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Time-resolved Raman spectroscopy techniques offer various ways to study the dynamics of molecular vibrations in liquids or gases and optical phonons in crystals. While these techniques give access to the coherence time of the vibrational modes, they are not able to reveal the fragile quantum correlations that are spontaneously created between light and vibration during the Raman interaction. Here, we present a scheme leveraging universal properties of spontaneous Raman scattering to demonstrate Bell correlations between light and a collective molecular vibration. We measure the decay of these hybrid photon-phonon Bell correlations with sub-picosecond time resolution and find that they survive over several hundred oscillations at ambient conditions. Our method offers a universal approach to generate entanglement between light and molecular vibrations. Moreover, our results pave the way for the study of quantum correlations in more complex solid-state and molecular systems in their natural state.
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Nitrogen vacancy (NV) centres in diamond are attractive as quantum sensors owing to their superb coherence under ambient conditions. However, the NV centre spin resonances are relatively insensitive to some important parameters such as temperature. Here we design and experimentally demonstrate a hybrid nano-thermometer composed of NV centres and a magnetic nanoparticle (MNP), in which the temperature sensitivity is enhanced by the critical magnetization of the MNP near the ferromagnetic-paramagnetic transition temperature. The temperature susceptibility of the NV center spin resonance reached 14 MHz/K, enhanced from the value without the MNP by two orders of magnitude. The sensitivity of a hybrid nano-thermometer composed of a Cu_{1-x}Ni_{x} MNP and a nanodiamond was measured to be 11 mK/Hz^{1/2} under ambient conditions. With such high-sensitivity, we monitored nanometer-scale temperature variation of 0.3 degree with a time resolution of 60 msec. This hybrid nano-thermometer provides a novel approach to studying a broad range of thermal processes at nanoscales such as nano-plasmonics, sub-cellular heat-stimulated processes, thermodynamics of nanostructures, and thermal remanent magnetization of nanoparticles.
Strong coupling of two-dimensional semiconductor excitons with plasmonic resonators enables control of light-matter interaction at the subwavelength scale. Here we develop strong coupling in plasmonic nano-gap resonators that allow modification of exciton number contributing to the coupling. Using this system, we not only demonstrate a large vacuum Rabi splitting up to 163 meV and splitting features in photoluminescence spectra, but also reveal that the exciton number can be reduced down to single-digit level (N<10), which is an order lower than that of traditional systems, close to single-exciton based strong coupling. In addition, we prove that the strong coupling process is not affected by the large exciton coherence size that was previously believed to be detrimental to the formation of plasmon-exciton interaction. Our work provides a deeper understanding of storng coupling in two-dimensional semiconductors, paving the way for room temperature quantum optics applications.
We show that spin systems with infinite-range interactions can violate at thermal equilibrium a multipartite Bell inequality, up to a finite critical temperature $T_c$. Our framework can be applied to a wide class of spin systems and Bell inequalities, to study whether nonlocality occurs naturally in quantum many-body systems close to the ground state. Moreover, we also show that the low-energy spectrum of the Bell operator associated to such systems can be well approximated by the one of a quantum harmonic oscillator, and that spin-squeezed states are optimal in displaying Bell correlations for such Bell inequalities.
We use the electronic spin of a single Nitrogen-Vacancy (NV) defect in diamond to observe the real-time evolution of neighboring single nuclear spins under ambient conditions. Using a diamond sample with a natural abundance of $^{13}$C isotopes, we first demonstrate high fidelity initialization and single-shot readout of an individual $^{13}$C nuclear spin. By including the intrinsic $^{14}$N nuclear spin of the NV defect in the quantum register, we then report the simultaneous observation of quantum jumps linked to both nuclear spin species, providing an efficient initialization of the two qubits. These results open up new avenues for diamond-based quantum information processing including active feedback in quantum error correction protocols and tests of quantum correlations with solid-state single spins at room temperature.
Entanglement is a vital property of multipartite quantum systems, characterised by the inseparability of quantum states of objects regardless of their spatial separation. Generation of entanglement between increasingly macroscopic and disparate systems is an ongoing effort in quantum science which enables hybrid quantum networks, quantum-enhanced sensing, and probing the fundamental limits of quantum theory. The disparity of hybrid systems and the vulnerability of quantum correlations have thus far hampered the generation of macroscopic hybrid entanglement. Here we demonstrate, for the first time, generation of an entangled state between the motion of a macroscopic mechanical oscillator and a collective atomic spin oscillator, as witnessed by an Einstein-Podolsky-Rosen variance below the separability limit, $0.83 pm 0.02<1$. The mechanical oscillator is a millimeter-size dielectric membrane and the spin oscillator is an ensemble of $10^9$ atoms in a magnetic field. Light propagating through the two spatially separated systems generates entanglement due to the collective spin playing the role of an effective negative-mass reference frame and providing, under ideal circumstances, a backaction-free subspace; in the experiment, quantum backaction is suppressed by 4.6 dB. Our results pave the road towards measurement of motion beyond the standard quantum limits of sensitivity with applications in force, acceleration,and gravitational wave detection, as well as towards teleportation-based protocols in hybrid quantum networks.
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