Electron Spin Excitation Research Articles

Effects of finite material size on axion-magnon conversion

Magnetic materials are particularly favorable targets for detecting axions interacting with electrons because the collective excitation of electron spins, the magnon, can be excited through the axion-magnon conversion process. It is often assumed that only the zero-momentum uniformly precessing magnetostatic (Kittel) mode of the magnon is excited. This is justified if the de Broglie wavelength of the axion is much longer than the size of the target magnetic material. However, if the de Broglie wavelength is shorter, finite-momentum magnon modes can also be excited. We systematically analyze the target material size dependence of the axion-magnon conversion rate. We discuss the importance of these effects in the detection of relativistic axions as well as in the detection of axion dark matter of relatively heavy mass with large material size.

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.

Nanosheet fabrication from magnon thermal conductivity cuprates for the advanced thermal management

Spin-chain–spin-ladder cuprates, such as La5Ca9Cu24O41, have notable electronic and thermal properties because of their unique electron spin arrangement. Among them, magnon thermal conductivity, which originates from the excitation of paired electron spins, is promising for the advanced thermal management applications that enable dynamic control of heat flow. This is because of its high, anisotropic thermal conductivity at room temperature and its dynamic controllability. In this study, we report nanosheet fabrications from polycrystalline La5Ca9Cu24O41 to enhance the control width. We obtained that the nanosheets with a thickness of about 3 nm are obtained via immersion of the polycrystals in a NaOH aqueous solution. We propose the exfoliation model based on the chemical reaction between the (La/Ca)2Cu2O3 subsystem and NaOH solution. The nanosheet fabrications can also lead to new research development on spin-ladder system and other strongly correlated cuprates.

Spin excitations in the quantum dipolar magnet Yb(BaBO3)3

We report results of magnetization, specific-heat and muon-spin relaxation measurements on single crystals of disorder-free Yb$^{3+}$ triangular lattice Yb(BaBO$_3$)$_3$. The magnetization experiments show anisotropic magnetic properties with Curie-Weiss temperatures $\theta_{\perp}=-1.40$~K ($H \perp c$) and $\theta_{\parallel}=-1.16$~K ($H \parallel c$) determined from low temperature data. The absence of both long-range antiferromagnetic order and spin freezing is confirmed down to 0.27 K at zero field. A two-level Schottky anomaly due to the opening of the ground-state Kramers doublet is observed from the low-temperature specific-heat measurements when the applied magnetic fields $\mu_0H >0.7$~T. At zero field, the increase of both $C_{\rm mag}/T$ and the muon spin relaxation rate $\lambda$ below 1~K is due to the electronic spin excitations, which often exist in quantum magnets where dipole-dipole interaction creates an anisotropy of magnetic properties. The spin excitation is also supported by the unusual maximum of field dependence of $\lambda$ due to the field-induced increase of the density of excitations. We argue that dipolar interaction is dominant and induces the spin dynamics in the quantum magnet Yb(BaBO$_3$)$_3$.

Magnonics Based on Thin-Film Iron Garnets

Spin waves and their quanta magnons are collective excitation of electron spins in magnetic materials which can serve as information carriers for future low-power-consumption computing systems. Fer...

Suppression of thermally excited electron-spin relaxation in InGaAs quantum dots using p-doped capping layers toward enhanced room-temperature spin polarization

The suppression of a thermally excited electron-spin relaxation in InGaAs quantum dots (QDs) using p-doped capping layers toward enhanced room-temperature (RT) spin polarization has been demonstrated, in which the electron-spin polarization in QD excited states (ESs) was measured through time-resolved spin-dependent photoluminescence. We revealed that the p-doping of QDs can enhance the emission intensity of QD-ES by approximately twofold to threefold over a wide temperature range. An electron-spin relaxation time of 106 ps was observed at 293 K for p-doped QDs, which is approximately three times longer than the radiative lifetime of 36 ps, relative to the shorter electron-spin relaxation time of 71 ps for undoped QDs. The increased electron-spin lifetime was mainly attributed to the suppressed relaxation of the electron spin reinjected from the p-doped capping barrier after thermal escape from an ES, where the D'yakonov-Perel' spin relaxation in the barrier was potentially weakened through impurity scattering. These results suggest that InGaAs QDs with p-doped capping layers have a significant advantage for use in spin-functional optical active layers with a higher spin polarization toward RT.

Adiabatic generalized gradient approximation kernel in time-dependent density functional theory

A complete understanding of a material requires both knowledge of the excited states as well as of the ground state. In particular, the low energy excitations are of utmost importance while studying the electronic, magnetic, dynamical, and thermodynamical properties of the material. Time-Dependent Density Functional Theory (TDDFT), within the linear regime, is a successful \textit{ab-initio} method to access the electronic charge and spin excitations. However, it requires an approximation to the exchange-correlation (XC) kernel which encapsulates the effect of electron-electron interactions in the many-body system. In this work we derive and implement the spin-polarized XC kernel for semi-local approximations such as the adiabatic Generalized Gradient Approximation (AGGA). This kernel has a quadratic dependence on the wavevector, {\bf q}, of the perturbation, however the impact of this on the electron energy loss spectra (EELS) is small. Although the GGA functional is good in predicting structural properties, it generality overestimates the exchange spin-splitting. This leads to higher magnon energies, as compared to both ALDA and experiment. In addition, interaction with the Stoner spin-flip continuum is enhanced by AGGA, which strongly suppresses the intensity of spin-waves.

Single crystal, spectral and electronic transition studies on (E)-N-(3-methoxy-4-hydroxybenzylidene)-4-nitrobenzohydrazide monohydrate

The single crystal of (E)-N-(3-Methoxy-4-hydroxybenzylidene)-4-nitrobenzohydrazide monohydrate (MHBNB) was grown by a slow evaporation method. The crystal structure was determined by single crystal X-ray diffraction method. The electron density, Hirshfeld surface and fingerprint analysis reveals that the crystal packing is governed by several weak OH⋯C, OH⋯O and OH⋯N intermolecular interactions. The analysis of bond critical points (BCP) and topology of the crystalline form of MHBNB were done. The intrusion of H2O molecule does not affect the aromaticity of the pheyl rings but marginally disturbs the aromaticity of hydrazide link. The FT-IR (4000-400 cm−1) and FT-Raman (3500-50 cm−1) spectra were recorded to study the vibrational behavior of MHBNB molecule. To explore the electronic transition of MHBNB, the UV absorbance spectrum was recorded in the range of 200–800 nm. Furthermore, the Density functional theory (DFT) and Time-dependent DFT (TD-DFT) calculations were performed to investigate the molecular geometry, vibrational behavior, electronic excitation and inter-intramolecular charge transfers within the molecule. The singlet (S) and Triplet (T) electronic excited states (n state = 6) of MHBNB were examined, in which, the electron spin density (s), excitation energy (ΔE1-6), oscillator strength (f) and electric dipole moment (μ) were examined. The frontier molecular orbitals (FMOs) were studied to find the band gap of FMOs. The natural atomic orbitals (NAO) and natural localized molecular orbitals (NLMO) of MHBNB were analyzed. The density of states (DOS) and Total density of states (TDOS) of functional groups in MHBNB molecule were also evaluated. This compound has very good first order hyperpolarizability (β0) coefficient.

Antioxidant and antimicrobial activity of bioactive prodigiosin produces from Serratia marcescens using agricultural waste as a substrate.

The objective of this investigation was to explore the antioxidant and antimicrobial property of bioactive prodigiosin produced from Serratia marcescens using rice bran. The antioxidant potential of prodigiosin was examined by 2, 2-diphenyl-1-picrylhydrazyl (DPPH) and 2, 2'-azino-bis 3-ethylbenzthiazoline-6-sulfonic acid (ABTS) radical scavenging method via UV-visible, electron spin resonance spectrum (ESR), cyclic voltammetry and excitation emission spectrum. The antimicrobial activity of prodigiosin was examined against foodborne pathogens. The shelf life extending capacity of prodigiosin was evaluated with meat extract powder (MEP) as a model food material. The DPPH and ABTS radicals were completely scavenged by prodigiosin at the concentration of 10mg/L. The food spoilage was inhibited by the addition of prodigiosin with MEP and it was compared with conventional preservative. The prodigiosin has prohibited the growth of foodborne pathogens effectively and the shelf life of the food was also extended significantly. The antimicrobial edible preservative developed in this study inhibited the growth of the microbial populations that produced through storage of the MEP and free radical scavenging activity. The results reveal that the bioactive prodigiosin effectively scavenged the free radical and inhibited the bacterial growth in food stuff.

Excited State Magnetic Exchange Interactions Enable Large Spin Polarization Effects.

Excited state processes involving multiple electron spin centers are crucial elements for both spintronics and quantum information processing. Herein, we describe an addressable excited state mechanism for precise control of electron spin polarization. This mechanism derives from excited state magnetic exchange couplings that occur between the electron spins of a photogenerated electron-hole pair and that of an organic radical. The process is initiated by absorption of a photon followed by ultrafast relaxation within the excited state spin manifold. This leads to dramatic changes in spin polarization between excited states of the same multiplicity. Moreover, this photoinitiated spin polarization process can be "read" spectroscopically using a magnetooptical technique that is sensitive to the excited state electron spin polarizations and allows for the evaluation of wave functions that give rise to these polarizations. This system is unique in that it requires neither intersystem crossing nor magnetic resonance techniques to create dynamic spin-polarization effects in molecules.

Full cycle rapid scan EPR deconvolution algorithm

Rapid scan electron paramagnetic resonance (RS EPR) is a continuous-wave (CW) method that combines narrowband excitation and broadband detection. Sinusoidal magnetic field scans that span the entire EPR spectrum cause electron spin excitations twice during the scan period. Periodic transient RS signals are digitized and time-averaged. Deconvolution of absorption spectrum from the measured full-cycle signal is an ill-posed problem that does not have a stable solution because the magnetic field passes the same EPR line twice per sinusoidal scan during up- and down-field passages. As a result, RS signals consist of two contributions that need to be separated and postprocessed individually. Deconvolution of either of the contributions is a well-posed problem that has a stable solution. The current version of the RS EPR algorithm solves the separation problem by cutting the full-scan signal into two half-period pieces. This imposes a constraint on the experiment; the EPR signal must completely decay by the end of each half-scan in order to not be truncated. The constraint limits the maximum scan frequency and, therefore, the RS signal-to-noise gain. Faster scans permit the use of higher excitation powers without saturating the spin system, translating into a higher EPR sensitivity. A stable, full-scan algorithm is described in this paper that does not require truncation of the periodic response. This algorithm utilizes the additive property of linear systems: the response to a sum of two inputs is equal the sum of responses to each of the inputs separately. Based on this property, the mathematical model for CW RS EPR can be replaced by that of a sum of two independent full-cycle pulsed field-modulated experiments. In each of these experiments, the excitation power equals to zero during either up- or down-field scan. The full-cycle algorithm permits approaching the upper theoretical scan frequency limit; the transient spin system response must decay within the scan period. Separation of the interfering up- and down-field scan responses remains a challenge for reaching the full potential of this new method. For this reason, only a factor of two increase in the scan rate was achieved, in comparison with the standard half-scan RS EPR algorithm. It is important for practical use that faster scans not necessarily increase the signal bandwidth because acceleration of the Larmor frequency driven by the changing magnetic field changes its sign after passing the inflection points on the scan. The half-scan and full-scan algorithms are compared using a LiNC-BuO spin probe of known line-shape, demonstrating that the new method produces stable solutions when RS signals do not completely decay by the end of each half-scan.

Tuning the spin coherence time of Cu(II)-(bis)oxamato and Cu(II)-(bis)oxamidato complexes by advanced ESR pulse protocols.

We have investigated with the pulsed ESR technique at X- and Q-band frequencies the coherence and relaxation of Cu spins S = 1/2 in single crystals of diamagnetically diluted mononuclear [n-Bu4N]2[Cu(opba)] (1%) in the host lattice of [n-Bu4N]2[Ni(opba)] (99%, opba = o-phenylenebis(oxamato)) and of diamagnetically diluted mononuclear [n-Bu4N]2[Cu(opbon-Pr2)] (1%) in the host lattice of [n-Bu4N]2[Ni(opbon-Pr2)] (99%, opbon-Pr2 = o-phenylenebis(N(propyl)oxamidato)). For that we have measured the electron spin dephasing time Tm at different temperatures with the two-pulse primary echo and with the special Carr–Purcell–Meiboom–Gill (CPMG) multiple microwave pulse sequence. Application of the CPMG protocol has led to a substantial increase of the spin coherence lifetime in both complexes as compared to the primary echo results. It shows the efficiency of the suppression of the electron spin decoherence channel in the studied complexes arising due to spectral diffusion induced by a random modulation of the hyperfine interaction with the nuclear spins. We argue that this method can be used as a test for the relevance of the spectral diffusion for the electron spin decoherence. Our results have revealed a prominent role of the opba4– and opbon-Pr24– ligands for the dephasing of the Cu spins. The presence of additional 14N nuclei and protons in [Cu(opbon-Pr2)]2– as compared to [Cu(opba)]2– yields significantly shorter Tm times. Such a detrimental effect of the opbon-Pr24− ligands has to be considered when discussing a potential application of the Cu(II)−(bis)oxamato and Cu(II)−(bis)oxamidato complexes as building blocks of more complex molecular structures in prototype spintronic devices. Furthermore, in our work we propose an improved CPMG pulse protocol that enables elimination of unwanted echoes that inevitably appear in the case of inhomogeneously broadened ESR spectra due to the selective excitation of electron spins.

Phase diagram and neutron spin resonance of superconducting NaFe1−xCuxAs

We use transport and neutron scattering to study the electronic phase diagram and spin excitations of NaFe$_{1-x}$Cu$_x$As single crystals. Similar to Co- and Ni-doped NaFeAs, a bulk superconducting phase appears near $x\approx2\%$ with the suppression of stripe-type magnetic order in NaFeAs. Upon further increasing Cu concentration the system becomes insulating, culminating in an antiferromagnetically ordered insulating phase near $x\approx 50\%$. Using transport measurements, we demonstrate that the resistivity in NaFe$_{1-x}$Cu$_x$As exhibits non-Fermi-liquid behavior near $x\approx1.8\%$. Our inelastic neutron scattering experiments reveal a single neutron spin resonance mode exhibiting weak dispersion along $c$-axis in NaFe$_{0.98}$Cu$_{0.02}$As. The resonance is high in energy relative to the superconducting transition temperature $T_{\rm c}$ but weak in intensity, likely resulting from impurity effects. These results are similar to other iron pnictides superconductors despite the superconducting phase in NaFe$_{1-x}$Cu$_x$As is continuously connected to an antiferromagnetically ordered insulating phase near $x\approx 50\%$ with significant electronic correlations. Therefore, electron correlations is an important ingredient of superconductivity in NaFe$_{1-x}$Cu$_x$As and other iron pnictides.

Inhomogeneous nuclear spin polarization induced by helicity-modulated optical excitation of fluorine-bound electron spins in ZnSe

Optically-induced nuclear spin polarization in a fluorine-doped ZnSe epilayer is studied by time-resolved Kerr rotation using resonant excitation of donor-bound excitons. Excitation with helicity-modulated laser pulses results in a transverse nuclear spin polarization, which is detected as a change of the Larmor precession frequency of the donor-bound electron spins. The frequency shift in dependence on the transverse magnetic field exhibits a pronounced dispersion-like shape with resonances at the fields of nuclear magnetic resonance of the constituent zinc and selenium isotopes. It is studied as a function of external parameters, particularly of constant and radio frequency external magnetic fields. The width of the resonance and its shape indicate a strong spatial inhomogeneity of the nuclear spin polarization in the vicinity of a fluorine donor. A mechanism of optically-induced nuclear spin polarization is suggested based on the concept of resonant nuclear spin cooling driven by the inhomogeneous Knight field of the donor-bound electron.

Mechanism for nuclear and electron spin excitation by radio frequency current

Recent radio frequency scanning tunneling spectroscopy (rf-STS) experiments have demonstrated nuclear and electron spin excitations up to $\pm12\hbar$ in a single molecular spin quantum dot (qudot). Despite the profound experimental evidence, the observed independence of the well-established dipole selection rules is not described by existing theory of magnetic resonance -- pointing to a new excitation mechanism. Here we solve the puzzle of the underlying mechanism by presenting all relevant mechanistic steps. At the heart of the mechanism, periodic transient charging and electric polarization due to the rf-modulated tunneling process cause a periodic asymmetric deformation of the qudot, enabling spin transitions via spin-phonon-like coupling. The mechanism has general relevance for a broad variety of different spin qudots exhibiting internal mechanical degrees of freedom (organic molecules, doped semiconductor qudots, nanocrystals, etc.).

Electronic structure, spin excitations, and orbital ordering in a three-orbital model for iron pnictides

A three-orbital itinerant-electron model involving dxz, dyz and dxy Fe 3d orbitals is proposed for iron pnictides towards understanding the () ordered magnetism and magnetic excitations in these materials. It is shown that this model at half filling yields a gapped () magnetic state, and simultaneously reproduces several experimentally observed features such as the electronic structure, spin excitations, as well as the ferro orbital order between the dxz and dyz orbitals.

Nanoengineered diamond waveguide as a robust bright platform for nanomagnetometry using shallow nitrogen vacancy centers.

Photonic structures in diamond are key to most of its application in quantum technology. Here, we demonstrate tapered nanowaveguides structured directly onto the diamond substrate hosting shallow-implanted nitrogen vacancy (NV) centers. By optimization based on simulations and precise experimental control of the geometry of these pillar-shaped nanowaveguides, we achieve a net photon flux up to ∼ 1.7 × 10(6) s(-1). This presents the brightest monolithic bulk diamond structure based on single NV centers so far. We observe no impact on excited state lifetime and electronic spin dephasing time (T2) due to the nanofabrication process. Possessing such high brightness with low background in addition to preserved spin quality, this geometry can improve the current nanomagnetometry sensitivity ∼ 5 times. In addition, it facilitates a wide range of diamond defects-based magnetometry applications. As a demonstration, we measure the temperature dependency of T1 relaxation time of a single shallow NV center electronic spin. We observe the two-phonon Raman process to be negligible in comparison to the dominant two-phonon Orbach process.

Time and spatially resolved electron spin detection in semiconductor heterostructures by magneto‐optical Kerr microscopy

We review on time and spatially resolved two‐color pump–probe magneto‐optical Kerr effect (MOKE) microscopy studies of electron spins in bulk n‐GaAs and GaAs (110) quantum wells (QWs) at low lattice temperatures. The influence of photocarrier heating by above‐bandgap optical spin excitation on the spatially resolved magneto‐optical spin detection is considered in detail. We demonstrate that a continuous‐wave (cw) measurement of the local Kerr rotation at a fixed arbitrary probe wavelength in general does not correctly reveal the local spin polarization when hot electrons are present. For bulk GaAs we determine the true lateral electron spin polarization profile from cw measurements of the spatial dependence of the full excitonic Kerr rotation spectrum. For the (110) QWs, we directly obtain the electron spin diffusion coefficient from picosecond real space imaging of the time evolution of an optically excited electron spin packet, which we observe with a spectrally broad probe pulse.

High-energy spin and charge excitations in electron-doped copper oxide superconductors

The evolution of electronic (spin and charge) excitations upon carrier doping is an extremely important issue in superconducting layered cuprates and the knowledge of its asymmetry between electron- and hole-dopings is still fragmentary. Here we combine X-ray and neutron inelastic scattering measurements to track the doping dependence of both spin and charge excitations in electron-doped materials. Copper L3 resonant inelastic X-ray scattering spectra show that magnetic excitations shift to higher energy upon doping. Their dispersion becomes steeper near the magnetic zone centre and they deeply mix with charge excitations, indicating that electrons acquire a highly itinerant character in the doped metallic state. Moreover, above the magnetic excitations, an additional dispersing feature is observed near the Γ-point, and we ascribe it to particle-hole charge excitations. These properties are in stark contrast with the more localized spin excitations (paramagnons) recently observed in hole-doped compounds even at high doping levels.

Electron-spin excitation by implanting hydrogen into metallofullerene: the synthesis and spectroscopic characterization of Sc4C2H@I(h)-C80.

A hydrogen-containing endohedral metallofullerene, Sc4C2H@Ih-C80, was synthesized and its paramagnetism was measured by the low-temperature EPR spectrometry with a broad EPR signal. The electron-spin excitation by implanting the H-atom would be a new method for preparation of stable paramagnetic metallofullerenes.