Search for the quantum delocalization of hydrogen on solid surfaces

氢的动力学作为最亮的原子在自然中是固有的量子力学，并且它在金属表面上的吸附状态已经被提议在表面上被分离。当前项目的目标是揭示氢吸收在纯金属和合金表面上的量子分离的可能性。为了完成这一任务，我们已经开发了一种新的零点振动光谱学技术，利用^1H（^<15>N，αy）^<12>C共振核反应。自从传统的光谱技术衡量了从地面到第一兴奋的状态的兴奋，振动地面状态的特征仍然没有经过实验的明确日期。与此零点振动光谱学与其他实验和理论方法组合在一起，我们找到了以下结果：1。H在硅上（111）的零点振动能量在永久和平行方向分别为123.4±4.6和44.6±6.2 meV，因此，它们与谐波潜力一致。Pt（111）的零点能量-H是80.8 A 3.9和62.1$A 6.0 meV，用于永久性和并行方向，因此，该指标表明拉伸模式是和谐的，而弯曲模式是强烈的不和谐的。H在Pt上的潜在能量表面（111）从第一原则的电子结构计算是强烈的非谐波性的，它与实验结果的质量一致。4. H在Pt（lll）上吸收的零点能量-2x2-Sn为75和57 meV，用于Perspecial和Parallel Directions，与Pt（111）-H.

Dynamics of hydrogen as the lightest atom is inherently quantum-mechanical in nature, and its adsorption state on a metal surface has been proposed to be delocalized over the surface. The purpose of the present project is to explore the possibility of quantum delocalization of hydrogen adsorbed on pure metal and alloy surfaces. In order to achieve this, we have developed a new technique of zero-point vibrational spectroscopy using the ^1H(^<15>N,αy)^<12>C resonance nuclear reaction. Since the conventional spectroscopic techniques measure the excitation from the ground to the first-excited state, characteristics of the vibrational ground state are not yet clarified experimentally to date. With this zero-point vibrational spectroscopy combined with other experimental and theoretical methods, we have found the following results:1. The zero-point vibrational energy of H on Si(111) in the perpendicular and parallel directions is 123.4±4.6 and 44.6±6.2 meV, respectively, which are consistent with harmonic potentials.2. The zero-point energy obtained for Pt(111)-H is 80.8ア3.9 and 62.1$ア6.0 meV for perpendicular and parallel directions, respectively, which indicate that the stretching mode is harmonic, while the bending mode is strongly anharmonic.3. The potential energy surfaces for H on Pt(111) obtained from first-principles electronic structure calculation are strongly anharmonic, which are qualitatively consistent with the experimental results. 4. The zero-point energy of H adsorbed on Pt(lll)-2x2-Sn is 75 and 57 meV for perpendicular and parallel directions, which are similar to the values measured for Pt(111)-H.