Though
most of the recently developed molecular ferroelectrics
(MFs) exhibit excellent ferroelectric properties, the practical applications
are still impeded by the limited polarization axes, poor processing
capability for a high-quality thin film, and the incompatibility with
matured lithography techniques for microelectronics. Here, we successfully
demonstrated MF-based single-crystalline microdevice arrays using
a lithography-compatible, solution-processed strategy that can avoid
the above-mentioned obstacles at one time, i.e., dewetting-assisted
patterning crystallization strategy. As a protype, uniform and well-aligned
single-crystalline thin-film arrays of multiaxial MF [3-oxoquinuclidinium]ClO4 ([3-O-Q]ClO4) are prepared. Owing to the well-aligned
crystallographic orientation and polarization direction, the obtained
single-crystalline nonvolatile memory (NVM) arrays can exhibit an
ultralow operating voltage of ∼1.6 V and long endurance cycles
of 106, which are superior to other organic NVM devices.
This work implies a promising route to high-density single-crystalline
memory arrays for data storage, especially for low-cost flexible electronics.