Molecular crystallization of rubrene thin films assisted by gold nanoparticles

We demonstrate that crystalline organic rubrene thin films can be obtained by a facile spin-coating method using gold (Au) nanoparticles (NPs). Dodecanethiol-functionalized Au NPs were dissolved with rubrene molecules in solvent and a thin film of Au/rubrene was prepared by a simple spin coating process. The results of confocal photoluminescence (PL) and absorption spectral mapping confirmed the local formation of orthorhombic crystalline structures of the Au/rubrene hybrid film, in contrast to the monoclinic structure of plain rubrene films. Further, the results of transmission electron microscopy (TEM) and X-ray diffraction analysis, as well as Raman spectroscopy measurements of the rubrene and Au/rubrene films suggested the formation of high crystalline Au/rubrene film. The molecular crystallization of the Au/rubrene hybrid film is attributed to the nucleation effect of the Au NPs.     

Spontaneous spin polarization in rubrene studied by density functional theory calculations

We theoretically studied the spontaneous spin polarization properties of organic molecule rubrene by using density functional theory calculations. Our investigations show that normally nonmagnetic molecule rubrene could be spin polarized by spinless-hole injection. Magnetic moment of the molecule increases linearly with the extra hole charge amount only when the injected hole charges reach a certain value. The spin density resides predominantly on the carbon atoms in the tetracene backbone of rubrene molecule and also the bond lengths change differently due to the injected charge. Spontaneous spin polarization can be explained as the preferably filling of the spin-splitted carbon p_z orbitals near the Fermi energy for the injected charge.     

Morphology and crystallographic properties of rubrene thin films grown on muscovite(0 0 1)

Thin films of the organic semiconductor rubrene were deposited on muscovite (0 0 1) substrates by hot wall epitaxy. The morphology of rubrene thin films in combination with their crystallographic properties was characterized by transmission electron microscopy. The initial growth proceeds in a partially wetting regime where amorphous droplets are formed. Through diffusive interactions the droplets merge together in partially crystalline open networks. At a more advanced growth stage, spherulites are formed and a variety of crystalline morphologies appears. Platelet- and needle-like morphologies can be assigned to the orthorhombic phase of rubrene with the [3 0 1] and [1 1 0] zone axes, respectively.     

Electron transport in granular amorphous silicon dioxide films with ferromagnetic nanoparticles placed in a magnetic field

Electron transport in amorphous silicon dioxide films with embedded nanoparticles (Co, Nb, Ta) was studied. The mean number of localized states in the interparticle tunneling channel was derived from the temperature dependence of conductivity for various grain concentrations under the assumption of the electron transport being governed by resonance tunneling in a chain of localized states between grains. To confirm the assumption of the inelastic character of tunneling, the dependences of the magnetoresistance on grain concentration, temperature, and magnetic field were studied. Accepting the single-orbital model, where the intergrain tunneling magnetoresistance is determined by s-s tunneling, it was found that the existence of weakly split localized states in the tunneling channel results in a lack of magnetoresistance saturation in strong magnetic fields. The combined effect of a decrease in the s-s tunneling coefficient and of growth in the probability of inelastic electron spin scattering with increasing length of the chain of localized states between particles in which the electron is tunneling accounts for the characteristic temperature-concentration dependences of the magnetoresistance. The experimental observation of these features provides an argument for the electron transport in a-SiO₂(Co,Nb,Ta) structures being governed by inelastic resonance tunneling through intergrain localized states.     

In-crystal and surface charge transport of electric-field-induced carriers in organic single-crystal semiconductors

Gate-voltage dependence of carrier mobility is measured in high-performance field-effect transistors of rubrene single crystals by simultaneous detection of the longitudinal conductivity sigma(square) and Hall coefficient R(H). The Hall mobility mu(H) (identical with sigma(square)R(H)) reaches nearly 10 cm(2)/V s when relatively low-density carriers (<10(11) cm(-2)) distribute into the crystal. mu(H) rapidly decreases with higher-density carriers as they are essentially confined to the surface and are subjected to randomness of the amorphous gate insulators. The mechanism to realize high carrier mobility in the organic transistor devices involves intrinsic-semiconductor character of the high-purity organic crystals and diffusive bandlike carrier transport in the bulk.     

Anderson-Mott transition driven by spin disorder: spin glass transition and magnetotransport in amorphous GdSi

A zero temperature Anderson-Mott transition driven by spin disorder can be "tuned" by an applied magnetic field to achieve colossal magnetoconductance. Usually this is not possible since spin disorder by itself cannot localize a high density electron system. However, the presence of strong structural disorder can realize this situation, self-consistently generating a disordered magnetic ground state. We explore such a model, constructed to understand amorphous GdSi, and highlight the emergence of a spin glass phase, Anderson-Mott signatures in transport and tunneling spectra, and unusual magneto-optical conductivity. We solve a disordered strong coupling fermion-spin-lattice problem essentially exactly on finite systems and account for all the qualitative features observed in magnetism, transport, and the optical spectra in this system.     

Spin transport and relaxation in graphene

We review our recent work on spin injection, transport and relaxation in graphene. The spin injection and transport in single layer graphene (SLG) were investigated using nonlocal magnetoresistance (MR) measurements. Spin injection was performed using either transparent contacts (Co/SLG) or tunneling contacts (Co/MgO/SLG). With tunneling contacts, the nonlocal MR was increased by a factor of ∼1000 and the spin injection/detection efficiency was greatly enhanced from ∼1% (transparent contacts) to ∼30%. Spin relaxation was investigated on graphene spin valves using nonlocal Hanle measurements. For transparent contacts, the spin lifetime was in the range of 50-100 ps. The effects of surface chemical doping showed that for spin lifetimes in the order of 100 ps, charged impurity scattering (Au) was not the dominant mechanism for spin relaxation. While using tunneling contacts to suppress the contact-induced spin relaxation, we observed the spin lifetimes as long as 771 ps at room temperature, 1.2 ns at 4 K in SLG, and 6.2 ns at 20 K in bilayer graphene (BLG). Furthermore, contrasting spin relaxation behaviors were observed in SLG and BLG. We found that Elliot-Yafet spin relaxation dominated in SLG at low temperatures whereas Dyakonov-Perel spin relaxation dominated in BLG at low temperatures. Gate tunable spin transport was studied using the SLG property of gate tunable conductivity and incorporating different types of contacts (transparent and tunneling contacts). Consistent with theoretical predictions, the nonlocal MR was proportional to the SLG conductivity for transparent contacts and varied inversely with the SLG conductivity for tunneling contacts. Finally, bipolar spin transport in SLG was studied and an electron-hole asymmetry was observed for SLG spin valves with transparent contacts, in which nonlocal MR was roughly independent of DC bias current for electrons, but varied significantly with DC bias current for holes. These results are very important for the use of graphene for spin-based logic and information storage applications.     

高效率和色稳定性的双超薄发光层的黄光有机电致发光器件

主要对rubrene黄光发光材料制作0.1nm厚度的超薄发光层的有机电致发光器件作了研究,并配合BCP空穴阻挡层探讨了对器件效率和色坐标稳定性的影响。双超薄rubrene发光层配合BCP空穴阻挡层的有机电致发光器件的性能得到了很好的改善,外加电压6V时,器件电流效率为6.35cd.A-1;外加电压10V时,器件发光亮度达到了7068cd.m-2。另外,在较大的外加电压驱动范围内,器件的色坐标一直保持在(0.49,0.49)。增加的发光效率和良好的色坐标稳定性主要是取决于空穴与电子的注入与输运平衡以及激子在超薄rubrene发光层中稳定性的复合平衡。     

Room-temperature tunnel magnetoresistance and spin-polarized tunneling through an organic semiconductor barrier

Electron spin-polarized tunneling is observed through an ultrathin layer of the molecular organic semiconductor tris(8-hydroxyquinolinato)aluminum (Alq3). Significant tunnel magnetoresistance (TMR) was measured in a Co/Al2O3/Alq3/NiFe magnetic tunnel junction at room temperature, which increased when cooled to low temperatures. Tunneling characteristics, such as the current-voltage behavior and temperature and bias dependence of the TMR, show the good quality of the organic tunnel barrier. Spin polarization (P) of the tunnel current through the Alq3 layer, directly measured using superconducting Al as the spin detector, shows that minimizing formation of an interfacial dipole layer between the metal electrode and organic barrier significantly improves spin transport.     

自旋场效应晶体管中隧道磁阻的势垒相关反转效应

考虑自旋场效应晶体管中Rashba自旋轨道相互作用和自旋输运量子相干性,研究了势垒强度对自旋场效应晶体管的自旋相关量子输运的影响. 研究发现,势垒强度较低时,隧道结电导随Rashba自旋轨道相互作用强度的变化呈现明显的振荡现象,势垒强度较高时,电导表现出明显的势垒相关“电导开关”现象. 当势垒强度逐渐增强时,平行结构电导呈现出单调下降趋势,而反平行结构电导产生波动,这种波动导致该隧道磁阻也随势垒强度的变化表现出振荡现象,且在合适的准一维电子气厚度情况下隧道磁阻值可以产生正负反转,这个效应将会在基于自旋的电子器件信息的存储上获得应用. 关键词： 自旋场效应管 开关效应 量子相干 隧道磁阻     

掺杂型红色有机电致发光显示器件

全色显示是有机电致发光显示(OLED)器件发展的目标,而高性能红色发光器件一直是制约全彩色OLED器件实用化的瓶颈,也是目前有机电致发光显示研究的热点。制作了掺杂DCJTB和不同浓度的rubrene两种荧光染料的红色有机电致发光显示器件,以NPB和Alq₃分别作为空穴传输层和电子传输层,发现器件性能与只掺杂DCJTB的器件相比有明显提高,发光效率提高到2～3倍。通过Frster理论和能带理论分析了器件的能量转移机理,研究发现Frster能量转移不是掺杂器件能量转移的主要形式,载流子俘获机制才是器件效率提高的主要原因;rubrene的引入使得能量能够更有效地从Alq₃转移到DCJTB,从而显著地提高了器件的发光效率和性能。     

Organic single-quantum-well electroluminescent device

A new kind of single-quantum-well electroluminescent (EL) device consists of a hole transport N,N-Bis(3-methyphenyl)-N,N-diphenylbenzidine(TPD) layer, and electron transport 8-(quinolinolate)-aluminum(Alq) layer and a light emitting layer of Alq doped with 5,6,11,12-tetraphenylnaphthacene (rubrene) has been fabricated by the multisource-type high-vaccum organic molecular deposition. The dopant rubrene is as a potential well, and the undoped Alq layer is as a barrier layer. The EL spectra shows the spectral narrowing and the emission peak energy blue-shift, and the efficiency and luminance of the device have been significantly improved. The experimental phenomena is explained as the result of recombination of carriers from the quantized energy state.     

Optical properties of a novel yellow fluorescent dopant for use in organic LEDs

In this paper, the optical properties of a novel organic, 2,8-di(t-butyl)-5,11-di[4(t-butyl) phenyl]-6,12-diphenylnaphthacene (tetra(t-butyl)rubrene) have been investigated. Our results show that there are two peaks in the photoluminescence (PL) spectra of tetra(t-butyl)rubrene (TBRb) which are also confirmed in the electroluminescence (EL) spectra. Photo-quenching of the PL intensity is observed when the irradiation time increases. It is shown that oxidation is the dominant reason for photo-quenching. The absolute refractive index and absorption coefficient have also been determined and the results correlate well with the PL results. The results show that TBRb can be a good dopant to achieve the Förster energy transfer and to assist light emission. The optical properties of TBRb are similar to those of rubrene; however, the PL of TBRb is much stronger than that of rubrene. Finally, although crystalline organics have been commonly reported by heating the sample, we report crystallization of TBRb at low temperature <230 K when the TBRb film is in an amorphous form before cooling. PACS 78.47.+p; 78.55.-m; 81.05.Lg; 85.60.-q     

Berry-phase blockade in single-molecule magnets

We formulate the problem of electron transport through a single-molecule magnet (SMM) in the Coulomb blockade regime taking into account topological interference effects for the tunneling of the large spin of a SMM. The interference originates from spin Berry phases associated with different tunneling paths. We show that, in the case of incoherent spin states, it is essential to place the SMM between oppositely spin-polarized source and drain leads in order to detect the spin tunneling in the stationary current, which exhibits topological zeros as a function of the transverse magnetic field.     

Voltage-controlled spin selection in a magnetic resonant tunneling diode

We have fabricated all II-VI semiconductor resonant tunneling diodes based on the (Zn,Mn,Be)Se material system, containing dilute magnetic material in the quantum well, and studied their current-voltage characteristics. When subjected to an external magnetic field the resulting spin splitting of the levels in the quantum well leads to a splitting of the transmission resonance into two separate peaks. This is interpreted as evidence of tunneling transport through spin polarized levels, and could be the first step towards a voltage controlled spin filter.     

Competition between quantum spin tunneling and Kondo effect

Quantum spin tunneling and Kondo effect are two very different quantum phenomena that produce the same effect on quantized spins, namely, the quenching of their magnetization. However, the nature of this quenching is very different so that quantum spin tunneling and Kondo effect compete with each other. Importantly, both quantum spin tunneling and Kondo effect produce very characteristic features in the spectral function that can be measured by means of single spin scanning tunneling spectroscopy and allows to probe the crossover from one regime to the other. We model this crossover, and the resulting changes in transport, using a non-perturbative treatment of a generalized Anderson model including magnetic anisotropy that leads to quantum spin tunneling. We predict that, at zero magnetic field, integer spins can feature a split-Kondo peak driven by quantum spin tunneling.     

Mobility-independent doping in crystalline rubrene field-effect transistors

We report doping effects in an organic semiconductor, crystalline rubrene. Oxygen-related states are introduced (removed) by annealing in oxygen (vacuum), at an elevated temperature. Room temperature stability is found in the resulting effects: (1) about two orders of magnitude increase in carrier density at equilibrium, (2) significant modification of threshold voltages, and (3) an unchanged field-effect mobility in the on-current state. Density of states data are modeled as tunneling from the valence band in the channel region into deep-level acceptors in the adjacent region. These oxygen acceptors are the likely dopant species.     

Spin tunneling in junctions with disordered ferromagnets

We provide compelling evidence to establish that, contrary to one's elementary guess, the tunneling spin polarization (TSP) of amorphous CoFeB is larger than that of fcc CoFeB. First-principles atomic and electronic structure calculations reveal striking agreement between the measured TSP and the predicted s-electron spin polarization. Given the disordered structure of the ternary alloy, not only do these results strongly endorse our communal understanding of tunneling through AlO(x), but they also portray the key concepts that demand primary consideration in such complex systems.     

Tunneling spin injection into single layer graphene

We achieve tunneling spin injection from Co into single layer graphene (SLG) using TiO? seeded MgO barriers. A nonlocal magnetoresistance (ΔR(NL)) of 130 Ω is observed at room temperature, which is the largest value observed in any material. Investigating ΔR(NL) vs SLG conductivity from the transparent to the tunneling contact regimes demonstrates the contrasting behaviors predicted by the drift-diffusion theory of spin transport. Furthermore, tunnel barriers reduce the contact-induced spin relaxation and are therefore important for future investigations of spin relaxation in graphene.     

Interface resistance dependence of spin transport in a ferromagnet–semiconductor hybrid structure

The spin transport signals from NiFe and Co into two-dimensional electron gas layers are measured for various thicknesses of transmission barriers. A stable and reproducible electrical detection of spin transport was obtained only when the barrier thickness is less than 10 nm. The typical interface resistance to observe spin signals in this experiment is about 0.5–250 Ω, which is a neither transparent nor a severe tunneling limit. The optimal interface resistance depends on the ferromagnetic materials, but severe tunneling barrier is not proper for fully electrical spin transport. Device size is also a critical factor to decide the proper range of interface resistance.