ArXiv · 2026
Optical nonlinearity of materials with broken inversion symmetry enables two-photon processes where an incoming pair of photons can generate an up-converted photon with the combined frequency, or a high-energy photon can be split into a correlated pair of down-converted photons. Here, we identify few-layer graphene films that offer up/down-conversion capability in the infrared spectral range. For mixed stacking tetralayers (ABCB), which are non-centrosymmetric 2D crystals, we find highly efficient nearly resonant up/down-conversion of [ω₁,ω₂] photon pairs into/from a photon with 0.7eV<Ω=ω₁+ω₂<1.1eV. We also note that a pronounced second-order nonlinearity in the spectral range of 0.7eV<Ω<0.9eV can be promoted in rhombohedral tri- and tetralayers by asymmetrical encapsulation. Potentially, for fibers coated with few-layer graphene, this opens the door for ``in fiber" production of photon pairs with correlated polarizations.
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