Intraparticle entanglement of individual particles such as neutrons could enable another class of scattering probes that are sensitive to entanglement in quantum systems and materials. In this work, we present experimental results demonstrating quantum contextuality as a result of entanglement between the spin and energy modes (i.e., degrees of freedom) of single neutrons in a beam using a pair of resonant radio-frequency neutron spin flippers in the modulated intensity with zero effort configuration. We verified the mode entanglement by measuring a Clauser-Horne-Shimony-Holt contextuality witness 𝑆 defined in the spin and energy subsystems, observing a clear breach of the classical bound of |𝑆|≤2, obtaining 𝑆=2.40±0.02. These entangled beams could enable alternative approaches for directly probing dynamics and entanglement in quantum materials whose low-energy excitation scales match those of the incident entangled neutron.@en

We describe an experiment that strongly supports a two-path interferometric model in which the spin-up and spin-down components of each neutron propagate coherently along spatially separated parallel paths in a typical neutron spin-echo small-angle scattering (SESANS) experiment. Specifically, we show that the usual semi-classical, single-path treatment of Larmor precession of a polarized neutron in an external magnetic field predicts a damping as a function of the spin-echo length of the SESANS signal obtained with a periodic phase grating when the transverse width of the neutron wave packet is finite. However, no such damping is observed experimentally, implying either that the Larmor model is incorrect or that the transverse extent of the wave packet is very large. In contrast, we demonstrate theoretically that a quantum-mechanical interferometric model in which the two mode-entangled (i.e., intraparticle entangled) spin states of a single neutron are separated in space when they interact with the grating accurately predicts the measured SESANS signal, which is independent of the wave packet width.

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The development of direct probes of entanglement is integral to the rapidly expanding field of complex quantum materials. Here we test the robustness of entangled neutrons as a quantum probe by measuring the Clauser-Horne-Shimony-Holt contextuality witness while varying the beam properties. Specifically, we show that the mode entanglement of the spin and path subsystems of individual neutrons prepared in two different experiments using two different apparatuses persists even after varying the entanglement length, coherence length, and neutron energy difference of the paths. The two independent apparatuses acting as entangler-disentangler pairs are static-field magnetic Wollaston prisms and resonance-field radio-frequency flippers. Our results show that the spatial and energy properties of the neutron beam may be significantly altered without reducing the contextuality witness value below the Tsirelson bound, meaning that maximum entanglement is preserved. We also show that two paths may be considered distinguishable even when the path states significantly overlap. Therefore, we have shown that our experimental results are consistent with the distinguishable subsystem assumption down to a separation of less than 100 nm, proving entanglement and the contextual nature of reality on short length scales. This work is the key step in the realization of the modular, robust technique of entangled neutron scattering, which can extract entanglement information from a sample without the knowledge of the microscopic sample Hamiltonian: only semiquantitative knowledge of the correlation lengths of the relevant degrees of freedom and the timescales of the characteristic dynamics is required.

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