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Second-order nonlinear-optical effects Symmetry issues Phase-matching in SHG Phase-matching bandwidth Group-velocity mismatch Nonlinear-optical crystals Practical numbers for SHG Electro-optics Difference-frequency generation and optical parametric generation First demonstration of second-harmonic generation P.A. Franken, et al, Physical Review Letters 7, p. 118 (1961) The second-harmonic beam was very weak because the process was not phase-matched. First demonstration of SHG: the data The actual published results Input beamThe second harmonic Note that the very weak spot due to the second harmonic is missing. It was removed by an overzealous Physical Review Letters editor, who thought it was a speck of dirt and didnt ask the authors first. Symmetry in second-harmonic generation For this to hold, (2) must be zero for media with inversion symmetry. Most materials have inversion symmetry, so you just dont see SHG or any other even-order nonlinear-optical effectevery day. E (t)E 2(t) Esig(x,t) (2)E 2(x,t) If we imagine inverting space: Esig(x,t) -Esig(x,t) E (x,t) -E (x,t) Now, if the medium is symmetrical, (2) remains unchanged. So: -Esig(x,t) (2) -E (x,t) 2 = (2)E (x,t)2 Esig(x,t) Phase-matching in second-harmonic generation How does phase-matching affect SHG? Its a major effect, another important reason you just dont see SHGor any other nonlinear-optical effectsevery day. Sinusoidal dependence of SHG intensity on length Large DkSmall Dk The SHG intensity is sharply maximized if Dk = 0. which will only be satisfied when: Unfortunately, dispersion prevents this from ever happening! Phase-matching second-harmonic generation So were creating light at wsig = 2w. Frequency Refractive index And the k-vector of the polarization is: The phase-matching condition is: The k-vector of the second-harmonic is: We can now satisfy the phase-matching condition. Use the extraordinary polarization for w and the ordinary for 2w. Phase-matching second-harmonic generation using birefringence Birefringent materials have different refractive indices for different polarizations. Ordinary and extraordinary refractive indices can be different by up to 0.1 for SHG crystals. Frequency Refractive index ne depends on the propagation angle, so we can tune for a given w. Some crystals have ne widler Difference-Frequency Generation: Optical Parametric Generation, Amplification, Oscillation w1 w3 w2 Optical Parametric Amplification (OPA) w1 w1 w3 w2 Optical Parametric Generation (OPG) Difference-frequency generation takes many useful forms. mirrormirror Optical Parametric Generation Equations are just about identical to those for SHG: where: ki = wave vector of ith wave Dk = k1 + k2 - k3 vgi = group velocity of ith wave The solutions for E1 and E2 involve exponential gain! OPAs etc. are ideal uses of ultrashort pulses, whose intensities are high. Phase-matching applies. We can vary the crystal angle in the usual manner, or we can vary the crystal temperature (since n depends on T). Free code to perform OPO, OPA, and OPG calculations Public domain software maintained by Arlee Smith at Sandia National Labs. Just web-search SNLO. You can use it to select the best nonlinear crystal for your particular application or perform detailed simulations of nonlinear mixing processes in crystals. Functions in SNLO: 1. Crystal properties 2. Modeling of nonlinear crystals in various applications. 3. Designing of stable cavities, computing Gaussian focus parameters and displaying the help file. Optical Parametric Generation Results using the nonlinear medium, periodically poled RbTiOAsO4 Sibbett, et al., Opt. Lett., 22, 1397 (1997). signal: idler: An ultrafast noncol- linear OPA (NOPA) Continuum generates an arbitrary-color seed pulse. NOPA specs Crystals for far-IR generation With unusual crystals, such as AgGaS2, AgGaSe2 or GaSe, one can obtain radiation to wavelengths as long as 20 m. These long wavelengths are useful for vibrational spectroscopy. Gavin D. Reid, University of Leeds, and Klaas Wynne, University of Strathclyde 10 m1 m Wavelength Elsaesser, et al., Opt. Lett., 23, 861 (1998) Difference- frequency generation in GaSe Angle-tuned wavelength Another 2nd-order process: Electro-optics Applying a voltage to a crystal changes its refractive indices and introduces birefringence. In a sense, this is sum-frequency generation with a beam of zero frequency (but not zero field!). A few kV can turn a crystal into a half- or quarter-wave plate. V If V = 0, the pulse polarization

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