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1.
The differential cross section for the H + D(2) --> HD + D reaction has been measured using a technique called reaction product imaging. In this experiment, a photolytically produced beam of hydrogen (H) atoms crossed a beam of cold deuterium (D(2)) molecules. Product D atoms were ionized at the intersection of the two particle beams and accelerated toward a position-sensitive detector. The ion images appearing on the detector are two-dimensional projections of the three-dimensional velocity distribution of the D atom products. The reaction was studied at nominal center-of-mass collision energies of 0.54 and 1.29 electron volts. At the lower collision energy, the measured differential cross section for D atom production, summed over all final states of the HD(v,J) product, is in good agreement with recent quasi-classical trajectory calculations. At the higher collision energy, the agreement between the theoretical predictions and experimental results is less favorable.  相似文献   

2.
Flynn GW 《Science (New York, N.Y.)》1989,246(4933):1009-1015
Very high resolution lasers allow spectroscopic pictures to be taken following a collision between two molecular reactants. The features of these "pictures" are the electronic, vibrational, rotational, and translational motions of the atomic particles, which relate the quantum states of the reactants to the quantum states of the products. Such state-to-state kinetic information can be used to test the shape and nature of the interaction potential that controls the collision process. The potential itself is akin to a map of the terrain through mountains and valleys where elevation is a measure of energy instead of height. Accurate mapping of this potential surface leads to an understanding of the forces which control rates and mechanisms of chemical reactions. The application of four different advanced laser techniques to the study of collisions between "hot" hydrogen(H) atoms and carbon dioxide(CO(2)) molecules has provided a wealth of information about both reactive and nonreactive collisions for this system. The availability of data for rotationally, vibrationally, and translationally inelastic excitation of CO(2) by H atoms, when compared with data for reactive events producing OH + CO, provides insights into the dynamics of collisions between H and CO(2), and illustrates the future promise of these powerful techniques for elucidating features of potential energy surfaces.  相似文献   

3.
Interactions between particles can be strongly altered by their environment. We demonstrate a technique for modifying interactions between ultracold atoms by dressing the bare atomic states with light, creating an effective interaction of vastly increased range that scatters states of finite relative angular momentum at collision energies where only s-wave scattering would normally be expected. We collided two optically dressed neutral atomic Bose-Einstein condensates with equal, and opposite, momenta and observed that the usual s-wave distribution of scattered atoms was altered by the appearance of d- and g-wave contributions. This technique is expected to enable quantum simulation of exotic systems, including those predicted to support Majorana fermions.  相似文献   

4.
The preferred sense of product molecule rotation (clockwise or counterclockwise) in a bimolecular collision system has been measured. Rotationally inelastic collisions of nitric oxide (NO) molecules with Ar atoms were studied by combining crossed molecular beams, circularly polarized resonant multiphoton ionization probing, and velocity-mapped ion imaging detection. The observed sense of NO product rotation varies with deflection angle and is a strong function of the NO final rotational state. The largest preferences for sense of rotation are observed at the highest kinematically allowed product rotational states; for lower rotational states, the variation with deflection angle becomes oscillatory. Quantum calculations on the most recently reported NO-Ar potential give good agreement with the observed oscillation patterns in the sense of rotation.  相似文献   

5.
Riboflavin and 12 of its derivatives have been shown to form solvated electrons under ultraviolet irradiation (253.7 nanometers) in various water-methanol solvent mixtures. The highest quantum yield of solvated electrons (about 0.03) was obtained for flavins containing tyrosine on a side chain in the isoalloxazine N-3 or N-10 position. The splitting of hydrogen atoms from excited flavin molecules was also observed. From the results presented here, it can be determined that the semiquinone transients are formed not only by way of the flavin triplet, as usually suggested, but also by the attack of the electrons and hydrogen atoms on flavin molecules in the ground state. This is important, because the flavin radicals remaining after the electron-ejection or hydrogen-splitting processes must also be considered in the subsequent reaction mechanisms. The electron-ejection process from electronically excited flavins has important implications in the photobiology of these compounds.  相似文献   

6.
The spatially dependent de-excitation of a beam of metastable argon atoms, traveling through an optical standing wave, produced a periodic array of localized metastable atoms with position and momentum spreads approaching the limit stated by the Heisenberg uncertainty principle. Silicon and silicon dioxide substrates placed in the path of the atom beam were patterned by the metastable atoms. The de-excitation of metastable atoms upon collision with the surface promoted the deposition of a carbonaceous film from a vapor-phase hydrocarbon precursor. The resulting patterns were imaged both directly and after chemical etching. Thus, quantum-mechanical steady-state atom distributions can be used for sub-0.1-micrometer lithography.  相似文献   

7.
We report the observation of unusually strong and systematic changes in the electron transport in metallic single-walled carbon nanotubes that are undergoing collisions with inert gas atoms or small molecules. At fixed gas temperature and pressure, changes in the resistance and thermopower of thin films are observed that scale as roughly M(1/3), where M is the mass of the colliding gas species (He, Ar, Ne, Kr, Xe, CH4, and N2). Results of molecular dynamics simulations are also presented that show that the maximum deformation of the tube wall upon collision and the total energy transfer between the colliding atom and the nanotube also exhibit a roughly M(1/3) dependence. It appears that the transient deformation (or dent) in the tube wall may provide a previously unknown scattering mechanism needed to explain the atom collision-induced changes in the electrical transport.  相似文献   

8.
The existence of synthetic macrocyclic molecules with hydrophilic cavities containing multiple binding atoms and with hydrophobic exteriors gives rise to extraordinary possibilities with respect to the design and synthesis of molecules with specific cation and anion binding properties. The preparation of many new macrocyclic compounds has recently been reported, but few practical applications for them have been suggested. From the information available, it is becoming clear that it should be possible to synthesize macrocycles that will have specified, or selected, ion binding properties. Cavity size can be varied to accommodate only those cations or anions within a specified narrow band of sizes. Numbers and types of coordinating atoms can be chosen to give essentially electrostatic or covalent bonding or a combination of the two in a metalmacrocycle complex. The metal ligand bond appears to be predominantly ionic in the case of the cyclic polyethers but the covalent character increases on substitution of sulfur or nitrogen for oxygen donor atoms. The essential hydrophobic exteriors of the macrocycles can be modified by the addition of side chains and groups to facilitate the solution of anions and cations in organic solvents. The structures of many macrocycles can be made to approximate naturally occurring molecules, that is, cyclic polyethers similar to macrocyclic antibiotics of the valinomycin and nonactin types and cyclic polyamines similar to porphyrins. Macrocycles are also useful as model compounds for the study of metal interactions with biological systems. The synthetic macrocycles thus represent an intriguing new area of coordination chemistry, the systematic study of which should lead to many interesting and useful chemical applications in the field of metal complexation in solution.  相似文献   

9.
Narten AH  Hahn RL 《Science (New York, N.Y.)》1982,217(4566):1249-1250
Much information on ionic solvation in electrolyte solutions has been inferred from macroscopic thermodynamic and transport properties and from spectroscopy. These ion-water interactions can now be probed directly and unambiguously by neutron diffraction. Such measurements have been done with neodymium trichloride solutions in heavy water that are identical in every respect except the isotopic state of the neodymium ions; these experiments yield in a straightforward manner the distribution of oxygen and deuterium atoms from the water molecules in the first hydration sphere of the neodymium ion. Each ion is surrounded by 8.6 oxygen atoms at a distance of 2.48 angstroms and 16.7 deuterium atoms at 3.13 angstroms indicating a well-defined first hydration sphere of water molecules, the deuterium atoms pointing away from the cation.  相似文献   

10.
Chemistry resulting in the formation of large carbon-bearing molecules and dust in the interior of an expanding supernova was explored, and the equations governing their abundances were solved numerically. Carbon dust condenses from initially gaseous carbon and oxygen atoms because energetic electrons produced by radioactivity in the supernova cause dissociation of the carbon monoxide molecules, which would otherwise form and limit the supply of carbon atoms. The resulting free carbon atoms enable carbon dust to grow faster by carbon association than the rate at which the dust can be destroyed by oxidation. The origin of presolar micrometer-sized carbon solids that are found in meteorites is thereby altered.  相似文献   

11.
Understanding how molecules can restructure the surfaces of heterogeneous catalysts under reaction conditions requires methods that can visualize atoms in real space and time. We applied a newly developed aberration-corrected environmental transmission electron microscopy to show that adsorbed carbon monoxide (CO) molecules caused the {100} facets of a gold nanoparticle to reconstruct during CO oxidation at room temperature. The CO molecules adsorbed at the on-top sites of gold atoms in the reconstructed surface, and the energetic favorability of this reconstructed structure was confirmed by ab initio calculations and image simulations. This atomic-scale visualizing method can be applied to help elucidate reaction mechanisms in heterogeneous catalysis.  相似文献   

12.
The electronic connection of single molecules to nanoelectrodes on a surface is a basic, unsolved problem in the emerging field of molecular nanoelectronics. By means of variable temperature scanning tunneling microscopy, we show that an organic molecule (C90H98), known as the Lander, can cause the rearrangement of atoms on a Cu(110) surface. These molecules act as templates accommodating metal atoms at the step edges of the copper substrate, forming metallic nanostructures (0.75 nanometers wide and 1.85 nanometers long) that are adapted to the dimensions of the molecule.  相似文献   

13.
An unusual distribution of particle sizes has been observed following the formation of molybdenum particles by argon ion sputtering. Many of the molybdenum particles produced by sputtering at the threshold pressure for particle formation in the vapor appear to be single crystalline cubes. There are two prominent peaks in the edge length distribution of the cubes, one centered at 4.8 nanometers with a halfwidth of approximately 1.3 nanometers and the other at 17.5 nanometers. The peak for the larger cubes is approximately square and has a total width of 7.0 nanometers. Evidence is presented that the larger cubes are formed by a 3 by 3 by 3 self-arrangement of the smaller cubes, which contain approximately 7000 atoms. Self-arrangement in inorganic structures is normally only observed when the building blocks are atoms, molecules, or clusters of less than 100 atoms.  相似文献   

14.
Recent developments in ion-scattering spectrometry have led to a surface crystallography that is sensitive to all elements, including hydrogen. Time-of-flight techniques for the detection of atoms scattered and recoiled from surfaces in simple collision sequences, together with calculations of shadowing and blocking cones, can be used to make direct measurements of interatomic spacings and adsorption sites within an accuracy of 相似文献   

15.
An ultracold molecular quantum gas is created by application of a magnetic field sweep across a Feshbach resonance to a Bose-Einstein condensate of cesium atoms. The ability to separate the molecules from the atoms permits direct imaging of the pure molecular sample. Magnetic levitation enables study of the dynamics of the ensemble on extended time scales. We measured ultralow expansion energies in the range of a few nanokelvin for a sample of 3000 molecules. Our observations are consistent with the presence of a macroscopic molecular matter wave.  相似文献   

16.
Twenty years ago the first scanning probe instrument, the scanning tunneling microscope, opened up new realms for our perception of the world. Atoms that had been abstract entities were now real objects, clearly seen as distinguishable individuals at particular positions in space. A whole family of scanning probe instruments has been developed, extending our sense of touching to the scale of atoms and molecules. Such instruments are especially useful for imaging of biomolecular structures because they can produce topographic images with submolecular resolution in aqueous environments. Instruments with increased imaging rates, lower probe-specimen force interactions, and probe configurations not constrained to planar surfaces are being developed, with the goal of imaging processes at the single-molecule level-not only at surfaces but also within three-dimensional volumes-in real time.  相似文献   

17.
The prospect of manipulating matter on the atomic scale has fascinated scientists for decades. This fascination may be motivated by scientific and technological opportunities, or from a curiosity about the consequences of being able to place atoms in a particular location. Advances in scanning tunneling microscopy have made this prospect a reality; single atoms can be placed at selected positions and structures can be built to a particular design atom-by-atom. Atoms and molecules may be manipulated in a variety of ways by using the interactions present in the tunnel junction of a scanning tunneling microscope. Some of these recent developments and some of the possible uses of atomic and molecular manipulation as a tool for science are discussed.  相似文献   

18.
The methods producing cold molecules from cold atoms tend to leave molecular ensembles with substantial residual internal energy. For instance, cesium molecules initially formed via photoassociation of cold cesium atoms are in several vibrational levels nu of the electronic ground state. We applied a broadband femtosecond laser that redistributes the vibrational population in the ground state via a few electronic excitation/spontaneous emission cycles. The laser pulses are shaped to remove the excitation frequency band of the nu = 0 level, preventing re-excitation from that state. We observed a fast and efficient accumulation ( approximately 70% of the initially detected molecules) in the lowest vibrational level, nu = 0, of the singlet electronic state. The validity of this incoherent depopulation pumping method is very general and opens exciting prospects for laser cooling and manipulation of molecules.  相似文献   

19.
Scanning tunneling microscopy and monoenergetic molecular beams have been used to obtain real-space atomic images of the competition between abstractive and dissociative chemisorption. The size distribution of Si-F adsorbates on the Si(111)-(7x7) surface was examined as a function of the incident translational energy of the F(2) molecules. For F(2) molecules with 0.03 electron volt of incident energy, the dominant adsorbate sites were isolated Si-F species. As an F(2) molecule with low translational energy collides with the surface, abstraction occurs and only one of the F atoms chemisorbs; the other is ejected into the gas phase. For F(2) molecules with 0.27 electron volt of incident energy, many adjacent Si-F adsorbates (dimer sites) were observed because F(2) molecules with high translational energy collide with the surface and chemisorb dissociatively so that both F atoms react to form adjacent Si-F adsorbates. For halogens with very high incident energy (0.5-electron volt Br(2)), dissociative chemisorption is the dominant adsorption mechanism and dimer sites account for nearly all adsorbates.  相似文献   

20.
A carbon allotrope based on "sp" hybridization containing alternating triple and single bonds (an acetylenic or linear carbon allotrope) has been prepared. Studies of small (8 to 28 carbon atoms) acetylenic carbon model compounds show that such species are quite stable (130 degrees to 140 degrees C) provided that nonreactive terminal groups or end caps (such as tert-butyl or trifluoromethyl) are present to stabilize these molecules against further reactions. In the presence of end capping groups, laser-based synthetic techniques similar to those normally used to generate fullerenes, produce thermally stable acetylenic carbon species capped with trifluoromethyl or nitrile groups with chain lengths in excess of 300 carbon atoms. Under these conditions, only a negligible quantity of fullerenes is produced. Acetylenic carbon compounds are not particularly moisture or oxygen sensitive but are moderately light sensitive.  相似文献   

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