Transient vibrational mode renormalization in dipole‐coupled adsorbates at surfaces

摘要: Dipole interactions among adsorbates at solid surfaces can strongly affect the intensities, positions, and line shapes of vibrational resonances. An understanding these effects has been important in spectroscopic investigations surface structure. Here, adsorbate dipole are shown to create transient spectral intensity resonance position changes when modes excited ultrafast pump–probe laser experiments surfaces. The occur because intensities positions resonances dependent upon magnitude interadsorbate interactions, excitation modifies effective oscillator dynamic dipoles that determine interactions. different (renormalized) after change coupling. account for unusual transients observed recent on Si–H stretching vicinal H/Si(111) [K. Kuhnke, M. Morin, P. Jakob, N. J. Levinos, Y. Chabal, A. L. Harris, Chem. Phys. 99, 6114 (1993)]. predicted serve as a novel time‐resolved probe strength dipolar layers, will arise any layer where large enough cause borrowing adsorption sites or adsorbates.