Dipolar Interactions Research Articles

Cutting-edge applications of oleic acid-modified CdSiO3: Ce3+ phosphors: Artificial intelligence enhanced latent fingerprint detection, anti-counterfeiting and optical thermometry

A series of (1–11 mol%) Ce³⁺ doped CdSiO₃ phosphors are synthesized via a solution combustion method, and the sample with the optimal doping concentration underwent surface modification with oleic acid (OA). X-ray diffraction (XRD) analysis confirmed the formation of high-purity, well-crystallized CdSiO3:Ce3+ phosphors. Upon 347 nm UV excitation, the phosphor exhibited intense blue emission at 400 nm, with an optimized Ce³⁺ concentration of 5 mol%, attributed to dipole-dipole interactions. The OA-modified phosphor demonstrated significantly enhanced properties, achieving a color purity (CP) of 97.2% and Internal quantum efficiency (IQE) of 82.5%. The phosphor also exhibited excellent thermal stability, retaining 93.0% of its emission intensity at 423 K and a thermal quenching temperature exceeding 483 K, with a high activation energy (Eₐ) of 0.384 eV. In practical applications, the OA modified phosphor showed exceptional performance in latent fingerprints (LFPs) detection and anti-counterfeiting (AC) across different substrates, offering high resolution, contrast, and minimal background interference. MATLAB based analysis yielded a matching score of 94.52%, surpassing conventional benchmarks, underscoring the phosphor's potential for advanced fingerprint identification. These results demonstrate that the CdSiO₃:5Ce³⁺ phosphor is a promising candidate for applications in white light-emitting diodes (w-LEDs), optical thermometry, forensic analysis and AC technologies.

The growth mechanism and optical properties of flower-like porous Gd2O2S:Er3+/Yb3+ phosphor

The self-assembly mechanism of porous materials has always been a hot topic and a challenging issue in research. What factors induce the self-assembly process, and how is the temperature sensing performance related to it? Innovatively, in this paper, Gd2O2S:Er3+/Yb3+ phosphors with different morphologies were synthesized, and elucidated the formation mechanism of flower-like structures through relevant theorems, formulas, and experiments, proposing that polar molecules and dipole-dipole interactions guide the synergistic effect of van der Waals forces and hydrogen bonding, which ultimately induces the self-assembly of spherical structures into flower-like ones. In addition, four representative intermediates were selected to investigate their luminescence and temperature sensing properties. The results show that the flower-like sample can respond more effectively to changes in ambient temperature because of its rich pore structures, and thus exhibit better temperature sensing performance. In-depth research on the self-assembly mechanism of materials helps to predict and regulate their properties, and the unique characteristics of flower-like sample provide new ideas for material selection in the field of high-precision temperature measurement.

Illuminating the dark: mono-γ signals at NA62

Dipole interactions between dark sector states or between a Standard Model particle and a dark state can efficiently be searched for via high-intensity fixed-target facilities. We propose to look for the associated mono-γ signature at the NA62 experiment running in beam dump mode. Focusing on models of dipole inelastic Dark Matter and active-sterile neutrino dipole interactions, we compute the corresponding expected sensitivities finding promising prospects for discovery already with ~ 1017 proton-on-target, corresponding to the present accumulated dataset.

Topological photon pumping in quantum optical systems

We establish the concept of topological pumping in one-dimensional systems with long-range couplings and apply it to the transport of a photon in quantum optical systems. In our theoretical investigation, we introduce an extended version of the Rice-Mele model with all-to-all couplings. By analyzing its properties, we identify the general conditions for topological pumping and theoretically and numerically demonstrate topologically protected and dispersionless transport of a photon on a one-dimensional emitter chain. As concrete examples, we investigate three different popular quantum optics platforms, namely Ryd-berg atom lattices, dense lattices of atoms excited to low-lying electronic states, and atoms coupled to waveguides, using experimentally relevant parameters. We observe that despite the long-ranged character of the dipole-dipole interactions, topological pumping facilitates the transport of a photon with a fidelity per cycle which can reach 99.9%. Moreover, we find that the photon pumping process remains topologically protected against local disorder in the coupling parameters.

Magnetization States and Coupled Spin-Wave Modes in Concentric Double Nanorings.

Concentric multiple nanorings have previously been fabricated and investigated mainly for their different static magnetization states. Here, we present a theoretical analysis for the magnetization dynamics in double nanorings arranged concentrically, where there is coupling across a nonmagnetic spacer due to the long-range dipole-dipole interactions. We employ a microscopic, or Hamiltonian-based, formalism to study the discrete spin waves that exist in the magnetic states where the individual rings may be in either a vortex or an onion state. Numerical results are shown for the frequencies and the spatial amplitudes (with relative phase included) of the spin-wave modes. Cases are considered in which the magnetic materials of the rings are the same (taken to be permalloy) or two different materials such as permalloy and cobalt. The dependence of these properties on the mean radial position of the spacer were studied, showing, in most cases, the existence of two distinct transition fields. The special cases, where the radial spacer width becomes very small (less than 1 nm) were analyzed to study direct interfaces between dissimilar materials and/or effects of interfacial exchange interactions such as Ruderman-Kittel-Kasuya-Yoshida coupling. These spin-wave properties may be of importance for magnetic switching devices and sensors.

Highly efficient Y3-xBaxAl5-xSixO12:Cr3+ near-infrared phosphor for plant growth

Near-infrared (NIR) phosphors enhance the growth of plants due to their superior penetration. However, relatively high thermal quenching and low quantum efficiency restrict the development of NIR phosphors. In this study, Y3-xBaxAl5-xSixO12:Cr3+ phosphors (YBAS:Cr3+) with varying concentrations of Ba2+-Si4+ and Cr3+ were studied. The results demonstrate high-purity phases are obtained with doping Ba2+-Si4+ and Cr3+. The Ba2+-Si4+ doping enhances crystallinity and near-spherical particles are synthesized. The theoretical calculations indicate a significant reduction in bandgap with doping Ba2+-Si4+, resulting in impurity levels appearing in the valence band region. The state density calculation shows that the band formation is contributed by all elements. The optimal Ba2+-Si4+ doping concentration is 0.05 mol and the Cr3+ doping content is 0.09 mol. The critical distance (R c ) is 16.62 Å. Dipole–dipole interactions and radiation reabsorptions are main concentration quenching mechanisms. Lattice distortions occur with the introduction of Ba2+-Si4+ and the value (D r ) is 0.052. The YBAS:0.09Cr3+ phosphor shows a crystal field strength with a Dq/B value of 2.76. The phosphor exhibits a high quantum efficiency (73.42%), superior thermal quenching resistance (∼70% initial intensity at 150°C), and a suitable fluorescence lifetime (130.04 µs). A near-infrared pc-LED with YBAS:0.09Cr3+ phosphor displays a high output power of 167.12 mW and a moderate conversion efficiency of 3.82%.

Multifunctional BiOCl: Sm3+ nanophosphors: A luminescent platform for solid-state lighting applications, optical thermometry, photocatalytic and forensic applications

Rare earth-activated phosphor materials have been widely used as active probes in optical materials for multidimensional applications. Here, we report a series of ultrahigh purity orange-red emitting BiOCl: xSm3+ (x= 0.5- 2.5 mol %) nanophosphors synthesized via conventional solid-state method at relatively low temperatures for various photonic and forensic applications. XRD and Rietveld refinement results confirmed the tetragonal crystal structure of the synthesized phosphor materials with space group P4/nmm. Fourier transform infrared (FT-IR) and Raman spectroscopy were used to perform the functional group analysis. The UV-Vis-NIR spectra were analyzed to determine the Judd-Ofelt (JO) intensity parameters (Ω2, Ω4, Ω6) and to identify the bonding structure and spontaneous emission properties of the samples. The prepared phosphors exhibit intense orange-red emission under 408 nm excitation and beyond 1 mol% doping of Sm3+ ions, the emission intensity decreases due to concentration quenching mechanism via, dipole-dipole interaction between the optically active Sm3+ ions in the phosphor sample. The synthesized BiOCl: Sm3+ nanophosphors possess low correlated color temperature (CCT), admirable high color purity (99.4%) and outstanding internal quantum efficiency (IQE) of 95.27%. The optical thermometry behavior of the optimized sample has been investigated in detail. Moreover, the optimized nanophosphor stains on porous and non-porous surfaces show clear ridge patterns with high sensitivity, efficiency, and minimal background hindrance for latent fingerprints and lip print detection in forensic applications and are used as security ink in anti-counterfeiting applications. Overall, the results revealed the potential prospects of BiOCl: Sm3+ nanophosphors in the field of display applications, optical thermometry, and forensic sciences.

Drug-amino acid interaction: Molecular dynamics in aqueous medium using time domain reflectometry

Present work reports dielectric response of the non-steroidal anti-inflammatory drug (NSAID) aceclofenac in aqueous valine solutions at various concentrations and temperatures (278.15 K–298.15 K) in the frequency range of 0.01 GHz to 30 GHz using Time-domain reflectometry (TDR) technique. The frequency dependent complex dielectric permittivity has been analyzed by Harviliak-Negami equation. Debye model is used for the description of complex dielectric permittivity spectra ε*(ν). The structural and dynamical properties of water has been investigated at different concentrations of valine and aceclofenac using dielectric as well as thermodynamic parameters that includes static dielectric constant (ε0), relaxation time (τ0), Kirkwood correlation factor (g), free energy of activation (ΔF), entropy of activation (ΔS), and enthalpy of activation (ΔH). Towards the measured low temperature and high concentrations of Valine and Aceclofenac (ACF), static dielectric constant (ε0) was found to be increasing. This could be due to increased effective dipole-dipole parallel alignment and can be confirmed by the increasing values of correlation factor (g > 1). The dipole-dipole interaction between Drug-Amino acid resulted in increased dielectric relaxation time (τ0) of system due to increased steric hindrance for the rotation of dipoles. The free energy of activation was found to be in the range of 2.22 and 2.58 Kcal mol-1. The entropy is more negative at high concentration suggesting more ordered structure. The slope of log (Tτ0) vs. 1000/T gives the value of enthalpy (ΔH).

Non-exchange bias hysteresis loop shifts in dense composites of soft-hard magnetic nanoparticles: New possibilities for simple reference layers in magnetic devices

Exchange bias has been extensively studied in both exchange-coupled thin films and nanoparticle composite systems. However, the role of non-exchange mechanisms in the overall hysteresis loop bias is far from being understood. Here, dense soft-hard binary nanoparticle composites are used not only as a novel tool to unravel the effect of dipolar interactions on the hysteresis loop shift but also as a new strategy to enhance the bias of any magnet exhibiting an asymmetric magnetization reversal. Mixtures of equally sized, 6.8 nm, soft maghemite (γ-Fe2O3) nanoparticles (no bias—symmetric reversal) and hard cobalt doped γ-Fe2O3 nanoparticles (large exchange bias—asymmetric reversal) reveal that, for certain fractions of soft particles, the loop shift of the composite can be significantly larger than the exchange-bias field of the hard particles in the mixture. Simple calculations indicate how this emerging phenomenon can be further enhanced by optimizing the parameters of the hard particles (coercivity and loop asymmetry). In addition, the existence of a dipolar-induced loop shift (“dipolar bias”) is demonstrated both experimentally and theoretically, where, for example, a bias is induced in the initially unbiased γ-Fe2O3 nanoparticles due to the dipolar interaction with the exchange-biased hard nanoparticles. These results open a new paradigm in the large field of hysteresis bias and pave the way for novel approaches to tune loop shifts in magnetic hybrid systems beyond interface exchange coupling.

Coercivity mechanism and magnetization reversal of anisotropic La-Nd-Dy-Fe-B micron-sized films

The coercivity mechanism and magnetization reversal process of anisotropic La-Nd-Dy-Fe-B micron-sized films have been investigated. By varying the thickness of the single-layer film from 500 nm to 6 μm, the highest coercivity of 1.88 T in the film with 3 μm thickness is achieved at 300 K, due to the large dipole interaction and domain pinning effect. When the thickness is further increased to 6um, the coercivity decreases sharply to 1.11T due to the microstructure and phase formation in the film. In the 6 μm multilayer film, the addition of a Ta spacer layer further enhances perpendicular magnetic anisotropy, the dipole interaction, and adjusts the phase distribution, collectively boosting the coercivity of the micron-sized film (1.63 T). As thickness of the film increases, the dominant mechanism of coercivity shifts from a pinning mechanism to a nucleation mechanism. This study contributes to the understanding of the coercivity mechanism and magnetization reversal process in La-Nd-Dy-Fe-B permanent magnet micron-sized films.

Diffracting crystals of an intrinsically disordered protein (IDP) AtPP16-1 grown in 1.3 V cm−1 DC field

DC electric field as weak as ∼1.3 V cm−1 induces crystal nucleation in very dilute protein solutions lacking precipitant. The basis of such growth is the microscopic model of interaction of protein dipoles with the Stark field, leading to glass-like amorphous aggregation and reconfiguration of the aggregates for crystal nucleation. This modest approach is very different from an earlier and rather ‘aggressive’ one in which electric field of ∼1 kV or orders of magnitude in excess is used to influence charge migration in a highly concentrated protein solution having precipitant confined to the crystallization drop. As an application of the precipitant-lacking ultralow protein method, the present work seeks the assistance of internally supplied 1.3 V cm−1 DC field to crystallize an intrinsically disordered protein (IDP) called AtPP16-1 in a 0.017 mg mL−1 solution. Crystallization is allowed in cuvette cells of spectrometers with online electric field, enabling measurement of real time changes in spectral features. The average crystal size increases with the time of passage of the electric field, from ∼0.042 at 10 min to 0.165 µm at the end of 300 min. The cubic crystals diffract electron and X-ray. Electron diffraction spot indexing yields lattice spacing dhkl ∼ 2.85 Å, consistent with 2.88 Å found from powder X-ray diffraction analysis. This level of lattice spacing will correspond to moderately resolved crystal structure of the IDP.

Structural determination, energy transfer and color-tunable photoluminescence of stable LiYSiO4: Ce/Tb/Sm Phosphors toward nUV pumped wLEDs application

Study on photon emission of Ce3+-doped phosphors is essential for advanced optoelectronic application. However, it remains quite difficult to design near-ultraviolet excitable Ce3+-activated silicate blue/cyan-emitting phosphors because of the combined influence of iconicity of Ce3+, crystal field strength, and nephelauxetic effect. Herein, Ce3+ incorporated into a proper host LiYSiO4 (LYS) phosphor is mechanistically investigated and shown efficient blue/cyan photoluminescence (PL) owing to Ce3+ 5d1 electronic state experiencing appropriate crystal field splitting. The comprehensive analysis based on structural refinement, dynamic/static spectra, and density functional theory calculations indicates that Ce3+ ions are energetically favored in octahedral Y site as compared with Li site in the host, resulting in attractive PL properties. According to the principle of color superposition and via cascading energy transfer (ET) from Ce3+ → Tb3+ → Sm3+, systematic PL tuning in a large color gamut is realized by further codoping with the green- and red-emissions of Tb3+ and Sm3+ in the phosphor LYS: Ce3+/Tb3+/Sm3+. The direct ET from Ce3+ → Sm3+ is difficult to occur due to the metal-metal charge transfer effect. Of note, the PL thermal-quenching of Ce3+ is mainly associated with multiphonon relaxation, while the quenching of Tb3+/ Sm3+ is primarily due to the cross relaxation (CR) process via dipole-dipole (d-d) interaction. The appropriate distance between the two nearest adjacent Y sites in the host together with the ET are conducive to weaken the CR process of Tb3+/Sm3+, leading to high PL efficiency. Finally, a prototype pc-wLED assembled via a remote ‘capping’ packaging strategy and by using only the stably composition-optimized white-emitting LYS: Ce3+/Tb3+/Sm3+ demonstrates that the phosphor is promising for high-quality of light.

Explication of the luminescent and optically active RE3+ triply-doped silica phosphate glass films for photonic applications

The multi-component silicate glass films triply-doped with Er3+/Yb3+/Nd3+ were fabricated by spin coating technique. X-ray diffraction revealed a cristobalite phase in the glasses doped above 0.6 mol% of Nd3+. The transparency of the films increases with the addition of the co-dopant, due to the increase in optical band gap by the Burstein-Moss shift. The high value of the correlated color temperature of the blue emission indicates enhanced visual perception, suggestive of cool blue film lasers. The red emission from upconversion exhibits potentiality for flat display panels. The gain cross-section of the glass with 0.6 mol% of Nd3+ was 13.54 ×10−20 cm2 which makes it ideal for NIR film lasers in the S-band region. The Inokuti-Hirayama model predicts luminescence quenching due to dipole-dipole interactions in the glasses co-doped beyond 0.6 mol% of Nd3+. The 4F9/2→4I13/2 transition observed in the films, suggests their suitability for O + E + S band NIR film lasers in telecommunication sectors.

Magnetically Tunable Electric Dipolar Interactions of Ultracold Polar Molecules in the Quantum Ergodic Regime.

By leveraging the hyperfine interaction between the rotational and nuclear spin degrees of freedom, we demonstrate extensive magnetic control over the electric dipole moments, electric dipolar interactions, and ac Stark shifts of ground-state alkali-dimer molecules such as KRb(X^{1}Σ^{+}). The control is enabled by narrow avoided crossings and the highly ergodic character of molecular eigenstates at low magnetic fields, offering a general and robust way of continuously tuning the intermolecular electric dipolar interaction for applications in quantum simulation, quantum sensing, and dipolar spinor physics.

“Nutation” of electron spins in biradicals

In this work, the nutation of the spins of unpaired electrons in the nitroxide biradical of bis‑methano[60]fullerene was experimentally studied. Nutation frequencies were found in a wide range of microwave field power. To interpret the obtained results, numerical calculations of the nutation of biradicals were carried out for a set of parameters of the spin–spin interaction of a pair of unpaired electrons and for different values of the Rabi frequency of the microwave field. At comparing numerical results with experimental data, we also used the results of analytical calculations of nutation for some model situations. As a result of the analysis of experimental data on nutation, an estimate of the exchange and dipole–dipole interactions for the studied biradical was obtained. They are consistent with the results obtained from analysis of the shape of the EPR spectrum for a given biradical.

Asymptotic solutions of the quantum scattering problem for binary collisions in a system of three charged particles. The inclusion of the dipole interaction

Asymptotic solutions of the quantum scattering problem for binary collisions in a system of three charged particles. The inclusion of the dipole interaction

Functionalized fillers as “ions relay stations” enabling Li+ ordered transport in quasi-solid electrolytes for high-stability lithium metal batteries

Quasi–solid–state lithium–metal batteries (QSLMBs) are promising candidates for next–generation battery systems due to their high energy density and enhanced safety. However, their practical application has been hindered by low ionic conductivity and the growth of lithium dendrites. To achieve ordered transport of Li+ ions in quasi–solid electrolytes (QSEs), improve ionic conductivity, and homogenize Li+ fluxes on the surface of the lithium metal anode (LMA), we propose a novel method. This method involves constructing “ion relay stations” in QSEs by introducing cyano–functionalized boron nitride nanosheets into pentaerythritol tetraacrylate (PETEA) –based polymer electrolytes. The functionalized boron nitride nanosheets promote the dissociation of lithium salts through ion–dipole interactions, optimizing the solvated structure to facilitate the orderly transport of Li+ ions, resulting in an ionic conductivity of 2.5 × 10−3 S cm−1 at 30 °C. Notably, this strategy regulates the Li+ distribution on the surface of the LMA, effectively inhibiting the growth of lithium dendrites. Li||Li symmetrical cells using this type of electrolyte maintain stability for over 2000 h at 2 mA cm−2 and 2 mAh cm−2. Additionally, with a high LiNi0.8Co0.1Mn0.1O2 (NCM811) loading of 8.5 mg cm−2, the cells exhibit excellent cycling performance, retaining a high capacity after 400 cycles. This innovative QSE design strategy represents a significant advancement towards the development of high–performance QSLMBs.

Highly Stretchable, Transparent, Solvent-Resistant Multifunctional Ionogel with Underwater Self-Healing and Adhesion for Wearable Strain Sensors and Barrier-Free Information Transfer.

Ionogels with excellent deformability, high ionic conductivity, and a sensitive stimulus response have been widely used and rapidly developed in flexible wearable systems. However, previously reported ionogels are mainly limited to atmospheric environments applications and have difficulty meeting the requirements of solvent-resistant, self-healing, and adhesion properties in underwater environments. Herein, a multifunctional ionogel capable of underwater applications is prepared by one-step photoinitiated polymerization of a fluorine-containing monomer (2,2,3,4,4,4-hexafluorobutyl acrylate, HFBA) and acrylic acid (AA) in a hydrophobic ionic liquid ([EMIM][TFSI]). The dynamic physical interactions of hydrogen bonds and ionic dipoles endow the ionogel with remarkable transparency, tunable mechanical properties, and underwater self-healing properties. Moreover, the fluoropolymer matrix offers high resistance to water and various solvents and exhibits strong underwater adhesion on different substrates. Thus, the sensor based on the ionogel exhibits excellent sensing properties, including high sensitivity, fast response, and superior durability. In particular, the ionogel can be used as a wearable underwater sensor to perform barrier-free information transfer. This study provides a design idea for the development of underwater flexible strain sensors.

Formulating the Relationship Between Intermolecular Interactions and Photodynamic Effects Based on the Optical Regularity Exhibited by Rare Earth‐BODIPY Crystalline Frameworks System

AbstractThis research commenced with an exploration of how metal nodes in metal‐organic frameworks (MOFs) influence photodynamic therapy (PDT) outcomes. Ultimately, it is revealed that intermolecular interactions are the core mechanism determining the optical properties and PDT efficacy of MOFs. An advanced system of MOFs based on the integration of twelve rare earth ions (RE3+) with boron dipyrromethene (BODIPY)‐derived ligands is reported. Intriguingly, this series of MOFs exhibits a reverse relationship between the radius of RE3+ and PDT efficacy. Single‐crystal X‐ray diffraction analyses along with theoretical calculations indicate that varying RE3+ results in a spatial displacement of the ligands along the dipole direction, diminishing electrostatic (dipole–dipole) interactions while enhancing dispersion (π–π) interactions, thereby enhancing the generation of triplet excitons. Consequently, a novel parameter, Ae‐v = EvdW / Eint × 100%, is proposed to quantify the interplay between non‐radiative energy dissipation via electrostatic interactions and efficient energy utilization in generating singlet oxygen through dispersion interactions. Furthermore, with consistent acoustic sensitivity aligned with the sonoluminescence mechanism, RE‐DCBs are employed in sono‐photodynamic cancer therapy, attaining significant therapeutic results in tumor treatment during in vivo experiments.

Aligned colloidal clusters in an alternating rotating magnetic field elucidated by magnetic relaxation

Precise control at the colloidal scale is one of the most promising bottom-up approaches to fabricating new materials and devices with tunable and precisely engineered properties. Magnetically driven colloidal assembly offers great versatility because of the ability to externally tune particle-particle interactions and to construct a host of particle arrangements. However, despite previous efforts to probe the parameter space, global orientational control in conjunction with two-dimensional microstructural control has remained out of reach. Furthermore, the magnetic relaxation time of superparamagnetic beads has been largely overlooked despite being a key feature of the magnetic response. Here, we take advantage of the magnetic relaxation time of superparamagnetic beads in an alternating rotating magnetic field and show how harnessing this feature facilitates the formation of oriented clusters. The orientation of these clusters can be controlled by field parameters. Using experiments, simulations, and theory, we probe a two-particle system (dimer) under this alternating rotating magnetic field and use its dynamics to provide insights into the collective response that forms clusters. We find that the type of field has significant implications for the dipolar interactions between the colloids because of the nonnegligible magnetic relaxation. Moreover, we find that the competing time scales of the magnetic relaxation and the alternating field generate an anisotropic interaction potential that drives cluster alignment. By exploiting the magnetic relaxation time of magnetic systems, we can tailor new types of interparticle interactions, thereby expanding the capabilities of colloidal assembly in engineering unique materials and devices.