Nonlinear Quantum Optics
Nonlinear quantum optics uses intensity-dependent or wave-mixing responses to transform quantum states of electromagnetic modes. The material response may be described macroscopically by susceptibilities, but the predictions of interest are quantum:
- vacuum fluctuations are amplified into photons;
- photons are created in correlated pairs;
- one frequency mode is coherently converted into another;
- one quadrature is squeezed while its conjugate is anti-squeezed;
- photon number produces a state-dependent phase;
- multimode dispersion determines heralded purity and entanglement.
A useful calculation proceeds from material response to a mode-overlap integral, an effective Hamiltonian, and finally a measured output state. A large susceptibility alone does not guarantee useful quantum light: phase matching, pump noise, loss, and the collected modes also matter.
Required background. Quantized modes supplies field normalization, coherent light the pump approximation, photon-number states the creation operators, and dynamic polarizability the frequency-dependent material response. Detailed pair-source states are developed in parametric down-conversion.
Nonlinear Polarization
Section titled “Nonlinear Polarization”Local polynomial shorthand
Section titled “Local polynomial shorthand”For a weak enough field and a medium with a regular perturbative response, the induced polarization can be expanded as
with repeated Cartesian indices summed. In SI units, has units of and has units of .
This compact equation suppresses frequency arguments and memory. A real material is generally dispersive, so the response is a time convolution. For example, the second-order frequency-domain polarization has the structure
up to Fourier-transform normalization. The delta function expresses time translation invariance of a stationary medium. A finite pump pulse broadens the field spectra, not this delta constraint. Modulating the medium itself breaks time-translation invariance and can supply additional frequencies.
The susceptibility is a tensor with polarization selection rules, intrinsic permutation symmetries, resonant denominators, and generally complex frequency dependence. Its imaginary part is tied to absorption and dissipation; a purely Hermitian few-mode Hamiltonian is then incomplete without corresponding reservoir noise.
Inversion symmetry
Section titled “Inversion symmetry”Under spatial inversion in an electric-dipole bulk medium,
If the material is centrosymmetric, a term quadratic in cannot respect this relation, so the bulk electric-dipole vanishes. Third-order response is allowed. This rule does not forbid
- surface or interface second-order response;
- electric-quadrupole or magnetic-dipole contributions;
- a response induced by a static bias field;
- effective behavior in deliberately asymmetric structures.
Crystal point-group symmetry further determines which tensor components survive. Stating only “the material has ” is insufficient; the propagation direction, polarizations, and contracted tensor element must be specified.
Perturbative does not mean quantum
Section titled “Perturbative does not mean quantum”The susceptibility expansion is a constitutive description. It becomes quantum optical only after the participating field modes are quantized or coupled consistently to quantum reservoirs. A classical nonlinear wave equation can predict frequency conversion and gain, but it cannot by itself predict vacuum-seeded pair production, commutator-preserving amplifier noise, heralded states, or photon correlations.
From Susceptibility to a Mode Hamiltonian
Section titled “From Susceptibility to a Mode Hamiltonian”Start with consistently normalized linear modes and derive the nonlinear energy in canonical field variables. In a dielectric, treating the full electric field as a linear combination of bosonic operators can give wrong couplings; the electric displacement is a natural canonical variable (Quesada and Sipe). Perturbative mode projection and selection of slowly rotating operator products then produce an effective Hamiltonian. Its coupling constants contain
- the relevant tensor contraction of ;
- the vacuum field per quantum of every quantized mode;
- the classical amplitude of any undepleted pump;
- a spatial overlap integral;
- temporal and spectral overlap;
- phase-matching factors;
- convention-dependent numerical and permutation factors.
For three-wave mixing, a representative overlap is
Here the mode normalizations are part of the definition of . Comparing coupling constants from two papers without comparing those normalizations is unsafe.
In a dispersive or absorptive medium, deriving the Hamiltonian by naively writing can miss energy-density, normalization, and reservoir terms. Effective couplings should be derived within a declared mode normalization or inferred from a calibrated classical conversion process with the same geometry.
Three-Wave Mixing and χ²
Section titled “Three-Wave Mixing and χ²”Trilinear interaction
Section titled “Trilinear interaction”For pump, signal, and idler modes satisfying , a convenient phase convention is
The first term annihilates one pump quantum and creates one signal and one idler quantum. The Hermitian-conjugate term recombines signal and idler into the pump. The interaction conserves the Manley–Rowe combinations
These are mode-counting invariants of the ideal closed interaction, not statements that each occupation is separately fixed.
One susceptibility, several processes
Section titled “One susceptibility, several processes”Which process is named depends on the chosen frequencies, inputs, and output:
- Second-harmonic generation: two quanta near combine into one near .
- Sum-frequency generation: inputs at and produce .
- Difference-frequency generation: inputs at and generate . Replacing the highest-frequency mode by a pump gives pair amplification of the two lower modes; replacing one lower-frequency mode by a pump instead gives number-conserving conversion between the other two.
- Parametric amplification: a seeded signal is amplified while an idler is generated.
- Spontaneous parametric down-conversion: vacuum fluctuations seed signal-idler pair creation.
These are not unrelated effects. They are different operating points, rotating-wave terms, and boundary conditions of the same nonlinear response.
Energy and longitudinal mismatch for pair generation in a collinear model; arrows identify modes, rather than their physical angles. A reciprocal vector is available only when the relevant coupling or structure is modulated. After replacing the strong pump mode or modes by classical amplitudes, both processes can reduce to the same two-mode squeezing Hamiltonian, but their pump scaling, selection rules, parasitic processes, and phase-matching conditions differ.
Energy and Momentum Matching
Section titled “Energy and Momentum Matching”Longitudinal phase accumulation
Section titled “Longitudinal phase accumulation”Energy matching prevents rapid temporal phase winding. Spatial mode overlap must also add coherently along the device. For uniform collinear three-wave mixing, define
where for ordinary phase matching and is a reciprocal poling vector for quasi-phase matching. The longitudinal amplitude contains
where . The generated intensity or pair probability therefore carries
At exact phase matching, amplitudes from the full length add in phase. The central acceptance range narrows as in mismatch. At fixed nonzero , the generated intensity oscillates with length and is bounded by times the other coupling factors.
How phase matching is engineered
Section titled “How phase matching is engineered”Common strategies include
- birefringent phase matching;
- periodic poling and higher-order quasi-phase matching;
- waveguide dispersion and transverse-mode engineering;
- cavity resonance matching;
- noncollinear geometry;
- temperature, strain, or electric-field tuning.
The vector equation also enforces transverse momentum or spatial-mode correlations. In a focused beam or a waveguide, replacing every mode by one plane-wave vector is an approximation; the full overlap integral is the reliable object.
Pump bandwidth and group velocity
Section titled “Pump bandwidth and group velocity”For pulsed operation, the pump envelope constrains while the phase-matching function constrains a different combination of frequencies. Group-velocity mismatch tilts and narrows these constraints. Their product determines the joint spectral amplitude of a pair source.
Energy matching alone therefore does not determine the state. Two sources with the same central frequencies and brightness may have very different spectral entanglement, heralded purity, timing correlations, and collection efficiency.
Parametric Amplification
Section titled “Parametric Amplification”Undepleted-pump approximation
Section titled “Undepleted-pump approximation”If the pump is bright and changes negligibly during the interaction, replace its operator by a coherent amplitude,
After moving to resonant rotating frames, the three-mode Hamiltonian becomes the two-mode squeezing interaction
This approximation removes pump depletion, pump quantum fluctuations, and pump-output entanglement. It is excellent when conversion is a negligible fraction of a stable pump. Strong depletion, few-pump-photon operation, or important pump fluctuations invalidate it. In a resonator, approaching the linear oscillation threshold can make the predicted signal large enough that depletion and saturation must be included.
For constant over an effective interaction time , define . The Heisenberg transformation is
The identity
preserves bosonic commutators. Omitting the conjugated idler term would appear to amplify a mode but would violate .
Vacuum-seeded output
Section titled “Vacuum-seeded output”With both inputs in vacuum,
The source has zero mean field, , but nonzero occupation and pair correlation. Vacuum is not a hidden classical seed; it is the input quantum state whose fluctuations are transformed by the interaction.
The exact ideal output is
Signal and idler photon numbers are equal term by term. Either mode alone is thermal, while the joint state is pure and entangled for .
Seeded phase-preserving gain
Section titled “Seeded phase-preserving gain”Let the idler input be vacuum and seed the signal without signal-idler correlations. With power gain
the output signal occupation is
The final term is spontaneous amplifier noise. A phase-preserving amplifier must treat both signal quadratures equally and requires an independent idler degree of freedom; at high gain, an ideal linear amplifier adds at least the equivalent of half a quantum when noise is referred to its input. Real loss or a thermally occupied idler can raise it. With independent vacuum idler, each input-referred quadrature has added variance in the convention ; the half-quantum value is the high-gain limit.
Degenerate phase-sensitive gain
Section titled “Degenerate phase-sensitive gain”If signal and idler are the same mode, the Hamiltonian is
With
an appropriate pair of orthogonal quadratures transforms as
One quadrature is amplified and the other deamplified. This ideal phase-sensitive amplifier need not add noise to the amplified quadrature, but it requires a phase reference and does not amplify an unknown phase equally. Squeezed Light develops state, quadrature, decibel, loss, and verification conventions.
Resonators and threshold
Section titled “Resonators and threshold”A resonator increases interaction time and selects modes. For an ideal degenerate mode exactly resonant with half the pump frequency, with energy-decay rate , a linearized equation has the form
Here the plus drive sign is paired with . The small-signal threshold occurs at in this convention. Below threshold, the device is an optical parametric amplifier or oscillator source of squeezed output. At threshold, the linearized gain diverges mathematically, signaling the failure of the undepleted-pump approximation. Above threshold, pump depletion and nonlinear saturation determine the field. At detuning from half the pump frequency, the drift eigenvalues are , so the threshold becomes . Below threshold does not mean the fluctuations remain negligible arbitrarily close to it.
Frequency Conversion Is a Different Interaction
Section titled “Frequency Conversion Is a Different Interaction”A strong pump can select a number-conserving difference-frequency term rather than pair creation:
This is an beam-splitter rotation in frequency space. For constant ,
where and . The conversion probability is .
Unlike a two-mode squeezer, this interaction preserves and cannot create photons from vacuum. It can translate a single-photon wavepacket, squeezed state, or entanglement between frequency bands if noise and mode mismatch are controlled. The retained modes conserve photon number, but not their bare optical energy: the pump supplies or receives per converted photon.
χ³ Processes
Section titled “χ³ Processes”Four-wave mixing
Section titled “Four-wave mixing”A third-order medium supports interactions among four waves. For two pump modes and signal-idler generation, a representative quantum Hamiltonian is
Replacing the pumps by classical amplitudes gives the same two-mode squeezing form as parametric down-conversion, with
For a single degenerate pump,
A nonzero here requires an actual periodic modulation of the relevant third-order coupling or structure. Reversing ferroelectric domains to flip does not automatically flip .
Self- and cross-phase modulation can add intensity-dependent contributions to the actual phase mismatch. A source model that includes pair generation but omits those shifts can predict the wrong bandwidth or optimum pump power.
Four-wave mixing is used in fibers, integrated waveguides, atomic vapors, microresonators, and superconducting circuits. Its desired pair process may compete with Raman scattering, fluorescence, pump leakage, two-photon absorption, free-carrier effects, or thermal noise. Those backgrounds do not share one universal scaling law, so they must be measured rather than folded into an unexplained “efficiency.”
Self-phase modulation and the Kerr Hamiltonian
Section titled “Self-phase modulation and the Kerr Hamiltonian”Projecting a dispersive third-order response onto one ideal mode gives the Kerr Hamiltonian
Each Fock component acquires a number-dependent phase,
A coherent state therefore does not merely rotate rigidly in phase space: its different number components shear, producing quadrature squeezing at short times and non-Gaussian interference at special longer times. Loss rapidly erases the fine phase-space structure.
For two modes, an ideal cross-Kerr interaction is
It produces a phase in one mode conditioned on occupation of the other. This compact Hamiltonian is useful in resonators and effective circuit models, but a large clean single-photon cross-phase shift is difficult in a broadband traveling medium. Causality, finite response time, spectral entanglement, absorption, and Langevin noise must be included before claiming a deterministic photonic controlled phase.
Multimode Pair Generation
Section titled “Multimode Pair Generation”A traveling-wave source creates continua of signal and idler modes. At low gain, first-order evolution of vacuum gives a normalized two-photon component
Here is the time-integrated pair amplitude, not an instantaneous Hamiltonian coefficient. Beyond first order, time ordering can alter the mode functions and gains (Quesada and Sipe).
The joint amplitude has the schematic structure
where is the pump envelope, the phase-matching function, and collects spatial, polarization, and collection-mode overlaps.
A Schmidt decomposition writes the normalized amplitude as
The effective spectral-mode number is
For a pure one-pair state, tracing over an unresolved idler leaves signal purity . Thus gives a pure heralded photon even without resolving the idler’s spectral mode, provided the herald selects the one-pair sector. Conversely, a rank-one coherent projection on the idler can herald a pure signal even when ; this differs from an incoherent frequency-bin sum. Filtering can reduce the accepted Schmidt number but usually sacrifices rate and heralding efficiency. Source engineering aims to shape pump and phase matching before detection rather than discarding most of the state afterward.
Gaussian transformations and non-Gaussian light
Section titled “Gaussian transformations and non-Gaussian light”Quadratic Hamiltonians implement Gaussian unitaries: parametric processes squeeze, frequency conversion rotates modes, and coherent drives displace. Applied to Gaussian inputs, these transformations cannot create Wigner negativity. Kerr evolution, discrete emitters, non-Gaussian inputs, or photon-counting conditioning can supply the missing resource. Pair-number correlation alone does not prove entanglement: an incoherent mixture of is correlated but separable.
Loss, Noise, and Open-System Completion
Section titled “Loss, Noise, and Open-System Completion”Loss is not merely a final reduction in count rate. It can
- mix vacuum or thermal noise into squeezed quadratures;
- destroy pair-number correlations asymmetrically;
- reduce heralding efficiency;
- make the surviving heralded state mixed;
- compete with coherent buildup inside a resonator;
- remove photons during Kerr evolution and randomize conditional phase.
An absorptive susceptibility must be accompanied by reservoir operators so output commutators remain correct. In a waveguide, distributed loss can act before, during, and after pair creation; replacing it by one beam splitter at the output is accurate only under stated conditions.
Photon counting and homodyne detection connect the output state to observed counts and quadratures. Resonator boundary conditions are developed in input–output theory.
Exercises
Section titled “Exercises”Exercise 1: Inversion symmetry and an induced second-order response
Section titled “Exercise 1: Inversion symmetry and an induced second-order response”In a scalar model,
- Show that inversion symmetry forces every even-order coefficient to vanish.
- Suppose the centrosymmetric medium has a static bias and a small optical field , so . Find the effective coefficient of generated by the term.
Solution
Inversion symmetry requires
The polarization must therefore be an odd function of . Comparing the series term by term gives
for the ideal bulk electric-dipole response.
With a static bias,
The term quadratic in the optical field is . In this scalar convention,
The tensor result depends on the bias direction and contracted indices. This is the electric-field-induced second-harmonic mechanism in its simplest form.
Exercise 2: Finite-length phase matching
Section titled “Exercise 2: Finite-length phase matching”A uniform waveguide has length and constant phase mismatch .
- Find the generated intensity relative to exact phase matching, using only the longitudinal factor.
- Find the magnitude of the first nonzero for which the longitudinal amplitude vanishes.
Solution
The dimensionless argument is
Therefore
The first zero occurs when
so
A longer device raises the exactly matched amplitude but narrows the accepted mismatch range.
Exercise 3: One pump quantum in a three-wave mixer
Section titled “Exercise 3: One pump quantum in a three-wave mixer”Take real and
Start in .
- Show that evolution remains in the span of and .
- Find the exact state and conversion probability.
- Verify the Manley–Rowe invariants.
Solution
The Hamiltonian acts as
No other state is connected because there is at most one pump quantum and one signal-idler pair. Exponentiating this two-state generator gives
Thus
Both basis states have
Every superposition in the invariant subspace has the same eigenvalues of those three combinations.
Exercise 4: Gain and spontaneous amplifier output
Section titled “Exercise 4: Gain and spontaneous amplifier output”A nondegenerate parametric amplifier has . Its idler input is vacuum, and its signal input has mean occupation with no signal-idler correlation.
- Find the power gain .
- Find the output signal and idler occupations.
- Verify that their mean difference equals the input signal-idler difference.
Solution
The gain is
and
For a vacuum idler,
Their difference is
equal to its input value. The added photons appear as pairs, preserving .
Exercise 5: Phase matching with domain reversal
Section titled “Exercise 5: Phase matching with domain reversal”Suppose and the bare mismatch is . Over many periods, find the effective resonant coupling compared with a uniform, perfectly phase-matched crystal. Why is there a conversion penalty despite compensating the mismatch?
Solution
The Fourier expansion begins . Multiplication by selects the constant component of the negative first harmonic, of amplitude . Thus the effective coupling is , and the low-gain intensity is of ideal uniform phase matching for the same length and local susceptibility. Domain reversal prevents destructive accumulation but allocates part of the nonlinear profile to nonresonant harmonics. Finite-length edge corrections vanish for an integer number of periods.
Exercise 6: Single-photon frequency conversion
Section titled “Exercise 6: Single-photon frequency conversion”A frequency converter has mixing angle and pump phase . It acts on an input .
- Find the output state.
- Find the conversion probability.
- Explain what happens to vacuum input.
Solution
The creation-operator transformation gives
At ,
The conversion probability is
The two-mode vacuum remains vacuum because the interaction conserves total photon number. This is a coherent frequency beam splitter, not a vacuum-seeded amplifier.
Exercise 7: Kerr phases are not a rigid rotation
Section titled “Exercise 7: Kerr phases are not a rigid rotation”The initial state is
It evolves under
for a time .
- Find the final state.
- Compare before and after.
- Compare before and after.
Solution
The phases for are respectively
Therefore
The number probabilities are unchanged, so
both before and after. Initially,
whereas afterward,
Kerr evolution preserves number while changing relative phases between number sectors. A rigid phase-space rotation would instead multiply by a unit-modulus phase without changing its magnitude.
Exercise 8: Compare second- and third-order pump scaling
Section titled “Exercise 8: Compare second- and third-order pump scaling”A selected low-gain second-order pair process has
while degenerate-pump four-wave mixing has
Assume pump power satisfies and hold all other parameters fixed.
- Find the low-gain pair-probability scaling with for each process.
- By what factor does each probability change when the pump power doubles?
- Give two reasons the simple power laws can fail experimentally.
Solution
At low gain, pair probability is proportional to squared interaction amplitude. Therefore
Doubling therefore gives
The laws assume undepleted pumps, fixed mode overlap, and fixed phase matching. Pump depletion, self- and cross-phase modulation, thermal or photorefractive detuning, nonlinear absorption, Raman background, and detector saturation can all change the measured scaling.
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