单分子磁体的自旋电子输运
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摘要
在分子自旋电子学领域,单分子磁体因其具有独特的大自旋和磁单轴各向异性,使其在信息存储和处理方面有潜在的应用价值,因此它的电子输运受到广泛关注。在实验和理论的研究中,由于传输电子与分子之间存在自旋交换作用,一系列有趣的物理效应被发现,比如Berry相阻塞,分子磁体的磁化反转,热电效应诱导的纯自旋流等。自旋极化输运是自旋电子学的核心问题,在本论文中,运用率方程方法,我们关注于单分子磁体耦合铁磁电极体系的自旋相关输运。
首先,研究了与两个铁磁电极连接的单分子磁体系统中的电荷流和自旋流,其中铁磁电极的磁化方向与分子磁体的易磁化轴是共线的。在顺序隧穿和共隧穿区域,我们考虑了铁磁电极在平行和反平行构型以及传输电子自旋和分子局域大自旋为铁磁和反铁磁交换作用四种情形下的电子输运,其中包括电荷流,微分电导,自旋流和电流极化率。在这个系统中,我们发现了一个新奇有趣的物理现象：在铁磁电极处于反平行构型并且电子和分子局域自旋是反铁磁交换作用的情形下,自旋流的方向在偏压的操控下可以反转,它不需要偏压的反向。此特性可以用来设计一个偏压调控的自旋流反转电子器件。
其次,在顺序隧穿和共隧穿区域,研究了内在自旋弛豫对单分子磁体自旋极化输运特性的影响,重点讨论了对隧穿磁阻的影响。我们发现隧穿磁阻在顺序隧穿区域内随着自旋弛豫的增强几乎消失；而在共隧穿区域内可以从一个很大的正值变为一个较小的负值。当沿着单分子磁体的易磁化轴施加一个磁场时,隧穿磁阻将关于正负偏压不对称。在共隧穿区域,自旋弛豫对负偏压区域的隧穿磁阻影响较小；而在正偏压区域内隧穿磁阻可以从正值变到负值。特别是,在顺序隧穿区域,很快的自旋弛豫过程可以使正偏压区域内的隧穿磁阻从正值变为一个比较大的负值。此外,对于大偏压极限的情形,在负偏压区域的隧穿磁阻随着内禀自旋弛豫的增强将稍大于典型的顺序隧穿磁阻值,而隧穿磁阻在正偏压区域从正值变为负值。
然后,我们研究了由单分子磁体耦合一个铁磁电极和一个正常金属电极所组成的隧穿结的顺序隧穿输运,发现了典型的隧穿各向异性磁阻效应,它随着铁磁电极磁化方向与分子易磁化轴之间的夹角的改变而变化,从而可以在实验上来确定单分子磁体的易磁化轴的相对取向。我们还发现偏压可以有效地调控隧穿各向异性磁阻值的大小和正负。此性质可以用来设计基于分子磁体的单铁磁电极的自旋阀器件。
最后,在铁磁金属/单分子磁体/正常金属的隧穿结的自旋注入研究中,我们发现可以产生远大于铁磁电极极化率的自旋流,并且在偏压的控制下,自旋流的方向和大小都可以改变。因此,基于单分子磁体,可以实现高效自旋注入和有效调控的自旋器件。
In molecular spintronics, single-molecule magnets (SMMs) possess high spins and uniaxial magnetic anisotropy with an easy axis, which have potential applications in information storage and processing, and electron transport through SMMs has received much attention. In both experimental and theoretical aspects, since the spin-exchange interaction between the tunneling electron and the molecule, many interesting properties have been found, such as Berry-phase blockade, the magnetization reversal of SMM, and thermoelectric effect induced pure spin-current. Spin-polarized transport is at the heart of spintronics, and thus in this thesis, within a rate-equation approach we focus on the spin-dependent transport through a SMM weakly coupled to magnetic electrodes.
First, we theoretically study the charge and spin currents through a SMM between ferromagnetic leads, where the magnetizations of two magnetic electrodes are collinear with the magnetic easy-axis of the SMM. In both sequential and cotunneling regimes, we systematically study the cases of ferromagnetic and antiferromagnetic coupling between a tunneling electron and the local molecular spin in the parallel and antiparallel lead magnetizations. We exhibit the charge and spin current, the differential conductance, and the current spin polarization as functions of bias voltage for all cases. An interesting observation is that the polarization reversal of spin-current can be realized and manipulated by the variation of bias voltage (but not inverting) in the case of antiferromagnetic exchange-coupling with antiparallel lead-configuration. The above effect may be useful in the development of spintronic devices, which can reverse the direction of spin current.
Secondly, we investigate the effects of intrinsic spin relaxation on the spin-dependent transport through a SMM with ferromagnetic leads in both the sequential and cotunneling regimes, and discuss mainly the effect on the tunneling magnetoresistance (TMR). It is shown that the TMR disappears almost under the fast spin-relaxation in the sequential regime while can vary from large positive to small negative values in the cotunneling regime. Moreover, when a magnetic field is applied along the easy-axis of SMM, a large negative TMR is obtained with the increase of the relaxation strength. Finally in the large-bias voltage limit, the TMR for the negative bias is slightly larger than its characteristic value in the sequential regime, but for the positive bias it becomes a negative value due to the fast spin-relaxation.
Then, we study electron transport through SMM junctions with one ferromagnetic lead and one normal-metal lead in the sequential regime, and find the typical tunneling anisotropic magnetoresistance (TAMR) effect, which varies with the angle between the magnetization direction of ferromagnetic lead and the easy-axis of SMM. The angular dependence of TAMR can serve as a probe to determine experimentally the easy-axis of SMM. Moreover, it is demonstrated that both the magnitude and sign of TAMR are tunable by the bias voltage, suggesting a new spin-valve device with only one magnetic electrode in molecular spintronics.
Finally, we present a proposal for a voltage-tunable SMM based spin current injector. The device consists of a SMM that is weakly coupled to one ferromagnetic electrode and one nonmagnetic electrode. We show that the current polarization can be dramatically enhanced. Moreover, the sign of spin-polarization can be changed by the gate or the bias voltage.
首先,研究了与两个铁磁电极连接的单分子磁体系统中的电荷流和自旋流,其中铁磁电极的磁化方向与分子磁体的易磁化轴是共线的。在顺序隧穿和共隧穿区域,我们考虑了铁磁电极在平行和反平行构型以及传输电子自旋和分子局域大自旋为铁磁和反铁磁交换作用四种情形下的电子输运,其中包括电荷流,微分电导,自旋流和电流极化率。在这个系统中,我们发现了一个新奇有趣的物理现象：在铁磁电极处于反平行构型并且电子和分子局域自旋是反铁磁交换作用的情形下,自旋流的方向在偏压的操控下可以反转,它不需要偏压的反向。此特性可以用来设计一个偏压调控的自旋流反转电子器件。
其次,在顺序隧穿和共隧穿区域,研究了内在自旋弛豫对单分子磁体自旋极化输运特性的影响,重点讨论了对隧穿磁阻的影响。我们发现隧穿磁阻在顺序隧穿区域内随着自旋弛豫的增强几乎消失；而在共隧穿区域内可以从一个很大的正值变为一个较小的负值。当沿着单分子磁体的易磁化轴施加一个磁场时,隧穿磁阻将关于正负偏压不对称。在共隧穿区域,自旋弛豫对负偏压区域的隧穿磁阻影响较小；而在正偏压区域内隧穿磁阻可以从正值变到负值。特别是,在顺序隧穿区域,很快的自旋弛豫过程可以使正偏压区域内的隧穿磁阻从正值变为一个比较大的负值。此外,对于大偏压极限的情形,在负偏压区域的隧穿磁阻随着内禀自旋弛豫的增强将稍大于典型的顺序隧穿磁阻值,而隧穿磁阻在正偏压区域从正值变为负值。
然后,我们研究了由单分子磁体耦合一个铁磁电极和一个正常金属电极所组成的隧穿结的顺序隧穿输运,发现了典型的隧穿各向异性磁阻效应,它随着铁磁电极磁化方向与分子易磁化轴之间的夹角的改变而变化,从而可以在实验上来确定单分子磁体的易磁化轴的相对取向。我们还发现偏压可以有效地调控隧穿各向异性磁阻值的大小和正负。此性质可以用来设计基于分子磁体的单铁磁电极的自旋阀器件。
最后,在铁磁金属/单分子磁体/正常金属的隧穿结的自旋注入研究中,我们发现可以产生远大于铁磁电极极化率的自旋流,并且在偏压的控制下,自旋流的方向和大小都可以改变。因此,基于单分子磁体,可以实现高效自旋注入和有效调控的自旋器件。
In molecular spintronics, single-molecule magnets (SMMs) possess high spins and uniaxial magnetic anisotropy with an easy axis, which have potential applications in information storage and processing, and electron transport through SMMs has received much attention. In both experimental and theoretical aspects, since the spin-exchange interaction between the tunneling electron and the molecule, many interesting properties have been found, such as Berry-phase blockade, the magnetization reversal of SMM, and thermoelectric effect induced pure spin-current. Spin-polarized transport is at the heart of spintronics, and thus in this thesis, within a rate-equation approach we focus on the spin-dependent transport through a SMM weakly coupled to magnetic electrodes.
First, we theoretically study the charge and spin currents through a SMM between ferromagnetic leads, where the magnetizations of two magnetic electrodes are collinear with the magnetic easy-axis of the SMM. In both sequential and cotunneling regimes, we systematically study the cases of ferromagnetic and antiferromagnetic coupling between a tunneling electron and the local molecular spin in the parallel and antiparallel lead magnetizations. We exhibit the charge and spin current, the differential conductance, and the current spin polarization as functions of bias voltage for all cases. An interesting observation is that the polarization reversal of spin-current can be realized and manipulated by the variation of bias voltage (but not inverting) in the case of antiferromagnetic exchange-coupling with antiparallel lead-configuration. The above effect may be useful in the development of spintronic devices, which can reverse the direction of spin current.
Secondly, we investigate the effects of intrinsic spin relaxation on the spin-dependent transport through a SMM with ferromagnetic leads in both the sequential and cotunneling regimes, and discuss mainly the effect on the tunneling magnetoresistance (TMR). It is shown that the TMR disappears almost under the fast spin-relaxation in the sequential regime while can vary from large positive to small negative values in the cotunneling regime. Moreover, when a magnetic field is applied along the easy-axis of SMM, a large negative TMR is obtained with the increase of the relaxation strength. Finally in the large-bias voltage limit, the TMR for the negative bias is slightly larger than its characteristic value in the sequential regime, but for the positive bias it becomes a negative value due to the fast spin-relaxation.
Then, we study electron transport through SMM junctions with one ferromagnetic lead and one normal-metal lead in the sequential regime, and find the typical tunneling anisotropic magnetoresistance (TAMR) effect, which varies with the angle between the magnetization direction of ferromagnetic lead and the easy-axis of SMM. The angular dependence of TAMR can serve as a probe to determine experimentally the easy-axis of SMM. Moreover, it is demonstrated that both the magnitude and sign of TAMR are tunable by the bias voltage, suggesting a new spin-valve device with only one magnetic electrode in molecular spintronics.
Finally, we present a proposal for a voltage-tunable SMM based spin current injector. The device consists of a SMM that is weakly coupled to one ferromagnetic electrode and one nonmagnetic electrode. We show that the current polarization can be dramatically enhanced. Moreover, the sign of spin-polarization can be changed by the gate or the bias voltage.
引文
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