2D correlation analysis of the magnetic excitations in Raman spectra of HoMnO3

• 2D correlation analysis is performed on the temperature-dependent Raman spectra of HoMnO3 thin films.
• The power spectrum shows the strongest changes at 766 cm−1 especially below ∼70 K.
• The peaks at ∼336, 656, and 1304 cm-1 are negatively correlated with the 766 cm-1 peak.
• The depletion of the spectral weight at ∼336, 656, and 1304 cm-1 occurs at higher temperatures than the Neel temperature.

2D correlation analysis is performed on the temperature-dependent Raman spectra of HoMnO3 thin films. As the temperature of the HoMnO3 thin films decrease, the depletion of the spectral weight at 336, 656, and 1304 cm−1 occurs at higher temperatures than the increase of the intensity at 508, 766, and 945 cm−1 below ∼70 K, the Néel temperature. The power spectrum asserts that all the changes in the spectral weight are strongly correlated. Most of the temperature-induced spectral changes of HoMnO3 occur at lower temperature than 70 K, while there is slight depletion of the spectral weight at 336, 656, and 1304 cm−1 even at higher temperature than 70 K. PCA scores and loading vectors plots also support these 2D correlation results. Our 2D correlation analysis supports the existence of the short range spin correlations between Mn sites in HoMnO3 even above the Néel temperature.