Mapping the Extended Ground State Reactivity Landscape of a Photoswitchable Molecule at a Single Molecular Level.

Photoswitchable molecules with structural flexibility can exhibit a complex ground state potential energy landscape due to the accessibility of multiple metastable states at merely low energy barriers. However, conventional bulk analytical techniques are limited in their ability to probe these metastable ground states and their relative energies. This is partially due to the difficulty of inducing changes in small molecules in their ground state, as they do not respond to external stimuli, such as mechanical force, unless they are incorporated into larger polymer networks.

Mimicking on-water surface synthesis through micellar interfaces.

The chemistry of the on-water surface, characterized by enhanced reactivity, distinct selectivity, and confined reaction geometry, offers significant potential for chemical and materials syntheses. However, the utilization of on-water surface synthesis is currently limited by the requirement for a stable air-water interface, which restricts its broader synthetic applications. In this work, we present a approach that mimics on-water surface chemistry using micelles.

Chiral spin selectivity and chiroptical activity in helical molecules.

Chiral structures, breaking spatial inversion symmetry, exhibit non-zero chiroptical activity (COA) due to the coupling between their electric and magnetic responses under external electromagnetic fields, an effect absent in achiral systems. Non-magnetic chiral structures also exhibit Chiral-Induced Spin Selectivity (CISS), primarily detected in two terminal measurements in the linear regime, where spin selection emerges without external magnetic influence. Despite the different origins of these physical phenomena, our model captures the relevant physics required to address CISS as an intrinsic molecular effect with the basic ingredients: (i) chirality/inversion asymmetry, (ii) meV atomic spin-orbit coupling, and (iii) decoherence as a source of reciprocity breaking.

Enantiospecificity in NMR enabled by chirality-induced spin selectivity.

Spin polarization in chiral molecules is a magnetic molecular response associated with electron transport and enantioselective bond polarization that occurs even in the absence of an external magnetic field. An unexpected finding by Santos and co-workers reported enantiospecific NMR responses in solid-state cross-polarization (CP) experiments, suggesting a possible additional contribution to the indirect nuclear spin-spin coupling in chiral molecules induced by bond polarization in the presence of spin-orbit coupling. Herein we provide a theoretical treatment for this phenomenon, presenting an effective spin-Hamiltonian for helical molecules like DNA and density functional theory (DFT) results on amino acids that confirm the dependence of J-couplings on the choice of enantiomer.

Inverse mapping of quantum properties to structures for chemical space of small organic molecules.

Computer-driven molecular design combines the principles of chemistry, physics, and artificial intelligence to identify chemical compounds with tailored properties. While quantum-mechanical (QM) methods, coupled with machine learning, already offer a direct mapping from 3D molecular structures to their properties, effective methodologies for the inverse mapping in chemical space remain elusive. We address this challenge by demonstrating the possibility of parametrizing a chemical space with a finite set of QM properties.

Dataset for quantum-mechanical exploration of conformers and solvent effects in large drug-like molecules.

We here introduce the Aquamarine (AQM) dataset, an extensive quantum-mechanical (QM) dataset that contains the structural and electronic information of 59,783 low-and high-energy conformers of 1,653 molecules with a total number of atoms ranging from 2 to 92 (mean: 50.9), and containing up to 54 (mean: 28.2) non-hydrogen atoms.

Chiral-Induced Spin Selectivity Modulated Time-Correlated Single-Photon Counting for DNA Hybridization Detection.

The chiral-induced spin selectivity (CISS) effect can distinguish between the spin of electrons as they pass through chiral molecules by backscattering one of the spin components. Herein, we explore the role of the CISS effect in time-correlated single-photon counting measurements to detect DNA hybridization. We observe that the average lifetime of optical excited states of quantum dots attached to double-stranded DNA (dsDNA) varies with directions of the applied magnetic field.

Site-selective chemical reactions by on-water surface sequential assembly.

Controlling site-selectivity and reactivity in chemical reactions continues to be a key challenge in modern synthetic chemistry. Here, we demonstrate the discovery of site-selective chemical reactions on the water surface via a sequential assembly approach. A negatively charged surfactant monolayer on the water surface guides the electrostatically driven, epitaxial, and aligned assembly of reagent amino-substituted porphyrin molecules, resulting in a well-defined J-aggregated structure.

Probing chiral discrimination in biological systems using atomic force microscopy: The role of van der Waals and exchange interactions.

We analyze from a theoretical perspective recent experiments where chiral discrimination in biological systems was established using Atomic Force Microscopy (AFM). Even though intermolecular forces involved in AFM measurements have different origins, i.e.

Enhancing the Carrier Transport in Monolayer MoS through Interlayer Coupling with 2D Covalent Organic Frameworks.

The coupling of different 2D materials (2DMs) to form van der Waals heterostructures (vdWHs) is a powerful strategy for adjusting the electronic properties of 2D semiconductors, for applications in opto-electronics and quantum computing. 2D molybdenum disulfide (MoS ) represents an archetypical semiconducting, monolayer thick versatile platform for the generation of hybrid vdWH with tunable charge transport characteristics through its interfacing with molecules and assemblies thereof. However, the physisorption of (macro)molecules on 2D MoS yields hybrids possessing a limited thermal stability, thereby jeopardizing their technological applications.

Sequence-controlled chiral induced spin selectivity effect in ds-DNA.

In this research, we explore sequence-dependent chiral-induced spin selectivity (CISS) in double-stranded (ds)-DNA using time-correlated single-photon counting and electrochemical impedance spectroscopy supplemented by tight-binding calculations of the phenomenon for the first time. The average lifetime of the photo-excited electrons in a Quantum Dot-DNA system is influenced by the CISS effect generated by the DNA molecule, and the difference in average time decay of electrons was found to be 345 ps for opposite polarity ("UP" and "DOWN") of spins due to the CISS effect. Moreover, the yield of spin-polarized electrons due to the CISS effect was reduced by more than 35% from perfect DNA to DNA with point mutations.

Spin-phonon coupling in a double-stranded model of DNA.

We address the electron-spin-phonon coupling in an effective model Hamiltonian for DNA to assess its role in spin transfer involved in the Chiral-Induced Spin Selectivity (CISS) effect. The envelope function approach is used to describe semiclassical electron transfer in a tight-binding model of DNA at half filling in the presence of intrinsic spin-orbit coupling. Spin-phonon coupling arises from the orbital-configuration dependence of the spin-orbit interaction.

Dithienylethene-Based Single Molecular Photothermal Linear Actuator.

By employing a mechanically controllable break junction technique, we have realized an ideal single molecular linear actuator based on dithienylethene (DTE) based molecular architecture, which undergoes reversible photothermal isomerization when subjected to UV irradiation under ambient conditions. As a result, open form (compressed, UV OFF) and closed form (elongated, UV ON) of dithienylethene-based molecular junctions are achieved. Interestingly, the mechanical actuation is achieved without changing the conductance of the molecular junction around the Fermi level over several cycles, which is an essential property required for an ideal single molecular actuator.

Applications of Graphene in Five Senses, Nervous System, and Artificial Muscles.

Graphene remains of great interest in biomedical applications because of biocompatibility. Diseases relating to human senses interfere with life satisfaction and happiness. Therefore, the restoration by artificial organs or sensory devices may bring a bright future by the recovery of senses in patients.

Toward Smart Sensing by MXene.

The Internet of Things era has promoted enormous research on sensors, communications, data fusion, and actuators. Among them, sensors are a prerequisite for acquiring the environmental information for delivering to an artificial data center to make decisions. The MXene-based sensors have aroused tremendous interest because of their extraordinary performances.

The contribution of intermolecular spin interactions to the London dispersion forces between chiral molecules.

Dispersion interactions are one of the components of van der Waals (vdW) forces that play a key role in the understanding of intermolecular interactions in many physical, chemical, and biological processes. The theory of dispersion forces was developed by London in the early years of quantum mechanics. However, it was only in the 1960s that it was recognized that for molecules lacking an inversion center, such as chiral and helical molecules, there are chirality-sensitive corrections to the dispersion forces proportional to the rotatory power known from the theory of circular dichroism and with the same distance scaling law R as the London energy.

Real-Time Monitoring of Blood Parameters in the Intensive Care Unit: State-of-the-Art and Perspectives.

The number of patients in intensive care units has increased over the past years. Critically ill patients are treated with a real time support of the instruments that offer monitoring of relevant blood parameters. These parameters include blood gases, lactate, and glucose, as well as pH and temperature.

Exploring the similarity of single-layer covalent organic frameworks using electronic structure calculations.

Two-dimensional Covalent Organic Frameworks (2D COFs) have attracted considerable interest because of their potential for a broad range of applications. Different combinations of the monomeric units can lead to potentially novel materials with varying physico-chemical properties. In this study, we investigate the electronic properties of various 2D COFs with square lattice topology based on a tight-binding density functional theory approach.

Sustainable Microbial and Heavy Metal Reduction in Water Purification Systems Based on PVA/IC Nanofiber Membrane Doped with PANI/GO.

Effective and efficient removal of both heavy metal pollutants and bacterial contamination from fresh water is an open issue, especially in developing countries. In this work, a novel eco-friendly functional composite for water treatment application was investigated. The composite consisted of electrospun nanofiber membrane from blended polyvinyl alcohol (PVA)/iota carrageenan (IC) polymers doped with equal concentrations of graphene oxide (GO) nanoparticles and polyaniline (PANI).

A Chirality-Based Quantum Leap.

There is increasing interest in the study of chiral degrees of freedom occurring in matter and in electromagnetic fields. Opportunities in quantum sciences will likely exploit two main areas that are the focus of this Review: (1) recent observations of the chiral-induced spin selectivity (CISS) effect in chiral molecules and engineered nanomaterials and (2) rapidly evolving nanophotonic strategies designed to amplify chiral light-matter interactions. On the one hand, the CISS effect underpins the observation that charge transport through nanoscopic chiral structures favors a particular electronic spin orientation, resulting in large room-temperature spin polarizations.

An effective formaldehyde gas sensor based on oxygen-rich three-dimensional graphene.

Three-dimensional (3D) graphene with a high specific surface area and excellent electrical conductivity holds extraordinary potential for molecular gas sensing. Gas molecules adsorbed onto graphene serve as electron donors, leading to an increase in conductivity. However, several challenges remain for 3D graphene-based gas sensors, such as slow response and long recovery time.

Effect of lubricants on the rotational transmission between solid-state gears.

Lubricants are widely used in macroscopic mechanical systems to reduce friction and wear. However, on the microscopic scale, it is not clear to what extent lubricants are beneficial. Therefore, in this study, we consider two diamond solid-state gears at the nanoscale immersed in different lubricant molecules and perform classical MD simulations to investigate the rotational transmission of motion.

A nanographene disk rotating a single molecule gear on a Cu(111) surface.

On Cu(111) surface and in interaction with a single hexa-tert-butylphenylbenzene molecule-gear, the rotation of a graphene nanodisk was studied using the large-scale atomic/molecular massively parallel simulator molecular dynamics simulator. To ensure a transmission of rotation to the molecule-gear, the graphene nanodisk is functionalized on its circumference by-butylphenyl chemical groups. The rotational motion can be categorized underdriving, driving and overdriving regimes calculating the locking coefficient of this mechanical machinery as a function of external torque applied to the nanodisk.

Graphene Biodevices for Early Disease Diagnosis Based on Biomarker Detection.

The early diagnosis of diseases plays a vital role in healthcare and the extension of human life. Graphene-based biosensors have boosted the early diagnosis of diseases by detecting and monitoring related biomarkers, providing a better understanding of various physiological and pathological processes. They have generated tremendous interest, made significant advances, and offered promising application prospects.

Applications of Carbon Nanotubes in the Internet of Things Era.

The post-Moore's era has boosted the progress in carbon nanotube-based transistors. Indeed, the 5G communication and cloud computing stimulate the research in applications of carbon nanotubes in electronic devices. In this perspective, we deliver the readers with the latest trends in carbon nanotube research, including high-frequency transistors, biomedical sensors and actuators, brain-machine interfaces, and flexible logic devices and energy storages.