Trapping Dynamics Research Articles

Encasing Few-Layer MoS2 within 2D Ordered Cubic Graphitic Cages to Smooth Trapping-Conversion of Lithium Polysulfides for Dendrite-Free Lithium-Sulfur Batteries.

The industrialization of lithium-sulfur (Li-S) batteries faces challenges due to the shuttling effect of lithium polysulfides (LiPSs) and the growth of lithium dendrites. To address these issues, a simple and scalable method is proposed to synthesize 2D membranes comprising a single layer of cubic graphitic cages encased with few-layer, curved MoS2. The distinctive 2D architecture is achieved by confining the epitaxial growth of MoS2 within the open cages of a 2D-ordered mesoporous graphitic framework (MGF), resulting in MoS2@MGF heterostructures with abundant sulfur vacancies. The experimental and theoretical studies establish that these MoS2@MGF membranes can act as a multifunctional interlayer in Li-S batteries to boost their comprehensive performance. The inclusion of the MoS2@MGF interlayer facilitates the trapping and conversion kinetics of LiPSs, preventing their shuttling effect, while simultaneously promoting uniform lithium deposition to inhibit dendrite growth. As a result, Li-S batteries with the MoS2@MGF interlayer exhibit high electrochemical performance even under high sulfur loading and lean electrolyte conditions. This work highlights the potential of designing advanced MoS2-encased heterostructures as interlayers, offering a viable solution to the current limitations plaguing Li-S batteries.

Removal of Pseudomonas type IV pili by a small RNA virus.

The retractile type IV pilus (T4P) is important for virulence of the opportunistic human pathogen Pseudomonas aeruginosa. The single-stranded RNA (ssRNA) phage PP7 binds to T4P and is brought to the cell surface through pilus retraction. Using fluorescence microscopy, we discovered that PP7 detaches T4P, which impairs cell motility and restricts the pathogen's virulence. Using cryo-electron microscopy, mutagenesis, optical trapping, and Langevin dynamics simulation, we resolved the structure of PP7, T4P, and the PP7/T4P complex and showed that T4P detachment is driven by the affinity between the phage maturation protein and its bound pilin, plus the pilus retraction force and speed, and pilus bending. Pilus detachment may be widespread among other ssRNA phages and their retractile pilus systems and offers new prospects for antibacterial prophylaxis and therapeutics.

Significant Impact of Defect Fluctuation on Charge Dynamics in CsPbI3: A Study Combining Machine Learning with Quantum Dynamics.

In this study, we developed a machine-learned force field for CsPbI3 using a neural network potential, enabling molecular dynamics simulations (MD) with ab initio accuracy over nanoseconds. This approach, combined with ab initio MD and nonadiabatic MD, was used to study the charge trapping and recombination dynamics in both pristine and defective CsPbI3. Our simulations revealed key transitions affecting carrier lifetimes, especially in systems with iodine vacancy and interstitial iodine defects. An iodine trimer, formed when iodine replaces cesium, exhibits a high-frequency phonon mode. This mode enhances nonadiabatic coupling, accelerating charge recombination in defective systems compared to pristine ones. In the iodine vacancy system, recombination times varied significantly due to differences in NA coupling and energy gaps. The interplay between nonadiabatic coupling and pure dephasing time is crucial in determining recombination times for interstitial iodine defects. Our findings highlight the role of defect evolution in perovskites, offering insights for enhancing perovskite performance.

Deep insights into the mechanism of nitrogen on the endurance enhancement in ferroelectric field effect transistors: Trap behavior during memory window degradation

The nitridation process can significantly improve the quality of the interfacial layer and suppress the unrecoverable electron trapping of the interfacial states during cycling, which is the main cause of endurance enhancement. In this work, through in-depth analysis of defect behavior during memory window (MW) degradation in ferroelectric field effect transistors (FeFETs), it is found that the degradation of FeFET devices with SiON interfacial layer starts within the HZO layer, while the degradation process of FeFET devices with SiO2 interlayer initially begins at the interlayer and then penetrates into the HZO layer. First, the MW degradation processes of nitridation/non-nitridation devices are measured and compared. Moreover, through the extended measure-stress-measure method, three types of defects are defined and the defect behaviors including trapping kinetics and energy locations during degradation are systematically investigated. The mechanism of nitrogen on the endurance enhancement is finally revealed. These results are valuable to better understand the reliability issues of FeFET and pave the way for future process optimization.

Capturing ion trapping and detrapping dynamics in electrochromic thin films

Ion trapping has been found to be responsible for the performance degradation in electrochromic oxide thin films, and a detrapping procedure was proved to be effective to rejuvenate the degraded films. Despite of the studies on ion trapping and detrapping, its dynamics remain largely unknown. Moreover, coloration mechanisms of electrochromic oxides are also far from clear, limiting the development of superior devices. Here, we visualize ion trapping and detrapping dynamics in a model electrochromic material, amorphous WO3. Specifically, formation of orthorhombic Li2WO4 during long-term cycling accounts for the origin of shallow traps. Deep traps are multiple-step-determined, composed of mixed W4+-Li2WO4, amorphous Li2WO4 and W4+-Li2O. The non-decomposable W4+-Li2WO4 couple is the origin of the irreversible traps. Furthermore, we demonstrate that, besides the typical small polaron hopping between W5+ ↔ W6+ sites, bipolaron hopping between W4+ ↔ W6+ sites gives rise to optical absorption in the short-wavelength region. Overall, we provide a general picture of electrochromism based on polaron hopping. Ion trapping and detrapping were demonstrated to also prevail in other cathodic electrochromic oxides. This work not only provides the ion trapping and detrapping dynamics of WO3, but also open avenues to study other cathodic electrochromic oxides and develop superior electrochromic devices with great durability.

Difference of carrier dynamics in a semiconductor saturable absorber mirror with and without B+ ion-implantation.

Three samples whose growth temperatures were 450°C, 500°C, and 560°C for S E S A M 1, S E S A M 2, and S E S A M 3, respectively, were tested by femto-second time-resolved transient absorption spectroscopy. The results indicate that the carrier dynamics of excited state absorption were dominant, and the lifetimes of carriers trapped by defect levels were about tens of pico-seconds. To further study the influence of carrier dynamics and recovery time of samples by ion-implantation, B + ions of 80 and 130 KeV were implanted into the samples with dose of 1014/c m 2. The modified samples showed a dominance of ultra-fast carrier dynamics of ground-state bleaching and direct recombination, which lasted for hundreds of femto-seconds, over excited state absorption. Additionally, carrier fast trapping was observed to be competitive with the excited state absorption process. After ion-implantation, the carrier dynamics of carrier trapping were enhanced, which contributed to forming an ultra-short laser, while the carrier dynamics of absorption of the excited state were suppressed. The conclusion that defect levels were partially eliminated by B + ion-implantation can be drawn.

Charge-Localized Retention and Long-Term Memory Enabled by Cooperating Sterically Confined Molecular Crystallization with Spiro[fluorene-9,9'-xanthene]-Based Csp3-Hindrance.

Charge localization of memory materials plays a crucial role in the endurance and retention ability of organic nonvolatile memory, which is completely opposite from the charge delocalization of high-mobility materials. However, charge transfer of both though-space and through-bond based on molecular design principles still faces challenges. Herein, a nonplanar wide-bandgap semiconductor with Csp3-hindrance (DOCH3-DDPA-SFX) has been designed and synthesized. An effective crystallization effect of self-assembled two-dimensional nanosheets on charge trapping dynamics and kinetics is visualized by Kelvin probe force microscopy (KPFM). The trapped charges are localized completely on a single nanosheet, which has better charge trapping and retention properties than an amorphous film. Meanwhile, crystallization also greatly improves structure stability. Combining DFT theoretical calculations, the mechanisms of localization and long-term retention are discussed. The steric crystallization effects on the charge localization will guide the effective design of single-component semiconducting charge-memory materials by molecular assembly and aggregate control for high-performance organic memory.

Efficient characterization of blinking quantum emitters from scarce data sets via machine learning

Single photon emitters are core building blocks of quantum technologies, with established and emerging applications ranging from quantum computing and communication to metrology and sensing. Regardless of their nature, quantum emitters universally display fluorescence intermittency or photoblinking: interaction with the environment can cause the emitters to undergo quantum jumps between on and off states that correlate with higher and lower photoemission events, respectively. Understanding and quantifying the mechanism and dynamics of photoblinking is important for both fundamental and practical reasons. However, the analysis of blinking time traces is often afflicted by data scarcity. Blinking emitters can photo-bleach and cease to fluoresce over time scales that are too short for their photodynamics to be captured by traditional statistical methods. Here, we demonstrate two approaches based on machine learning that directly address this problem. We present a multi-feature regression algorithm and a genetic algorithm that allow for the extraction of blinking on/off switching rates with ⩾85% accuracy, and with ⩾10× less data and ⩾20× higher precision than traditional methods based on statistical inference. Our algorithms effectively extend the range of surveyable blinking systems and trapping dynamics to those that would otherwise be considered too short-lived to be investigated. They are therefore a powerful tool to help gain a better understanding of the physical mechanism of photoblinking, with practical benefits for applications based on quantum emitters that rely on either mitigating or harnessing the phenomenon.

RC-Effects on the Oxide of SOI MOSFET under Off-State TDDB Degradation: RF Characterization and Modeling.

Based on S-parameter measurements, the effect of dynamic trapping and de-trapping of charge in the gate oxide, the increase of dielectric loss due to polarization, and the impact of leakage current on the small-signal input impedance at RF is analyzed and represented. This is achieved by systematically extracting the corresponding model parameters from single device measurements at different frequency ranges, and then the methodology is applied to analyze the evolution of these parameters when the device is submitted to non-conducting electrical stress. This approach not only allows to inspect the impact of effects not occurring under DC conditions, such as the current due to the time varying dielectric polarization, but also to clearly distinguish effects in accordance with the functional form of their contribution to the device's impedance. In fact, it is shown that minor changes in the model of the gate capacitance by including additional resistive and capacitive components allows for an excellent model-experiment correlation up to 30 GHz. Moreover, the accuracy of the correlation is shown to be maintained when applying the proposal to the device under different gate-to-source bias conditions and at several stages during off-state degradation.

Simulations of CO2 Dissolution in Porous Media Using the Volume-of-Fluid Method

Traditional investigations of fluid flow in porous media often rely on a continuum approach, but this method has limitations as it does not account for microscale details. However, recent progress in imaging technology allows us to visualize structures within the porous medium directly. This capability provides a means to confirm and validate continuum relationships. In this study, we present a detailed analysis of the dissolution trapping dynamics that take place when supercritical CO2 (scCO2) is injected into a heterogeneous porous medium saturated with brine. We present simulations based on the volume-of-fluid (VOF) method to model the combined behavior of two-phase fluid flow and mass transfer at the pore scale. These simulations are designed to capture the dynamic dissolution of scCO2 in a brine solution. Based on our simulation results, we have revised the Sherwood correlations: We expanded the correlation between Sherwood and Peclet numbers, revealing how the mobility ratio affects the equation. The expanded correlation gave improved correlations built on the underlying displacement patterns at different mobility ratios. Further, we analyzed the relationship between the Sherwood number, which is based on the Reynolds number, and the Schmidt number. Our regression on free parameters yielded constants similar to those previously reported. Our mass transfer model was compared to experimental models in the literature, showing good agreement for interfacial mass transfer of CO2 into water. The results of this study provide new perspectives on the application of non-dimensional numbers in large-scale (field-scale) applications, with implications for continuum scale modeling, e.g., in the field of geological storage of CO2 in saline aquifers.

Ultrafast exciton trapping dynamics in oxygen-functionalized single-walled carbon nanotubes

Artificial zero-dimensional quantum defects within single-walled carbon nanotubes hold immense promise for diverse optoelectronic applications such as bioimaging, near-infrared light emission, nanolasing, and single-photon generation. This study delves into the temporal behavior of excitons within oxygen-functionalized single-walled carbon nanotubes, employing ultrafast transient absorption spectroscopy. Our investigation unveils the emergence of functionalization-induced excitonic states, distinguished by a long-lasting induced transmittance signal. Remarkably, even at low degree of functionalization, we observe a reduction in the lifetime of band-edge excitons. In contrast, the population dynamics of deep-band excitons exhibit resilience against low and moderate functionalization degrees, with a pronounced reduction manifesting only at high degrees of functionalization. Our findings align closely with a kinetic model that accounts for an additional relaxation channel prompted by functionalization. This empirical evidence provides a significant breakthrough, establishing that the formation of functionalization-induced excitonic states within oxygen-functionalized single-walled carbon nanotubes is a consequence of the diffusive trapping of free band edge excitons, while interaction of deep band excitons with oxygen defect sites rather yields in exciton recombination. These insights shed light on the intricate dynamics of excitons within single-walled carbon nanotube with artificially embedded quantum defects, advancing our understanding and potential applications in the realm of optoelectronics.

Dynamic trap of Ni at elevated temperature for yielding high-efficiency methane dry reforming catalyst

Highly dispersed and stable metal catalysts with small nanoparticles have received extensive attention in elevated-temperature thermocatalytic process. However, the available strategies to stabilize metal sites, by constructing defective structures on catalyst supports and developing controllable preparation steps at room temperature, show limited effect, because these active metal sites can be mobile and sintering at elevated temperature. Herein, dealuminated Beta zeolite with abundant surface defects of silanol nests is applied as support, then dynamic trap strategy and subsequent reduction process at elevated temperature is devoted to transfer Ni-based precursors into the silanol nests, thus obtaining small nanoparticles Ni catalysts that are suitable for high-temperature methane dry reforming (DRM). Some in-situ characterization processes and the ingenious designed experiments are performed to identify the dynamic trapping process. The rational fabricated catalysts exhibit high catalytic reactivity for DRM reaction in long-term operation.

Trapped vortex dynamics implemented in composite Bessel beams

The divergence-free nature of Bessel beams can be harnessed to effectively trap optical vortices in free space laser propagation. We show how to generate arbitrary vortex configurations in Bessel traps to investigate few-body vortex interactions within a dynamically evolving fluid of light, which is a formal analog to a non-interacting Bose gas. We implement—theoretically and experimentally—initial conditions of vortex configurations first predicted in harmonically trapped quantum fluids, in the limit of weak atomic interactions, and model and measure the resultant dynamics. These hard trap dynamics are distinct from the harmonic trap predictions due to the non-local interactions that occur among the hard-wall boundary and steep phase gradients that nucleate other vortices. By simultaneously presenting experimental demonstrations with the theoretical proposal, we validate the potential application of using Bessel hard-wall traps as testing grounds for engineering few-body vortex interactions within trapped, two-dimensional compressible fluids.

Long-term mercury loading and trapping dynamics in a Western North America reservoir

Study RegionThe Carson River including Lahontan Reservoir in Northwestern Nevada, USA Study FocusThe discovery, mining, and processing of silver and gold from the Comstock Lode in northwestern Nevada heavily contaminated the Carson River system with mercury (Hg). The river now contains some of the highest recorded water column and bed sediment Hg concentrations reported in peer-reviewed literature. Acute Hg contamination in river and reservoir bed sediment has led to elevated methylmercury (MeHg) concentrations across all trophic levels of Lahontan Reservoir, culminating in significant health risks to humans. Lahontan Reservoir, located downstream from the mills that processed Comstock ore, has served as a Hg trap since the completion of the dam in 1915. Starting in 1997 and extending through 2021, the U.S. Geological Survey has collected and analyzed hundreds of discrete water samples entering and exiting Lahontan Reservoir for unfiltered total Hg (uf.THg), thereby providing a first-of-its-kind opportunity for studying long-term Hg trapping efficiencies within a western North American reservoir. Continuous time series of uf.THg concentration and flux above and below the reservoir were estimated using the weighted regressions on time, discharge, and season with the Kalman filtering (WRTDS-K) method employed with newly developed methods to account for non-natural (i.e., managed) hydrographs below a reservoir. New hydrological insights for the regionAn estimated 31,650 kg (34.89 US tons) of uf.THg entered Lahontan Reservoir during the 25 year period of analysis, accounting for approximately 0.5% of the total uf.THg estimated to have been released to the Carson River system [6.8 million kg (7500 US tons)] over a multi-decade mining boom. Moreover, approximately 92% of the estimated uf.THg entering Lahontan Reservoir was trapped. On an annual basis, however, trapping efficiencies range between 34% and 98%, and are closely related to the total annual discharge. Results also indicate that flow-normalized uf.THg concentrations and loads above and below the reservoir are trending down.

Acoustic Trapping and Manipulation of Hollow Microparticles under Fluid Flow Using a Single-Lens Focused Ultrasound Transducer.

Microparticle manipulation and trapping play pivotal roles in biotechnology. To achieve effective manipulation within fluidic flow conditions and confined spaces, it is necessary to consider the physical properties of microparticles and the types of trapping forces applied. While acoustic waves have shown potential for manipulating microparticles, the existing setups involve complex actuation mechanisms and unstable microbubbles. Consequently, the need persists for an easily deployable acoustic actuation setup with stable microparticles. Here, we propose the use of hollow borosilicate microparticles possessing a rigid thin shell, which can be efficiently trapped and manipulated using a single-lens focused ultrasound (FUS) transducer under physiologically relevant flow conditions. These hollow microparticles offer stability and advantageous acoustic properties. They can be scaled up and mass-produced, making them suitable for systemic delivery. Our research demonstrates the successful trapping dynamics of FUS within circular tubings of varying diameters, validating the effectiveness of the method under realistic flow rates and ultrasound amplitudes. We also showcase the ability to remove hollow microparticles by steering the FUS transducer against the flow. Furthermore, we present potential biomedical applications, such as active cell tagging and navigation in bifurcated channels as well as ultrasound imaging in mouse cadaver liver tissue.

Evidence of trapping and electrothermal effects in vertical junctionless nanowire transistors

Understanding trap dynamics and formation of localized temperature hot-spots due to self-heating is crucial for the design optimization of emerging vertical junctionless nanowire transistors (VNWFET). This work investigates the operation of an 18 nm VNWFET technology, for the first time, leveraging pulsed current–voltage measurements. Results indicate increased trap activity as well as electrothermal effects with increasing pulse width. Multiphysics simulations are then used to provide a deeper insight into the nanoscale transport of the VNWFETs. We then incorporated these effects into the SPICE-compatible VNWFET compact model and further investigated the behaviors of trapping and electrothermal effects in basic logic circuits based on the compact model simulation.

Ion trap and release dynamics enables nonintrusive tactile augmentation in monolithic sensory neuron.

An iontronic-based artificial tactile nerve is a promising technology for emulating the tactile recognition and learning of human skin with low power consumption. However, its weak tactile memory and complex integration structure remain challenging. We present an ion trap and release dynamics (iTRD)-driven, neuro-inspired monolithic artificial tactile neuron (NeuroMAT) that can achieve tactile perception and memory consolidation in a single device. Through the tactile-driven release of ions initially trapped within iTRD-iongel, NeuroMAT only generates nonintrusive synaptic memory signals when mechanical stress is applied under voltage stimulation. The induced tactile memory is augmented by auxiliary voltage pulses independent of tactile sensing signals. We integrate NeuroMAT with an anthropomorphic robotic hand system to imitate memory-based human motion; the robust tactile memory of NeuroMAT enables the hand to consistently perform reliable gripping motion.

Spectral widths and Stokes shifts in InP-based quantum dots.

InP-based quantum dots (QDs) have Stokes shifts and photoluminescence (PL) line widths that are larger than in II-VI semiconductor QDs with comparable exciton energies. The mechanisms responsible for these spectral characteristics are investigated in this paper. Upon comparing different semiconductors, we find the Stokes shift decreases in the following order: InP > CdTe > CdSe. We also find that the Stokes shift decreases with core size and decreases upon deposition of a ZnSe shell. We suggest that the Stokes shift is largely due to different absorption and luminescent states in the angular momentum fine structure. The energy difference between the fine structure levels, and hence the Stokes shifts, are controlled by the electron-hole exchange interaction. Luminescence polarization results are reported and are consistent with this assignment. Spectral widths are controlled by the extent of homogeneous and inhomogeneous broadening. We report PL and PL excitation (PLE) spectra that facilitate assessing the roles of homogeneous and different inhomogeneous broadening mechanisms in the spectra of zinc-treated InP and InP/ZnSe/ZnS particles. There are two distinct types of inhomogeneous broadening: size inhomogeneity and core-shell interface inhomogeneity. The latter results in a distribution of core-shell band offsets and is caused by interfacial dipoles associated with In-Se or P-Zn bonding. Quantitative modeling of the spectra shows that the offset inhomogeneity is comparable to but somewhat smaller than the size inhomogeneity. The combination of these two types of inhomogeneity also explains several aspects of reversible hole trapping dynamics involving localized In3+/VZn2- impurity states in the ZnSe shells.

(Invited) On-the-Fly Non-Adiabatic Dynamics Simulations of Single-Walled Carbon Nanotubes with Covalent Defects

Single-walled carbon nanotubes (SWCNTs) with covalent surface defects have been explored recently due to their promise for use in single-photon telecommunication emission and in spintronic applications. The dynamical evolution of excitons (the primary electronic excitations) in these systems has only been loosely explored using atomistic modeling due to the size-limitations of these large systems. We present computational modeling of non-radiative relaxation on a variety of SWCNT chiralities with single-defect functionalization schemes. Our modeling uses a trajectory surface hopping algorithm accounting for excitonic effects with a configuration interaction approach. We find a strong chirality and defect-composition dependence on the population relaxation (50 – 500 fs) between the nanotube band-gap excitation and the defect-associated, single-photon-emitting state, giving insight into the dynamic trapping nature of these localized excitonic states. Engineering fast population decay into the quasi-two-level sub-system with weak coupling to higher-energy states increases the effectiveness and controllability of these quantum light emitters.

Use of Food Attractant to Monitor and Forecast Population Dynamics of Cnaphalocrocis medinalis (Lepidoptera: Pyralidae), a Long-Distance Migratory Pest

The rice leaf folder, Cnaphalocrocis medinalis, is a significant migratory pest that restricts rice production in Asia and Africa, and monitoring and early warning measures are the basis for its management. Based on its regional migratory path in China, the pest population dynamics were monitored from 2020 to 2021 using food attractants. In this study, we also used internal reproductive system dissection to determine the adult age and reproductive developmental state. The monitoring results indicated that the trapping dynamics of C. medinalis males using food attractants and sex pheromones were approximately similar. Both trapping methods yielded C. medinalis males of different ages, with an identical age structure for both trap types. Dissection analysis of the reproductive system of females trapped using the food attractants indicated that in 2020, the population of C. medinalis in Liling, Hunan Province, was indigenous, while populations in other monitoring sites mainly comprised migrants from other areas. The ovarian development level of females trapped using food attractants showed a positive correlation with the age of males, and there was also a significant positive correlation between the index of ovarian development of females and the mating time. Furthermore, a dynamic prediction method for fecundity in field populations was established based on the quantity of eggs held by the females. This study provides a new method for the monitoring and early warning of the existence of C. medinalis populations.