B、N掺杂4-ZGNR电子输运性质的理论计算

运用密度泛函理论结合非平衡格林函数的方法,对锯齿型石墨烯纳米带4-ZGNR掺杂B、N原子的电子输运进行了计算.结果得到在0～1.0V的电压范围内,4-ZGNR及其分别掺杂B、N原子3种纳米器件的电流-电压曲线具有明显的非线性关系;掺杂B、N对4-ZGNR费米能级附近电子的输运起到了一定抑制作用,在一定能量区域的电子存在完全共振背散射;4-ZGNR掺杂B原子后表现出负微分电阻现象.     

分子间距及洞位占据对碳双原子链电子输运性质的影响

模拟了两条平行碳原子链通过硫原子连接在一对半无限大的金电极(111)面之间组成的双分子器件的电子输运特性。计算结果表明,当原子链间距比较小时,原子链之间的距离是决定双分子器件电子输运性质的关键因素。随着原子链的间距增大到一定数值时,硫原子在金电极上的洞位占据类型在整个双分子结系统的电子输运过程中起决定作用。     

中心掺杂对CNT—C60—CNT分子结电子输运性质影响的第一性原理研究

用第一性原理计算方法研究了在C60中心掺入Si、Li、Au等单原子后对CNT-C60-CNT分子结电子输运性质的影响,包括掺杂前后各体系在不同接触距离下输运性质的变化．计算结果表明：在C60中心,Li原子的存在显著增大了其平衡电导,而Si,Au等原子对体系电子输运性质的影响比较复杂．最后,研究并比较了各体系在非平衡态下的I-V特性．     

中心掺杂对CNT-C_(60)-CNT分子结电子输运性质影响的第一性原理研究

用第一性原理计算方法研究了在C60中心掺入Si、Li、Au等单原子后对CNT-C60-CNT分子结电子输运性质的影响,包括掺杂前后各体系在不同接触距离下输运性质的变化.计算结果表明:在C60中心,Li原子的存在显著增大了其平衡电导,而Si,Au等原子对体系电子输运性质的影响比较复杂.最后,研究并比较了各体系在非平衡态下的I-V特性.     

PdFe(110)电子结构及电催化性能的理论研究

利用密度泛函理论(DFT)的平面波赝势方法计算了不同注入电荷和掺杂Fe原子比例的PdxFey(110)表面原子结构和电子结构特性。结果表明,Fe原子比例对表面褶皱s影响较小,注入电荷数量对表面褶皱s影响很大;Fe原子掺杂使Pd的4d10轨道电子向低能级轨道移动,增加了d空穴。布居分析表明电极的表层电荷分布比金属态表面增多;Fe掺杂的表层电荷分布比不掺杂电极表面增多。电子结构分析表明,电极表面的s、p、d轨道电子和总电子均比金属态表面减少;Fe掺杂后,Pd和Fe的表面原子趋向于杂化构型,Pd表层原子向Fe表层原子发生电子转移,增加表面反应活性,有利于电催化反应。     

La_(1-x)Ca_xMnO_3的电子结构与磁有序研究

采用DV-Xa分子轨道法计算了不同掺杂浓度的立方结构钙钛矿La_(1-x)Ca_xMnO_3体系的电子结构,分析了体系磁电特性随钙浓度变化的特征.结果表明:自旋相关的锰3d—氧2p轨道杂化出现在整个体系中.未掺杂体系具有金属型导电性,费米能级处多数自旋子带的态密度高于少数子带.随着掺杂浓度的提高,体系发生金属-半金属相变.与此同时,锰离子磁矩单调降低,与3d带自旋交换劈裂的变化规律一致.掺杂的钙提高了锰3d和氧2p电子波函数的交迭,加强了Mn-O-Mn超交换作用,使CaMnO3呈现G型反铁磁态.LaMnO_3中锰3d和氧2p波函数的交迭最弱,呈铁磁有序.     

La2/3Sr1/3Mn1-xCoxO3(x=0,0.2,0.25)体系的热膨胀和电性能研究

制备了钙钛矿锰氧化物La2/3Sr1/3Mn1-xCoxO3(x=0,0.2,0,25)体系,研究该材料的热膨胀性能和电输运性质.研究发现,所有样品具有相近的热膨胀性能,200-800 ℃温区内的平均线热膨胀系数约为1.2×10-5K-1;x=0和x=0.2掺杂样品在高温下的电输运机制符合小极化子模型;x=0.25掺杂样品具有最高的电导率,在800℃时的电导率为100S/cm.     

金属Fe、Y单掺杂TaON的电子结构和光学性质研究

采用基于密度泛函理论的从头算平面波超软赝势方法,研究金属Fe、Y单掺杂对斜锆石相TaON电子结构和光学性质的影响.研究结果表明,掺杂后TaON电子结构和光学性质的变化主要源于杂质原子d态电子的贡献.Fe、Y掺杂均在禁带中引入了新的杂质能级,并使费米能级处的态密度值有所增加,带隙宽度有所减小,从而导致吸收光谱的吸收边沿发生明显的红移,说明Fe、Y掺杂对于提高TaON的可见光催化性能和电输运性能起到很好的促进作用.两相比较,就提高光催化性能和电输运性能来说,Fe掺杂的效果优于Y掺杂.     

硅烯电极材料的第一性原理计算

用第一性原理计算硅烯在N和S原子共掺杂时的能带及电子态密度, 并研究硅烯量子电容与不同掺杂构型间的关系. 结果表明: 引入N/S和N/B共掺杂原子可导致Fermi能级处产生局域态; 在-0.6~0.6 V内, 用NSS,NS,NBB,NNB和NB掺杂硅烯的量子电容均增加, 其中NSS掺杂单空位硅烯在Fermi能级附近, 其量子电容为43.9 μF/cm2, 量子电容增加明显.     

化学改性二氧化锰结构表征

应用扩展X射线精细结构（EXAFS）技术及光电子能谱研究改性MnO2的结构,结果表明：掺杂原子进入了MnO2晶格中,锰的第一壳层配位数下降,并且增大高壳层配位原子的无序度。     

耦合于铁磁电极平行双量子点的自旋极化输运

利用双杂质的Anderson模型的哈密顿量,从理论上研究了耦合于铁磁电极的平行双量子点的自旋极化输运性质,并借助运动方程方法求解了哈密顿量.结果表明,该系统在费米能级处的Kondo共振峰与自旋极化强度和磁通量的取值有关.与此同时,在平行组态情况下,Kondo共振峰位置发生了偏移,而在反平行组态情况下,Kondo共振峰出现在相同位置处.这些现象使得这一双量子点系统的物理特性更加丰富,它们将有助于解释自旋电子学中的电子关联问题.     

量子点Kondo单态相移测量退相干效应

对于QPC实验中量子点Kondo单态的退相干强度,实验测量比理论预测大30倍的谜团至今尚未解决。本文利用格林函数方法,计算了QPC实验装置中量子点的输运特性,计算结果表明相移测量有可能是该谜团的原因之一。     

Kondo effect in quantum dots and molecular devices

Kondo effect is a very important many-body phenomenon in condensed mailer physics, which explains why the resistance increases as the temperature is lowered （usually 〈10 K） in dilute magnetic alloy, and why the conductance increases as temperature is decreased in quantum dots. This paper simply introduces equilihrium and nonequilibrium Kondo effects in quantum dots together with the Kondo effect in quantum dots with even number of electrons （when the singlet and triplet states are degenerate）. Furthermore, Kondn effect in single aton/molecular transistorss is introduced, which indicates a new way in study Kondo effect.     

Mn掺杂ZnSe量子点的无膦合成及稳定性研究

以十八烯溶解硒粉为硒源,系统研究了十一烯酸锌、十四酸锌和硬脂酸锌为锌前驱体对Mn掺杂ZnSe量子点光学性质的影响,初步探讨了三种锌前驱体的由于碳链长度不同、反应活性差异导致Mn离子在量子点晶格中掺杂位置变化,以及Mn离子掺杂位置对量子点光学性质和稳定性的影响。通过改变油胺的添加量,调控晶面的表面势能,研究了其对Mn掺杂ZnSe量子点粒子形貌及光学性质的影响。     

磁性杂质对量子点内电子态密度Kondo峰的影响

讨论了一个耦合于量子点的磁性杂质,当两边是铁磁性导线时量子点上电子的态密度Kondo峰的变化情况。用格林函数运动方程的方法和特定的自洽方法得到了态密度的解析表达式。杂质与量子点上电子的耦合使得原本简并的电子能级分裂。数值计算结果表明当两边的铁磁导线极化反平行时,态密度的Kondo峰几乎不随着磁性杂质方位角的变化而变化。当极化平行时,会出现3个Kondo峰,并且峰之间的间隔随着杂质的方位角的增大而增大。如果选取适当极化率的铁磁导线,由导线的铁磁性引起的Kondo峰的分裂可以被杂质的耦合作用抵?消掉。?     

Quantum quench of Kondo correlations in optical absorption

The interaction between a single confined spin and the spins of an electron reservoir leads to one of the most remarkable phenomena of many-body physics--the Kondo effect. Electronic transport measurements on single artificial atoms, or quantum dots, have made it possible to study the effect in great detail. Here we report optical measurements on a single semiconductor quantum dot tunnel-coupled to a degenerate electron gas which show that absorption of a single photon leads to an abrupt change in the system Hamiltonian and a quantum quench of Kondo correlations. By inferring the characteristic power-law exponents from the experimental absorption line shapes, we find a unique signature of the quench in the form of an Anderson orthogonality catastrophe, induced by a vanishing overlap between the initial and final many-body wavefunctions. We show that the power-law exponent that determines the degree of orthogonality can be tuned using an external magnetic field, which unequivocally demonstrates that the observed absorption line shape originates from Kondo correlations. Our experiments demonstrate that optical measurements on single artificial atoms offer new perspectives on many-body phenomena previously studied using transport spectroscopy only.     

Kondo physics in carbon nanotubes

The connection of electrical leads to wire-like molecules is a logical step in the development of molecular electronics, but also allows studies of fundamental physics. For example, metallic carbon nanotubes are quantum wires that have been found to act as one-dimensional quantum dots, Luttinger liquids, proximity-induced superconductors and ballistic and diffusive one-dimensional metals. Here we report that electrically contacted single-walled carbon nanotubes can serve as powerful probes of Kondo physics, demonstrating the universality of the Kondo effect. Arising in the prototypical case from the interaction between a localized impurity magnetic moment and delocalized electrons in a metallic host, the Kondo effect has been used to explain enhanced low-temperature scattering from magnetic impurities in metals, and also occurs in transport through semiconductor quantum dots. The far greater tunability of dots (in our case, nanotubes) compared with atomic impurities renders new classes of Kondo-like effects accessible. Our nanotube devices differ from previous systems in which Kondo effects have been observed, in that they are one-dimensional quantum dots with three-dimensional metal (gold) reservoirs. This allows us to observe Kondo resonances for very large electron numbers (N) in the dot, and approaching the unitary limit (where the transmission reaches its maximum possible value). Moreover, we detect a previously unobserved Kondo effect, occurring for even values of N in a magnetic field.     

Sensitized chemiluminescence reaction between hydrogen peroxide and periodate of different types of Mn-doped ZnS quantum dots

In this work, different types of Mn-doped ZnS QDs were prepared and applied to study of the chemiluminescence reaction of hydrogen peroxide and periodate. The effects of the size of nanoparticles, shell protection and the stabilizing agents on chemilu-minescence intensity were studied. The results indicated that the size of quantum dots was not the only factor to enhance the intensity of chemiluminescence system. Different stabilizing agents and the silica film protection will also influence the performance of the quantum dots in the chemiluminescence reaction. A CL spectrum was examined by using a series of high-energy cut-off optical filters and a possible mechanism of the CL was also proposed.     

Kondo resonance in a single-molecule transistor

When an individual molecule, nanocrystal, nanotube or lithographically defined quantum dot is attached to metallic electrodes via tunnel barriers, electron transport is dominated by single-electron charging and energy-level quantization. As the coupling to the electrodes increases, higher-order tunnelling and correlated electron motion give rise to new phenomena, including the Kondo resonance. To date, all of the studies of Kondo phenomena in quantum dots have been performed on systems where precise control over the spin degrees of freedom is difficult. Molecules incorporating transition-metal atoms provide powerful new systems in this regard, because the spin and orbital degrees of freedom can be controlled through well-defined chemistry. Here we report the observation of the Kondo effect in single-molecule transistors, where an individual divanadium molecule serves as a spin impurity. We find that the Kondo resonance can be tuned reversibly using the gate voltage to alter the charge and spin state of the molecule. The resonance persists at temperatures up to 30 K and when the energy separation between the molecular state and the Fermi level of the metal exceeds 100 meV.