Research of spinterface in organic spintronic devices

Li Jing; Ding Shuai-Shuai; Hu Wen-Ping

doi:10.7498/aps.71.20211786

Abstract

Spintronics are attractive to the utilization in next-generation quantum-computing and memory. Compared with inorganic spintronics, organic spintronics not only controls the spin degree-of-freedom but also possesses advantages such as chemical tailorability, flexibility, and low-cost fabrication process. Besides, the organic spin valve with a sandwich configuration that is composed of two ferromagnetic electrodes and an organic space layer is one of the classical devices in organic spintronics. Greatly enhanced or inversed magnetoresistance (MR) sign appearing in organic spin valve is induced by the unique interfacial effect an organic semiconductor/ferromagnetic interface. The significant enhancement or inversion of MR is later proved to be caused by the spin-dependent hybridization between molecular and ferromagnetic interface, i.e., the spinterface. The hybridization is ascribed to spin-dependent broadening and shifting of molecular orbitals. The spinterface takes place at one molecular layer when attaching to the surface of ferromagnetic metal. It indicates that the MR response can be modulated artificially in a specific device by converting the nature of spinterface. Despite lots of researches aiming at exploring the mechanism of spinterface, several questions need urgently to be resolved. For instance, the spin polarization, which is difficult to identify and observe with the surface sensitive technique and the inversion or enhancement of MR signal, which is also hard to explain accurately. The solid evidence of spinterface existing in real spintronic device also needs to be further testified. Besides, the precise manipulation of the MR sign by changing the nature of spinterface is quite difficult. According to the above background, this review summarizes the advance in spinterface and prospects future controllable utilization of spinterface. In Section 2, we introduce the basic principle of spintronic device and spinterface. The formation of unique spinterface in organic spin valve is clarified by using the difference in energy level alignment between inorganic and organic materials. Enhancement and inversion of MR sign are related to the broadening and shifting of the molecular level. In Section 3, several examples about identification of spinterface are listed, containing characterization by surface sensitive techniques and identification in real working devices. In Section 4 some methods about the manipulation of spinterface are exhibited, including modulation of ferroelectric organic barrier, interface engineering, regulation of electronic phase separation in ferromagnetic electrodes, etc. Finally, in this review some unresolved questions in spintronics are given, such as multi-functional and room-temperature organic spin valve and improvement of the spin injection efficiency. Spinterface is of great importance for both scientific research and future industrial interest in organic spintronics. The present study paves the way for the further development of novel excellent organic spin valves.

Keywords:

Authors and contacts

1.
Tianjin Key Laboratory of Molecular Optoelectronic Sciences, School of Science, Tianjin University, Tianjin 300072, China
2.
Joint School in Fuzhou, Tianjin University, Fuzhou 350207, China

Corresponding author: Ding Shuai-Shuai, dingshuaishuai@tju.edu.cn ; Hu Wen-Ping, huwp@tju.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 52003190, 21875158, 91833306, 51633006, 51733004) and the National Key R&D Program of China (Grant No. 2017YFA0204503).

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Cited By

图 1 (a)有机自旋阀器件示意图; (b)有机自旋阀器件中随着施加磁场变化的理想磁电阻曲线

Figure 1. (a) Schematic of organic spin valve device; (b) ideal MR curve when sweeping the applied magnetic field on organic spin valve devices.

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图 2 (a)和(b)磁性隧道结中铁磁电极在平行和反平行磁化状态的结构示意图; (c)和(d)在平行和反平行磁化状态下铁磁层的能带结构; (e)和(f)在磁化方向平行和反平行状态下的双电阻网络模型^[54]

Figure 2. (a) and (b) Schematics shows different states of ferromagnetic electrode with parallel and antiparallel magnetization in MTJ; (c) and (d) band structure of ferromagnetic layer for parallel and antiparallel magnetization; (e) and (f) two-resistor network model for magnetization of parallel and antiparallel alignment^[54].

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图 3 无机材料和有机物材料分子的能级结构示意图, 以及无机和有机材料在接近铁磁电极后能级发生的不同变化的示意图^[46]

Figure 3. Schematic diagram of the band structure of inorganic materials and organic materials, and the schematic diagram of the energy difference between inorganic and organic molecule closed to a ferromagnetic electrode^[46].

DownLoad: Full-Size Img PowerPoint

图 4 自旋界面的示意图　(a)无机物和铁磁电极接触界面的导带和价带示意图; (b)自旋界面处当$\varGamma \gg \Delta E$时会诱导自旋极化的反转; (c)$\varGamma \ll \Delta E$时会造成自旋极化增强^[46]

Figure 4. Schematics of spinterface^[46]: (a) Schematics of conduction and valence band structure at inorganic/FM interface; (b) inversed spin-polarization case of $\varGamma \gg \Delta E$ at the spinterface; (c) enhanced spin-polarization case of $\varGamma \ll \Delta E$ at the interface^[46].

DownLoad: Full-Size Img PowerPoint

图 5 (a) H₂Pc吸附在Fe上的SP-STM图^[64]; (b) 两个吸附在Cr (001)表面的C₆₀分子上的电导图^[65]; 吸附于Co基底上不同厚度TNAP的UPS图, 其中(c)—(e)分别对应(c)二次电子截止边、(d)价带边、(e)价带的细节谱图; (f)在Co上TNAP吸附前后Co的L边XMCD图; (g) 单层和多层TNAP在Co上N元素的K边NEXAFS图^[66]

Figure 5. (a) SP-STM image of H₂Pc absorbed on Fe^[64]. (b) conductance maps measured over two C₆₀ molecules absorbed on Cr (001) surface^[65]. UPS spectra of TNAP with different thickness deposited on Co substrate: (c) Secondary electron cutoff; (d) valence band; (e) detail spectral features of valence band. (f) Co L-edge XMCD results before and after adsorption of TNAP on Co; (g) NEXAFS N K-edge spectra of monolayer and multilayer TNAP on Co^[66].

DownLoad: Full-Size Img PowerPoint

图 6 (a) AlO_x绝缘层对Co渗透的阻挡作用及渗透的Co和P3HT间形成自旋界面的示意图; (b) LSMO/P3HT/AlO_x/Co器件中自旋依赖电子隧穿过程示意图^[48]

Figure 6. (a) Schematic drawing of blocking effect for the insulated AlO_x to penetrated Co, and the formation of spinterface between penetrated Co and P3HT molecular; (b) schematics of spin-dependent electron tunneling in LSMO/P3HT/AlO_x/Co junction^[48].

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图 7 (a)和(b)分别为器件A和器件B的磁输运测试; (c)无LiF层、具有反铁磁双氟层和LiF沉积在氧化铝上的器件结构以及对应的磁电阻信号示意图^[49]

Figure 7. (a) and (b) Magnetotransport measurements of device A and device B, respectively; (c) schematics of devices with no LiF layer, an anti-ferromagnetic difluoride layer and LiF deposited on an alumina and their respective MR curves ^[49].

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图 8 (a) Fe₃O₄/P3HT/Co有机自旋阀器件示意图; (b) 不同电流下Fe₃O₄/P3HT/Co有机自旋阀器件和Fe₃O₄电极MR值与温度的关系; (c) 不同温度下孪晶界对自旋注入调制过程的模型图^[70]

Figure 8. (a) Schematic of organic spin valve device of Fe₃O₄/P3HT/Co; (b) relationship between MR ratio and temperature for Fe₃O₄/P3HT/Co OSV device and Fe₃O₄ electrode at different bias current; (c) model of twin boundary-modulated spin injection at different temperature^[70].

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图 9 (a) LSMO/PVDF/Co器件示意图; (b)在PVDF表面测得的PFM相图; (c) 极化后器件所测得的隧穿磁电阻信号; (d)在10 mV, 10 K条件下测得LSMO/PVDF/Co器件的隧穿磁电阻; (e)在10 mV, 10 K条件下测得LSMO/PVDF/MgO/Co器件的隧穿磁电阻^[51]

Figure 9. (a) Schematic of LSMO/PVDF/Co device; (b) PFM phase image measured on the PVDF surface; (c) tunneling magnetoresistance measured after polarizing the device; (d) tunneling magneto resistance of a LSMO/PVDF/Co device measured under 10 mV at 10 K; (e) tunneling magneto resistance of a LSMO/PVDF/MgO/Co device measured under 10 mV at 10 K^[51].

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图 10 (a) Au/Co/Alq₃/PZT/LSMO有机自旋阀的器件示意图; (b)和(c)施加不同预设电压后MR的偏移; (d)当PZT的电极化向上和向下时器件的能级关系示意图^[71]

Figure 10. (a) Schematic of a Au/Co/Alq₃/PZT/LSMO organic spin valve device; (b) and (c) MR shift after applying different ramping voltage; (d) the energy relationship schematic of device when the electric polarization of the PZT is “up” and “down”^[71].

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图 11 在LPCMO有机自旋阀中(a) FMM和COI相共存和(b)全FE相时的EPS调制自旋注入示意图; (c)在LPCMO有机自旋阀中不同预设磁场强度下的MR信号^[72]

Figure 11. Illustration of EPS-modulated spin current injection in the LPCMO-OSVs under the co-existed FM/COI phase (a) and fully FM phase (b) of the LPCMO thin film; (c) MR loops of the LPCMO-OSV device under different pre-set magnetic field strength^[72].

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图 12 (a) ZMP分子化学吸附于Co电极的示意图^[4]; (b) 单铁磁电极器件所测得的磁电阻信号^[4]

Figure 12. (a) Schematic of ZMP molecular chemisorbed on Co ferromagnetic electrode^[4]; (b) magnetoresistance of device with a single ferromagnetic^[4].

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