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In the study, we prepared and compared sub-5 nm nanodiamonds (ND) prepared by detonation and high-pressure high-temperature (HPHT) synthesis. The work contributed to a better understanding of the Raman spectra of nanodiamonds and their size dependence down to 3 nm and opened up new possibilities in determining their size using low-frequency "breathing" modes, which were detected in nanodiamonds for the first time.