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E. Coronado

Publications and source records attributed to E. Coronado.

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Strong spin-magnon coupling in a van der Waals magnet with tunable chiral symmetry

Quantum technologies require platforms that can coherently interface qubits with bosonic excitations. Photons have traditionally played this role in cavity quantum electrodynamics, but achieving the same goal using solid-state bosons remains challenging. Here we demonstrate strong and tunable spin-magnon coupling between molecular spin qubits and magnons in a van der Waals antiferromagnetic insulator. Using [Gd(W$_5$O$_{18}$)$_{2}$]$^{9-}$ as the spin ensemble and CrSBr as the magnonic resonator, we observe anticrossings and coherent hybridization, realizing magnon quantum electrodynamics for the first time. Crucially, by rotating the magnetic field, we can dynamically change the magnon symmetry from linear to chiral, enabling in-situ tuning of the coupling strength. Our results establish magnonic cavities as a platform for scalable chiral quantum optics with magnetic materials.

quant-ph

Spin liquid properties of the kagome material Cu$_3$(HOTP)$_2$

The metal-organic-framework (MOF) compound Cu$_3$(HOTP)$_2$, a.k.a. Cu$_3$(HHTP)$_2$, is a small-gap semiconductor containing a kagome lattice of antiferromagnetically coupled $S$=1/2 Cu$^\mathrm{II}$ spins with intra-layer nearest-neighbor exchange coupling $J \sim $ 2 K. The intra-layer $J$ value obtained from DFT+U calculations is shown to match with the experimental value for reasonable values of U. Muon spin relaxation confirms no magnetic ordering down to 50~mK and sees spin fluctuations diffusing on a 2D lattice, consistent with a quantum spin liquid (QSL) ground state being present within highly decoupled kagome layers. Reduction of the spin diffusion rate on cooling from the paramagnetic region to the low-temperature QSL region reflects quantum entanglement. It is also found that the layers become more strongly decoupled in the low-temperature QSL region. Comparison of results for the spin diffusion, magnetic susceptibility and specific heat in the QSL region suggests close proximity to a quantum critical point and a large density of low energy spinless electronic excitations. A Z$_2$-linear Dirac model for the spin excitations of the QSL is found to provide the best match with experiment.

cond-mat.str-el

Laser-induced Demagnetization in van der Waals $XY$- and Ising-like Antiferromagnets NiPS$_3$ and FePS$_3$

The critical behaviour of laser-induced changes in magnetic ordering is studied experimentally in two-dimensional zigzag antiferromagnets $XY$-like NiPS$_3$ and Ising-like FePS$_3$. To examine laser-induced dynamics in flakes of these compounds, we employ time-resolved exchange linear dichroism effect sensitive to zigzag magnetic ordering and independent of the orientation of the antiferromagnetic vector. In both compounds laser excitation in the vicinity of the absorption edge induces partial quenching of the antiferromagnetic ordering manifested by exchange linear dichroism reduction. The amplitude of the effect varies with temperature as the derivative of the antiferromagnetic vector and exhibits a critical behaviour with the exponents corresponding to $XY$- and Ising-models for NiPS$_3$ and FePS$_3$, respectively. Critical slowing down of the demagnetization in the vicinity of Néel temperature is found, however, only in FePS$_3$. In contrast, the increase of the demagnetization time near the ordering temperature in NiPS$_3$ is minor. We show that the difference in the demagnetization times correlates well with the spin specific heat in both compounds. Beyond the range of slowing down, the demagnetization times in NiPS$_3$ and FePS$_3$ are comparable, about 5 - 10 ps, and are longer than those reported earlier for CoPS$_3$ and considerably shorter than for MnPS$_3$. This points to the importance of the unquenched angular momentum of transition-metal ions in laser-induced demagnetization process.

cond-mat.mes-hall

Ultrafast laser-induced spin-lattice dynamics in the van der Waals antiferromagnet CoPS3

CoPS3 stands out in the family of the van der Waals antiferromagnets XPS3 (X=Mn, Ni, Fe, Co) due to the unquenched orbital momentum of the magnetic Co2+ ions which is known to facilitate the coupling of spins to both electromagnetic waves and lattice vibrations. Here, using a time-resolved magneto-optical pump-probe technique we experimentally study the ultrafast laser-induced dynamics of mutually correlated spins and lattice. It is shown that a femtosecond laser pulse acts as an ultrafast heater and thus results in the melting of the antiferromagnetic order. At the same time, the resonant pumping of the 4T1g - 4T2g electronic transition in Co2+ ions effectively changes their orbital momentum, giving rise to a mechanical force that moves the ions in the direction parallel to the orientation of their spins, thus generating a coherent Bg phonon mode at the frequency of about 4.7 THz.

cond-mat.mtrl-sci

Controlling magnetism with light in a zero orbital angular momentum antiferromagnet

Antiferromagnetic materials feature intrinsic ultrafast spin dynamics, making them ideal candidates for future magnonic devices operating at THz frequencies. A major focus of current research is the investigation of optical methods for the efficient generation of coherent magnons in antiferromagnetic insulators. In magnetic lattices endowed with orbital angular momentum, spin-orbit coupling enables spin dynamics through the resonant excitation of low-energy electric dipoles such as phonons and orbital resonances which interact with spins. However, in magnetic systems with zero orbital angular momentum, microscopic pathways for the resonant and low-energy optical excitation of coherent spin dynamics are lacking. Here, we consider experimentally the relative merits of electronic and vibrational excitations for the optical control of zero orbital angular momentum magnets, focusing on a limit case: the antiferromagnet manganese thiophoshate (MnPS3), constituted by orbital singlet Mn2+ ions. We study the correlation of spins with two types of excitations within its band gap: a bound electron orbital excitation from the singlet orbital ground state of Mn2+ into an orbital triplet state, which causes coherent spin precession, and a vibrational excitation of the crystal field that causes thermal spin disorder. Our findings cast orbital transitions as key targets for magnetic control in insulators constituted by magnetic centers of zero orbital angular momentum.

cond-mat.mtrl-sci

Controlling the anisotropy of a van der Waals antiferromagnet with light

Magnetic van der Waals materials provide an ideal playground for exploring the fundamentals of low-dimensional magnetism and open new opportunities for ultrathin spin processing devices. The Mermin-Wagner theorem dictates that as in reduced dimensions isotropic spin interactions cannot retain long-range correlations; the order is stabilized by magnetic anisotropy. Here, using ultrashort pulses of light, we demonstrate all-optical control of magnetic anisotropy in the two-dimensional van der Waals antiferromagnet NiPS$_3$. Tuning the photon energy in resonance with an orbital transition between crystal-field split levels of the nickel ions, we demonstrate the selective activation of a sub-THz two-dimensional magnon mode. The pump polarization control of the magnon amplitude confirms that the activation is governed by the instantaneous magnetic anisotropy axis emergent in response to photoexcitation of orbital states with a lowered symmetry. Our results establish pumping of orbital resonances as a universal route for manipulating magnetic order in low-dimensional (anti)ferromagnets.

cond-mat.mtrl-sci

Design of high-temperature f-block molecular nanomagnets through the control of vibration-induced spin relaxation

One of the main roadblocks that still hampers the practical use of molecular nanomagnets is their cryogenic working temperature. In the pursuit of rational strategies to design new molecular nanomagnets with increasing blocking temperature, ab initio methodologies play an important role by guiding synthetic efforts at the lab stage. Nevertheless, when evaluating vibration-induced spin relaxation, these methodologies are still far from being computationally fast enough to provide a useful predictive framework. Herein, we present an inexpensive first-principles method devoted to evaluating vibration-induced spin relaxation in molecular f-block single-ion magnets, with the important advantage of requiring only one CASSCF calculation. We use a case study to illustrate the method, and propose chemical modifications in the ligand environment with the aim of suppressing spin relaxation.

cond-mat.mes-hall

Design and Experimental Validation of a Software-Defined Radio Access Network Testbed with Slicing Support

Network slicing is a fundamental feature of 5G systems to partition a single network into a number of segregated logical networks, each optimized for a particular type of service, or dedicated to a particular customer or application. The realization of network slicing is particularly challenging in the Radio Access Network (RAN) part, where multiple slices can be multiplexed over the same radio channel and Radio Resource Management (RRM) functions shall be used to split the cell radio resources and achieve the expected behaviour per slice. In this context, this paper describes the key design and implementation aspects of a Software-Defined RAN (SD-RAN) experimental testbed with slicing support. The testbed has been designed consistently with the slicing capabilities and related management framework established by 3GPP in Release 15. The testbed is used to demonstrate the provisioning of RAN slices (e.g. preparation, commissioning and activation phases) and the operation of the implemented RRM functionality for slice-aware admission control and scheduling.

cs.NI

Enhancing Light Emission in Interface Engineered Spin-OLEDs Through Spin-Polarized Injection at High Voltages

The quest for a spin-polarized organic light emitting diode (spin-OLED) is a common goal in the emerging fields of molecular electronics and spintronics. In this device two ferromagnetic electrodes are used to enhance the electroluminescence intensity of the OLED through a magnetic control of the spin polarization of the injected carriers. The major difficulty is that the driving voltage of an OLED device exceeds of a few volts, while spin injection in organic materials is only efficient at low voltages. We report here the fabrication of a spin-OLED that uses a conjugated polymer as bipolar spin collector layer and ferromagnetic electrodes. Through a careful engineering of the organic/inorganic interfaces we have succeeded in obtaining a light-emitting device showing spin-valve effects at high voltages (up to 14 V). This has allowed us to detect a magneto-electroluminescence enhancement on the order of a 2.4 % at 9 V for the antiparallel configuration of the magnetic electrodes. This observation provides evidence for the long-standing fundamental issue of injecting spins from magnetic electrodes into the frontier levels of a molecular semiconductor. Our finding opens the way for the design of multifunctional devices coupling the light and the spin degrees of freedom.

cond-mat.mes-hall

Unveiling the limits in the coherence of spin qubits against magnetic noise

The realization of spin-based logical gates crucially depends on magnetically-coupled spin qubits. Thus, understanding decoherence when spin qubits are in close proximity will become a roadblock to overcome. Herein, we provide a general first-principles model that straightforwardly evaluates the spin bath effect on the qubit phase memory time $T_m$ . The method is applied to a ground-spin $J=8$ magnetic molecule 1 displaying atomic clock transitions, which remarkably increase $T_m$ at unusually high spin concentrations. Besides reproducing experimental $T_m$ values calculated by recent models in simple spin-1/2 systems, our approach unveils the causes that limit the coherence reached at the clock transitions in more challenging systems such as 1, where these previous models fail.

cond-mat.mes-hall

Force-free state in a superconducting single crystal and angle-dependent vortex helical instability

Superconducting 2H-NbSe2 single crystals show intrinsic low pinning values. Therefore, they are ideal materials with which to explore fundamental properties of vortices. (V, I) characteristics are the experimental data we have used to investigate the dissipation mechanisms in a rectangular shape 2H-NbSe2 single crystal. Particularly, we have studied dissipation behavior with magnetic fields applied in the plane of the crystal and parallel to the injected currents, i.e. in the force-free state where the vortex helical instability governs the vortex dynamics. In this regime, the data follow the elliptic critical state model and the voltage dissipation shows an exponential dependence.Moreover, this exponential dependence can be observed for in-plane applied magnetic fields up to 40 degrees off the current direction, which implies that the vortex helical instability plays a role in dissipation even out of the force-free configuration.

cond-mat.supr-con

Phase-transitions in spin-crossover thin films probed by graphene transport measurements

Future multi-functional hybrid devices might combine switchable molecules and 2D material-based devices. Spin-crossover compounds are of particular interest in this context since they exhibit bistability and memory effects at room temperature while responding to numerous external stimuli. Atomically-thin 2D materials such as graphene attract a lot of attention for their fascinating electrical, optical, and mechanical properties, but also for their reliability for room-temperature operations. Here, we demonstrate that thermally-induced spin-state switching of spin-crossover nanoparticle thin films can be monitored through the electrical transport properties of graphene lying underneath the films. Model calculations indicate that the charge carrier scattering mechanism in graphene is sensitive to the spin-state dependence of the relative dielectric constants of the spin-crossover nanoparticles. This graphene sensor approach can be applied to a wide class of (molecular) systems with tunable electronic polarizabilities.

cond-mat.mes-hall

Field dependence of the vortex core size probed by STM

We study the spatial distribution of the density of states (DOS) at zero bias N(r) in the mixed state of single and multigap superconductors. We provide an analytic expression for N(r) based on deGennes' relation between DOS and the order parameter that reproduces well Scanning Tunneling Microscopy (STM) data in several superconducting materials. In the single gap superconductor $β$-Bi$_2$Pd, we find that N(r) is governed by a length scale $ξ_H=\sqrt{ϕ_0/2πH}$, which decreases in rising fields. The vortex core size $\cal C$, defined via the slope of the order parameter at the vortex center, $\cal C$ $\propto (d Δ/dr |_{r \to 0})^{-1}$, differs from $ξ_H$ by a material dependent numerical factor. For two gap superconductors 2H-NbSe$_{1.8}$S$_{0.2}$ and 2H-NbS$_2$, we find that $\cal C$ is field independent and has the same value for both bands. We conclude that, independently of the magnetic field induced variation of the order parameter values in both bands, the spatial variation of the order parameter close to the vortex core is the same for all bands.

cond-mat.supr-con

Current rectification in a single molecule diode: the role of electrode coupling

We demonstrate large rectification ratios (> 100) in single-molecule junctions based on a metal-oxide cluster (polyoxometalate), using a scanning tunneling microscope (STM) both at ambient conditions and at low temperature. These rectification ratios are the largest ever observed in a single-molecule junction, and in addition these junctions sustain current densities larger than 10^5 A/cm^2. By following the variation of the I-V characteristics with tip-molecule separation we demonstrate unambiguously that rectification is due to asymmetric coupling to the electrodes of a molecule with an asymmetric level structure. This mechanism can be implemented in other type of molecular junctions using both organic and inorganic molecules and provides a simple strategy for the rational design of molecular diodes.

cond-mat.mes-hall

Zero-bias conductance peak in detached flakes of superconducting 2H-TaS$_2$ probed by scanning tunneling spectroscopy

We report an anomalous tunneling conductance with a zero bias peak in flakes of superconducting 2H-TaS$_2$ detached through mechanical exfoliation. To explain the observed phenomenon, we construct a minimal model for a single unit cell layer of superconducting 2H-TaS$_2$ with a simplified 2D Fermi surface and sign-changing Cooper pair wavefunction induced by Coulomb repulsion. Superconductivity is induced in the central $Γ$ pocket, where it becomes nodal. We show that weak scattering at the nodal Fermi surface, produced by non-perturbative coupling between tip and sample, gives Andreev states that lead to a zero bias peak in the tunneling conductance. We suggest that reducing dimensionality down to a few atom thick crystals could drive a crossover from conventional to sign changing pairing in the superconductor 2H-TaS$_2$.

cond-mat.supr-con

Scanning tunneling spectroscopy of layers of superconducting 2H-TaSe$_\textbf{2}$: Evidence for a zero bias anomaly in single layers

We report a characterization of surfaces of the dichalcogenide TaSe$_2$ using scanning tunneling microscopy and spectroscopy (STM/S) at 150 mK. When the top layer has the 2H structure and the layer immediately below the 1T structure, we find a singular spatial dependence of the tunneling conductance below 1 K, changing from a zero bias peak on top of Se atoms to a gap in between Se atoms. The zero bias peak is additionally modulated by the commensurate $3a_0 \times 3a_0$ charge density wave of 2H-TaSe$_2$. Multilayers of 2H-TaSe$_2$ show a spatially homogeneous superconducting gap with a critical temperature also of 1 K. We discuss possible origins for the peculiar tunneling conductance in single layers.

cond-mat.supr-con

Chiral charge order in the superconductor 2H-TaS2

We find chiral charge order in the superconductor 2H-TaS2 using Scanning Tunneling Microscopy and Spectroscopy (STM/S) at 0.1 K. Topographic images show hexagonal atomic lattice and charge density wave (CDW) with clockwise and counterclockwise charge modulations. Tunneling spectroscopy reveals the superconducting density of states, disappearing at Tc = 1.75 K and showing a wide distribution of values of the superconducting gap, centered around Δ=0.28 meV.

cond-mat.supr-con

Quadrature formulas for integrals transforms generated by orthogonal polynomials

By using the three-term recurrence equation satisfied by a family of orthogonal polynomials, the Christoffel-Darboux-type bilinear generating function and their asymptotic expressions, we obtain quadrature formulas for integral transforms generated by the classical orthogonal polynomials. These integral transforms, related to the so-called Poisson integrals, correspond to a modified Fourier Transform in the case of the Hermite polynomials, a Bessel Transform in the case of the Laguerre polynomials and to an Appell Transform in the case of the Jacobi polynomials.

math.NA