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The enhancement of spin-phonon coupling in gadolinium filled double walledcarbon nanotubes (GdCl3@DWNTs) is demonstrated through temperature dependentmagnetrometry and polarized Raman Spectroscopy (PRS). Temperature dependentsusceptibility measurements show that the GdCl3@DWNTs undergo asuperparamagnetic phase transion at temperatures below 100 K with a blockingtemperature at approximately 47 K. From the temperature dependent PRS, it isobserved that a distinct phonon hardening occurs for the G-band modes attemperatures close to the onset of the superparamagentic phase. This is incontract to pristine DWNTs where phonon modes saturates to a constant frequencyat low temperatures. The abrupt increase in phonon frequency is indicative of apronounced spin-phonon coupling. The enhanced coupling in the GdCl3@DWNTs isbelieved to occur due to resonance between nanotube phonon mode and spin flipfrequency as temperature decreases.

Observation of spin-phonon coupling in GdCl3 filled carbon nanotubes