In
this study, we investigate the thermochemical stability of graphene
on the GaN substrate for metal–organic chemical vapor deposition
(MOCVD)-based remote epitaxy. Despite excellent physical properties
of GaN, making it a compelling choice for high-performance electronic
and light-emitting device applications, the challenge of thermochemical
decomposition of graphene on a GaN substrate at high temperatures
has obstructed the achievement of remote homoepitaxy via MOCVD. Our
research uncovers an unexpected stability of graphene on N-polar GaN,
thereby enabling the MOCVD-based remote homoepitaxy of N-polar GaN.
Our comparative analysis of N- and Ga-polar GaN substrates reveals
markedly different outcomes: while a graphene/N-polar GaN substrate
produces releasable microcrystals (μCs), a graphene/Ga-polar
GaN substrate yields nonreleasable thin films. We attribute this discrepancy
to the polarity-dependent thermochemical stability of graphene on
the GaN substrate and its subsequent reaction with hydrogen. Evidence
obtained from Raman spectroscopy, electron microscopic analyses, and
overlayer delamination points to a pronounced thermochemical stability
of graphene on N-polar GaN during MOCVD-based remote homoepitaxy.
Molecular dynamics simulations, corroborated by experimental data,
further substantiate that the thermochemical stability of graphene
is reliant on the polarity of GaN, due to different reactions with
hydrogen at high temperatures. Based on the N-polar remote homoepitaxy
of μCs, the practical application of our findings was demonstrated
in fabrication of flexible light-emitting diodes composed of p–n
junction μCs with InGaN heterostructures.