Improved midgap recombination lifetimes in GaN crystals grown by the low-pressure acidic ammonothermal method

To investigate the carrier recombination processes in GaN crystals grown by the low-pressure acidic ammonothermal (LPAAT) method, the photoluminescence (PL) spectra and PL lifetimes of LPAAT GaN crystals grown on acidic ammonothermal (AAT) GaN seed crystals were correlated with the growth polarity and species/concentration of point defects. The PL spectra of LPAAT GaN grown toward the (000 1) direction (-c region), which provided the highest growth rate, exhibited a predominant near-band edge (NBE) emission. Neither bandgap narrowing nor Burstein-Moss shifts due to high concentration residual impurities were observed in the NBE emissions, indicating higher purity than the previously reported AAT GaN crystals. In addition, strain-induced energy shift or energy broadening of excitonic emission peaks was not observed, indicating excellent crystal coherency. Because of the reduced concentration of midgap recombination centers, a record-long room-temperature PL lifetime for the NBE emission of ammonothermal GaN (40 ps) was obtained from the -c region. Meanwhile, the PL spectra also exhibited the yellow and blue luminescence bands originating from particular deep-state radiative recombination centers. The major vacancy-type defects acting as midgap recombination centers are identified as vacancy complexes comprising a Ga vacancy (V-Ga) and a few N vacancies (V-N), namely, V-Ga(V-N)(n) buried by H and/or O, where n is an integer. Further reduction of such defect complexes will allow less compensated stable carrier concentration in the LPAAT GaN crystals.