We show that entangled radiation-matter states with broken symmetries can be prepared by using nonclassical light in the coherent control techniques. We demonstrate the method by realizing the entanglement in degenerate continuum electronic momentum states of opposite directionality and discrete states of opposite handedness in chiral molecules. When the material system is excited simultaneously by classical light and quantum light in a state with several semiclassical phases, the interference

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... , the interference conditions guide the system to such entangled radiation-matter states.