Surface chemistry investigations of 1,1-dimethylhydrazine (DMHy) and dimethylethylamine alane (DMEAA) on Si(100) and DMHy on aluminum were conducted using X-ray photoelectron spectroscopy (XPS) and temperature programmed desorption (TPD). DMHy and DMEAA both showed adsorption and decomposition behavior under certain conditions on Si(100) that was promising for aluminum nitride (AlN) deposition. For DMHy, a temperature window existed between approximately 600-720 K where adsorption of only NHx (x = 0-2) species occurred. DMEAA adsorption was self-limiting below approximately 420 K with the predominant species at 420 K being AlHy (y = 0-3). DMHy also showed promising adsorption and decomposition behavior under certain conditions on an aluminum film deposited on Si(100). At 660 K, nitridation of aluminum is observed with carbon contamination at the noise level. Using these results, a growth strategy was developed for the deposition of AlN thin films at low temperature employing a temperature modulated atomic layer growth (ALG) process. Exposure temperatures of 420 K for the DMEAA and 660 K for DMHy were selected. The growth strategy was implemented in an investigation of the first few cycles of ALG, and AlN was successfully deposited with carbon contamination at the noise level. No distinct advantage was observed for beginning the cycle with either DMEAA or DMHy. In either sequence, the growth proceeded primarily through the dehydrogenation of AlHyNHx, where regeneration of these species occurred in each cycle. This was also found to be the primary mechanism for ALG of AlN under similar processing conditions using DMEAA and ammonia.