Atomic Polarization Research Articles

A Multipole-Based Reactive Force Field for Hydrocarbons.

The computational complexity of quantum chemistry methods has prompted the development of reactive force fields, facilitating practical applications of molecular dynamics simulations for large-scale reactive systems. Current reactive force fields typically employ intricate corrections based on prior chemical knowledge, which severely impedes their further advancement. This study presents a new atomic multipole-based reactive model with bond free (OPERATOR). The force field is constructed on a simple, physically motivated model within the AMOEBA framework that closely resembles the physical representation of the chemical reaction processes. In the force field, the atomic multipoles are generated dynamically according to the atomic environments, aiming to effectively capture significant changes in the electrostatic environments during chemical reactions. Subsequently, atomic multipole-based charge penetration, polarization, and charge transfer effects are incorporated into the force field to describe the complex electrostatic interactions in the system. The force field also includes van der Waals interactions and three-body potentials. In addition, to extend these nonreactive interactions to chemical reactions, the atom distribution multipole moments are used to characterize different chemical environments. The force field has been optimized using the dataset of potential energy surfaces (PESs) of hydrocarbons derived from DFT results of millions of conformations with six degrees of freedom (DOFs). The results demonstrate that the new force field effectively replicates both the monopoles and the energies. In comparison to ReaxFF, the new force field exhibits comparable or superior performance. Furthermore, molecular dynamics simulations of n-heptane decomposition effectively reproduce the primary products and reactions observed in the experiments. Given the simplicity and physically motivated nature of the model, it is expected that the new force field will be utilized in future studies to investigate chemical reaction mechanisms involving more elements.

Femtotesla atomic magnetometer with counter-propagating optical sideband pumping.

The ultrasensitive magnetometer has a vital importance in fundamental research and applications. Currently, the spin-exchange relaxation-free (SERF) atomic magnetometer has been reported with a sensitivity around the level of fT/Hz1/2. To enhance the sensitivity, a gradiometer configuration has usually been introduced to cancel the common-mode noise between two separate channels. However, the signal and response from different channels are not the same due to the attenuation of the pump beam. Here, we proposed a counter-propagating optical sideband pumping method to polarize the atoms, using the electro-optic modulator to modulate the single-pump beam, generating two symmetrically red- and blue-detuned sidebands of frequency. This scheme leads to a significant reduction of undesirable effects coming along with the optical pumping, such as light shifts and spatial inhomogeneity in atomic spin polarization. With the help of this pumping scheme, the two channels have the same magnetic response, and we have built a gradiometer atomic magnetometer with a sensitivity of 0.5 fT/Hz1/2 ranging from 5 to 40 Hz. Our results propose the possibility of creating larger arrays of atomic magnetometers (AMs) with high sensitivity and spatial resolution based on single-vapor cells for magnetocardiography and magnetoencephalography imaging or searching for exotic spin-dependent interactions.

Electrochemical Switching of Electromagnetism by Hierarchical Disorder Tailored Atomic Scale Polarization.

High-frequency electronic response governs a broad spectrum of electromagnetic applications from radiation protection, and signal compatibility, to energy recovery. Despite various efforts to manage electric conductivity, dynamic control over dielectric polarization for real-time electromagnetic modulation remains a notable challenge. Herein, an electrochemical lithiation-driven hierarchical disordering strategy is demonstrated for actively modulating electromagnetic properties. The controllable formation and diffusion of coherent interfaces and cation vacancies tailor the coupling of atomic electric field and thus the locally polarized domains, which leads to the reversible electromagnetic transparency/absorption switching with a tunable range of -0.8--20.4 dB for the reflection loss and a broad operation bandwidth of 4.6 GHz. Compared to traditional methods of heteroatomic doping, hydrogenation, mechanical deformation, and phase transition, the electrochemical strategy shows a larger regulation scope of dielectric permittivity with the maximum increase ratios of 260% and 1950% for real and imaginary parts, respectively. This enables the construction of various device architectures including the adaptive window and pixelated metasurface. The results offer opportunities to achieve intelligent electromagnetic devices and pave an avenue to rejuvenate various electromagnetic functions of semiconductive oxides.

Regulating Spin Polarization via Axial Nitrogen Traction at Fe−N5 Sites Enhanced Electrocatalytic CO2 Reduction for Zn−CO2 Batteries

AbstractSingle Fe sites have been explored as promising catalysts for the CO2 reduction reaction to value‐added CO. Herein, we introduce a novel molten salt synthesis strategy for developing axial nitrogen‐coordinated Fe‐N5 sites on ultrathin defect‐rich carbon nanosheets, aiming to modulate the reaction pathway precisely. This distinctive architecture weakens the spin polarization at the Fe sites, promoting a dynamic equilibrium of activated intermediates and facilitating the balance between *COOH formation and *CO desorption at the active Fe site. Notably, the synthesized FeN5, supported on defect‐rich in nitrogen‐doped carbon (FeN5@DNC), exhibits superior performance in CO2RR, achieving a Faraday efficiency of 99 % for CO production (−0.4 V vs. RHE) in an H‐cell, and maintaining a Faraday efficiency of 98 % at a current density of 270 mA cm−2 (−1.0 V vs. RHE) in the flow cell. Furthermore, the FeN5@DNC catalyst is assembled as a reversible Zn−CO2 battery with a cycle durability of 24 hours. In situ IR spectroscopy and density functional theory (DFT) calculations reveal that the axial N coordination traction induces a transformation in the crystal field and local symmetry, therefore weakening the spin polarization of the central Fe atom and lowering the energy barrier for *CO desorption.

Regulating Spin Polarization via Axial Nitrogen Traction at Fe-N5 Sites Enhanced Electrocatalytic CO2 Reduction for Zn-CO2 Batteries.

Single Fe sites have been explored as promising catalysts for the CO2 reduction reaction to value-added CO. Herein, we introduce a novel molten salt synthesis strategy for developing axial nitrogen-coordinated Fe-N5 sites on ultrathin defect-rich carbon nanosheets, aiming to modulate the reaction pathway precisely. This distinctive architecture weakens the spin polarization at the Fe sites, promoting a dynamic equilibrium of activated intermediates and facilitating the balance between *COOH formation and *CO desorption at the active Fe site. Notably, the synthesized FeN5, supported on defect-rich in nitrogen-doped carbon (FeN5@DNC), exhibits superior performance in CO2RR, achieving a Faraday efficiency of 99 % for CO production (-0.4 V vs. RHE) in an H-cell, and maintaining a Faraday efficiency of 98 % at a current density of 270 mA cm-2 (-1.0 V vs. RHE) in the flow cell. Furthermore, the FeN5@DNC catalyst is assembled as a reversible Zn-CO2 battery with a cycle durability of 24 hours. In situ IR spectroscopy and density functional theory (DFT) calculations reveal that the axial N coordination traction induces a transformation in the crystal field and local symmetry, therefore weakening the spin polarization of the central Fe atom and lowering the energy barrier for *CO desorption.

Atomic-level quantitative analysis of electronic functional materials by aberration-corrected STEM

Abstract The stable sub-angstrom resolution of the aberration-corrected scanning transmission electron microscope (AC-STEM) makes it an advanced and practical characterization technique for all materials. Owing to the prosperous advancement in computational technology, specialized software and programs have emerged as potent facilitators across the entirety of electron microscopy characterization process. Utilizing advanced image processing algorithms promotes the rectification of image distortions, concurrently elevating the overall image quality to superior standards. Extracting high-resolution, pixel-level discrete information and converting it into atomic-scale, followed by performing statistical calculations on the physical matters of interest through quantitative analysis, represent an effective strategy to maximize the value of electron microscope images. The efficacious utilization of quantitative analysis of electron microscope images has become a progressively prominent consideration for materials scientists and electron microscopy researchers. This article offers a concise overview of the pivotal procedures in quantitative analysis and summarizes the computational methodologies involved from three perspectives: contrast, lattice and strain, as well as atomic displacements and polarization. It further elaborates on practical applications of these methods in electronic functional materials, notably in piezoelectrics/ferroelectrics and thermoelectrics. It emphasizes the indispensable role of quantitative analysis in fundamental theoretical research, elucidating the structure–property correlations in high-performance systems, and guiding synthesis strategies.

A new experimental method to study the flame inhibition performance of low concentration halogenated gas

The minimum fire extinguishing concentration is a key index for the development of next generation chemical clean fire extinguishing gases, which is usually got by the cup-burner. The fire suppression performance of low concentration of chemical gas is hard to be understood by the available methods. In this work, the fundamental acknowledgement of steady flame surface attacking mechanism by halon functional group is newly discussed by conducting a series of bench scale tests with a cylindrical channel under a varied fluorinated gases. The characteristics of flame propagation under differentiated air atmosphere environmental conditions is obtained. The influence of fluorine-containing gas flow rate on flame propagation speed is clarified. A dimensionless relationship including atomic radius, bond length, polarization degree, molar mass and molar volume are proposed to describe the influence of low concentration of fluorine-containing gas on flame propagation speed. It provides an insight for the understanding of the flame inhibition performance of low concentration halogenated gas.

Identification and Manipulation of Atomic Polarization Moments for Nonlinear Magneto‐Optical Rotation Atomic Magnetometers

AbstractPolarization moments play a crucial role in measuring magnetic fields for nonlinear magneto‐optical rotation (NMOR) atomic magnetometers. However, it is challenging to distinguish between each polarization moment and evaluate its effect on the magnetic resonance response signal in an alkali vapor cell with buffer gas. To address this issue, a method is proposed to identify different polarization moments through the frequency shift of the magnetic resonance response signal. The proportion of each polarization moment is determined, and it is demonstrated that the magnetic resonance response signal is affected by the hexadecapole moment, resulting in a frequency shift and a decrease in signal amplitude. To mitigate this effect, an approach is investigated to manipulate the polarization moments by flipping the phase of the pump light. Ultimately, a 15.19% increase in response amplitude is achieved in the simulated geomagnetic environment within the magnetic shield barrel. The theory and method presented here provide strong support for the study of the polarization moments in an alkali vapor cell with buffer gas, which potentially enhance the performance of NMOR atomic magnetometers.

Adhesion promotion and corrosion resistance of mixed phosphonic acid monolayers on AA 2024

Mixed monolayers were used to prepare surfaces of AA 2024 with precisely controlled corrosion protective and adhesive properties. In this study, the corrosion inhibition and adhesion promotion as a function of the composition of mixed phosphonic acid monolayers on AA 2024 was investigated. Mixed monolayers were formed by competitive adsorption of n-dodecylphosphonic acid (DPA) and 12-aminododecylphosphonic acid (ADPA) from ethanolic solution. Their compositions were determined by X-ray photoelectron spectroscopy. Atomic force microscopy studies and polarization modulation infrared reflection–absorption spectroscopy as well as contact angle studies proved the formation of monolayers with varying surface chemistry. The wet-adhesion strength was tested by 90° peel tests after application of an epoxy-amine adhesive. Linear sweep voltammetry was performed to evaluate the corrosion inhibition of the monolayers, and the corrosion resistance of the metal/adhesive composite was investigated by means of its corrosive delamination behavior. The electrochemical measurements demonstrated that reducing the surface concentration of ADPA improved the corrosion inhibition of the monolayer. However, the corrosive delamination experiments revealed that the improved corrosion inhibition by the self-organized DPA is of minor importance for the corrosion behavior of the metal/adhesive composite, as the adhesive properties dominate.

Bidentate mode coordinated Ti3CNTx MXene-controlled interfacial engineering enables high-performance indoor organic photovoltaic devices

Two-dimensional MXenes demonstrate exceptional optoelectronic properties and tunable surface terminations, making them highly desirable materials for advanced organic photovoltaic (OPV) devices in indoor settings. This study introduced a solution-processed hybrid hole-transport layer (HTL) composed of a blend of 2-(9H-carbazol-9-yl)ethyl]phosphonic acid and titanium carbonitride (2PACz–Ti3CNTx). Introducing Ti3CNTx into 2PACz enhanced the work function for improved hole transport and also induced molecular alignment and interface dipole changes via formation of Ti–O–P covalent bond. This synergistic interaction led to atomic charge polarization, improving the hole-transport kinetics at the heterointerface of 2PACz and Ti3CNTx. Furthermore, the large surface area of conductive MXene and its chemical interaction with π-conjugated 2PACz promote the conductivity and charge-transfer pathways, improving the device’s performance. Consequently, OPV devices employing 2PACz–Ti3CNTx HTLs achieved the maximum power conversion efficiency of 30.3 % under a light-emitting diode lamp (1000 lx) and an output power density of 413 µW·cm−2 under a halogen lamp (1000 lx), corresponding to enhancements of approximately 16 % and 12 %, respectively, compared to OPV devices based on undoped HTLs. These results highlight new opportunities for further exploration of MXene compositions in high-performance indoor OPV devices.

Tunable atomic spontaneous radiation in cylindrical waveguide

The chiral interaction between light and matter has brought chiral quantum optics into a flourishing stage. Here, we explore the perfect chiral interaction between the atoms with elliptically polarized dipoles and waveguide modes, and find that ideal unidirectional radiation can be obtained by adjusting the position and polarization of atoms. When there are two waveguide modes in the system, by controlling the polarization of the dipoles, the dipoles can radiate not only the unidirectional single waveguide mode, but also two seperated waveguide modes.

Real-time measurement of pump beam polarization through the transmitted light intensity in a polarized alkali metal vapor cell.

A laser beam with left-/right-handed circular polarization is generally used to create the oriented atomic spins for precision measurements in a spin-exchange relaxation-free (SERF) co-magnetometer. The fluctuation of laser polarization interferes with the spin polarization of alkali metal atoms, leading to the system performance degradation. Here, we report a method for real-time polarization state measurement by using the transmitted light intensity of the pump beam passing through the vapor cell. Based on the principle of circular dichroism, the optical absorption model of polarized alkali metal atoms is established. The simulation results of the transmittance of the pump laser with different polarization states through the alkali metal vapor cell are given and verified by experiments. The experimental results show that the circularly polarized beam has the weakest absorption, while the linearly polarized laser beam is absorbed the strongest. The achieved measurement accuracy stands at an impressive 98.83 %. This work provides a simple and easy-to-use way to measure the polarization state of the laser beam used in the vapor cell devices, particularly the microfabricated prototypes with limited space.

The Xe isotope nuclear resonance frequency shift of NMR angular velocity sensors due to transverse gradient magnetic fields

The nuclear magnetic resonance (NMR) angular velocity sensor detects angular velocity by measuring the shift in the nuclear spin precession frequency, which is of fundamental interest. Recent studies have revealed the parameter dependency of nuclei frequency shifts induced by non-uniformly distributed polarized pump beams, temperature, and magnetic field properties. In this study, we investigated the effect of the linear transverse gradient magnetic field on the frequency ratio shift of the Xe isotope nuclear resonance frequency in the NMR sensors. A theoretical analysis method was proposed based on the Fermi contact interaction in atomic polarization and the spin-diffusion relaxation of 129Xe and 131Xe nuclei. The frequency ratio shift of the Xe isotope under different x-axis gradient magnetic fields was measured experimentally. Furthermore, we eliminated the equivalent residual magnetic field through a feedback system and compensated for the original gradient magnetic field in the system, which contributed to accurately revealing the frequency shift induced by the magnetic field gradient. The results indicate that the frequency ratio shift of the Xe isotope is proportional to the strength of the second-order linear transverse gradient magnetic field. This study provides a reference for the analysis and evaluation of the presence of the gradient magnetic field in the NMR angular velocity sensor.

Protruding‐Shaped Co Polarization Field on Ultrathin Covalent Triazine Framework Nanosheets for Efficient CO2 Photoreduction

AbstractSingle‐atom photocatalysts (SAPs) engineered on various supports offer a promising pathway to efficiently convert CO2 into high‐valued products. However, most SAPs with near‐planar metal atom coordination structure suffer from low conversion efficiency, mainly due to the weak local polarized electric field which retards the reaction kinetics. Herein, this study reports for the first time a photocatalyst which simultaneously integrates protruding‐shaped Co single atom and strong polarization field in ultrathin crystalline covalent‐triazine‐framework nanosheets (donate as Co1/CTF‐NSs). Both experimental results and theoretical simulations demonstrated that giant local polarization field is successfully triggered on the Co1/CTF‐NSs, which induced directional charge migration and greatly promoted the separation of photogenerated carriers. The protruding‐Co centers enhanced the overlap between CO2 2p and Co 3d orbitals, thereby facilitating a strong affinity for CO2 adsorption. Furthermore, the local polarization fields between the protruding‐Co and CO2 drove the injection of a substantial number of electrons from Co 3d into CO2 π antibonding orbitals, leading to the effective activation and reduction of the CO2 molecules. Consequently, the as‐synthesized Co1/CTF‐NSs exhibited a remarkable CO production rate of 5391 µmol g−1 h−1 and a high selectivity (97.3%) under visible light irradiation, which represents one of the best molecular framework photocatalysts to date.

Tilting and Distortion in the Multiferroic Aurivillius Phase Bi6Ti3Fe1.5Mn0.5O18.

Aurivillius structured Bi6Ti3Fe1.5Mn0.5O18 (B6TFMO) has emerged as a rare room temperature multiferroic, exhibiting reversible magnetoelectric switching of ferroelectric domains under cycled magnetic fields. This layered oxide presents exceptional avenues for advancing data storage technologies owing to its distinctive ferroelectric and ferrimagnetic characteristics. Despite its immense potential, a comprehensive understanding of the underlying mechanisms driving multiferroic behavior remains elusive. Herein, we employ atomic resolution electron microscopy to elucidate the interplay of octahedral tilting and atomic-level structural distortions within B6TFMO, associating these phenomena with functional properties. Fundamental electronic features at varying bonding environments within this complex system are scrutinized using electron energy loss spectroscopy (EELS), revealing that the electronic nature of the Ti4+ cations within perovskite BO6 octahedra is influenced by position within the Aurivillius structure. Layer-by-layer EELS analysis shows an ascending crystal field splitting (Δ) trend from outer to center perovskite layers, with an average increase in Δ of 0.13 ± 0.06 eV. Density functional theory calculations, supported by atomic resolution polarization vector mapping of B-site cations, underscore the correlation between the evolving nature of Ti4+ cations, the extent of tetragonal distortion and ferroelectric behavior. Integrated differential phase contrast imaging unveils the position of light oxygen atoms in B6TFMO for the first time, exposing an escalating degree of octahedral tilting toward the center layers, which competes with the magnitude of BO6 tetragonal distortion. The observed octahedral tilting, influenced by B-site cation arrangement, is deemed crucial for juxtaposing magnetic cations and establishing long-range ferrimagnetic order in multiferroic B6TFMO.

Manipulating optical absorption and polarization using microwave control in an atomic vapor

The multiplicity of atomic states (and the transitions between them) offer an innate, coherent platform through which microwave and optical fields effectively interact. In an atomic vapor near room temperature, we combine optical and microwave fields to generate a macroscopic internal angular momentum among the atoms—an atomic polarization—at an arbitrary angle with respect to the optical (laser) beam. This geometric freedom enables microwave control over photonic degrees of freedom, which we use in two demonstrations: using microwave-assisted optical pumping, we can rotate linear polarization through several degrees, and we can control the absorption for specific transitions and polarizations, which has applications for microwave-to-optical transduction.

Analysis of effect of pump light wavelength on the magnetic noise suppression of the SERF co-magnetometer

Spin Exchange Relaxation-Free Co-Magnetometer (SERFCM) possesses ultra-sensitive rotation measurement capabilities, offering broad application prospects in inertial navigation and fundamental physics research. Precision of SERFCM in rotation measurements is directly influenced by its ability to suppress magnetic noise. In this study, a state-space method is used to establish a SERFCM response model, considering the effect of pump light wavelength. An analysis is conducted to assess the effect of pump light wavelength detuning on the ability to suppress magnetic noise of SERFCM. Theoretical results indicate that detuned pump light wavelength can effectively reduce the magnetic field gradient generated by atomic polarization, thereby improving overall system performance. Experimental validation demonstrates that a slight detuning of the pump light wavelength results in a 21% improvement in the ability to suppress low-frequency magnetic fields.

Measuring the Optical Concurrence of Vector Beams with an Atomic-State Interferometer

We investigate the transmission of vector beams, correlated in their polarization and spatial degrees of freedom, through cold atoms in the presence of a transverse magnetic coupling field. The resulting phase-dependent dynamics allow us to imprint the spatially varying polarization of a vector beam onto atomic spin polarizations, thereby establishing a direct link between optical space-polarization correlations and atomic-state interference. We find that the resulting absorption profiles show interference fringes whose modulation strength is given by the squared concurrence of the vector beam, letting us identify optical concurrence from a single absorption image. We expect impact across a diverse range of applications, including spintronics, quantum memories, metrology, and clocks. Published by the American Physical Society 2024

Ground state of two-species spin–orbit-coupled in mass-imbalanced Bose condensates

In this paper, we study the ground state of two-component spin–orbit-coupled (SOC) Bose–Einstein condensates with mass imbalance. Our results are based on the framework of mean-field Gross–Pitaevskii theory. The effects of unequal atomic mass and SOC strength are studied. Different density structures such as heliciform stripes, linear stripes and string vortex chains are found. Different density structures such as heliciform stripes, linear stripes and string vortex chains are found. With the increase of SOC strength, the azimuthal phase separation is kept while radial phase separation is broken. In addition, increasing the mass ratio is unfavorable to vortex formation, whereas more vortices can be generated by increasing the SOC strength. We also discuss the physical quantities such as angular momentum per atom and spin polarisation, for a larger mass ratio, showing that angular momentum gets a little bigger as the SOC strength increases and the first-order phase transition does not exist.

Uniform optically pumped spin-exchange relaxation-free comagnetometer based on optical compensation

In the spin-exchange relaxation-free (SERF) comagnetometer, the atomic polarization gradient caused by light absorption can cause significant but unexpected nuclear spin transverse relaxation, which affects the system’s accuracy and sensitivity. This paper proposes the SERF comagnetometer configuration based on optical compensation to suppress polarization gradient in the vapor cell. The influence of polarization gradient on the system’s magnetic field suppression ability is analyzed by the state-space method. In addition, the atomic polarization distribution simulation and the performance testing between the traditional SERF comagnetometer and the proposed configuration are conducted. Compared to traditional configuration, the polarization gradient relaxation of the proposed configuration is effectively suppressed by 62%, the magnetic field suppression ability of the system is improved by 51%, and the rotation sensitivity is increased by 25.4%. This work investigates the influence of polarization gradient on system characteristics and proposes a comagnetometer configuration to suppress polarization gradient, enhancing the system’s magnetic field suppression ability and improving sensitivity. The demonstration of the polarization gradient suppression method is of significance for improving the performance of other inertial measurement devices such as nuclear magnetic resonance gyroscopes.