Controlling Isomerization of Photoswitches to Modulate 2D Logic‐in‐Memory Devices by Organic–Inorganic Interfacial Strategy

Abstract

Logic‐in‐memory devices are a promising and powerful approach to realize data processing and storage driven by electrical bias. Here, an innovative strategy is reported to achieve the multistage photomodulation of 2D logic‐in‐memory devices, which is realized by controlling the photoisomerization of donor–acceptor Stenhouse adducts (DASAs) on the surface of graphene. Alkyl chains with various carbon spacer lengths (n = 1, 5, 11, and 17) are introduced onto DASAs to optimize the organic–inorganic interfaces: 1) Prolonging the carbon spacers weakens the intermolecular aggregation and promotes isomerization in the solid state. 2) Too long alkyl chains induce crystallization on the surface and hinder the photoisomerization. Density functional theory calculation indicates that the photoisomerization of DASAs on the graphene surface is thermodynamically promoted by increasing the carbon spacer lengths. The 2D logic‐in‐memory devices are fabricated by assembling DASAs onto the surface. Green light irradiation increases the drain–source current (Ids) of the devices, while heat triggers a reversed transfer. The multistage photomodulation is achieved by well‐controlling the irradiation time and intensity. The strategy based on the dynamic control of 2D electronics by light integrates molecular programmability into the next generation of nanoelectronics.

Optical Phenomena in Molecule-Based Magnetic Materials

“…In basics, every one of these processes can be reversed by different light irradiation but, moving to the solid state, this feature is often easily quenched by supramolecular interactions. However, up to now, numerous studies have been undertaken to achieve light-modulated (bio)­sensors, luminophores, optical memory devices, and molecular machines. , Recent reports regarding photoswitchable conductors, separating membranes, and catalysts − also utilize the effect of light-induced structural modifications, broadening the application horizon of this class of molecular materials. Despite the intrinsic switchability of the above-mentioned organic entities, serving as ligands, they also enrich various functionalities of MOF materials …”

Visible light-responsive materials: the (photo)chemistry and applications of donor–acceptor Stenhouse adducts in polymer science

“…148 Some of these methods have also been explored for DASAs, including MOF nanocages, 55 structural modifications of the DASA with bulky, flexible groups ( e.g. , long alkyl chains), 54 and other nanoencapsulation strategies. 118…”

“…2,4 Consequently, solution-cast pure DASA films typically show very limited photochromism (although concentration effects are likely also contributing factors, see Section 2.5.3). 54,94,136 The discussion of mechanical effects in DASA-containing polymers is separated into two categories: bulk materials (Section 2.5.1.1) and materials applied in solution/suspension (Section 2.5.1.2).…”

“…This is one reason for the limited photochromism observed in pure DASAs in the solid state (crystalline and amorphous). 54,94,136 Aggregation could also contribute to reduced fatigue resistance (cf. Section 2.6).…”

“…The few examples of DASA in combination with biopolymers/-oligomers are briefly discussed in the third part. Examples of the integration of DASAs into functional materials other than polymers lie outside the scope of this review, including inorganic and metal nanoparticles, [50][51][52][53] graphene, 54 metal-organic frameworks (MOFs), 55,56 polyoxometalates, 57 supramolecular complexes with metal-ligand/ organic molecular vessels, 58,59 or with hydrogen bonding receptors, 60 and self-assembled structures of small molecule DASA-based amphiphiles. 61,62 1.1 Donor-acceptor Stenhouse adducts In 2014, the photochromism of DASAs was discovered by Read de Alaniz and co-workers.…”