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Non-Linear Optics Chapter 12 Physics 208, Electro-optics Peter Beyersdorf Document info ch 12. 1 Non-Linear Optics We’ve seen that an externally applied electric field can alter the index of refraction of a material. At sufficiently high intensities, the electric field associated with a propagating wave can have the same effect. This is the premise behind the field of non-linear optics. ch 12. 2 Non-Linear Response Consider the response (material polarization) of a material to an applied electric field (i.e. a propagating wave) Pi = !0 Xij Ej + 2dijk Ej Ek + 4Xijkl Ej Ek El + . . . When the applied electric field is small compared to the internal binding fields of the material, the response is primarily linear Pi ≈ !0 Xij Ej At higher intensities the higher order terms in the material polarization come into play. Like the electrooptic effect, centro-symmetric crystals do not have a 2nd order nonlinearity (i.e. dijk=0) ch 12. 3 Non-Linear dijk Coefficients In a non-linear material (dijk≠0) the material polarization will have a component at twice the optical frequency. From: Pi (t) = 2dijk Ej (t)Ek (t) the fields can be written# in complex form ! # ! Pi (t) = 2dijk leading to ! "j eiω1 t + E " ∗ e−iω1 t E j 2 "k eiω2 t + E " ∗ e−iω2 t E k 2 # 1 ∗ i(ω −ω )t ∗ −i(ω −ω )t i(ω +ω )t ∗ ∗ −i(ω +ω )t 1 2 1 2 "j E " e 1 2 +E " E " "j E "k e 1 2 + E " E " Pi (t) = dijk E +E k j ke j ke 2 giving !j (ω1 )E !k (ω2 ) P!i (ω1 + ω2 ) = dijk E ch 12. 4 Non-Linear dijk Coefficients The dijk tensor can be written in contracted form so that Px d11 Py = d21 d31 Pz d12 d22 d32 d13 d23 d33 d14 d24 d34 d15 d25 d35 d16 d26 d36 Ex2 Ey2 Ez2 2Ez Ey 2Ez Ex 2Ex Ey and has the same form constraints due to crystal symmetry groups as the electrooptic tensor rijk More specifically: dijk = − !ii !jj rijk 4!0 ch 12. 5 Wave Equation in a Non-Linear Medium Starting with the usual Maxwell’s equations ! " ! ∂ D ∂ ! + P! ! ×H ! = J! + ∇ = J! + #0 E ∂t ∂t ! " ∂ ! ×E ! =− ! ∇ µ0 H ∂t and writing the first of these equations in terms of the linear and non-linear polarization components ! + P!N L P! = "0 χL E where we have and ! P!N L " i = 2d!ijk Ej Ek ! " ∂ P! ∂ NL ! + ! ×H ! = σE !+ ∇ $E ∂t ∂t ∂ ! !" ! ! ∇×E =− µ0 H ∂t ch 12. 6 Wave Equation in a Non-Linear Medium which can be combined to get ! ! ∂E ∂2E ∂2 ! ∇ E = µ0 σ + µ0 $ 2 + µ0 2 PN L ∂t ∂t ∂t 2! considering the one-dimensional case of propagation in the z-direction with fields of the form ! " 1 E1i (z) ei(ω1 t−k1 z) + c.c. 2 " 1! i(ω2 t−k2 z) Ek (ω2 , z, t) = E2k (z) e + c.c. 2 " 1! i(ω3 t−k3 z) Ej (ω3 , z, t) = E3j (z) e + c.c. 2 Ei (ω1 , z, t) = c.c. stands for “complex conjugate” where i,j, and k can be either the x or y directions, and ω3=ω1+ω2. ch 12. 7 Wave Equation in a Non-Linear Medium computing the derivative with the plane-wave solutions gives at frequency ωl ! " 1 dE (z) li ∇2 Ei (ωl , z, t) = − kl2 Eli (z) + 2ikl ei(ωl t−kl z) + c.c. 2 dz for l=1,2,3 where Eli(z)=Ei(ωl) and we have neglected terms of the form d2E/dz2 because we assume the field amplitudes are varying slowly compared to the optical period, i.e. dEli d2 Eli kl ! dz dz 2 ch 12. 8 Wave Equation in a Non-Linear Medium ! The wave equation can thus be written as " ! " # $ k12 dE1i i(ω1 t−k1 z) 1 ∂2 2 i(ω1 t−k1 z) E1i + ik1 e + c.c = −iω1 µ0 σ + ω1 µ0 # E1i e + c.c − µ0 2 [PN L (z, t)]i 2 dz 2 ∂t ! which can be written using"" k12=ω12μ0ε and ω1=ω3-ω2 as ik1 " ! " j E"k P"N L " =" 2d"!ijk E i , dE1i −ik1 z iω1 σµ0 ∗ −i(k3 −k2)z e =− E1i e−ik1 z + µ0 ω12 d"ijk E3j E2k e dz 2 giving components of E(ω1), E(ω2) and E(ω3) of ! ! µ0 µ0 ! ∗ −i(k3 −k2 −k1 )z E1i − iω1 dijk E3j E2k e "1 "1 ! ! ∗ dE2k σ2 µ0 ∗ µ0 " ∗ −i(k1 −k3 +k2 )z =− E2k + iω2 dkij E1i E3j e dz 2 "2 "2 ! ! dE3j σ3 µ0 µ0 ! =− E3j − iω3 djik E1i E2k e−i(k1 +k2 −k3 )z dz 2 "3 "3 dE1i σ1 =− dz 2 ch 12. 9 Wave Equation in a Non-Linear Medium dE1i σ1 =− dz 2 ! µ0 E1i − iω1 "1 Absorption, i.e. for solution E=E0e-αz/2 we have α=σ ! µ0 # ! µ0 ! ∗ −i(k3 −k2 −k1 )z dijk E3j E2k e "1 Conversion to/from other frequencies. Whether conversion is from or to this field depends on the phase of this field relative to E2 and E3. If Δkz , i.e. (k3-k2-k1)z changes by π the conversion switches signs. ch 12.10 Second Harmonic Generation Consider case of ω1=ω2=ω3/2 and define Δk k3-(k1+k2) where Δk=0 in the absence of dispersion (i.e. dn/dλ=0). Assume the “pump” wave at ω1 is not depleted (dE1/dz=0) and the material is transparent at frequency ω3 (i.e. σ=0) and solve for dE3/dz to get dE3j σ3 =− dz 2 ! µ0 E3j − iω3 "3 dE3j = −iω dz ! ! µ0 ! djik E1i E2k e−i(k1 +k2 −k3 )z "3 µ0 ! djik E1i E1k ei∆kz " ch 12. 11 Second Harmonic Generation dE3j = −ω dz ! µ0 ! djik E1i E1k ei∆kz " giving at the end of a crystal of length L E3j (L) = −iω or ! µ0 ! ei∆kL − 1 d E1i E1k " jik i∆k E3j (L) = −2iei∆kL/2 ω ! µ0 ! sin(∆kL/2) djik E1i E1k " ∆k or for the intensity of the sum frequency component 1 !I(ω3 )" = 2 ! " ∗ E (L) E3j (L) = 2 µ0 3j ! µ0 2 " " #2 2 2 2 sin2 12 ∆kL ω dijk E1i E1k L " #2 1 " ∆kL 2 ! µ " 32 ω 2 d!2 L2 sin2 12 ∆kL 0 ijk !Ij (2ω)" = 8 !Ii (ω1 )" !Ik (ω1 )" # $2 1 " n3 ∆kL 2 ch 12. 12 Phase Matching From the expression of the intensity of the sum frequency wave ! µ " 32 ω 2 d!2 L2 sin2 12 ∆kL 0 ijk !Ij (2ω)" = 8 !Ii (ω1 )" !Ik (ω1 )" # $2 1 " n3 ∆kL 2 we can see that a long crystal benefits frequency conversion efficiency, but the length is limited by the sinc2(ΔkL/2) factor unless Δk=0. sin2 12 ∆kL !1 "2 2 ∆kL ch 12.13 Sinc2ΔkL/2 term sin2 12 ∆kL !1 "2 2 ∆kL 1 0.75 0.5 0.25 ΔkL -10! -8! -6! -4! -2! 0 2! 4! 6! 8! 10! 2 1 sin 2 2 ∆kL < I(ω ) >∝ L !1 "2 3 Since ∆kL 2 1 2π < I(ω3 ) >max ∝ L = 2 at max (∆k) ∆k Thus Δk should be minimized for maximum conversion efficiency ch 12.14 Phase Matching Physical interpretation of the Sinc2ΔkL/2 term is that if Δk≠0 the pump wave at ω and the second harmonic wave at 2ω will drift out of phase over a distance lc/2=π/Δk causing the conversion to cancel the second harmonic wave rather than augment it. In normally dispersive materials (dn/dω>0) Δk is not zero without special efforts to arrange it to be so. In typical materials, lc≈100 μm ch 12.15 Angle Phase Matching In crystals the index of refraction seen by one polarization can be tuned by adjusting the angle, for example in a uniaxial crystal 1 cos2 θ sin2 θ + = n2e (θ) n20 n2e allowing the value of Δk to be adjusted if the waves at ω1, ω2 and ω3 do not all have the same polarization state. Depending on the relative polarization states we have different “types” of phase matching Scheme Polarizations E(ω1) E(ω1) E(ω2) E(ω3) o o e I e o e II (IIA) e e III (IIB) o e e e IV o o o V e o o VI (IIB) e o VII (IIA) o e e o VIII (I) For ω1≤ω2<ω3 ch 12. 16 Angle Phase Matching 1 cos2 θ sin2 θ + = n2e (θ) n20 n2e Most common non-linear crystal are negative uniaxial and normally Scheme Polarizations dispersive (dn/dω>0) therefore E(ω1) E(ω1) E(ω2) E(ω3) requiring type I, II or III phase o o e I matching. e o e II (IIA) What types of phase matching e e III (IIB) o would be useful in a positive e e e IV uniaxial crystal with normal o o o V dispersion? e o o VI (IIB) e o VII (IIA) o e e o VIII (I) For ω1≤ω2<ω3 ch 12.17 Type I and II phase matching The most common angle phase matching is type I and II: Type I phase-matching has the sum frequency wave E(ω3) with a different polarization than the other two waves Type II phase-matching has one of either E (ω1) or E(ω2) with a different polarization state than the other two waves. ch 12.18 Type I Phase Matching Technically this is type VIII, but it is commonly referred to as type 1 since the sum frequency wave is orthogonally polarized to both pump waves Normal shells can be used as a geometric tool to determine proper phase matching angle. In a positive uniaxial crystal with normal dispersion: → k θm z-axis Normal shells for ω1=ω2 requiring Normal shells for ω3=2ω1 1 cos2 θm sin2 θm = 2 + 2 n2o (2ω) no (ω) ne (ω) neω(θm)=n02ω ch 12.19 Type I Phase Matching Normal shells can be used as a geometric tool to determine proper phase matching angle. In a negative uniaxial crystal with normal dispersion: → k θm z-axis Normal shells for ω1=ω2 requiring Normal shells for ω3 1 cos2 θm sin2 θm = 2 + 2 n2o (ω) no (2ω) ne (2ω) noω(θm)=ne2ω ch 12.20 Quasi Phase Matching If the crystal domain polarity can be engineered to flip signs every lc the polarity of the sum frequency wave being generated can flip every time the sum frequency wave drifts π out-of-phase with the driving waves. Conversion efficiency (AU) 10 +z +z +z 7.5 Phase matched Quasi-Phase matched 5 2.5 0 Not phase matched 1 2 Z/lc 3 ch 12. Engineered QPM materials Periodically Poled Lithium Niobate (PPLN) Periodically Poled Lithium Tantalate (PPLT) Orientation Patterned Gallium Arsenide (OpGaAs) Lithium niobate crystal Photoresist Conducting gel Constant current HV source 0.5–1mm 50mm Poling method for PPLN Phase contrast image of PPLN ch 12.22 Momentum Conservation Phase matching is a form of momentum conservation (k1+k2=k3) that must be satisfied along with energy conservation (ω1+ω2=ω3) in non-linear processes. If we don’t require the beams be collinear then phase matching can be achieved by crossing beams k1 k2 k1 k2 k1 k2 kg k1 k2 k3 k3 k3 k3 collinear type I phase matching collinear type II phase matching Quasi phase matching non-collinear type IV phase matching ch 12.23 Example of SHG in KDP Determine the type of phase matching to use for second harmonic generation in KDP with a fundamental wavelength of λ=694.3 nm, and determine the phase matching angle using " " ne(ω)=1.466"" " ne(2ω)=1.487 " " no(ω)=1.506"" " no(2ω)=1.534 ch 12.24 Example of SHG in KDP → k With"ne(ω)=1.466"" " ne(2ω)=1.487 " " no(ω)=1.506"" " no(2ω)=1.534 this is a negative uniaxial crystal with normal dispersion. We can use type I phase matching and require θm z-axis ne2ω(θm)=n0ω 1 cos2 θm sin2 θm = 2 + 2 n2o (ω) no (2ω) ne (2ω) ch 12.25 References Yariv & Yeh “Optical Waves in Crystals” chapter 12 ch 12.26