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Filippo Caracciolo

Publications and source records attributed to Filippo Caracciolo.

2 recordsLinked to original sources

Spin fluctuations in the light-induced high spin state of Cobalt valence tautomers

We present a study of the static magnetic properties and spin dynamics in Cobalt valence tautomers (VT), molecules where a low-spin (LS) to high-spin (HS) crossover driven by an intramolecular electron transfer can be controlled by the temperature, by the external pressure or by light irradiation. In the investigated complex, a LS-Co(III) ion bound to a dinegative organic ligand can be reversibly converted into the HS-Co(II) bound to a mononegative one. By combining magnetization measurements with Nuclear Magnetic Resonance (NMR) and Muon Spin Relaxation (μSR), we have investigated the static magnetic properties and the spin dynamics as a function of the temperature. Moreover, the effect of the external pressure as well as of the infrared light irradiation have been explored through magnetometry and NMR measurements to determine the spin dynamics of the HS state. The photoinduced HS state, which can have a lifetime of several hours below 30 K, is characterized by spin dynamics in the MHz range, which persist at least down to 10 K. The application of an external pressure causes a progressive increase of the LS-HS crossover, which reaches room temperature for pressures around 10 kbar.

cond-mat.mtrl-sci

Evidences of spin-temperature in Dynamic Nuclear Polarization: an exact computation of the EPR spectrum

In dynamic nuclear polarization (DNP) experiments, the compound is driven out-of-equilibrium by microwave (MW) irradiation of the radical electron spins. Their stationary state has been recently probed via electron double resonance (ELDOR) techniques showing, at low temperature, a broad depolarization of the electron paramagnetic resonance (EPR) spectrum under microwave irradiation. In this theoretical manuscript, we develop a numerical method to compute exactly the EPR spectrum in presence of dipolar interactions. Our results reproduce the observed broad depolarisation and provide a microscopic justification for spectral diffusion mechanism. We show the validity of the spin-temperature approach for typical radical concentration used in dissolution DNP protocols. In particular once the interactions are properly taken into account, the spin-temperature is consistent with the non-monotonic behavior of the EPR spectrum with a wide minimum around the irradiated frequency.

cond-mat.str-el