advanced28 min studyLesson 228 in Physics

Nonlinear polarization creates new optical frequencies

Expand a material response, track real-field amplitude conventions, and derive a second harmonic.

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What you’ll understand

  • Distinguish nonlinear polarization density from optical polarization direction.
  • Derive the DC and second-harmonic terms of a quadratic response.
  • Apply inversion symmetry with its electric-dipole scope.

A linear material responds at the frequencies already present in the applied field. A nonlinear response multiplies field components, so sums and differences of their frequencies appear in the induced polarization. That polarization acts as a source for additional electromagnetic waves. The algebra identifies possible source frequencies, while symmetry and propagation decide which are appreciable. We will keep the real-field amplitude convention explicit to avoid a common factor-of-two error in second-harmonic calculations.

The response expansion is a model with units

Polarization density is electric dipole moment per volume, measured in coulombs per square metre. It is distinct from the direction or ellipse called the polarization of a light beam. In a weakly nonlinear instantaneous scalar model, expand this density in powers of the local electric field. The linear susceptibility is dimensionless, the quadratic susceptibility has units metres per volt, and each higher order supplies another inverse field factor. The expansion is useful only while omitted terms remain sufficiently small.

Real optical materials have memory, dispersion, and vector response. More generally the quadratic susceptibility is a tensor with an output index and two input indices, and it depends on the participating frequencies. A scalar coefficient represents a specified projection for a chosen geometry and polarization. Near resonances or for broad pulses, one must use the frequency-dependent response or a time-domain convolution rather than assume one instantaneous constant describes every frequency component.

P(t)=ϵ0 ⁣[χ(1)E(t)+χ(2)E2(t)+χ(3)E3(t)+⋯ ]P(t)=\epsilon_0\!\left[\chi^{(1)}E(t)+\chi^{(2)}E^2(t)+\chi^{(3)}E^3(t)+\cdots\right]
P is polarization density in C/m², E is the real electric field in V/m, and ε₀ is vacuum permittivity in F/m. This displayed scalar polynomial assumes an instantaneous weak-field response for the selected components.↔ Scroll wide equations horizontally.

A square generates zero and doubled frequencies

Choose the real driving field E(t)=E₀ cos(ωt), where E₀ is its peak amplitude. Squaring the cosine gives one half plus one half cosine of twice the angular frequency. The quadratic polarization therefore contains a constant optical-rectification term and a source oscillating at the second harmonic. Its peak second-harmonic polarization amplitude is ε₀χ⁽²⁾E₀²/2, with χ⁽²⁾ here meaning the second-order susceptibility, not the square of the linear one.

For two real driving tones, the cross product of their cosines produces both sum and difference frequencies. Their separate squares also produce doubled frequencies and DC. The relative coefficients depend on whether one uses real peak fields or complex positive-frequency amplitudes; switching conventions midway changes apparent factors of two. Most importantly, identifying a nonlinear source does not calculate the outgoing optical power. Boundary conditions, absorption, phase matching, and any pump depletion still have to be considered.

P(2)(t)=ϵ0χ(2)E022[1+cos⁡(2ωt)],2cos⁡(ω1t)cos⁡(ω2t)=cos⁡((ω1+ω2)t)+cos⁡((ω1−ω2)t)P^{(2)}(t)=\frac{\epsilon_0\chi^{(2)}E_0^2}{2}\left[1+\cos(2\omega t)\right],\qquad 2\cos(\omega_1t)\cos(\omega_2t)=\cos((\omega_1+\omega_2)t)+\cos((\omega_1-\omega_2)t)
E₀ is a real peak field in V/m; ω,ω₁,ω₂ are angular frequencies in rad/s. The superscript (2) labels response order and is not an exponent applied to χ.↔ Scroll wide equations horizontally.

Symmetry can forbid the bulk quadratic term

In a centrosymmetric bulk material under the local electric-dipole approximation, reversing every electric-field component reverses the induced polarization: P(−E)=−P(E). Even powers do not change sign under that operation. Their coefficients must therefore vanish in this bulk response expansion, including every second-order tensor component. Third-order effects remain possible. The argument is a symmetry constraint on this constitutive response, not a claim that all nonlinear optical phenomena vanish in an inversion-symmetric material.

Surfaces, interfaces, applied static fields, magnetic-dipole or electric-quadrupole effects, and broken structural symmetry can change the scope of that conclusion. State those mechanisms explicitly rather than declaring an observed second harmonic impossible. The function lab can isolate quadratic scaling: Reset and set both controls to coefficient one and position one, predicting output one. Reset again and set coefficient one and position two, predicting output four. Its curve y=ax² is dimensionless here; it does not contain an optical carrier, a susceptibility tensor, or emitted radiation.

Compute a quadratic source amplitude

In the stated scalar real-field model, χ⁽²⁾=2.0×10⁻¹² m/V, χ⁽¹⁾=1, and E₀=1.0×10⁶ V/m. Use ε₀=8.85×10⁻¹² F/m. Find the second-harmonic peak polarization and its ratio to the linear fundamental peak.

  1. Square the peak field to obtain 1.0×10¹² V²/m². Multiplying by χ⁽²⁾ gives 2.0 V/m, and the cosine-square identity contributes the factor one half.

  2. The second-harmonic peak polarization is therefore ε₀ times 1.0 V/m, or 8.85×10⁻¹² C/m². The DC term has the same coefficient in this instantaneous example.

  3. The linear fundamental peak is ε₀χ⁽¹⁾E₀=8.85×10⁻⁶ C/m². Dividing gives a source-amplitude ratio of 10⁻⁶, consistent with treating the quadratic correction as weak at this field.

The result

The second-harmonic polarization peak is 8.85×10⁻¹² C/m², one millionth of the linear peak; this is a polarization ratio, not an emitted-power ratio.

Explore the model

Interactive lab

Interactive lab · function

Test quadratic response scaling

Reset and set BOTH controls to coefficient a=1 and position x=1; predict y=1. Reset and set a=1 and x=2; predict y=4. This dimensionless parabola tests scaling, with no optical frequency or material tensor.

Test quadratic response scalingThis lab uses only y = ax². Playback traces the curve within the fixed integration interval from 0 to x; it does not estimate numerical error or change the chosen point. Current readings: y at chosen x: 0.608; Tangent slope · 2ax: 1.35; Signed area · ax³/3: 0.182. All parameters are adjustable with the labeled controls below.−2.4−1.201.22.4−9−4.504.59xy(x, ax²)
y = ax²TangentSigned integral
y at chosen x
0.608
Tangent slope · 2ax
1.35
Signed area · ax³/3
0.182
t = 0 s

This lab uses only y = ax². Playback traces the curve within the fixed integration interval from 0 to x; it does not estimate numerical error or change the chosen point. Parameter changes pause playback and recompute the model at the current elapsed time. Reset restores both parameters and returns time to zero. Playback starts paused. Adjust either parameter, then choose Play or Step.

Look forDoubling a real field quadruples its quadratic source term while only doubling a linear term.

Check your understanding

What follows from bulk inversion symmetry within the local electric-dipole constitutive approximation?

Try it yourself

Two real input tones have ordinary frequencies 200 THz and 300 THz. List the nonnegative frequencies present in the quadratic polarization, assuming its effective coefficient is nonzero. Does this list alone guarantee efficient radiation at each frequency?

Take a moment to make a prediction or work it out on paper. Open a hint when you need one.

Give me a hint

Include each tone squared as well as the cross product; ordinary frequencies add just as angular frequencies do.

Compare with the solution

The separate squares give DC, 400 THz, and 600 THz. The cross product gives 500 THz and 100 THz. Thus the list is 0,100,400,500,600 THz. It identifies source terms only. Tensor selection, phase mismatch, absorption, and collection geometry can suppress outgoing signals even when a source term is allowed.

Take it with you

  • Multiplication of fields produces sum and difference frequencies.
  • Real peak amplitudes fix the numerical factors in harmonic sources.
  • Bulk electric-dipole inversion symmetry excludes χ⁽²⁾ while leaving other mechanisms possible.

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