从对称到非对称双势阱中量子隧穿特性的研究

利用二能级近似通过对对称和非对称双势阱波函数的研究,揭示了基态和激发态量子隧穿随外场变化的规律。对称势阱内的量子隧穿是自发的、活跃的。非对称势阱内,即使附加静电场相当小时波函数就出现了定域,量子隧穿现象完全消失。根据波函数的动态定域特点得到了量子隧穿的动态消失过程。     

细胞骨架微管管壁中电子的隧道效应

该文基于细胞骨架微管结构的对称性,将其壁上的原丝纤维视为一维的动力学系统,采用“双势阱”模型和量子力学的基本方法,对发生在微管壁上的一根原丝纤维上电子的势垒穿透几率和由隧道效应引起的基态能级劈裂进行了理论计算,得到了一些有意义的物理结果.     

色关联噪声驱动双稳系统平均首通时间的研究

 研究了色关联噪声驱动双稳系统的瞬时性质,根据Novikov定理和Fox近似方法得到相应的Fokker-Planck方程,使用最陡下降法得到了2个相反方向平均首通时间的解析表达式,即T⁺(从左势阱到右势阱)和T^-(从右势阱到左势阱).经过数值计算,结果表明:①加性和乘性噪声的色关联效应使得一个方向上的逃逸变得更加容易,而另一个方向上的逃逸更加困难;②在正关联情况下,加性和乘性噪声的关联时间的增加会使得左势阱到右势阱的逃逸抑制现象减弱;而在负关联情况下,加性和乘性噪声的关联时间的增加会使得右势阱到左势阱的逃逸抑制现象减弱;并且噪声关联的色效应对正关联和负关联任意方向上的平均首通时间的影响完全相反.     

静电场作用下非对称双势阱中本征问题的研究

利用二能级近似和迭代方法,研究了静电场作用下W型双势阱的本征问题和对称及非对称双势阱内本征值所呈现的各种特性.结果表明,对称势阱内存在双能级结构和确定宇称的波函数.在非对称势阱中,外场较小时,仍为双能级结构,但波函数出现定域;外场较强时,双势阱向单阱过渡,能级分布失去双能级结构,即类似单阱内能级分布.     

石墨烯双势垒结构中的输运特性

利用Landauer-Büttiker散射理论和传递矩阵方法研究了单层石墨烯双势垒结构中的隧穿几率和电导.计算结果表明:即使存在克莱因隧穿效应,单层石墨烯双势垒结构中的量子隧穿仍然与势阱宽度和势垒高度密切相关.隧穿几率和电导表现出复杂的振荡行为,振荡的振幅和周期敏感地依赖于势阱宽度、势垒高度、电子的入射能量和入射角度....     

一维双势垒结构的谐振隧穿效应

分析和计算了一维双势垒结构发生谐振效应的物理机制、条件和透射几率,发现在此结构中电子的运动情况与一维无限深势阱情况基本一致。     

一维模型原子高次谐波特性研究

通过数值计算求解含时的薛定谔方程,研究了在隧道电离区域16个激光脉冲作用于不同势阱势函数对应的一维模型原子产生的高次谐波特性,结果表明：在隧道电离区域势函数势阱的形状对一维模型原子的高次谐波强度产生较大影响,同时谐波的平台宽度的高阶区域也受到势函数的影响.     

δ复数势阱的隧穿时间的研究

首先通过边界条件求解薛定谔方程,计算出粒子穿过单个δ复数势阱和双δ复数势阱的相时,然后运用Matlab和Origin数学软件,分析系统中的相关因素对相时的影响.研究表明,两种情况下相时受势阱的实部和虚部以及入射能量等因素的影响是不同的,对于单个δ复数势阱有一个相时最大值,而对于双δ复数势阱却有一个相时最小值.并把两种情况分别作了比较说明.     

C_4~(2+)分子的E_g b_(1g)系统的Jahn-Teller效应及其各向异性现象

依据Jahn-Teller效应理论与量子理论,利用群论和对称性分析的方法探讨了C42+分子的Eg b1g系统的Jahn-Teller效应及其各向异性现象,构建了Eg b1g系统的电声耦合哈密顿量,借助幺正平移变换计算出了系统的电子基态与激发态及其能量.结果表明,由于电声耦合作用的缘故,系统发生了Jahn-Teller畸变,畸变使得系统在其势能面上形成了两个具有D2h对称性势阱.无论系统处在哪一个势阱中,系统的二重简并的电子基态能级都将发生分裂,因此畸变导致系统电子基态的简并性完全被消除.经过Jahn-Teller畸变,C42+分子就会从D4h对称性降低到D2h对称性,同时C42+分子的振动频率发生分解,频率的分解就意味着C42+分子的各向同性遭到破坏而呈现出各向异性.     

C24+分子的Eg(⊙)b1g系统的Jahn-Teller效应及其各向异性现象

依据Jahn-Teller效应理论与量子理论,利用群论和对称性分析的方法探讨了C24+分子的Eg(⊙)b1g系统的Jahn-Teller效应及其各向异性现象,构建了Eg(⊙)b1g系统的电声耦合哈密顿量,借助幺正平移变换计算出了系统的电子基态与激发态及其能量.结果表明,由于电声耦合作用的缘故,系统发生了Jahn-Teller畸变,畸变使得系统在其势能面上形成了两个具有D2h对称性势阱.无论系统处在哪一个势阱中,系统的二重简并的电子基态能级都将发生分裂,因此畸变导致系统电子基态的简并性完全被消除.经过Jahn-Teller畸变,C24+分子就会从D4h对称性降低到D2h对称性,同时C24+分子的振动频率发生分解,频率的分解就意味着C24+分子的各向同性遭到破坏而呈现出各向异性.     

Direct observation of second-order atom tunnelling

Tunnelling of material particles through a classically impenetrable barrier constitutes one of the hallmark effects of quantum physics. When interactions between the particles compete with their mobility through a tunnel junction, intriguing dynamical behaviour can arise because the particles do not tunnel independently. In single-electron or Bloch transistors, for example, the tunnelling of an electron or Cooper pair can be enabled or suppressed by the presence of a second charge carrier due to Coulomb blockade. Here we report direct, time-resolved observations of the correlated tunnelling of two interacting ultracold atoms through a barrier in a double-well potential. For the regime in which the interactions between the atoms are weak and tunnel coupling dominates, individual atoms can tunnel independently, similar to the case of a normal Josephson junction. However, when strong repulsive interactions are present, two atoms located on one side of the barrier cannot separate, but are observed to tunnel together as a pair in a second-order co-tunnelling process. By recording both the atom position and phase coherence over time, we fully characterize the tunnelling process for a single atom as well as the correlated dynamics of a pair of atoms for weak and strong interactions. In addition, we identify a conditional tunnelling regime in which a single atom can only tunnel in the presence of a second particle, acting as a single atom switch. Such second-order tunnelling events, which are the dominating dynamical effect in the strongly interacting regime, have not been previously observed with ultracold atoms. Similar second-order processes form the basis of superexchange interactions between atoms on neighbouring lattice sites of a periodic potential, a central component of proposals for realizing quantum magnetism.     

Enzyme dynamics and hydrogen tunnelling in a thermophilic alcohol dehydrogenase.

Biological catalysts (enzymes) speed up reactions by many orders of magnitude using fundamental physical processes to increase chemical reactivity. Hydrogen tunnelling has increasingly been found to contribute to enzyme reactions at room temperature. Tunnelling is the phenomenon by which a particle transfers through a reaction barrier as a result of its wave-like property. In reactions involving small molecules, the relative importance of tunnelling increases as the temperature is reduced. We have now investigated whether hydrogen tunnelling occurs at elevated temperatures in a biological system that functions physiologically under such conditions. Using a thermophilic alcohol dehydrogenase (ADH), we find that hydrogen tunnelling makes a significant contribution at 65 degrees C; this is analogous to previous findings with mesophilic ADH at 25 degrees C. Contrary to predictions for tunnelling through a rigid barrier, the tunnelling with the thermophilic ADH decreases at and below room temperature. These findings provide experimental evidence for a role of thermally excited enzyme fluctuations in modulating enzyme-catalysed bond cleavage.     

Attosecond real-time observation of electron tunnelling in atoms

Atoms exposed to intense light lose one or more electrons and become ions. In strong fields, the process is predicted to occur via tunnelling through the binding potential that is suppressed by the light field near the peaks of its oscillations. Here we report the real-time observation of this most elementary step in strong-field interactions: light-induced electron tunnelling. The process is found to deplete atomic bound states in sharp steps lasting several hundred attoseconds. This suggests a new technique, attosecond tunnelling, for probing short-lived, transient states of atoms or molecules with high temporal resolution. The utility of attosecond tunnelling is demonstrated by capturing multi-electron excitation (shake-up) and relaxation (cascaded Auger decay) processes with subfemtosecond resolution.     

Two-electron dissociation of single molecules by atomic manipulation at room temperature

Using the tip of a scanning tunnelling microscope (STM) to mechanically manipulate individual atoms and molecules on a surface is now a well established procedure. Similarly, selective vibrational excitation of adsorbed molecules with an STM tip to induce motion or dissociation has been widely demonstrated. Such experiments are usually performed on weakly bound atoms that need to be stabilized by operating at cryogenic temperatures. Analogous experiments at room temperature are more difficult, because they require relatively strongly bound species that are not perturbed by random thermal fluctuations. But manipulation can still be achieved through electronic excitation of the atom or molecule by the electron current tunnelling between STM tip and surface at relatively high bias voltages, typically 1-5 V. Here we use this approach to selectively dissociate chlorine atoms from individual oriented chlorobenzene molecules adsorbed on a Si(111)-7 x 7 surface. We map out the final destination of the chlorine daughter atoms, finding that their radial and angular distributions depend on the tunnelling current and hence excitation rate. In our system, one tunnelling electron has nominally sufficient energy to induce dissociation, yet the process requires two electrons. We explain these observations by a two-electron mechanism that couples vibrational excitation and dissociative electron attachment steps.     

Exchange-biased quantum tunnelling in a supramolecular dimer of single-molecule magnets

Various present and future specialized applications of magnets require monodisperse, small magnetic particles, and the discovery of molecules that can function as nanoscale magnets was an important development in this regard. These molecules act as single-domain magnetic particles that, below their blocking temperature, exhibit magnetization hysteresis, a classical property of macroscopic magnets. Such 'single-molecule magnets' (SMMs) straddle the interface between classical and quantum mechanical behaviour because they also display quantum tunnelling of magnetization and quantum phase interference. Quantum tunnelling of magnetization can be advantageous for some potential applications of SMMs, for example, in providing the quantum superposition of states required for quantum computing. However, it is a disadvantage in other applications, such as information storage, where it would lead to information loss. Thus it is important to both understand and control the quantum properties of SMMs. Here we report a supramolecular SMM dimer in which antiferromagnetic coupling between the two components results in quantum behaviour different from that of the individual SMMs. Our experimental observations and theoretical analysis suggest a means of tuning the quantum tunnelling of magnetization in SMMs. This system may also prove useful for studying quantum tunnelling of relevance to mesoscopic antiferromagnets.     

Selectivity in vibrationally mediated single-molecule chemistry

The selective excitation of molecular vibrations provides a means to directly influence the speed and outcome of chemical reactions. Such mode-selective chemistry has traditionally used laser pulses to prepare reactants in specific vibrational states to enhance reactivity or modify the distribution of product species. Inelastic tunnelling electrons may also excite molecular vibrations and have been used to that effect on adsorbed molecules, to cleave individual chemical bonds and induce molecular motion or dissociation. Here we demonstrate that inelastic tunnelling electrons can be tuned to induce selectively either the translation or desorption of individual ammonia molecules on a Cu(100) surface. We are able to select a particular reaction pathway by adjusting the electronic tunnelling current and energy during the reaction induction such that we activate either the stretching vibration of ammonia or the inversion of its pyramidal structure. Our results illustrate the ability of the scanning tunnelling microscope to probe single-molecule events in the limit of very low yield and very low power irradiation, which should allow the investigation of reaction pathways not readily amenable to study by more conventional approaches.     

Resolving the time when an electron exits a tunnelling barrier

The tunnelling of a particle through a barrier is one of the most fundamental and ubiquitous quantum processes. When induced by an intense laser field, electron tunnelling from atoms and molecules initiates a broad range of phenomena such as the generation of attosecond pulses, laser-induced electron diffraction and holography. These processes evolve on the attosecond timescale (1?attosecond?≡?1?as = 10(-18)?seconds) and are well suited to the investigation of a general issue much debated since the early days of quantum mechanics--the link between the tunnelling of an electron through a barrier and its dynamics outside the barrier. Previous experiments have measured tunnelling rates with attosecond time resolution and tunnelling delay times. Here we study laser-induced tunnelling by using a weak probe field to steer the tunnelled electron in the lateral direction and then monitor the effect on the attosecond light bursts emitted when the liberated electron re-encounters the parent ion. We show that this approach allows us to measure the time at which the electron exits from the tunnelling barrier. We demonstrate the high sensitivity of the measurement by detecting subtle delays in ionization times from two orbitals of a carbon dioxide molecule. Measurement of the tunnelling process is essential for all attosecond experiments where strong-field ionization initiates ultrafast dynamics. Our approach provides a general tool for time-resolving multi-electron rearrangements in atoms and molecules--one of the key challenges in ultrafast science.     

Molecular manipulation using a tunnelling microscope

In a very short time the scanning tunnelling microscope has become an important tool in surface science, and physics in general. Its primary use has been to obtain atomic-resolution images of surfaces, but recently, efforts have been made to use it to manipulate materials as well as image them. One may now reasonably ask if it is possible to move and alter matter predictably on an atomic scale. Here we report the accomplishment of the smallest yet, purposeful, spatially localized changes in matter, effected on a graphite surface. We believe that the changes result from the pinning of individual organic molecules to the graphite. The reverse manipulation, the removal of pinned molecules, has also been demonstrated. Finally, we have evidence that we can remove a portion of a pinned molecule, effectively performing transformations on single molecules using the tunnelling microscope.     

A nanometre-scale electronic switch consisting of a metal cluster and redox-addressable groups

So-called bottom-up fabrication methods aim to assemble and integrate molecular components exhibiting specific functions into electronic devices that are orders of magnitude smaller than can be fabricated by lithographic techniques. Fundamental to the success of the bottom-up approach is the ability to control electron transport across molecular components. Organic molecules containing redox centres-chemical species whose oxidation number, and hence electronic structure, can be changed reversibly-support resonant tunnelling and display promising functional behaviour when sandwiched as molecular layers between electrical contacts, but their integration into more complex assemblies remains challenging. For this reason, functionalized metal nanoparticles have attracted much interest: they exhibit single-electron characteristics (such as quantized capacitance charging) and can be organized through simple self-assembly methods into well ordered structures, with the nanoparticles at controlled locations. Here we report scanning tunnelling microscopy measurements showing that organic molecules containing redox centres can be used to attach metal nanoparticles to electrode surfaces and so control the electron transport between them. Our system consists of gold nanoclusters a few nanometres across and functionalized with polymethylene chains that carry a central, reversibly reducible bipyridinium moiety. We expect that the ability to electronically contact metal nanoparticles via redox-active molecules, and to alter profoundly their tunnelling properties by charge injection into these molecules, can form the basis for a range of nanoscale electronic switches.