Towards Nanoscale and Element-Specific Lattice Temperature Measurements using Core-Loss Electron Energy-Loss Spectroscopy

Measuring nanoscale local temperatures, particularly in vertically integrated and multi-component systems, remains challenging. Spectroscopic techniques like X-ray absorption and core-loss electron energy-loss spectroscopy (EELS) are sensitive to lattice temperature, but understanding thermal effects is nontrivial. This work explores the potential for nanoscale and element-specific core-loss thermometry by comparing the Si L2,3 edge's temperature-dependent redshift against plasmon energy expansion thermometry (PEET) in a scanning TEM. Using density functional theory (DFT), time-dependent DFT, and the Bethe-Salpeter equation, we ab initio model both the Si L2,3 and plasmon redshift. We find that the core-loss redshift is due to bandgap reduction from electron-phonon renormalization. Our results indicate that despite lower core-loss signal intensity and thus accuracy compared to PEET, core-loss thermometry still has important advantages. Specifically, we show that the Varshni equation easily interprets the core-loss redshift, which avoids plasmon spectral convolution for PEET in complex materials. We also find that core-loss thermometry is more accurate than PEET at modeling thermal lattice expansion unless the temperature-dependent effective mass and dielectric constant are known. Furthermore, core-loss thermometry has the potential to measure nanoscale heating in multi-component materials and stacked interfaces with elemental specificity at length scales smaller than the plasmon's wavefunction.
Comment: 33 pages, 5 main text figures, 1 table