Negative differential resistance in the unsymmetrical C121-based molecular junction

Using first-principles density functional theory and non-equilibrium Green?s function formalism for quantum transport calculation, we have investigated the electronic transport properties of the unsymmetrical C₁₂₁-based molecular junction. Our results show that the current-voltage curve displays a negative differential resistance phenomenon in a certain bias voltage range. The mechanism for the negative differential resistance phenomenon is suggested. The present findings could be helpful for the application of the C₁₂₁ molecule in the field of single molecular devices or nanometer electronics.     

Orientation effect on the electronic transport properties of C24 fullerene molecule

The transport properties of the cage-like molecule depend on its orientation between the electrodes, but the investigation on the mechanism has not been found. Using first-principle density-functional theory (DFT) and non-equilibrium Green’s function (NEGF) formalism for quantum transport calculation, we study the electronic transport properties of C₂₄ fullerene molecule with different orientations in Au–C₂₄–Au two-probe system. The effects of k-point sampling on the Brillouin zone are explored. Our results show that the negative differential resistance of C₂₄ molecule is found in such a system and can be tuned by the molecule's orientation in the two-probe system. We also proposed a mechanism for it. The I–V characteristic under bias voltage is determined. The present findings could be helpful for the application of the C₂₄ molecule in the field of single molecular devices or nanometer electronics.     

Rectifying properties of a boron/nitrogen-doped C131-based molecular junction: A first-principles study

Using first-principles density functional theory and non-equilibrium Green′s function formalism for quantum transport calculation, we have investigated the electronic transport properties of the boron/nitrogen-doped C₁₃₁-based molecular junction. Our results show that an obvious rectifying behavior is observed. Moreover, the rectifying performance can be tuned by adjusting the doping sites. The mechanism for the rectifying phenomenon is suggested. The present findings could be helpful for the application of the C₁₃₁ molecule in the field of single molecular devices or nanometer electronics.     

Au电极连接富勒烯C32分子的电子结构与传输特性

采用基于密度泛函理论(DFT)和非平衡格林函数(NEGF)的第一性原理方法对富勒烯C₃₂分子及在C₃₂分子的距离最远的两个碳原子处连接Au(1,1,1)电极的分子器件进行了电子结构和电子输运性质的研究.考虑到中间分子与Au电极间距离变化的情况,通过计算得出了在不同距离下分子器件的电子传输谱和I-V特性,分析了各器件的电子结构和电子输运特性产生的原因,并分析了电极与中间分子的连接距离及门电压对分子器件电子输运的影响.得出了电极与所连接的中间分子之     

First-principles study of the electronic transport properties of a C131 -based molecular junction

Using first-principles density functional theory and the non-equilibrium Green’s function formalism, we have studied the electronic transport properties of the dumbbell-like fullerene dimer C₁₃₁-based molecular junction. Our results show that the current-voltage curve displays an obvious negative differential resistance phenomenon in a certain bias voltage range. The negative differential resistance behavior can be understood in terms of the evolution of the transmission spectrum and the projected density of states with applied bias voltage. The present findings could be helpful for the application of the C₁₃₁ molecule in the field of single molecular devices or nanometer electronics.     

Transport in fullerene device coupled to Cu,Ag and Au electrodes

We present an ab initio approach of the electronic transport through a single molecular junction based on C₂₀ fullerene. The electronic properties of a single molecular junction constrained within two semi-infinite metallic electrodes are largely affected by the choice of electrode material. The two-probe device formed by the mechanically control break technique has been modelled with three distinct electrode materials from group IB of the periodic table, namely copper, silver and gold. The quantum characteristics of these mechanically stable devices are obtained by utilising first-principle density functional theory together with non-equilibrium green function method. We evaluate the quantum characteristics, namely density of states, transmission spectrum, energy levels, current and conductance, which essentially determine the behaviour of a molecule linked to different electrodes. Our investigation concludes that copper, silver and gold electrode configuration in conjunction with C₂₀ fullerene behaves as metallic, non-metallic and semi-metallic in nature, respectively.     

碳原子线的电子传输特性

单分子电子器件的电子传输特性是当前分子电子学领域研究的热点.本文采用第一原理的ab inito法与格林函数方法,对Au电极-碳原子线-Au电极体系的电子结构以及电子传输等特性进行了分析,给出了C5、C10与C15原子线的电导 -电压曲线与伏安曲线.研究结果表明:碳原子线与Au电极之间的"接触"(结合)既有共价键的成分,又有离子键的成分;碳原子线的电导率及伏安特性具有特殊的量子效应和尺寸效应.     

The assignment of molecular infrared spectra from a laser magnetic resonance spectrometer

Mathematical techniques are presented which have proved useful in assigning the laser magnetic resonance pure-rotation spectrum of HO₂, i.e., useful in assigning an absorption spectrum obtained when molecular energy levels are Zeeman shifted by an external magnetic field until transition frequencies coincide with a fixed-frequency radiation source. The techniques described should have general applicability to the laser magnetic resonance vibration-rotation spectrum of any molecule in an orbitally nondegenerate electronic state and a doublet electronic spin state ($\text{S =}\text{1}\text{2}$). Equations involving both Zeeman line positions and Zeeman line intensities are presented. These allow the assignment of M_J quantum numbers, the determination of the spin-rotation interaction constant γ and rotational quantum number N for both the upper and the lower state, and the determination of the zero-field transition frequency. The equations can be used without prior knowledge of the molecular structure or energy levels.     

InAs quantum dot field effect transistors

We have studied single electron and hole storage in self-assembled InAs quantum dots (QDs) embedded in GaAs/n-AlGaAs field effect transistors (QD-FETs). We prepared two types of QD-FETs. A single electron and a photo-generated single hole can be stored in each QD in Type 1. In the new Type II, single-electron discharge processes can be controlled by a surface gate voltage (V_g) as well as single-electron storage processes. We demonstrate possible application to novel photo devices and quantum dot memory devices.     

Intramolecular Hamiltonian logic gates

An intramolecular computing model is presented that is based on the quantum time evolution of a single molecule driven by the preparation of a non-stationary single-electron state. In our scheme, the input bits are encoded into the coupling constants of the Hamiltonian that governs the molecular quantum dynamics. The results of the computation are obtained by carrying out a quantum measurement on the molecule. We design reliable , , and logic gates. This opens new avenues for the design of more complex logic circuits at a single-molecular scale.     

Entanglement in the supermolecular dimer [Mn4]2

This paper investigates the entanglement in the supermolecular dimer [Mn4]2 consisting of a pair of single molecular magnets with antiferromagnetic exchange-coupllng J. The conventional yon Neumann entropy as a function of the exchange-coupling is calculated explicitly for all eigenstates with the quantum number range from M = M1 ＋ M2 = -9 to 0. It is shown that the yon Neumann entropy is not a monotonic function of the coupling strength. However, it is significant that the entropy of entanglement has the maximum values and the minimum values for most eigenstates, which is extremely useful in the quantum computing. It also presents the time-evolution of entanglement from various initial states. The results are useful in the design of devices based on the entanglement of two molecular magnets.     

Switching an electrical current with atoms: the reproducible operation of a multi-atom relay

The demonstration of a multi-atom quantum point contact relay is reported, which can be reversibly switched between a quantized conducting ‘on-state’ and an insulating ‘off-state’ by applying an electrochemical control potential to a separate, third electrode, the control or gate electrode. The transition occurs directly from the conducting ‘on-state’ at 5 G₀ (G₀=2e²/h being the conductance quantum) to the insulating ‘off-state’. No stable intermediate levels are observed during the switching process, indicating a reproducible bistable reconfiguration of one single multi-atom contact rather than a deposition and dissolution of different parallel contacts. The results at the same time demonstrate the feasibility and reproducible operation of a configurable electronic device based on a multi-atom contact, which exhibits the functionality of an atomic relay or a transistor, opening intriguing perspectives for electronics and logics on the atomic scale.     

Magnetocaloric features of complex molecular magnets: The (Cr7Ni)2Cu molecular magnet and beyond

We study the new kind of systems represented by the Cr₇Ni-M-Cr₇Ni (M=Cu⁺²) molecule, which is a promising molecular achievement from the perspective of molecular electronics. By using an effective quantum Hamiltonian, an exact calculation of the magnetic specific heat C_Mag and the magnetocaloric features, namely, the adiabatic change of the entropy ΔS_Mag and temperature ΔT_ad, respectively, are developed. A systematic simulation of the magnetocaloric properties is generated by modifying the effective exchange couplings into the molecular system. Extended discussion of calculated magnetocaloric features and its possible realization by experimental methods, are performed. In addition, comparisons with an exact numerical result and with a Van Vleck transformation, which has important application in similar micromagnetic structures with no exact analytical solution and larger Hilbert space, are presented. Moreover, an expression for the entangling-excitation frequencies of these systems is given as first application of our simplified solution to the effective molecular Hamiltonian.     

Molecular-scale electronics

Molecular electronics is envisioned as a promising candidate for the nanoelectronics of the future. More than a possible answer to the ultimate miniaturization problem in nanoelectronics, molecular electronics is foreseen as a possible and reasonable way to assemble a large numbers of nanoscale objects (molecules, nanoparticles, nanotubes and nanowires) to form new devices and circuit architectures. It is also an interesting approach to significantly reduce the fabrication costs, as well as the energetical costs of computation, compared to usual semiconductor technologies. Moreover, molecular electronics is a field with a large spectrum of investigations: from quantum objects for testing new paradigms, to hybrid molecular-silicon CMOS devices. To cite this article: D. Vuillaume, C. R. Physique 9 (2008).     

Laser spectroscopy of NO2 under very high resolution: Fluorescence spectra from selectively excited hfs levels

Absorption spectra of NO₂ with reduced Doppler width and resolved hyperfine structure have been obtained by crossing the beam from a single mode argon laser, tunable around 4880 and 5145 Å, with a well-collimated NO₂ beam at low pressures. With the laser frequency stabilized onto selected NO₂ absorption lines the fluorescence spectra of NO₂ molecules in selectively populated hfs levels of an excited electronic state were examined through a grating monochromator which resolved the different rotational lines. From the fluorescence spectra the quantum numbers N′ and K′ of the emitting levels could be determined. The analysis proved that some emitting levels have K′-values differing from that of the primarily excited level. This implies radiationless transitions between different electronic states in the free molecule, which can change the value of K′ but preserve that of N′.     

Lifetimes of the electronic-vibrational-rotational states of hydrogen molecule (Review)

Data on the lifetimes of the vibrational-rotational levels of the excited electronic states of hydrogen molecule (including H₂, D₂, HD, DT, and T₂ isotopomers) are reviewed. All data on the rotational sublevels of the lowest vibrational levels of various electronic states are presented, which were available before June 2001. A comparative analysis of the data obtained by various researchers using different methods (experimental, semi-empirical, and non-empirical) is performed for the first time. The influence of non-adiabatic intramolecular interactions on the dependence of lifetimes of the rovibronic levels of hydrogen molecule on the vibrational and rotational quantum numbers is discussed. A set of reliable data is selected which can be recommended for use in various applications.     

Quantum size effects of CO reactivity on metallic quantum dots

We study the reactivity of a metallic quantum dot when exposed to a gas phase CO molecule. First, we perform a Newns-Anderson model calculation in which the valence electrons of the quantum dot are confined by a finite potential well and the molecule is characterized by its lowest unoccupied molecular orbital in the gas phase. A pronounced quantum size effect regarding the charge transfer between the quantum dot and molecule is observed. We then perform a first-principles calculation for a selected size interval. The quantum dot is described within the jellium model and the molecule by pseudopotentials. Our results show that the charge transfer between the quantum dot and the molecule depends critically on the size of the quantum dot, and that this dependence is intimately connected with the electronic structure. The key factor for charge transfer is the presence of states with the symmetry of the chemically active molecular orbital at the Fermi level.     

Evidence on single-molecule transport in electrostatically-gated molecular transistors

We show that, if adequately formulated for molecular electronics, the barrier picture can quantitatively reproduce the currents and describe the orbital gating in the molecular transistors fabricated by Song et al. [H. Song, Y. Kim, Y.H. Jang, H. Jeong, M.A. Reed, T. Lee, Nature 462 (2009) 1039]. Based on our results, we demonstrate (i) that the measured current represents the contribution of a single   molecule, and (ii) the linear dependence of the molecular orbital energy offset _εg${\epsilon }_g$ on the voltage _Vt$V_t$ at the Fowler–Nordheim minimum, validating thereby the transition voltage spectroscopy for the gated single molecule devices of Song et al.     

利用电子结构数据拟合H2分子的电子壳模型势函数参数

电子壳模型势函数在离子晶体的原子级计算机模拟中有广泛应用,其势参数主要通过拟合晶体的实验数据或电子结构数据得到.提出了通过拟合双原子分子的量子化学从头计算电子结构数据来获得该势函数的方法,并由H₂分子的电子结构数据建立了H原子间的电子壳模型势函数.此外,还应用该势函数对H⁺₂分子离子进行了计算.该势函数拟合方案更适合于共价键型的分子. 关键词： 电子壳模型势 参数拟合 共价键 2分子')" href="#">H₂分子