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In the past few years, the effect of strain on the optical and electronic properties of MoS2 layers has attracted particular attention as it can improve the performance of optoelectronic and spintronic devices. Although several approaches have been explored, strain is typically externally applied on the two-dimensional material. In this work, we describe the preparation of a reversible ‘self-strainable’ system in which the strain is generated at the molecular level by one component of a MoS2-based composite material. Spin-crossover nanoparticles were covalently grafted onto functionalized layers of semiconducting MoS2 to form a hybrid heterostructure. Their ability to switch between two spin states on applying an external stimulus (light irradiation or temperature change) serves to generate strain over the MoS2 layer. A volume change accompanies this spin crossover, and the created strain induces a substantial and reversible change of the electrical and optical properties of the heterostructure.Spin-crossover nanoparticles have been covalently grafted onto a semiconducting MoS2 layer to form a self-strainable heterostructure. Under light or thermal stimulus, the nanoparticles switch between their high- and low-spin states, in which they have different volumes. This generates a reversible strain over the MoS2 layer and, in turn, alters the electrical and optical properties of the heterostructure.

Stimuli-responsive systems are an emerging class of materials in fields as diverse as electronics, optoelectronics, cancer detection, drug delivery, or sensing. Especially focusing on nanomaterials, 2D transition metal dichalcogenides have recently attracted the scientific community's attention due to their remarkable intrinsic stimuli-responsive behaviour upon external stimuli such as pH, light, voltage, or certain pathogens. This significant response can be further enhanced by forming mixed-dimensional heterostructures and by molecular functionalization, capitalizing on chemistry to manipulate and boost their intrinsic stimuli-responsive properties. Furthermore, thanks to the endless possibilities of chemistry, a new class of smart materials based on the combination of stimuli-responsive molecular systems with transition metal dichalcogenides has recently been synthesized. In these materials, the physical properties of the 2D layers are reversibly modified by the switchable molecules, not only enhancing their stimuli-responsive behaviour but also providing memory to the hybrid. Therefore, this review explores the recent breakthroughs in the chemical design of smart transition metal dichalcogenides with built-in responsiveness. Transition metal dichalcogenides not only possess intrinsic stimuli-responsive behaviours upon exposure to external stimuli, but molecular functionalization of these materials and/or combination with other materials to form mixed-dimensional heterostructures enables the manipulation and enhancement of their stimuli-responsive properties. Here, the authors review recent breakthroughs in the chemical design of smart transition metal dichalcogenides with built-in responsiveness.

Chiral-induced spin selectivity (CISS), whereby helical molecules polarize the spin of electrical current, is an intriguing effect with potential applications in nanospintronics. In this nascent field, the study of paramagnetic chiral molecules, which could introduce another degree of freedom in the control of the spin transport, remains so far unexplored. To address this challenge, herein, we propose the use of self-assembled monolayers of helical lanthanide-binding peptides. In order to elucidate the effect of the paramagnetic nuclei, monolayers of the peptide coordinating paramagnetic or diamagnetic ions are prepared. By means of spin-dependent electrochemistry, CISS effect is demonstrated by cyclic voltammetry and impedance measurements for both samples. Additionally, an implementation of the standard liquid-metal drop electron transport setup has been carried out, demonstrating their suitability for solid-state devices. Remarkably, the inclusion of a paramagnetic center in the peptide increases the spin polarization as independently proved by different techniques. These findings permit the inclusion of magnetic biomolecules in the CISS field, paving the way to their implementation in a new generation of spintronic nanodevices.

We use the electrode-less time-resolved microwave conductivity (TRMC) technique to characterize spin-crossover (SCO) nanoparticles. We show that TRMC is a simple and accurate mean for simultaneously as-sessing the magnetic state of SCO compounds and charge transport information on the nanometre length scale. In the low-spin state from liquid nitrogen temperature up to 360 K the TRMC measurements present two well-defined regimes in the mobility and in the half-life times, possessing similar transition tempera-tures TR near 225 K. Below TR, an activation-less regime associated with short lifetimes of the charge carri-ers points at the presence of shallow-trap states. Above TR, these states are thermally released yielding a thermally activated hopping regime where longer hops increases the mobility and, concomitantly, the barrier energy. The activation energy could originate from intricate contributions such as polaronic self-localizations, but also from dynamic disorder due to phonons and/or thermal fluctuations of SCO moieties.

In this work we showcase the potential of peptides as versatile scaffolds for quantum computing and molecular spintronics. In particular, we focus on lanthanide-binding tags, which were originally developed in the field of biotechnology for the study of protein structure and dynamics. Firstly, we demonstrate quantum coherent oscillations in a Neodymium peptidic qubit. Then, employing bacterial biosynthesis, we investigate the possibility of increasing the number of qubits in the same molecular system, with the case studies being a double spin qubit with two distinct coordination environments, and an asymmetric chain of 9 spin qubits with a spin-spin separation of about 2 nm and in an arbitrarily chosen sequence of coordination environments. Finally, we take advantage of biochemical modification for the preparation of paramagnetic, chiral, Self-Assembled Monolayers (SAMs) on Au(111).Our experimental and theoretical characterization shows that this is a promising structure for spintronic applications, and in particular to improve on two state-of-the-art approaches to molecular spin qubits. We conclude with an overview of the challenges and new opportunities opened by this emerging field.