. However, at very low concentrations, the advantages of the coherent addition for the CARS signal are reduced and the presence of the incoherent background becomes an increasing problem.
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molecule is no longer in a superposition, as it resides again in one state, the ground state. In the quantum mechanical model, no energy is deposited in the molecule during the CARS process. Instead, the molecule acts like a medium for converting the frequencies of the three incoming waves into a CARS signal (a parametric process). There are, however, related coherent Raman processes that occur simultaneously which do deposit energy into the molecule.
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used as an indication of the order of magnitude of the signals. 200 mW average power input (CW for the Raman), in a 0.9NA objective with a center wavelength around 800 nm, constitutes a power density of 26 MW/cm, (focus length = 1.5 micrometre, focus volume = 1.16 micrometre, photon energy = 2.31×10 J or 1.44 eV). The Raman cross section for the vibration of the aromatic ring in
237:) between the pump and the Stokes beams instead. This driving mechanism is similar to hearing the low combination tone when striking two different high tone piano keys: your ear is sensitive to the difference in the frequencies of the high tones. Similarly, the Raman oscillator is susceptible to the difference in frequency between two optical waves. When the difference of frequency ω
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CARS spectroscopy can be used for temperature measurements; because the CARS signal is temperature dependent. The strength of the signal scales (non-linearly) with the difference in the ground state population and the vibrationally excited state population. Since the population of states follows the
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between the incident beams matches a Raman frequency of the sample. Maker and
Terhune called their technique simply 'three wave mixing experiments'. The name coherent anti-Stokes Raman spectroscopy was assigned almost ten years later, by Begley et al. at Stanford University in 1974. Since then, this
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can be used as an instantaneous gateway to address a vibrational eigenstate of the molecule. The joint action of the pump and the Stokes has effectively established a coupling between the ground state and the vibrationally excited state of the molecule. The molecule is now in two states at the same
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CARS is often compared to Raman spectroscopy as both techniques probe the same Raman active modes. Raman can be done using a single continuous wave (CW) laser whereas CARS requires (generally) two pulsed laser sources. The Raman signal is detected on the red side of the incoming radiation where it
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Since CARS is such a nonlinear process there are not really any 'typical' experimental numbers. One example is given below under the explicit warning that just changing the pulse duration by one order of magnitude changes the CARS signal by three orders of magnitude. The comparison should only be
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Theoretically Raman spectroscopy and CARS spectroscopy are equally sensitive as they use the same molecular transitions. However, given the limits on input power (damage threshold) and detector noise (integration time), the signal from a single transition can be collected much faster in practical
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of states. This coherence between the states can be probed by the probe beam, which promotes the system to a virtual state. Again, the molecule cannot stay in the virtual state and will fall back instantaneously to the ground state under the emission of a photon at the anti-Stokes frequency. The
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around 1000 cm is on the order of 10cm/molecule·steradian. Therefore, the Raman signal is around 26×10 W/molecule·steradian or 3.3×10 W/molecule (over 4π steradians). That is 0.014 photon/sec·molecule. The density of toluene = 0.8668×10 kg/m, molecular mass =
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It is very similar to the more common CARS except it uses an anti-Stokes frequency stimulation beam and a Stokes frequency beam is observed (the opposite of CARS). This is disadvantageous because anti-stokes processes must start in a less populated excited state.
122:, P. D. Maker and R. W. Terhune, in which the CARS phenomenon was reported for the first time. Maker and Terhune used a pulsed ruby laser to investigate the third order response of several materials. They first passed the ruby beam of frequency ω through a
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of the material. This periodic modulation can be probed by a third laser beam, the probe beam. When the probe beam is propagating through the periodically altered medium, it acquires the same modulation. Part of the probe, originally at
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pronounced as "scissors") is closely related to Raman spectroscopy and lasing processes. It is very similar to CARS except it uses an anti-Stokes frequency stimulation beam and a Stokes frequency beam is observed (the opposite of CARS).
887:"An introduction to some of the more exciting recent advances and dynamic current areas of development in biomedical Raman spectroscopy. Illuminating disease and enlightening biomedicine: Raman spectroscopy as a diagnostic tool"
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While intuitive, this classical picture does not take into account the quantum mechanical energy levels of the molecule. Quantum mechanically, the CARS process can be understood as follows. Our molecule is initially in the
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Coherent Stokes Raman spectroscopy (CSRS pronounced as "scissors") is a form of spectroscopy used primarily in chemistry, physics and related fields. It is closely related to Raman spectroscopy and
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which is shifted with respect to the Raman signal. To compare the spectra from multi-component compounds, the (resonant) CARS spectral amplitude should be compared to the Raman spectral intensity.
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of the molecule and it can not be occupied but it does allow for transitions between otherwise unoccupied real states. If a Stokes beam is simultaneously present along with the pump, the
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278:, which is the observed anti-Stokes emission. Under certain beam geometries, the anti-Stokes emission may diffract away from the probe beam, and can be detected in a separate direction.
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The sensitivity in many CARS experiments is not limited by the detection of CARS photons but rather by the distinction between the resonant and non-resonant part of the CARS signal.
249:, the oscillator is driven very efficiently. On a molecular level, this implies that the electron cloud surrounding the chemical bond is vigorously oscillating with the frequency ω
130:, and then directed the two beams simultaneously onto the sample. When the pulses from both beams overlapped in space and time, the Ford researchers observed a signal at ω+ω
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39:, typically the nuclear vibrations of chemical bonds. Unlike Raman spectroscopy, CARS employs multiple photons to address the molecular vibrations, and produces a
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Tolles, W.M.; Nibler, J.W.; McDonald, J.R.3; Harvey, A.B. (1977). "A Review of the Theory and
Application of Coherent Anti-Stokes Raman Spectroscopy (CARS)".
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CARS is used for species selective microscopy and combustion diagnostics. The first exploits the selectivity of vibrational spectroscopy. More recently,
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607:"Coherent anti-Stokes Raman scattering: from proof-of-the-principle experiments to femtosecond CARS and higher order wave-mixing generalizations"
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Maker, P.D.; Terhune, R.W. (1965). "Study of
Optical Effects Due to an Induced Polarization Third Order in the Electric Field Strength".
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134:, which is the blue-shifted CARS signal. They also demonstrated that the signal increases significantly when the difference frequency ω
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Deckert, V.; Deckert-Gaudig, T.; Cialla-May, D.; Popp, J.; Zell, R.; Deinhard-Emmer, S.; Sokolov, A.V.; Yi, Z.; Scully, M.O. (2020).
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Evans, C.L.; Xie, X.S. (2008). "Coherent Anti-Stokes Raman
Scattering Microscopy: Chemical Imaging for Biology and Medicine".
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model that incorporates the energy levels of the molecule. Classically, the Raman active vibrator is modeled as a (damped)
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processes. It is very similar to Raman spectroscopy, but involves a lasing process that dramatically improves the signal.
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Ellis, David I.; Cowcher, David P.; Ashton, Lorna; O'Hagan, Steve; Goodacre, Royston (2013). Ellis, David I. (ed.).
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signal. As a result, CARS is orders of magnitude stronger than spontaneous Raman emission. CARS is a third-order
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The CARS process can be physically explained by using either a classical oscillator model or by using a
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and related fields. It is sensitive to the same vibrational signatures of molecules as seen in
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716:"Laser spectroscopic technique for direct identification of a single virus : FASTER CARS"
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has been utilized as a method for non-invasive imaging of lipids in biological samples, both
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and team used femtosecond adaptive spectroscopic techniques via CARS to identify individual
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Begley, R.F.; Harvey, A.B.; Byer, R.L. (1974). "Coherent anti-Stokes Raman spectroscopy".
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In 1965, a paper was published by two researchers of the
Scientific Laboratory at the
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vibrationally sensitive nonlinear optical technique has been commonly known as CARS.
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Proceedings of the
National Academy of Sciences of the United States of America
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Ori Katz; Adi Natan; Salman
Rosenwaks; Yaron Silberberg (December 2008).
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10.1002/1097-4555(200008/09)31:8/9<653::AID-JRS597>3.0.CO;2-W
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Rotating-polarization coherent anti-Stokes Raman spectroscopy
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Rotating-polarization coherent anti-Stokes Raman spectroscopy
788:"Shaped Femtosecond Pulses for Remote Chemical Detection"
816:"Laser beam 'kicks' molecules to detect roadside bombs"
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Coherent anti-Stokes Raman spectrum of microscopy oil.
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Scattering, absorption and radiative transfer (optics)
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392:anti-Stokes emission: centered to -1250 cm (CH
390:Stokes beam: broadband from 1000 nm to 1100 nm;
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587:: CS1 maint: numeric names: authors list (
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605:Zheltikov, A.M. (August–September 2000).
358:Learn how and when to remove this message
197:Learn how and when to remove this message
1155:Extended X-ray absorption fine structure
321:This section includes a list of general
160:This section includes a list of general
1523:Coherent anti-Stokes Raman spectroscopy
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17:Coherent anti-Stokes Raman spectroscopy
862:10.1146/annurev.anchem.1.031207.112754
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842:Annual Review of Analytical Chemistry
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515:Coherent Raman scattering microscopy
444:Coherent Raman scattering microscopy
225:with a characteristic frequency of ω
91:) coincides with the frequency of a
1553:Surface-enhanced Raman spectroscopy
1543:Spatially offset Raman spectroscopy
1604:Stimulated Raman adiabatic passage
417:Coherent Stokes Raman spectroscopy
327:it lacks sufficient corresponding
166:it lacks sufficient corresponding
103:Coherent Stokes Raman spectroscopy
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1372:Deep-level transient spectroscopy
1124:Saturated absorption spectroscopy
51:beams: a pump beam of frequency ω
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1377:Dual-polarization interferometry
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304:Comparison to Raman spectroscopy
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1563:Transmission Raman spectroscopy
1558:Tip-enhanced Raman spectroscopy
1392:Scanning tunneling spectroscopy
1367:Circular dichroism spectroscopy
1362:Acoustic resonance spectroscopy
295:time: it resides in a coherent
63:and a probe beam at frequency ω
1321:Fourier-transform spectroscopy
1009:Vibrational circular dichroism
126:to create a second beam at ω-ω
97:vibrational contrast mechanism
1:
1667:Journal of Raman Spectroscopy
1548:Stimulated Raman spectroscopy
1119:Cavity ring-down spectroscopy
1024:Thermal infrared spectroscopy
611:Journal of Raman Spectroscopy
1533:Resonance Raman spectroscopy
1253:Inelastic neutron scattering
396:groups symmetric vibration).
1314:Data collection, processing
1190:Photoelectron/photoemission
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1399:Photoacoustic spectroscopy
1341:Time-resolved spectroscopy
567:10.1366/000370277774463625
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266:will now get modified to ω
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1425:Astronomical spectroscopy
1404:Photothermal spectroscopy
501:CARS-based detectors for
1674:Vibrational Spectroscopy
1645:Rule of mutual exclusion
666:10.1103/PhysRev.137.A801
373:spectroscopic line shape
47:process involving three
1409:Pump–probe spectroscopy
1298:Ferromagnetic resonance
1090:Laser-induced breakdown
754:10.1073/pnas.2013169117
681:Applied Physics Letters
505:are under development.
342:more precise citations.
181:more precise citations.
1528:Raman optical activity
1105:Glow-discharge optical
1085:Raman optical activity
999:Rotational–vibrational
491:Boltzmann distribution
489:temperature dependent
484:Combustion diagnostics
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1740:Instrumental analysis
1326:Hyperspectral imaging
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1620:Depolarization ratio
1078:Coherent anti-Stokes
1033:UV–Vis–NIR "Optical"
547:Applied Spectroscopy
1640:Rayleigh scattering
1579:Raman amplification
1382:Hadron spectroscopy
1172:Conversion electron
1133:X-ray and Gamma ray
1040:Ultraviolet–visible
906:2013Ana...138.3871E
854:2008ARAC....1..883E
745:2020PNAS..11727820D
729:(45): 27820–27824.
693:1974ApPhL..25..387B
658:1965PhRv..137..801M
623:2000JRSp...31..653Z
559:1977ApSpe..31..253T
388:Pump beam: 800 nm;
223:harmonic oscillator
213:CARS energy diagram
59:beam of frequency ω
1735:Raman spectroscopy
1509:Raman spectroscopy
1430:Force spectroscopy
1355:Measured phenomena
1346:Video spectroscopy
1050:Cold vapour atomic
915:10.1039/C3AN00698K
497:Other applications
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219:quantum mechanical
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120:Ford Motor Company
37:Raman spectroscopy
27:used primarily in
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1232:Beta spectroscopy
1145:Energy-dispersive
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1062:Near-infrared
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1713:Spectroscopy
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1650:Stokes shift
1572:Applications
1522:
1464:
1452:
1432:(a misnomer)
1418:Applications
1336:Time-stretch
1227:paramagnetic
1077:
1045:Fluorescence
963:Spectroscopy
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893:
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799:the original
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583:cite journal
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470:myelopathies
460:. Moreover,
457:
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433:Applications
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377:Fano profile
369:
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284:ground state
280:
245:approaches ω
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71:frequency (ω
25:spectroscopy
20:
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1589:Raman laser
1004:Vibrational
848:: 883–909.
480:particles.
472:. In 2020,
340:introducing
179:introducing
69:anti-Stokes
1729:Categories
1516:Techniques
1210:Two-photon
1112:absorption
994:Rotational
736:2003.07951
532:References
348:April 2024
323:references
288:eigenstate
187:April 2024
162:references
1288:Terahertz
1269:Radiowave
1167:Mössbauer
527:(RP-CARS)
143:Principle
29:chemistry
1694:Category
1659:Journals
1454:Category
1183:Electron
1150:Emission
1100:emission
1057:Vibronic
924:23722248
878:15904719
870:20636101
773:33093197
575:98395453
509:See also
458:in vitro
41:coherent
1706:Commons
1599:SHERLOC
1466:Commons
1293:ESR/EPR
1241:Nucleon
1069:(REMPI)
902:Bibcode
894:Analyst
850:Bibcode
764:7668096
741:Bibcode
689:Bibcode
654:Bibcode
619:Bibcode
555:Bibcode
462:RP-CARS
454:in vivo
407:toluene
336:improve
175:improve
114:History
33:physics
1613:Theory
1307:Others
1095:Atomic
922:
876:
868:
771:
761:
573:
474:Scully
466:myelin
423:lasing
325:, but
164:, but
57:Stokes
1248:Alpha
1217:Auger
1195:X-ray
1162:Gamma
1140:X-ray
1073:Raman
984:Raman
979:FT-IR
890:(PDF)
874:S2CID
802:(PDF)
791:(PDF)
731:arXiv
719:(PDF)
571:S2CID
478:virus
49:laser
920:PMID
866:PMID
769:PMID
589:link
468:and
456:and
107:CSRS
55:, a
21:CARS
1276:NMR
910:doi
898:138
858:doi
821:BBC
795:OPN
759:PMC
749:doi
727:117
697:doi
662:doi
650:137
627:doi
563:doi
1731::
1281:2D
1200:UV
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