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For bulk electric-dipole second-harmonic generation, the crystal must lack inversion symmetry and have a nonzero relevant component of its second-order nonlinear optical susceptibility. It should transmit both pump and harmonic, tolerate the required intensity, and allow phase matching by suitable birefringence or another phase-compensation mechanism. A large nonlinear coefficient, low optical loss and good optical quality are desirable. Noncentrosymmetry permits a response but does not guarantee one in every chosen geometry.

In the undepleted plane wave limit, contributions from successive layers give a harmonic amplitude proportional to ${\int }_0^L{e}^{i\Delta kz}dz$, where $\Delta k=k_{2\omega }-2k_{\omega }$. HenceTune orientation, temperature and pump polarization to maximize the nonlinear coupling and cancel phase mismatch. For continuous operation, an impedance-matched enhancement optical resonator, or intracavity doubling, raises the circulating intensity. Focus the Gaussian beam to balance intensity against diffraction and spatial walk-off; arbitrarily tight focusing shortens the useful overlap. Antireflection surfaces, stable resonance locking and efficient heat removal reduce avoidable loss and drift.

Type-I phase matching requires $n_{e,2\omega }(\theta )=n_{o,\omega }$, because both pump photons are ordinary and the harmonic is extraordinary. Apply the direction-dependent index equation to the harmonic, not to the pump. Solving givesFor the ruby-laser data this is $0.626210$, whereas the shorter-wavelength data give $0.958873$. ThereforeThe second calculation uses the supplied $257\mathrm{nm}$ indices as rounded harmonic data: the exact half-wavelength of $515\mathrm{nm}$ is $257.5\mathrm{nm}$. The index dispersion between those two ultraviolet values was not supplied.

For an extraordinary wave, its Poynting vector makes an angle ${\theta }_S$ with the optic axis satisfying $\tan {\theta }_S=(n_o^2/n_e^2)\tan \theta$. Thus the spatial walk-off angle relative to the wave vector isBoth angles refer to the harmonic. The ordinary pump does not have this angular walk-off. For beam radius $w_b$, the approximate overlap length is $w_b/\tan \rho$, so the shorter-wavelength geometry has about $2.19$ times the walk-off-limited interaction length.^[ref]

To compare coupling, take propagation azimuth $\phi$ and ordinary unit polarization $(-\sin \phi ,\cos \phi ,0)$. Its quadratic source is $P_z=-{ϵ}_0{d}_{36}{E}_0^2\sin 2\phi$. Projection onto an extraordinary displacement direction with $z$ component proportional to $\sin \theta$ gives $|d_{\mathrm{eff}}|\propto |d_{36}\sin \theta \sin 2\phi |$, up to the small anisotropic normalization correction. The optimal azimuth is $45^{\circ }$. At equal beam area, interaction length, input power and approximately equal nonlinear coefficients, the shorter pump has both stronger angular coupling and the favorable frequency-squared factor:Here $\eta =P_{2\omega }/P_{\omega }$ in the small-conversion, equal-area model, with harmonic index phase-matched to the pump. Its smaller spatial walk-off further favors the $515\mathrm{nm}$ pump in a walk-off-limited geometry. Equal input power alone does not determine an absolute efficiency ranking: ultraviolet absorption, wavelength-dependent $d_{36}$, beam size, crystal length and coatings are unspecified. For example, a sufficiently strongly absorbing $257.5\mathrm{nm}$ output can reverse the ideal ranking. The stated preference is conditional on comparable transparent crystals and comparable focusing, not a prediction independent of those parameters.

A crystal needs a nonzero effective second-order nonlinear optical susceptibility for the chosen polarizations. In the bulk electric-dipole approximation, centrosymmetry forbids this response. Transparency at the relevant frequencies and phase matching over the interaction length permit efficient buildup. Nonzero local generation can occur without exact phase matching, but contributions then tend to cancel as they propagate.

Write ${\psi }_j=k_{j}z-{\omega }_{j}t+{\varphi }_j$. Expanding the square and using the product-to-sum identity givesThese are respectively optical rectification, the two second-harmonic generation terms, sum-frequency generation and difference-frequency generation. Their phases and wavevectors are the corresponding sums or differences, not independently adjustable quantities.

For a vector field, $P_i^{(2)}=2{ϵ}_0{\sum }_{jk}{d}_{ijk}{E}_j{E}_k$. In the stated single-frequency amplitude convention, $E_j=(A_j{e}^{i\psi }+A_j^{\ast }{e}^{-i\psi })/2$. If $P_i^{(2\omega )}=[{\mathcal{P}}_i{e}^{2i\psi }+{\mathcal{P}}_i^{\ast }{e}^{-2i\psi }]/2$, comparison givesFor a real instantaneous tensor the zero-frequency contribution is $P_i^{(0)}={ϵ}_0{\sum }_{jk}{d}_{ijk}\mathrm{Re}(A_j{A}_k^{\ast })$. In a dispersive treatment, the tensors must carry their respective input and output frequency arguments.

The identical input-frequency pair is symmetric under $j\leftrightarrow k$, allowing contracted nonlinear susceptibility notation: replace the six pairs $xx,yy,zz,yz,zx,xy$ by $J=1,\dots ,6$. ThusThis contraction of a symmetric pair does not turn the physical susceptibility into a rank-two tensor. The factors of two account for both off-diagonal input orderings, and the prefactor follows from the question's explicit $1/2$ field convention.

For the proposed type-I process, energy conservation requires ${\omega }_1={\omega }_2+{\omega }_3$. HenceThe extraordinary pump and two ordinary output waves can be collinearly phase matched ifPut $n_{\ast }={\lambda }_{1}S$. Substituting the supplied angular extraordinary index and solving for ${\sin }^2\theta$ yieldsThe required index $n_{\ast }\simeq 2.2143$ lies between $2.1782$ and $2.2579$, so a real angle exists. Using the rounded 2922 nm wavelength in the supplied data gives $\theta \simeq 46.94^{\circ }$; retaining the energy-conserving 2922.25 nm value gives about $46.98^{\circ }$. Their common meaningful scale is about 47 degrees.

The spatial walk-off angle is the angle between the extraordinary wave's Poynting vector and its wavevector. For an optic-axis angle $\theta$, the extraordinary dispersion surface givesHere the indices are those of the 780 nm pump. Since this is a negative uniaxial crystal, its energy flow is farther from the optic axis than its wavevector. The ordinary waves' energy flows follow their wavevectors. The pump therefore drifts out of spatial overlap by roughly $L\tan \rho \simeq 0.0357L$, about $36\mu \mathrm{m}$ over a millimetre. This limits the useful nonlinear interaction length even when phase matching is exact.

The process is sum-frequency generation, with ${\omega }_3={\omega }_1+{\omega }_2$. The same reversible three-wave mixing interaction permits the reverse conversion when the higher-frequency field supplies the pump. The second-order nonlinear polarization couples the three waves; its effective coefficient includes the crystal orientation and polarizations.

One efficiency limit is phase mismatch: contributions generated at different positions acquire different phases and can cancel. A second practical limit is spatial walk-off, which reduces the overlap of finite beams in a birefringent crystal. A beam radius $w$ and relative walk-off angle $\rho$ give an overlap length of order $w/|\tan \rho |$. Absorption and scattering provide further losses. Group-velocity mismatch matters for pulses, and pump depletion eventually invalidates an undepleted-pump calculation; none of these effects should be silently included in the ideal lossless plane-wave equations.

Define ${\kappa }_j=2d_{\mathrm{eff}}{\omega }_j/(n_{j}c)$ and hold $A_1,A_2$ constant. Direct integration of the driven equation giveswhere $\mathrm{sinc}x=\sin x/x$. The second expression has a continuous phase-matched limit. If the generated field is initially absent,For $\Delta k\ne 0$ this is proportional to ${\sin }^2(\Delta kz/2)$: the first maximum is at the nonlinear optical coherence length ${\ell }_c=\pi /|\Delta k|$, and the first subsequent zero is at $2{\ell }_c$. A seed $A_3(0)\ne 0$ adds interference with the generated amplitude and can change that pattern. At exact phase matching, the unseeded result grows as $z^2$ only while pump depletion remains negligible.

To retain depletion consistently, differentiate each intensity before inserting the coupled equations:For real $d_{\mathrm{eff}}$ in the lossless convention, put $Q=A_1{A}_2{A}_3^{\ast }{e}^{i\Delta kz}$. The result isThe signs follow the printed amplitude equations. In initial up-conversion, the newly generated $A_3$ makes $\mathrm{Im}Q<0$, so the two input intensities decrease while the sum-frequency intensity increases. Adding the derivatives gives zero because ${\omega }_1+{\omega }_2-{\omega }_3=0$. The total intensity is conserved, even though the three individual intensities change.

The Manley-Rowe relations areDividing an intensity by $\hslash {\omega }_j$ gives photon flux density. A conversion event removes one photon from each lower-frequency mode and adds one to the upper mode, or does the reverse. Therefore $C_1/\hslash$ and $C_2/\hslash$ count conserved sums of photon fluxes, while $C_3/\hslash$ counts the conserved lower-frequency difference. They are not three independent invariants: $C_3=C_2-C_1$. Energy conservation is also recovered as $I={\omega }_1{C}_2+{\omega }_2{C}_1$.

The unweighted combinations generally fail because the exchanged photons have different energies. Explicitly,The qualification “generally” matters: $D_3$ is conserved for equal lower frequencies in a distinct-mode degenerate case, and every derivative vanishes when there is no exchange. The equations establish nonconservation for generic unequal-frequency interaction, not for all special solutions.

In a homogeneous lossless dielectric, let $\mathbf{D}=\mathbf{\epsilon }\mathbf{E}$ with a real symmetric permittivity tensor, and $\mathbf{B}=\mu \mathbf{H}$ with scalar positive magnetic permeability. A source-free plane electromagnetic wave with angular frequency $\omega \ne 0$, real wavevector $\mathbf{k}$ and electric field amplitude $\mathbf{e}$ satisfiesThe second equation follows from Gauss's law. It makes the electric displacement field transverse; the electric field itself need not be transverse in an anisotropic medium.

If $\mathbf{e}$ is an eigenvector of the permittivity tensor with nonzero eigenvalue ${\epsilon }_e$, then ${\epsilon }_e\mathbf{k}\cdot \mathbf{e}=0$, so $\mathbf{e}\perp \mathbf{k}$. The first equation reduces to the dispersion relation $|\mathbf{k}{|}^2={\omega }^2\mu {\epsilon }_e$. For a propagating solution the time-averaged Poynting vector is $⟨\mathbf{S}⟩=|\mathbf{e}{|}^2\mathbf{k}/(2\omega \mu )$ and is parallel to the wavevector.

A general anisotropic eigenmode need not have its electric field along a principal dielectric direction. Its energy flux can then depart from the wavevector, producing spatial walk-off. The nonzero-${\epsilon }_e$ assumption matters: at a zero permittivity eigenvalue, Gauss's law alone no longer forces $\mathbf{k}\cdot \mathbf{e}=0$.^[ref]

The self-gated second-harmonic spectrogram has the displayed ideal form. Its delay marginal is proportional to the intensity autocorrelation by the Parseval identity. Absolute time and wave phase are undetermined; $A(t)$ and $A^{\ast }(-t)$ also give the same record. Finite crystal acceptance and spatial walk-off modify the ideal gate.

The daughter photons occupy orthogonal ordinary and extraordinary polarization classes. Alternative assignments to two collected paths can interfere if timing, spectrum and spatial mode do not distinguish them. spatial walk-off and unequal group delays often require compensation.