Interaction Strength Research Articles

Responsive Organic Fluorescent Aggregates Based on Ion-π Interactions Away from Fluorescent Conjugated Groups.

Responsive organic luminescent aggregates have a wide range of application fields, but currently there is still a lack of reasonable molecular design strategies. Introducing ion-π interactions into molecules can effectively alter their luminescent properties. However, current research typically focuses on ion localization at luminescent conjugated groups with the strong interaction forces. In this work, we introduce the flexible alkoxy chain spacers between fluorescent conjugated groups and ion-π interaction sites, and then adjust the fluorescence performance of the molecule by changing the strength of ion-π interactions. Bromine ion-based molecules with strong ion-π interactions exhibit high and stable fluorescence quantum yields in crystals and amorphous powders under the external stimuli. Hexafluorophosphate ion-based molecules with weak ion-π interactions have the high fluorescence quantum yield in crystals and very low fluorescence quantum yield in amorphous powders, showing variable fluorescence intensities under external stimuli. This demonstrates a new class of responsive organic luminescent solid-state materials.

Reentrant phase behavior in systems with density-induced tunneling

We show that correlations in strongly interacting many-particle systems can create quantum decoherence, leading to a mechanism of dissipation that does not rely on an external source. Using analytical methods, we study a bosonic many body system in two dimensions, with extended interactions between particles. We show that, as expected, the system can be driven out of a coherent state. Surprisingly, when the interaction strength is sufficiently large, the system reenters the superfluid phase even after coherence is lost. The breakdown of quantum coherence is a certainty, but interpreting the process correctly relies on understanding and preserving the nature of the coupling between the constituents of the many particle system. The methods used provide a natural cutoff point at the critical temperature, where superfluidity breaks down.

Which Coverages of Arc-Shaped Proteins Are Required for Membrane Tubulation?

Arc-shaped BIN/Amphiphysin/Rvs (BAR) domain proteins generate curvature by binding to membranes and induce membrane tubulation at sufficiently large protein coverages. For the amphiphysin N-BAR domain, Le Roux et al., Nat. Commun. 2021, 12, 6550, measured a threshold coverage of 0.44 ± 0.097 for nanotubules emerging from the supported lipid bilayer. In this article, we systematically investigate membrane tubulation induced by arc-shaped protein-like particles with coarse-grained modeling and simulations and determine the threshold coverages at different particle-particle interaction strengths and membrane spontaneous curvatures. In our simulations, the binding of arc-shaped particles induces a membrane shape transition from spherical vesicles to tubules at a particle threshold coverage of about 0.5, which is rather robust to variations of the direct attractive particle interactions or spontaneous membrane curvature in the coarse-grained model. Our study suggests that threshold coverages of around or slightly below 0.5 are a general requirement for membrane tubulation by arc-shaped BAR domain proteins.

Ionic Pairs-Engineered Fluorinated Covalent Organic Frameworks Toward Direct Air Capture of CO2.

The covalent organic frameworks (COFs) possessing high crystallinity and capability to capture low-concentration CO2 (400ppm) from air are still underdeveloped. The challenge lies in simultaneously incorporating high-density active sites for CO2 insertion and maintaining the ordered structure. Herein, a structure engineering approach is developed to afford an ionic pair-functionalized crystalline and stable fluorinated COF (F-COF) skeleton. The ordered structure of the F-COF is well maintained after the integration of abundant basic fluorinated alcoholate anions, as revealed by synchrotron X-ray scattering experiments. The breakthrough test demonstrates its attractive performance in capturing (400ppm) CO2 from gas mixtures via O─C bond formation, as indicated by the in situ spectroscopy and operando nuclear magnetic resonance spectroscopy using 13C-labeled CO2 sources. Both theoretical and experimental thermodynamic studies reveal the reaction enthalpy of ≈-40kJmol-1 between CO2 and the COF scaffolds. This implies weaker interaction strength compared with state-of-the-art amine-derived sorbents, thus allowing complete CO2 release with less energy input. The structure evolution study from synchrotron X-ray scattering and small-angle neutron scattering confirms the well-maintained crystalline patterns after CO2 insertion. The as-developed proof-of-concept approach provides guidance on anchoring binding sites for direct air capture (DAC) of CO2 in crystalline scaffolds.

The relationship between anaemia and the use of treated bed nets among pregnant and non-pregnant women in Ghana.

Studies have indicated that the risk of malaria, particularly its association with anaemia in pregnant women, increases when treated bed nets are not used. This paper utilizes a statistical mechanical model to investigate whether there is a statistical relationship between the presence or absence of anaemia in pregnant and non-pregnant women and their decision to sleep under treated bed nets. Data from the Ghana Malaria Indicator Survey (GMIS), which includes both rural and urban malaria-endemic areas in Ghana, were employed in this study. A total of 2,434 women, comprising 215 pregnant and 2,219 non-pregnant participants, were involved. Among these, 4.76% of the pregnant and anaemic women and 45.89% of the non-pregnant and anaemic women slept under treated bed nets, while 0.86% of the pregnant and anaemic and 6.82% of the non-pregnant and anaemic women did not. The findings revealed that, in the absence of social interaction, non-anaemic pregnant women have a lower prevalence of choosing to use bed nets compared to their anaemic counterparts. Additionally, non-pregnant anaemic women showed a positive private incentive (30.87%) to use treated bed nets, implying a positive correlation between anaemia and the choice to sleep in a treated bed net. Furthermore, the study demonstrated that both pregnancy and anaemia status have a relationship with the use of treated bed nets in Ghana, especially when social interactions are considered. The interaction strength between non-pregnant and anaemic women interacting with each other shows a negative estimate (-1.49%), implying that there is no rewarding effect from imitation. These insights are crucial for malaria prevention and control programs, emphasizing the need for targeted interventions to enhance the use of treated bed nets among both pregnant and non-pregnant women in Ghana's malaria-endemic regions.

Interfacial Second-Harmonic Generation via Superposition of Symmetries in a Double-Resonance-Enhanced Plasmonic Nanocavity.

Second-harmonic generation (SHG) has rapidly advanced with the miniaturization of on-chip devices and has found many applications, including optical frequency conversion, nonlinear imaging, and quantum technology. However, owing to the obvious phase-matching constraints involved in nonlinear optical interactions in bulk crystals and the decrease in the length and strength of nonlinear interactions in nanophotonic and surface/interface systems, improving the SHG efficiency and manipulating its optical properties at the nanoscale are challenging tasks. Herein, a monocrystalline silver microplate and nanocube-coupled nanocavity with double-resonance plasmonic modes and an ultrasmall gap were constructed, resulting in efficiently enhanced SHG. In particular, the SHG from the silver microplate (111) is polarization-dependent, and the anisotropy of the SHG in the plasmonic nanocavity can be further controlled via the superposition of symmetries at the interface and plasmonic waveguide-cavity modes. The interfacial SHG provides technology for developing lattice surface atomic arrangement and nanostructure rapid characterization, nonlinear light sources, and on-chip nonlinear nanophotonic devices.

Non-monotonic thermal conductivity modulation in colloidal quantum dot superlattices via ligand engineering

Colloidal quantum dots (QDs), which consist of inorganic cores surrounded by soft organic ligands, can self-assemble into superlattices exhibiting long-range order. Their tunability, in terms of size, shape, and ligand properties, makes them promising for applications in solar cells, photodetectors, and light-emitting diodes. However, the complex interplay between ligand stiffness, QDs cores-ligands coupling strength, and its impact on QDs' morphology and thermal properties is not well understood. This work employs molecular dynamics simulations to investigate the possibility of modulating the thermal conductivity of QDs superlattices via ligand engineering. It is found that the structural stability of QDs superlattices depends significantly on the interaction strength between the QDs cores and ligands. At lower interaction strengths, the instability manifests itself in a random fusion of the QDs cores, while at intermediate strengths a stable simple cubic lattice structure is maintained. Conversely, higher interaction strengths lead to amorphization in the surface regions of QDs core. We observed a nonlinear trend in the thermal conductivity with varying QD-ligand interaction strengths due to competing factors: fusion of QDs cores at lower interaction strengths and increased crosslinking interaction among ligands at higher interaction strengths. The influence of ligand stiffness on thermal conductivity was found to be minimal. This study provides a deep insight into the role of ligand stiffness and interaction strength on structural dynamics and thermal transport in QDs superlattice and demonstrates the feasibility of engineering thermal transport in QDs superlattice via ligand engineering.

Tensile Control of Vibrational Strong Light‐Matter Coupling with Flexible Polyester Films

AbstractPolaritons are generated by strong interaction between photons and matter, with the hybridization fundamentally changing the energy landscape of the system. Future exploitation of polaritons will benefit from implementing low‐cost, flexible, and easily tuneable configurations, as electronics have before. Here, coherent coupling of the carbonyl stretch vibrations of polyester (poly(ethylene terephthalate), PET) films to the optical modes of a Fabry–Perot (FP) cavity is presented, in which the FP cavity is directly formed on flexible, free‐standing, and commercially available PET films. For 2‐µm thick PET films, the carbonyl stretch vibration of the PET overlaps with the half‐wavelength FP cavity mode, leading to the coupling of the two modes, a Rabi splitting above 160 cm−1, and associated anticrossing in angular dispersion measurements. The study demonstrates dynamic control of light‐matter interaction strength by modulating film thickness under tension, finding that a 25% tensile stretch can tune the light‐matter interaction from 20:80 mixing to near‐perfect 50:50 hybridization at normal incidence. These findings are discussed in the context of future foldable/twistable/wearable polaritonic devices.

Thermal Welding of Liquids.

Welding of thermoplastics is a common practice in many industrial sectors, but it has yet to be realized with fluids. Here, the thermal welding of liquids by using the assembly and jamming of nanoparticle surfactants (NPSs) at liquid-liquid interfaces is reported. By fine-tuning the dynamic interaction strength within NPSs, the interfacial activity of NPSs, as well as the binding energy of NPSs to the interface can be precisely controlled, leading to a dynamic exchange of NPSs, maximizing the reduction in the interfacial energy. With NPSs jammed at the interface, the structures of liquids can be manipulated to complex geometries by applying an external force and, due to the temperature responsiveness of NPSs, when bringing liquids into contact and heating the system, welding of liquids can be achieved. This work provides a straightforward strategy for the construction of modular all-liquid fluidics, opening up numerous opportunities in fields like biotechnology, healthcare, and materials science.

Non-thermal phonon dynamics and a quenched exciton condensate probed by surface-sensitive electron diffraction.

Interactions among and between electrons and phonons steer the energy flow in photo-excited materials and govern the emergence of correlated phases. The strength of electron-phonon interactions, decay channels of strongly coupled modes and the evolution of three-dimensional order are revealed by electron or X-ray pulses tracking non-equilibrium structural dynamics. Despite such capabilities, the growing relevance of inherently anisotropic two-dimensional materials and functional heterostructures still calls for techniques with monolayer sensitivity and, specifically, access to out-of-plane phonon polarizations. Here, we resolve non-equilibrium phonon dynamics and quantify the excitonic contribution to the structural order parameter in 1T-TiSe2. To this end, we introduce ultrafast low-energy electron diffuse scattering and trace strongly momentum- and fluence-dependent phonon populations. Mediated by phonon-phonon scattering, a few-picosecond build-up near the zone boundary precedes a far slower generation of zone-centre acoustic modes. These weakly coupled phonons are shown to substantially delay overall equilibration in layered materials. Moreover, we record the surface structural response to a quench of the material's widely investigated exciton condensate, identifying an approximate 30:70 ratio of excitonic versus Peierls contributions to the total lattice distortion in the charge density wave phase. The surface-sensitive approach complements the ultrafast structural toolbox and may further elucidate the impact of phonon scattering in numerous other phenomena within two-dimensional materials, such as the formation of interlayer excitons in twisted bilayers.

Cholesterol Changes Interfacial Water Alignment in Model Cell Membranes.

The nanoscopic layer of water that directly hydrates biological membranes plays a critical role in maintaining the cell structure, regulating biochemical processes, and managing intermolecular interactions at the membrane interface. Therefore, comprehending the membrane structure, including its hydration, is essential for understanding the chemistry of life. While cholesterol is a fundamental lipid molecule in mammalian cells, influencing both the structure and dynamics of cell membranes, its impact on the structure of interfacial water has remained unknown. We used surface-specific vibrational sum-frequency generation spectroscopy to study the effect of cholesterol on the structure and hydration of monolayers of the lipids 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC), 1,2-dioleoyl-sn-glycero-3-phosphocholine (DOPC), and egg sphingomyelin (SM). We found that for the unsaturated lipid DOPC, cholesterol intercalates in the membrane without significantly changing the orientation of the lipid tails and the orientation of the water molecules hydrating the headgroups of DOPC. In contrast, for the saturated lipids DPPC and SM, the addition of cholesterol leads to clearly enhanced packing and ordering of the hydrophobic tails. It is also observed that the orientation of the water hydrating the lipid headgroups is enhanced upon the addition of cholesterol. These results are important because the orientation of interfacial water molecules influences the cell membranes' dipole potential and the strength and specificity of interactions between cell membranes and peripheral proteins and other biomolecules. The lipid nature-dependent role of cholesterol in altering the arrangement of interfacial water molecules offers a fresh perspective on domain-selective cellular processes, such as protein binding.

Topologically protected subradiant cavity polaritons through linewidth narrowing enabled by dissipationless edge states

Cavity polaritons derived from strong light–matter interaction provide a basis for efficient manipulation of quantum states via cavity field. Polaritons with narrow linewidth and long lifetime are appealing in applications, such as quantum sensing and storage. Here, we propose a prototypical arrangement to implement a whispering-gallery-mode resonator with one-dimensional topological atom mirror, which allows to boost the lifetime of cavity polaritons over an order of magnitude. This considerable enhancement attributes to the coupling of polaritonic states to dissipationless edge states protected by the topological bandgap of atom mirror that suppresses the leakage of cavity modes. When exceeding the width of Rabi splitting, topological bandgap can further reduce the dissipation from polaritonic states to bulk states, giving arise to subradiant cavity polaritons with extremely sharp linewidth. The resultant Rabi oscillation experiences decay rate lower than the free-space decay of a single quantum emitter. Inheriting from the topologically protected properties of edge states, the subradiance of cavity polaritons can be preserved in disordered atom mirror with moderate perturbations involving the atomic frequency, interaction strengths and location fluctuations. Our work opens up a new paradigm of topology-engineered quantum states with robust quantum coherence for future applications in quantum computing and network.

Tunable and Switchable Thermochromism in Cholesteric Liquid Crystalline Elastomers.

Thermochromic materials have found widespread commercial use in packaging as temperature indicators. Often, these products utilize leuco dyes that are mixed into conventional polymeric resins to prepare coatings or films that exhibit temperature-dependent color change. Here, we consider a distinctive approach to thermochromism via the selective reflection of liquid crystalline elastomers that retain the helicoidal structure of the cholesteric phase (CLCEs). Upon heating, the order of the CLCEs reduces and approaches zero, resulting in a change in birefringence as well as material thickness, both of which manifest as changes in the selective reflection to heating. This examination systematically prepares CLCEs capable of reversible thermochromic response as a function of cross-link density and liquid crystalline composition. A particular focus of this examination is the preparation of CLCEs composed of chiral and achiral liquid crystalline monomers that reduce the strength of the mesogen-mesogen interaction and accordingly reduce the nematic-isotropic transition temperature. The low birefringence of some of the CLCE compositions facilitates thermochromic reflection tuning, followed by switching.

Topological properties of a class of generalized Su–Schrieffer–Heeger networks: Chains and meshes

We analyze the topological properties of a family of generalized Su-Schrieffer-Heeger (SSH) chains and mesh geometries. In both the geometries the usual staggering in the distribution of the two overlap integrals is delayed (in space) by the inclusion of a third (additional) hopping term. A tight-binding Hamiltonian is used to unravel the topological phases, characterized by a topological invariant. While in the linear chains, the topological invariant (the Zak phase) always appears to be quantized, in the quasi-one dimensional strip geometries and the generalized SSH mesh patterns the quantization of the Zak phase is sensitive to the strength of the additional interaction (the ‘extra’ hopping integral). We study its influence thoroughly and explore the edge states and their robustness against disorder in the cross-linked generalized SSH mesh geometries. The systems considered here can be taken to model (though crudely) two-dimensional polymers where the cross-linking brings in non-trivial modification of the energy bands and transport properties. In addition to the topological features studied, we provide a prescription to unravel any flat, non-dispersive energy bands in the mesh geometries, along with the structure and distribution of the compact localized eigenstates. Our results are analytically exact.

Effect of the magnetic field on the conductance and spin polarization in phosphorene superlattice

The spin-dependent conductance and spin polarization are investigated theoretically in a phosphorene superlattice in the presence of external magnetic field and Rashba interaction. It is demonstrate that, the spin-dependent conductance with and without spin-flip as well as spin polarization can be effectively controlled by changing the magnetic field strength and the number of the superlattice barriers. For small magnetic field strength, the conductance for with and without spin-flip shows an oscillating behavior as increasing the strength of the Rashba interaction, and by increasing the number of barriers, the oscillating behavior becomes prominent. Further, when the magnetic field is greater than a limit value, the spin conductance will be zero. The size of the spin-dependent transmission window in the phosphorene superlattice under external magnetic field decreases drastically. The magnitude, sign and behavior of the spin polarization can be tuned by the amount of the external magnetic field.

Modelling non-Markovian noise in driven superconducting qubits

Non-Markovian noise can be a significant source of errors in superconducting qubits. We develop gate sequences utilising mirrored pseudoidentities that allow us to characterise and model the effects of non-Markovian noise on both idle and driven qubits. We compare three approaches to modelling the observed noise: (i) a Markovian noise model, (ii) a model including interactions with a two-level system (TLS), (iii) a model utilising the post Markovian master equation, which we show to be equivalent to the qubit-TLS model in certain regimes. When running our noise characterisation circuits on a superconducting qubit device we find that purely Markovian noise models cannot reproduce the experimental data. Our model based on a qubit-TLS interaction, on the other hand, is able to closely capture the observed experimental behaviour for both idle and driven qubits. We investigate the stability of the noise properties of the hardware over time, and find that the parameter governing the qubit-TLS interaction strength fluctuates significantly even over short time-scales of a few minutes. Finally, we evaluate the changes in the noise parameters when increasing the qubit drive pulse amplitude. We find that although the hardware noise parameters fluctuate significantly over different days, their drive pulse induced relative variation is rather well defined within computed uncertainties: both the phase error and the qubit-TLS interaction strength change significantly with the pulse strength, with the phase error changing quadratically with the amplitude of the applied pulse. Since our noise model can closely describe the behaviour of idle and driven qubits, it is ideally suited to be used in the development of quantum error mitigation and correction methods.

Favored CH-π interaction between enzymatically modified high amylose starch and resveratrol improves digestion resistance

Starch-stilbene polyphenol complexes, a novel form of resistant starch (RS), have received considerable attention due to their potential health benefits. To enhance the functionality of this type of complex, we examined the interactions between resveratrol (RA) and high-amylose starch with different molecular weights, achieved through enzymatic modification followed by high-pressure homogenization (HPH). We examined how these interactions affect the digestibility and ordered structures of the complexes. Our findings reveal that, notwithstanding the inhibition of double helix and B-type crystalline structure formation, RA-starch complexation markedly boosted single helix content, V-type crystalline structure formation, and aggregate structure density. These effects contributed notably to increased RS content. Interestingly, the formation of the V6-type crystalline structure within the complexes was primarily facilitated by the CH-π interaction between the aromatic rings of RA and the C–H of starch, rather than conventional hydrogen bonding and electrostatic forces. The strength of the CH-π interaction increased with higher amylose content and lower molecular weight of the starch, achievable through a 12-h pullulanase hydrolysis followed by a 2-h α-amylase hydrolysis. The resulting HPH-Pα2-RA complexes exhibited remarkable levels of the V-type crystalline structure and RS content, reaching up to 25.45% and 57.37%, respectively. Overall, this study offers valuable insights into the design of starch-polyphenols complexes with a high RS content.

Spatial Network Analysis of Coupling Coordination between Digital Financial Inclusion and Common Prosperity in the Yangtze River Delta Urban Agglomeration

Digital financial inclusion and common prosperity are pivotal elements in promoting the sustainable socioeconomic development of China. This study introduces a novel Multi-Criteria Decision Analysis (MCDA) method to evaluate the Common Prosperity Index (CPI). Using this index, alongside the Digital Financial Inclusion Index (DFII) released by Peking University, it examines the evolution of the coupling coordination relationship between digital financial inclusion and common prosperity within the Yangtze River Delta (YRD) urban agglomeration from 2011 to 2021. By integrating gravity models and social network analysis, in this paper, we thoroughly investigate the spatiotemporal evolution characteristics of the spatial network of this coupling coordination relationship. The results indicate that both the DFII and CPI generally exhibit an upward trend, but the decline in the coupling degree reflects a weakened interaction strength between them. Specifically, Anhui significantly lags behind Jiangsu, Zhejiang, and Shanghai in the development of digital financial inclusion and common prosperity, indicating regional development imbalances. Furthermore, the strength of spatial connections in city coupling coordination has significantly increased, with Nanjing’s siphon effect on cities in Anhui becoming markedly stronger, and the number of core cities in the network increasing, which demonstrates a geographical proximity feature in network development. Additionally, the overall network characteristics are transitioning towards higher density and “small-world” properties, suggesting a trend toward network stabilization. The disparity in centrality among cities has decreased, with an overall enhancement in centrality, where the spatial spillover effects from core areas such as Hangzhou-Ningbo, Nanjing-Changzhou, and Shanghai-Suzhou-Wuxi significantly promote the development of peripheral cities. Based on these findings, this paper proposes policy recommendations for the sustainable development of digital financial inclusion and common prosperity in the YRD region.

Density functional theory investigation of the contributions of π-π stacking and hydrogen bonding with water to the supramolecular aggregation interactions of model asphaltene heterocyclic compounds

ContextA complex supramolecular process involving electrostatic and dispersion interactions and asphaltene aggregation is associated with detrimental petroleum deposition and scaling that pose challenges to petroleum recovery, transportation, and upgrading. The homodimers of seven heterocyclic model compounds, representative of moieties commonly found in asphaltene structures, were studied: pyridine, thiophene, furan, isoquinoline, pyrazine, thiazole, and 1,3-oxazole. The contributions of hydrogen bonding involving water bridges spanning between dimers and π-π stacking to the total interaction energy were calculated and analyzed. The distance between the planes of the aromatic rings is correlated with the π-π stacking interaction strength. All the dimerization reactions were exothermic, although not spontaneous. This was mostly modulated by the strength of the hydrogen bond of the water bridge and the π-π stacking interaction. Dimers bridged by two water molecules were more stable than those with additional water molecules or without any water molecule in the bridge. Energy decomposition analysis showed that the electrostatic and polarization components were the main stabilizing terms for the hydrogen bond interaction in the bridge, contributing at least 80% of the interaction energy in all dimers. The non-covalent interaction analysis confirmed the molecular sites that had the strongest (hydrogen bond) and weak (π-π stacking) attractive interactions. They were concentrated in the water bridge and in the plane between the aromatic rings, respectively.MethodsThe density functional ωB97X-D with a dispersion correction and the Def2-SVP basis set were employed to investigate supramolecular aggregates incorporating heterocycles dimers with 0, 1, 2, and 3 water molecules forming a stabilizing bridge connecting the monomers. The non-covalent interactions were analyzed using the NCIplot software and plotted as isosurface maps using Visual Molecular Dynamics.

Electrically tunable correlated domain wall network in twisted bilayer graphene

We investigate the domain wall network in twisted bilayer graphene (TBG) under the influence of interlayer bias and screening effect from the layered structure. Starting from the continuum model, we analyze the low-energy domain wall modes within the moiré bilayer structure and obtain an analytic form representing charge density distributions of the two-dimensional structure. By computing the screened electron–electron interaction strengths both within and between the domain walls, we develop a bosonized model that describes the correlated domain wall network. We demonstrate that these interaction strengths can be modified through an applied interlayer bias, screening length and dielectric materials, and show how the model can be employed to investigate various properties of the domain wall network and its stability. We compute correlation functions both without and with phonons. Including electron–phonon coupling in the network, we establish phase diagrams from these correlation functions. These diagrams illustrate electrical tunability of the network between various phases, such as density wave states and superconductivity. Our findings reveal the domain wall network as a promising platform for the experimental manipulation of electron–electron interactions in low dimensions and the study of strongly correlated matter. We point out that our investigation not only enhances the understanding of domain wall modes in TBG but also has broader implications for the development of moiré devices.