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Action spectroscopy of single molecules reactions with STM – My personal view back from 2001- 用STM进行单分子反应的作用光谱——我个人从2001年开始的观点
IF 6.4 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2018-12-01 Epub Date: 2018-10-25 DOI: 10.1016/j.progsurf.2018.09.001
H. Ueba
<div><p>Having obtained an invitation to submit this personal view back to 2001 when I started to work with Prof. Maki Kawai for developing a theory of lateral hopping of a single CO molecule on Pd (1<!--> <!-->1<!--> <span><span>0) with Bo Persson, I briefly describe how I got an idea for elementary processes of vibrationally mediated reactions of single molecules on metal surfaces. During the work with Prof. S.G. Thihodeev on a theory of inelastic </span>electron tunneling<span> spectroscopy (IETS) with scanning tunneling spectrum (STM-IETS), I found that IET current is expressed in terms of a vibrational density of states of a single molecule. This enabled me to propose a formula for a reaction rate </span></span><span><math><mrow><mi>R</mi><mo>(</mo><mi>V</mi><mo>)</mo></mrow></math></span> or yield per electron <span><math><mrow><mi>Y</mi><mo>(</mo><mi>V</mi><mo>)</mo><mo>=</mo><mi>R</mi><mo>(</mo><mi>V</mi><mo>)</mo><mo>/</mo><mi>I</mi></mrow></math></span>, here <em>I</em> is a tunneling current, <em>i.e.,</em> action spectrum (STM-AS) of a single molecule reaction. I applied this formula to reproduce the experimental result of a CO molecule hopping on Pd (1<!--> <!-->1<!--> <!-->0) surface and more insights into the elementary process were revealed. Thomas Frederiksen and Magus Paulsson jointed me to develop a general formula of <span><math><mrow><mi>Y</mi><mo>(</mo><mi>V</mi><mo>)</mo></mrow></math></span> and successfully applied it to analyse the experimental results of H-atom relay reaction of a linear chain, H(D)<sub>2</sub>O-OH(D)-O(D) H → H(D)-H(D)<sub>2</sub>-OH(D)  → H(D)-H(D)-OH(D)<sub>2</sub><span> that was observed by Takashi Kumagai and Hiroshi Okuyama. Actually a hydrogen atom excited at one end of a linear chain composed of H</span><sub>2</sub>O and several OH generates another one at the other end. We employed our formula of to reproduce the experimental result of <span><math><mrow><mi>Y</mi><mo>(</mo><mi>V</mi><mo>)</mo></mrow></math></span>. It was found that excitation of the three characteristic vibrational modes (free OH/OD stretch, OH<sup>∗</sup> = OD<sup>∗</sup> stretch, and H<sub>2</sub>O scissors, where H<sup>∗</sup> = D<sup>∗</sup> denotes the shared H/D<sup>∗</sup> atom in the H bond) were involved in the relay reaction. It was remarked that the OH(D<sup>∗</sup>) = OD(D<sup>∗</sup><span><span> stretch modes are significantly redshifted from free OH/OD stretch and also characterized by very large broadening. The significant mode softening with respect to the free stretch modes and spectacular enhancement of the width are known to originate in the strong anharmonic character of a single H bond. Thomas investigated the reaction pathway from total energy calculations for the H-atom transfer reaction by the nudged elastic band method. The initial step is translation of the shared H-atom to the center </span>hydroxyl, which is almost barrierless. The subsequent H-bond cleavage between OH and the center water molecule
2001年,我受邀提交了这一个人观点,当时我开始与Maki Kawai教授合作,与Bo Persson一起开发Pd(110)上单个CO分子的横向跳跃理论,我简要描述了我是如何得到金属表面上单个分子振动介导反应的基本过程的想法。在与S.G. Thihodeev教授一起研究非弹性电子隧道能谱(IETS)和扫描隧道能谱(STM-IETS)理论的过程中,我发现IET电流是用单个分子的振动态密度来表示的。这使我提出了反应速率R(V)或每电子产率Y(V)=R(V)/I的公式,这里I是隧穿电流,即单分子反应的作用谱(STM-AS)。我应用这个公式重现了CO分子在Pd(110)表面跳跃的实验结果,揭示了对基本过程的更多认识。Thomas Frederiksen和Magus Paulsson与我共同开发了Y(V)的通式,并成功地应用于熊谷隆和奥山宏观察到的线性链H(D) 20 -OH(D)-O(D) H → H(D)-H(D)2-OH(D) → H(D)-H(D)-OH(D)2的实验结果。实际上,一个氢原子在由H2O和几个OH组成的线性链的一端被激发,在另一端产生另一个。我们用的公式再现了Y(V)的实验结果。发现三种特征振动模式(自由OH/OD拉伸,OH∗ = OD∗拉伸和H2O剪子,其中H∗ = D∗表示H键中共享的H/D∗原子)的激发参与了接力反应。结果表明,OH(D∗) = OD(D∗)的拉伸模式与自由OH/OD拉伸模式有明显的红移,并且具有很大的展宽。相对于自由拉伸模式的显著模式软化和宽度的显著增强是由单个氢键的强非调和特性引起的。Thomas用微推弹性带法从h原子转移反应的总能量计算出发,研究了反应途径。第一步是将共用的h原子转移到中心的羟基上,这几乎是没有障碍的。随后OH与中心水分子之间的氢键劈裂构成了最高位垒,主要涉及中心水分子沿[0 0 1]方向的位移。因此,假设OH, OH *拉伸和H2O剪刀模式与氢键裂解的反应坐标偶联。我们已经证明了在铜(11 10)上组装的h键链中振动诱导的h原子-键接力反应。在该反应中,h原子转移导致水分子从链的一端“结构”转移到另一端,而不改变链的平台,或实际上转移分子。自1998年W. Ho小组发表C2H(D)2在Cu(1 0 0)上的旋转问题以来,我一直在思考这个悬而未决的问题。这种实验方法和结果作为单分子开关的首次演示,被广泛认为是单分子操纵的里程碑式的报道,通过隧道电流和施加偏压来激发分子的振动模式。他们观察到STM图像在施加适当的偏置电压前后以90度旋转。他们进一步比较了IETS光谱和自转的Y(V)。观察到的峰值与阈值偏置电压非常吻合,这清楚地证明了旋转是由C2H(D)2的特定振动模式激发引起的。特别是随着隧穿电流的增加,从单电子过程到双电子过程的交叉是非常有趣的。当时Sergei和他的博士生Yulia E. Shchadilova以及Magnus帮助我重现了所有的实验结果,他们利用Keldysh Green函数理论结合从头算密度泛函数理论(DFT)计算了优化的吸附几何形状,并进行了精密的振动分析。Y(V)的实验结果通过假设一个单电子过程激发C-H拉伸模式,两个电子过程(C-H振动能级的阶梯攀登)和一个组合带的激发得到再现。我还简要介绍了我与Bo、Sergei、Magnus和Thomas共同开发的STM-AS理论。
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引用次数: 1
Nitride layers on uranium surfaces 铀表面的氮化物层
IF 6.4 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2018-08-01 Epub Date: 2018-09-01 DOI: 10.1016/j.progsurf.2018.08.002
Kezhao Liu , Xiaofang Wang , Jing Liu , Yin Hu , Huoping Zhong , Qifa Pan , Lizhu Luo , Shouchuang Chen , Yongbin Zhang , Zhong Long

Uranium as an important energy material plays a significant role within the field of material sciences and nuclear industrial applications. However, metallic uranium is chemically active in ambient environment and is easily oxidized and corroded, leading to not only deterioration of its properties and failure of performance as working components but also nuclear pollution of the environment. Therefore, the development of corrosion protection systems for metallic uranium is an issue of prime importance. In view of the nitridation technology in Ti and Fe-based alloys, the successful application to improve the surface wear hardness and corrosion resistance, several nitridation methods have been developed for the surface modification of metallic uranium. Many studies have shown that the surface nitridation of metallic uranium can efficiently improve its corrosion resistance. The surface oxidation layer thickness is as thin as several nanometers even if placed 4 years in the atmosphere. At the present, nitridation of uranium surface is considered as the most promising surface modification way to protect uranium from corrosion. To design and fabricate nitride layers on uranium surface with reliable long-term protective effects, however, one needs deep understanding on the relationships among the physical and chemical properties of the nitride layers, the composition and structure of the layers, and the dependence on the techniques and the processing parameters. One also needs deep understanding on the corrosion behavior of the prepared nitride layers in the environment, and the related corrosion mechanism.

In this review, we bring to the readers the achievements and recent advances on the uranium nitridation in the world, including the processing techniques and the related studies on the formation mechanism of the nitride layers, and the understanding on the property-processing-corrosion performance relationship of the layers, aiming at the development of high-performance resistance layers for metallic uranium by the surface nitridation technique. In the review (1) the surface nitridation techniques developed recently, the relationship between the preparation parameters and the composition as well as the structure of the surface layer are summarized; (2) the fundamental physical properties of the uranium nitrides are summarized, depicted and discussed; (3) the influence of the nitrides structure and composition and of the environment on resistance to corrosion as well as the formation mechanism of corroded products in oxidizing environments are depicted and discussed; (4) the potential application of uranium nitrides in other application field such as the application of thermal-electrical conversion is also discussed. Finally, the prospective on the investigations of nitride layers is suggested.

铀作为一种重要的能源材料,在材料科学和核工业应用领域发挥着重要作用。然而,金属铀在环境中具有化学活性,易被氧化和腐蚀,不仅导致其性能恶化和工作部件性能失效,而且对环境造成核污染。因此,开发金属铀的腐蚀防护系统是一个至关重要的问题。鉴于氮化技术在Ti和fe基合金中的成功应用,提高了金属铀的表面磨损硬度和耐蚀性,开发了几种氮化方法用于金属铀的表面改性。许多研究表明,金属铀的表面氮化可以有效地提高其耐蚀性。即使在大气中放置4 年,表面氧化层厚度也只有几纳米薄。目前,铀表面氮化处理被认为是最有前途的防止铀腐蚀的表面改性方法。然而,要在铀表面设计和制造具有可靠的长期保护作用的氮化层,需要深入了解氮化层的物理化学性质与氮化层的组成和结构之间的关系,以及对技术和工艺参数的依赖性。还需要深入了解所制备的氮化物层在环境中的腐蚀行为及其腐蚀机理。本文综述了国内外在铀氮化方面取得的成就和最新进展,包括氮化层的加工技术和形成机理的相关研究,以及对氮化层性能-加工-腐蚀性能关系的认识,旨在利用表面氮化技术开发高性能金属铀电阻层。(1)综述了近年来国内外表面氮化技术的研究进展,综述了制备工艺参数与表面氮化层的组成及结构之间的关系;(2)总结、描述和讨论了氮化铀的基本物理性质;(3)描述和讨论了氮化物的结构、组成和环境对耐蚀性的影响,以及氧化环境中腐蚀产物的形成机理;(4)讨论了氮化铀在热电转换等其他应用领域的潜在应用。最后,对氮化层的研究进行了展望。
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引用次数: 20
In situ studies of oxide nucleation, growth, and transformation using slow electrons 用慢电子进行氧化物成核、生长和转变的原位研究
IF 6.4 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2018-05-01 Epub Date: 2018-04-03 DOI: 10.1016/j.progsurf.2018.02.001
Jan Ingo Flege , David C. Grinter

Surface processes such as metal oxidation and metal oxide growth invariably influence the physical and chemical properties of materials and determine their interaction with their surroundings and hence their functionality in many technical applications. On a fundamental level, these processes are found to be governed by a complex interplay of thermodynamic variables and kinetic constraints, resulting in a rich variety of material-specific phenomena. In this review article, we discuss recent results and insights on transition metal oxidation and rare-earth oxide growth acquired by low-energy electron microscopy and related techniques. We demonstrate that the use of in situ surface sensitive methods is a prerequisite to gaining a deeper understanding of the underlying concepts and the mechanisms responsible for the emerging oxide structure and morphology. Furthermore, examples will be provided on how structural and chemical modifications of the oxide films and nanostructures can be followed in real-time and analyzed in terms of local reactivity and cooperative effects relevant for heterogeneous model catalysis.

金属氧化和金属氧化物生长等表面过程不可避免地影响材料的物理和化学性质,并决定它们与周围环境的相互作用,从而决定它们在许多技术应用中的功能。在基本层面上,这些过程被发现是由热力学变量和动力学约束的复杂相互作用所控制的,导致了丰富多样的材料特定现象。本文综述了利用低能电镜及相关技术对过渡金属氧化和稀土氧化物生长的最新研究成果和见解。我们证明,使用原位表面敏感方法是获得对新出现的氧化物结构和形态的基本概念和机制的更深入理解的先决条件。此外,还将举例说明如何实时跟踪氧化膜和纳米结构的结构和化学修饰,并根据与多相模型催化相关的局部反应性和协同效应进行分析。
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引用次数: 12
Single magnetic adsorbates on s-wave superconductors s波超导体上的单磁吸附
IF 6.4 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2018-02-01 Epub Date: 2018-03-13 DOI: 10.1016/j.progsurf.2018.01.001
Benjamin W. Heinrich , Jose I. Pascual , Katharina J. Franke

In superconductors, magnetic impurities induce a pair-breaking potential for Cooper pairs, which locally affects the Bogoliubov quasiparticles and gives rise to Yu-Shiba-Rusinov (YSR or Shiba, in short) bound states in the density of states (DoS). These states carry information on the magnetic coupling strength of the impurity with the superconductor, which determines the many-body ground state properties of the system. Recently, the interest in Shiba physics was boosted by the prediction of topological superconductivity and Majorana modes in magnetically coupled chains and arrays of Shiba impurities.

Here, we review the physical insights obtained by scanning tunneling microscopy into single magnetic adsorbates on the s-wave superconductor lead (Pb). We explore the tunneling processes into Shiba states, show how magnetic anisotropy affects many-body excitations, and determine the crossing of the many-body ground state through a quantum phase transition. Finally, we discuss the coupling of impurities into dimers and chains and their relation to Majorana physics.

在超导体中,磁性杂质诱发库珀对的破对电位,局部影响Bogoliubov准粒子,并在态密度(DoS)中产生Yu-Shiba-Rusinov (YSR或简称Shiba)束缚态。这些态携带着杂质与超导体的磁耦合强度的信息,这决定了系统的多体基态性质。最近,柴巴杂质的磁耦合链和阵列的拓扑超导性和马约拉纳模式的预测促进了对柴巴物理的兴趣。在这里,我们回顾了通过扫描隧道显微镜对s波超导体铅(Pb)上的单磁吸附所获得的物理见解。我们探索了进入Shiba态的隧穿过程,展示了磁各向异性如何影响多体激发,并确定了通过量子相变的多体基态的交叉。最后,我们讨论了杂质耦合成二聚体和链及其与马约拉纳物理的关系。
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引用次数: 142
Photon upconversion towards applications in energy conversion and bioimaging 光子上转换在能量转换和生物成像中的应用
IF 6.4 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2017-12-01 Epub Date: 2017-10-04 DOI: 10.1016/j.progsurf.2017.09.003
Qi-C. Sun , Yuchen C. Ding , Dodderi M. Sagar , Prashant Nagpal

The field of plasmonics can play an important role in developing novel devices for application in energy and healthcare. In this review article, we consider the progress made in design and fabrication of upconverting nanoparticles and metal nanostructures for precisely manipulating light photons, with a wavelength of several hundred nanometers, at nanometer length scales, and describe how to tailor their interactions with molecules and surfaces so that two or more lower energy photons can be used to generate a single higher energy photon in a process called photon upconversion. This review begins by introducing the current state-of-the-art in upconverting nanoparticle synthesis and achievements in color tuning and upconversion enhancement. Through understanding and tailoring physical processes, color tuning and strong upconversion enhancement have been demonstrated by coupling with surface plasmon polariton waves, especially for low intensity or diffuse infrared radiation. Since more than 30% of incident sunlight is not utilized in most photovoltaic cells, this photon upconversion is one of the promising approaches to break the so-called Shockley-Queisser thermodynamic limit for a single junction solar cell. Furthermore, since the low energy photons typically cover the biological window of optical transparency, this approach can also be particularly beneficial for novel biosensing and bioimaging techniques. Taken together, the recent research boosts the applications of photon upconversion using designed metal nanostructures and nanoparticles for green energy, bioimaging, and therapy.

等离子体领域在开发应用于能源和医疗保健的新型器件方面发挥着重要作用。在这篇综述文章中,我们考虑了在设计和制造上转换纳米粒子和金属纳米结构方面取得的进展,以精确地操纵波长为几百纳米的光子,在纳米尺度上,并描述了如何定制它们与分子和表面的相互作用,以便两个或多个低能量光子可以在光子上转换过程中产生单个高能量光子。本文首先介绍了目前上转换纳米粒子合成的最新技术以及在颜色调谐和上转换增强方面的成就。通过对物理过程的理解和剪裁,颜色调谐和强上转换增强已被证明与表面等离子激元极化子波耦合,特别是对低强度或漫射红外辐射。由于在大多数光伏电池中,超过30%的入射阳光没有被利用,这种光子上转换是打破单结太阳能电池所谓的Shockley-Queisser热力学极限的有前途的方法之一。此外,由于低能量光子通常覆盖光学透明的生物窗口,这种方法也可以特别有利于新的生物传感和生物成像技术。综上所述,最近的研究促进了光子上转换的应用,利用设计的金属纳米结构和纳米粒子用于绿色能源,生物成像和治疗。
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引用次数: 31
Two-dimensional silica opens new perspectives 二维二氧化硅开启了新的视角
IF 6.4 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2017-12-01 Epub Date: 2017-10-06 DOI: 10.1016/j.progsurf.2017.09.001
Christin Büchner, Markus Heyde

In recent years, silica films have emerged as a novel class of two-dimensional (2D) materials. Several groups succeeded in epitaxial growth of ultrathin SiO2 layers using different growth methods and various substrates. The structures consist of tetrahedral [SiO4] building blocks in two mirror symmetrical planes, connected via oxygen bridges. This arrangement is called a silica bilayer as it is the thinnest 2D arrangement with the stoichiometry SiO2 known today. With all bonds saturated within the nano-sheet, the interaction with the substrate is based on van der Waals forces. Complex ring networks are observed, including hexagonal honeycomb lattices, point defects and domain boundaries, as well as amorphous domains. The network structures are highly tuneable through variation of the substrate, deposition parameters, cooling procedure, introducing dopants or intercalating small species.

The amorphous networks and structural defects were resolved with atomic resolution microscopy and modeled with density functional theory and molecular dynamics. Such data contribute to our understanding of the formation and characteristic motifs of glassy systems. Growth studies and doping with other chemical elements reveal ways to tune ring sizes and defects as well as chemical reactivities. The pristine films have been utilized as molecular sieves and for confining molecules in nanocatalysis. Post growth hydroxylation can be used to tweak the reactivity as well.

The electronic properties of silica bilayers are favourable for using silica as insulators in 2D material stacks. Due to the fully saturated atomic structure, the bilayer interacts weakly with the substrate and can be described as quasi-freestanding. Recently, a mm-scale film transfer under structure retention has been demonstrated. The chemical and mechanical stability of silica bilayers is very promising for technological applications in 2D heterostacks.

Due to the impact of this bilayer system for glass science, catalysis and the field of 2D materials, a large number of theoretical and experimental studies on silica bilayers have been reported in the last years. This review aims to provide an overview on the insights gained on this material and to point out opportunities for further discovery in various fields.

近年来,二氧化硅薄膜作为一种新型的二维(2D)材料出现。几个研究组使用不同的生长方法和不同的衬底成功地外延生长了超薄SiO2层。该结构由两个镜面对称平面上的四面体[SiO4]建筑块组成,通过氧桥连接。这种排列被称为二氧化硅双分子层,因为它是目前已知的具有化学计量SiO2的最薄的二维排列。当纳米片内的所有键都饱和时,与衬底的相互作用是基于范德华力的。观察到复杂的环形网络,包括六边形蜂窝晶格,点缺陷和区域边界,以及非晶区域。通过改变衬底、沉积参数、冷却程序、引入掺杂剂或插入小物质,网络结构具有高度可调谐性。利用原子分辨显微镜分析了非晶态网络和结构缺陷,并用密度泛函理论和分子动力学建模。这些数据有助于我们理解玻璃系的形成和特征基序。生长研究和掺杂其他化学元素揭示了调整环尺寸和缺陷以及化学反应的方法。原始膜已被用作分子筛和限制分子在纳米催化。生长后羟基化也可以用来调整反应性。二氧化硅双分子层的电子特性有利于在二维材料堆中使用二氧化硅作为绝缘体。由于完全饱和的原子结构,双分子层与底物的相互作用弱,可以描述为准独立的。最近,研究人员证实了结构保留下的毫米尺度薄膜转移。二氧化硅双分子层的化学和机械稳定性在二维异质堆叠中具有广阔的应用前景。由于这种双层体系对玻璃科学、催化和二维材料领域的影响,近年来有大量关于二氧化硅双层的理论和实验研究报道。这篇综述的目的是提供对这些材料的见解的概述,并指出在各个领域进一步发现的机会。
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引用次数: 69
Surface and interface sciences of Li-ion batteries 锂离子电池的表面和界面科学
IF 6.4 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2017-12-01 Epub Date: 2017-11-14 DOI: 10.1016/j.progsurf.2017.10.001
Taketoshi Minato , Takeshi Abe

The application potential of Li-ion batteries is growing as demand increases in different fields at various stages in energy systems, in addition to their conventional role as power sources for portable devices. In particular, applications in electric vehicles and renewable energy storage are increasing for Li-ion batteries. For these applications, improvements in battery performance are necessary. The Li-ion battery produces and stores electric power from the electrochemical redox reactions between the electrode materials. The interface between the electrodes and electrolyte strongly affects the battery performance because the charge transfer causing the electrode redox reaction begins at this interface. Understanding of the surface structure, electronic structure, and chemical reactions at the electrode–electrolyte interface is necessary to improve battery performance. However, the interface is located between the electrode and electrolyte materials, hindering the experimental analysis of the interface; thus, the physical properties and chemical processes have remained poorly understood until recently. Investigations of the physical properties and chemical processes at the interface have been performed using advanced surface science techniques. In this review, current knowledge and future research prospects regarding the electrode–electrolyte interface are described for the further development of Li-ion batteries.

随着锂离子电池在能源系统不同阶段、不同领域的需求增加,其应用潜力也在不断增长,除了它们作为便携式设备电源的传统角色之外。特别是锂离子电池在电动汽车和可再生能源存储方面的应用正在增加。对于这些应用,改进电池性能是必要的。锂离子电池通过电极材料之间的电化学氧化还原反应产生并储存电能。电极和电解质之间的界面对电池性能有很大影响,因为引起电极氧化还原反应的电荷转移始于该界面。了解表面结构、电子结构和电极-电解质界面的化学反应对提高电池性能是必要的。然而,界面位于电极和电解质材料之间,阻碍了界面的实验分析;因此,直到最近,人们对其物理性质和化学过程仍然知之甚少。使用先进的表面科学技术对界面的物理性质和化学过程进行了研究。本文综述了锂离子电池在电极-电解质界面方面的研究现状和未来的研究前景,为锂离子电池的进一步发展提供参考。
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引用次数: 67
Doped and codoped silicon nanocrystals: The role of surfaces and interfaces 掺杂和共掺杂硅纳米晶体:表面和界面的作用
IF 6.4 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2017-12-01 Epub Date: 2017-10-12 DOI: 10.1016/j.progsurf.2017.07.003
Ivan Marri, Elena Degoli, Stefano Ossicini

Si nanocrystals have been extensively studied because of their novel properties and their potential applications in electronic, optoelectronic, photovoltaic, thermoelectric and biological devices. These new properties are achieved through the combination of the quantum confinement of carriers and the strong influence of surface chemistry. As in the case of bulk Si the tuning of the electronic, optical and transport properties is related to the possibility of doping, in a controlled way, the nanocrystals. This is a big challenge since several studies have revealed that doping in Si nanocrystals differs from the one of the bulk. Theory and experiments have underlined that doping and codoping are influenced by a large number of parameters such as size, shape, passivation and chemical environment of the silicon nanocrystals. However, the connection between these parameters and dopant localization as well as the occurrence of self-purification effects are still not clear. In this review we summarize the latest progress in this fascinating research field considering free-standing and matrix-embedded Si nanocrystals both from the theoretical and experimental point of view, with special attention given to the results obtained by ab-initio calculations and to size-, surface- and interface-induced effects.

硅纳米晶体由于其新颖的性质和在电子、光电、光伏、热电和生物器件方面的潜在应用而受到广泛的研究。这些新性质是通过载流子的量子约束和表面化学的强大影响相结合而实现的。与体硅的情况一样,电子、光学和输运性质的调整与纳米晶体以可控方式掺杂的可能性有关。这是一个巨大的挑战,因为几项研究表明,硅纳米晶体中的掺杂与体中的掺杂不同。理论和实验表明,掺杂和共掺杂受到硅纳米晶体尺寸、形状、钝化和化学环境等诸多参数的影响。然而,这些参数与掺杂剂的定位以及自净化效应的发生之间的关系尚不清楚。在这篇综述中,我们从理论和实验的角度总结了这一引人注目的研究领域的最新进展,包括独立的和基质嵌入的硅纳米晶体,特别关注通过从头计算得到的结果以及尺寸、表面和界面诱导的效应。
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引用次数: 29
Surface chemistry and microscopy of food powders 食品粉末的表面化学和显微学
IF 6.4 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2017-12-01 Epub Date: 2017-08-10 DOI: 10.1016/j.progsurf.2017.07.002
Jennifer Burgain , Jeremy Petit , Joël Scher , Ron Rasch , Bhesh Bhandari , Claire Gaiani

Despite high industrial and scientific interest, a comprehensive review of the surface science of food powders is still lacking. There is a real gap between scientific concerns of the field and accessible reviews on the subject. The global description of the surface of food powders by multi-scale microscopy approaches seems to be essential in order to investigate their complexity and take advantage of their high innovation potential.

Links between these techniques and the interest to develop a multi-analytical approach to investigate scientific questions dealing with powder functionality are discussed in the second part of the review. Finally, some techniques used in others fields and showing promising possibilities in the food powder domain will be highlighted.

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尽管工业和科学对食品粉末的表面科学有很高的兴趣,但对食品粉末表面科学的全面审查仍然缺乏。在该领域的科学关注和对该主题的可获得的评论之间存在着真正的差距。为了研究食品粉末的复杂性和利用其巨大的创新潜力,用多尺度显微镜方法对食品粉末表面进行全局描述似乎是必不可少的。这些技术和兴趣之间的联系,以开发一种多分析方法来调查处理粉末功能的科学问题,讨论在审查的第二部分。最后,将重点介绍一些在其他领域应用的技术,并在食品粉末领域显示出良好的可能性。下载:下载高清图片(202KB)下载:下载全尺寸图片
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引用次数: 35
Atomic-scale investigation of nuclear quantum effects of surface water: Experiments and theory 地表水核量子效应的原子尺度研究:实验与理论
IF 6.4 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2017-12-01 Epub Date: 2017-11-21 DOI: 10.1016/j.progsurf.2017.11.001
Jing Guo , Xin-Zheng Li , Jinbo Peng , En-Ge Wang , Ying Jiang

Quantum behaviors of protons in terms of tunneling and zero-point motion have significant effects on the macroscopic properties, structure, and dynamics of water even at room temperature or higher. In spite of tremendous theoretical and experimental efforts, accurate and quantitative description of the nuclear quantum effects (NQEs) is still challenging. The main difficulty lies in that the NQEs are extremely susceptible to the structural inhomogeneity and local environments, especially when interfacial systems are concerned. In this review article, we will highlight the recent advances of scanning tunneling microscopy and spectroscopy (STM/S), which allows the access to the quantum degree of freedom of protons both in real and energy space. In addition, we will also introduce recent development of ab initio path-integral molecular dynamics (PIMD) simulations at surfaces/interfaces, in which both the electrons and nuclei are treated as quantum particles in contrast to traditional ab initio molecular dynamics (MD). Then we will discuss how the combination of STM/S and PIMD are used to directly visualize the concerted quantum tunneling of protons within the water clusters and quantify the impact of zero-point motion on the strength of a single hydrogen bond (H bond) at a water/solid interface. Those results may open up the new possibility of exploring the exotic quantum states of light nuclei at surfaces, as well as the quantum coupling between the electrons and nuclei.

即使在室温或更高温度下,质子隧穿和零点运动的量子行为对水的宏观性质、结构和动力学也有显著影响。尽管在理论和实验方面做出了巨大的努力,但准确、定量地描述核量子效应仍然具有挑战性。主要困难在于nqe极易受到结构不均匀性和局部环境的影响,特别是在涉及界面系统时。在这篇综述文章中,我们将重点介绍扫描隧道显微镜和光谱学(STM/S)的最新进展,它允许在实空间和能量空间中获得质子的量子自由度。此外,我们还将介绍表面/界面上从头算路径积分分子动力学(PIMD)模拟的最新发展,与传统的从头算分子动力学(MD)相比,电子和原子核都被视为量子粒子。然后,我们将讨论如何使用STM/S和PIMD的组合来直接可视化水团内质子的协调量子隧穿,并量化零点运动对水/固体界面上单个氢键(H键)强度的影响。这些结果可能为探索表面轻核的奇异量子态以及电子和原子核之间的量子耦合开辟了新的可能性。
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引用次数: 23
期刊
Progress in Surface Science
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