The development of qualitatively new measurement capabilities is often a prerequisite for critical scientific and technological advances. The dramatic progress made by modern probe techniques to uncover the microscopic structure of matter is fundamentally rooted in our control of two defining traits of quantum mechanics: discreteness of physical properties and interference phenomena. Magnetic Resonance Imaging, for instance, exploits the fact that protons have spin and can absorb photons at frequencies that depend on the medium to image the anatomy and physiology of living systems. Scattering techniques, in which photons, electrons, protons or neutrons are used as probes, make use of quantum interference to directly image the spatial position of individual atoms, their magnetic structure, or even unveil their concomitant dynamical correlations. None of these probes have so far exploited a unique characteristic of the quantum world: entanglement. Here we introduce a fundamentally new quantum probe, an entangled neutron beam, where individual neutrons can be entangled in spin, trajectory and energy. Its tunable entanglement length from nanometers to microns and energy differences from peV to neV will enable new investigations of microscopic magnetic correlations in systems with strongly entangled phases, such as those believed to emerge in unconventional superconductors. We develop an interferometer to prove entanglement of these distinguishable properties of the neutron beam by observing clear violations of both Clauser-Horne-Shimony-Holt and Mermin contextuality inequalities in the same experimental setup. Our work opens a pathway to a future era of entangled neutron scattering in matter. Text:A most amazing aspect of quantum reality is the possibility to share information non-locally between two or more spacelike separated subsystems, a "spooky action at a distance", as Einstein liked to call it and Bell epitomized in an inequality 1,2 . The fact that measuring compatible observables does not unveil predetermined physical properties, as pointed out by Kochen and Specker 3,4 , reveals the contextual nature of quantum measurements. Behind all these non-classical statistical correlations is the property of entanglement wherein "the state of the whole is more than the sum of its [constituent] parts'' 5 . Developing novel quantum probes that exploit these correlations as a means for investigating entanglement in matter could lead to novel insight into some of the most interesting materials studied today, such as frustrated magnets hosting quantum spin liquids and unconventional superconductors with strange metallic behavior 6 .

We develop an operator-based description of two types of multimode-entangled single-neutron quantum optical devices: Wollaston prisms and radio-frequency spin flippers in inclined magnetic field gradients. This treatment is similar to the approach used in quantum optics, and is convenient for the analysis of quantum contextuality measurements in certain types of neutron interferometers. We describe operationally the way multimode-entangled single-neutron states evolve in these devices, and provide expressions for the associated operators describing the dynamics, in the limit in which the neutron state space is approximated by a finite tensor product of distinguishable subsystems. We design entangled-neutron interferometers to measure entanglement witnesses for the Clauser, Horne, Shimony and Holt, and Mermin inequalities, and compare the theoretical predictions with recent experimental results. We present the generalization of these expressions to n entangled distinguishable subsystems, which could become relevant in the future if it becomes possible to add neutron orbital angular momentum to the experimentally-accessible list of entangled modes. We view this work as a necessary first step towards a theoretical description of entangled neutron scattering from strongly entangled matter, and we explain why it should be possible to formulate a useful generalization of the usual Van Hove linear response theory for this case. We also briefly describe some other scientific extensions and applications which can benefit from interferometric measurements using the types of single-neutron multimode entanglement described by this analysis.

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