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Definition: a nonlinear scattering process involving optical phonons
The nonlinear response of a transparent optical medium to the optical intensity of light propagating through the medium is very fast, but not instantaneous. In particular, a non-instantaneous response is caused by vibrations of the crystal (or glass) lattice. When these vibrations are associated with optical phonons, the effect is called Raman scattering, whereas acoustical phonons are associated with Brillouin scattering. When e.g. two laser beams with different wavelengths (and normally with the same polarization direction) propagate together through a Raman-active medium, the longer wavelength beam (called the Stokes wave) can experience optical amplification at the expense of the shorter wavelength beam. In addition, lattice vibrations are excited, leading to a temperature rise. The Raman gain for the longer wavelength beam can be exploited in Raman amplifiers and Raman lasers. That gain can be substantial if the Stokes shift corresponds to a frequency difference of several terahertz.
In the Raman scattering process, one pump photon is converted into one lower-energy signal photon, and the difference of photon energies is carried away by a phonon (a quantum of the lattice vibrations). In principle, it is also possible that an already existing phonon interacts with a pump photon to generate one higher-energy photon, belonging to an anti-Stokes wave at a shorter wavelength. That process, however, is usually weak, particularly at low temperatures. Note, however, that strong anti-Stokes light can also arise from four wave mixing if that process is phase-matched.
When the intensity of the generated Stokes wave becomes sufficiently high, that wave may again act as the pump for a further Raman process. Particularly in some Raman lasers, it is possible to observe several Stokes orders (cascaded Raman lasers).
Apart from the mentioned stimulated Raman scattering effect, which can be described with classical physics, there is also spontaneous Raman scattering, caused by quantum effects.
Raman scattering can also occur within the broad optical spectrum of, e.g., an ultrashort optical pulse, effectively shifting the spectral envelope of the pulse towards longer wavelengths (Raman self-frequency shift, also called soliton self-frequency shift).
Some typical Raman-active media are
- certain gases, e.g. hydrogen (H2), methane (CH4) and carbon dioxide (CO2), used in, e.g., high pressure cells for Raman shifters
- solid-state media such as glass fibers or certain crystals, e.g. barium nitride = Ba(NO3)2 or various tungstates such as KGd(WO4)2 = KGW and KY(WO4)2 = KYW
The Raman effect occurs together with the Kerr effect, which results from the (nearly) instantaneous response of the electrons.
In optical fiber devices such as fiber amplifiers for intense pulses, Raman scattering can be detrimental: it can transfer much of the pulse energy into a wavelength range where laser amplification does not occur. This effect can limit the peak power achievable with such devices. Even in continuous-wave high-power fiber lasers and amplifiers, Raman scattering can be a problem. There are, however, various kinds of solutions to such problems, including chirped-pulse amplification and the use of special fiber designs (see e.g. ) which suppress Raman scattering by attenuating the Raman-shifted wavelength component.
In bulk media, such as certain nonlinear crystal materials, unwanted stimulated Raman scattering can occur even via non-collinear phase matching, if the pump intensity is rather high and the beam width is large enough. This can occur e.g. in optical parametric generators operated with intense pump pulses.
Raman scattering is also used in spectroscopy. In particular, it allows one to investigate the vibrational modes of materials.
|||V. V. Raman and K. S. Krishnan, “A new type of secondary radiation”, Nature 121, 501 (1928)|
|||G. Eckhardt et al., “Stimulated emission of Stokes and anti-Stokes Raman lines from diamond, calcite and alpha-sulfur single crystals”, Appl. Phys. Lett. 3, 137 (1963) (first report of stimulated Raman scattering in insulating crystals)|
|||N. Bloembergen, “The stimulated Raman effect”, Am. J. Phys. 35 (11), 989 (1967)|
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|||J. M. Fini et al., “Distributed suppression of stimulated Raman scattering in an Yb-doped filter-fiber amplifier”, Opt. Lett. 31 (17), 2550 (2006)|
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|||D. J. Spence and R. P. Mildren, “Mode locking using stimulated Raman scattering”, Opt. Express 15 (13), 8170 (2007)|
|||X. Ma et al., “Propagation-length independent SRS threshold in chirally-coupled-core fibers”, Opt. Express 19 (23), 22575 (2011)|
|||G. P. Agrawal, Nonlinear Fiber Optics, 4th edn., Academic Press, New York (2007)|
|||R. Paschotta, case study on the soliton self-frequency shift|