Aggarwal, R. L.Farrar, L. W.Saikin, S. K.Andrade, X.Aspuru-Guzik, AlanPolla, D. L.2014-03-122012Aggarwal, R. L., L. W. Farrar, S. K. Saikin, X. Andrade, Alan Aspuru-Guzik, and D. L. Polla. 2012. “Measurement of the Absolute Raman Cross Section of the Optical Phonons in Type Ia Natural Diamond.” Solid State Communications 152 (3) (February): 204–209. doi:10.1016/j.ssc.2011.11.005. http://dx.doi.org/10.1016/j.ssc.2011.11.005.0038-10981879-2766http://nrs.harvard.edu/urn-3:HUL.InstRepos:11880473The absolute Raman cross section \(\sigma_{RS}\)of the first-order \(1332-cm^{−1}\) optical phonons in type Ia natural diamond was measured using 785- and 1064-nm pump lasers for the excitation of Raman scattering. A small temperature-controlled blackbody was used for the signal calibration of the 785- and 1064-nm Raman systems. Measurements were made with a 0.9-mm thick (111) natural diamond sample. Values of \(2.7\pm0.6×10^{−29}\) and \(0.95\pm0.2×10^{−29} cm^2\) per carbon atom were determined for \(\sigma_{RS}\) for 785- and 1064-nm excitation, respectively. The corresponding values of the Raman scattering efficiency S are \(3.8\pm0.8×10^{−7}\) and \(1.3\pm0.3×10^{−7} cm^{−1} sr^{−1}\). The values of the Raman polarizability |d| for 785-, and 1064-nm excitation are \(6.8\pm0.7×10^{−16}\) and \(8.1\pm0.8×10^{−16} cm^2\), respectively. Our measured values of |d| are larger than the previously measured values of \(4.4\pm0.3×10^{−16}\) and \(4.6\pm0.7×10^{−16} cm^2\) using 514.5- and 694-nm excitation, respectively. |d| vs. excitation photon energy was computed for the range from 1.0 eV (1240 nm) to 4.0 eV (310 nm) using time-dependent density functional theory. The computed values of \(5.8×10^{−16}\) and \(5.3×10^{−16} cm^2\) for 514.4- and 694-nm excitation, respectively, are larger than the corresponding measured values of |d|. The computed values of \(5.2×10^{−16}\), and \(5.0×10^{−16} cm^2\) for 785- and 1064-nm excitation are smaller than the corresponding values of |d| measured in this work. The computed value of |d| in the static limit is \(4.7×10^{−16} cm^2\). Modification of |d| due to IaA and IaB defects, computed for a 64-atom supercell, is less than 5%.en-USsemiconductorsphotonsinelastic light scatteringJournal Article10.1016/j.ssc.2011.11.005