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Register a new userCoherence Time Extension by Large Scale Optical Spin Polarization in a Rare-Earth Doped Crystal
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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.
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The inhomogeneity of an electron spin ensemble as well as fluctuating environment acting upon individual spins drastically shorten the spin coherence time $T_2$ and hinder coherent spin manipulation. We show that this problem can be solved by the simultaneous application of a radiofrequency (rf) field, which stimulates coherent spin precession decoupled from an inhomogeneous environment, and periodic optical pulses, which amplify this precession. The resulting resonance, taking place when the rf field frequency approaches the laser pulse repetition frequency, has a width determined by the spin coherence time $T_2$ that is free from the inhomogeneity effects. We measure a 50-Hz-narrow electron spin resonance and milliseconds-long $T_2$ for electrons in the ground state of Ce$^{3+}$ ions in the YAG lattice at low temperatures, while the inhomogeneous spin dephasing time $T_2^*$ is only 25 ns. This study paves the way to coherent optical manipulation in spin systems decoupled from their inhomogeneous environment.
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.
Inelastic neutron scattering was employed to study the crystal-field interaction in the strontium-doped rare-earth compounds R(x)Sr(1-x)CoO(3-z) (R=Pr, Nd, Ho, and Er). Particular emphasis is laid on the effect of oxygen deficiencies which naturally occur in the synthesis of these compounds. The observed energy spectra are found to be the result of a superposition of crystal fields with different nearest-neighbor oxygen coordination at the R sites. The experimental data are interpreted in terms of crystal-field parameters which behave in a consistent manner through the rare-earth series, thereby allowing a reliable extrapolation for rare-earth ions not considered in the present work.
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.
Based on the electronic band structure obtained from first principles DFT calculations, the opticalspectra of yttrium and neodymium nickelates are computed. We show that the results are in fairagreement with available experimental data. We clarify the electronic transitions at the origin of thefirst two peaks, highlighting the important role of transitions from t2g states neglected in previousmodels. We discuss the evolution of the optical spectra from small to large rare-earth cations andrelate the changes to the electronic band structure.
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