Entangled photons are a key resource in quantum technologies. While intense laser light propagating in nonlinear crystals is conventionally used to generate entangled photons, such schemes have low efficiency due to the weak nonlinear response of known materials and losses associated with in/out photon coupling. Here, we show how to generate entangled polariton pairs directly within optical waveguides using free electrons. The measured energy loss of undeflected electrons heralds the production of counter-propagating polariton pairs entangled in energy and emission direction. For illustration, we study the excitation of plasmon polaritons in metal strip waveguides that strongly enhance light-matter interactions, rendering two-plasmon generation dominant over single-plasmon excitation. We demonstrate that electron energy losses detected within optimal frequency ranges can reliably signal the generation of plasmon pairs entangled in energy and momentum. Our proposed scheme is directly applicable to other types of optical waveguides for in situ generation of entangled photon pairs.
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