Rational Modification of Small Molecules with High Device Reproducibility Induced by Improved Interfacial Contact through Intermolecular Hydrogen Bonds.

The interfacial contact between the semiconductor and the electrode can effectively affect the device performance through the penetration of metal atoms in semiconductors from the grain boundaries. Thus, how to design a novel molecule with few grain boundaries, namely, large grain size, in solid state is an important task to achieve excellent memory device with high reproducibility. Intermolecular hydrogen-bonding interaction has been proved to be a powerful driving force for molecules assembling into large crystalline aggregates. In this work, the molecular terminals with different numbers of electron-deficient imine (C═N) nitrogen atoms are designed to investigate the effect of hydrogen-bonding interaction on molecular crystalline grains and interfacial contact. X-ray diffraction and grazing-incidence small-angle X-ray scattering measurements verified the superior molecular aggregates and grain boundaries of the molecule with two hydrogen-bonding sites in solid state, donating the corresponding devices showing optimized ternary data-storage performance with lower threshold voltages and higher device reproducibility.

Solvents Effects on Film Morphologies and Memory Behavior of a Perylenediimide-Containing Pendent Polymer.

The large polydispersity index of functional pendant polymers has hindered their application in semiconductors. Herein, a novel pendant polymer with perylenediimide (PDI) in the side chains was successfully synthesized through ring-opening metathesis polymerization (ROMP) with a very low polydispersity index. The synthesized polymers were spin-coated on indium tin oxide (ITO) substrate by using a mixture of 1,2-dichlorobenzene (o-DCB) and methanol (MeOH) solvents. The surface morphologies and intermolecular π-π stacking of the fabricated film could be adjusted through tuning of the ratio of o-DCB and MeOH, and thus, the sandwich-structured device of ITO/polymer/aluminum exhibited different electrical behavior. The threshold voltages of the devices decreased as the MeOH content was increased from 0 to 30 % (v/v); however, the device changed from being unrewritable to rewritable if the MeOH content was increased to 40 %; a probable mechanism for this process is discussed. It is hoped that this new idea of synthesizing narrow polydispersity index pendant polymers, and the fabrication of high-quality films through the use of a mixture of solvents could allow high-performance memory devices to be prepared in the future.

The Effect of Random and Block Copolymerization with Pendent Carbozole Donors and Naphthalimide Acceptors on Multilevel Memory Performance.

Polymeric materials have been widely used in the fabrication of data-storage devices, owing to their unique advantages and defined conduction mechanisms. To date, the most-functional polymers that have been reported for memory devices were synthesized through random copolymerization, whilst there have been no reports regarding the memory effect of block polymers. Herein, we synthesized a random copolymer (PMCz8 -co-PMBNa2 ) and its corresponding block copolymer (PMCz8 -b-PMBNa2 ) to study the effect of the method of polymerization on the memory properties of the corresponding devices. Interestingly, both devices (ITO/PMCz8 -co-PMBNa2 /Al and ITO/PMCz8 -b-PMBNa2 /Al) exhibited ternary memory performance, with threshold voltages of -1.7 V/-3.3 V and -2.7 V/-3.8 V, respectively. However, based on comprehensive measurements, the memory properties of PMCz8 -co-PMBNa2 and PMCz8 -b-PMBNa2 were found to be owing to the operation of different conduction mechanisms, which resulted from different molecular stacking in the film state. Therefore, we expect that this work will be helpful for improving our understanding of the conduction mechanisms in polymer-based data-storage devices.

A Novel Bat-Shaped Dicyanomethylene-4H-pyran-Functionalized Naphthalimide for Highly Efficient Solution-Processed Multilevel Memory Devices.

Small-molecule-based multilevel memory devices have attracted increasing attention because of their advantages, such as super-high storage density, fast reading speed, light weight, low energy consumption, and shock resistance. However, the fabrication of small-molecule-based devices always requires expensive vacuum-deposition techniques or high temperatures for spin-coating. Herein, through rational tailoring of a previous molecule, DPCNCANA (4,4'-(6,6'-bis(2-octyl-1,3-dioxo-2,3-dihydro-1H-benzo[de]isoquinolin-6-yl)-9H,9'H-[3,3'-bicarbazole]-9,9'-diyl)dibenzonitrile), a novel bat-shaped A-D-A-type (A-D-A=acceptor-donor-acceptor) symmetric framework has been successfully synthesized and can be dissolved in common solvents at room temperature. Additionally, it has a low-energy bandgap and dense intramolecular stacking in the film state. The solution-processed memory devices exhibited high-performance nonvolatile multilevel data-storage properties with low switching threshold voltages of about -1.3 and -2.7 V, which is beneficial for low power consumption. Our result should prompt the study of highly efficient solution-processed multilevel memory devices in the field of organic electronics.

Ternary Flexible Electro-resistive Memory Device based on Small Molecules.

Flexible memory devices have continued to attract more attention due to the increasing requirement for miniaturization, flexibility, and portability for further electronic applications. However, all reported flexible memory devices have binary memory characteristics, which cannot meet the demand of ever-growing information explosion. Organic resistive switching random access memory (RRAM) has plenty of advantages such as simple structure, facile processing, low power consumption, high packaging density, as well as the ability to store multiple states per bit (multilevel). In this study, we report a small molecule-based flexible ternary memory device for the first time. The flexible device maintains its ternary memory behavior under different bending conditions and within 500 bending cycles. The length of the alkyl chains in the molecular backbone play a significant role in molecular stacking, thus guaranteeing satisfactory memory and mechanical properties.