Lecture 10: Non-local response Petr Kužel Nonlocal response: • in time (frequency dispersion) ! ! Fourier transform Causality, Kramers-Kronig relations • in space (spatial dispersion) ! Optical activity phenomenological description connection to the spatial dispersion Consecutive relations In the first lecture we have discussed the consecutive relations: D = εE = ε 0 E + P P = ε 0 χE B = µH = µ 0 H + M It is valid only if • The electromagnetic wave is monochromatic • The material shows no dispersion within spectrum of the wave • The field vectors represent the spectral components of the wave: D(ω) = ε(ω) E (ω) P (ω) = ε 0 χ(ω) E (ω) " Response non-local in time Let us study the meaning of these relations in the time domain: D(t ) = ~ε (t ) = ∞ ∫ D(ω) e −∞ ∞ ∫ ε(ω) e −∞ iω t iωt ∞ iω t ( ) ( ) e dω ε ω ω E ∫ dω = −∞ # Fourier transform dω ∞ 1 ~ −iωt ( ) t e dt ε(ω) = ε ∫ 2π − ∞ The time-domain consecutive relation is a convolution of the field with the response function: ∞ ∞ ∞ ∞ 1 ~ε (t ′)e −iω(t′−t ) dt ′ = 1 ~ε (t ′) dω E (ω)e −iω(t′−t ) = ′ ω ω ( ) D(t ) = E d d t ∫ ∫ ∫ 2π −∫∞ 2 π −∞ −∞ −∞ ∞ 1 dt ′~ε (t ′) E (t − t ′) = ∫ 2π − ∞ $ Fourier transform: definitions The Fourier pairs of functions can have several possible definitions: 1. The natural conjugated variables are ν and t: 2. In optics we think usually in terms of the angular frequency ω = 2πν: 3. In order to work with the spectral density in ω, we substitute: F''(ω) = F'(ω) /2π: F (ν ) = ∞ ∫ f (t )e − 2 πiνt dt −∞ F ′(ω) = ∞ f (t ) = 2 πiνt ( ) F e dν ν ∫ −∞ ∞ ∫ f (t )e − iω t ∞ dt −∞ ∞ 1 − iω t ( ) F ′′(ω) = f t e dt ∫ 2π − ∞ 1 iω t ′ ( ) f (t ) = F e dω ω 2π −∫∞ f (t ) = ∞ iω t ′ ′ ( ) F e dω ω ∫ −∞ Properties of Fourier transform Properties of FT function Fourier transform Definition 1 Definition 2 Definition 3 f ∗g F (ν ) ⋅ G(ν ) F ′(ω) ⋅ G ′(ω) 2π F ′′(ω) ⋅ G ′′(ω) f ⋅g F ∗ G (ν ) F ′′ ∗ G ′′ (ω) df dt 2πiνF (ν ) 1 F ′ ∗ G ′ (ω) 2π iωF ′(ω) δ(t0) e−2πiνt0 e−iωt0 e−iωt0/2π e −αt 2 vp 1/t sign t π e α − π 2ν 2 α − πi sign(ν ) − 1 i vp π ν iωF ′′(ω) ω2 π i 4α e α − πi sign(ω) − 2i vp 1 ω 1 e 4πα − − ν2 4α i sign(ω) 2 − 1 i vp π ω Fourier pair vp(1/t) — sign(ω) ∞ e −2 π i ν t 1 FT vp = vp ∫ dt = ! t t −∞ For ν > 0 the following contour is used: ∞ e −2 πiνt vp ∫ dt t −∞ e − 2 πiνt = − πi Res t =0 t Im(t) 0 = − πi For ν < 0 a similar contour with Im(t) > 0 is used. One finds the result: πi 1 FT vp = −πi sign (ν ) t Re(t) Causality ∞ 1 dt ′~ε (t ′) E (t − t ′) D(t ) = ∫ 2π − ∞ In a dispersive material D(t0) depends, in principle, on E(t ≤ t0), i.e. on all the previous values of the electric field. D and P express the reaction of the matter to the applied field and should not depend on the future values of E: ∞ 1 dt ′~ε (t ′) E (t − t ′) D(t ) = ∫ 2π 0 The above relations are equivalent if ε(t < 0) = 0: this relation will then automatically ensure the causality. Causality: continued Let us define: lim ε(ω) = ε ∞ ω→∞ ~ε (t ) = 1 ∞ iω t ( ( ) ) e dω ε ω − ε ∞ ∫ −∞ Then we can decompose the time response into 2 parts: ~ε (t ) = ~ε (t ) + 2πε δ(0 ) 1 ∞ The causality condition is then fulfilled just when ~ε (t ) = ~ε (t ) sign (t ) 1 1 Finally: ~ε (t ) = ~ε (t ) sign (t ) + 2πε δ(0) 1 ∞ This is a general form of the response function which obeys the causality relation Kramers-Kronig relations The time-domain form of the response function ~ε (t ) = ~ε (t ) sign (t ) + 2πε δ(0) 1 ∞ Leads to the Kramers-Kronig relations in the frequency domain: i 1 ε(ω) − ε ∞ i ε(ω0 ) = (ε(ω) − ε ∞ )∗ − vp + ε ∞ = − vp ∫ dω + ε ∞ = π ω π ω − ω 0 −∞ ∞ i ε(ω) dω = ε ∞ − vp ∫ π −∞ ω0 − ω ∞ 1 ε′′(ω)dω ε′(ω0 ) = ε ∞ − vp ∫ π −∞ ω0 − ω ∞ 1 ε′(ω)dω ε′′(ω0 ) = vp ∫ π − ∞ ω0 − ω ∞ 1 κ(ω)dω n(ω0 ) = 1 − vp ∫ π − ∞ ω0 − ω ∞ 1 n(ω)dω κ(ω0 ) = vp ∫ π −∞ ω0 − ω ∞ Note Which other physical phenomena are connected to vp — sign transformation? Mathematicians thought useful to introduce so called Hilbert transformation which is closely related to that: i 1 H ( y ) = y ∗ vp π x E(t), e(ν) is an electric field Fourier pair of an arbitrary waveform ∞ e(ν ) = ∫ E (t )exp(− 2πiνt )dt −∞ Frequency components e(ν) within the pulse bandwidth acquire a constant phase change θ [strictly speaking: θ × sign(ν) because e(−ν) = e*(ν)] E ′(t ) = ∞ ∫ e(v )exp(iθsign(ν))exp(2πiνt )dν −∞ Note: continued It means in the time domain: sin θ 1 E ′(t ) = E (t )∗ cos θ δ(t ) − vp t π In particular, for θ=π/2: E ′(t ) = − E (t ) 1 ∗ vp t π Monochromatic wave [cos(t) becomes sin(t)]: Half-cycle or single-cycle pulse: Optical activity: description of the phenomenon Experimental fact: rotation of the polarization plane in some materials (quartz). This rotation can be right- or left-handed. Angle of the rotation is proportional to the length of the sample: a specific rotation angle (per unit length) can be defined Direction of the rotation is related to the propagation direction: the total rotation for a propagation back and forth is zero. Phenomenologically, it can be described as a circular birefringence Eigenmodes: R ei (ωt −k0 z nR ) L ei (ωt − k0 z nL ) R and L are the Jones vectors for the right and left circular polarizations Optical activity: continued At z = 0 (input face of the sample) the polarization of the beam is linear: 1 1 A iω t A e (R + L) = eiωt + = A eiωt 2 2 i − i 1 0 At z = d (output face of the sample) the polarization writes: ( ) A iωt e R e −ik0d nR + L e −ik0d nL = 2 cos β = A eiωt −ik0d (nR + nL ) 2 sin β It is a linear polarization in the direction given by the angle β: β = k0 d nR − nL d = π (nR − nL ) 2 λ Quartz at 546 nm: ne − no = 0.009, |nR − nL| = 8×10−5. Response non-local in space An electric field in one place can produce a polarization in the near vicinity D(r ) = 1 ~ε (r ′) E (r − r ′)dr ′ 3 ∫∫∫ (2π) ε χ(r ′) E (r − r ′)dr ′ P (r ) = 0 3 ∫∫∫ ~ (2π) The above response functions take the form of a Dirac δ in the local response approximation In the reciprocal space the following relations are obtained D (ω, k ) = ε(ω, k ) E (ω, k ) P (ω, k ) = ε 0 χ(ω, k ) E (ω, k ) Dependence on k (namely on its direction): spatial dispersion In the following we will search for the consequences of the spatial dispersion Spatial dispersion We take a first-order Taylor development of ε(k): the linear term does not vanish in the non-centrosymmetric materials ε ij (k ) = εij0 3 + ε 0 ∑ γ ijl kl l =1 γijl is a 3rd-rank tensor. Its intrinsic symmetry properties can be derived from those of the dielectric constant: ε ij = ε∗ji γ ijl = iδijl γ iil = 0 δijl = −δ jil and ε ij (k ) = ε∗ij (− k ) (γijl is imaginary, δijl is real) An antisymmetric tensor gij can be defined: g ij = δijl kl Spatial dispersion: continued 0 g = − g12 − g 13 g ij = δijl kl g12 0 − g 23 g13 g 23 0 One can also introduce the gyration vector: G = (g 23 − g13 g12 ) The electric induction is then equal to: Di = ε ij0 E j + iε 0 g ij E j D = εE + iε 0G ∧ E Note: the tensor g is not characteristic for a medium, it is given for the medium and a specific wave vector. I.e. if we apply a symmetry operation (like a rotation or a mirror) on the tensor g the crystal sample turns consequently but the radiation wave vector turns as well! Light waves in non-local media We have to solve the wave equation: s(s ⋅ E ) − E + 1 ε ⋅E =0 2 r n ( or k (k ⋅ E ) − k 2 E + ω2µ 0 ε ⋅ E = 0 ) where the dielectric constant εr is replaced by: ε 0xx ε = − ig12 − ig13 ig12 ε 0yy − ig 23 ig13 ig 23 ε 0zz Let us study the case of the quartz (uniaxial crystal) which allows to discuss the most important features. The quartz has only two independent components of the 3rd-rank tensor δ. δ123 = −δ213; δ231 = δ312 = −δ321 = −δ132 Propagation // optic axis (//z) g13 = δ123 k, g13 = 0, g23 = 0 we define: ∆ 3 = g12 c 2 ω2 Wave equation: no2 − n 2 − i∆ 3 0 i∆ 3 no2 − n 2 0 0 Ex 0 Ey = 0 ne2 E z Eigenvalues (effective refractive index): nI , II ≈ no ± ∆3 2no Eigenvectors (polarization of the waves): 1 − i , 0 1 i 0 Propagation ⊥ optic axis (//x) g23 = δ231 k, g13 = 0, g12 = 0 we define: ∆1 = g 23 c 2 ω2 Wave equation: no2 0 0 0 no2 − n 2 − i∆1 Ex i∆1 E y = 0 ne2 − n 2 E z 0 As the birefringence is usually larger than the optical activity, we can assume: no2 − ne2 >> ∆1 Propagation ⊥ optic axis (//x): continued Wave equation: no2 0 0 0 no2 − n 2 − i∆1 Ex i∆1 E y = 0 ne2 − n 2 E z 0 Eigenvalues: nI ≈ no + ∆1 ∆1 2no no2 − ne2 nII ≈ ne − ∆1 ∆1 2ne no2 − ne2 Eigenvectors: 0 1 , − i∆1 n2 − n2 e o 0 ∆ i 1 2 2 no − ne 1
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