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Register a new userFemtosecond Coherence and Quantum Control of Single Molecules at Room Temperature
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Quantum mechanical phenomena, such as electronic coherence and entanglement, play a key role in achieving the unrivalled efficiencies of light-energy conversion in natural photosynthetic light-harvesting complexes, and triggered the growing interest in the possibility of organic quantum computing. Since biological systems are intrinsically heterogeneous, clear relations between structural and quantum-mechanical properties can only be obtained by investigating individual assemblies. However, single-molecule techniques to access ultrafast coherences at physiological conditions were not available so far. Here we show by employing femtosecond pulse-shaping techniques that quantum coherences in single organic molecules can be created, probed, and manipulated at ambient conditions even in highly disordered solid environments. We find broadly distributed coherence decay times for different individual molecules giving direct insight into the structural heterogeneity of the local surroundings. Most importantly, we induce Rabi-oscillations and control the coherent superposition state in a single molecule, thus performing a basic femtosecond single-qubit operation at room temperature.
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The ability to accurately control the dynamics of physical systems by measurement and feedback is a pillar of modern engineering. Today, the increasing demand for applied quantum technologies requires to adapt this level of control to individual quantum systems. Achieving this in an optimal way is a challenging task that relies on both quantum-limited measurements and specifically tailored algorithms for state estimation and feedback. Successful implementations thus far include experiments on the level of optical and atomic systems. Here we demonstrate real-time optimal control of the quantum trajectory of an optically trapped nanoparticle. We combine confocal position sensing close to the Heisenberg limit with optimal state estimation via Kalman filtering to track the particle motion in phase space in real time with a position uncertainty of 1.3 times the zero point fluctuation. Optimal feedback allows us to stabilize the quantum harmonic oscillator to a mean occupation of $n=0.56pm0.02$ quanta, realizing quantum ground state cooling from room temperature. Our work establishes quantum Kalman filtering as a method to achieve quantum control of mechanical motion, with potential implications for sensing on all scales. In combination with levitation, this paves the way to full-scale control over the wavepacket dynamics of solid-state macroscopic quantum objects in linear and nonlinear systems.
Coherent coupling between single quantum objects is at the heart of modern quantum physics. When coupling is strong enough to prevail over decoherence, it can be used for the engineering of correlated quantum states. Especially for solid-state systems, control of quantum correlations has attracted widespread attention because of applications in quantum computing. Such coherent coupling has been demonstrated in a variety of systems at low temperature1, 2. Of all quantum systems, spins are potentially the most important, because they offer very long phase memories, sometimes even at room temperature. Although precise control of spins is well established in conventional magnetic resonance3, 4, existing techniques usually do not allow the readout of single spins because of limited sensitivity. In this paper, we explore dipolar magnetic coupling between two single defects in diamond (nitrogen-vacancy and nitrogen) using optical readout of the single nitrogen-vacancy spin states. Long phase memory combined with a defect separation of a few lattice spacings allow us to explore the strong magnetic coupling regime. As the two-defect system was well-isolated from other defects, the long phase memory times of the single spins was not diminished, despite the fact that dipolar interactions are usually seen as undesirable sources of decoherence. A coherent superposition of spin pair quantum states was achieved. The dipolar coupling was used to transfer spin polarisation from a nitrogen-vacancy centre spin to a nitrogen spin, with optical pumping of a nitrogen-vacancy centre leading to efficient initialisation. At the level anticrossing efficient nuclear spin polarisation was achieved. Our results demonstrate an important step towards controlled spin coupling and multi-particle entanglement in the solid state.
Single photon emitters are indispensable to photonic quantum technologies. Here we demonstrate waveform-controlled high-purity single photons from room-temperature colloidal quantum dots. The purity of the single photons does not vary with the excitation power, thereby allowing the generation rate to be increased without compromising the single-photon quality.
We formulate a mixed-state analog of the NLTS conjecture [FH14] by asking whether there exist topologically-ordered systems for which the thermal Gibbs state for constant temperature is globally-entangled in the sense that it cannot even be approximated by shallow quantum circuits. We then prove this conjecture holds for nearly optimal parameters: when the inverse temperature is almost a constant (temperature decays as 1/loglog(n))) and the Hamiltonian is nearly local (log(n)-local). The construction and proof combine quantum codes that arise from high-dimensional manifolds [Has17, LLZ19], the local-decoding approach to quantum codes [LTZ15, FGL18] and quantum locally-testable codes [AE15].
Quantum coherence control usually requires extremely low temperature environments. Even for spins in diamond, a remarkable exception, the coherence signal is lost as temperature approaches 700 K. Here we demonstrate quantum coherence control of the electron spins of nitrogen-vacancy centers in nanodiamonds at temperatures near 1000 K. The scheme is based on initialization and readout of the spins at room temperature and control at high temperature, which is enabled by pulse laser heating and rapid diffusion cooling of nanodiamonds on amorphous carbon films. Using high-temperature spin control, we observe the magnetic phase transition of a single nickel nanoparticle at about 615 K. This work enables nano-thermometry and nano-magnetometry in the high-temperature regime.
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