A new phenomenon of structural reorganization is discovered and characterized
for a gold-carbon system by in-situ atomic-resolution imaging at temperatures
up to 1300 K. Here, a graphene sheet serves in three ways, as a quasi
transparent substrate for aberration-corrected high-resolution transmission
electron microscopy, as an in-situ heater, and as carbon supplier. The sheet
has been decorated with gold nanoislands beforehand. During electron irradiation
at 80 kV and at elevated temperatures, the accumulation of gold atoms
has been observed on defective graphene sites or edges as well as at the facets
of gold nanocrystals. Both resulted in clustering, forming unusual crystalline
structures. Their lattice parameters and surface termination differ significantly
from standard gold nanocrystals. The experimental data, supported by electron
energy loss spectroscopy and density-functional theory calculations, suggests
that isolated gold and carbon atoms form – under conditions of heat
and electron irradiation – a novel type of compound crystal, Au-C in
zincblende structure. The novel material is metastable, but surprisingly robust,
even under annealing condition.