In 2011, we proposed a novel magnetron sputtering method. It involved the use of pulsed injection of working gas for the initiation and control of gas discharge during reactive sputtering of an AlN layer (Gas Injection Magnetron Sputtering — GIMS). Unfortunately, the presence of Al-Al bonds was found in XPS spectra of the AlN layers deposited by GIMS onto Si substrate. Our studies reported in this paper proved that the synchronization of time duration of the pulses of both gas injection and applied voltage, resulted in the elimination of Al-Al bonds in the AlN layer material, which was confirmed by the XPS studies. In our opinion the most probable reason of Al-Al bonds in the AlN layers deposited by the GIMS was the self-sputtering of the Al target in the final stage of the pulsed discharge.