Second-harmonic generation

Second-harmonic generation converts an incident optical frequency $\nu$ into $2\nu$ through a material's nonlinear response. In the photon description of an ideal lossless conversion, two input photons supply one output photon:Here $h$ is the Planck constant. The relation states conservation of energy; the material mediates the interaction. It does not say that each input photon independently splits its wavelength in half.

For vacuum wavelengths, ${\lambda }_{0,\omega }=c/\nu$ and ${\lambda }_{0,2\omega }=c/(2\nu )$, where $c$ is the speed of light. HenceThe second relation uses the refractive index for each propagating mode and frequency. Within a medium with optical dispersion, the wavelength need not halve. For an invented example, ${\lambda }_{0,\omega }=800\mathrm{nm}$, $n_{\omega }=1.5$, and $n_{2\omega }=1.6$ give $400\mathrm{nm}$ in vacuum, but in the material the two wavelengths are $533.33\mathrm{nm}$ and $250\mathrm{nm}$; their ratio is $0.46875$.

In 1961, Peter Alden Franken, Alan Hill, C. Wilbur Peters and Gabriel Weinreich focused a pulsed ruby laser through a red optical filter into quartz. The filter suppressed xenon-flash background. A quartz-prism spectrograph used red-insensitive Eastman Type 103 plates. A single shot recorded a feature near $347.2\mathrm{nm}$ from $694.3\mathrm{nm}$ input. Removing the quartz or substituting glass removed the feature; changing polarization of waves and orientation followed their predicted pattern. These controls supported second-harmonic generation; photographic density gave an estimated yield.^[ref]

A spectrograph turns output frequency into a recording position. Its spectral separation makes a faint new component distinguishable from bright input light. The reported rounded wavelengths do not constitute an independent precision measurement of the ratio two. Nor do these observations demonstrate perfect phase matching or complete conversion. The experiment and Nicolaas S later theoretical account are distinct contributions to nonlinear optics.

Phase matching makes wave amplitudes emitted at different depths add coherently. Consider collinear plane waves in a uniform transparent material of length $L$, with fixed polarization of waves and nonzero selected nonlinear optical susceptibility. Assume negligible pump depletion, negligible absorption, an initially absent harmonic, and a wide beam for which diffraction is negligible. The pump's wave amplitude is then constant throughout the interaction.

The pump electric field has spatial wave phase $k_{\omega }z$; its quadratic source has spatial wave phase $2k_{\omega }z$. The freely propagating harmonic has wave number $k_{2\omega }$. Define the second-harmonic phase mismatch byFor the chosen complex-field convention, the outgoing harmonic wave amplitude, up to an overall constant and propagation phase, is proportional toChoosing the conjugate complex-field convention reverses the exponent's sign without changing the wave intensity. Taking the squared complex modulus givesHere $C$ is fixed for the chosen modes and material; its dimensions accommodate the stated wave intensity convention. The quadratic pump dependence follows because the source wave amplitude is proportional to $E_0^2$, whereas $I_{\omega }$ is proportional to $E_0^2$. The sinc function comes from summing contributions along the whole material, just as a finite aperture produces diffraction through addition of complex amplitudes.

At $\Delta k=0$, the integral is $L$ and the harmonic wave intensity grows as $L^2$. At $\Delta kL=2\pi$, all those contributions cancel. This cancellation needs no absorption: their wave phases wind through a full turn. At high conversion, the constant-pump assumption fails, so the $L^2$ law cannot continue indefinitely. Tight focusing, finite optical pulses, absorption, and transverse separation of modes also require a more complete model.

Optical dispersion generally makes $n_{2\omega }\ne n_{\omega }$. In a suitable crystal, birefringence allows modes with different polarization of waves to experience different refractive indices, making their selected values equal. The appropriate crystal direction and allowed nonlinear optical susceptibility component must both work.^[ref]

For a worked calculation, choose $L_0=1\mathrm{mm}$ and $\Delta k=\pi \mathrm{m}{\mathrm{m}}^{-1}$. At $L=L_0$, the harmonic wave intensity is $4/{\pi }^2\simeq 0.4053$ of its perfectly matched value. At $L=2L_0$ it vanishes in this model. More material can therefore reduce the output. If instead $\Delta k=0$, doubling $L$ multiplies output by four. The two curves retain that common normalization, so their different peak heights are meaningful.

The difference between the harmonic's wave number and that of the quadratic driving electric polarization. It has units of inverse length. For collinear modes, $\Delta k=2\omega (n_{2\omega }-n_{\omega })/c$, so matching frequencies alone does not ensure matching spatial wave phases.

The length over which the harmonic and its quadratic source accumulate a relative wave phase of $\pi$. For nonzero second-harmonic phase mismatch, $L_c=\pi /|\Delta k|$; the first output zero of the uniform undepleted model occurs at $2L_c$. This is a propagation mismatch length, distinct from the pump's optical coherence length. It diverges as perfect phase matching is approached.