Spin Relaxation Mechanism Research Articles

Impact of γ-Irradiation on Separation of Nuclear Spin-Relaxation Mechanisms Under Magnetic Saturation in a NaF Crystal

Impact of γ-Irradiation on Separation of Nuclear Spin-Relaxation Mechanisms Under Magnetic Saturation in a NaF Crystal

A novel non-adiabatic spin relaxation mechanism in molecular qubits.

The interaction of electronic spin and molecular vibrations mediated by spin-orbit coupling governs spin relaxation in molecular qubits. We derive an extended molecular spin Hamiltonian that includes both adiabatic and non-adiabatic spin-dependent interactions, and we implement the computation of its matrix elements using state-of-the-art density functional theory. The new molecular spin Hamiltonian contains a novel spin-vibrational orbit interaction with a non-adiabatic origin, together with the traditional molecular Zeeman and zero-field splitting interactions with an adiabatic origin. The spin-vibrational orbit interaction represents a non-Abelian Berry curvature on the ground-state electronic manifold and corresponds to an effective magnetic field in the electronic spin dynamics. We further develop a spin relaxation rate model that estimates the spin relaxation time via the two-phonon Raman process. An application of the extended molecular spin Hamiltonian together with the spin relaxation rate model to Cu(II) porphyrin, a prototypical S = 1/2 molecular qubit, demonstrates that the spin relaxation time at elevated temperatures is dominated by the non-adiabatic spin-vibrational orbit interaction. The computed spin relaxation rate and its magnetic field orientation dependence are in excellent agreement with experimental measurements.

Tuning Spin-Polarized Lifetime at High Carrier Density through Deformation Potential in Dion-Jacobson-Phase Perovskites.

The control of spin relaxation mechanisms is of great importance for spintronics applications as well as for fundamental studies. Layered metal-halide perovskites represent an emerging class of semiconductors with rich optical spin physics, showing potential for spintronic applications. However, a major hurdle arises in layered metal-halide perovskites with strong spin-orbit coupling, where the spin lifetime becomes extremely short due to D'yakonov-Perel' scattering and Bir-Aronov-Pikus at high carrier density. Using the circularly polarized pump-probe transient reflection technique, we experimentally reveal the important scattering for spin relaxation beyond the electron-hole exchange strength in the Dion-Jacobson (DJ)-type 2D perovskites (3AMP)(MA)n-1PbnI3n+1 [3AMP = 3-(aminomethyl)piperidinium, n = 1-4]. Despite a more than 10-fold increase in carrier concentration, the spin lifetimes for n = 3 and 4 are effectively maintained. We reveal neutral impurity and polar optical phonon scatterings as significant contributors to the momentum relaxation rate. Furthermore, we show that more octahedral distortions induce a larger deformation potential which is reflected on the acoustic phonon properties. Coherent acoustic phonon analysis indicates that the polaronic effect is crucial in achieving control over the scattering mechanism and ensuring spin lifetime protection, highlighting the potential of DJ-phase perovskites for spintronic applications.

Evidence of Ferromagnetism and Ultrafast Dynamics of Demagnetization in an Epitaxial FeCl2 Monolayer.

The development of two-dimensional (2D) magnetism is driven not only by the interest of low-dimensional physics but also by potential applications in high-density miniaturized spintronic devices. However, 2D materials possessing a ferromagnetic order with a relatively high Curie temperature (Tc) are rare. In this paper, the evidence of ferromagnetism in monolayer FeCl2 on Au(111) surfaces, as well as the interlayer antiferromagnetic coupling of bilayer FeCl2, is characterized by using spin-polarized scanning tunneling microscopy. A Curie temperature (Tc) of ∼147 K is revealed for monolayer FeCl2, based on our static magneto-optical Kerr effect measurements. Furthermore, temperature-dependent magnetization dynamics is investigated by the time-resolved magneto-optical Kerr effect. A transition from one- to two-step demagnetization occurs as the lattice temperature approaches Tc, which supports the Elliott-Yafet spin relaxation mechanism. The findings contribute to a deeper understanding of the underlying mechanisms governing ultrafast magnetization in 2D ferromagnetic materials.

Direct Observation of Circularly Polarized Nonlinear Optical Activities in Chiral Hybrid Lead Halides.

Circularly polarized light emission is a crucial application in imaging, sensing, and photonics. However, utilizing low-energy photons to excite materials, as opposed to high-energy light excitation, can facilitate deep-tissue imaging and sensing applications. The challenge lies in finding materials capable of directly generating circularly polarized nonlinear optical effects. In this study, we introduce a chiral hybrid lead halide (CHLH) material system, R/S-DPEDPb3Br8·H2O (DPED = 1,2-diphenylethylenediammonium), which can directly produce circularly polarized second harmonic generation (CP-SHG) through linearly polarized infrared light excitation, exhibiting a polarization efficiency as high as 37% at room temperature. To understand the spin relaxation mechanisms behind the high polarization efficiency, we utilized two models, so-called D'yakonov-Perel' (DP) and Bir-Aronov-Pikus (BAP) mechanisms. The unique zigzag inorganic frameworks within the hybrid structure are believed to reduce the dielectric confinement and exciton binding energy, thus enhancing spin polarization, especially in regions with a high excitation pump fluence based on the DP mechanism. In the case of low excitation pump fluence, the BAP mechanism dominates, as evidenced by the observed decrease in the polarization ratio from CP-SHG measurement. Using density functional theory analysis, we elucidate how the distinctive 8-coordination environment of lead bromide building blocks effectively suppresses spin-orbit coupling at the conduction band minimum. This suppression significantly diminishes spin-splitting, thereby slowing the spin relaxation rate.

New series of mononuclear β-diketonate cerium(III) field induced single-molecule magnets.

Five new β-diketonate Ce3+ mononuclear complexes, [Ce(Btfa)3(H2O)2] (1), [Ce(Btfa)3(phen)] (2), [Ce(Btfa)3(bipy)] (3), [Ce(Btfa)3(terpy)] (4) and [Ce(Btfa)3(bathophen)(DMF)] (5), where Btfa- = 4,4,4-trifluoro-1-phenyl-1,3-butanedionate, phen = 1,10-phenanthroline, bipy = 2,2'-bipyridyl, terpy = 2,2':6',2''-terpyridine and bathophen = 4,7-diphenyl-1,10-phenanthroline, have been synthesized and structurally characterized through X-ray diffraction of single crystals. The central Ce3+ atom displays a coordination number of 8 for 1, 2 and 3 and of 9 for 4 and 5. Under a 0 T external magnetic field, none of the given compounds exhibits single molecule magnet (SMM) behaviour. However, a small magnetic field, between 0.02 and 0.1 T, is enough for all the compounds to exhibit slow relaxation of the magnetization. A comprehensive magnetic analysis, with experimental magnetic data and ab initio calculations, was undertaken for all the complexes, and the study highlights the significance of the different spin relaxation mechanisms that must be considered for a Ce3+ lanthanide ion.

Optical Electron-Nuclear Resonance in Semiconductors

A considerable number of investigations have by now been made on optical pumping of spin-oriented electrons in semiconductors. The optical-pumping method makes it possible to produce easily a high polarization of the electron spins in the conduction band, and to detect it optically [1–3]. The use of this method for the investigation of semiconductors turned out to be very fruitful; the spin orientation of the minority [1–3] and majority [4] carriers was determined, the lifetimes of the non-equilibrium electrons were measured [2, 3, 5], the mechanisms of spin relaxation of “cold” [2, 5] and “hot” [2, 6] electrons were investigated, spin orientation of excitons was effected [7], and electron paramagnetic resonance with non-equilibrium electrons was registered [8].

T1 Anisotropy Elucidates Spin Relaxation Mechanisms in an S = 1 Cr(IV) Optically Addressable Molecular Qubit.

Paramagnetic molecules offer unique advantages for quantum information science owing to their spatial compactness, synthetic tunability, room-temperature quantum coherence, and potential for optical state initialization and readout. However, current optically addressable molecular qubits are hampered by rapid spin-lattice relaxation (T1) even at sub-liquid nitrogen temperatures. Here, we use temperature- and orientation-dependent pulsed electron paramagnetic resonance (EPR) to elucidate the negative sign of the ground state zero-field splitting (ZFS) and assign T1 anisotropy to specific types of motion in an optically addressable S = 1 Cr(o-tolyl)4 molecular qubit. The anisotropy displays a distinct sin2(2θ) functional form that is not observed in S = 1/2 Cu(acac)2 or other Cu(II)/V(IV) microwave addressable molecular qubits. The Cr(o-tolyl)4 T1 anisotropy is ascribed to couplings between electron spins and rotational motion in low-energy acoustic or pseudoacoustic phonons. Our findings suggest that rotational degrees of freedom should be suppressed to maximize the coherence temperature of optically addressable qubits.

Isolated spin-pair analysis of 13C NMR relaxation rates in liquids

In small organic molecules, dipolar relaxation rate R1DD is the most important mechanism for 13C NMR spin relaxation. Herein, the R1DD was used to analyze force-field molecular dynamics trajectories, corresponding to some neat liquids and solutions, in order to simulate 13C relaxation. The results show a satisfactory correlation between simulated and experimental values, structure-dependent behavior and self-diffusion effects due to differences in inertia axes that could be observed by the isolated spin-pair approach that avoids the solution of relaxation matrices, which helps in interpreting 13C relaxation experimental data from a molecular dynamics approach.

Hybrid organic/inorganic interface: in situ and ex situ characterization in terms of structure, morphology, electronic and magnetic properties

Organic conjugated molecules are promising media to host spin-polarized carriers, due to their weak spin relaxation mechanisms. Here, we fabricated a metal–hybrid organic–inorganic complex oxide heterostructure made of Fe–Phthalocyanine (FePc): Co(0.5 nm)/FePc(0; 0.5; 1 nm)/La0.67Sr0.33MnO3/SrTiO3 and investigated the interface structure and chemical bonding, and overall magnetic properties. Details about the Co/FePc and FePc/LSMO interfaces were obtained through X-ray photoelectron and absorption characterizations. The combined in-situ and ex-situ magnetic measurements of the heterostructure indicates the contribution of FePc and Co moments to the overall magnetic response. Moreover, these measurements indicate that the LSMO bulk magnetic properties were not canceled out by the surface treatment, but favored the formation of a magnetic dead layer. The hybrid heterostructure presents a modification of the saturation magnetization attributed to the contribution of the molecular layer. The present results are a step forward in the engineering of hybrid organic/inorganic interfaces.

Comprehensive analysis on the magnetic field error of a K–Rb–21Ne comagnetometer with low-frequency bias magnetic field sensitivity

The spin-exchange relaxation-free comagnetometer (SERFC) is of important research value compared to existing high-precision gyroscopes because of its extremely high theoretical limit sensitivity and long-term stability, in which one significant limiting factor is the magnetic field error. First, the relationship between the magnetic field gradient and the nuclear spin relaxation mechanism is introduced into the frequency response and steady-state response models of SERFC. Then, a novel method for suppression of the low-frequency magnetic field error based on the modified bias magnetic field sensitivity model is proposed. Finally, the effectiveness of the proposed suppression methods is demonstrated by optimizing the cell temperature, pump light power, and compensation magnetic field gradient to increase the suppression factor by 72.19%, 20.24%, and 69.86%, and the corresponding bias instability increased by 55.41%, 20.84%, and 27.63%, respectively. This study contributes to improving the long-term zero bias stability of the SERFC.

Model for 1/f flux noise in superconducting aluminum devices: Impact of external magnetic fields

Superconducting quantum interference devices and related circuits made of aluminum are known to display 1/ω flux noise, where ω is frequency. A recent experiment showed that the application of an external magnetic field in the 10–100 G range changed the noise to a single Lorentzian peaked at ω = 0. Here, it is shown that a model based on independent impurity spin flips with coexisting cross and direct mechanisms of spin relaxation may explain these experiments. The model shows that application of an external magnetic field can be used to reduce the impact of flux noise in qubits.

Unlocking hidden spins in centrosymmetric 1T transition metal dichalcogenides by vacancy-controlled spin-orbit scattering

Spin current generation and manipulation remain the key challenge of spintronics, in which relativistic spin-orbit coupling (SOC) plays a ubiquitous role. In this paper, we demonstrate that hidden Rashba spins in the nonmagnetic, centrosymmetric lattice of multilayer ${\mathrm{SnSe}}_{2}$ can be efficiently activated by spin-orbit scattering introduced by Se vacancies. Via vacancy scattering, conduction electrons with hidden spin-momentum locked polarizations acquire out-of-plane magnetization components, which effectively break the chiral symmetry between the two Se sublattices of an ${\mathrm{SnSe}}_{2}$ monolayer when electron spins start precession in the strong built-in Rashba SOC field. The resulting spin separations are manifested in quantum transport as vacancy concentration- and temperature-dependent crossovers from weak antilocalization to weak localization, with the distinctive spin relaxation mechanism of the D'yakonov-Perel' type. In a nonlocal geometry, the generated spins exhibit a long diffusion length exceeding 5 $\textmu{}\mathrm{m}$, when fast momentum scattering protects the effective spin polarizations by driving the random-walk evolution of spin precessions subject to rapidly changing Rashba SOC field. Our study shows the great potential of two-dimensional systems with hidden-spin textures for spintronics.

Microscopic theory of spin relaxation of a single Fe adatom coupled to substrate vibrations

Understanding the spin-relaxation mechanism of single adatoms is an essential step towards creating atomic magnetic memory bits or even qubits. Here we present an essentially parameter-free theory by combining \textit{ab-initio} electronic and vibrational properties with the many-body nature of atomic states. Our calculations account for the millisecond spin lifetime measured recently on Fe adatoms on MgO/Ag(100) and reproduce the dependence on the number of decoupling layers and the external magnetic field. We show how the atomic interaction with the environment should be tuned in order to enhance the magnetic stability, and propose a clear fingerprint for experimentally detecting a localized spin-phonon excitation.

Scanning inverse spin Hall effect spectrometer by shorted coaxial probes.

In this work, a scanning inverse spin Hall effect measurement system based on a shorted coaxial resonator has been built, which provides a high throughput method to characterize spin transport properties. The system is capable of performing spin pumping measurements on patterned samples within an area of 100 × 100mm2. Its capability was demonstrated with Py/Ta bilayer stripes deposited on the same substrate with different thicknesses of Ta. The results show that the spin diffusion length is about 4.2nm with a conductivity of about 7.5 × 105Ω-1m-1, which leads to the conclusion that the intrinsic mechanism of spin relaxation of Ta is the Elliott-Yafet interactions. The spin Hall angle of Ta is estimated to be about -0.014 at room temperature. The setup developed in this work provides a convenient, efficient, and nondestructive way to obtain the spin and electron transportation characteristics of the spintronic materials, which will fertilize this community by developing new materials and figuring out their mechanism.

Spin-relaxation mechanisms in InAs quantum well heterostructures

Spin–orbit interaction and spin-relaxation mechanisms of a shallow InAs quantum well heterostructure are investigated by magnetoconductance measurements as a function of an applied top-gate voltage. The data are fit using a Iordanskii–Lyanda-Geller–Pikus model and two distinct transport regimes are identified. The spin–orbit interaction splitting energy is extracted from the fits to the data, which also displays two distinct regimes. The different regimes exhibit different spin-scattering mechanisms, the identification of which is of relevance for device platforms of reduced dimensionality which utilize the spin–orbit interaction.

Unraveling the spin current flow in Bi layers

Although heavy metal materials, due to their large spin-orbit interaction, would be expected to act as an efficient converter of spin current to charge current, Bismuth does not obey this rule. Heterostructures of yttrium iron garnet (YIG)/Bi are investigated by means of the spin pumping technique and the results show that Bi exhibits negligible spin-charge conversion. In addition to not converting spin to charge, Bi exhibits an exotic spin relaxation mechanism, which is driven by its large diamagnetic response. By considering a nonlinear stochastic model of diffusing spin particles, the results show that the Bi layer acts as a binary classifier device that categorizes the pumped spins into relaxed spins and those that flow upwards and eventually reach the top layer of Pt. This shows that the investigation reported here opens different perspectives involving fundamental aspects in the fields of machine learning and condensed matter physics.

Unraveling the Contributions to Spin-Lattice Relaxation in Kramers Single-Molecule Magnets.

The study of how spin interacts with lattice vibrations and relaxes to equilibrium provides unique insights into its chemical environment and the relation between electronic structure and molecular composition. Despite its importance for several disciplines, ranging from magnetic resonance to quantum technologies, a convincing interpretation of spin dynamics in crystals of magnetic molecules is still lacking due to the challenging experimental determination of the correct spin relaxation mechanism. We apply ab initio spin dynamics to a series of 12 coordination complexes of Co2+ and Dy3+ ions selected among ∼240 compounds that largely cover the literature on single-molecule magnets and well represent different regimes of spin relaxation. Simulations reveal that the Orbach spin relaxation rate of known compounds mostly depends on the ions' zero-field splitting and little on the details of molecular vibrations. Raman relaxation is instead found to be also significantly affected by the features of low-energy phonons. These results provide a complete understanding of the factors limiting spin lifetime in single-molecule magnets and revisit years of experimental investigations by making it possible to transparently distinguish Orbach and Raman relaxation mechanisms.

Illuminating Ligand Field Contributions to Molecular Qubit Spin Relaxation via T1 Anisotropy.

Electron spin relaxation in paramagnetic transition metal complexes constitutes a key limitation on the growth of molecular quantum information science. However, there exist very few experimental observables for probing spin relaxation mechanisms, leading to a proliferation of inconsistent theoretical models. Here we demonstrate that spin relaxation anisotropy in pulsed electron paramagnetic resonance is a powerful spectroscopic probe for molecular spin dynamics across a library of highly coherent Cu(II) and V(IV) complexes. Neither the static spin Hamiltonian anisotropy nor contemporary computational models of spin relaxation are able to account for the experimental T1 anisotropy. Through analysis of the spin-orbit coupled wave functions, we derive an analytical theory for the T1 anisotropy that accurately reproduces the average experimental anisotropy of 2.5. Furthermore, compound-by-compound deviations from the average anisotropy provide a promising approach for observing specific ligand field and vibronic excited state coupling effects on spin relaxation. Finally, we present a simple density functional theory workflow for computationally predicting T1 anisotropy. Analysis of spin relaxation anisotropy leads to deeper fundamental understanding of spin-phonon coupling and relaxation mechanisms, promising to complement temperature-dependent relaxation rates as a key metric for understanding molecular spin qubits.

Transient and steady state magneto-optical studies of the CsPbBr3 crystal

We have studied the magneto-optical properties of photoexcitations in $\mathrm{CsPb}{\mathrm{Br}}_{3}$ single crystal using the technique of picosecond time-resolved quantum beatings (QBs) in the circularly polarized photoinduced reflection as well as steady state magnetocircular dichroism (MCD) in $\mathrm{CsPb}{\mathrm{Br}}_{3}$ film. In the Voigt geometry at magnetic field strength $B$ > 0, we observed fast and slow QB oscillations that we attribute to the Larmor precession frequency of electrons and holes, respectively. From the linear frequency dependence on $B$, we extract the carrier anisotropic Land\'e $g$ factors for applied B along [010] and [001]; for electrons $|{g}_{[001]}^{\mathrm{e}}|=1.95\ifmmode\pm\else\textpm\fi{}0.04$ and $|{g}_{[010]}^{\mathrm{e}}|=1.82\ifmmode\pm\else\textpm\fi{}0.04$, whereas for holes $|{g}_{[001]}^{\mathrm{h}}|=0.69\ifmmode\pm\else\textpm\fi{}0.02$ and $|{g}_{[010]}^{\mathrm{h}}|=0.76\ifmmode\pm\else\textpm\fi{}0.02$. These values are in excellent agreement with a k\ifmmode\cdot\else\textperiodcentered\fi{}p model calculation applied to $\mathrm{CsPb}{\mathrm{Br}}_{3}$. Surprisingly, at $B=0$, we still observed QB oscillation of \ensuremath{\sim}500 MHz that we interpret as due to the Overhauser field that originates from the spin-aligned nuclei caused by the Knight field. From the measured MCD spectrum vs $B$, we obtained the $g$ factor of the bright excitons ${g}_{\mathrm{ex}}=2.18\ifmmode\pm\else\textpm\fi{}0.08$ showing that the $g$ value of holes in $\mathrm{CsPb}{\mathrm{Br}}_{3}$ is positive. We also measured the temperature and magnetic field dependencies of the electron and hole spin dephasing times which support the Elliot-Yafet spin-relaxation mechanism.