基于散射实验极化靶的2.5T/1.3K的动态核极化(DNP)系统的开发

动态核极化法(Dynamic Nuclear Polarization,DNP)是利用热平衡下的电子在磁场中的高自旋极化率转移到原子核自旋的技术,从而极大的提高原子核自旋极化率.多种动态极化靶材料已广泛的用于自旋物理散射实验.本文介绍一种简单实用,共同开发的日本山形大学DNP系统,包括超导磁场,氦4蒸发恒冷器,微波系统以及NMR核磁共振检测系统,测得中子靶材料氘带丁醇(D-butanol)中氘核的极化率在2.5 T/1.3 K达到+6.5%.     

自旋相关的电子隧穿和自旋极化

研究了电子的自旋相关的隧穿和极化。在外加磁场的作用下，自旋向上的电子与自旋向下的电子具有不同的隧穿系数。当电子的自旋方向与磁场方向相反时，其隧穿概率受到磁场的抑制而变小；反之，当两平行时，电子的了隧穿系数增大。这种差异可以用本中定义的自旋极化率来表示。本对不同磁场下的自旋极化率进行了计算，结果也表明当电子的动能较小，这种自旋极化的效应越显。     

一种可用于极化~3He实验的新型磁场系统

原子核自旋极化的~3He气体已被深入研究并广泛用于各种科学实验.在过去的极化~3He实验中,为了减小磁场梯度对纵向弛豫时间的影响,通常会建造大尺寸的亥姆霍兹线圈来提供所需均匀度的主磁场环境.本文通过计算得到了新的六正方形线圈系统,可以为极化~3He实验提供小型高均匀性的磁场装置.其中线圈系√统内部超过30%的区域磁场梯度满足(|▽B_x|~2+|▽B_y|~2)/B_0 10~(-4)cm~(-1),这一均匀区域比例超过了现在所有用于极化~3He实验的线圈装置.对于其他需要大均匀区域磁场环境的研究实验,新的六线圈系统也具有很好的应用价值.     

装置极化效率对极化中子成像质量的影响及修正分析

极化中子照相技术通过分析极化中子束的自旋相移对样品磁场进行成像, 自旋极化/分析装置是照相系统的主要组成部分. 引入中子自旋极化/分析装置的极化效率参数, 从中子极化矢量与磁场相互作用机理出发, 重新推导探测中子强度与磁场分布的定量关系, 利用谱仪模拟软件VITESS, 选取bender型超镜极化器和 ³He 自旋过滤器作为极化/分析装置, 对量化修正式进行验证, 并综合装置极化效率、单色器能量分辨精度和bender型极化器的几何结构等参数, 初步分析极化中子照相技术的磁场定量检测能力, 相关结果可为极化中子照相的实验数据处理技术研究及装置设计提供参考. 关键词： 极化效率 中子照相 磁场成像     

极化子比率变化对自旋注入有机半导体性质的影响

从自旋扩散方程和欧姆定律出发研究了铁磁层到有机半导体的自旋注入,得到了系统的电流自旋极化率。有机半导体中的载流子为自旋极化子和不带自旋的双极化子,极化子比率在有机半导体内随输运距离变化。通过计算发现匹配的铁磁和有机半导体电导率有利于自旋注入;通过调节界面电阻自旋相关性,电流自旋极化率可获得很大程度提高;极化子比率衰减速率对有机半导体电流自旋极化率具有非常重要的影响。     

极化子和双极化子在齐聚物中的稳定性

导电聚合物中的元激发稳定性问题对于认识和理解有机材料中的自旋极化输运现象是极其重要的.针对目前存在的极化子与双极化子之间的争论,本文从半经验的Austin Model 1(AM1)方法出发,对齐分子噻吩的掺杂态进行了研究.通过对极化子和双极化子体系能量的比较,发现双极化子可以转换为极化子,从而揭示出在有机半导体材料中可以实现自旋极化输运.     

伴随强光子辐射的自旋极化等离子体研究进展

强光子辐射导致的自旋极化等离子体是强激光与物质相互作用领域兴起的新研究方向。基于等离子体的自旋极化粒子束在固态材料诊断、原子核结构探测、弱电相互作用分析等方面具有广泛应用。同时,自旋作为电子的固有属性,它可为描述等离子体的行为状态提供新的信息自由度,因此自旋极化信号在强场等离子体自诊断也具有潜在应用。概述了在超强相对论等离子体中,由伽马光子辐射伴随的自旋翻转产生的自旋极化等离子体的物理机制,并对其在超高能量密度等离子体瞬态动力学反演的可能进行了介绍。     

激光极化129Xe的生物磁共振成像研究进展

激光光抽运自旋交换方法能够极大地增强＾１２９Ｘｅ核自旋极化,其获得的非平衡极化度远远高于在相同磁场里玻尔兹曼平衡值。     

含stubs量子波导系统的电子自旋极化输运性质

理论上研究了含stubs的Rashba自旋轨道耦合（spin-orbit coupling, SOC）量子波导系统的自旋极化输运性质. 利用晶格格林函数方法,发现由于stubs和SOC产生的势阱使系统中出现束缚态,这些束缚态与传播态之间相互干涉导致电导中出现Fano共振结构,同时在对应的自旋极化率中也出现Fano共振或反共振结构. 此外,由于系统结构的突变使电子被反向散射和量子干涉效应,电导中出现一系列的共振峰. 但是,当系统加上外磁场后,所有这些效应都被抑制, 系统重新出现量子化电导, 同时自旋电导也出 关键词： 量子波导 自旋极化输运 自旋轨道耦合     

动态核极化谱仪的技术改造

介绍了动态核极化(DNP)谱仪数字系统的改造和一套的射频发射和接收系统的建立.谱仪射频通道的90°脉冲宽度为5μs,能完全满足固体交叉极化和大功率去耦的实验要求.实现了DNP增强曲线的自动测量     

The theory of nuclear orientation via electron spin locking (NOVEL)

Nuclear orientation via electron spin locking (NOVEL) is a technique to orient nuclear spins embedded in a solid. Like other methods of dynamic nuclear polarization (DNP) it employs a small amount of unpaired electron spins and uses a microwave field to transfer the polarization of these unpaired electron spins to the nuclear spins. Traditional DNP uses CW microwave fields, but NOVEL uses pulsed electron spin resonance (ESR) techniques: a 90 degree pulse–90 degree phase shift–locking pulse sequence is applied and during the locking pulse the polarization transfer is assured by satisfying the Hartmann–Hahn condition. The transfer is coherent and similar to coherence transfer between nuclear spins. However, NOVEL requires an extension of the existing theory to many, inequivalent nuclear spins and to arbitrary, i.e. high electron and nuclear spin polarization. In this paper both extensions are presented. The theory is applied to the system naphthalene doped with pentacene, where the proton spins are polarized using the photo-excited triplet states of the pentacene molecules and found to show excellent agreement with the experimentally observed evolution of the polarization transfer during the locking pulse.     

Polarizing agents and mechanisms for high-field dynamic nuclear polarization of frozen dielectric solids

This article provides an overview of polarizing mechanisms involved in high-frequency dynamic nuclear polarization (DNP) of frozen biological samples at temperatures maintained using liquid nitrogen, compatible with contemporary magic-angle spinning (MAS) nuclear magnetic resonance (NMR). Typical DNP experiments require unpaired electrons that are usually exogenous in samples via paramagnetic doping with polarizing agents. Thus, the resulting nuclear polarization mechanism depends on the electron and nuclear spin interactions induced by the paramagnetic species. The Overhauser Effect (OE) DNP, which relies on time-dependent spin–spin interactions, is excluded from our discussion due the lack of conducting electrons in frozen aqueous solutions containing biological entities. DNP of particular interest to us relies primarily on time-independent, spin-spin interactions for significant electron–nucleus polarization transfer through mechanisms such as the Solid Effect (SE), the Cross Effect (CE) or Thermal Mixing (TM), involving one, two or multiple electron spins, respectively. Derived from monomeric radicals initially used in high-field DNP experiments, bi- or multiple-radical polarizing agents facilitate CE/TM to generate significant NMR signal enhancements in dielectric solids at low temperatures (<100 K). For example, large DNP enhancements (∼300 times at 5 T) from a biologically compatible biradical, 1-(TEMPO-4-oxy)-3-(TEMPO-4-amino)propan-2-ol (TOTAPOL), have enabled high-resolution MAS NMR in sample systems existing in submicron domains or embedded in larger biomolecular complexes. The scope of this review is focused on recently developed DNP polarizing agents for high-field applications and leads up to future developments per the CE DNP mechanism. Because DNP experiments are feasible with a solid-state microwave source when performed at <20 K, nuclear polarization using lower microwave power (<100 mW) is possible by forcing a high proportion of biradicals to fulfill the frequency matching condition of CE (two EPR frequencies separated by the NMR frequency) using the strategies involving hetero-radical moieties and/or molecular alignment. In addition, the combination of an excited triplet and a stable radical might provide alternative DNP mechanisms without the microwave requirement.     

Dynamic Nuclear Polarization in III–V Semiconductors

We report on electron spin resonance, nuclear magnetic resonance and Overhauser shift experiments on two of the most commonly used III–V semiconductors, GaAs and InP. Localized electron centers in these semiconductors have extended wavefunctions and exhibit strong electron–nuclear hyperfine coupling with the nuclei in their vicinity. These interactions not only play a critical role in electron and nuclear spin relaxation mechanisms, but also result in transfer of spin polarization from the electron spin system to the nuclear spin system. This transfer of polarization, known as dynamic nuclear polarization (DNP), may result in an enhancement of the nuclear spin polarization by several orders of magnitude under suitable conditions. We determine the critical range of doping concentration and temperature conducive to DNP effects by studying these semiconductors with varying doping concentration in a wide temperature range. We show that the electron spin system in undoped InP exhibits electric current-induced spin polarization. This is consistent with model predictions in zinc-blende semiconductors with strong spin–orbit effects.     

Polarization enhancement technique for nuclear quadrupole resonance detection

We demonstrate a dramatic increase in the signal-to-noise ratio (SNR) of a nuclear quadrupole resonance (NQR) signal by using a polarization enhancement technique. By first applying a static magnetic field to pre-polarize one spin subsystem of a material, and then allowing that net polarization to be transferred to the quadrupole subsystem, we increased the SNR of a sample of ammonium nitrate by one-order of magnitude.     

~(129)Xe核自旋极化转移增强分子的核磁共振信号

激光极化的12 9Xe核具有极高的非平衡极化度和长的弛豫时间 ,这一特点使得它能够极化转移增强液体、固体或者固体表面分子中原子核自旋极化。因而 ,提高了它们的核磁共振探测灵敏度和扩展了在材料和表面科学研究中的应用。综述激光极化12 9Xe核与其它分子中原子核之间的极化转移研究与进展 ,介绍相关物理机制和参数的测量。     

Theoretical aspects of dynamic nuclear polarization in the solid state - the solid effect

Dynamic nuclear polarization has gained high popularity in recent years, due to advances in the experimental aspects of this methodology for increasing the NMR and MRI signals of relevant chemical and biological compounds. The DNP mechanism relies on the microwave (MW) irradiation induced polarization transfer from unpaired electrons to the nuclei in a sample. In this publication we present nuclear polarization enhancements of model systems in the solid state at high magnetic fields. These results were obtained by numerical calculations based on the spin density operator formalism. Here we restrict ourselves to samples with low electron concentrations, where the dipolar electron-electron interactions can be ignored. Thus the DNP enhancement of the polarizations of the nuclei close to the electrons is described by the Solid Effect mechanism. Our numerical results demonstrate the dependence of the polarization enhancement on the MW irradiation power and frequency, the hyperfine and nuclear dipole-dipole spin interactions, and the relaxation parameters of the system. The largest spin system considered in this study contains one electron and eight nuclei. In particular, we discuss the influence of the nuclear concentration and relaxation on the polarization of the core nuclei, which are coupled to an electron, and are responsible for the transfer of polarization to the bulk nuclei in the sample via spin diffusion.     

Overhauser dynamic nuclear polarization and molecular dynamics simulations using pyrroline and piperidine ring nitroxide radicals

The efficiency of Overhauser dynamic nuclear polarization (DNP) depends on the local dynamics modulating the dipolar coupling between the two interacting spins. By attaching nitroxide based spin labels to molecules and by measuring the ¹H DNP response of solvent water, information about the local hydration dynamics near the spin label can be obtained. However, there are two commonly used types of nitroxide ring structures; a pyrroline based and a piperidine based molecule. It is important to know when comparing different experiments, whether changes in DNP enhancements are due to changes in local hydration dynamics or because of the different spin label structures. In this study we investigate the key parameters affecting DNP signal enhancements for 3-carbamoyl-2,2,5,5-tetramethyl-3-pyrrolin-1-oxyl, a 5-membered ring nitroxide radical, and for 4-oxo-2,2,6,6-tetramethyl-1-piperidinyloxy, a 6-membered ring nitroxide radical. Using X-Band DNP, field cycling relaxometry, and molecular dynamics simulations, we conclude that the key parameters affecting the DNP amplitude of the ¹H signal of water to be equal when using either nitroxide. Thus, experiments measuring hydration dynamics using either type of spin labels may be compared.     

Observation of hysteretic transport due to dynamic nuclear spin polarization in a GaAs lateral double quantum dot

We report a new transport feature in a GaAs lateral double quantum dot that emerges for magnetic-field sweeps and shows hysteresis due to dynamic nuclear spin polarization (DNP). This DNP signal appears in the Coulomb blockade regime by virtue of the finite interdot tunnel coupling and originates from the crossing between ground levels of the spin triplet and singlet extensively used for nuclear spin manipulations in pulsed-gate experiments. The magnetic-field dependence of the current level is suggestive of unbalanced DNP between the two dots, which opens up the possibility of controlling electron and nuclear spin states via dc transport.     

DNP-EPR多功能谱仪中微波桥的设计与实现

在自主研制的动态核极化（Dynamic Nuclear Polarization,DNP）分子影像装置的基础上,提出了一种集DNP和电子顺磁共振（Electron Paramagnetic Resonance,EPR）于一体的多功能谱仪,并对其中的关键部件之一--微波桥进行了设计.微波桥的引入,实现了DNP微波发射机的集成化,以及在DNP谱仪基础上的EPR功能扩展.通过结构设计、电路仿真及系统测试,完成了高频谱纯度、高动态范围的微波发射机以及低噪声系数的微波检测系统的设计与制作.并通过DNP增强实验以及连续波EPR实验对微波桥的性能进行了验证.