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At the fundamental level, full description of light-matter interactionrequires quantum treatment of both matter and light. However, for standardlight sources generating intense laser pulses carrying quadrillions of photonsin a coherent state, classical description of light during intense laser-matterinteraction has been expected to be adequate. Here we show how nonlinearoptical response of matter can be controlled to generate dramatic deviationsfrom this standard picture, including generation of multiple harmonics of theincident laser light entangled across many octaves. In particular, non-trivialquantum states of harmonics are generated as soon as one of the harmonicsinduces a transition between different laser-dressed states of the materialsystem. Such transitions generate an entangled light-matter wavefunction, whichemerges as the key condition for generating quantum states of harmonics,sufficient even in the absence of a quantum driving field or materialcorrelations. In turn, entanglement of the material system with a singleharmonic generates and controls entanglement between different harmonics.Hence, nonlinear media that are near-resonant with at least one of theharmonics appear to be most attractive for controlled generation of massivelyentangled quantum states of light. Our analysis opens remarkable opportunitiesat the interface of attosecond physics and quantum optics, with implicationsfor quantum information science.

Generation of massively entangled bright states of light during harmonic generation in resonant media