Atomic Interactions Research Articles

Programming higher-order interactions of Rydberg atoms

Programming higher-order interactions of Rydberg atoms

Thouless pumping and trapping of two-component gap solitons

We study Thouless pumping and arresting of gap solitons in a two-component Bose gas loaded into an optical superlattice. We show that, depending on the atomic interactions and chemical potentials, the two solitons can be simultaneously pumped or trapped, but we also identify regimes where one soliton is pumped and the other arrested. These behaviors can be understood by considering an effective model of the system based on a variational approach, which reveals that the soliton width is a suitable qualifier for the observed behaviors: solitons with a larger width get transported, while solitons with a smaller width get trapped. Since these widths can be controlled by tuning interactions, it should be possible to observe all behaviors experimentally. Published by the American Physical Society 2024

Response Matching for Generating Materials and Molecules.

Diffusion models have recently emerged as powerful tools for the generation of new molecular and material structures. The key insight is that the noise in these models is related to the response of the atoms to displacement, and the denoising step is thus analogous to the geometry relaxation of atomistic systems starting from a random structure. Building on this, we present a generative method called Response Matching (RM), which leverages the fact that each stable material or molecule exists at the minimum of its potential energy surface. Any perturbation induces a response in energy and stress, driving the structure back to equilibrium. Matching this response is closely related to score matching in diffusion models. Another important aspect of state-of-the-art diffusion models is the incorporation of physical symmetries such as translation, rotation, and periodicity. RM employs a machine learning interatomic potential and random structure search as the denoising model, inherently respecting these symmetries and exploiting the locality of atomic interactions. RM handles both molecules and bulk materials under the same framework. Its efficiency and generalization are demonstrated on three systems: a small organic molecular data set, stable crystals from the Materials Project, and one-shot learning on a single diamond configuration.

Phonon-Lithium Ion Interactions: A Case Study of LiM(SeO3)2 (M = Al, Ga, In, Sc, Y, and La).

Li ion diffusion is fundamentally a thermally activated ion hopping process. Recently, soft lattice, anharmonic phonon, and paddlewheel mechanism have been proposed to potentially benefit the ion transport, while the understanding of vibrational couplings of mobile ions and anions is still very limited but essential. Herein, we accessed the ionic conductivity, stability, and especially, lattice dynamics in LiM(SeO3)2 (M = Al, Ga, In, Sc, Y, and La) with two different types of oxygen anions within a LiO4 polyhedron, namely, edge-shared and corner-shared with MO6 polyhedra, the prototype of which, LiGa(SeO3)2, has been theoretically reported before with the similar structural features to NASICON and later experimentally synthesized with the room temperature conductivity ∼0.11 mS cm-1. It is interesting to note that LiM(SeO3)2 with a higher Li phonon band center shows higher Li conductivity, which is in contradiction to the conventional understanding of the importance for soft lattice to superionic conductors. The anharmonic and harmonic phonon interactions as well as the couplings between the vibration of the edge-bonded or corner-bonded anion in Li polyanions and the Li ion diffusion have been studied in detail. With transition metal M changing from La, Y, In, Ga, Al, and Sc, anharmonic phonons increase with reduced activation energy for Li diffusion. The phonon modes dominated by the edge-bonded oxygen anions contribute more to the migration of the Li ion than those dominated by the corner-bonded oxygen anions because of the greater atomic interaction between the Li ion and the edge-bonded anions. Thus, rather than the overall lattice softness, attention shall be given to reduce the frequency of the critical phonons contributing to Li ion diffusion as well as to increase the anharmonicity, i.e., through asymmetric Li polyhedra, for the design of Li ion superionic conductors for all-solid-state batteries.

Improving Crystal Property Prediction from a Multiplex Graph Perspective.

Graph neural networks (GNNs) have proven to be effective tools for the rapid and accurate prediction of crystal properties. While most existing methods focus on enriching representations of crystal structures, they do not deeply explore the characteristics of crystal graphs and leverage their intrinsic information from a data science perspective. In this work, we propose the potential multiplex crystal graph neural network (PMCGNN) for crystal property prediction. Based on the characteristics of crystal graphs, we reconstruct the crystal graph into a multiplex graph that includes two views: a global crystal graph embodying infinite potentials and a local crystal graph capturing local atomic interactions. We employ graph transformers (GTs) and message passing neural networks (MPNNs) architectures to learn the atomic representations of these two perspectives. Specifically, we augment the GT by incorporating positional encodings and structural encodings from the local crystal graph. This approach promotes interaction between the two perspectives, enabling the model to learn both node positional and graph structural information from different viewpoints through an attention mechanism. As a result, it enhances the model's ability to learn crystal representations. We conduct comprehensive experiments on the JARVIS and the Materials Project data sets for evaluation. Results show that PMCGNN presents superior performance in 9 crystal prediction tasks while maintaining reasonable computational expense.

Insights on the mechanical properties and failure mechanisms of calcium silicate hydrates based on deep-learning potential molecular dynamics

The molecular-scale mechanical properties of calcium silicate hydrates are crucial to the macro performance of cementitious materials, while achieving coincidence between accuracy and efficiency in computational simulations still remains a challenge. This study utilizes a deep-learning potential, specifically developed for calcium silicate hydrates based on artificial neural network, to achieve molecular dynamics simulations with accuracy comparable to first-principle methods. With this potential, the elastic properties and uniaxial mechanical behaviors are explored, wherein the anisotropy and impact mechanism of calcium ratios are analyzed. The results add to evidence that the deep-learning potential possess a higher accuracy than common force fields. The anisotropy of elastic modulus is mainly attributed to different atomic interactions in various directions, while the anisotropy of strength is additionally affected by the form of failure. This study may advance the accurate molecular-scale simulation and deepen the understanding of the strength source and cohesion mechanism of cement-based materials.

Vibrational, optical and elastic properties of Cs2AgBiX6 (X= Br, Cl) double perovskite materials: DFT, PL, Raman and Brillouin scattering studies

In this study, we explore the temperature-dependent Raman, photoluminescence (PL) and Brillouin spectroscopy, as well as Density Functional Theory (DFT) calculation results of Cs2AgBiBr6 and Cs2AgBiCl6 double perovskites. Single crystals of Cs2AgBiBr6 and Cs2AgBiCl6 were synthesized via a hydrothermal method. The lattice structure has been clearly defined, and the electronic band structures, validated by DFT calculations, are consistent with previously reported data. Optical properties calculated via DFT approach indicate superior energy storage capacity for Cs2AgBiBr6. Changes in optical properties at room temperature suggest potential suitability for specific applications, ranging from photovoltaics to lasers. Raman and Brillouin spectroscopy have revealed significant insights regarding the vibrational properties and atomic interactions within the materials, thereby contributing to a better understanding of the atomic interactions within the perovskite structures. Experimental data has highlighted anomalies in the Raman shifts, indicating the presence of a phase transition in Cs2AgBiBr6 at 115 K. However, no such phase transition was observed in Cs2AgBiCl6. This observation is further supported by Brillouin spectroscopy. PL measurements on Cs2AgBiBr6 revealed the presence of a low-temperature phase transition at 35 K. DFT calculations also provide detailed insights into the elastic properties of these perovskites, notably indicating superior mechanical strength for Cs2AgBiCl6. These findings will enhance the understanding of perovskite materials and expand their potential technological applications, especially in environments with varying thermal conditions

Review on Grounds state Hanle effect on paraffin coated alkali atoms under condition EIT and EIA

IntroductionThis review is specifically aimed at a higher level of understanding of the ground-state Hanle effect through novel methods of atomic vapor interaction with resonant light. Electromagnetically Induced Transparency (EIT) and absorption (EIA) are the primary phenomena in this context. EIT is a process in which destructive interference at absorption frequencies within a medium is caused by a control laser and makes the medium clear to the probe laser light. It should be noted that this transparency is crucial for turning on/off the light pulses, slowing down or stopping in several cases, thus enhancing the effectiveness of atomic magnetometers. However, constructive interference that occurs in EIA raises the density of the medium, which is advantageous for profit-making precise measurements and the improvement of atomic clocks. ObjectiveThe objective of this study is to review the fundamental principles of the Hanle effect, EIT, EIA, and coating methods for alkali atoms. These principles and techniques are critical for improving the sensitivity and functionality of atomic magnetometers and other quantum devices. By understanding and leveraging these phenomena, significant progress has been made in the development of high-precision measurement tools and quantum technologies. ResultsAdvancements in atomic magnetometer sensitivity represent a rapidly growing area of interest, driving significant progress in the development of quantum devices. This review consolidates the existing knowledge and recent findings, offering a thorough understanding of the fundamental principles and practical applications of the Hanle effect, EIT, EIA, and coating methods for alkali atoms. This review highlights how advancements in EIT and EIA have contributed to the sensitivity improvements of atomic magnetometers, and underscores the importance of coating methods for maintaining system integrity and performance. These developments are essential to the evolution of modern quantum technologies and precision measurement devices.

Enantioselective Binding of Proton Pump Inhibitors to Alpha1-Acid Glycoprotein and Human Serum Albumin-A Chromatographic, Spectroscopic, and In Silico Study.

The enantioselective binding of three proton pump inhibitors (PPIs)-omeprazole, rabeprazole, and lansoprazole-to two key plasma proteins, α1-acid glycoprotein (AGP) and human serum albumin (HSA), was characterized. The interactions between PPI enantiomers and proteins were investigated using a multifaceted analytical approach, including high-performance liquid chromatography (HPLC), fluorescence and UV spectroscopy, as well as in silico molecular docking. HPLC analysis demonstrated that all three PPIs exhibited enantioseparation on an AGP-based chiral stationary phase, suggesting stereoselective binding to AGP, while only lansoprazole showed enantioselective binding on the HSA-based column. Quantitatively, the S-enantiomers of omeprazole and rabeprazole showed higher binding affinity to AGP, while the R-enantiomer of lansoprazole displayed greater affinity for AGP, with a reversal in the elution order observed between the two protein-based columns. Protein binding percentages, calculated via HPLC, were greater than 88% for each enantiomer across both transport proteins, with all enantiomers displaying higher affinity for AGP compared to HSA. Thermodynamic analysis indicated that on the HSA, the more common, enthalpy-controlled enantioseparation was found, while in contrast, on the AGP, entropy-controlled enantioseparation was observed. The study also identified limitations in using fluorescence titration due to the high native fluorescence of the compounds, whereas UV titration was effective for both proteins. The determined logK values were in the range of 4.47-4.83 for AGP and 4.02-4.66 for HSA. Molecular docking supported the experimental findings by revealing the atomic interactions driving the binding process, with the predicted enantiomer elution orders aligning with experimental data. The comprehensive use of these analytical methods provides detailed insights into the enantioselective binding properties of PPIs, contributing to the understanding of their pharmacokinetic differences and aiding in the development of more effective therapeutic strategies.

The hierarchical energy landscape of edge dislocation glide in refractory high-entropy alloys

Refractory high-entropy alloys (RHEAs) are considered as potential candidates for high-temperature applications, with the glide resistance of edge dislocations being a crucial factor in determining the high-temperature strength. However, the solid-solution strengthening mechanism of edge dislocations in RHEAs is not fully understood. The existing Labusch-type models mainly focus on the long-range interaction of solute atoms with the dislocation stress field, while there is little attention paid to the short-range interaction in the dislocation core region. Here, we conduct carefully designed atomic simulations to decouple the long-range and short-range interactions in a typical RHEA, NbMoTaW. Furthermore, the total change in solute-dislocation interaction energy is decomposed, and a hierarchical energy landscape is revealed, demonstrating that the short-range interaction at the core region gains more importance in the solid-solution strengthening of edge dislocations in NbMoTaW. Then, we determine the Larkin length, which signifies the transition from size-dependent to size-independent dislocation behavior. The activation barrier extracted from the simulation with the dislocation length above the Larkin length is incorporated into the crystal plasticity model, and the high-temperature yield strength is well predicted by the strengthening from edge dislocations. Our work provides deep insight into the solid-solution strengthening mechanism in random solution solids, elucidating the importance of the local atomic configuration around the dislocation core.

Pressure-induced extreme anisotropic behavior of thermoelectric properties in crystalline β-CuSCN

Applying hydrostatic pressure has emerged as a promising strategy for regulating the properties of thermoelectric materials, particularly in the case of β-CuSCN, which has garnered attention due to its ultra-low thermal conductivity and potential applications in thermoelectric devices. Herein, we investigate the intrinsic mechanism governing the electron-thermal transport properties of β-CuSCN under hydrostatic pressure. It was found that ZT decreased by 30 % along the in-plane direction while increasing by 24 % along the out-of-plane direction following the application of hydrostatic pressure, respectively. Our results reveal that the competitive relationship between pressure-driven effects on phonon dynamics and electronic structure influences the thermoelectric properties of β-CuSCN. For the transport mechanism, the compression alters phonon dispersion by enhancing atomic interactions, which leads to an increase in lattice thermal conductivity. On the other hand, despite strong coupling between electrical transport parameters, a net increase in power factor is achieved through pressure-induced bandgap narrowing. As a result, the thermoelectric properties demonstrate contrary variation tendency along the in-plane and out-of-plane directions. Our research deepens our understanding of transport behavior under extreme pressure conditions and provides valuable insights into the fundamental relationship between structural deformation and thermoelectric performance.

An Improved Model for Prediction of Critical Velocity of Cold-Spray by First-Principles Calculations

The first-principles calculation was applied to predict the critical velocity of Cu/Al cold-spray bonding for the first time. The bonding mechanism of cold-spray was clarified by analyzing the energy variation and atomic interaction during the cold-spray impact process. Our results showed that the shear deformation played a key role in the cold-spray bonding. The atomic interaction determined the effective absorption of impact kinetic energy and finally determined the successful bonding of the cold-spray. The heterogeneous atoms absorbed the impact kinetic energy by interatomic attraction to achieve cold-spray bonding, while the homogeneous atoms absorbed the impact kinetic energy by the deformation of interface layers. An excellent agreement between the predicted critical velocity and the experimental one could be obtained, especially for the heterogeneous material cold-spray. Our present method proved to be a simple and highly efficient computing method in critical velocity prediction. Most importantly, the critical velocity for cold-spray could be predicted without using any empirical or experimental parameters.

Indirect to direct band gap transition of ABI3 (A = Rb, Cs; B = Ca, Sr) perovskites under hydrostatic pressure for photovoltaic and optoelectronic applications: A DFT study

The objective of this study is to enhance the utilization of ABI3 (A = Rb, Cs; B = Ca, Sr) metal-halide perovskites in multiple forms of technological applications by investigating their structural, electronic, optical, and mechanical characteristics using the ab initio method. At ambient pressure, the geometry-optimized lattice constants for RbCaI3, RbSrI3, CsCaI3, and CsSrI3 are 6.19 Å, 6.45 Å, 6.22 Å, and 6.47 Å, respectively, consistent with prior research. Additionally, a significant decrease in lattice parameters and bond length is observed, which leads to increased levels of atomic interactions. Pressure narrows the band gap from the ultraviolet-to-visible region. This phenomenon promotes the transfer of electrons from the valence-to-conduction band, hence improving the performance of optoelectronic devices. Furthermore, a shift from an indirect to a direct band gap is induced by the application of pressure, which improves the material's suitability for photovoltaic applications. The covalent and ionic nature of Ca/Sr-I and Rb/Cs-I under pressure and without pressure conditions was determined using the charge density maps. Enhanced pressure significantly boosts optical absorption and conductivity in the visible spectrum, implying substantial potential for improving the efficacy of perovskite solar cells and photonic devices. Additionally, applied pressure significantly influences the mechanical properties of the entitled perovskites, leading to higher ductility and anisotropy. As a whole, this study offers insights into the scientific applications of non-toxic perovskites in different pressure environments.

Surprises in the theory of elasticity: pairwise atomic interactions, central forces, and Cauchy relations

Although the theory of elasticity has been well known for many years there are still some commonly accepted misconceptions that continue to be taught in solid-state physics courses. In this paper we review some of these misconceptions through a detailed study of the relationship between macroscopic and microscopic theories of elasticity in a simple-cubic crystal with one atom per primitive cell. The analysis is performed at different stages of complexity. In the first-neighbor approximation we find that the crystal is simply unstable. If pairwise interaction up to second neighbors is considered the crystal is stable but the elastic constants present additional symmetries known as Cauchy relations which are not observed experimentally. The reasons for this behavior are analyzed, pointing out that the invariance of the potential energy with respect to rotations implies necessarily that pairwise interactions must be central. Only if the atomic interactions involve the participation of 3-bodies or more, the forces are non-central and the resulting elastic tensor may be acceptable.

Quadrupole Coupling of Circular Rydberg Qubits to Inner Shell Excitations.

Divalent atoms provide excellent means for advancing control in Rydberg atom-based quantum simulation and computing due to the second optically active valence electron available. Particularly promising in this context are circular Rydberg atoms, for which long-lived ionic core excitations can be exploited without suffering from detrimental autoionization. Here, we report the implementation of electric quadrupole coupling between the metastable 4D_{3/2} level and a very high-n (n=79) circular Rydberg qubit, realized in doubly excited ^{88}Sr atoms prepared from an optical tweezer array. We measure the kHz-scale differential level shift on the circular Rydberg qubit via beat-node Ramsey interferometry comprising spin echo. Observing this coupling requires coherent interrogation of the Rydberg states for more than 100 μs, which is assisted by tweezer trapping and circular state lifetime enhancement in a black-body radiation suppressing capacitor. Further, we find no noticeable loss of qubit coherence under continuous photon scattering on the ion core, paving the way for laser cooling and imaging of Rydberg atoms. Our results demonstrate access to weak electron-electron interactions in Rydberg atoms and expand the quantum simulation toolbox for optical control of highly excited circular state qubits via ionic core manipulation.

Novel Schiff base decorated cyclotriphosphazene chemosensors for Fe and Cu ions detection

In this study, new 2-aminobenzothiazole derivative Schiff base decorated cyclotriphosphazene compounds (SBCTP 1 and 2), which are likely to have chemical sensor properties, were designed and synthesized successfully. The compounds were structurally characterized by mass analysis and NMR (1H, 13C and 31P) spectroscopies. Photophysical and chemosensory properties of SBCTP 1 and 2 against some analytes were examined by UV–vis and Fluorescence spectrophotometry. While a significant increase was observed in the UV–vis absorption signals observed at 350 nm with the addition of Fe3+ and Fe2+ ions and a new absorption band was observed at 290 nm with the addition of Cu2+. In addition, according to Job's plot obtained from UV–vis absorption titrations, the complex stoichiometries of SBCTP 1 and 2 with selective analytes were determined as 1:1 (L/M) and 1:2 (L/M), respectively. The selective interaction of donor atoms on SBCTP 1 and 2 with Cu2+, Fe2+ and Fe3+ ions give these compounds chemosensory properties. This study showed that the synthesized Schiff base decorated cyclotriphosphazene compounds (SBCTP 1 and 2) could be new chemosensors with high selective and immediate sensitivity for the detection of iron and copper ions.

CRYOCHEMICAL SYNTHESIS OF HYBRID NANOFORMS BASED ON SILVER AND THE ANTIBACTERIAL DRUG SUBSTANCE DIOXIDINE

Hybrid nanoforms based on silver and antibacterial drug dioxidine (2,3-bis-(hydroxymethyl)quinoxaline 1,4-di-N-oxide) were prepared by the method of joint co-condensation of metal and ligand vapors on a liquid nitrogen cooled surface. The samples obtained by low temperature co-condensation were characterized by FTIR-, UV-Vis and XPS-spectroscopy, ТЕМ, SEM and powder X-ray phase analysis (ХРА). It was shown that cryomodified nanoforms preferably consist of anhydrous triclinic (T-phase) crystal phase of dioxidine, the dimensions of dioxidine particles ranges from 50 to 300 nm, the average size of included silver nanoparticles is (15±3) nm. Broadening of the diffraction patterns belonging to silver shows the transition of metallic silver to the nanoscale state. The FTIR results indicate for hybrid nanoforms stabilized by donor-acceptor interactions of surface silver atoms with hydroxyl groups and with donor N-atoms of quinoxaline cycles of dioxidine molecules.

Nanowire arrays with abundant Cu–Ni interfaces for electroreduction of CO2 to ethylene

Electrochemical reduction of CO2 to ethylene (C2H4), driven by renewable electricity, represents a strategy for sustainable development and carbon neutrality. However, continuous production of C2H4 at high efficiency and low cost remains a significant challenge. Herein, a synergistic approach using non-precious metals was employed, and in situ construction of a nanoarray structure with abundant Cu–Ni interfaces (Ni/Cu NWs) on a gas diffusion layer (GDL) was performed. The atomic interactions at the interface significantly enhanced the efficiency of C–C coupling. The Faraday efficiency (FE) for C2H4 production reached 58.65 %, and the current density of 253.42 mA cm−2 at −1.1 V, markedly surpassing that of bare Cu nanowire (Cu NWs, 25.33 %). By virtue of the in-situ construction on the GDL, the Cu–Ni interface catalyst demonstrated excellent stability, operating under high current for more than 72 h. In situ infrared characterization and theoretical calculations demonstrate that the incorporation of Ni effectively enhanced the CO2 activation process, which is beneficial for the accumulation of key intermediate of C–C coupling. At the Cu–Ni interface, the energy barrier for C–C coupling was reduced, thereby effectively promoting the conversion of C2H4. This work presents a solution strategy for the interfacial engineering of non-precious metal catalysts.

The reverse-DADI method: Computation of frequency-dependent atomic polarizabilities for carbon and hydrogen atoms in hydrocarbon structures

A specific method, combining some ingredients of the well-known DDA and PDI approaches, has been developed in our group since many years to calculate the absorption cross-sections of carbonaceous nanoparticles based on their atomistic details. This method, here named the Dynamic Atomic Dipole Interaction (DADI) model, requires the knowledge of the position and frequency-dependent polarizability of each atom constituting the nanoparticles. While the atomic positions can be quite easily obtained, for example as the results of molecular dynamics simulations, obtaining the frequency-dependent atomic polarizabilities is a trickier task. Here, a fitting procedure, named the reverse-DADI method, has been applied to calculate the frequency-dependent atomic polarizability values for carbon and hydrogen atoms involved in aromatic cycles or in aliphatic chains, on the basis of frequency-dependent molecular polarizabilities of various PAH and alkane molecules, calculated with the TD-DFT theory, in the UV–Visible range. Then, using these frequency-dependent atomic polarizabilities as input parameters in the DADI model has been shown to lead to an accurate representation of the absorption cross-sections of various PAH and alkane molecules with respect to the corresponding values obtained at the TD-DFT level, with however the great advantage of a much shorter time of calculations. Furthermore, these results are indications of a good transferability of the frequency-dependent atomic polarizability values obtained here to any C or H atom of any PAH or alkane molecule. This opens the way for building large databases of optical properties for carbonaceous species of atmospheric or astrophysical interests.

Investigation of pH-dependent Paclitaxel delivery mechanism employing Chitosan-Eudragit bioresponsive nanocarriers: a molecular dynamics simulation

Before embarking on any experimental research endeavor, it is advisable to do a mathematical computation and thoroughly examine the methodology. Despite the use of polymeric nanocarriers, the regulation of bioavailability and drug release at the disease site remains insufficient. Several effective methods have been devised to address this issue, including the creation of polymeric nanocarriers that can react to stimuli such as redox potential, temperature, pH, and light. The present study has been utilized all-atom molecular dynamics (AA-MD) and coarse-grained molecular dynamics (CG-MD) methods and illustrated the drug release mechanism, which is influenced by pH, for Chitosan-Eudragit bioresponsive nanocarriers. The aim of current work is to study the molecular mechanism and atomistic interactions of PAX delivery using a Chitosan-Eudragit carrier. The ability of Eudragit polymers to dissolve in various organic solvents employed in the process of solvent evaporation is a crucial benefit in enhancing the solubility of pharmaceuticals. This study investigated the use of Chitosan-Eudragit nanocarriers for delivering an anti-tumor drug, namely Paclitaxel (PAX). Upon analyzing several significant factors affecting the stability of the drug and nanocarrier, it has been shown that the level of stability is more significant in the neutral state than the acidic state. Furthermore, the system exhibits higher stability in the neutral state. The used Chitosan-Eudragit nanocarriers exhibit a stable structure under alkaline conditions, but undergo deformation and release their payloads under acidic conditions. It was demonstrated that the in silico analysis of anti-tumor drugs and carriers’ integration could be quantified and validated by experimental results (from previous works) at an acceptable level.Graphical abstract