We study the spin dynamics of an electron-hole pair in a random hyperfine magnetic field and an external field, B0, under a resonant drive with frequency omega0 = gamma B0. The fact that the pair decays by recombination exclusively from a singlet configuration, S, in which the spins of the pair-partners are entangled, makes this dynamics highly nontivial. Namely, as the amplitude, B1, of the driving field grows, mixing all of the triplet components, the long-living modes do not disappear, but evolve from T+, T- into (T+ +/- sqrt(2) T0 + T-)/2. Upon further increase of B1, the lifetime of the S-mode is cut in half, while the T0-mode transforms into an antisymmetric combination (T- - T-)/sqrt(2) and acquires a long lifetime, in full analogy to the superradiant and subradiant modes in the Dicke effect. Peculiar spin dynamics translates into a peculiar dependence on B1. In particular, at small B1, the radiation-induced correction to the current is linear in B1.
We predict that singly-occupied carrier traps, produced by electrical stress or irradiation within organic semiconductors, can cause spin blockades and the large room-temperature magnetoresistance known as organic magnetoresistance. The blockade occurs because many singly-occupied traps can only become doubly occupied in a spin-singlet configuration. Magnetic-field effects on spin mixing during transport dramatically modify the effects of this blockade and produce magnetoresistance.We calculate the quantitative effects of these traps on organic magnetoresistance from percolation theory and fin…
Giant magnetoresistance (GMR) material has great potential as next generation magnetic field sensing devices, have magnetic properties and high electrical potential to be developed into various applications such as: magnetic field sensor measurements, current measurements, linear and rotational position sensor, data storage, head recording, and non-volatile magnetic random access memory (MRAM). Today, the new GMR materials based on organic material obtained after allowing for Organic Magnetoresistance (OMAR) was found in OLEDs (organic light-emitting diodes). This organic material is used as a…
Nanoscale multifunctional perpendicular organic spin valves have been fabricated. The devices based on an La$_{0.7}$Sr$_{0.3}$MnO$_3$/Alq$_3$/Co trilayer show resistive switching of up to 4-5 orders of magnitude and magnetoresistance as high as -70% the latter even changing sign when voltage pulses are applied. This combination of phenomena is typically observed in multiferroic tunnel junctions where it is attributed to magnetoelectric coupling between a ferromagnet and a ferroelectric material. Modeling indicates that here the switching originates from a modification of the La$_{0.7}$Sr$_{0.3…
We derive kinetic equations describing injection and transport of spin polarized carriers in organic semiconductors with hopping conductivity via an impurity level. The model predicts a strongly voltage dependent magnetoresistance, defined as resistance variation between devices with parallel and antiparallel electrode magnetizations (spin valve effect). The voltage dependence of the magnetoresistance splits into three distinct regimes. The first regime matches well known inorganic spintronic regimes, corresponding to barrier controlled spin injection or the well known conductivity mismatch ca…
We calculate the spin-polarized electronic transport through a molecular bilayer spin valve from first principles, and establish the link between the magnetoresistance and the spin-dependent inter- actions at the metal-molecule interfaces. The magnetoresistance of a Fe|bilayer-C70|Fe spin valve attains a high value of 70% in the linear response regime, but it drops sharply as a function of the applied bias. The current polarization has a value of 80% in linear response, and also decreases as a function of bias. Both these trends can be modelled in terms of prominent spin-dependent Fe|C70 inter…
Random hyperfine fields are essential to mechanisms of low-field magnetoresistance in organic semiconductors. Recent experiments have shown that another type of random field --- fringe fields due to a nearby ferromagnet --- can also dramatically affect the magnetoresistance. A theoretical analysis of the effect of these fringe fields is challenging, as the fringe field magnitudes and their correlation lengths are orders of magnitude larger than that of the hyperfine couplings. We extend a recent theory of organic magnetoresistance to calculate the magnetoresistance with both hyperfine and frin…
A recent theory of magnetoresistance in positionally disordered organic semiconductors is extended to include exchange and dipolar couplings between polarons. Analytic results are discovered when the hyperfine, exchange, and dipolar interactions have little time to operate between hopping events. We find an angle-of-field dependence of the magnetoresistance that agrees with previous experiments and numerical simulations. In addition we report new magnetoresistive behavior that critically depends upon the amount of anisotropy in the dipolar interaction.
A model of a spin valve in which electron transport between the magnetized electrodes is due to multistep tunneling is analyzed. Motivated by recent experiments on organic spin valves, we assume that spin memory loss in the course of transport is due to random hyperfine fields acting on electron while it waits for the next tunneling step. Amazingly, we identify the three-step configurations of sites, for which the tunnel magnetoresistance (TMR) is negative, suggesting that the resistance for antiparallel magnetizations of the electrodes is smaller than for parallel magnetizations. We analyze t…
We present a theory of organic magnetoresistance (OMR) based on the quenching of the quantum correlation between the carrier's spin and its local environment when the incoherent hopping takes place. We prove that this process contributes a spin-dependent prefactor to the attempt-to-escape frequency in the hopping rate, with its value modulated by the magnetic field. The resulting OMR exhibits a positive Lorentzian saturation component and a negative small-field component, which are independent of model parameters. These behaviors, with their isotope effects, are in good agreement with experime…
Motivated by recent experiments, where the tunnel magnetoresitance (TMR) of a spin valve was measured locally, we theoretically study the distribution of TMR along the surface of magnetized electrodes. We show that, even in the absence of interfacial effects (like hybridization due to donor and acceptor molecules), this distribution is very broad, and the portion of area with negative TMR is appreciable even if on average the TMR is positive. The origin of the local sign reversal is quantum interference of subsequent spin-rotation amplitudes in course of incoherent transport of carriers betwee…
We report the successful fabrication of lateral organic spin valves with a channel length in the sub $100\,nm$ regime. The fabication process is based on in-situ shadow evaporation under UHV conditions and therefore yields clean and oxygen-free interfaces between the ferromagnetic metallic electrodes and the organic semiconductor. The spin valve devices consist of Nickel and Cobalt-iron electrodes and the high mobility \emph{n}-type organic semiconductor $N,N'$-bis(heptafluorobutyl)-$3,4:9,10$-perylene diimide. Our studies comprise fundamental investigations of the process' and materials' suit…
The magneto-electronic field effects in organic semiconductors at high magnetic fields are described by field-dependent mixing between singlet and triplet states of weakly bound charge carrier pairs due to small differences in their Landé g-factors that arise from the weak spin-orbit coupling in the material. In this work, we corroborate theoretical models for the high-field magnetoresistance of organic semiconductors, in particular of diodes made of the conducting polymer poly(3,4-ethylenedioxythiophene):poly(styrene-sulfonate) (PEDOT:PSS) at low temperatures, by conducting magnetoresistance …
Organic spintronics is a promising emerging field, but the sign of the tunneling magnetoresistance (TMR) is highly sensitive to interface effects, a crucial hindrance to applications. A key breakthrough in molecular electronics was the discovery of amine-Au link groups that give reproducible conductance. Using first principles calculations, we predict that amine-Au links give improved reproducibility in organic spintronics junctions with Au-covered Fe leads. The Au layers allow only states with sp character to tunnel into the molecule, and the flexibility of amine-Au links results in a narrow …
A fabrication process for vertical organic spin-valve devices has been developed which offers the possibility to achieve active device areas of less than 500x500 nm^2 and is flexible in terms of material choice for the active layers. Characterization of the resulting devices shows a large magnetoresistance of sometimes more than 100%, however with equally large variation from device to device. Comparison with large-area spin-valves indicates that the magnetoresistance of both, large and small devices most likely originates from tunneling through pinholes and tunneling magnetoresistance.
We demonstrate that nuclear spin fluctuations lead to the electric current noise in the mesoscopic samples of organic semiconductors showing the pronounced magnetoresistance in weak fields. For the bipolaron and electron-hole mechanisms of organic magnetoresistance, the current noise spectrum consists of the high frequency peak related to the nuclear spin precession in the Knight field of the charge carriers and the low frequency peak related to the nuclear spin relaxation. The shape of the spectrum depends on the external magnetic and radiofrequency fields, which allows one to prove the role …
Highly-anisotropic in-plane magneto-resistance (MR) in graphite (HOPG) samples has been recently observed (Y. Kopelevich et al., arXiv:1202.5642) which is negative and linear in low fields in some current direction while it is giant, super-linear and positive in the perpendicular direction. In the framework of the hopping conductance theory via non-zero angular momentum orbitals we link extraordinary MRs in graphite and in organic insulators (OMAR) observed in about the same magnetic fields. The theory predicts quadratic negative MR (NMR) when there is a time-reversal symmetry (TRS), and linea…
In organic light emitting diodes with small area the current may be dominated by a finite number, N of sites in which the electron-hole recombination occurs. As a result, averaging over the hyperfine magnetic fields, b_h, that are generated in these sites by the environment nuclei is incomplete. This creates a random (mesoscopic) current component, ΔI(B), at field B having relative magnitude ~ N^(-1/2). To quantify the statistical properties of ΔI(B) we calculate the correlator K(B, ΔB)= <δI(B - ΔB/2)δI(B + ΔB/2)> for parallel and perpendicular orientations of ΔB. We demonstrate that mesoscopi…
We present calculations of spin-dependent electron transport through single organic molecules bridging pairs of iron nanocontacts. We predict the magnetoresistance of these systems to switch from positive to negative with increasing applied bias for both conducting and insulating molecules. This novel inverse magnetoresistance phenomenon is robust, does not depend on the presence of impurities, and is unique to molecular and atomic nanoscale magnetic junctions. Its physical origin is identified and its relevance to experiment and to potential technological applications is discussed.
In an external magnetic field B, the spins of the electron and hole will precess in effective fields b_e + B and b_h + B, where b_e and b_h are random hyperfine fields acting on the electron and hole, respectively. For sparse "soft" pairs the magnitudes of these effective fields coincide. The dynamics of precession for these pairs acquires a slow component, which leads to a slowing down of recombination. We study the effect of soft pairs on organic magnetoresistance, where slow recombination translates into blocking of the passage of current. It appears that when b_e and b_h have identical gau…
A universal mechanism for strong magnetic-field effects of nonmagnetic organic semiconductors is presented. A weak magnetic field (less than hundreds mT) can substantially change the charge carrier hopping coefficient between two neighboring organic molecules when the two hopping states are not too symmetric. Under the illumination of lights or under a high electric field, the change of hopping coefficients leads also to the change of polaron density so that photocurrent, photoluminescence, electroluminescence, magnetoresistance and electrical-injection current become sensitive to a weak magne…
Whereas spintronics brings the spin degree of freedom to electronic devices, molecular/organic electronics adds the opportunity to play with the chemical versatility. Here we show how, as a contender to commonly used inorganic materials, organic/molecular based spintronics devices can exhibit very large magnetoresistance and lead to tailored spin polarizations. We report on giant tunnel magnetoresistance of up to 300% in a (La,Sr)MnO3/Alq3/Co nanometer size magnetic tunnel junction. Moreover, we propose a spin dependent transport model giving a new understanding of spin injection into organic …
The field dependence of interlayer magnetoresistance of the pressurized (to the normal state) layered organic metal $α$-(BEDT-TTF)$_{2}$KHg(SCN)$_{4}$ is investigated. The high quasi-two-dimensional anisotropy, when the interlayer hopping time is longer than the electron mean-free time and than the cyclotron period, leads to a dimensional crossover and to strong violations of the conventional three-dimensional theory of magnetoresistance. The monotonic field dependence is found to change from the conventional behavior at low magnetic fields to an anomalous one at high fields. The shape of Land…
The chirality-induced spin selectivity (CISS) effect gives rise to strongly spin-dependent transport through many organic molecules and structures. Its discovery raises fascinating fundamental questions as well as the prospect of possible applications. The basic phenomenology, a strongly asymmetric magnetoresistance despite the absence of magnetism, is now understood to result from the combination of spin-orbit coupling and chiral geometry. However, experimental signatures of electronic helicity were observed at room temperature, i.e., at an energy scale that exceeds the typical spin-orbit cou…
We perform electronic measurements of unidirectional spin Hall magnetoresistance (USMR) in a Permalloy/Pt bilayer, in conjunction with magneto-optical Brillouin light spectroscopy of spin current-driven magnon population. We show that the current dependence of USMR closely follows the dipolar magnon density, and that both dependencies exhibit the same scaling over a large temperature range of 80-400 K. These findings demonstrate a close relationship between spin current-driven magnon generation and USMR, and indicate that the latter is likely dominated by the dipolar magnons.
We investigate spin precession (Hanle effect) in the prototypical organic spintronic giant magnetoresistance (GMR) device La0.7Sr0.3MnO3(LSMO)/tris(8-hydroxyquinoline)(Alq3)/AlOx/Co. The Hanle effect is not observed in measurements taken by sweeping a magnetic field at different angles from the plane of the device. As possible explanations we discuss the tilting out of plane of the magnetization of the electrodes, exceptionally high mobility or hot spots. Our results call for a greater understanding of spin injection and transport in such devices.
Over the last two decades organic spintronics has developed into a striving field with exciting reports of long spin diffusion lengths and spin relaxation times in organic semiconductors (OSCs). Easily processed and inexpensive, OSCs are considered a potential alternative to inorganic materials for use in spintronic applications. Spin currents have been detected in a wide range of materials, however, there is still uncertainty over the origin of the signals. Recently, we explored spin transport through an organic semiconductor with lateral spin injection and detection architectures, where the …
A universal mechanism for strong magnetic-field effects of nonmagnetic organic semiconductors is presented. A weak magnetic field (less than hundreds mT) can substantially change the charge carrier hopping coefficient between two neighboring organic molecules when the magnetic length is not too much longer than the molecule-molecule separation and localization length of electronic states involved. Under the illumination of lights or under a high electric field, the change of hopping coefficients leads also to the change of polaron density so that photocurrent, photoluminescence, electrolumines…
We present a microscopic theory on the observation of a beating pattern in the radiation-induced magnetoresistance oscillations at very low magnetic field. We con- sider that such a beating pattern develops as a result of the coupling between two oscillatory components: the first is a system of electron Landau states being harmon- ically driven by radiation. The second is a lattice oscillation, i.e., an acoustic phonon mode. We analyze the dependence of the beating pattern on temperature, radiation frequency and power. We conclude that the beating pattern is an evidence of the radiation-driven…
Spin-orbit-torque-driven dynamics have recently gained interest in the field of magnetism due to the reduced requirement of current densities and an increase in efficiency, as well as the ease of implementation of different devices and materials. From a practical point of view, the low-frequency dynamics below 1 GHz is particularly interesting since dynamics associated with magnetic domains lie in this frequency range. While spin-torque excitation of high-frequency modes has been extensively studied, the intermediate low-frequency dynamics have received less attention, although spin torques co…
In a bilayer consisting of an insulator (I) and a ferromagnetic metal (FM), interfacial spin orbit scattering leads to spin mixing of the two conducting channels of the FM, which results in an unconventional anisotropic magnetoresistance (AMR). We theoretically investigate the magnetotransport in such bilayer structures by solving the spinor Boltzmann transport equation with generalized Fuchs-Sondheimer boundary condition that takes into account the effect of spin orbit scattering at the interface. We find that the new AMR exhibits a peculiar angular dependence which can serve as a genuine exp…
We use electrical spin injection to probe exchange interactions in phosphorus doped silicon (Si:P). The detection is enabled by a magnetoresistance effect that demonstrates the efficiency of exchange in imprinting spin information from the magnetic lead onto the localized moments in the Si:P region. A unique Lorentzian-shaped signal existing only at low temperatures ($\lesssim 25 K$) is observed experimentally and analyzed theoretically in electrical Hanle effect measurement. It stems from spin-dependent scattering of electrons by neutral impurities in Si:P. The shape of this signal is not dir…
It is shown that in rather strong magnetic field the interlayer electron conductivity is exponentially damped by the Coulomb barrier arising from the formation of polaron around each localized electron state. The theoretical model is developed to describe this effect, and the calculation of the temperature and field dependence of interlayer magnetoresistance is performed. The results obtained agree well with the experimental data in GaAs/AlGaAs heterostructures and in strongly anisotropic organic metals. The proposed theory allows to use the experiments on interlayer magnetoresistance to inves…
Observations of $ν=1$ Quantum Hall Effect and Inter-Band Effects of Magnetic fields on Hall Conductivity in Organic Massless Dirac Fermion System $α$-(BETS)$_2$I$_3$ under Pressure
本文在压力下的 α-(BETS)₂I₃ 有机无质量 Dirac 费米子体系中观测到 ν=1 量子 Hall 态，并通过化学势跨越 Dirac 点揭示了磁场对 Hall 电导率的带间效应。
We studied spin transport in four organic semiconductors (OSCs) with different electronic properties, with Fe and Co as the top and bottom ferromagnetic (FM) contacts, respectively. Magnetoresistance (MR) effects were observed up to room temperature in junctions based on an electron-carrying OSC, tris(8-hyroxyquinoline) aluminum (Alq$_3$) and a hole-carrying OSC, copper phthalocyanine (CuPc). The MR shows similar temperature dependence for these two OSCs, which suggests that the FM leads rather than the OSCs play a dominant role on the spin-transport degradation with increasing temperature. We…
Colossal Magnetoresistance and Phonon Driven Exchange Dynamics in Eu$_5$Sn$_2$As$_6$
University of Tokyo（东京大学）；University of California, Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；National High Magnetic Field Laboratory, Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室国家高磁场实验室）；Molecular Foundry, Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室分子发现中心）；Physikalisch-Technische Bundesanstalt（德国物理技术联邦研究院）
Long-range energy transfer in organic molecules has been experimentally obtained by strongly coupling their electronic excitations to a confined electromagnetic cavity mode. Here, we shed light into the polariton-mediated mechanism behind this process for different configurations: donor and acceptor molecules either intermixed or physically separated. We numerically address the phenomenon by means of Bloch-Redfield theory, which allows us to reproduce the effect of complex vibrational reservoirs characteristic of organic molecules. Our findings reveal the key role played by the middle polarito…
The LAO/STO interface hosts a two-dimensional electron system that is unusually sensitive to the application of an in-plane magnetic field. Low-temperature experiments have revealed a giant negative magnetoresistance (dropping by 70\%), attributed to a magnetic-field induced transition between interacting phases of conduction electrons with Kondo-screened magnetic impurities. Here we report on experiments over a broad temperature range, showing the persistence of the magnetoresistance up to the 20~K range --- indicative of a single-particle mechanism. Motivated by a striking correspondence bet…
We report on the temperature and electric field driven evolution of the magnetoresistance lineshape at an interface between Ni/AlO$_x$ and Nb-doped SrTiO$_3$. This is manifested as a superposition of the Lorentzian lineshape due to spin accumulation and a parabolic background related to tunneling anisotropic magnetoresistance (TAMR). The characteristic Lorentzian line shape of the spin voltage is retrieved only at low temperatures and large positive applied bias. This is caused by the reduction of electric field at large positive applied bias which results in a simultaneous reduction of the ba…
