Temperature Dependence Of Dynamics Research Articles

Temperature-dependent lattice dynamics study on phase stability, martensitic transformation mechanism, and vibrational entropy properties of B2-type Ni–Mn–Ti Heusler alloy

The all-d-metal Ni–Mn–Ti Heusler alloy with its good mechanical properties and colossal caloric effects has attracted significant attention for mechanocaloric refrigeration. However, the phase stability of the B2-type disordered structure at finite temperatures and the physical origin of large phase transformation entropy change in theoretical calculation remain unclear. In view of thermal and strongly anharmonic effects, we combined the first-principles and temperature dependent effective potential calculations to systematically study the phase stability, martensitic transformation mechanism, and vibrational entropy properties of B2 partial disordered structures for Ni8Mn5Ti3 and Ni8Mn6Ti2. Our results showed the austenitic structures of Ni8Mn5Ti3 and Ni8Mn6Ti2 both exhibit antiferromagnetic interaction behaviors at targeted temperatures, resolving the contradiction between previous calculations and experiments. By the analysis of phonon dispersion relations and Helmholtz free energies at low and high temperatures, we provided a deeper explanation for the underlying mechanism of martensitic transformation. Meanwhile, the phase transformation temperatures and vibrational entropy changes were accurately predicted compared with the experiment results. Specifically, we demonstrated that the large vibrational entropy change of Ni–Mn–Ti material originates from the contributions of both the tetragonal distortion ratio and volume change, which provides important theoretical guidance and has great practical significance for designing the solid-state material with large vibrational entropy change in the application of solid-state refrigeration.

Evaluation of machine tool dynamics in dry gear hobbing considering time-varying thermal effects

Effective stability analysis strongly depends on accurately predicting machine tool dynamics. However, the nonlinear thermal effects during the machining operations present a significant challenge to accurately modeling the machine tool dynamics. To this end, the evolution of the machine tool dynamics under the thermal growth during the dry gear hobbing process is investigated, and a rapid evaluation model of the temperature-dependent dynamics is developed. Firstly, a preliminary test was conducted to explore thermal effects on the machine tool dynamics. Then, the free vibrations at the spindle nose during the hobbing operations were filtered, and the corresponding modal parameters were estimated. Subsequently, the influence of temperature rise on the modal parameters is analyzed. The results show that the first- and third-order natural frequencies increase by 142 and 95 Hz, respectively, and the damping ratios for all modes are reduced with the machine tool temperature rise. Finally, the relationship between the feature temperatures and modal parameters is described using the multi-output Gaussian Process regression (MOGPR) model. The overall prediction accuracy is 95.6 %, and the relative errors in the test data set are within 10 %. The findings can provide an essential basis for the machining stability analysis of dry gear hobbing.

Quantum and classical spin dynamics across temperature scales in the S=1/2 Heisenberg antiferromagnet

Using the framework of semiclassical Landau-Lifshitz dynamics (LLD), we conduct a systematic investigation of the temperature-dependent spin dynamics in the S=1/2 Heisenberg square-lattice antiferromagnet (SAFM). By performing inelastic neutron scattering measurements on Zn2VO(PO4)2 (ZVPO) and corresponding finite-temperature spin dynamics simulations based on LLD, we present a comprehensive analysis that bridges quantum and classical spin dynamics over a broad temperature range. First, remarkable agreement between experimental data and LLD simulations is found in the paramagnetic phase of ZVPO, demonstrating the capability of LLD in accurately determining the spin Hamiltonian of S=1/2 systems and capturing the quantum-to-classical crossover of their spin dynamics. Second, by analyzing the discrepancies between the experimental data and the LLD simulations at lower temperatures, we determine the experimental temperature dependence of the quantum effects in the excitation spectrum of the S=1/2 SAFM: the quantum renormalization factor for the magnon energies and the quantum continuum above the one-magnon bands. Notably, the emergence of each quantum effect is found to correlate with the formation of three-dimensional long-range order. This work demonstrates the utility of LLD in gaining experimental insights into the temperature-induced modifications of quantum spin dynamics and their convergence towards classical expectations at higher temperatures. This motivates further applications to more challenging quantum antiferromagnets dominated by stronger quantum fluctuations. Published by the American Physical Society 2024

Temperature-Dependent Rotational Dynamics of Non-Polar Solute in Non-Polar Solvents: Influence of Boundary Conditions.

Rotational dynamics of 3-(benzo[d]thiazol-2-yl)-7-(diethylamino)-2H-chromen-2-one (3BT7D2H-one) non-polar solute in non-polar solvents has been studied by varying temperature to find out how hydrodynamic friction is influenced by solute-size ratio. It has been observed that the rotational dynamics of 3BT7D2H-one follow the Stoke's-Einstein-Debye (SED) model in an n-hexane solvent and it follows the Gierer and Wirtz (GW) model in an n-decane solvent. The probable reason is due to the solute-solvent size ratio which influences boundary conditions parameters and consequently on rotational dynamics of solute.

Investigating Temperature-Dependent Dynamics of SEI Growth and Battery Degradation

Several studies have contributed to the current understanding of the temperature-dependent behavior of solid-electrolyte interphase (SEI) formation in lithium-ion batteries and its impact on battery capacity and lifespan. Liu et al. developed a thermal-electrochemical model that revealed the complex interplay between diffusivity, reaction kinetics, and temperature on SEI growth1. Leng et al. presented an electrochemistry-based electrical model to examine the temperature's effect on battery aging2. Alipour et al. reviewed temperature-dependent electrochemical properties3, while Lubhani Mishra et al. provided a detailed physics-based analysis of battery degradation and temperature inhomogeneities4. These studies collectively indicate higher temperatures accelerating and promoting growth of compact and less permeable SEI structures leading to an increase in capacity loss and cell resistance, and lower temperatures resulting in slow ionic transport through the SEI also causing higher ohmic loss. In the present work, we study SEI growth and resulting effect on battery capacity fade using continuum scale modeling under the assumption of constant battery cell temperature as well as considering actual dynamically changing temperature data from experiments. SEI growth under these two considerations is compared and the comparison is used in determining scenarios where considering dynamically varying temperature is crucial for accuracy. The detailed analysis of the internal states from the simulation results contributes to the understanding of the effect of the thermal dynamics on battery cell degradation due to SEI growth. To achieve these objectives, a physics-based model, specifically the Single Particle Model (SPM), is utilized. The model uses temporal temperature data obtained from past experimental studies as well as temperature dependent properties of SEI provided in the literature as inputs for this investigation. The ultimate aim of this study is to better understand how temperature influences SEI characteristics, thereby contributing to improved battery performance and longevity across diverse thermal environments. References Liu, L., Park, J., Lin, X., Sastry, A. M., & Lu, W. (2014). A thermal-electrochemical model that gives spatial-dependent growth of solid electrolyte interphase in a Li-ion battery. Journal of power sources, 268, 482-490.Leng, F., Tan, C. M., & Pecht, M. (2015). Effect of temperature on the aging rate of Li-ion battery operating above room temperature. Scientific reports, 5(1), 12967.Alipour, M., Ziebert, C., Conte, F. V., & Kizilel, R. (2020). A review on temperature-dependent electrochemical properties, aging, and performance of lithium-ion cells. Batteries, 6(3), 35.Mishra, L., Subramaniam, A., Jang, T., Garrick, T. R., & Subramanian, V. R. (2022, October). Model Development for Temperature-Dependent Degradation in Large Format Lithium-Ion Batteries. In Electrochemical Society Meeting s 242 (No. 28, pp. 1075-1075). The Electrochemical Society, Inc.

Temperature Dependent Early-Stage Oxidation Dynamics of Cu(100) Film with Faceted Holes

Temperature Dependent Early-Stage Oxidation Dynamics of Cu(100) Film with Faceted Holes

Unifying the temperature dependent dynamics of glass formers.

Strong changes in bulk properties, such as modulus and viscosity, are observed near the glass transition temperature, Tg, of amorphous materials. For more than a century, intense efforts have been made to define a microscopic origin for these macroscopic changes in properties. Using transition state theory (TST), we delve into the atomic/molecular level picture of how microscopic localized unit relaxations, or "cage rattles," evolve to macroscopic structural relaxations above Tg. Unit motion is broken down into two populations: (1) simultaneous rearrangement occurs among a critical number of units, nα, which ranges from 1 to 4, allowing a systematic classification of glass formers, GFs, that is compared to fragility; and (2) near Tg, adjacent units provide additional free volume for rearrangement, not simultaneously, but within the "primitive" lifetime, τ1, of one unit rattling in its cage. Relaxation maps illustrate how Johari-Goldstein β-relaxations stem from the rattle of nα units. We analyzed a wide variety of glassy materials and materials with a glassy response using literature data. Our four-parameter equation fits "strong" and "weak" GFs over the entire range of temperatures and also extends to other glassy systems, such as ion-transporting polymers and ferroelectric relaxors. The role of activation entropy in boosting preexponential factors to high "unphysical" apparent frequencies is discussed. Enthalpy-entropy compensation is clearly illustrated using the TST approach.

Temperature and medium structurization effect on spontaneous evolution of domains and bubbles in magnetic nanostructures

Spontaneous evolutions of domains in magnetic nanowires and of magnetic bubbles in open ferromagnetic nanolayers are investigated using micromagnetic simulations. We compare temperature dependent dynamics of domain wall (DW) systems in Permalloy (Py) nanowires and systems of chiral DWs in ultra-thin nanowires with perpendicular magnetic anisotropy (PMA) and Dzyaloshinskii-Moriya interaction (DMI). In Py nanowires DWs collide and, in majority of cases, the collision leads to the DW annihilation in disagreement with the expectation of topological protection of sums of all the magnetic charges attached to the nanowire edges which are carried by DWs. For our purpose of discussing the DW collision in the presence of thermal excitations, we revisit the problem of field-driven collisions of DWs in Py nanowires at zero temperature. We claim that thermal fluctuations can counteract the collision-induced annihilation of DWs, thought further improvement of stabilization of domain structures is achievable via structurization of the magnetic nanowires (dividing them into grains). In PMA-DMI nanowires, thermally-excited chiral DWs can be randomly approaching or moving away while not being annihilated. A problem related to the motion of chiral DWs is the spontaneous motion of magnetic bubbles in open PMA-DMI planes. The magnetic bubbles expand or shrink to vanishing dependent on strength of the DMI interaction. Such a motion appears to be be strongly influenced by temperature and by structural discontinuities of the magnetic layer.

Biorealistic Neuronal Temperature-Sensitive Dynamics within Threshold Switching Memristors: Toward Neuromorphic Thermosensation.

Neuromorphic nanoelectronic devices that can emulate the temperature-sensitive dynamics of biological neurons are of great interest for bioinspired robotics and advanced applications such as in silico neuroscience. In this work, we demonstrate the biomimetic thermosensitive properties of two-terminal V3O5 memristive devices and showcase their similarity to the firing characteristics of thermosensitive biological neurons. The temperature-dependent electrical characteristics of V3O5-based memristors are used to understand the spiking response of a simple relaxation oscillator. The temperature-dependent dynamics of these oscillators are then compared with those of biological neurons through numerical simulations of a conductance-based neuron model, the Morris-Lecar neuron model. Finally, we demonstrate a robust neuromorphic thermosensation system inspired by biological thermoreceptors for bioinspired thermal perception and representation. These results not only demonstrate the biorealistic emulative potential of threshold-switching memristors but also establish V3O5 as a functional material for realizing solid-state neurons for neuromorphic computing and sensing applications.

Research on high-carbon ether-based oxygen additives: Catalytic transformation of 2-methylfuran and furfural to ethers via CuMgAlOx catalysts

The surge in aviation fuel consumption has intensified environmental concerns, driving research efforts towards discovering oxygen-enriched additives that can boost their performance. This investigation employs 2-methylfuran and furfural as precursors, undergoing catalytic conversion into high-performance high-carbon ethers. The study initiates by employing Amberlyst-15 resin as a catalyst, converting 2-methylfuran and furfural into a high-carbon polymer (1A). A continuous polymerization process in a fixed-bed reactor highlights the exceptional stability of Amberlyst-15, maintaining a conversion rate of approximately 70 % over 140 h. A kinetics model elucidates the temperature-dependent dynamics of the polymerization reaction. Following this, the polymer undergoes hydrogenation (HDO) using CuMgAlOx catalyst, yielding an ether compound (2A) with a remarkable selectivity of 95.7 % and a carbon yield of 95.5 %. Characterization techniques reveal uniform elemental distribution and a high abundance of mesopores in the CuMgAlOx catalyst, substantiating its superior hydrogenation efficiency. Notably, even after six cycles, the CuMgAlOx catalyst retains an impressive 94.8 % polymer conversion rate, underscoring its exceptional stability.

Nuclear Quantum Effects on Nonadiabatic Dynamics of a Green Fluorescent Protein Chromophore Analogue: Ring-Polymer Surface-Hopping Simulation.

Herein, we have used the "on-the-fly" ring-polymer surface-hopping simulation method with the centroid approximation (RPSH-CA), in combination with the multireference OM2/MRCI electronic structure calculations to study the photoinduced dynamics of a green fluorescent protein (GFP) chromophore analogue in the gas phase, i.e., o-HBI, at 50, 100, and 300 K with 1, 5, 10, and 15 beads (3600 1 ps trajectories). The electronic structure calculations identified five new minimum-energy conical intersection (MECI) structures, which, together with the previous one, play crucial roles in the excited-state decay dynamics of o-HBI. It is also found that the excited-state intramolecular proton transfer (ESIPT) occurs in an ultrafast manner and is completed within 20 fs in all the simulation conditions because there is no barrier associated with this ESIPT process in the S1 state. However, the other excited-state dynamical results are strongly related to the number of beads. At 50 and 100 K, the nuclear quantum effects (NQEs) are very important; therefore, the excited-state dynamical results change significantly with the bead number. For example, the S1 decay time deduced from time-dependent state populations becomes longer as the bead number increases. Nevertheless, an essentially convergent trend is observed when the bead number is close to 10. In contrast, at 300 K, the NQEs become weaker and the above dynamical results converge very quickly even with 1 bead. Most importantly, the NQEs seriously affect the excited-state decay mechanism of o-HBI. At 50 and 100 K, most trajectories decay to the S0 state via perpendicular keto MECIs, whereas, at 300 K, only twisted keto MECIs are responsible for the excited-state decay. The present work not only comprehensively explores the temperature-dependent photoinduced dynamics of o-HBI, but also demonstrates the importance and necessity of NQEs in nonadiabatic dynamics simulations, especially at relatively low temperatures.

Evidence of Ferromagnetism and Ultrafast Dynamics of Demagnetization in an Epitaxial FeCl2 Monolayer.

The development of two-dimensional (2D) magnetism is driven not only by the interest of low-dimensional physics but also by potential applications in high-density miniaturized spintronic devices. However, 2D materials possessing a ferromagnetic order with a relatively high Curie temperature (Tc) are rare. In this paper, the evidence of ferromagnetism in monolayer FeCl2 on Au(111) surfaces, as well as the interlayer antiferromagnetic coupling of bilayer FeCl2, is characterized by using spin-polarized scanning tunneling microscopy. A Curie temperature (Tc) of ∼147 K is revealed for monolayer FeCl2, based on our static magneto-optical Kerr effect measurements. Furthermore, temperature-dependent magnetization dynamics is investigated by the time-resolved magneto-optical Kerr effect. A transition from one- to two-step demagnetization occurs as the lattice temperature approaches Tc, which supports the Elliott-Yafet spin relaxation mechanism. The findings contribute to a deeper understanding of the underlying mechanisms governing ultrafast magnetization in 2D ferromagnetic materials.

Experimental Investigation of a 64 Ah Lithium-Ion Pouch Cell

This study presents a meticulous investigation and characterization of a 64 Ah commercial lithium-ion pouch cell. Notably, an exhaustive analysis of the cell’s open-circuit voltage and kinetics attributes is conducted, with particular emphasis on the temperature-dependent dynamics. Subsequently, a teardown experiment is performed, offering an incisive insight into the macro-geometrical properties underpinning the cell’s architecture. Further details about the microstructural features and formulation inherent to the cathode and anode are revealed after image processing of the electrodes’ cross sections. The details of cell balancing and cycling window of the electrodes in the pouch cell are determined and discussed based on the open-circuit-voltage measurements of the individual electrodes and a simple optimization algorithm. The methodologies presented in this work are insightful on the characterization and model parametrization of the high-capacity commercial lithium-ion cells.

Diffusion and magnetization of metal adatoms on single-layer molybdenum disulfide at elevated temperatures

The present work models temperature-dependent (500−1300K) diffusion dynamics of Ag, Au, and Cu adatoms on MoS2 as well as electronic and magnetic properties of adatom (Ag, Au, and Cu)/MoS2 systems. Modeling is done by means of ab initio molecular dynamics (AIMD) simulations that account for van der Waals corrections and electronic spin degrees of freedom in the framework of density functional theory. It is found that Ag and Au adatoms exhibit super-diffusive motion on MoS2 at all temperatures, while Cu adatoms follow a random walk pattern of uncorrelated surface jumps. The observed behavior is consistent with AIMD-calculated effective migration barriers Ea (EaAg=190±50meV, EaAu=67±7meV, and EaCu=300±100meV) and can be understood on the basis of the considerably flatter potential energy landscapes encountered by Ag and Au adatoms on the MoS2 surface (corrugation of the order of tens of meV), as compared to Cu adatoms (corrugation >100meV). Moreover, evaluation of the electronic and magnetic properties of AIMD configurations suggest that Ag, Au, and Cu monomer adsorption induces semimetallic features in at least one spin channel of the adatom/MoS2 electronic structure at elevated temperatures. The overall results presented herein may provide insights into fabricating 2D-material-based heterostructure devices beyond graphene.

Molecular-level insights into the temperature-dependent formation dynamics and mechanism of water-soluble dissolved organic carbon derived from biomass pyrolysis smoke

Water soluble organic carbon (WSOC) derived from biomass pyrolytic smoke is deposited through atmospheric aerosols, negatively affecting aquatic ecological quality and safety. However, the temperature-dependent molecular diversity and dynamic formation of smoke-derived WSOC remain poorly understood in water. Herein, we explored the molecular-level formation mechanism of pyrolytic smoke-derived WSOC in water to explain the evolution, heterogeneous correlations, and sequential responses of molecules and functional groups to increasing pyrolysis temperature. Two-dimensional correlation spectroscopy was used to innovatively establish the characteristic correlations between spectroscopy and Fourier transform-ion cyclotron resonance mass spectrometry. Temperature-dependent formation of WSOC exhibited diversity in absorbance/fluorescent components, unique/common molecules, and their chemical parameters, showing the simultaneous formation and degradation reactions. The common WSOC molecules with lower and higher degrees of oxidation showed significant positive and negative correlations with the fluorescent components, respectively. The primary sequential response of WSOC molecules to increasing pyrolysis temperature (lignin-like molecules → unsaturated hydrocarbons, condensed aromatic molecules → lipid-like/aliphatic-/peptide-like molecules) corresponded to the temperature response of functional groups (carboxylic/alcoholic → polysaccharides → aromatics/amides/phenolic/aliphatic groups), demonstrating well synergistic relationships between them. These novel findings will contribute to the comprehensive understanding and assessments of potential environmental behavior or risks of WSOC in aquatic ecosystems.

COOLAIR and PRC2 function in parallel to silence FLC during vernalization

Noncoding transcription induces chromatin changes that can mediate environmental responsiveness, but the causes and consequences of these mechanisms are still unclear. Here, we investigate how antisense transcription (termed COOLAIR) interfaces with Polycomb Repressive Complex 2 (PRC2) silencing during winter-induced epigenetic regulation of Arabidopsis FLOWERING LOCUS C (FLC). We use genetic and chromatin analyses on lines ineffective or hyperactive for the antisense pathway in combination with computational modeling to define the mechanisms underlying FLC repression. Our results show that FLC is silenced through pathways that function with different dynamics: a COOLAIR transcription-mediated pathway capable of fast response and in parallel a slow PRC2 switching mechanism that maintains each allele in an epigenetically silenced state. Components of both the COOLAIR and PRC2 pathways are regulated by a common transcriptional regulator (NTL8), which accumulates by reduced dilution due to slow growth at low temperature. The parallel activities of the regulatory steps, and their control by temperature-dependent growth dynamics, create a flexible system for registering widely fluctuating natural temperature conditions that change year on year, and yet ensure robust epigenetic silencing of FLC.

Bridging Soft Interaction and Excluded Volume in Crowded Milieu through Subtle Protein Dynamics.

The impact of macromolecular crowding on biological macromolecules has been elucidated through the excluded volume phenomenon and soft interactions. However, it has often been difficult to provide a clear demarcation between the two regions. Here, using temperature-dependent dynamics (local and global) of the multidomain protein human serum albumin (HSA) in the presence of commonly used synthetic crowders (Dextran 40, PEG 8, Ficoll 70, and Dextran 70), we have shown the presence of a transition that serves as a bridge between the soft and hard regimes. The bridging region is independent of the crowder identity and displays no apparent correlation with the critical overlap concentration of the polymeric crowding agents. Moreover, the dynamics of domains I and II and the protein gating motion respond differently, thereby bringing to the fore the asymmetry underlying the crowder influence on HSA. In addition, solvent-coupled and decoupled protein motions indicate the heterogeneity of the dynamic landscape in the crowded milieu. We also propose an intriguing correlation between protein stability and dynamics, with increased global stability being accompanied by eased local domain motion.

Temperature-dependent ultrafast hot carrier dynamics in the dilute bismide alloy GaSb1−xBix (x ≾ 0.4%)

We report temperature-dependent hot carrier dynamics in liquid-phase epitaxy-grown GaSb1−xBix epilayers with dilute amounts of Bi (x ≾ 0.4%). Degenerate pump–probe (λ = 800 nm) transient reflectivity (PPTR) was used to investigate the carrier dynamics in the epilayers. The PPTR signal consists of two transient processes (fast and slow) at all temperatures for all epilayers. The fast, hot carrier relaxation time, which is attributed to the combined effect of intervalley scattering and thermalization of carriers below cryogenic temperatures (<100 K), is observed to increase with an increase in temperature (≈0.8–2 ps at 6.6 K and ≈4–5 ps at 300 K). However, at higher temperatures (>100 K), the interband CHSH-Auger recombination process affects the band-to-band recombination, leading to an increase in the slower decay time. The findings offer crucial insights for optimizing GaSbBi for hot carrier solar cell applications.

A tool for live-cell confocal imaging of temperature-dependent organelle dynamics.

Intracellular organelles alter their morphology in response to ambient conditions such as temperature to optimize physiological activities in cells. Observing organelle dynamics at various temperatures deepens our understanding of cellular responses to the environment. Confocal laser microscopy is a powerful tool for live-cell imaging of fluorescently labeled organelles. However, the large contact area between the specimen and the ambient air on the microscope stage makes it difficult to maintain accurate cellular temperatures. Here, we present a method for precisely controlling cellular temperatures using a custom-made adaptor that can be installed on a commercially available temperature-controlled microscope stage. Using this adaptor, we observed temperature-dependent organelle dynamics in living plant cells; morphological changes in chloroplasts and peroxisomes were temperature dependent. This newly developed adaptor can be easily placed on a temperature-controlled stage to capture intracellular responses to temperature at unprecedentedly high resolution.

Application of temperature-dependent and steered molecular dynamics simulation to screen anti-dengue compounds against Marburg virus

Marburg virus infections are extremely fatal with a fatality range of 23% to 90%, therefore there is an urgent requirement to design and develop efficient therapeutic molecules. Here, a comprehensive temperature-dependent molecular dynamics (MD) simulation method was implemented to identify the potential molecule from the anti-dengue compound library that can inhibit the function of the VP24 protein of Marburg. Virtual high throughput screening identified five effective binders of VP24 after screening 484 anti-dengue compounds. These compounds were treated in MD simulation at four different temperatures: 300, 340, 380, and 420 K. Higher temperatures showed dissociation of hit compounds from the protein. Further, triplicates of 100 ns MD simulation were conducted which showed that compounds ID = 118717693, and ID = 5361 showed strong stability with the protein molecule. These compounds were further validated using Δ G binding free energies and they showed: −30.38 kcal/mol, and −67.83 kcal/mol binding free energies, respectively. Later, these two compounds were used in steered MD simulation to detect its dissociation. Compound ID = 5361 showed the maximum pulling force of 199.02 kcal/mol/nm to dissociate the protein-ligand complex while ID = 118717693 had a pulling force of 101.11 kcal/mol/nm, respectively. This ligand highest number of hydrogen bonds with varying occupancies at 89.93%, 69.80%, 57.93%, 52.33%, and 50.63%. This study showed that ID = 5361 can bind with the VP24 strongly and has the potential to inhibit its function which can be validated in the in-vitro experiment. Communicated by Ramaswamy H. Sarma