Calculating the frequencies and intensities of strongly anharmonic modes of adsorbates on surfaces: A low-cost but accurate computational approach
| Autor: | Chris Hooley, Neville V. Richardson, Jan P. Götze, José A. Garrido Torres, Renald Schaub, Federico Grillo, Herbert A. Früchtl |
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| Přispěvatelé: | Scottish Funding Council, University of St Andrews. School of Chemistry, University of St Andrews. EaSTCHEM, University of St Andrews. Centre for Designer Quantum Materials, University of St Andrews. Condensed Matter Physics, University of St Andrews. School of Physics and Astronomy |
| Rok vydání: | 2019 |
| Předmět: |
Terephthalic acid
Materials science Computation Electron energy loss spectroscopy Anharmonicity NDAS 02 engineering and technology QD Chemistry 021001 nanoscience & nanotechnology 01 natural sciences Molecular physics Vibration chemistry.chemical_compound QC Physics chemistry Molecular vibration 0103 physical sciences QD Physics::Chemical Physics Perturbation theory 010306 general physics 0210 nano-technology Benzene QC |
| Zdroj: | Physical Review B. 100 |
| ISSN: | 2469-9969 2469-9950 |
| DOI: | 10.1103/physrevb.100.035433 |
| Popis: | Funding: Scottish Funding Council (through EaStCHEM and SRD-Grant HR07003) and from EPSRC (PhD studentship for JAGT, EP/M506631/1). We present a new method for calculating the frequencies and intensities of the vibrational modes of adsorbates on surfaces. Our method is based on density functional perturbation theory (DFPT) and provides accurate estimates of the vibrational intensities even when the vibrations are strongly anharmonic. Furthermore, it does so at a negligible additional computation cost compared to conventional DFPT calculation. We illustrate our method by calculating the vibrational spectra of three example systems — ethylidyne on Rh(111), benzene on Rh(111) coadsorbed with CO, and terephthalic acid (TPA) on Cu(100) — and comparing them to experimental measurements performed using High-Resolution Electron Energy Loss Spectroscopy (HREELS). We find excellent agreement between our predictions and the experimentally measured frequencies and intensities in all three cases. Postprint Postprint |
| Databáze: | OpenAIRE |
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