Condensation in pulsed free jets of silane-argon mixture: Time characteristics of the pulses

Condensation of a 5% SiH₄ + 95% Ar mixture in pulsed supersonic jets was studied. The sequence of process steps was determined from time characteristics of the jet that were recorded by pulse molecular-beam mass spectrometry. It is shown that pulsed jet condensation of the silane-argon mixture causes selective heating of the components, the heating process being dependent on the density of the mixture in the settling chamber of a nozzle.     

Composition of a water vapor-argon mixture determined by the mass spectrometry of a supersonic molecular beam

It is found that the composition of a pulsed supersonic molecular beam depends on the preparation conditions of the initial mixture containing water molecules and argon atoms. The mass spectra of the molecular beam components are obtained, and the time evolution of the signal intensities for some of the ions (T form) is traced. It is shown that stable water complexes remaining intact during supersonic flow of the mixture into a vacuum may form depending on the water partial pressure.     

二元混合超声气流的剖面和质量分布

用气相电子衍射法和质谱相联合,分析了二元混合超声气流的剖面和质量分布情况。证明质谱利于确定气流剖面和气流中粒子的质量分布,而电子衍射则可以给出气流剖面和气流中生成了何种固相的信息。     

Electron impact ionization of large krypton clusters

We show that the detection of ionization of very large van der Waals clusters in a pulsed jet or a beam can be realized by using a fast ion gauge. Rapid positive feedback electron impact ionization and fragmentation processes, which are initially ignited by electron impact ionization of the krypton clusters with the electron current of the ion gauge, result in the appearance of a progressional oscillation-like ion spectrum, or just of a single fast event under critical conditions. Each line in the spectrum represents a correlated explosion or avalanche ionization of the clusters. The phenomena have been analysed qualitatively along with a Rayleigh scattering experiment of the corresponding cluster jet.     

Detonation simulations in supersonic flow under circumstances of injection and mixing

The unsteady, reactive Navier-Stokes equations with a detailed chemical mechanism of 11 species and 27 steps were employed to simulate the mixing, flame acceleration and deflagration-to-detonation transition (DDT) triggered by transverse jet obstacles. Results show that multiple transverse jet obstacles ejecting into the chamber can be used to activate DDT. But the occurrence of DDT is tremendously difficult in a non-uniform supersonic mixture so that it required several groups of transverse jets with increasing stagnation pressure. The jets introduce flow turbulence and produce oblique and bow shock waves even in an inhomogeneous supersonic mixture. The DDT is enhanced by multiple explosion points that are generated by the intense shock wave focusing of the leading flame front. It is found that the partial detonation front decouples into shock and flame, which is mainly caused by the fuel deficiency, nevertheless the decoupled shock wave is strong enough to reignite the mixture to detonation conditions. The resulting transverse wave leads to further mixing and burning of the downstream non-equilibrium chemical reaction, resulting in a high combustion temperature and intense flow instabilities. Additionally, the longitudinal and transverse gradients of the non-uniform supersonic mixture induce highly dynamic behaviors with sudden propagation speed increase and detonation front instabilities.     

Effect of small methane and monosilane additives on clustering in pulsed supersonic argon jets

Condensation of argon-methane and argon-monosilane gas mixtures in pulsed supersonic jets is studied experimentally. The signal intensities from monomer and cluster ions are studied as functions of the stagnation pressure, and the parameters characterizing the flow-condensation transition are determined. Features of methane clustering are considered. It is shown that silicon-carbon complexes may form in the ternary mixture.     

Equation of state of mixtures of simple fluids at high pressures

Recently Lee and Levesque have extended the Weeks-Chandler-Andersen pure fluid perturbation theory to mixtures and have compared the results to the Leonard-Henderson-Barker mixture theory. The results seem to favour the Leonard-Henderson-Barker theory. This and other previous comparisons of mixture theories have been mostly confined to the study of ‘zero pressure’ thermodynamic properties. In this paper we compare the Lee-Levesque, Leonard-Henderson-Barker and the van der Waals one-fluid theories to high pressure equation of state data for helium-xenon mixtures. This system is modelled by a binary mixture of Lennard-Jones fluids and the hard sphere reference system is characterized by the Grundke-Henderson hard sphere mixture radial distribution function. The Lee-Levesque theory compares favourably with experimental equation of state data up to pressures of 2000 atmospheres. The Leonard-Henderson-Barker and van der Waals one theories are satisfactory. Although the van der Waals one theory yields the poorest results, it does offer the advantage of having the greatest ease of computation.

Previous theoretical and Monte Carlo calculations of mixture properties have assumed the geometric mean rule for the mixed interaction energy parameter, ε ₁₂, with consequent disagreement with experimental results. We point out that ε ₁₂ can be determined from mixed second virial coefficient data and use such improved determinations of ε ₁₂. We show that this method yields significantly improved theoretical predictions.     

He-HF（DF，TF）碰撞体系分波截面的理论计算

运用质心变换-拟合方法,使用Murrell-Sorbie势能函数拟合在对称性匹配微扰理论下精确计算He-HF体系的相互作用能数据,得到了He原子与同位素分子HF（DF,TF）复合物的相互作用势的解析形式.完成了入射He原子能量从30 meV至120 meV时,He-HF（DF,TF）碰撞体系分波截面的密耦计算,获得了分波截面等信息,进一步讨论了分波截面的变化趋势及特征,并确定了He-HF（DF,TF）碰撞体系开始产生弹性和非弹性散射的有效相互作用范围. 关键词： He-HF（DF TF）复合物 密耦近似 分波截面 质心偏移     

二维范德瓦尔斯异质结构的制备与物性研究

二维范德瓦尔斯材料(可简称二维材料)已发展成为备受瞩目的材料大家族,而由其衍生的二维范德瓦尔斯异质结构的集成、性能及应用是现今凝聚态物理和材料科学领域的研究热点之一.二维范德瓦尔斯异质结构为探索丰富多彩的物理效应和新奇的物理现象,以及构建新型的自旋电子学器件提供了灵活而广阔的平台.本文从二维材料的转移技术着手,介绍二维范德瓦尔斯异质结构的构筑、性能及应用.首先,依据湿法转移和干法转移的分类,详细介绍二维范德瓦尔斯异质结构的制备技术,内容包括转移技术的通用设备、常用转移方法的具体操作步骤、三维操纵二维材料的方法、异质界面清洁.随后介绍二维范德瓦尔斯异质结构的性能和应用,重点介绍二维磁性范德瓦尔斯异质结构,并列举在二维范德瓦尔斯磁隧道结和摩尔超晶格领域的应用.因此,二维材料转移技术的发展和优化将进一步助力二维范德瓦尔斯异质结构在基础科学研究和实际应用上取得突破性的成果.     

二维范德瓦尔斯异质结构的制备与物性研究

二维范德瓦尔斯材料(可简称二维材料)已发展成为备受瞩目的材料大家族,而由其衍生的二维范德瓦尔斯异质结构的集成、性能及应用是现今凝聚态物理和材料科学领域的研究热点之一.二维范德瓦尔斯异质结构为探索丰富多彩的物理效应和新奇的物理现象,以及构建新型的自旋电子学器件提供了灵活而广阔的平台.本文从二维材料的转移技术着手,介绍二维范德瓦尔斯异质结构的构筑、性能及应用.首先,依据湿法转移和干法转移的分类,详细介绍二维范德瓦尔斯异质结构的制备技术,内容包括转移技术的通用设备、常用转移方法的具体操作步骤、三维操纵二维材料的方法、异质界面清洁.随后介绍二维范德瓦尔斯异质结构的性能和应用,重点介绍二维磁性范德瓦尔斯异质结构,并列举在二维范德瓦尔斯磁隧道结和摩尔超晶格领域的应用.因此,二维材料转移技术的发展和优化将进一步助力二维范德瓦尔斯异质结构在基础科学研究和实际应用上取得突破性的成果.     

Submillimeter-wave spectroscopy of the K = 2–1 subband of the Ne–CO complex

The pure rotational spectrum of the Ne–CO van der Waals complex has been measured in the frequency range of 208–230 GHz by using the Cologne supersonic jet spectrometer for terahertz applications (SuJeSTA). Eleven new transitions were assigned as belonging to two R- and two Q-branches of the K = 2–1 subband detected for the first time in the ground vibrational state of CO (ν_CO = 0). Improved molecular parameters of the Ne–CO complex were obtained which allowed for a sensitive test of the available intermolecular potential energy surfaces of the Ne–CO system.     

Absorption Measurements of Ar–COb-Type Rotational Transitions with a Supersonic Jet Millimeter-Wave Spectrometer

Pure rotationalb-type transitions of Ar–CO were observed in the frequency range from 70 to 103 GHz using a combination of millimeter-wave absorption spectroscopy with supersonic jet expansion. The millimeter-wave radiation was generated by precision tunable synthesizers equipped with backward wave oscillators. Altogether 14 transitions belonging toQandRbranches withK_a= 1 − 0 have been measured with an accuracy of about 50 kHz. Our results confirm the microwave–millimeter-wave double resonance experiments of Jäger and Gerry [J. Chem. Phys.102,3587–3592 (1995)] and demonstrate the sensitivity of the direct absorption technique for the detection of van der Waals clusters with a small dipole moment.     

Observation of a high lying van der Waals mode in the intermolecular potential of Ar-CO

A continuous two-dimensional jet expansion in combination with an infrared diode laser spectrometer has been used to record a new subband of the weakly bound complex Ar-CO in the 2168cm^?1 region. Twenty-two transitions were assigned to a thus far unobserved K _a = 0 van der Waals state at 36.765 cm^?l above the ground state. This is the highest van der Waals mode of Ar-CO reported so far. These high lying energy levels will provide a very sensitive test for future ab initio and Semiempirical potential energy surfaces.     

On the ultraviolet absorption of nitrous oxide and its van der Waals complexes

The possibility of simultaneous characterization of N₂O and N₂O van der Waals complexes in supersonic jet expansions is demonstrated for neat N₂O samples. Room temperature and jet-cooled spectra of the Rydberg transitions 3pπ¹Δ ←← X¹Σ⁺ and 3pσ¹Π ←← X¹Σ⁺ are presented. Theoretical calculations support the assignment of the Rydberg transitions used. For stagnation pressures above 2 bar, a hitherto unreported broad spectral feature at 84 650 cm⁻¹ is observed, where calculations predict absorption of the (N₂O)₂ dimer essentially due to excitation of the 4sσ and 3pπ Rydberg orbitals. Consequences for the use of N₂O as a precursor for O(¹D) atoms in reactive scattering experiments are discussed.     

Influence of complexation and solid environment on the vibrational coherence of DCl

The vibrational dynamics of DCl molecules embedded in different cryogenic matrices is studied by time resolved infrared Degenerate Four Wave Mixing experiments using the infrared free electron laser CLIO. The coherence behaviour of the D-Cl stretch in pure argon as well as in mixed argon/nitrogen van der Waals solids is investigated. Different interactions between the excited molecules and their environment are probed: the van der Waals interaction between the trapped molecules and the solid lattice and the interaction binding complexes trapped in the matrix (either the vdW interaction between DCl and nitrogen or weak H bonds in (DCl)_n clusters). The dependence of the dephasing time on the solid and on specific interactions is clearly observed.     

Attainable superheating of solutions of cryogenic liquids

The kinetics of spontaneous boiling-up of superheated binary solutions of cryogenic liquids is studied. Within the framework of the Kramers-Zeldovich method, an expression is obtained for the steady state rate of homogeneous nucleation in a solution that takes into account free-molecular and diffusion regimes of the substance supply to a growing bubble. Viscous and inertial forces are also taken into account in the study of the nucleus growth dynamics. The work of critical nucleus formation is determined within the framework of the Gibbs and van der Waals capillarity theories. The dependence of the surface tension of critical bubbles in the solution on their size is investigated. The temperature of attainable superheating and nucleation rates in superheated solutions of cryogenic liquids with complete or partial solubility of the components are determined by a method of lifetime measurement. The experiments were conducted in a wide range of pressures and solution concentrations. The measurement results are compared with the theory of homogeneous nucleation taking or not taking into account the size effect in nucleation. It has been found that, by taking into account the size dependence of the surface tension of a nucleus, better agreement between the theory and experiment is obtained. The boundary of essential instability of the solution, that is, the diffusion spinodal, is computed.     

The infrared spectrum of the Ar-CO complex Comprehensive analysis including van der Waals stretching and bending states

The infrared spectrum of the weakly-bound Ar-CO van der Waals complex in the 2150 cm^-1 region of the CO stretch has been studied using a continuous supersonic slit jet expansion coupled with a tunable laser spectrometer, and also with a cooled (57 K) long-path cell coupled with a Fourier transform spectrometer. Seven new subbands were observed, and previously observed bands were observed in greater detail. Four substates were thus identified for the first time, including the excited van der Waals stretching state, v ₃ = 1, and the excited bend, v ₂ = 1, within the ground CO stretching state, v _CO = 0. A comprehensive simultaneous analysis was made of all the existing infrared and microwave data on the complex for levels with K < 5, in order to obtain an accurate and self-consistent set of substate origins, rotational parameters, and centrifugal distortion parameters. A strong Coriolis interaction between K = 1 of the excited bend and K = 0 of the excited stretch was analysed in detail.     

Nonlinear dipole-dipole interactions and spectroscopic properties of van der waals complexes in the gas phase

We suggest a semiempirical approach to describing the influence of local nonlinear dipole-dipole interactions on the formation of van der Waals complexes of 1: 1 composition in the gas phase. Based on this approach, we quantitatively interpret the experimental data on the patterns of the shift in the electronic (complexes of a 3-aminophthalimide molecule with water and methanol molecules) and vibrational (complexes of a HCl molecule with acetone and acetonitrile molecules) absorption spectra attributable to the processes of complex formation. We confirm the conclusion that a nonlinear dipole-dipole interaction should be considered as one of the most important physical mechanisms that result in the association of molecules both in the gas phase and, under certain conditions, in the condensed state.     

Tunable diode laser spectroscopy of helium clusters

Helium clusters, He_N-X, containing a probe molecule, X, are studied by infrared spectroscopy for the size range N≈1∼100. Spectra are observed using a supersonic jet expansion and a tunable diode laser source operating in a rapid-scan (sweep integration) mode. The pulsed jet uses a dilute gas mixture of the probe molecule in helium, with relatively high backing pressures (5–50 bar), and a cooled (80–295 K) nozzle. Sensitivity is enhanced by multi-passing the laser beam through the jet with a toroidal mirror system. The clusters are larger than van der Waals dimers and trimers, but smaller than those encountered in the field of helium nanodroplets (N≈10³–10⁵). Furthermore, individual cluster sizes are resolved here, but not with nanodroplets, and infrared absorption is detected directly (change in transmitted laser intensity), rather than indirectly (change in cluster fragmentation). Trends in the spectra are described for five probe molecules, X=CO, SiH₄, OCS, N₂O, and CO₂. Superfluid effects dominate for clusters larger than N≈8. Notable results include the unexpected observation of broad oscillations in the effective rotational constants as a function of cluster size. PACS 33.20.Ea; 34.30.+h; 36.40.Mr; 42.55.Px     

Force spectroscopy in noncontact mode

We have analyzed the possibility of using noncontact scanning force microscopy (NCAFM) to detect variations in surface composition, i.e., to detect a ‘spectroscopic image' of the sample. This ability stems from the fact that the long-range forces, acting between the AFM tip and sample, depend on the composition of the AFM tip and sample. The long-range force can be magnetic, electrostatic, or van der Waals forces. Detection of the first two forces is presently used in scanning force microscopy technique, but van der Waals forces have not been used. We demonstrate that the recovery of spectroscopic image has a unique solution. Furthermore, the spectroscopic resolution can be as good as lateral one.