Low-frequency Vibrational Modes Research Articles

Comparative study of the vibrational contributions to electrochemical potential in Na[formula omitted]-Mn-DOBDC and Li[formula omitted]-Mn-DOBDC electrodes

We present a theoretical analysis of the vibrational contributions to the equilibrium voltage for Li-MOF and Na-MOF electrochemical cells. Our analysis relies on DFT calculations and ab-initio molecular dynamics. We explore factors that affect these vibrational contributions to the electrochemical potential, such as the mass of alkali ions and temperature dependency. We show that substituting Li with Na results in significant alterations to the electrochemical potential, primarily driven by atomic vibrations. Furthermore, we demonstrate that the temperature dependency of the electrochemical potential can be predominantly attributed to the low-frequency vibrational modes within the systems.

Heat Transfer Enhancement in Tree-Structured Polymer Linked Gold Nanoparticle Networks.

Human brains use a tree-like neuron network for information processing at high efficiency and low energy consumption. Tree-like structures have also been engineered to enhance mass and heat transfer in various applications. In this work, we reveal the heat transfer mechanism in tree-structured polymer linked gold nanoparticle (AuNP) networks using atomistic simulations. We report both upward and downward heat fluxes between root and leaf nodes in tree-structured polyethylene (PE) and poly(p-phenylene) (PPP) linked AuNP networks at tree levels from 1 to 5. We found that the heat conductance increases with an increasing polymer tree level. The heat transfer enhancement is due to the resulting increase in the low-frequency vibrational modes. This and other thermal properties are affected by the location of the AuNPs in the tree. Moreover, complex tree structures with at least five levels were found to be robust in the sense that disabling half of the leaves did not change the overall heat conductance.

Effect of Support Stiffness Nonlinearity on the Low-Frequency Vibro-Acoustic Characteristics for a Mechanical Equipment—Floating Raft—Underwater Cylindrical Shell Coupled System

The low-frequency vibro-acoustic characteristics of a mechanical equipment—floating raft—cylindrical shell—underwater acoustic field coupled system with nonlinear supports are studied in this paper. Firstly, the state space equations were established by a modal superposition theory for the coupled system, and a modal parameter identification method was deduced and verified for the cylindrical shell—underwater acoustic field coupled subsystem. On this basis, the formulas were derived for transmitted power flow in the coupled system, and the nonlinear stiffness constitutive relation of the vibration isolation supports was expressed by softening and hardening characteristics. Finally, dynamic simulations were carried out by the Runge—Kutta method to analyze the effect of nonlinear stiffness characteristic parameters on the low-frequency vibration modes and vibro-acoustic transfer characteristics in the coupled system. The research shows that a superharmonic phenomenon is common in the steady vibration mode of the coupled system with a nonlinear softening (or hardening) stiffness characteristic under harmonic excitation. The stronger the softening (or hardening) stiffness characteristic is, the more complex the vibration form is, and the smaller (or larger) the low-frequency vibro-acoustic transfer level in resonance regions is.

Enhanced vibrational stability in glass droplets.

We show through simulations of amorphous solids prepared in open-boundary conditions that they possess significantly fewer low-frequency vibrational modes compared to their periodic boundary counterparts. Specifically, using measurements of the vibrational density of states, we find that the law changes to with in two dimensions and in three dimensions. Crucially, this enhanced stability is achieved when utilizing slow annealing protocols to generate solid configurations. We perform an anharmonic analysis of the minima corresponding to the lowest frequency modes in such open-boundary systems and discuss their correlation with the density of states. A study of various system sizes further reveals that small systems display a higher degree of localization in vibrations. Lastly, we confine open-boundary solids in order to introduce macroscopic stresses in the system, which are absent in the unconfined system and find that the behavior is recovered.

Analysis of the Seismic Performance of ±500 kV Flexible DC Converter Valves

The converter valve is the core equipment of flexible DC transmission, but it has been severely damaged in previous earthquakes. Therefore, the seismic performance of its structure has a significant impact on the safety and reliability of power transmission. To study the seismic performance of ±500 kV flexible DC converter valves and identify weak links in the supporting valve tower, this article first established a refined finite-element model of a valve tower based on its physical structure; then modal analysis on the valve tower was conducted; finally, time-domain analysis of the valve tower under three seismic excitations, namely Wenchuan, EI Centro, and artificial, was conducted, and the equivalent stress and directional displacement cloud maps of the key parts of the valve tower were obtained. The research results indicate that the dynamic characteristics of the valve tower are relatively complex, with low fundamental frequency and diverse natural vibration modes. Under earthquake action, the predominant frequency of EI Centro waves is close to the fundamental frequency of the valve tower, which is prone to resonance and causes significant damage to the valve structure. The improved design of the valve tower meets the seismic strength requirements of level 8 seismic intensity.

Phonon-mediated superconductivity in the Sb square-net compound LaCuSb2

We investigated the electronic structure and superconducting properties of single-crystalline LaCuSb$_2$. The resistivity, magnetization, and specific heat measurements showed that LaCuSb$_2$ is a bulk superconductor. The observed Shubnikov-de Haas oscillation and magnetic field dependence of the Hall resistivity can be reasonably understood assuming a slightly hole-doped Fermi surface. Electron-phonon coupling calculation clarified the difference from the isostructural compound LaAgSb$_2$ indicating that (i) low-frequency vibration modes related to the interstitial layer sandwiched between the Sb-square nets significantly contribute to the superconductivity and (ii) carriers with sizable electron--phonon coupling distribute isotropically on the Fermi surface. These are assumed to be the origin of higher superconducting transition temperature compared with LaAgSb$_2$. We conclude that the superconducting properties of LaCuSb$_2$ can be understood within the framework of conventional phonon-mediated mechanism.

Insight on charge-transfer regimes in electron-phonon coupled molecular systems via numerically exact simulations

Various simulation approaches exist to describe charge transport in organic solids, offering significantly different descriptions of the physics of electron-phonon coupling. This variety introduces method-dependent biases, which inevitably result in difficulties to interpret charge transport processes in a unified picture. Here, we combine numerical and analytical quantum approaches to investigate the charge-transfer dynamics in an unbiased framework. We unveil the fading of transient localisation and the formation of polarons in a broad range of vibrational frequencies and temperatures. By studying the joint electron-phonon dynamics from femtoseconds to nanoseconds, we identify three distinct charge-transport regimes: transient localisation, Soft Gating, and polaron transport. The dynamic transitions between such regimes are ruled by a buildup of the correlations between electronic motion and nuclei, which lead to the crossover between transient localisation and polaron transport. This transition is seamless at all temperatures and adiabaticities, even in the limit of low-frequency vibrational modes.

Atomistic Insights into the Origin of High-Performance Thermoelectric Response in Hybrid Perovskites.

Due to their tantalizing prospect of heat-electricity interconversion, hybrid organic-inorganic perovskites have sparked considerable research interests recently. Nevertheless, understanding their complex interplay between the macroscopic properties, nonintuitive transport processes, and basic chemical structures still remains far from completion, although it plays a fundamental role in systematic materials development. On the basis of multiscale first-principles calculations, this understanding is herein advanced by establishing a comprehensive picture consisting of atomic and charge dynamics. It is unveiled that the ultralow room-temperature lattice thermal conductivity (≈0.20W m-1 K-1 ) of hybrid perovskites is critical to their decent thermoelectric figure of merit (≈0.34), and such phonon-glass behavior stems from not only the inherent softness but also the strong anharmonicity. It is identified that the 3D electrostatic interaction and hydrogen-bonded networks between the PbI3- cage and embedded cations result in the strongly coupled motions of inorganic framework and cation, giving rise to their high degree of anharmonicity. Furthermore, such coupled motions bring about low-frequency optical vibrational modes, which leads to the dominant role of electron scattering with optical phonons in charge transport. It is expected that these new atomistic-level insights offer a standing point where the performance of thermoelectric perovskites can be further enhanced.

Femtosecond symmetry breaking and coherent relaxation of methane cations via x-ray spectroscopy

Understanding the relaxation pathways of photoexcited molecules is essential to gain atomistic-level insight into photochemistry. We performed a time-resolved study of ultrafast molecular symmetry breaking through geometric relaxation (Jahn-Teller distortion) on the methane cation. Attosecond transient absorption spectroscopy with soft x-rays at the carbon K-edge revealed that the distortion occurred within 10 ± 2 femtoseconds after few-femtosecond strong-field ionization of methane. The distortion activated coherent oscillations in the asymmetric scissoring vibrational mode of the symmetry-broken cation, which were detected in the x-ray signal. These oscillations were damped within 58 ± 13 femtoseconds because vibrational coherence was lost with the energy redistributing into lower-frequency vibrational modes. This study completely reconstructs the molecular relaxation dynamics of this prototypical example and opens avenues for exploring complex systems.

Terahertz emission from transient currents and coherent phonons in layered MoSe2 and WSe2

Terahertz (THz) time-domain emission spectroscopy was performed on layered 2H-MoSe 2 and 2H-WSe 2. The THz emission shows an initial cycle attributed to surge currents and is followed by oscillations attributed to coherent interlayer phonon modes. To obtain the frequencies of the interlayer vibrations, an analysis of the THz emission waveforms was performed, separating the two contributions to the total waveform. Results of the fitting show several vibrational modes in the range of 5.87–32.75 cm − 1 for the samples, attributed to infrared-active interlayer shear and breathing modes. This study demonstrates that THz emission spectroscopy provides a means of observing these low-frequency vibrational modes in layered materials.

Scaling of the non-phononic spectrum of two-dimensional glasses.

Low-frequency vibrational harmonic modes of glasses are frequently used to rationalize their universal low-temperature properties. One well studied feature is the excess low-frequency density of states over the Debye model prediction. Here, we examine the system size dependence of the density of states for two-dimensional glasses. For systems of fewer than 100 particles, the density of states scales with the system size as if all the modes were plane-wave-like. However, for systems greater than 100 particles, we find a different system-size scaling of the cumulative density of states below the first transverse sound mode frequency, which can be derived from the assumption that these modes are quasi-localized. Moreover, for systems greater than 100 particles, we find that the cumulative density of states scales with the frequency as a power law with the exponent that leads to the exponent β = 3.5 for the density of states. For systems whose sizes were investigated, we do not see a size-dependence of exponent β.

Radiation from UV-A to Red Light Induces ROS-Dependent Release of Neutrophil Extracellular Traps

Neutrophils release decondensed chromatin or extracellular traps (NETs) in response to various physiological and pharmacological stimuli. Apart from host defensive functions, NETs play an essential role in the pathogenesis of various autoimmune, inflammatory, and malignant diseases. In recent years, studies have been performed on photo-induced NET formation, mainly activated by UV radiation. Understanding the mechanisms of NET release under the influence of UV and visible light is important to control the consequences of the damaging effects of electromagnetic radiation. Raman spectroscopy was applied to record characteristic Raman frequencies of various reactive oxygen species (ROS) and low-frequency lattice vibrational modes for citrulline. NETosis was induced by irradiation with wavelength-switchable LED sources. Fluorescence microscopy was used to visualize and quantify NET release. The ability of five wavelengths of radiation, from UV-A to red light, to induce NETosis was investigated at three different energy doses. We demonstrated, for the first time, that NET formation is activated not only by UV-A but also by three spectra of visible light: blue, green, and orange, in a dose-dependent manner. Using inhibitory analysis, we established that light-induced NETosis proceeds through NADPH oxidase and PAD4. The development of new drugs designed to suppress NETosis, especially when induced by exposure to intense UV and visible light, can help to mitigate light-induced photoaging and other damaging effects of electromagnetic radiation.

A Future with Machine Learning: Review of Condition Assessment of Structures and Mechanical Systems in Nuclear Facilities

The nuclear industry is exploring applications of Artificial Intelligence (AI), including autonomous control and management of reactors and components. A condition assessment framework that utilizes AI and sensor data is an important part of such an autonomous control system. A nuclear power plant has various structures, systems, and components (SSCs) such as piping-equipment that carries coolant to the reactor. Piping systems can degrade over time because of flow-accelerated corrosion and erosion. Any cracks and leakages can cause loss of coolant accident (LOCA). The current industry standards for conducting maintenance of vital SSCs can be time and cost-intensive. AI can play a greater role in the condition assessment and can be extended to recognize concrete degradation (chloride-induced damage and alkali–silica reaction) before cracks develop. This paper reviews developments in condition assessment and AI applications of structural and mechanical systems. The applicability of existing techniques to nuclear systems is somewhat limited because its response requires characterization of high and low-frequency vibration modes, whereas previous studies focus on systems where a single vibration mode can define the degraded state. Data assimilation and storage is another challenging aspect of autonomous control. Advances in AI and data mining world can help to address these challenges.

Identification and low-frequency vibrational analysis of three free anthraquinones via terahertz spectroscopy

In this study, terahertz time-domain spectroscopy (THz-TDS) was used to obtain the terahertz absorption spectra of three free anthraquinones (Chrysophanol, Emodin, Physcion) in the frequency range of 0.2–4.3 THz. The results show that terahertz spectroscopy is an effective detecting such compounds. Meanwhile, the theoretical spectrum using density functional theory calculations agrees well with the experimental spectrum. A modal decoupling method was used to identify each low-frequency vibrational mode and determine the average contribution of different atoms and groups. Modal decoupling provides a better understanding of molecules' mixed vibrational modes and enables quantifying the atoms' vibrational contributions. Results show that the substituent group facilitates the transition between the fundamental vibrational modes; subsequently, the substituent group shifts the vibrational centre of gravity of the three molecules and affects the vibrational contribution of hydrogen bonds. Furthermore, insignificant Emodin absorption is related to the nearly symmetrical structure formed by the substituents. The feasibility of terahertz analysis of differential molecular structures has also been confirmed.

Element- and enantiomer-selective visualization of molecular motion in real-time

Ultrafast optical-domain spectroscopies allow to monitor in real time the motion of nuclei in molecules. Achieving element-selectivity had to await the advent of time resolved X-ray spectroscopy, which is now commonly carried at X-ray free electron lasers. However, detecting light element that are commonly encountered in organic molecules, remained elusive due to the need to work under vacuum. Here, we present an impulsive stimulated Raman scattering (ISRS) pump/carbon K-edge absorption probe investigation, which allowed observation of the low-frequency vibrational modes involving specific selected carbon atoms in the Ibuprofen RS dimer. Remarkably, by controlling the probe light polarization we can preferentially access the enantiomer of the dimer to which the carbon atoms belong.

Detection of Delaminations in Concrete Plates Using a Laser Ablation Impact Echo Technique

This study investigates the non-destructive detection of delaminations in concrete plates using non-contact laser ablation, instead of the conventional hammer excitation, as part of the impact echo method. We performed tests on five concrete specimens of different sizes, two of which contained artificial delaminations. A range of steel ball hammers was used as reference impulse sources, the responses of which were compared with wave excitation generated by a 7 ns pulsed 1064 nm Nd:YAG laser with 150 mJ pulse energy. Signals were recorded by surface-mounted accelerometers and two contactless methods: microphones and a laser Doppler vibrometer. The laser generates frequencies across a broad range of frequencies (0 to 150 kHz) but with much less energy than the hammers' narrower frequency spectra; the laser pulse energy transferred into the specimen is 0.07 mJ, corresponding to about 0.5 ‰ of the impulse source energy. Because of this, the thick intact plates' characteristic thickness stretch resonance frequency can be reliably detected by the hammer excitations but not when using laser excitation. However, the laser can excite low-frequency flexural vibration modes over a shallow delamination at 3 cm depth. The low-frequency flexural vibration results are verified by numerical natural frequency analysis.

Highly efficient transient stimulated Raman scattering on secondary vibrational mode of BaWO4 crystal due to its constructive interference with self-phase modulation

An exceptionally high stimulated Raman scattering (SRS) conversion efficiency to the first Stokes component associated with the secondary (low-frequency and low intensity) vibrational mode ν2 (∼330 cm-1) was observed in a BaWO4 crystal in a highly transient regime of interaction. The effect takes place in the range of pump pulse energy from ∼0.1 to ∼0.5 µJ with maximum energy conversion efficiency up to 35% at 0.2 µJ. The nature of the observed effects is explained by interference of SRS and self-phase modulation, where the latter is related to a noninstantaneous orientational Kerr nonlinearity in the BaWO4 crystal.

A two-dimensional nonlinear vibration absorber using elliptical impacts and sliding

Highly flexible structures often exhibit multiple low-frequency modes of vibration in multiple directions that vibrate with relatively high amplitudes. As a result, new two-dimensional vibration absorbers that target the motion of multiple modes are needed to mitigate motion of these structures. This research proposes a novel two-dimensional nonlinear vibration absorber (2D-NVA) as a method of vibration reduction for flexible structures that possess multiple low-frequency modes in multiple directions. The proposed 2D-NVA is composed of two low-mass bodies, called the housing and impactor, that are installed on the linear primary structure using strong and weak coupling stiffness, respectively. The housing is composed of a ring-like rigid body with the cavity in the shape of an ellipse, and the impactor is composed of a rigid body or particle that resides inside the housing. The nonlinearity arises through contact between the interior of the housing and impactor, and both impacts and constrained sliding with friction are allowed. The behavior of the proposed 2D-NVA is investigated both computationally and experimentally, and it is shown to dramatically reduce motion of a two-dimensional linear structure in both directions under varying amplitude of impulsive excitations.

High-temperature superconductivity in two-dimensional hydrogenated titanium diboride: Ti2B2H4

In recent years, superconductivity in two-dimensional (2D) layered hexagonal metal borides has aroused much interests. Here, based on first-principles calculations, we theoretically report a new type of 2D hydrogenated transition-metal diboride: Ti2B2H4. Results reveal that the introduction of hydrogen atoms expands the frequency range of phonon spectrum of monolayer Ti2B2, and significantly increases the electron-phonon coupling (EPC). The calculated EPC constant λ of Ti2B2H4 is 1.18, and the corresponding superconducting critical temperature (Tc) is 48.6 K, exceeding the McMillan limit (39 K). The EPC mainly originates from the coupling between electrons in Ti-3d orbitals and the low-frequency vibration modes of Ti atoms as well as high-frequency vibration modes of H atoms. Additionally, the coupling strength can be further increased to 1.61 by applying appropriate biaxial compressive strain, and the corresponding Tc can be boosted to 69.4 K, approaching to liquid nitrogen (N2) temperature. The predicted Ti2B2H4 provides a new platform for 2D superconductivity and may have potential applications in 2D nanodevices.

Entangling mechanical vibrations of two massive ferrimagnets by fully exploiting the nonlinearity of magnetostriction

Quantum entanglement in the motion of macroscopic objects is of significance to both fundamental studies and quantum technologies. Here we show how to entangle the mechanical vibration modes of two massive ferrimagnets that are placed in the same microwave cavity. Each ferrimagnet supports a magnon mode and a low-frequency vibration mode coupled by the magnetostrictive force. The two magnon modes are, respectively, coupled to the microwave cavity by the magnetic dipole interaction. We first generate a stationary nonlocal entangled state between the vibration mode of the ferrimagnet-1 and the magnon mode of the ferrimagnet-2. This is realized by continuously driving the ferrimagnet-1 with a strong red-detuned microwave field and the entanglement is achieved by exploiting the magnomechanical parametric down-conversion and the cavity–magnon state-swap interaction. We then switch off the pump on the ferrimagnet-1 and, simultaneously, turn on a red-detuned pulsed drive on the ferrimagnet-2. The latter drive is used to activate the magnomechanical beamsplitter interaction, which swaps the magnonic and mechanical states of the ferrimagnet-2. Consequently, the previously generated phonon–magnon entanglement is transferred to the mechanical modes of two ferrimagnets. The work provides a scheme to prepare entangled states of mechanical motion of two massive objects, which may find applications in various studies exploiting macroscopic entangled states.