Initial Spin Polarization Research Articles

Estimation of Heisenberg exchange interaction in rigid photoexcited chromophore-radical compound by transient EPR.

The magnetic field dependence of the spin polarization in a photoexcited rigid chromophore-radical conjugate is theoretically investigated. The excitation of the chromophore-radical conjugate often populates the metastable doublet and quartet states formed by the interactions of the unpaired electrons of the triplet chromophore and the radical. The intensities of the +1/2 ↔ - 1/2 transitions of the doublet and quartet manifolds are sensitive to the ratio jω = 3J/ω0 between the triplet-doublet exchange interaction J and the Zeeman energy ω0. It is shown that the analytical expressions of these intensities previously found for the triplet mechanism of the initial spin polarization can be expanded and applied to a broader class of compounds that may have other intersystem crossing pathways of the depopulation of the excited singlet state of the chromophore. It is also shown that the exchange interaction can be evaluated not only by comparing the electron paramagnetic resonance spectra obtained in different microwave frequency bands but also by comparing the data obtained in the same microwave band but with a shift of the frequency of the resonator. The results obtained broaden the potential applications of the previously proposed approach for analyzing the correlation between the exchange coupling and the distance separating the radical and the chromophore spins, as well as the structure of the bridge connecting their fragments.

Effect of dilute nitride GaNAs quantum well thickness on spin amplification dynamics of tunnel-coupled InAs quantum dots

Electron spin dynamics of dilute nitride GaNAs quantum well (QW)-InAs quantum dots (QDs) tunnel-coupled structures having different QW thicknesses were studied via circularly polarized time-resolved photoluminescence. The rate equation fitting considering a capture of QD electron spins by the GaNAs localized states via tunnel transfer revealed that the spin amplification dynamics of the QDs depended on the QW thickness. For the QW thickness of 5 nm, although the temporal amplification of QD electron spin polarization was slow owing to the weak wavefunction coupling between the QW and QD, the long duration of high electron spin polarization was observed because of the suppressed capture of QD majority spins relative to the efficient removal of QD minority spins. When the QW thickness increased from 5 to 20 nm, the strong spin filtering in GaNAs and strong wavefunction coupling led to the fast amplification of QD electron spin polarization with high initial spin polarization. However, the spin polarization rapidly decays after the amplification owing to the removal of both QD majority and minority spins, originating from many effective localized states. These results indicate that the time-dependent QD electron spin polarization and the resultant spin amplification can be widely tuned by changing the thickness of the tunnel-coupled GaNAs QW.

Conservation of longitudinal spin polarization of positrons emitted from a thin Ni(100) foil

We have discovered that 5 keV bursts of $5\ifmmode\times\else\texttimes\fi{}10{}^{7}$ positrons with an initial longitudinal spin polarization of $(28.8\ifmmode\pm\else\textpm\fi{}0.7)%$, when implanted into a thin Ni(100) crystal, are emitted with 20% efficiency at thermal energies from its surface with $(30.9\ifmmode\pm\else\textpm\fi{}0.5)%$ polarization. We conclude that the positron spin polarization is preserved while interacting with the Ni, despite the 0.61 T average transverse magnetization of the Ni at room temperature. The resulting polarized beam has been focused to a 0.025-mm mean-diameter spot when accelerated to 5 keV and will be uniquely suited for experiments on a neutral spin aligned ${e}^{+}\ensuremath{-}{e}^{\ensuremath{-}}$ plasma, spin- and angle-resolved positronium emission spectroscopy, and critical for producing a triplet positronium Bose-Einstein condensate.

Ballistic-electron coherent spin precession in a Rashba two-dimensional electron system

In a remarkable manifestation of the Rashba spin-orbit coupling effect, spin polarized carriers injected into a narrow two-dimensional electron system channel have ballistic trajectories and a weakly relativistic Fermi velocity. In the carrier rest frame, the intrinsic electric field in the quantum well transforms as an effective magnetic field, ${H}^{*}$, transverse to the trajectories. Electrons with initial spin momentum and polarization orientations along the channel precess because of ${H}^{*}$ with a wavelength $\ensuremath{\lambda}$. For long mean free paths $l$, spin detection probes at distances $L$ $l$ record conductance oscillations with wavelength $\ensuremath{\lambda}$. Two unique experiments that demonstrate these oscillations are discussed.

Nonlinear dynamics of tunable spin-orbit coupled Bose-Einstein condensates in deep optical lattices

We discuss the localization and spin dynamics of tunable spin-orbit coupled Bose-Einstein condensates in deep optical lattices. Rich localized phenomena (breather, soliton, self-trapping, and diffusion) are observed. The critical conditions for occurring different localized states are obtained analytically and confirmed numerically. Under the critical conditions, we observe localized states with fixed initial spin polarization. When the critical condition is not satisfied, because of spin-momentum locking, quenching of Raman coupling from soliton state excites spin dynamics. If initially the soliton is in a nearly unpolarized (polarized) state, persistent (damped) spin dynamics is excited. The system finally transforms to a new polarized state in the damped spin dynamics. The localization and spin dynamics can be well controlled by periodic modulation of Raman coupling.

Novel magnetic ordering in LiYbO2 probed by muon spin relaxation

The stretched diamond lattice material LiYbO2 has recently been reported to exhibit two magnetic transitions ($T_{N1} = 1.1 K$, $T_{N2} = 0.45 K$) via specific heat, magnetization, and neutron scattering measurements [Bordelon et al., Phys. Rev. B 103, 014420 (2021)]. Here we report complementary magnetic measurements down to T = 0.28 K via the local probe technique of muon spin relaxation. While we observe a rapid increase in the zero-field muon depolarization rate at $T_{N1}$, we do not observe any spontaneous muon precession for $T < T_{N1}$, which is typically associated with long-range magnetic ordering. The depolarization rate in the ordered state shows a surprising sensitivity to magnetic fields applied along the initial spin polarization direction. Using a simple one-dimensional model, we show that these results are consistent with the unusual random-phase bipartite incommensurate magnetic structure proposed by Bordelon et al. for the intermediate temperature range $T_{N2} < T < T_{N1}$. We also find evidence for temperature-independent magnetic fluctuations persisting to our lowest temperatures, but no obvious signature of the transition or spontaneous muon precession at and below TN2, respectively. This result is suggestive of quantum dynamics within a highly degenerate ground state.

Optically controllable magnetism in atomically thin semiconductors.

We report evidence that ferromagnetic order in electrostatically doped, monolayer transition metal dichalcogenide (TMD) semiconductors can be stabilized and controlled at zero magnetic field by local optical pumping. We use circular dichroism (CD) in reflectivity from excitonic states as a spatially resolved probe of charge-carrier spin polarization. At electron densities ne ~ 1012 cm−2, a diffraction-limited, circularly polarized optical pump breaks symmetry between oppositely polarized magnetic states and stabilizes long-range magnetic order, with carrier polarization exceeding 80% over an 8 μm by 5 μm extent. In time-resolved measurements with pulsed optical excitation, we observe that magnetic interactions amplify the initial pump-induced spin polarization by more than an order of magnitude. The optical control of magnetism with local optical pumps will unlock advancements in spin and optical technologies and provides a versatile tool in the study of correlated phases in two-dimensional electron gases.

Localization and spin dynamics of spin-orbit-coupled Bose-Einstein condensates in deep optical lattices.

We analytically and numerically discuss the dynamics of two pseudospin components Bose-Einstein condensates (BECs) with spin-orbit coupling (SOC) in deep optical lattices. Rich localized phenomena, such as breathers, solitons, self-trapping, and diffusion, are revealed and strongly depend on the strength of the atomic interaction, SOC, Raman detuning, and the spin polarization (i.e., the initial population difference of atoms between the two pseudospin components of BECs). The critical conditions for the transition of localized states are derived analytically. Based on the critical conditions, the detailed dynamical phase diagram describing the different dynamical regimes is derived. When the Raman detuning satisfies a critical condition, localized states with a fixed initial spin polarization can be observed. When the critical condition is not satisfied, we use two quenching methods, i.e., suddenly and linearly quenching Raman detuning from the soliton or breather state, to discuss the spin dynamics, phase transition, and wave packet dynamics by numerical simulation. The sudden quenching results in a damped oscillation of spin polarization and transforms the system to a new polarized state. Interestingly, the linear quenching of Raman detuning induces a controllable phase transition from an unpolarized phase to an expected polarized phase, while the soliton or breather dynamics is maintained.

Chirality of Bloch domain walls in exchange-biased CoO/Co bilayer studied by waveguide-enhanced neutron spin-flip scattering

The magnetic state of exchanged biased $\mathrm{CoO}(20\phantom{\rule{0.16em}{0ex}}\mathrm{nm})/\mathrm{Co}({d}_{F})$ bilayers (${d}_{F}=5\ensuremath{-}20\phantom{\rule{0.16em}{0ex}}\mathrm{nm}$) was studied by means of polarized neutron reflectometry. By introducing a Nb(20 nm) spacer layer between the CoO/Co bilayer and the ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}$ substrate, we designed a resonator structure with significantly enhanced intensity of the spin-flip (SF) scattering at the position of the optical resonances. For the trained sample with thinnest Co layer (${d}_{F}=5\phantom{\rule{0.16em}{0ex}}\mathrm{nm}$), we detected strong SF scattering at the resonance position to the amount of 30% of the incoming intensity, pointing to a high degree of non-collinearity of the magnetization. With increasing ${d}_{F}$, the intensity of the SF scattering decreases linearly. Furthermore, an unconventional asymmetry of up-down and down-up scattering channels at the resonance positions was observed, which we ascribe to the out-of-plane magnetic stray field generated by chiral Bloch domain walls. This field leads to Zeeman splitting of the neutron energies depending on the initial neutron spin polarization. The chirality of the domain walls is assigned to the Dzyaloshinskii-Moriya interaction emerging at the CoO/Co interface. Our observations might prove useful for the design of spintronic devices based on the exchange bias effect.

Magnetic structure determination of high-moment rare-earth-based laminates

The laminate (Mo${}_{2/3}$Gd${}_{1/3}$)${}_{2}$AlC, based on high-moment Gd, grows as pristine crystals and might exfoliate or be etched into two-dimensional magnets, but its properties are unknown since Gd is a strong neutron absorber. Bypassing this difficulty, the authors succeed in determining the magnetic structure by combining neutron diffraction studies on isostructural compounds with muon spin rotation studies including first-principles site calculations and, most importantly, initial muon spin polarization variations.

Na Diffusion in Hard Carbon Studied with Positive Muon Spin Rotation and Relaxation.

The diffusive nature of Na+ in Na-inserted hard carbon (C x Na), which is the most common anode material for a Na-ion battery, was studied with a positive muon spin rotation and relaxation (μ+SR) technique in transverse, zero, and longitudinal magnetic fields (TF, ZF, and LF) at temperatures between 50 and 375 K, where TF (LF) denotes the applied magnetic field perpendicular (parallel) to the initial muon spin polarization. At temperatures above 150 K, TF-μ+SR measurements showed a distinct motional narrowing behavior, implying that Na+ begins to diffuse above 150 K. The presence of two different muon sites in C x Na was confirmed with ZF- and LF-μ+SR measurements; one is in the Na-inserted graphene layer, and the other is in the Na-vacant graphene layer adjacent to the Na-inserted graphene layer. A systematic increase in the field fluctuation rate (ν) with increasing temperature also evidenced a thermally activated Na diffusion, particularly above 150 K. Assuming the two-dimensional diffusion of Na+ in the graphene layers, the self-diffusion coefficient of Na+ (D Na J) at 300 K was estimated to be 2.5 × 10-11 cm2/s with a thermal activation energy of 39(7) meV.

Spin-polarization effects in Cherenkov radiation from electrons

A quantum electrodynamical theory of Cherenkov radiation emitted by spin-polarized electrons moving in an isotropic medium is developed within the density matrix framework. Special attention is paid to the polarization properties of the emitted photons described by means of Stokes parameters. It is demonstrated that, although the Cherenkov radiation is primarily linearly polarized in the plane containing the direction of observation and the path of the electrons, the photons may have a small component of circular polarization of the order of 3 × 10−6 for electron kinetic energy of 500 keV due to the initial electron spin polarization, whose existence can be confirmed by sensitive measurements in the future.

Spin States Protected from Intrinsic Electron-Phonon Coupling Reaching 100 ns Lifetime at Room Temperature in MoSe2.

We present time-resolved Kerr rotation measurements, showing spin lifetimes of over 100 ns at room temperature in monolayer MoSe2. These long lifetimes are accompanied by an intriguing temperature-dependence of the Kerr amplitude, which increases with temperature up to 50 K and then abruptly switches sign. Using ab initio simulations, we explain the latter behavior in terms of the intrinsic electron-phonon coupling and the activation of transitions to secondary valleys. The phonon-assisted scattering of the photoexcited electron-hole pairs prepares a valley spin polarization within the first few ps after laser excitation. The sign of the total valley magnetization, and thus the Kerr amplitude, switches as a function of temperature, as conduction and valence band states exhibit different phonon-mediated intervalley scattering rates. However, the electron-phonon scattering on the ps time scale does not provide an explanation for the long spin lifetimes. Hence, we deduce that the initial spin polarization must be transferred into spin states, which are protected from the intrinsic electron-phonon coupling, and are most likely resident charge carriers, which are not part of the itinerant valence or conduction band states.

Resonating valence bonds and spinon pairing in the Dicke model

Resonating valence bond (RVB) states are a class of entangled quantum many body wavefunctions with great significance in condensed matter physics. We propose a scheme to synthesize a family of RVB states using a cavity QED setup with two-level atoms coupled to a common photon mode. In the lossy cavity limit, starting with an initial state with MM atoms excited and NN atoms in the ground state, we show that this setup can be configured as a Stern Gerlach experiment. A measurement of photon emission collapses the wavefunction of atoms onto an RVB state composed of resonating long-ranged singlets. Each emitted photon reduces the number of singlets by unity, replacing it with a pair of lone spins or ‘spinons’. As spinons are formed coherently in pairs, they are analogous to Cooper pairs in a superconductor. To simulate pair fluctuations, we propose a protocol in which photons are allowed to escape the cavity undetected. This leads to an inchoate superconductor – mixed quantum state with a fluctuating number of spinon pairs. Remarkably, in the limit of large system sizes, this protocol reveals an underlying quantum phase transition. Upon tuning the initial spin polarization, the emission exhibits a continuous transition from a dark state to a bright state. This opens an exciting route to simulate RVB states and superconductivity.

Quantum kinetic equations for the ultrafast spin dynamics of excitons in diluted magnetic semiconductor quantum wells after optical excitation

Quantum kinetic equations of motion for the description of the exciton spin dynamics in II-VI diluted magnetic semiconductor quantum wells with laser driving are derived. The model includes the magnetic as well as the nonmagnetic carrier-impurity interaction, the Coulomb interaction, Zeeman terms, and the light-matter coupling, allowing for an explicit treatment of arbitrary excitation pulses. Based on a dynamics-controlled truncation scheme, contributions to the equations of motion up to second order in the generating laser field are taken into account. The correlations between the carrier and the impurity subsystems are treated within the framework of a correlation expansion. For vanishing magnetic field, the Markov limit of the quantum kinetic equations formulated in the exciton basis agrees with existing theories based on Fermi's golden rule. For narrow quantum wells excited at the $1s$ exciton resonance, numerical quantum kinetic simulations reveal pronounced deviations from the Markovian behavior. In particular, the spin decays initially with approximately half the Markovian rate and a nonmonotonic decay in the form of an overshoot of up to $10%$ of the initial spin polarization is predicted.

Spin Polarization Transfer from a Photogenerated Radical Ion Pair to a Stable Radical Controlled by Charge Recombination

Photoexcitation of electron donor-acceptor molecules frequently produces radical ion pairs with well-defined initial spin-polarized states that have attracted significant interest for spintronics. Transfer of this initial spin polarization to a stable radical is predicted to depend on the rates of the radical ion pair recombination reactions, but this prediction has not been tested experimentally. In this study, a stable radical/electron donor/chromophore/electron acceptor molecule, BDPA•-mPD-ANI-NDI, where BDPA• is α,γ-bisdiphenylene-β-phenylallyl, mPD is m-phenylenediamine, ANI is 4-aminonaphthalene-1,8-dicarboximide, and NDI is naphthalene-1,4:5,8-bis(dicarboximide), was synthesized. Photoexcitation of ANI produces the triradical BDPA•-mPD+•-ANI-NDI-• in which the mPD+•-ANI-NDI-• radical ion pair is spin coupled to the BDPA• stable radical. BDPA•-mPD+•-ANI-NDI-• and its counterpart lacking the stable radical are found to exhibit spin-selective charge recombination in which the triplet radical ion pair 3(mPD+•-ANI-NDI-•) is in equilibrium with the 3*NDI charge recombination product. Time-resolved EPR measurements show that this process is associated with an inversion of the sign of the polarization transferred to BDPA• over time. The polarization transfer rates are found to be strongly solvent dependent, as shifts in this equilibrium affect the spin dynamics. These results demonstrate that even small changes in electron transfer dynamics can have a large effect on the spin dynamics of photogenerated multispin systems.

Electron spin fluctuation in intense laser fields.

The effects of the orientation, wavelength and carrier-envelope phase of laser pulses on the spin fluctuation in HeH2+ and LiH3+ molecular ions in their bound electronic states, during their interactions with linearly polarized intense laser pulses, were investigated by solving numerically the time-dependent Dirac equation with the Foldy-Wouthuysen transformation. The results of this study showed that an increase in the wavelength of the laser pulse at a fixed intensity reduces the lifetime of the coherent spin states and increases the sensitivity of the spin vector to the applied laser field in both HeH2+ and LiH3+ species. This sensitivity also depends on the carrier-envelope phase of the laser pulse due to the asymmetry of these systems. Furthermore, the influence of spin-orbit coupling on the dynamics of the spin in the interaction of the highly charged atomic species, N6+, with ultra-intense laser pulses was investigated by considering different initial orbitals and spin polarizations. The results show that significantly different spin-forces are induced when an interaction starts with two parallel and perpendicular polarized spin states with respect to the direction of the laser pulse propagation. Furthermore, spin-orbit coupling affects the quantization of the spin space and results in asymmetric spin fluctuation depending on the initial spin polarization state and the electron orbital momentum, which is induced by the electric field of the laser pulse.

Strong spin-orbit fields and Dyakonov-Perel spin dephasing in supported metallic films

Spin dephasing by the Dyakonov-Perel mechanism in metallic films deposited on insulating substrates is revealed, and quantitatively examined by means of density functional calculations combined with a kinetic equation. The surface-to-substrate asymmetry, probed by the metal wave functions in thin films, is found to produce strong spin-orbit fields and a fast Larmor precession, giving a dominant contribution to spin decay over the Elliott-Yafet spin relaxation up to a thickness of 70 nm. The spin dephasing is oscillatory in time with a rapid (sub-picosecond) initial decay. However, parts of the Fermi surface act as spin traps, causing a persistent tail signal lasting 1000 times longer than the initial decay time. It is also found that the decay depends on the direction of the initial spin polarization, resulting in a spin-dephasing anisotropy of 200% in the examined cases.

Power-dependent spin amplification in (In, Ga)As/GaAs quantum well via Pauli blocking by tunnel-coupled quantum dot ensembles

Power-dependent time-resolved optical spin orientation measurements were performed on In0.1Ga0.9As quantum well (QW) and In0.5Ga0.5As quantum dot (QD) tunnel-coupled structures with an 8-nm-thick GaAs barrier. A fast transient increase of electron spin polarization was observed at the QW ground state after circular-polarized pulse excitation. The temporal maximum of polarization increased with increasing pumping fluence owing to enhanced spin blocking in the QDs, yielding a highest amplification of 174% with respect to the initial spin polarization. Further elevation of the laser power gradually quenched the polarization dynamics, which was induced by saturated spin filling of both the QDs and the QW phase spaces.

Dynamics of a localized spin excitation close to the spin-helix regime

The time evolution of a local spin excitation in a (001)-confined two-dimensional electron gas subjected to Rashba and Dresselhaus spin-orbit interactions of similar strength is investigated theoretically and compared with experimental data. Specifically, the consequences of the finite spatial extension of the initial spin polarization is studied for non-balanced Rashba and Dresselhaus terms and for finite cubic Dresselhaus spin-orbit interaction. We show that the initial out-of-plane spin polarization evolves into a helical spin pattern with a wave number that gradually approaches the value $q_0$ of the persistent spin helix mode. In addition to an exponential decay of the spin polarization that is proportional to both the spin-orbit imbalance and the cubic Dresselhaus term, the finite width $w$ of the spin excitation reduces the spin polarization by a factor that approaches $\exp(-q_0^2 w^2/2)$ at longer times.