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1.
由于势能面崎岖不平存在大量的局部极小点,短程Morse团簇的全局优化极具挑战. 本文采用了最近自主发展的无偏模糊全局优化方法,系统地研究了原子数N≤400的短程(ρ=14)Morse团簇. 与目前已知的N≤400以及少数几个较大尺寸的短程Morse团簇结果对照,我们以较高的成功率得到了文献中报道过的所有全局最优结构,同时还发现了N=164,175,188,193,194,197,239,246,260,318和389团簇具有新的能量更低全局最小(和局部极小)构型. 通过拟合团簇最优结构能量与尺寸的依赖关系,确定了一系列具有魔幻尺寸的团簇. 研究表明,当N较大时,短程Morse团簇的最优结构倾向于密堆积.  相似文献   

2.
利用密度泛函理论通过计算吸附能量、HOMO/LUMO能隙变化、电荷转移、结构扭曲等研究二氧化氮分子在B12N12纳米笼的吸附.此外,通过计算B12N12的电子结合能、Gibbs自由能、态密度和分子表面的静电势研究其稳定性和其它特性.B12N12纳米笼吸附二氧化氮显示三种构型.B12N12团簇的HOMO/LUMO能隙变化对二氧化氮分子的存在非常敏感,从自由团簇的6.84 eV降为NO2/团簇稳定团簇的3.23 eV.团簇的导电性被极大地提高,表明B12N12纳米簇可能是潜在的二氧化氮气体分子检测传感器.  相似文献   

3.
赵文杰  王清林  任凤竹  罗有华 《物理学报》2007,56(10):5746-5753
从第一性原理出发,利用密度泛函理论中的广义梯度近似对ZrnFe(n=2—13)团簇进行了结构优化、能量和频率计算.在充分考虑自旋多重度的前提下,对每一具体尺寸的团簇,得到了多个平衡构型,并根据能量高低确定了团簇的基态结构.综合团簇的结合能、二阶能量差分以及团簇的最高占据轨道和最低未占据轨道间的能隙可知Zr5Fe,Zr7Fe和Zr12Fe团簇的稳定性相对较高,Zr12Fe团簇的结构是具有Ih对称性的正二十面体,而且Zr12Fe的稳定性在所有团簇中是最高的.另外,不仅Zr5Fe,Zr7Fe和Zr12Fe团簇的稳定性相对较高,而且它们均为磁性团簇(而Zrn团簇的磁矩在n≥5时已经发生了淬灭),由此可知通过选择合适的掺杂元素可能得到高稳定的磁性团簇.从Mulliken布居分析结果可知,除了在Zr12Fe团簇中Fe原子失去少量电荷外,其他团簇中Fe原子均从Zr原子那里得到了一定量电荷,即Fe原子在ZrnFe(n=2—13,n≠12)团簇中是电子受体.  相似文献   

4.
本文利用尺寸选择的负离子光电子能谱和理论计算探索Au2Gen-/0 (n=1∽8)团簇的结构演化和电子性质. 通过比较理论模拟谱与实验谱,并使用CCSD(T)理论方法计算异构体的相对能量,从而确定金锗混合团簇的全局最小结构. 本文发现Au2Gen-/0 (n=1∽8)团簇的两个Au原子具有较高的配位数和较弱的亲金相互作用. 负离子团簇和中性团簇的最稳定结构分别处于自旋双重态和自旋单重态. 除了Au2Ge4-/0和Au2Ge5-/0,负离子团簇和中性团簇的全局最小结构具有相似的结构特点. Au2Ge1-/0团簇是一个C2v对称的V形结构,而Au2Ge2-/0团簇是一个C2v对称的双桥连结构. Au2Ge1-负离子团簇是两个Au原子盖帽的Ge4四面体结构,而Au2Ge4中性团簇是两个Au原子盖帽的Ge4菱形结构. Au2Ge5∽8-/0团簇主要采用三棱柱、四棱柱、及五棱柱结构. Au2Ge6是一个C2v对称的四棱柱结构,并表现出σ和π双键性质.  相似文献   

5.
本文采用尺寸选择的负离子光电子能谱与高精度理论计算,对AlnC4-/0(n=2∽4))团簇的结构和成键性质进行了研究. Al2C4-团簇负离子的最稳定结构是一个C2v对称的平面结构,其中两个C2单元与两个铝原子分别相连. Al2C4-团簇负离子的次稳定结构是一个线型结构,两个铝原子位于C4线型结构两端,能量仅比最稳定结构高0.05 eV. 中性Al2C4团簇是一个线型结构. Al3C4-团簇负离子是一个平面结构,其中三个铝原子分别与两个C2单元相连. 而中性Al3C4团簇则是一个V字型结构. Al4C4-团簇负离子和中性Al4C4团簇均为C2h对称的平面结构,四个铝原子分别位于两个C2单元的末端. AlnC4-/0(n=2∽4))团簇负离子的自适应自然密度配分的分析结果表明这些团簇中铝原子与C2单元之间的化学键具有σ和π键特征.  相似文献   

6.
本文基于密度泛函理论系统地研究了(TiO2)n团簇上二氧化碳(CO2)的吸附和活化性质. 计算结果表明,CO2更倾向于吸附在(TiO2)n团簇的桥氧原子上,形成“化学吸附”碳酸盐络合物. 而CO更倾向于吸附到末端Ti-O的Ti原子上. 发现计算得到的碳酸盐振动频率值与实验获得的结果非常吻合,这表明配合物中CO2的几何构型与其线性型相比,有微小的弯转. 通过对电子结构、电荷密度、电离势、HOMO-LUMO以及态密度的分析,证实了CO2与团簇之间的电荷转移以及相互作用. 从预测的能量分布图来看,(TiO2)n团簇上的CO2活化与结构密切有关,相比于块体的TiO2,CO2在团簇结构上更易于吸附和活化.  相似文献   

7.
王晓坡  宋渤  吴江涛  刘志刚 《物理学报》2010,59(10):7158-7163
采用反转法计算得到了O2-CO2混合气体新的势能参数.在此基础上,根据分子动力学理论,计算了混合气体在零密度下的输运性质,包括黏度系数、热扩散系数和热扩散因子,计算的温度范围为273.15—3273.15 K.与实验值比较表明,计算结果可以满足实际工程应用.  相似文献   

8.
钼团簇因具有独特的结构、电子和物理化学性质,被期待在未来的纳米科技中扮演重要角色,但是它们的基态结构至今还存在争议. 本研究采用粒子群优化(CALYPSO)方法对Mon (n=2∽18)团簇的晶体结构进行全局域能量最小化搜索,并结合第一性原理方法进一步优化. 计算表明:当4s和4p半核态不作为价态时,Mon (n=2∽18)团簇有明显的二聚体趋势,原子数为偶数的团簇往往是“幻数”团簇,具有较高的稳定性;但是,将4s和4p电子作为价电子后,平均杂化指数HspHsdHpd显著降低,二聚体趋势急剧减弱. 本文报道了Mon(n=11,14,15)团簇的新基态结构,证明了半核态对于Mon团簇是十分重要的.  相似文献   

9.
张彩霞  郭虹  杨致  骆游桦 《物理学报》2012,61(19):193601-193601
利用密度泛函理论和非平衡格林函数方法, 本文对小尺寸团簇Tan(B3N3H6)n+1 (n ≤ 4)的磁性和量子输运性质进行了系统的研究. 计算结果表明, 此类体系采用三明治结构作为其基态并且具有较高的稳定性. 体系的磁矩随团簇尺寸的增大而线性增大. 当把Tan(B3N3H6)n+1团簇耦合到Au电极上时, 形成的Au-Tan(B3N3H6)n+1-Au体系在有限偏压下展示出了较强的自旋过滤能力, 因而可以被看做是一类新型的低维自旋过滤器.  相似文献   

10.
金蓉  谌晓洪 《物理学报》2010,59(10):6955-6962
用B3LYP/LANL2DZ方法对ZrnPd(n =1—13)团簇的平衡几何结构、能量、频率、电子性质和磁性进行了计算.研究表明,Pd原子位于表面的异构体更为稳定,其中Zr7Pd,Zr12Pd团簇稳定性高,是幻数团簇,此外,相对于ZrnCo与ZrnFe团簇,ZrnPd团簇参与化学反应的能力较弱,化学稳定性更  相似文献   

11.
It is shown that, when highly vibrationally excited SF6 molecules (with vibrational energy E vib ≥ 0.5–2 eV) collide with weakly bound van der Waals Ar N , Kr N , or (N2) N (N ≤ 30–40 atoms in a cluster) clusters in intersecting molecular and cluster beams, the molecules are trapped by the clusters, the clusters then undergo full disintegration, and the trapped molecules become free. The method of studying this process and the results obtained are described. The possibilities of application of this method for selective doping of clusters by molecules, laser separation of isotopes, and selective transportation of molecules to a surface are discussed.  相似文献   

12.
Based on the parent tetrazole 2N-oxide, six series of novel carbon-linked ditetrazole 2N-oxides with different energetic substituent groups (-NH2, -N3, -NO2, NF2, -NHNO2) and energetic bridge groups (-CH2-, -CH2-CH2-, -NH-, -N=N-, -NH-NH-) were designed. The overall performance and the effects of different energetic substituent groups and energetic bridge groups on the performance were investigated by density functional theory and electrostatic potential methods. The results showed that most of designed compounds have oxygen balance around zero, high heats of formation, high density, high energy, and acceptable sensitivity, indicating that tetrazole N-oxide is a useful parent energetic compound employed for obtaining high energy compounds, even only combined with some very common energetic substituent groups and bridge groups. Comprehensively considering the effects on energy and sensitivity, the -NO2, -NF2, -NH-and -NH-NH-are appropriate substituent groups for combining tetrozale N-oxide to design new energetic compounds, while -NH2, -N3, -CH2-CH2-, and -N=N-are inappropriate.  相似文献   

13.
A new ternary van der Waals complex of the type rare gas-rare gas'-linear molecule, ArNe-N2O, was investigated using a pulsed molecular beam cavity Fourier transform microwave spectrometer. The rotational spectra of six isotopomers of the trimer were studied in detail. These include Ar20Ne-14N14NO, Ar22Ne-14N14NO, Ar20Ne-15N14NO, Ar22Ne-15N14N0, Ar20Ne-14N15NO and Ar22Ne-14N15NO. Nuclear quadrupole hyperfine structures of the rotational transitions that are due to the one or two 14N nuclei were resolved and analysed. The resulting spectroscopic constants were used to provide structural and dynamical information about the trimer. Based on the quartic centrifugal distortion constants, a harmonic force field analysis was performed to estimate the frequencies of the van der Waals vibrational modes. A perturbation of the electronic charge distribution at the site of the central 14N nucleus of N20 upon complex formation was detected and discussed. Differences of structural parameters of the trimer as compared to those of the respective dimer units are indicative of the presence of significant three-body non-additive contributions to the interaction energy.  相似文献   

14.
Likely candidates are located for the global potential energy minima of Ar* n (3 ≤ n ≤ 25) clusters using the diatomics-in-molecules (DIM) approach. The favoured geometries are found to be different from the structures of Ar+ n and correspond to the trimer Ar*3 bound to the surface of an Ar n?2 core via a common atom. The Ar n?2 core is usually only slightly distorted from its own global potential minimum, although in a few cases it corresponds to a nearby local minimum. Therefore, the ‘magic’ sizes of the excimer systems are predicted to differ from those of the ions and correlate instead with the stability of Ar n?2. The predicted electronic photoabsorption and emission spectra of Ar* n , and photoexcitation spectra of Ar n are discussed in terms of experimental data. Global potential energy minima for neutral Ar n up to n = 55 with the Aziz potential are summarized also; the structure is the same as for the Lennard-Jones potential except at n = 21 where the stabilities of the two lowest Lennard-Jones minima are reversed.  相似文献   

15.
The electronic and geometric structure of rare gas clusters doped with rare-gas atoms Rg = Xe, Kr or Ar is investigated with fluorescence excitation spectroscopy in the VUV spectral range. Several absorption bands are observed in the region of the first electronic excitations of the impurity atoms, which are related to the lowest spin-orbit split atomic 3P1 and 1P1 states. Due to influence of surrounding atoms of the cluster, the atomic lines are shifted to the blue and broadened (“electronical cage effect”). From the known interaction potentials and the measured spectral shifts the coordination of the impurity atom in ArN, KrN, NeN and HeN could be studied in great detail. In the interior of KrN and ArN the Xe atoms are located in substitutional sites with 12 nearest neighbours and internuclear distances comparable to that of the host matrix. In NeN and HeN the cluster atoms (18 and 22, respectively) arrange themselves around the Xe impurity with a bondlength comparable to that of the heteronuclear dimer. The results confirm that He clusters are liquid while Ne clusters are solid for N≥ 300. Smaller Ne clusters exhibit a liquid like behaviour. When doping is strong, small Rgm-clusters (Rg = Xe, Kr, Ar, m≤10 2) are formed in the interior sites of the host cluster made of Ne or He. Specific electronically excited states, assigned to interface excitons are observed. Their absorption bands appear and shift towards lower energy when the cluster size m increases, according to the Frenkel exciton model. The characteristic bulk excitons appear in the spectra, only when the cluster radius exceeds the penetration depth of the interface exciton, which can be considerably larger than that in free Rgm clusters. This effect is sensitive to electron affinities of the guest and the host cluster.  相似文献   

16.
采用离子束增强沉积方法在Si和SiO2/Si衬底上制备In-N共掺杂ZnO薄膜(INZO),溅射靶是用ZnO和2 atm% In2O3粉体均匀混合并压制而成,在氩离子溅射ZnO靶的同时,氮、氩混合离子束垂直注入沉积的薄膜.实验结果显示INZO薄膜具有(002)的择优取向,并且为p型导电,电阻率最低为0.9Ωcm.薄膜在氮气、氧气气氛下退火,对薄膜的结构和电学特性与成膜和退火条件的关系进行了分析. 关键词: 氧化锌薄膜 p型掺杂 离子束增强沉积  相似文献   

17.
The solid-liquid phase transitions of Lennard-Jones clusters LJN (N=39–55) were simulated by a microcanonical molecular dynamics method using Lennard-Jones potential, and their thermodynamic quantities were calculated. The caloric curves of clusters (except N=42) have S-bend. To understand this behaviour, configurational and total entropies were evaluated, and dents on the entropy curves were taken as a sign of negative heat capacity. The heat capacities were evaluated for N=39–55 clusters using configurational entropy data. The potential energy distributions have bimodal behaviour for all clusters in the given range at the melting temperature. The distinct melting behaviour of LJ42 was explained by the topology of the potential energy surface by examining the isomer distributions at phase transitions for LJ39-LJ55. The isomer distributions were found to be a useful way to interpret this behaviour and melting dynamics in general. Melting temperature, latent heat and entropy change upon melting values were reported and are consistent with literature values and values calculated from bulk thermodynamic properties. The dependence of these quantities on the size of the clusters was examined and it is found that latent heat is the key quantity to determine the magic numbers.  相似文献   

18.
Z. Li  Z. Zhao  Q. Wang  T. Shi 《Phase Transitions》2019,92(6):537-545
Configurations, stabilities and adsorption mechanisms of ground-state MonN and MonN2 (n?=?1–8) clusters are calculated by using the density functional method within the PBE level. Evidently, N atoms tend to approach more Mo atoms. Doping with two N impurity prefers to occupy symmetrical position of the host Mon (n?=?1–8) cluster except for Mo2N2 clusters. Mo4N, Mo6N, Mo2N2, Mo4N2 and Mo6N2 clusters have higher structural stabilities than their neighbors by the second derivative of total binding energy. Mo2N, Mo4N and Mo7N, Mo2N2, Mo5N2 and Mo7N2 clusters have higher kinetic reactivity than their neighbors by the HOMO–LUMO gaps. The adsorption capacity of a N atom to Mo4 cluster is stronger than the other Mo–N clusters.  相似文献   

19.

Molecular-dynamics simulation of the evolution of bipartite bimetallic clusters consisting of 390 atoms during bombardment by Arn (n = 1, 2, 13) clusters with initial energies from 1 eV to 1.4 keV is performed. Binary Cu–Au and Ni–Al clusters consisting of equal atomic fractions of corresponding elements were used as a target. As a result of simulation, the temperatures, changes in the potential energy, sputtering yields, and intensities of collision-stimulated displacement of atoms through the interface of monometallic parts of binary clusters, depending on the size and energy of incident particle, are obtained.

  相似文献   

20.
It has been found that collisions of highly vibrationally excited SF6 molecules (with the vibrational energy E vib ≥ 0.5–2.0 eV) with Ar N clusters (where N ≤ 30–40 is the number of atoms in a cluster) in crossed molecular and cluster beams result in capture of molecules followed by complete disintegration of the clusters. Possible applications of the effect for selective doping of clusters with molecules, laser separation of isotopes, and selective transport of molecules to the surface are discussed.  相似文献   

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