准一维纳米线电子输运的梯度无序效应

考虑实际体系的梯度无序和结散射,发展格林函数矩阵分解消元方法,研究了准一维纳米线的电子输运性质. 结果表明,由于结散射,电导随能量呈现振荡行为,无序的引入破坏了电子相干性,在低无序度区平均电导呈现异常增加,呈现一个新的电导峰. 当表面存在无序但无梯度衰减时,体系的平均电导随无序度增强先减后增,出现类局域-退局域性转变. 当表面无序线性衰减时,平均电导在强无序区稍有增加,而当表面无序高斯型衰减时,平均电导指数衰减,类局域-退局域性转变消失,不同于以前的理论预言. 研究结果对准一维纳米线电子器件的结构设计和应用有指导作用. 关键词： 准一维纳米线 梯度无序 电子输运     

CaO表面CO对NO还原作用的实验与模型研究

循环流化床炉内石灰石脱硫对NOx排放产生影响,包括对挥发分氮氧化的催化作用以及对CO-NO还原的催化作用。利用固定床反应器对不同条件下CaO颗粒表面NO+CO的催化反应特性进行了探究。实验表明,无氧条件下,CaO能够显著催化CO还原NO,NO转化率与反应温度和CO浓度正相关,与NO浓度负相关.基于Langmuir-Hinshelwood机理建立了CaO催化NO+CO反应动力学模型,模型考虑了颗粒内、外扩散的影响.该模型适用于氧气浓度很低、CO浓度较高条件下。而在有氧气氛中,该反应受到明显抑制,且O2浓度越高,抑制作用越明显;当CaO周围氧气浓度远大于CO时,可忽略CaO对NO的催化还原作用。     

一维点阵局域势中玻色系统的相图

利用高斯波泛函方法，研究了处于一维点阵局域势cos［β（ｎR）］中的玻色系统基态的相变行为．研究结果表明，一维点阵局域势系统的稳定性取决于参量γ＝β₂/4π和重整化质量μ．在不同的参量区域，μ有不同的多值性，从而在参量空间中划出相区．γ＝γ₁时，相界随杂质浓度c而定，c趋于零时，与单杂质模型的结论相符，γ₂相界与连续模型的结论相符． 关键词：     

一维自旋1/2电子系统的单杂质散射研究

应用高斯波泛函方法，研究了单个局域杂质对一维自旋1/2传导电子的散射问题．研究结果表明，双粒子散射与单粒子散射具有同样的重要性．由于这两种散射机制相互竞争，形成了拉亭格液体中电荷密度波和自旋密度波的各自的重整化质量．随着这些质量的消失，在参量空间中出现了相界，在不同相区中系统呈现不同的动力学行为 关键词：     

SO2在催化剂表面上氧化反应的动力学相变

本文用“部分模拟”法计算了ＳＯ２在催化剂表面上氧化反应的动力学相变。当仅有Ｌａｎｇｍｕｉｒ－Ｈｉｎｓｈｅｌｗｏｏｄ过程起作用时，表面体系存在三个相，氧中毒相、反应相、ＳＯ２中毒相，当Ｅｌｅｙ－Ｒｉｄｅａｌ过程同时起作用时，氧中毒相消失。     

二元凝聚体中亮-亮孤子的振荡-局域转变行为

考虑时间相关的种间相互吸引作用,研究了局限于谐振外部势阱中的二元玻色-爱因斯坦凝聚体中亮-亮孤子的传播特性.结果表明,当种内和种间相互吸引作用都不变时,亮-亮孤子呈现出周期性的振荡;如果种内相互吸引作用仍保持不变,而种间相互吸引作用随时间指数增加时,发现凝聚体中产生振荡-局域转变行为,且这种振荡-局域的转变行为可通过调节谐振势阱的横向囚禁频率来控制.此外,还设计了实验方案来观察孤子的这种振荡-局域转变行为.     

均相条件下NO与CO、NCO的反应机理研究

基于量子化学密度泛函理论研究了NO与CO、NCO在均相条件下的反应机理并进行了动力学和平衡常数的分析. CO与NO的均相反应存在两条反应路径：两者首先反应形成中间体CNO₂,CNO₂不易稳定存在,其继续与CO、NO反应分别生成NCO、N₂O. NCO的生成速率大于N₂O,但两条反应路径的反应速率常数都很小.与已发现的反应路径相比,反应中间体CNO₂可以降低均相条件下CO与NO的反应能垒,分析发现CNO₂中的N原子是易发生反应的活性位点. NCO与NO的反应同样存在两条路径,优势反应路径随温度升高而改变,但非优势路径对反应的贡献不能忽略,分析平衡常数可知N₂的存在对反应影响可以忽略,因此燃烧环境中NCO与NO的反应既生成N₂O和CO,也生成N₂和CO₂.     

邻氨基苯甲酸BZ反应体系中的振荡与混沌：I.SCTR实验研究和非线…

本文研究了ＣＳＴＲ中邻氨基苯甲酸苯甲酸ＢＺ反应体系的振荡行为，总结了非化条件下各反应物浓度和流速变化以及温度变化对体系振荡反应的影响规律；同时还考察了催化条件下的体系振荡行为，发现了Ｍｎ（Ⅱ）催化出现复杂振荡筢应序列，非线性动力学理论分析的结果表明复杂振荡是由体系动力学本质决定的确定性行为，并发现由周期走向混沌的演变过程中存在倍周期分岔（或慢周期分岔）迹象；同时，还通过计算分维，研究反应条件对体系     

强非局域非线性介质中的非相干孤子研究

本文从一维强非局域非线性模型出发,推导出非相干光满足的非线性薛定谔方程.按照相干密度描述方法,写出非相干光的描述方式,求出了非相干光孤子的形成条件和孤子形式,还得到了相干光和非相干光在强非局域非线性介质中形成孤子的临界功率,结果说明非相干光形成孤子时,需要更高的能量.当非相干光孤子的条件不满足时,非相干光束以呈现振荡行为.空间振荡周期仅与介质、入射的非相干光的光功率有关,而与光源的非相干角功率谱宽度及具体组分无关.同时,我们还数值模拟了这种非相干光束的振荡行为和单一组分、一对组分的非相干强度演化过程.     

对氨基二苯甲酮光吸收和光反应活性的含时密度泛函研究

利用含时密度泛函理论研究了对氨基二苯甲酮(p-ABP )的气液相吸收光谱性质．结果表明，p-ABP单重态的性质随着溶剂极性的变化发生明显的改变．在极性溶剂乙腈、甲醇、乙醇、二甲亚砜和二甲基甲酰胺中，S1态是产生于π→π*跃迁的电荷转移态；在非极性溶剂环己烷和苯中，S1态是产生于n→π*跃迁的局域激发态．对于p-ABP三重态的计算结果表明，无论是极性溶剂中还是非极性溶剂中T1态都具有π→π*构型．不同溶剂中激发态构型和跃迁能的变化情况表明，对应于n→π*跃迁的吸收光谱随着溶剂极性的增加出现明显的蓝移，对应于π→π*跃迁的吸收光谱则随溶剂极性的增加出现明显红移．通过对计算结果进行分析，讨论了对氨基二苯甲酮三重态量子产率在不同溶剂中的变化情况和它在氢提取反应中表现出低光还原反应活性原因．     

The effect of inactive impurities on a surface in NO-CO reaction: A Monte Carlo simulation

The interaction among the reacting species in the NO-CO reaction on a metal catalytic surface that proceeds according to the Langmuir-Hinshelwood thermal mechanism is studied by means of Monte Carlo simulations. The study of this system is essential for the understanding of the influence of impurities on the catalytic oxidation of NO by CO. It is found that this complex system exhibits irreversible phase transitions between active states with sustained reaction and poisoned states without reaction. The same system has also been investigated by non-thermal (Eley-Rideal) mechanism. Both the phase diagrams of the surface coverage and the steady state production of CO₂ and N₂ are evaluated as a function of the partial pressures of the reactants in the gas phase. From this study, it is observed that with the increase of impurities, the production rate reduces and the reaction stops at a certain point. Moreover, the first order transition in the phase diagram converts into second order phase transition that is in accordance with the experimental findings. Therefore, the first order phase transition, which is a characteristic of such catalytic reactions, is eliminated.     

The temperature dependence of the interaction of NO + CO on Pt{1 0 0}

Infrared reflection absorption spectroscopy together with mass spectrometry has been used to investigate the interaction of NO and CO on Pt{1 0 0}, initially prepared in the reconstructed ‘hex’ phase, under ambient pressures of these gases, in the temperature range 300-500 K. The results allow the local and total coverages of adsorbed CO and NO to be related to the rate of reaction to produce gas phase CO₂, and provide insight into the species present on the surface during the so-called low temperature oscillatory reaction regime of this process. At temperatures below that at which NO dissociation occurs (approximately 390-400 K) adsorption is controlled by the non-reactive displacement of NO by CO and results in a CO-poisoned surface. Above 400 K when significant CO₂ production occurs, the NO coverage increases to produce a surface with NO and CO fully intermixed; the increase in NO coverage is attributed to the higher rate of NO arrival from the gas phase (with a partial pressure ratio of P_NO:P_CO>1) at free surface sites created by NO dissociation and subsequent reaction with CO. The competition between these two processes of non-reactive NO displacement by CO and reactive displacement of CO by NO is proposed to determine the parameter space of the low temperature oscillatory regime. Rapid equilibration between bridged and atop CO species leads to them appearing to exhibit identical reaction behaviour. Particularly at the lowest reaction temperatures (around 400 K), islands of pure CO may coexist on the surface but not participate in the reaction. Under conditions corresponding to the high temperature oscillatory regime, small quantities of absorbed CO, but no NO, are seen on the surface.     

Mixed-mode oscillations and cluster patterns in an electrochemical relaxation oscillator under galvanostatic control

We studied the dynamics of a prototypical electrochemical model, the electro-oxidation of hydrogen in the presence of poisons, under galvanostatic conditions. The lumped system exhibits relaxation oscillations, which develop mixed-mode oscillations (MMOs) for low preset currents. A fast-slow analysis of the homogeneous dynamics reveals that the MMOs arise from a fast oscillating subsystem and a one-dimensional slow manifold. In the spatially extended system, the galvanostatic constraint imposes a synchronizing global coupling that drives the system into cluster patterns. The properties of the cluster patterns (CPs) result from an intricate interplay of the nature of the local oscillators, the global constraint, and a nonlocal coupling through the electrolyte. In particular, we find that the global constraint suppresses small-amplitude oscillations of MMOs and prevents domains oscillating out of phase from occupying equal regions in phase space. The nonlocal coupling causes each individual clustered region to oscillate on a different limit cycle. Typically multistability of CPs is found. Coexisting patterns possess different oscillation periods and a different total fraction in space that occupies the in-phase or out-of-phase state, respectively.     

Resonance tongues in a system of globally coupled FitzHugh-Nagumo oscillators with time-periodic coupling strength

We investigate the dynamics of a population of globally coupled FitzHugh-Nagumo oscillators with a time-periodic coupling strength. While for synchronizing global coupling, the in-phase state is always stable, the oscillators split into several cluster states for desynchronizing global coupling, most commonly in two, irrespective of the coupling strength. This confines the ability of the system to form n:m locked states considerably. The prevalence of two and four cluster states leads to large 2:1 and 4:1 subharmonic resonance regions, while at low coupling strength for a harmonic 1:1 or a superharmonic 1:m time-periodic coupling coefficient, any resonances are absent and the system exhibits nonresonant phase drifting cluster states. Furthermore, in the unforced, globally coupled system the frequency of the oscillators in a cluster state is in general lower than that of the uncoupled oscillator and strongly depends on the coupling strength. Periodic variation of the coupling strength at twice the natural frequency causes each oscillator to keep oscillating with its autonomous oscillation period.     

Stochastic resonance in a locally excited system of bistable oscillators

Stochastic resonance is studied in a one-dimensional array of overdamped bistable oscillators in the presence of a local subthreshold periodic perturbation. The system can be treated as an ensemble of pseudospins tending to align parallel which are driven dynamically by an external periodic magnetic field. The oscillators are subjected to a dynamic white noise as well as to a static topological disorder. The latter is quantified by the fraction of randomly added long-range connections among ensemble elements. In the low connectivity regime the system displays an optimal global stochastic resonance response if a small-world network is formed. In the mean-field regime we explain strong changes in the dynamic disorder strength provoking a maximal stochastic resonance response via the variation of fraction of long-range connections by taking into account the ferromagnetic-paramagnetic phase transition of the pseudospins. The system size analysis shows only quantitative power-law type changes on increasing number of pseudospins.     

Uncertainty principle for control of ensembles of oscillators driven by common noise

We discuss control techniques for noisy self-sustained oscillators with a focus on reliability, stability of the response to noisy driving, and oscillation coherence understood in the sense of constancy of oscillation frequency. For any kind of linear feedback control — single and recursive delay feedback, linear frequency filter, etc. — the phase diffusion constant, quantifying coherence, and the Lyapunov exponent, quantifying reliability, can be efficiently controlled but their ratio remains constant. Thus, an “uncertainty principle” can be formulated: the loss of reliability occurs when coherence is enhanced and, vice versa, coherence is weakened when reliability is enhanced. Treatment of this principle for ensembles of oscillators synchronized by common noise or global coupling reveals a substantial difference between the cases of slightly non-identical oscillators and identical ones with intrinsic noise.     

Standing waves, clustering, and phase waves in 1D simulations of kinetic relaxation oscillations in NO+NH3 on Pt(1 0 0) coupled by diffusion

The Lombardo–Imbihl–Fink (LFI) ODE model of the NO+NH₃ reaction on a Pt(1 0 0) surface shows stable relaxation oscillations with very sharp transitions for temperatures T between 404 and 433 K. Here we study numerically the effect of linear diffusive coupling of these oscillators in one spatial dimension. Depending on the parameters and initial conditions we find a rich variety of spatio-temporal patterns which we group into four main regimes: bulk oscillations (BOs), standing waves (SW), phase clusters (PC), and phase waves (PW). Two key ingredients for SW and PC are identified, namely the relaxation type of the ODE oscillations and a nonlocal (and nonglobal) coupling due to relatively fast diffusion of the kinetically slaved variables NH₃ and H. In particular, the latter replaces the global coupling through the gas phase used to obtain SW and PC in models of related surface reactions. The PW exist only under the assumption of (relatively) slow diffusion of NH₃ and H.     

Mode locking in quantum optics

Mode locking phenomena in acoustics and in laser physics are discussed and are shown to share a feature of the forced oscillator: Oscillation takes place at the forcing frequency (or frequencies). The phenomena differ from simple forced oscillations in that they involve sustained oscillators (e.g., clocks, lasers) whose sustaining sources compete against the forcing signals in the choice of oscillation frequency. The locking phenomena are compared to second-order phase transitions in ferromagnetism and superconductivity where corresponding competition occurs between disordering thermal fluctuations and ordering correlations which reduce system energy.     

Phase Transitions of an Epidemic Spreading Model in Small-World Networks

We propose a modified susceptible-infected-refractory-susceptible (SIRS) model to investigate the global oscillations of the epidemic spreading inWatts-Strogatz (WS) small-world networks. It is found that when an individual immunity does not change or decays slowly in an immune period, the system can exhibit complex transition from an infecting stationary state to a large amplitude sustained oscillation or an absorbing state with no infection. When the immunity decays rapidly in the immune period, the transition to the global oscillation disappears and there is no oscillation. Furthermore, based on thespatio-temporal evolution patterns and the phase diagram, it is disclosed that a long immunity period takes an important role in the emergence of the global oscillation in small-world networks.     

The effect of NO/O2 ratio in NO-CO-O2 reaction on a catalytic surface: A computer simulation study

The interaction among the reacting species in the NO-CO-O₂ reaction on a metal catalytic surface that proceeds according to the Langmuir-Hinshelwood mechanism is studied by means of Monte Carlo simulation. The study of this three-component system is essential for the understanding of the influence of NO/O₂ ratio on the catalytic reduction of NO into N & O and oxidation of CO to CO₂. It is found that this complex system, which has not been studied on these lines before, exhibits irreversible phase transitions between active states with sustained reaction and poisoned states with the catalytic surface fully covered by the reactants. The phase diagrams of the surface coverage with CO, N or O and the steady state production of CO₂ are evaluated as a function of the partial pressure of CO in the gas phase. From this study, it is observed that with the addition of NO in the CO-O₂ reaction, the critical points in the phase diagram move towards lower values of CO partial pressure but the width of reaction window remains almost the same. However, the maximum production rate of CO₂ decreases continuously. On the other hand, the addition of O₂ in the NO-CO reaction shifts the critical points towards higher values of CO pressure. Moreover, the width of reaction window as well as the production rate of CO₂ increases with the increase in O₂ concentration.