Spin Excitations Research Articles

Exchange Interactions and Intermolecular Hybridization in a Spin-1/2 Nanographene Dimer.

Phenalenyl is a radical nanographene with a triangular shape hosting an unpaired electron with spin S = 1/2. The open-shell nature of the phenalenyl is expected to be retained in covalently bonded networks. As a first step, we report synthesis of the phenalenyl dimer by combining in-solution synthesis and on-surface activation and its characterization on Au(111) and on a NaCl decoupling layer by means of inelastic electron tunneling spectroscopy (IETS). IETS shows inelastic steps that are identified as singlet-triplet excitation arising from interphenalenyl exchange. Spin excitation energies with and without the NaCl decoupling layer are 48 and 41 meV, respectively, indicating significant renormalization due to exchange with Au(111) electrons. Furthermore, third-neighbor hopping-induced interphenalenyl hybridization is fundamental to explaining the position-dependent bias asymmetry of the inelastic steps and activation of kinetic interphenalenyl exchange. Our results pave the way for bottom-up synthesis of S = 1/2 spin-lattices with large exchange interactions.

Highly Efficient Spin Transport in a Paramagnetic Insulator at Room Temperature

AbstractThe exploration of new materials exhibiting excellent spin transport properties, particularly those capable of efficiently transmitting pure spin currents at room temperature, is a crucial aspect of spintronics. This work reports the observation of room‐temperature spin transport in a paramagnetic insulator Gd3Ga5O12 (GGG). By measuring the longitudinal spin Seebeck voltage, spin Hall magnetoresistance, and anomalous Hall resistance in a Y3Fe5O12 (YIG)/GGG/Pt heterostructure at room temperature, the spin current is found to propagate in GGG up to a distance of 7 nm through the paramagnons, which are the collective excitations of the local spin within the paramagnet. Remarkably, this spin propagation phenomenon occurs at a small magnetic field and irrespective of whether the spin current injected into GGG is thermally induced from YIG or electrically generated through the spin Hall effect of Pt. Moreover, the inclusion of a thin GGG spacer layer increases the thermal spin current from YIG to Pt by 31%. Calculations based on the diffusive magnon transport model indicate high spin conductance at the GGG/Pt interface. These findings highlight the potential of a wide range of paramagnetic materials in facilitating spin transport and advancing the development of spintronic devices.

Signature of spin-phonon coupling driven charge density wave in a kagome magnet

The intertwining between spin, charge, and lattice degrees of freedom can give rise to unusual macroscopic quantum states, including high-temperature superconductivity and quantum anomalous Hall effects. Recently, a charge density wave (CDW) has been observed in the kagome antiferromagnet FeGe, indicative of possible intertwining physics. An outstanding question is that whether magnetic correlation is fundamental for the spontaneous spatial symmetry breaking orders. Here, utilizing elastic and high-resolution inelastic x-ray scattering, we observe a c-axis superlattice vector that coexists with the 2times2times1 CDW vectors in the kagome plane. Most interestingly, between the magnetic and CDW transition temperatures, the phonon dynamical structure factor shows a giant phonon-energy hardening and a substantial phonon linewidth broadening near the c-axis wavevectors, both signaling the spin-phonon coupling. By first principles and model calculations, we show that both the static spin polarization and dynamic spin excitations intertwine with the phonon to drive the spatial symmetry breaking in FeGe.

Continuous Spin Excitations in the Three-Dimensional Frustrated Magnet K_{2}Ni_{2}(SO_{4})_{3}.

Continuous spin excitations are widely recognized as one of the hallmarks of novel spin states in quantum magnets, such as quantum spin liquids (QSLs). Here, we report the observation of such kind of excitations in K_{2}Ni_{2}(SO_{4})_{3}, which consists of two sets of intersected spin-1 (Ni^{2+}) trillium lattices. Our inelastic neutron scattering measurement on single crystals clearly shows a dominant excitation continuum, which exhibits a distinct temperature-dependent behavior from that of spin waves, and is rooted in strong quantum spin fluctuations. Further using the self-consistent-Gaussian-approximation method, we determine that the fourth- and fifth-nearest-neighbor exchange interactions are dominant. These two bonds together form a unique three-dimensional network of corner-sharing tetrahedra, which we name as a "hypertrillium" lattice. Our results provide direct evidence for the existence of QSL features in K_{2}Ni_{2}(SO_{4})_{3} and highlight the potential for the hypertrillium lattice to host frustrated quantum magnetism.

Anomalous Laser-Fluence Dependence of Electron Spin Excitation in CdS Colloidal Quantum Dots: Surface Effects.

Electron spin dynamics in CdS quantum dots (QDs) with hole acceptor 1-octanethiol organic molecules are investigated by time-resolved ellipticity spectroscopy. An anomalous dependence of laser fluences on electron spin excitation for the first time is reported. Increasing the laser fluence, the electron spin is switched from one direction to an antiparallel direction (spin direction switching, SDS) when adding enough 1-octanethiol hole acceptors in an air atmosphere. The analysis shows that the electron spin direction changes from heavy hole excitation defined to spin-orbit split hole excitation defined. In as-grown CdS QDs with native ligands, laser-fluence-dependent SDS phenomena are absent. Electron wave function spread into 1-octanethiol molecules is demonstrated to be important for the presence of SDS phenomena. The finding here thus reveals the importance of surface conditions on electron spin excitation processes in semiconductor QDs and that the surface can be used as an important factor to manipulate the spin.

Integrating magnons for quantum information

Magnons, the quanta of collective spin excitations in magnetically ordered materials, have distinct properties that make them uniquely appealing for quantum information applications. They can have ultra-small wavelengths down to the nanometer scale even at microwave frequencies. They can provide coupling to a diverse set of other quantum excitations, and their inherently gyrotropic dynamics forms the basis for pronounced nonreciprocities. In this article, we discuss what the current research challenges are for integrating magnetic materials into quantum information systems and provide a perspective on how to address them.

Complete field-induced spectral response of the spin-1/2 triangular-lattice antiferromagnet CsYbSe2

Fifty years after Anderson’s resonating valence-bond proposal, the spin-1/2 triangular-lattice Heisenberg antiferromagnet (TLHAF) remains the ultimate platform to explore highly entangled quantum spin states in proximity to magnetic order. Yb-based delafossites are ideal candidate TLHAF materials, which allow experimental access to the full range of applied in-plane magnetic fields. We perform a systematic neutron scattering study of CsYbSe2, first proving the Heisenberg character of the interactions and quantifying the second-neighbor coupling. We then measure the complex evolution of the excitation spectrum, finding extensive continuum features near the 120°-ordered state, throughout the 1/3-magnetization plateau and beyond this up to saturation. We perform cylinder matrix-product-state (MPS) calculations to obtain an unbiased numerical benchmark for the TLHAF and spectacular agreement with the experimental spectra. The measured and calculated longitudinal spectral functions reflect the role of multi-magnon bound and scattering states. These results provide valuable insight into unconventional field-induced spin excitations in frustrated quantum materials.

Long-lived spin waves in a metallic antiferromagnet

Collective spin excitations in magnetically ordered crystals, called magnons or spin waves, can serve as carriers in novel spintronic devices with ultralow energy consumption. The generation of well-detectable spin flows requires long lifetimes of high-frequency magnons. In general, the lifetime of spin waves in a metal is substantially reduced due to a strong coupling of magnons to the Stoner continuum. This makes metals unattractive for use as components for magnonic devices. Here, we present the metallic antiferromagnet CeCo2P2, which exhibits long-living magnons even in the terahertz (THz) regime. For CeCo2P2, our first-principle calculations predict a suppression of low-energy spin-flip Stoner excitations, which is verified by resonant inelastic X-ray scattering measurements. By comparison to the isostructural compound LaCo2P2, we show how small structural changes can dramatically alter the electronic structure around the Fermi level leading to the classical picture of the strongly damped magnons intrinsic to metallic systems. Our results not only demonstrate that long-lived magnons in the THz regime can exist in bulk metallic systems, but they also open a path for an efficient search for metallic magnetic systems in which undamped THz magnons can be excited.

Dynamical electric characteristics of a quantum paramagnet

We consider the quantum paramagnet with the coupling between spin and electric degrees of freedom. The dynamical electric characteristics of the system under the action of the ac electric field are calculated. It is shown that for the closed system the quadrupole spin moment oscillates with the frequency of the ac field. The oscillations are modulated by the Rabi-like frequency, while the amplitude of the modulation is minimal at resonance, at which the frequency of the electric field is equal to the double energy of spin excitation of the paramagnet. The open system in the steady-state regime manifests only oscillations with the frequency of the ac field. The calculated dynamical electric susceptibility is nonzero only for nonzero dc magnetic field, and, depending on the values of the single-ion magnetic anisotropy, can manifest nonmonotonic dependence on temperature, dc electric and magnetic fields.

Solution phase high repetition rate laser pump x-ray probe picosecond hard x-ray spectroscopy at the Stanford Synchrotron Radiation Lightsource.

We present a dedicated end-station for solution phase high repetition rate (MHz) picosecond hard x-ray spectroscopy at beamline 15-2 of the Stanford Synchrotron Radiation Lightsource. A high-power ultrafast ytterbium-doped fiber laser is used to photoexcite the samples at a repetition rate of 640 kHz, while the data acquisition operates at the 1.28 MHz repetition rate of the storage ring recording data in an alternating on-off mode. The time-resolved x-ray measurements are enabled via gating the x-ray detectors with the 20 mA/70 ps camshaft bunch of SPEAR3, a mode available during the routine operations of the Stanford Synchrotron Radiation Lightsource. As a benchmark study, aiming to demonstrate the advantageous capabilities of this end-station, we have conducted picosecond Fe K-edge x-ray absorption spectroscopy on aqueous [FeII(phen)3]2+, a prototypical spin crossover complex that undergoes light-induced excited spin state trapping forming an electronic excited state with a 0.6-0.7 ns lifetime. In addition, we report transient Fe Kβ main line and valence-to-core x-ray emission spectra, showing a unique detection sensitivity and an excellent agreement with model spectra and density functional theory calculations, respectively. Notably, the achieved signal-to-noise ratio, the overall performance, and the routine availability of the developed end-station have enabled a systematic time-resolved science program using the monochromatic beam at the Stanford Synchrotron Radiation Lightsource.

Momentum-independent magnetic excitation continuum in the honeycomb iridate H3LiIr2O6

Understanding the interplay between the inherent disorder and the correlated fluctuating-spin ground state is a key element in the search for quantum spin liquids. H3LiIr2O6 is considered to be a spin liquid that is proximate to the Kitaev-limit quantum spin liquid. Its ground state shows no magnetic order or spin freezing as expected for the spin liquid state. However, hydrogen zero-point motion and stacking faults are known to be present. The resulting bond disorder has been invoked to explain the existence of unexpected low-energy spin excitations, although data interpretation remains challenging. Here, we use resonant X-ray spectroscopies to map the collective excitations in H3LiIr2O6 and characterize its magnetic state. In the low-temperature correlated state, we reveal a broad bandwidth of magnetic excitations. The central energy and the high-energy tail of the continuum are consistent with expectations for dominant ferromagnetic Kitaev interactions between dynamically fluctuating spins. Furthermore, the absence of a momentum dependence to these excitations are consistent with disorder-induced broken translational invariance. Our low-energy data and the energy and width of the crystal field excitations support an interpretation of H3LiIr2O6 as a disordered topological spin liquid in close proximity to bond-disordered versions of the Kitaev quantum spin liquid.

Deeply nonlinear excitation of self-normalized short spin waves.

Spin waves are ideal candidates for wave-based computing, but the construction of magnetic circuits is blocked by a lack of an efficient mechanism to excite long-running exchange spin waves with normalized amplitudes. Here, we solve the challenge by exploiting a deeply nonlinear phenomenon for forward volume spin waves in 200-nm-wide nanoscale waveguides and validate our concept using microfocused Brillouin light scattering spectroscopy. An unprecedented nonlinear frequency shift of more than 2 GHz is achieved, corresponding to a magnetization precession angle of 55° and enabling the excitation of spin waves with wavelengths down to 200 nm. The amplitude of the excited spin waves is constant and independent of the input microwave power due to the self-locking nonlinear shift, enabling robust adjustment of the spin-wave amplitudes in future on-chip magnonic integrated circuits.

The peculiar SHG behaviour of Co-5,10,15,20-tetraphenilporphyrinate in the solid state. An experimental and theoretical study

We prepared and investigated the SHG behavior in the solid state of the Cobalt 5,10,15,20-tetraphenylporphyrinate that crystallizes in the acentric I4¯2d space group. The compound was synthesized and characterized, and the Second Harmonic Generation (SHG) response of a powdered sample was measured through a 1.907 μm pulsed laser radiation. During laser irradiation, a gradual increase of the intensity of the SH signal was observed until, after a few minutes, it reached a plateau of about fifty times the initial value. We attempted to understand the origin of this peculiar SHG behavior, both through experimental analysis and theoretical calculations. Mass spectrometry, absorption, emission, and vibrational spectroscopies in solution combined with powder X-ray diffraction analysis in solid state, both before and after irradiation, do not evidence any chemical degradation, phase transition or amorphization process. Theoretical calculations on little fragments of the Co-TPP structure simulate appropriately the structural feature of the complex and its initial experimental SHG response. UV–VIS and EPR spectra collected in the solid state before and after irradiation, in conjunction with DFT/B3LYP optimization of excited spin states and TDDFT calculation, highlight a change in the electronic and/or spin state due to the irradiation of the complex.

Chiral Excitation of Exchange Spin Waves Using Gold Nanowire Grating

We propose an experimental method for the unidirectional excitation of spin waves. By structuring Au nanowire arrays within a coplanar waveguide onto a thin yttrium iron garnet (YIG) film, we observe a chiral coupling between the excitation field geometry of the nanowire grating and several well-resolved propagating magnon modes. We report a propagating spin wave spectroscopy study with unprecedented spectral definition, wavelengths down to 130 nm and attenuation lengths well above 100 μm over the 20 GHz frequency band. The proposed experiment paves the way for future non-reciprocal magnonic devices.

Anderson–Fano resonances in Fock space: Adding electrons to two-dimensional materials in strong magnetic fields

The structure of the Hilbert–Fock space of electronic configurations determines the properties of atoms, molecules, and solids. A nontrivial example of such a structure at the single-particle level is described by Anderson–Fano resonances of localized states coupled to a continuum. Here we describe Anderson–Fano resonances in the Fock space of electronic configurations which can be realized by adding electrons to two-dimensional materials in a strong magnetic field. The resonances manifest themselves as a splitting of spectral functions in two maxima separated by the continuum of spin excitations.

Gapless fermionic excitation in the antiferromagnetic state of ytterbium zigzag chain

The emergence of charge-neutral fermionic excitations in magnetic systems is one of the unresolved issues in recent condensed matter physics. This type of excitations has been observed in various systems, such as low-dimensional quantum spin liquids, Kondo insulators, and antiferromagnetic insulators. Here, we report the presence of a pronounced gapless spin excitation in the low-temperature antiferromagnetic state of YbCuS2 semiconductor, where trivalent ytterbium atoms form a zigzag chain structure. We confirm the presence of this gapless excitations by a combination of experimental probes, namely 63/65Cu-nuclear magnetic resonance and nuclear quadrupole resonance, as well as specific heat measurements, revealing a linear low-temperature behavior of both the nuclear spin-lattice relaxation rate 1/T1 and the specific heat. This system provides a platform to investigate the origin of gapless excitations in spin chains and the relationship between emergent fermionic excitations and frustration.

Evidence of Kardar-Parisi-Zhang scaling on a digital quantum simulator

Understanding how hydrodynamic behaviour emerges from the unitary evolution of the many-particle Schrödinger equation is a central goal of non-equilibrium statistical mechanics. In this work we implement a digital simulation of the discrete time quantum dynamics of a spin-frac{1}{2} XXZ spin chain on a noisy near-term quantum device, and we extract the high temperature transport exponent at the isotropic point. We simulate the temporal decay of the relevant spin correlation function at high temperature using a pseudo-random state generated by a random circuit that is specifically tailored to the ibmq-montreal 27 qubit device. The resulting output is a spin excitation on a homogeneous background on a 21 qubit chain on the device. From the subsequent discrete time dynamics on the device we are able to extract an anomalous super-diffusive exponent consistent with the conjectured Kardar-Parisi-Zhang (KPZ) scaling at the isotropic point. Furthermore we simulate the restoration of spin diffusion with the application of an integrability breaking potential.

Programmable Quantum Simulations of Bosonic Systems with Trapped Ions.

Trapped atomic ion crystals are a leading platform for quantum simulations of spin systems, with programmable and long-range spin-spin interactions mediated by excitations of phonons in the crystal. We describe a complementary approach for quantum simulations of bosonic systems using phonons in trapped-ion crystals, here mediated by excitations of the trapped-ion spins. The scheme enables a high degree of programability across a dense graph of bosonic couplings, utilizing long-lived collective phonon modes in a trapped-ion chain. As such, it is well suited for tackling hard problems such as boson sampling and simulations of long-range bosonic and spin-boson Hamiltonians.

Tunable momentum pair creation of spin excitations in dipolar bilayers

Tunable momentum pair creation of spin excitations in dipolar bilayers

Stability and asymptotic interactions of chiral magnetic skyrmions in a tilted magnetic field

Using a general framework, interaction potentials between chiral magnetic solitons in a planar system with a tilted external magnetic field are calculated analytically in the limit of large separation. The results are compared to previous numerical results for solitons with topological charge \pm 1±1. A key feature of the calculation is the interpretation of Dzyaloshinskii-Moriya interaction (DMI) as a background SO(3)SO(3) gauge field. In a tilted field, this leads to a U(1)U(1)-gauged version of the usual equation for spin excitations, leading to a distinctive oscillating interaction profile. We also obtain predictions for skyrmion stability in a tilted field which closely match numerical observations.