Highly degenerate 2D ferroelectricity in pore decorated covalent/metal organic frameworks.

Two-dimensional (2D) ferroelectricity, a fundamental concept in low-dimensional physics, serves as the basis of non-volatile information storage and various electronic devices. Conventional 2D ferroelectric (FE) materials are usually two-fold degenerate, meaning that they can only store two logical states. In order to break such limitation, a new concept of highly degenerate ferroelectricity with multiple FE states (more than 2) coexisting in a single 2D material is proposed.

The critical role of ultra-low-energy vibrations in the relaxation dynamics of molecular qubits.

Improving the performance of molecular qubits is a fundamental milestone towards unleashing the power of molecular magnetism in the second quantum revolution. Taming spin relaxation and decoherence due to vibrations is crucial to reach this milestone, but this is hindered by our lack of understanding on the nature of vibrations and their coupling to spins. Here we propose a synergistic approach to study a prototypical molecular qubit.

Dynamical Screening of Local Spin Moments at Metal-Molecule Interfaces.

Transition-metal phthalocyanine molecules have attracted considerable interest in the context of spintronics device development due to their amenability to diverse bonding regimes and their intrinsic magnetism. The latter is highly influenced by the quantum fluctuations that arise at the inevitable metal-molecule interface in a device architecture. In this study, we have systematically investigated the dynamical screening effects in phthalocyanine molecules hosting a series of transition-metal ions (Ti, V, Cr, Mn, Fe, Co, and Ni) in contact with the Cu(111) surface.

Enabling Room-Temperature Triferroic Coupling in Dual Transition-Metal Dichalcogenide Monolayers Via Electronic Asymmetry.

Triferroic compounds are the ideal platform for multistate information devices but are rare in the two-dimensional (2D) form, and none of them can maintain macroscopic order at room temperature. Herein, we propose a general strategy for achieving 2D triferroicity by imposing electric polarization into a ferroelastic magnet. Accordingly, dual transition-metal dichalcogenides, for example, 1T'-CrCoS, are demonstrated to display room-temperature triferroicity.

A rule-free workflow for the automated generation of databases from scientific literature.

In recent times, transformer networks have achieved state-of-the-art performance in a wide range of natural language processing tasks. Here we present a workflow based on the fine-tuning of BERT models for different downstream tasks, which results in the automated extraction of structured information from unstructured natural language in scientific literature. Contrary to existing methods for the automated extraction of structured compound-property relations from similar sources, our workflow does not rely on the definition of intricate grammar rules.

Thermal ablation in pancreatic cancer: A scoping review of clinical studies.

Background: Pancreatic cancer is a deadly cancer with a 5-year survival rate less than 10%. Only 20% of patients are eligible to receive surgery at diagnosis. Hence, new therapies are needed to improve outcomes for non-surgical candidates.

Unraveling the Contributions to Spin-Lattice Relaxation in Kramers Single-Molecule Magnets.

The study of how spin interacts with lattice vibrations and relaxes to equilibrium provides unique insights into its chemical environment and the relation between electronic structure and molecular composition. Despite its importance for several disciplines, ranging from magnetic resonance to quantum technologies, a convincing interpretation of spin dynamics in crystals of magnetic molecules is still lacking due to the challenging experimental determination of the correct spin relaxation mechanism. We apply spin dynamics to a series of 12 coordination complexes of Co and Dy ions selected among ∼240 compounds that largely cover the literature on single-molecule magnets and well represent different regimes of spin relaxation.

Strain-induced stacking transition in bilayer graphene.

Strain, both naturally occurring and deliberately engineered, can have a considerable effect on the structural and electronic properties of 2D and layered materials. Uniaxial or biaxial heterostrain modifies the stacking arrangement of bilayer graphene (BLG) which subsequently influences the electronic structure of the bilayer. Here, we use density functional theory (DFT) calculations to investigate the interplay between an external applied heterostrain and the resulting stacking in BLG.

Determination of the Effects of Transcutaneous Auricular Vagus Nerve Stimulation on the Heart Rate Variability Using a Machine Learning Pipeline.

Background: We are all aware of day-to-day healthy stress, but, when sustained for long periods, stress is believed to lead to serious physical and mental health issues.

Materials And Methods: In this study, we investigated the potential effects of transcutaneous auricular vagus nerve stimulation (taVNS) on stress processing as reflected in the electrocardiogram (ECG)-derived biomarkers of stress adaptability. Stress reflecting biomarkers included a range of heart rate variability metrics: standard deviation of N-N intervals (SDNN), root mean squared of successive differences in heartbeat intervals (RMSSD), low-frequency component, high-frequency component and their ratio (LF, HF, and LF/HF).

Robust covalent pyrazine anchors forming highly conductive and polarity-tunable molecular junctions with carbon electrodes.

In molecular electronics, electrode-molecule anchoring strategies play a crucial role in the design of stable and high-performance functional single-molecule devices. Herein, we employ aromatic pyrazine as anchors to connect a central anthracene molecule to carbon electrodes including graphene and armchair single-walled carbon nanotubes (SWCNTs), and theoretically investigate their atomic structures and electronic transport properties. These molecular junctions can be constructed condensation reactions of the central molecules terminated with -phenylenediamines with -quinone-functionalized nanogaps of graphene and SWCNT electrodes.

Toward exact predictions of spin-phonon relaxation times: An ab initio implementation of open quantum systems theory.

Spin-phonon coupling is the main driver of spin relaxation and decoherence in solid-state semiconductors at finite temperature. Controlling this interaction is a central problem for many disciplines, ranging from magnetic resonance to quantum technologies. Spin relaxation theories have been developed for almost a century but often use a phenomenological description of phonons and their coupling to spin, resulting in a nonpredictive tool and hindering our detailed understanding of spin dynamics.

Electric Field Tunability of Photoluminescence from a Hybrid Peptide-Plasmonic Metal Microfabricated Chip.

Enhancement of fluorescence through the application of plasmonic metal nanostructures has gained substantial research attention due to the widespread use of fluorescence-based measurements and devices. Using a microfabricated plasmonic silver nanoparticle-organic semiconductor platform, we show experimentally the enhancement of fluorescence intensity achieved through electro-optical synergy. Fluorophores located sufficiently near silver nanoparticles are combined with diphenylalanine nanotubes (FFNTs) and subjected to a DC electric field.

Adhesion of thin metallic layers on Au surfaces.

We carried out first-principles density-functional theory calculations to study the work of separation for five different metal-metal interfaces, each of them comprising thin layers of selected metals (Cr, W, Ta, Al or Ti) lying on top of Au surfaces. We found that the highest work of separation is obtained for one-atom-thick layers. Increasing the number of atomic layers leads the work of separation to oscillate with the thickness, and ultimately tend to a limiting value for a large number of layers.

Photoluminescent, "ice-cream cone" like Cu-In-(Zn)-S/ZnS nanoheterostructures.

Copper based ternary and quaternary quantum confined nanostructures have attracted huge attention over recent years due to their potential applications in photonics, photovoltaics, imaging, sensing and other areas. However, anisotropic nanoheterostructures of this type are still poorly explored to date, despite numerous predictions of the distinctive optical properties of these highly fluorescent heavy metal free nanostructures. Here, we report new fluorescent multicomponent Cu-In-(Zn)-S/ZnS nanoheterostructures with a unique anisotropic "ice-cream cone" like morphology.

Near-Field Generation and Control of Ultrafast, Multipartite Entanglement for Quantum Nanoplasmonic Networks.

For a quantum Internet, one needs reliable sources of entangled particles that are compatible with measurement techniques enabling time-dependent, quantum error correction. Ideally, they will be operable at room temperature with a manageable decoherence versus generation time. To accomplish this, we theoretically establish a scalable, plasmonically based archetype that uses quantum dots (QD) as quantum emitters, known for relatively low decoherence rates near room temperature, that are excited using subdiffracted light from a near-field transducer (NFT).

Electrosynthesis of Biocompatible Free-Standing PEDOT Thin Films at a Polarized Liquid|Liquid Interface.

Conducting polymers (CPs) find applications in energy conversion and storage, sensors, and biomedical technologies once processed into thin films. Hydrophobic CPs, like poly(3,4-ethylenedioxythiophene) (PEDOT), typically require surfactant additives, such as poly(styrenesulfonate) (PSS), to aid their aqueous processability as thin films. However, excess PSS diminishes CP electrochemical performance, biocompatibility, and device stability.

Homochiral Mn Spin-Crossover Complexes: A Structural and Spectroscopic Study.

Structural, magnetic, and spectroscopic data on a Mn spin-crossover complex with Schiff base ligand 4-OMe-Sal323, isolated in crystal lattices with five different counteranions, are reported. Complexes of [Mn(4-OMe-Sal323)]X where X = ClO (), BF (), NO (), Br (), and I () crystallize isotypically in the chiral orthorhombic space group 222 with a range of spin state preferences for the [Mn(4-OMe-Sal323)] complex cation over the temperature range 5-300 K. Complexes and are high-spin, complex undergoes a gradual and complete thermal spin crossover, while complexes and show stepped crossovers with different ratios of spin triplet and quintet forms in the intermediate temperature range.

Hydrogen-Intercalated 2D Magnetic Bilayer: Controlled Magnetic Phase Transition and Half-Metallicity via Ferroelectric Switching.

Electrically controlled magnetism in two-dimensional (2D) multiferroics is highly desirable for both fundamental research and the future development of low-power nanodevices. Herein, inspired by the recently experimentally realized 2D antiferromagnetic MnPSe [ 2021, 16 (7), 782] and guided by a heteromagnetic structural design, we engineer strong magnetoelectric coupling in a hydrogen-intercalated 2D MnPSe bilayer. Hydrogen functionalization breaks the centrosymmetry of bilayer MnPSe, leading to out-of-plane ferroelectricity.

Quantifying Spin-Mixed States in Ferromagnets.

We quantify the presence of spin-mixed states in ferromagnetic 3D transition metals by precise measurement of the orbital moment. While central to phenomena such as Elliot-Yafet scattering, quantification of the spin-mixing parameter has hitherto been confined to theoretical calculations. We demonstrate that this information is also available by experimental means.

Temperature Dependence of Spin-Phonon Coupling in [VO(acac)]: A Computational and Spectroscopic Study.

Molecular electronic spins are good candidates as qubits since they are characterized by a large tunability of their electronic and magnetic properties through a rational chemical design. Coordination compounds of light transition metals are promising systems for spin-based quantum information technologies, thanks to their long spin coherence times up to room temperature. Our work aims at presenting an in-depth study on how the spin-phonon coupling in vanadyl-acetylacetonate, [VO(acac)], can change as a function of temperature using terahertz time-domain spectroscopy and density functional theory (DFT) calculations.

A Complete View of Orbach and Raman Spin-Lattice Relaxation in a Dysprosium Coordination Compound.

The unique electronic and magnetic properties of lanthanide molecular complexes place them at the forefront of the race toward high-temperature single-molecule magnets and magnetic quantum bits. The design of compounds of this class has so far being almost exclusively driven by static crystal field considerations, with an emphasis on increasing the magnetic anisotropy barrier. Now that this guideline has reached its maximum potential, a deeper understanding of spin-phonon relaxation mechanisms presents itself as key in order to drive synthetic chemistry beyond simple intuition.

In Situ Tuning of the Charge-Carrier Polarity in Imidazole-Linked Single-Molecule Junctions.

Manipulating the nature of the charge carriers at the single-molecule level is one of the major challenges of molecular electronics. Using first-principles quantum transport calculations, we have investigated the electronic transport properties of imidazole-linked single-molecule junctions and identified the hydrogen atom bonded to the pyrrole-like nitrogen in imidazole as a switch to tune the polarity of the charge carriers. Our calculations show that the chemical nature of the imidazole anchors is dramatically altered by dehydrogenation, which changes the dominant charge carriers from electrons to holes.

Using Weakly Supervised Deep Learning to Classify and Segment Single-Molecule Break-Junction Conductance Traces.

In order to design molecular electronic devices with high performance and stability, it is crucial to understand their structure-to-property relationships. Single-molecule break junction measurements yield a large number of conductance-distance traces, which are inherently highly stochastic. Here we propose a weakly supervised deep learning algorithm to classify and segment these conductance traces, a method that is mainly based on transfer learning with the pretrain-finetune technique.

Endotoxin contamination of engineered nanomaterials: Overcoming the hurdles associated with endotoxin testing.

Nanomaterials are highly susceptible to endotoxin contamination due their large surface-to-volume ratios and endotoxins propensity to associate readily to hydrophobic and cationic surfaces. Additionally, the stability of endotoxin ensures it cannot be removed efficiently through conventional sterilization techniques such as autoclaving and ionizing radiation. In recent times, the true significance of this hurdle has come to light with multiple reports from the United States Nanotechnology Characterization Laboratory, in particular, along with our own experiences of endotoxin testing from multiple Horizon 2020-funded projects which highlight the importance of this issue for the clinical translation of nanomaterials.