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I. Chiorescu

Publications and source records attributed to I. Chiorescu.

At least 19 recordsLinked to original sources

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

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

Quantum interference in asymmetric superconducting nanowire loops

Macroscopic phase coherence in superconductors enables quantum interference and phase manipulation at realistic device length scales. Numerous superconducting electronic devices are based on the modulation of the supercurrent in superconducting loops. While the overall behavior of symmetric superconducting loops have been studied, the effects of asymmetries in such devices remain under-explored and poorly understood. Here we report on an experimental and theoretical study of the flux modulation of the persistent current in a doubly-connected asymmetric aluminum nanowire loop. A model considering the length and electronic cross-section asymmetries in the loop provides a quantitative account of the observations. Comparison with experiments give essential parameters such as persistent and critical currents as well as the amount of asymmetry which can provide feedback into the design of superconducting quantum devices.

cond-mat.supr-con

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

A magnetic topological semimetal Sr1-yMn1-zSb2 (y, z< 0.1)

Weyl (WSMs) evolve from Dirac semimetals in the presence of broken time-reversal symmetry (TRS) or space-inversion symmetry. The WSM phases in TaAs-class materials and photonic crystals are due to the loss of space-inversion symmetry. For TRS-breaking WSMs, despite numerous theoretical and experimental efforts, few examples have been reported. In this Article, we report a new type of magnetic semimetal Sr1-yMn1-zSb2 (y,z<0.1) with nearly massless relativistic fermion behaviour (m*=0.04-0.05m0, where m0 is the free electron mass). This material exhibits a ferromagnetic order for 304K < T < 565K, but a canted antiferromagnetic order with a ferromagnetic component for T < 304K. The combination of relativistic fermion behaviour and ferromagnetism in Sr1-yMn1-zSb2 offers a rare opportunity to investigate the interplay between relativistic fermions and spontaneous TRS breaking.

cond-mat.mtrl-sci

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

Nearly massless Dirac fermions hosted by Sb square net in BaMnSb2

Layered compounds AMnBi2 (A=Ca, Sr, Ba, or rare earth element) have been established as Dirac materials. Dirac electrons generated by the two-dimensional (2D) Bi square net in these materials are normally massive due to the presence of a spin-orbital coupling (SOC) induced gap at Dirac nodes. Here we report that the Sb square net in an isostructural compound BaMnSb2 can host nearly massless Dirac fermions. We observed strong Shubnikov-de Haas (SdH) oscillations in this material. From the analyses of the SdH oscillations, we find key signatures of Dirac fermions, including light effective mass (~0.052m0; m0, mass of free electron), high quantum mobility (1280 cm2V-1S-1) and a Pi Berry phase accumulated along cyclotron orbit. Compared with AMnBi2, BaMnSb2 also exhibits much more significant quasi two-dimensional (2D) electronic structure, with the out-of-plane transport showing nonmetallic conduction below 120K and the ratio of the out-of-plane and in-plane resistivity reaching ~670. Additionally, BaMnSb2 also exhibits an antiferromagnetic order with a weak ferromagnetic component. The combination of nearly massless Dirac fermions on quasi-2D planes with a magnetic order makes BaMnSb2 an intriguing platform for seeking novel exotic phenomena of massless Dirac electrons.

cond-mat.mtrl-sci

Pi Berry phase and Zeeman splitting of TaP probed by high field magnetotransport measurements

The chiral anomaly-induced negative magnetoresistance and non-trivial Berry phase are two fundamental transport properties associated with the topological properties of Weyl fermions. In this work, we report the quantum transport of TaP single crystals in magnetic field up to 31T. Through the analyses of our magnetotransport data, we show TaP has the signatures of a Weyl state, including light effective quasiparticle masses, ultrahigh carrier mobility, as well as negative longitudinal magnetoresistance. Furthermore, we have generalized the Lifshitz-Kosevich formula for Shubnikov-de Haas (SdH) oscillations with multi-frequencies, and determined the non-trivial Berry phase of Pi for multiple Fermi pockets in TaP through the direct fitting of the quantum oscillations. In high fields, we also probed signatures of Zeeman splitting, from which the Landé g-factor is extracted.

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

NMR detection of dynamical processes in antiferroelectric nanoclusters during the order-disorder transition in NH4H2AsO4

We study the dynamics of inorganic antiferroelectric nanoclusters formed during an order-disorder transition and demonstrate the coexistence of the two phases in a region of 2-3 K around the transition temperature TN~215 K. Single crystals of NH4H2AsO4, a model hydrogen-bonded compound, show an antiferroelectric-paraelectric transition studied by means of highly sensitive magic angle spinning 15N NMR at 21.1 T. The phase co-existence is demonstrated by a double-peak structure of the chemical shift. Two-dimensional chemical exchange spectroscopy and spin-lattice relaxation time (T1) measurements show that the clusters are dynamic with sizes ~50 nm and lifetimes approaching seconds as T->TN. Their occupancy increases rapidly to fill the crystal volume below $T_N$. This study provides evidence for the commonality of the phase transitions in systems with electric properties and provides an improved spectroscopic method for such studies.

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

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.

cond-mat.str-el

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.

cond-mat.mes-hall

Level crossings and zero-field splitting in the \{Cr$_8$\}-cubane spin-cluster by inelastic neutron scattering and magnetization studies

Inelastic neutron scattering in variable magnetic field and high-field magnetization measurements, at the milikelvin temperature range, were performed to gain insight into the low-energy magnetic excitation spectrum and the field-induced level crossings in the molecular spin cluster \{Cr$_8$\}-cubane. These complementary techniques provide consistent estimates of the lowest level-crossing field. The overall features of the experimental data are explained using an isotropic Heisenberg model, based on three distinct exchange interactions linking the eight Cr$^{\text{III}}$ paramagnetic centers (spins $s = 3/2$), that is supplemented with a relatively large molecular magnetic anisotropy term for the lowest S=1 multiplet. It is noted that the existence of the anisotropy is clearly evident from the magnetic field dependence of the excitations in the INS measurements, while the magnetization measurements are not sensitive to its effects.

cond-mat.mes-hall

On-chip SQUID measurements in the presence of high magnetic fields

We report a low temperature measurement technique and magnetization data of a quantum molecular spin, by implementing an on-chip SQUID technique. This technique enables the SQUID magnetometery in high magnetic fields, up to 7 Tesla. The main challenges and the calibration process are detailed. The measurement protocol is used to observe quantum tunneling jumps of the S=10 molecular magnet, Mn12-tBuAc. The effect of transverse field on the tunneling splitting for this molecular system is addressed as well.

cond-mat.mes-hall

Spin transition in Gd$_3$N@C$_{80}$, detected by low-temperature on-chip SQUID technique

We present a magnetic study of the Gd$_3$N@C$_{80}$ molecule, consisting of a Gd-trimer via a Nitrogen atom, encapsulated in a C$_{80}$ cage. This molecular system can be an efficient contrast agent for Magnetic Resonance Imaging (MRI) applications. We used a low-temperature technique able to detect small magnetic signals by placing the sample in the vicinity of an on-chip SQUID. The technique implemented at NHMFL has the particularity to operate in high magnetic fields of up to 7 T. The Gd$_3$N@C$_{80}$ shows a paramagnetic behavior and we find a spin transition of the Gd$_3$N structure at 1.2 K. We perform quantum mechanical simulations, which indicate that one of the Gd ions changes from a $^8S_{7/2}$ state ($L=0, S=7/2$) to a $^7F_{6}$ state ($L=S=3, J=6$), likely due to a charge transfer between the C$_{80}$ cage and the ion.

cond-mat.mes-hall