首页> 外文学位 >Isotope effects in gas-surface interactions: Quantum-state resolved studies of deuterium scattering from copper(100) and palladium(111).
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Isotope effects in gas-surface interactions: Quantum-state resolved studies of deuterium scattering from copper(100) and palladium(111).

机译:同位素在气体-表面相互作用中的作用:氘从铜(100)和钯(111)散射的量子态解析研究。

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摘要

State resolved experiments are presented for the interaction of D 2 and HD with Cu(100) and Pd(111). For this work, D2(v = 1, J = 2) molecules were scattered off of single crystal surfaces at near normal incidence. The reflected molecules were probed using quantum state specific spectroscopy. For D2 scattered from Cu(100) the survival probability and some transition probabilities were measured over a range of incident energies. The survival probability was found to be larger then that found previously for H2(v = 1) scattered from the same surface. For H2 some of the incident flux was unaccounted for and could possibly have been lost by dissociative adsorption. In contrast, D2 molecules which do not reflect elastically from the surface are accounted for in other transition channels for most energies. The differences found for D2 compared to previous work with H2 are discussed in terms of the lower zero point energy and smaller vibrational energy spacings of D2. D2 translational energy exchange was studied for several different scattering channels and interpreted using simple classical calculations. These calculations agreed well with both the elastic scattering channel as well as the rotational relaxation channel. For rotational excitation some energy was gained by the molecule from the surface. The survival probability was also measured for D2(v = 1) scattered from Pd(111) at one incident energy. Pd is very reactive for D2 dissociation and this survival probability was measured to be much smaller than that for H2(v = 1) under similar conditions. Vibrational relaxation channels were studied for D2 scattering from both Cu(100) and Pd(111). The vibrational relaxation was also found to be smaller than that measured for comparable channels for H2. The smaller survival probability and vibrational relaxation probability for D2 on Pd(111) cannot be easily accounted for by the difference in zero point energy and vibrational energy spacings. Measurements were also done to study the rotational excitation of HD molecules scattered from one reactive surface, Pd(111), and two inert surfaces, Cu(100) and Pd(111):H(D). These measurements showed similar amounts of rotational excitation for HD molecules after scattering from these different surfaces.
机译:针对D 2和HD与Cu(100)和Pd(111)的相互作用提出了国家解决的实验。对于这项工作,D2(v = 1,J = 2)分子以接近法线入射的速度从单晶表面散射开。使用量子态特异性光谱仪探测反射的分子。对于从Cu(100)散射的D2,在一定范围的入射能量范围内测量了生存概率和一些跃迁概率。发现生存概率要大于先前从同一表面散布的H2(v = 1)的生存概率。对于H2,一些入射通量是无法解释的,并且可能由于解离吸附而丢失。相反,对于大多数能量,在其他过渡通道中占不到从表面弹性反射的D2分子。与D2的先前工作相比,D2的差异在较低的零点能量和较小的D2振动能间隔方面进行了讨论。研究了D2平移能量交换的几种不同散射通道,并使用简单的经典计算对其进行了解释。这些计算与弹性散射通道以及旋转松弛通道都非常吻合。对于旋转激发,分子从表面获得了一些能量。还测量了在一种入射能量下从Pd(111)散射的D2(v = 1)的存活概率。 Pd对D2的解离反应非常强,在相似的条件下,该存活率比H2(v = 1)小得多。研究了振动弛豫通道中D2从Cu(100)和Pd(111)的散射。还发现振动弛豫小于H2的可比较通道的振动弛豫。 Pd(111)上D2的较小的生存概率和振动弛豫概率无法通过零点能量和振动能量间隔的差异轻易地解决。还进行了测量以研究从一个反应性表面Pd(111)和两个惰性表面Cu(100)和Pd(111):H(D)散射的HD分子的旋转激发。这些测量结果显示,在从这些不同表面散射后,HD分子的旋转激励量相似。

著录项

  • 作者

    Shackman, Leah Caitlin.;

  • 作者单位

    The University of Texas at Austin.;

  • 授予单位 The University of Texas at Austin.;
  • 学科 Physics Molecular.
  • 学位 Ph.D.
  • 年度 2004
  • 页码 109 p.
  • 总页数 109
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 分子物理学、原子物理学;
  • 关键词

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