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S. Bertaina

Publications and source records attributed to S. Bertaina.

At least 19 recordsLinked to original sources

Precision hyperfine spectroscopy of an individual nuclear-spin-9/2

Single-spin magnetic resonance spectroscopy promises to yield structural and chemical information at the level of individual atoms or molecules, in a non-invasive way. Here, we use an Er3+ paramagnetic center in a CaWO4 crystal, detected by microwave photon counting at 10 mK, as a nanoscale magnetic sensor to measure the NMR spectrum of a proximal individual nuclear-spin-9/2 93Nb impurity with Hertz spectral resolution. From these measurements, we determine the 93Nb insertion site, its position relative to the Er3+ , and its complete quadrupolar tensor. We moreover harness the high spectral resolution of our measurements to establish the presence of two previously unobserved terms in the spin Hamiltonian. The first describes a coupling between the Er3+ spin and the 93Nb nuclear quadrupole; it possibly originates from a spin-dependent electrostatic interaction between the two systems. The second is a nuclear hexadecapolar term, and may be caused by the coupling of the electric field third derivative to the 93Nb nuclear hexadecapolar moment.

quant-ph

Exploring electron spin dynamics in spin chains using defects as a quantum probe

We investigate the quantum dynamics of the electron spin resonance of topological defects (edge state) in dimerized chains. These objects are discontinuities of the spin chain protected by the properties of the global system leading to a quantum many-body multiplet protected from the environment decoherence. Despite recent achievements in the realization of isolated and finite spin chains, the potential implementation in quantum devices needs the knowledge of the relaxation and decoherence sources. Our study reveals that electron spin lattice relaxation is governed at lowest temperatures by phonon-bottlenecked process and at high temperature by the chain dimerization gap. We show that the inter edge-state effective dipolar field is reduced by the intrachain exchange coupling leading to a longer coherence time than isolated ions at equivalent concentration. Ultimately, we demonstrate that the homogeneous broadening is governed by the intra-chain dipolar field, and we establish design principles for optimizing coherence in future materials.

cond-mat.str-el

All-microwave spectroscopy and polarization of individual nuclear spins in a solid

We report magnetic resonance spectroscopy measurements of individual nuclear spins in a crystal coupled to a neighbouring paramagnetic center, detected using microwave fluorescence at millikelvin temperatures. We observe real-time quantum jumps of the nuclear spin state, a proof of their individual nature. By driving the forbidden transitions of the coupled electron-nuclear spin system, we also achieve single-spin solid-effect dynamical nuclear polarization. Relying exclusively on microwave driving and microwave photon counting, the methods reported here are in principle applicable to a large number of electron-nuclear spin systems, in a wide variety of samples.

quant-ph

Electron Paramagnetic Resonance spectroscopy of a scheelite crystal using microwave photon counting

Counting the microwave photons emitted by an ensemble of electron spins when they relax radiatively has recently been introduced as a sensitive new method for electron paramagnetic resonance spectroscopy at millikelvin temperatures. Here, we apply this spin fluorescence method to a scheelite crystal of CaWO4, finding some known ($\mathrm{Er}^{3+}$, $\mathrm{Yb}^{3+}$, $\mathrm{Nd}^{3+}$ and $\mathrm{Fe}^{3+}$) and other unknown paramagnetic impurities. Investigating the zero nuclear spin isotope ($I=0$) transition of $\mathrm{Er}^{3+}:\mathrm{CaWO}_4$ as a model system, we provide a quantitative analysis of the time-dependent photon counting rate following an excitation pulse, as a function of its power. The achieved signal-to-noise ratio is found to be an order of magnitude higher than the one obtained by inductively-detected Hahn echo under identical conditions. Finally, we use spin fluorescence spectroscopy at low excitation power to probe the properties of rare-earth-ions close to a metallic wire deposited on the surface; our data reveal line distortion caused by the mechanical strain imparted by the thermal contractions of the metal relative to the underlying crystal. Coherent oscillations are also observed for the most highly strained ions.

quant-ph

Sustaining Rabi oscillations by using a phase-tunable image drive

Recent electron spin resonance experiments on CaWO$_4$:Gd$^{3+}$ and on other magnetic impurities have demonstrated that sustained Rabi oscillations can be created by driving a magnetic moment with a microwave field frequency slightly larger than the Larmor frequency and tuned to the Floquet resonance together with another microwave field (image drive). These observations are confirmed by the new experimental results reported in this paper. We investigate several mechanisms of decoherence and dissipation by using a combination of numerical and analytical techniques. The first microscopic model describes a magnetic moment in external magnetic fields, interacting with a bath of two-level systems acting as a source of decoherence and dissipation. The second model describes a collection of the identical, interacting magnetics moments, all subject to the same magnetic fields. In this case, the many-body interactions causes a decay of the Rabi oscillations. In addition, we also study the effect of the inhomogeneity of the microwave radiation on the decay of the Rabi oscillations. Our simulation results show that the dynamics of a magnetic moment subject to the two microwave fields with different frequencies and in contact with an environment is highly nontrivial. We show that under appropriate conditions, and in particular at the Floquet resonance, the magnetization exhibits sustained Rabi oscillations, in some cases with additional beatings. Although these two microscopic models separately describe the experimental data well, a simulation study that simultaneously accounts for both types of interactions is currently prohibitively costly. To gain further insight into the microscopic dynamics of these two different models, we study the time dependence of the bath and system energy and of the correlations of the spins, data that is not readily accessible experimentally.

cond-mat.other

On-Chip Detection of Electronuclear Transitions in the $^{155,157}$Gd Multilevel Spin System

The properties of rare-earth elements diluted in non-magnetic crystals make them a promising candidate for a quantum memory due to their limited Hilbert space. The control and readout of the qubit states require a highly sensitive measurement and large coupling of the spin ensemble with the electro-magnetic mode of a superconducting resonator. We report sensitive detection of forbidden transitions of electronuclear states from the minority species of $^{155}$Gd and $^{157}$Gd isotopes which opens the possibility of connecting quantum states with very different spin projections. Cavity perturbation measurements seen in the reflected signal allows the detection of about 7.6$\times10^{7}$ spins and the measurement of spin decoherence rate and spin-photon coupling strength.

quant-ph

Superlattice Induced by Charge Order in the Organic Spin Chain (TMTTF)$_2X$ ($X=$ SbF$_6$, AsF$_6$ and PF$_6$) Revealed by High Field EPR

We have investigated the charge ordering phase of the quasi one dimensional quantum antiferromagnet (TMTTF)$_2X$ ($X=$ SbF$_6$, AsF$_6$ and PF$_6$) using high fields/frequencies electron paramagnetic resonance. In addition to the uniform displacement of the counter anions involved in the charge order phase, we report the existence of a superlattice between the spin chains in the direction $c$, caused by the space modulation of the charge order. When the field is high enough, the magnetic decoupling of the spin chains allows us to estimate the interaction between the chains, $J_c<1$~mK, three orders of magnitude lower than expected from the mean field theory.

cond-mat.str-el

Quantum dynamics of Mn$^{2+}$ in dimethylammonium magnesium formate

Dimethylammonium magnesium formate, [(CH$_3$)$_2$NH$_2$][Mg(HCOO)$_3$] or DMAMgF, is a model to study high temperature hybrid perovskite-like dielectrics. This compound displays a phase transition from para to ferroelectric at about 260~K. Using multifrequency electron spin resonance in continuous wave and pulsed modes, we herein present the quantum dynamic of Mn$^{2+}$ ion probe in DMAMgF. In the high temperature paraelectric phase, we observe a large distribution of the zero field splitting that is attributed to high local disorder and further supported by DFT computations. In the low temperature ferroelectric phase, a single structure phase is detected and shown to contain two magnetic structures. The complex EPR signals were identifed by the means of Rabi oscillation method combined to crystal fields kernel density estimation.

cond-mat.mtrl-sci

Electron Spin Resonance of Defects in Spin Chains. o-(DMTTF)2X : a versatile system behaving like molecular magnet

The paper presents the Electron Paramagnetic Resonance study of defects in the spin chain o- (DMTTF)2X family using continuous wave and pulsed techniques. The defects in spin chains are strongly correlated and present similar microscopic structure as a molecular magnet. By means of 2D-HYSCORE and DFT calculations we show a strong reduction of hyperfine coupling between the defects and the nuclear spin bath. We assume that the reduction is due to the Heisenberg exchange interaction which screens the effect of the nuclei.

cond-mat.str-el

Coherent spin dynamics of solitons in the organic spin chain compounds ($o$-DMTTF)$_2X$ ($X$ = Cl, Br)

We studied the magnetic properties, in particular dynamics, of the correlated spins associated with natural defects in the organic spin chain compounds ($o$-DMTTF)$_2X$ ($X$ = Br, Cl) by means of electron spin resonance (ESR) spectroscopy. Both materials exhibit spin-Peierls transitions at temperatures around 50 K [P. Foury-Leylekian et al. Phys. Rev. B 84, 195134 (2011)], which allow a separation of the properties of defects inside the chains from the magnetic response of the spin chains. Indeed, continuous wave ESR measurements performed over a wide temperature range evidence the evolution of the spin dynamics from being governed by the spins in the chains at elevated temperatures to a low-temperature regime which is dominated by defects within the spin-dimerized chains. Such defects polarize the antiferromagnetically coupled spins in their vicinity, thereby leading to a finite local alternating magnetization around the defect site which can be described in terms of a soliton, i.e. a spin 1/2 quasiparticle built of many correlated spins, pinned to the defect. In addition, contributions of triplon excitations of the spin-dimerized state to the ESR response below the transition temperature were observed which provides a spectroscopic estimate for the spin-gap of the studied systems. Moreover, details of spin dynamics deep in the spin-Peierls phase were investigated by pulse ESR experiments which revealed Rabi-oscillations as signatures of coherent spin dynamics. From a comparison of the characteristic damping times of the Rabi oscillations with measurements of the spin relaxation times by means of primary-echo decay and CPMG methods it becomes evident that inhomogeneities in local magnetic fields strongly contribute to the soliton decoherence.

cond-mat.str-el

Sensitive spin detection using an on-chip SQUID-waveguide resonator

Precise detection of spin resonance is of paramount importance to achieve coherent spin control in quantum computing. We present a novel setup for spin resonance measurements, which uses a dc-SQUID flux detector coupled to an antenna from a coplanar waveguide. The SQUID and the waveguide are fabricated from 20~nm Nb thin film, allowing high magnetic field operation with the field applied parallel to the chip. We observe a resonance signal between the first and third excited states of Gd spins $S=7/2$ in a CaWO$_4$ crystal, relevant for state control in multi-level systems.

cond-mat.mes-hall

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.

cond-mat.mes-hall

Forbidden coherent transfer observed between two realizations of quasi-harmonic spin system

The multi-level system $^{55}$Mn$^{2+}$ is used to generate two pseudo-harmonic level systems, as representations of the same electronic sextuplet at different nuclear spin projections. The systems are coupled using a forbidden nuclear transition induced by the crystalline anisotropy. We demonstrate Rabi oscillations between the two representations in conditions similar to two coupled quasi-harmonic quantum oscillators. Rabi oscillations are performed at a detuned pumping frequency which matches energy difference between electro-nuclear states of different oscillators. We measure a coupling stronger than the decoherence rate, to indicate the possibility fast information exchange between the systems.

cond-mat.str-el

High Curie temperature Mn 5 Ge 3 thin films produced by non-diffusive reaction

Polycrystalline Mn 5 Ge 3 thin films were produced on SiO 2 using magnetron sputtering and reactive diffusion (RD) or non-diffusive reaction (NDR). In situ X-ray diffraction and atomic force microscopy were used to determine the layer structures, and magnetic force microscopy, superconducting quantum interference device and ferromagnetic resonance were used to determine their magnetic properties. RD-mediated layers exhibit similar magnetic properties as MBE-grown monocrystalline Mn 5 Ge 3 thin films, while NDR-mediated layers show magnetic properties similar to monocrystalline C-doped Mn 5 Ge 3 C x thin films with $0.1 \leq x \leq 0.2.$ NDR appears as a CMOS-compatible efficient method to produce good magnetic quality high-curie temperature Mn 5 Ge 3 thin films.

cond-mat.mes-hall

Ferromagnetic resonance and magnetic damping in C-doped Mn5Ge3

Ferromagnetic resonance (FMR) was used to investigate the static and dynamic magnetic properties of carbon-doped Mn5Ge3 (C$_{0.1}$ and C$_{0.2}$) thin films grown on Ge(111). The temperature dependence of magnetic anisotropy shows an increased perpendicular magneto-crystalline contribution at 80K with an in-plane easy axis due to the large shape contribution. We find that our samples show a small FMR linewidth (corresponding to an intrinsic magnetic damping parameter $α$=0.005), which is a measure of the spin relaxation and directly related with the magnetic and structural quality of the material. In the perpendicular-to-plane geometry, the FMR linewidth shows a minimum at around 200K for all the samples, which seems to be not correlated to the C-doping. The magnetic relaxation parameters have been determined and indicate the two-magnon scattering as the main extrinsic contribution. We observe a change in the main contribution from scattering centres in Mn5Ge3C0.2 at low temperatures, which could be related to the minimum in linewidth.

cond-mat.mtrl-sci

Resonant single and multi-photon coherent transitions in a detuned regime

We performed quantum manipulations of the multi-level spin system S=5/2 of a Mn$^{2+}$ ion, by means of a two-tone pulse drive. The detuning between the excitation and readout radio frequency pulses allows one to select the number of photons involved in a Rabi oscillation as well as increase the frequency of this nutation. Thus detuning can lead to a resonant multi-photon process. Our analytical model for a two-photon process as well as a numerical generalization fit well the experimental findings, with implications in the use of multi-level spin systems as tunable solid state qubits.

cond-mat.mes-hall

Anisotropy of the molecular magnet V$_{15}$ spin Hamiltonian detected by high-field electron spin resonance

The molecular compound K$_6$[V$^{IV}_{15}$As$^{III}_6$O$_{42}$(H$_2$O)] $\cdot$ 8H$_2$O, in short V$_{15}$, has shown important quantum effects such as coherent spin oscillations. The details of the spin quantum dynamics depend on the exact form of the spin Hamiltonian. In this study, we present a precise analysis of the intramolecular interactions in V$_{15}$. To that purpose, we performed high-field electron spin resonance measurements at 120 GHz and extracted the resonance fields as a function of crystal orientation and temperature. The data are compared against simulations using exact diagonalization to obtain the parameters of the molecular spin Hamiltonian.

cond-mat.mes-hall

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.

cond-mat.mes-hall