High-throughput computation of Raman spectra from first principles.

ABSTRACT

Raman spectroscopy is a widely-used non-destructive material characterization method, which provides information about the vibrational modes of the material and therefore of its atomic structure and chemical composition. Interpretation of the spectra requires comparison to known references and to this end, experimental databases of spectra have been collected. Reference Raman spectra could also be simulated using atomistic first-principles methods but these are computationally demanding and thus the existing databases of computational Raman spectra are fairly small. In this work, we developed an optimized workflow to calculate the Raman spectra efficiently and taking full advantage of the phonon properties found in existing material databases. The workflow was benchmarked and validated by comparison to experiments and previous computational methods for select technologically relevant material systems. Using the workflow, we performed high-throughput calculations for a large set of materials (5099) belonging to many different material classes, and collected the results to a database. Finally, the contents of database are analyzed and the calculated spectra are shown to agree well with the experimental ones.