No Arabic abstract
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.
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.
Nitrogen-vacancy (NV) centers in diamond are promising quantum sensors for their long spin coherence time under ambient conditions. However, their spin resonances are relatively insensitive to non-magnetic parameters such as temperature. A magnetic-nanoparticle-nanodiamond hybrid thermometer, where the temperature change is converted to the magnetic field variation near the Curie temperature, was demonstrated to have enhanced temperature sensitivity (11 mK Hz^{-1/2}) [Phys. Rev. X 8, 011042 (2018)], but the sensitivity was limited by the large spectral broadening of ensemble spins in nanodiamonds. To overcome this limitation, here we showed an improved design of a hybrid nanothermometer using a single NV center in a diamond nanopillar coupled with a single magnetic nanoparticle of copper-nickel alloy, and demonstrated a temperature sensitivity of 76 uK Hz^{-1/2}. This hybrid design enabled detection of 2 millikelvins temperature changes with temporal resolution of 5 milliseconds. The ultra-sensitive nanothermometer offers a new tool to investigate thermal processes in nanoscale systems.
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.
Metal nanoantennas supporting localized surface plasmon resonances have become an indispensable tool in bio(chemical) sensing and nanoscale imaging applications. The high plasmon-enhanced electric field intensity in the visible or near-IR range that enables the above applications may also cause local heating of nanoantennas. We present a design of hybrid optical-thermal antennas that simultaneously enable intensity enhancement at the operating wavelength in the visible and nanoscale local temperature control. We demonstrate a possibility to reduce the hybrid antenna operating temperature via enhanced infrared thermal emission. We predict via rigorous numerical modeling that hybrid optical-thermal antennas that support high-quality-factor photonic-plasmonic modes enable up to two orders of magnitude enhancement of localized electric fields and of the optical power absorbed in the nanoscale metal volume. At the same time, the hybrid antenna temperature can be lowered by several hundred degrees with respect to its all-metal counterpart under continuous irradiance of 104-105 W/m2. The temperature reduction effect is attributed to the enhanced radiative cooling, which is mediated by the thermally-excited localized surface phonon polariton modes. We further show that temperature reduction under even higher irradiances can be achieved by a combination of enhanced radiative and convective cooling in hybrid antennas. Finally, we demonstrate how hybrid optical-thermal antennas can be used to achieve strong localized heating of nanoparticles while keeping the rest of the optical chip at low temperature.
Many classes of two-dimensional (2D) materials have emerged as potential platforms for novel electronic and optical devices. However, the physical properties are strongly influenced by nanoscale heterogeneities in the form of edges, grain boundaries, and nucleation sites. Using combined tip-enhanced Raman scattering (TERS) and photoluminescence (TEPL) nano-spectroscopy and -imaging, we study the associated effects on the excitonic properties in monolayer WSe2 grown by physical vapor deposition (PVD). With <15 nm spatial resolution we resolve nonlocal nanoscale correlations of PL spectral intensity and shifts with crystal edges and internal twin boundaries associated with the expected exciton diffusion length. Through an active atomic force tip interaction we can control the crystal strain on the nanoscale, and tune the local bandgap in reversible (up to 24 meV shift) and irreversible (up to 48 meV shift) fashion. This allows us to distinguish the effect of strain from the dominant influence of defects on the PL modification at the different structural heterogeneities. Hybrid nano-optical and nano-mechanical imaging and spectroscopy thus enables the systematic study of the coupling of structural and mechanical degrees of freedom to the nanoscale electronic and optical properties in layered 2D materials.