Related papers: Raman relaxation in Yb(III) molecular qubits: non-…
Spin-phonon coupling is the main drive of spin relaxation and decoherence in solid-state semiconductors at finite temperature. Controlling this interaction is a central problem for many disciplines, ranging from magnetic resonance to…
Paramagnetic molecules can show long spin-coherence times, which make them good candidates as quantum bits. Reducing the efficiency of the spin-phonon interaction is the primary challenge towards achieving long coherence times over a wide…
Magnetic relaxation in coordination compounds is largely dominated by the interaction of the spin with phonons. Large zero-field splitting and exchange coupling values have been empirically found to strongly suppress spin relaxation and…
To design molecular spin qubits with enhanced quantum coherence, a control of the coupling between the local vibrations and the spin states is crucial, which could be realized in principle by engineering molecular structures via…
We study the spin-phonon relaxation rate of both Kramers and non-Kramers molecular magnets in strongly diluted samples at low temperature. Using the "rotational" contribution to the spin-phonon Hamiltonian, universal formulae for the…
The study of how spin interacts with lattice vibrations and relaxes to equilibrium provides unique insights on its chemical environment and the relation between electronic structure and molecular composition. Despite its importance for…
The unique electronic and magnetic properties of Lanthanides molecular complexes place them at the forefront of the race towards high-temperature single-ion magnets and magnetic quantum bits. The design of compounds of this class has so far…
Time resolved measurements provide a new way to disentangle complex interactions in quantum materials due to their different timescales. We used pump-probe Raman scattering to investigate the apical oxygen vibration in…
We present a comprehensive study of spin relaxation dynamics at cryogenic temperatures in a rare-earth-doped crystal used for quantum memory applications: $^{171}$Yb:Y$_2$SiO$_5$. Spin relaxation is indeed a major limiting factor for both…
Paramagnetic defects in diamond and hexagonal boron nitride possess a unique combination of spin and optical properties that make them prototypical solid-state qubits. Despite the coherence of these spin qubits being critically limited by…
Spin-phonon interaction is known to drive magnetic relaxation in solid-state systems, but little evidence is available on how it affects coherence time. Here we extend fourth-order quantum master equations to account for coherence terms and…
Electronic spin superposition states enable nanoscale sensing through their sensitivity to the local environment, yet their sensitivity to vibrational motion also limits their coherence times. In molecular spin systems, chemical tunability…
Understanding and controlling spin relaxation in molecular qubits is essential for developing chemically tunable quantum information platforms. We present a fully first-principles framework for computing the spin relaxation tensor in a…
The coupling between electronic spins and lattice vibrations is fundamental for driving relaxation in magnetic materials. The debate over the nature of spin-phonon coupling dates back to the 40's, but the role of spin-spin, spin-orbit and…
The interaction of electronic spin and molecular vibrations mediated by spin-orbit coupling governs spin relaxation in molecular qubits. I derive an extended molecular spin Hamiltonian that includes both adiabatic and non-adiabatic…
Molecular electron spin qubits offer atomic-level tunability and room-temperature quantum coherence. Their integration into engineered solid-state matrices can enhance performance towards ambient quantum information technologies. Herein, we…
We present a first-principles investigation of spin-phonon relaxation in a molecular crystal of Co(II) single-ion magnets. Our study combines electronic structure calculations with machine-learning force fields and unravels the nature of…
Spin-lattice relaxation theory has been developed over almost a century, but some cardinal assumptions on the nature of the interactions involved have never been fully verified. This includes the weak coupling approximation, which makes it…
Single-molecule magnets (SMMs) are promising candidates for molecular-scale data storage and processing due to their strong magnetic anisotropy and long spin relaxation times. However, as temperature rises, interactions between electronic…
Spin-lattice relaxation within the nitrogen-vacancy (NV) center's electronic ground-state spin triplet limits its coherence times, and thereby impacts its performance in quantum applications. We report measurements of the relaxation rates…