Charge Dynamics Research Articles

Elucidating Li+‐Ion Interactions with Ethylene Carbonate: Insights from Vibrational Infrared Spectroscopy, Electron Affinity Analysis, and Charge Dynamics to Enhance Lithium‐Ion Battery Performance

Elucidating Li⁺‐Ion Interactions with Ethylene Carbonate: Insights from Vibrational Infrared Spectroscopy, Electron Affinity Analysis, and Charge Dynamics to Enhance Lithium‐Ion Battery Performance

Imaging hot photocarrier transfer across a semiconductor heterojunction with ultrafast electron microscopy

Semiconductor heterojunctions have gained significant attention for efficient optoelectronic devices owing to their unique interfaces and synergistic effects. Interaction between charge carriers with the heterojunction plays a crucial role in determining device performance, while its spatial-temporal mapping remains lacking. In this study, we employ scanning ultrafast electron microscopy (SUEM), an emerging technique that combines high spatial-temporal resolution and surface sensitivity, to investigate photocarrier dynamics across a Si/Ge heterojunction. Charge dynamics are selectively examined across the junction and compared to far bulk areas, through which the impact of the built-in potential, band offsets, and surface effects is directly visualized. In particular, we find that the heterojunction drastically modifies the hot photocarrier diffusivities in both Si and Ge regions due to charge trapping. These findings are further elucidated with insights from the band structure and surface potential measured by complementary techniques. This work demonstrates the tremendous effect of heterointerfaces on hot photocarrier dynamics and showcases the potential of SUEM in characterizing realistic optoelectronic devices.

Origins of Electromagnetic Radiation from Spintronic Terahertz Emitters: A Time-Dependent Density Functional Theory plus Jefimenko Equations Approach.

Microscopic origins of charge currents and electromagnetic (EM) radiation generated by them in spintronic THz emitters-such as, femtosecond laser pulse-driven single magnetic layer or its heterostructures with a nonmagnetic layer hosting strong spin-orbit coupling (SOC)-remain poorly understood despite nearly three decades since the discovery of ultrafast demagnetization. We introduce a first-principles method to compute these quantities, where the dynamics of charge and current densities is obtained from real-time time-dependent density functional theory, which are then fed into the Jefimenko equations for properly retarded electric and magnetic field solutions of the Maxwell equations. By Fourier transforming different time-dependent terms in the Jefimenko equations, we unravel that in the 0.1-30THz range the electric field of far-field EM radiation by the Ni layer, chosen as an example, is dominated by charge current pumped by demagnetization, while often invoked magnetic dipole radiation from the time-dependent magnetization of a single magnetic layer is a negligible effect. Such an effect of charge current pumping by a time-dependent quantum system, whose magnetization is shrinking while its vector does not rotate, does not require any spin-to-charge conversion via SOC effects. In the Ni/Pt bilayer, EM radiation remains dominated by the charge current within the Ni layer, whose magnitude is larger than in the case of a single Ni layer due to faster demagnetization, while often invoked spin-to-charge conversion within the Pt layer provides an additional but smaller contribution. By using the Poynting vector and its flux, we also quantify the efficiency of conversion of light into emitted EM radiation, and its angular distribution.

Quantum Spin Probe of Single Charge Dynamics.

Electronic defects in semiconductors form the basis for emerging quantum technologies, but many defect centers are difficult to access at the single-particle level. A method for probing optically inactive spin defects would reveal semiconductor physics at the atomic scale and advance the study of new quantum systems. We exploit the intrinsic correlation between the charge and spin states of defect centers to measure the charge populations and dynamics of single substitutional nitrogen spin defects in diamond. By probing their steady-state spin population, read out at the single-defect level with a nearby nitrogen vacancy center, we directly measure the defect ionization-corroborated by first-principles calculations-an effect we do not have access to with traditional coherence-based quantum sensing.

Simulation of the effect of temperature on space charge transport in LDPE under DC electric field stress

Polymers are considered essential materials used in high-voltage direct current (HVDC) applications due to their excellent insulating properties. They are widely employed in various electrical equipment such as cables, transformers, and station insulators, providing effective protection against high currents and voltages. One of the main challenges in these applications is the effect of temperature on the performance of these insulators, as elevated temperatures can alter the electrical properties of polymers, potentially impacting the dynamics of electric charges within the material. In this work, bipolar charge transport (BCT) was used to study the effect of temperature on the dynamics of space charge in LDPE under a DC electric field. The model includes processes such as injection, migration, trapping, detrapping, and recombination. We applied a DC electric field of 50 kV/mm to low-density polyethylene (LDPE) films for 2 hours under different temperatures. The results indicate that higher temperatures significantly enhance charge mobility, leading to improved charge flux, reduced trapping, and increased detrapping of charges. This results in a more uniform distribution of the electric field within the material and a quicker transition to a steady-state condition. The increase in temperature within the applied electric field created a relative balance between trapped charge and mobile charge, indicating a positive effect of higher temperatures on the electrical insulation properties of LDPE.

Transient Electroluminescence Spectroscopy in Planar Electroluminescent Devices

AbstractThe emergence of planar electroluminescent diodes (including polymer light‐emitting diodes, organic light‐emitting diodes, quantum‐dot light‐emitting diodes, and perovskite light‐emitting diodes) is causing a revolution in displays, lighting, and wearable electronic devices. Continuous advancement in the comprehension and management of charge carrier dynamics in these devices has led to several significant breakthroughs, including diodes with ultrahigh luminance, memory devices, and amplified spontaneous emission. Transient electroluminescence (TrEL) spectroscopy is a relative powerful technology to investigate charge dynamics, including transport, distribution, and storage of charge carriers, in electrically‐driven planar light‐emitting diodes (LEDs). The aim of this review is to revisit the principle and applications of TrEL spectroscopy in planar electroluminescent diodes, and to evaluate the reliability of various parameters extracted using this technology. A particular focus is on electroluminescence response time, charge‐carrier transport and storage, and exciton species. First, the principle and equipment system of the TrEL, as well as specific attention during TrEL measurements are described in detail, following by the applications TrEL spectroscopy in planar LEDs. Further development on the TrEL technology is discussed in the third section. Finally, a summary and outlook for the TrEL are shown and challenges faced by the TrEL spectroscopy are also highlighted.

Linkage Regulation of Back‐To‐Back Connected Dimers as Guest Acceptors Enables Organic Solar Cells with Excellent Efficiency, Stability and Flexibility

AbstractHigh efficiency, stability, and flexibility are key prerequisites for the commercial applications of organic solar cells (OSCs). Herein, three back‐to‐back connected dimers (2Qx‐TT, 2Qx‐C3, 2Qx‐C6) are developed as the guest acceptors for OSCs with improved comprehensive performance. By regulating the linkage from rigid bithiophene to flexible alkyl chain, the back‐to‐back connected dimers display quite different molecular geometry and intermolecular interactions, consequently influencing their packing arrangement, film‐forming process, carrier mobilities, and the device efficiency, stability, and flexibility. By introducing these dimer acceptors as the guest into active layer, these dimers form alloy phases with the host acceptor, promoting film‐forming process and charge dynamics. All ternary devices exhibit improved PCEs of over 18% than the control binary device. Among them, 2Qx‐C3‐based ternary device obtains the best efficiency of as high as 19.03%. Moreover, thanks to the stronger entanglement favored by the dimers with flexible linkage, the PM6:BTP‐eC9:2Qx‐C3‐based device shows outstanding stability and flexibility. The flexible device displays an improved PCE of 16.09% with a crack‐onset strain of 15.0%, showing excellent mechanical robustness close to the all‐polymer devices. This work demonstrates the potential of the back‐to‐back connected dimer acceptors as the guest for highly efficient, stable and flexible OSCs.

Charge and Spin Dynamics and Destabilization of Shallow Nitrogen-Vacancy Centers under UV and Blue Excitation.

Shallow nitrogen-vacancy (NV) centers in diamond offer opportunities to study photochemical reactions, including photogeneration of radical pairs, at the single-molecule regime. A prerequisite is a detailed understanding of charge and spin dynamics of NVs exposed to the short-wavelength light required to excite chemical species. Here, we investigate the charge and spin dynamics of shallow NVs under 445 and 375 nm illumination. With blue excitation, charge-state preparation is power-dependent, and modest spin initialization fidelity is observed. Under UV excitation, charge-state preparation is power-independent and no spin polarization is observed. Aging of NVs under prolonged UV exposure manifests in a reduced charge stability and spin contrast. We attribute this aging to modified local charge environments of near-surface NVs and identify distinct electronic traps only accessible at short wavelengths. Finally, we evaluate the prospects of NVs to probe photogenerated radical pairs based on measured sensitivities and outline possible sensing schemes.

Coupling monoclinic Pb2(CrO4)O with Mn3O4 quantum dots as oxygen vacancies-rich S-scheme photocatalysts for visible-light-driven photocatalytic CO2 reduction with H2O

Simulating natural photosynthesis to convert CO2 and H2O into fuels achieving overall reaction is a promising solution for addressing environmental problems and energy crises. Constructing an S-scheme catalyst of two or more catalytic sites with rapid electron transfer and strong redox capability may be an effective strategy for coupling photocatalytic CO2 reduction and H2O oxidation. Here, an oxygen vacancies-rich S-scheme semiconductor photocatalyst composed of monoclinic lead chromate oxide (Pb2(CrO4)O) coupled with Mn3O4 quantum dots (QDs) (Pb2(CrO4)O@Mn3O4QDs) are synthesized and tested for photoconversion of CO2 with H2O under visible light. Through the integration of Pb2(CrO4)O with Mn3O4QDs, the photocatalytic C1-evolution rate on Pb2(CrO4)O@Mn3O4QDs is radically increased by 6.0 and 8.1 times, which is much faster than that of pristine Pb2(CrO4)O and Mn3O4. The origin of the greatly raised activity is revealed by advanced characterizations, and in situ X-ray photoelectron spectroscopy (XPS) confirms the electron transport pathway in Pb2(CrO4)O@Mn3O4QDs with light illumination, unveiling the efficient spatial separation/transfer of charge carriers in oxygen vacancies-rich Pb2(CrO4)O@Mn3O4QDs S-scheme heterojunction. Consequently, powerful photoelectrons and holes accumulate in the Mn3O4 conduction band and Pb2(CrO4)O valence band, respectively, exhibiting prolonged long lifetimes and facilitating their involvement in CO2 photoreduction and H2O photooxidation through altering the interfacial charge dynamics.

Enhancing Detection Frequency and Reducing Noise Through Continuous Structures via Release-Controlled Transfer Toward Light-Based Wireless Communication.

Organic photodetectors (OPDs) have received considerable attention owing to their superior absorption coefficient and tunable bandgap. The introduction of bulk-heterojunction (BHJ) structure aims to maximize charge generation, however, its response speed is constrained by the random distribution of donor and acceptor. Herein, a multiple-active layer design consisting of a single acceptor layer and a bulk-heterojunction layer (A/BHJ structure) is introduced, which combines the benefits of both the planar junction and the BHJ, improving photo-sensing. A transfer process is employed for this structure, which involves calculating the energy release rate at each interface, considering temperature and velocity. Consequently, the OPD with the A/BHJ structure is successfully fabricated through transfer printing, resulting in reduced dark current, superior detectivity (1.06 × 1013 Jones), and rapid response, achieved by creating a high hole injection barrier and suppressing trap sites within the interfaces. By thoroughly investigating charge dynamics in the structure, the A/BHJ structure-based OPD attains large bandwidth detection with high signal-to-noise. An efficient wireless data communication system with digital-to-analog conversion is showcased using the A/BHJ structure-based OPD.

Spin and charge dynamics of doped one-dimensional Mott insulators

Spin and charge dynamics of doped one-dimensional Mott insulators

Triadic Halobenzene Processing Additive Combined Advantages of Both Solvent and Solid Types for Efficient and Stable Organic Solar Cells.

Solvent additives with a high boiling point (BP) and low vapor pressure (VP) have formed a key handle for improving the performance of organic solar cells (OSCs). However, it is not always clear whether they remain in the active-layer film after deposition, which can negatively affect the reproducibility and stability of OSCs. In this study, an easily removable solvent additive (4-chloro-2-fluoroiodobenzene (CFIB)) with a low BP and high VP is introduced, behaving like volatile solid additives that can be completely removed during the device fabrication process. In-depth studies of CFIB addition into the D18-Cl donor and N3 acceptor validate its dominant non-covalent intermolecular interactions with N3 through effective electrostatic interactions. Such phenomena improve charge dynamics and kinetics by optimizing the morphology, leading to enhanced performance of D18-Cl:N3-based devices with a power conversion efficiency of 18.54%. The CFIB-treated device exhibits exceptional thermal stability (T80 lifetime = 120h) at 85°C compared with the CFIB-free device, because of its morphological robustness by evolving no residual CFIB in the film. The CFIB features a combination of advantages of solvent (easy application) and solid (high volatility) additives, demonstrating its great potential use in the commercial mass production of OSCs.

Unified Crystal Phase Control with MACl for Inducing Single-Crystal-Like Perovskite Thin Films in High-Pressure Fusion Toward High Efficiency Perovskite Solar Cell Modules.

Perovskite solar cells, recognized for their high photovoltaic conversion efficiency (PCE), cost-effectiveness, and simple fabrication, face challenges in PCE improvement due to structural defects in polycrystalline films. This study introduces a novel fabrication method for perovskite films using methylammonium chloride (MACl) to align grain orientation uniformly, followed by a high-pressure process to merge these grains into a texture resembling single-crystal perovskite. Employing advanced visual fluorescence microscopy, charge dynamics in these films are analyzed, uncovering the significant impact of grain boundaries on photo-generated charge transport within perovskite crystals. A key discovery is that optimal charge transport efficiency and speed occur in grain centers when the grain size exceeds 10µm, challenging the traditional view that efficiency peaks when grain size surpasses film thickness to form a monolayer. Additionally, the presence of large-sized grains enhances ion activation energy, reducing ion migration under light and improving resistance to photo-induced degradation. In application, a perovskite solar cell module with large grains achieve a PCE of 22.45%, maintaining performance with no significant degradation under continuous white LED light at 100 mA cm-2 for over 1000h. This study offers a new approach to perovskite film fabrication and insights into optimizing perovskite solar cell modules.

Exploring a novel feature of ellis spacetime: Insights into scalar field dynamics

We have studied neutral and charged massive particles dynamics in Ellis spacetime in the presence of the external scalar field. Focusing on the circular motion of massive particles, the impact of an external scalar field on the Innermost Stable Circular Orbit (ISCO) position is analyzed, revealing a non-linear relationship with the scalar field parameter. Perturbation techniques are employed to investigate oscillatory motion near stable orbits in the Ellis spacetime, yielding analytical expressions for radial and angular oscillations. The throat of the wormhole has been constrained by comparing theoretical and observational results for fundamental frequencies of particles from quasars. Finally, scalar and gravitational perturbations in the Ellis spacetime have been studied. It is shown that the equation for the scalar profile function is fully independent from the tensor functions and the solution can be represented in terms of the confluent Heun function. However, it has been shown that equations for the tensor profile functions strongly depend on the scalar profile functions in the Ellis spacetime and they are reduced to the Regge–Wheeler–Zerilli equation. Finally, numerical solutions to the Regge–Wheeler–Zerilli equation for the radial functions in the Ellis have been presented.

SPICE Simulation Assisted-Dynamic Rds(on) Characterization in 200V Commercial Schottky p-GaN HEMTs Under Unstable Phases

Abstract This paper presents a comprehensive analysis of dynamic and static RDS(ON) in Schottky p-GaN High Electron Mobility Transistors (HEMTs), highlighting the impact of off-state and hot electron trapping on device performance. The authors observed significant hysteresis in the transfer characteristics of a 200V commercial Schottky p-GaN, attributing this to charge trapping effects. A novel experimental setup, employing a multi-pulse test synchronous buck converter circuit with additional gate control and a clamping circuit, enabled precise characterization of dynamic RDS(ON) under varying conditions, including unstable phases with overcurrent. This method effectively mimics solar PV input scenarios, exposing the device to high dv/dt and di/dt stresses, which are critical for evaluating GaN device stability under transient conditions. This research also reveals that increased gate resistance reduces energy losses, challenging traditional expectations by demonstrating the nuanced gate charge dynamics of GaN HEMTs. This study overall contributes to the understanding of GaN device behavior, offering a novel approach for accurately characterizing dynamic RDS(ON) under unstable stages, furtherly advances the GaN device in complex renewable energy power converter applications.

Electronic correlations and partial gap in the bilayer nickelate La3Ni2O7

The discovery of superconductivity with a critical temperature of about 80 K in La3Ni2O7 single crystals under pressure has received enormous attention. La3Ni2O7 is not superconducting under ambient pressure but exhibits a transition at T ∗ ≃ 115 K. Understanding the electronic correlations and charge dynamics is an important step towards the origin of superconductivity and other instabilities. Here, our optical study shows that La3Ni2O7 features strong electronic correlations which significantly reduce the electron’s kinetic energy and place this system in the proximity of the Mott phase. The low-frequency optical conductivity reveals two Drude components arising from multiple bands at the Fermi level. The transition at T ∗ removes the Drude component exhibiting non-Fermi liquid behavior, whereas the one with Fermi-liquid behavior is barely affected. These observations in combination with theoretical results suggest that the Fermi surface dominated by the Ni-d3z2−r2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${d}_{3{z}^{2}-{r}^{2}}$$\\end{document} orbital is removed due to the transition at T ∗. Our experimental results provide pivotal information for understanding the transition at T ∗ and superconductivity in La3Ni2O7.

Cathodoluminescence of polarization-induced energy states at AlGaN/GaN interface

Abstract Recent progress in manufacturing high-electron-mobility transistors and optoelectronic devices highlights the necessity of understanding the charge dynamics and its impact on the optical properties inside heterostructures. Herein, we study the optical properties of GaN / A l 0.23 G a 0.77 N / GaN heterostructures using cathodoluminescence (CL) and photoluminescence (PL) spectroscopy. We explore the influence of generated secondary carriers after electron illumination and their penetration depth on the luminescence spectra. Our findings indicate that a higher laser power intensifies the PL response and establishes Fabry–Perot-like resonances. Furthermore, the intensity of the CL response shows a linear behavior versus the acceleration voltage and the current of electron beams for the yellow luminescence peak. A near-infrared CL peak (740 nm) is observed only when illuminating the sample with high currents that is attributed to the trapping of the secondary electrons within the Schottky barrier and the manipulation of the two-dimensional electron gas and the quantum-confined states within the barrier. Self-consistent Poisson–Schrödinger simulations verify this aspect. This research unveils the intricate charge dynamics associated with the interaction of electron beams with heterostructure systems, paving the way for innovative optoelectronic applications in semiconductor devices.

MOF derived hierarchical α-Bi2O3-BiVO4-CuFe2O4 multijunction heterostructure with conjugated S-scheme charge mobilization: Photocatalytic decontamination study, toxicity assessment and mechanistic elucidation

A series of hierarchical α-Bi2O3-BiVO4-CuFe2O4 multijunction heterostructure was designed by integrating one-pot MOF derived Bi2O3-BiVO4 microrods with CuFe2O4 nanosheets. The MOF-derived route afforded Bi2O3-BiVO4 with interconnecting porous architecture. Comprehensive investigations revealed preservation of crystalline phases, optimal light harvesting ability, higher lifetime, large electrochemically active surface area and improved charge dynamics. The heterostructure efficiently performed the photo-degradation of potentially toxic and mutagenic mesotrione (MTE) herbicide with rates 6–12 times greater than the parent semiconductors. The photo-degraded end products displayed profoundly less acute toxicity, bioaccumulation factor and mutagenic nature than parent MTE as analyzed by QSAR protocol. The heterostructure was equally effective for complete photo-inactivation of E. coli bacteria within 60 min of irradiation. SEM, AFM height profile and confocal microscopic investigation provided crucial information about the photo-inactivation process. A conjugated S-scheme electron transfer mechanism was proposed based on detailed band structure analysis to elucidate the improved activity of the multijunction photocatalyst.

Cerium rare-earth ions reinforced built-in electric field to enable efficient carrier extraction for highly efficient and stable perovskite solar cells

Perovskite solar cells prepared by inorganic-organic three-dimensional hybrid have good power conversion efficiency, but their operational stability remains a major challenge for commercialization. The defect of perovskite is an important factor restricting its charge dynamics and stability. Here, the rare earth metal chloride CeCl3 is introduced into perovskite solution to passivate the defects, where the Pb2+ part of the B position is replaced by Ce3+. The prepared films have the characteristics of increasing grain size, enhancing carrier mobility and excellent crystallinity. Meanwhile, via passivating interface defects and improving carrier transport capacity, the generation of non-radiative recombination is reduced, the carrier migration length is extended, and the device performance is improved. The results show that the PCE of the standard device is only 65 % after 2880 h of N2 atmosphere at room temperature, while the efficiency of the device doped with CeCl3 can remain at 93 %. When the unencapsulated sample was placed in an air environment (40–60 % humidity), the control sample was reduced to 72 % at 1060 h, while the CeCl3 was maintained at 87 %. Additionally, the reduction of residual stress in the perovskite layer also provides good bending stability for the flexible target device. These results show that the incorporation of rare earth metal ions is an effective way to stabilize and improve the efficiency of the device.

Flexible printed circuit-based triboelectric film sensor for integrity monitoring of tensile bolted joints

This study presents an improved design of a triboelectric film sensor for integrity monitoring of tensile bolted joints, which is designed to capture the micro-scale relative motion due to the bolt’s looseness by utilizing the triboelectric effect of the polymer layer of the sensor in contact with the metal surface of the fastened objects. The key idea is twofold: First, we use the triboelectric effect between the polymer layer and the fastened object itself, instead of the triboelectric effect between two polymer layers. This allows the sensor to be a single sheet configuration instead of two-piece. The second idea is to make the sensor design fabricable as a standard flexible printed circuit. This makes it possible to produce sensors accurately and inexpensively. Experimental tests incorporating the proposed sensor into a tensile bolted joint have demonstrated that the sensor’s voltage output is inversely related to the bolt’s tightness. Additionally, a modeling study adopting Persson’s contact theory has been conducted to refine the understanding of the real contact area, triboelectric charging, and separation dynamics between the polymer and metal layers, which is crucial for the accurate modeling of sensor outputs under dynamic loading conditions. It has been concluded that the integrated mechanical and triboelectric model successfully aligns with the experimental findings, indicating the sensor’s potential for practical applications in bolt integrity monitoring.