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Register a new userReducing decoherence in optical and spin transitions in rare-earth-ion doped materials
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In many important situations the dominant dephasing mechanism in cryogenic rare-earth-ion doped systems is due to magnetic field fluctuations from spins in the host crystal. Operating at a magnetic field where a transition has a zero first-order-Zeeman (ZEFOZ) shift can greatly reduce this dephasing. Here we identify the location of transitions with zero first-order Zeeman shift for optical transitions in Pr3+:YAG and for spin transitions in Er3+:Y2SiO5. The long coherence times that ZEFOZ would enable would make Pr3+:YAG a strong candidate for achieving the strong coupling regime of cavity QED, and would be an important step forward in creating long-lived telecommunications wavelength quantum memories in Er3+:Y2SiO5. This work relies mostly on published spin Hamiltonian parameters but Raman heterodyne spectroscopy was performed on Pr3+:YAG to measure the parameters for the excited state.
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Optically addressable spins are actively investigated in quantum communication, processing and sensing. Optical and spin coherence lifetimes, which determine quantum operation fidelity and storage time, are often limited by spin-spin interactions, which can be decreased by polarizing spins in their lower energy state using large magnetic fields and/or mK range temperatures. Here, we show that optical pumping of a small fraction of ions with a fixed frequency laser, coupled with spin-spin interactions and spin diffusion, leads to substantial spin polarization in a paramagnetic rare earth doped crystal, $^{171}$Yb$^{3+}$:YSO. Indeed, up to more than 90 % spin polarizations have been achieved at 2 K and zero magnetic field. Using this spin polarization mechanism, we furthermore demonstrate an increase in optical coherence lifetime from 0.3 ms to 0.8 ms, due to a strong decrease in spin-spin interactions. This effect opens the way to new schemes for obtaining long optical and spin coherence lifetimes in various solid-state systems such as ensembles of rare earth ions or color centers in diamond, which is of interest for a broad range of quantum technologies.
We investigate a novel hybrid system composed of an ensemble of room temperature rare-earth ions embedded in a bulk crystal, intrinsically coupled to internal strain via the surrounding crystal field. We evidence the generation of a mechanical response under resonant light excitation. Thanks to an ultra-sensitive time- and space-resolved photodeflection setup, we interpret this motion as the sum of two resonant optomechanical backaction processes: a conservative, piezoscopic process induced by the optical excitation of a well-defined electronic configuration, and a dissipative, non-radiative photothermal process related to the phonons generated throughout the atomic population relaxation. Parasitic heating processes, namely off-resonant dissipative contributions, are absent. This work demonstrates an unprecedented level of control of the conservative and dissipative relative parts of the optomechanical backaction, confirming the potential of rare-earth-based systems as promising hybrid mechanical systems.
Short coherence times present a primary obstacle in quantum computing and sensing applications. In atomic systems, clock transitions (CTs), formed from avoided crossings in an applied Zeeman field, can substantially increase coherence times. We show how CTs can dampen intrinsic and extrinsic sources of quantum noise in molecules. Conical intersections between two periodic potentials form CTs in electron paramagnetic resonance experiments of the spin-polarized singlet fission photoproduct. We report on a pair of CTs for a two-chromophore molecule in terms of the Zeeman field strength, molecular orientation relative to the field, and molecular geometry.
Nano-structuring impurity-doped crystals affects the phonon density of states and thereby modifies the atomic dynamics induced by interaction with phonons. We propose the use of nano-structured materials in the form of powders or phononic bandgap crystals to enable or improve persistent spectral hole-burning and coherence for inhomogeneously broadened absorption lines in rare-earth-ion-doped crystals. This is crucial for applications such as ultra-precise radio-frequency spectrum analyzers and optical quantum memories. As an example, we discuss how phonon engineering can enable spectral hole burning in erbium-doped materials operating in the convenient telecommunication band, and present simulations for density of states of nano-sized powders and phononic crystals for the case of Y2SiO5, a widely-used material in current quantum memory research.
We describe a high-resolution spectroscopy method, in which the detection of single excitation events is enhanced by a complete loss of coherence of a superposition of two ground states. Thereby, transitions of a single isolated atom nearly at rest are recorded efficiently with high signal-to-noise ratios. Spectra display symmetric line shapes without stray-light background from spectroscopy probes. We employ this method on a $^{25}$Mg$^+$ ion to measure one, two, and three-photon transition frequencies from the 3S ground state to the 3P, 3D, and 4P excited states, respectively. Our results are relevant for astrophysics and searches for drifts of fundamental constants. Furthermore, the method can be extended to other transitions, isotopes, and species. The currently achieved fractional frequency uncertainty of $5 times 10^{-9}$ is not limited by the method.
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