Well-ordered spin
arrays are highly desirable for next-generation molecule-based magnetic devices,
and yet its synthetic method remains a challenging task. Herein, we demonstrate
the realization of two-dimensional supramolecular spin arrays on surfaces via
halogen-bonding molecular self-assembly. A bromine-terminal perchlorotriphenymethyl
radical with net carbon spin was synthesized and deposited on Au(111) to
achieve two-dimensional supramolecular spin arrays. By taking advantage of the
diversity of halogen bonds, five supramolecular spin arrays are presented with
ultrahigh spin densities (up to the value
of 3 × 10<sup>13</sup> spins at the
size of a flash drive), as probed by low-temperature scanning tunneling
microscopy at the single-molecule level. First principle calculations verify
that the formation of three distinct types of halogen bonds can be used to
tailor supramolecular phases via molecular coverage and annealing temperature.
Our work demonstrates supramolecular self-assembly as a promising method to
engineering 2D spin arrays for potential application in magnetic devices.
Combining halogen bonding and chirality in a two-dimensional organic metal (EDT-TTF-I2)2(D-camphorsulfonate)·H2O
