Multi-photon Rabi oscillations in high spin paramagnetic impurity

We report on multiple photon monochromatic quantum oscillations (Rabi oscillations) observed by pulsed EPR (Electron Paramagnetic Resonance) of Mn$^{2+}$ (S=5/2) impurities in MgO. We find that when the microwave magnetic field is similar or large than the anisotropy splitting, the Rabi oscillations have a spectrum made of many frequencies not predicted by the S=1/2 Rabi model. We show that these new frequencies come from multiple photon coherent manipulation of the multi-level spin impurity. We develop a model based on the crystal field theory and the rotating frame approximation, describing the observed phenomenon with a very good agreement.Comment: International Conference: Resonance in Condensed Matter Altshuler 10

Magnetic strong coupling in a spin-photon system and transition to classical regime

We study the energy level structure of the Tavis-Cumming model applied to an ensemble of independent magnetic spins $s=1/2$ coupled to a variable number of photons. Rabi splittings are calculated and their distribution is analyzed as a functin of photon number $n_{\rm max}$ and spin system size $N$. A sharp transition in the distribution of the Rabi frequency is found at $n_{\rm max}\approx N$. The width of the Rabi frequency spectrum diverges as $\sqrt{N}$ at this point. For increased number of photons $n_{\rm max}>N$, the Rabi frequencies converge to a value proportional to $\sqrt{n_{\rm max}}$. This behavior is interpreted as analogous to the classical spin resonance mechanism where the photon is treated as a classical field and one resonance peak is expected. We also present experimental data demonstrating cooperative, magnetic strong coupling between a spin system and photons, measured at room temperature. This points towards quantum computing implementation with magnetic spins, using cavity quantum-electrodynamics techniques.Comment: Received 8 April 2010; revised manuscript received 17 June 2010; published 14 July 201

Entrapment of magnetic micro-crystals for on-chip electron spin resonance studies

On-chip Electron Spin Resonance (ESR) of magnetic molecules requires the ability to precisely position nanosized samples in antinodes of the electro-magnetic field for maximal magnetic interaction. A method is developed to entrap micro-crystals containing spins in a well defined location on a substrate's surface. Traditional cavity ESR measurements are then performed on a mesoscopic crystal at 34 GHz. Polycrystalline diluted Cr$^{5+}$ spins were entrapped as well and measured while approaching the lower limit of the ESR sensitivity. This method suggests the feasibility of on-chip ESR measurements at dilution refrigerator temperatures by enabling the positioning of samples atop an on-chip superconducting cavity.Comment: to appear in Journal of Applied Physic

Spin-Orbit Coupling Fluctuations as a Mechanism of Spin Decoherence

We discuss a general framework to address spin decoherence resulting from fluctuations in a spin Hamiltonian. We performed a systematic study on spin decoherence in the compound K$_6$[V$_{15}$As$_6$O$_{42}$(D$_2$O)] $\cdot$ 8D$_2$O, using high-field Electron Spin Resonance (ESR). By analyzing the anisotropy of resonance linewidths as a function of orientation, temperature and field, we find that the spin-orbit term is a major decoherence source. The demonstrated mechanism can alter the lifetime of any spin qubit and we discuss how to mitigate it by sample design and field orientation.Comment: submitte

Tunable multi-photon Rabi oscillations in an electronic spin system

We report on multi-photon Rabi oscillations and controlled tuning of a multi-level system at room temperature (S=5/2 for Mn2+:MgO) in and out of a quasi-harmonic level configuration. The anisotropy is much smaller than the Zeeman splittings, such as the six level scheme shows only a small deviation from an equidistant diagram. This allows us to tune the spin dynamics by either compensating the cubic anisotropy with a precise static field orientation, or by microwave field intensity. Using the rotating frame approximation, the experiments are very well explained by both an analytical model and a generalized numerical model. The calculated multi-photon Rabi frequencies are in excellent agreement with the experimental data

Photon and spin dependence of the resonance lines shape in the strong coupling regime

We study the quantum dynamics of a spin ensemble coupled to cavity photons. Recently, related experimental results have been reported, showing the existence of the strong coupling regime in such systems. We study the eigenenergy distribution of the multi-spin system (following the Tavis-Cummings model) which shows a peculiar structure as a function of the number of cavity photons and of spins. We study how this structure causes changes in the spectrum of the admittance in the linear response theory, and also the frequency dependence of the excited quantities in the stationary state under a probing field. In particular, we investigate how the structure of the higher excited energy levels changes the spectrum from a double-peak structure (the so-called vacuum field Rabi splitting) to a single peak structure. We also point out that the spin dynamics in the region of the double-peak structure corresponds to recent experiments using cavity ringing while in region of the single peak structure, it corresponds to the coherent Rabi oscillation in a driving electromagnetic filed. Using a standard Lindblad type mechanism, we study the effect of dissipations on the line width and separation in the computed spectra. In particular, we study the relaxation of the total spin in the general case of a spin ensemble in which the total spin of the system is not specified. The theoretical results are correlated with experimental evidence of the strong coupling regime, achieved with a spin 1/2 ensemble

Author Correction:Experimental protection of quantum coherence by using a phase-tunable image drive (Scientific Reports, (2020), 10, 1, (21643), 10.1038/s41598-020-77047-5)

The original version of this Article contained an error

Decoherence window and electron-nuclear cross-relaxation in the molecular magnet V 15

Rabi oscillations in the V_15 Single Molecule Magnet (SMM) embedded in the surfactant DODA have been studied at different microwave powers. An intense damping peak is observed when the Rabi frequency Omega_R falls in the vicinity of the Larmor frequency of protons w_N, while the damping time t_R of oscillations reaches values 10 times shorter than the phase coherence time t_2 measured at the same temperature. The experiments are interpreted by the N-spin model showing that t_R is directly associated with the decoherence via electronic/nuclear spin cross-relaxation in the rotating reference frame. It is shown that this decoherence is accompanied with energy dissipation in the range of the Rabi frequencies w_N - sigma_e < Omega_R < w_N, where sigma_e is the mean super-hyperfine field (in frequency units) induced by protons at SMMs. Weaker damping without dissipation takes place outside this dissipation window. Simple local field estimations suggest that this rapid cross-relaxation in resonant microwave field observed for the first time in SMMV_15 should take place in other SMMs like Fe_8 and Mn_12 containing protons, too

Multiphoton coherent manipulation in large-spin qubits

Large spin Mn2+ ions (S=5/2) diluted in a non-magnetic MgO matrix of high crystalline symmetry are used to realize a six level system that can be operated by means of multi-photon coherent Rabi oscillations. This spin system has a very small anisotropy which can be tuned in-situ to reversibly transform the system between harmonic and non-harmonic level configurations. Decoherence effects are strongly suppressed as a result of the quasi-isotropic electron interaction with the crystal field and with the 55Mn nuclear spins. These results suggest new ways of manipulating, reading and resetting spin quantum states which can be applied to encode a qubit across several quantum levels.Comment: Published versio