Breathing Mode Research Articles

All-optical quality control of indenene intercalation into graphene/SiC

Intercalating two-dimensional quantum materials beneath a sheet of graphene provides effective environmental protection and facilitates ex situ device fabrication. However, developing a functional device requires rapid, large-scale screening methods to evaluate the quality of the intercalant, which to date can be monitored only by slow, ultra-high vacuum-based surface science techniques. In this study, we utilize ex situ Raman micro-spectroscopy to optically and nondestructively identify the quantum spin Hall insulator indenene, a monolayer of indium sandwiched between a SiC(0001) substrate and a single sheet of graphene. Color modulation combined with indenene's distinctive low-frequency Raman fingerprint enables rapid assessment of its homogeneity and crystalline quality. Density functional perturbation theory indicates that this Raman signature originates mainly from indenene's shear and breathing modes, while additional higher order modes are tentatively attributed to defect-assisted and two-phonon Raman processes.

A comprehensive study of beam modal functions in the free vibration analysis of cylindrical shells: Critical examination on the applicability to the clamped-free boundary condition

Over the past few decades, approximate methods that can provide solutions of sufficient accuracy have received considerable attention in the free vibration analysis of cylindrical shells, where a great deal of studies adopted the beam modal functions as the trial functions for the axial mode shapes of cylindrical shells. Nevertheless, most studies were restricted to the application of single term beam modal function and failed to simulate elastic boundary conditions of cylindrical shells, while the accuracy of the corresponding methods has recently sparked significant controversy, especially for cylindrical shells under the clamped-free boundary condition. This paper presents a comparative study of three forms of beam modal functions in the free vibration analysis of cylindrical shells, one of which is proposed for the first time to simulate elastic boundary conditions of cylindrical shells. A unified model is developed using the general Rayleigh–Ritz method, incorporating the breathing modes with circumferential orders being zero, and four types of commonly used thin shell theories, namely the Donnell, Reissner, Love, and Sanders theories. From both perspectives of natural frequencies and mode shapes, numerical results are validated by comparison with those existing in the literature and those calculated from the finite element method (FEM). The results not only clarify the distinction of different forms of beam modal functions used in the Rayleigh-Ritz method, but also provide explanations for the controversy raised in recent studies. Furthermore, the unified formulations can be extended to vibration analysis of various forms of shell structures, and can also be helpful to the vibration analysis of beams and plates with elastic boundary conditions.

Cyclic and helical symmetry-informed machine learned force fields: Application to lattice vibrations in carbon nanotubes

We present a formalism for developing cyclic and helical symmetry-informed machine learned force fields (MLFFs). In particular, employing the smooth overlap of atomic positions descriptors with the polynomial kernel method, we derive cyclic and helical symmetry-adapted expressions for the energy, atomic forces, and phonons, i.e., lattice vibration frequencies and modes. We use this formulation to construct a symmetry-informed MLFF for carbon nanotubes (CNTs), where the model is trained through Bayesian linear regression, with the data generated from ab initio density functional theory (DFT) calculations performed during on-the-fly symmetry-informed MLFF molecular dynamics simulations of representative CNTs. We demonstrate the accuracy of the MLFF model by comparisons with DFT calculations for the energies and forces, and density functional perturbation theory calculations for the phonons, while considering CNTs not used in the training. In particular, we obtain a root mean square error of 1.4×10−4 Ha/atom, 4.7×10−4 Ha/Bohr, and 4.8 cm−1 in the energy, forces, and phonon frequencies, respectively, which are well within the accuracy targeted in ab initio calculations. We apply this framework to study phonons in CNTs of various diameters and chiralities, where we identify the torsional rigid body mode that is unique to cylindrical structures and establish laws for variation of the phonon frequencies associated with the ring modes and radial breathing modes. Overall, the proposed formalism provides an avenue for studying nanostructures with cyclic and helical symmetry at ab initio accuracy, while providing orders-of-magnitude speedup relative to such methods.

A numerical study on the oscillatory dynamics of tip vortex cavitation

In this paper, we numerically study the mechanism of the oscillatory flow dynamics associated with the tip vortex cavitation (TVC) over an elliptical hydrofoil section. Using our recently developed three-dimensional variational multiphase flow solver, we investigate the TVC phenomenon at Reynolds number $Re = 8.95 \times 10^5$ via dynamic subgrid-scale modelling and the homogeneous mixture theory. To begin, we examine the grid resolution requirements and introduce a length scale considering both the tip vortex strength and the core radius. This length scale is then employed to non-dimensionalize the spatial resolution in the tip vortex region, the results of which serve as a basis for estimation of the required mesh resolution in large eddy simulations of TVC. We next perform simulations to analyse the dynamical modes of tip vortex cavity oscillation at different cavitation numbers, and compare them with the semi-analytical solution. The breathing mode of cavity surface oscillation is extracted from the spatial-temporal evolution of the cavity's effective radius. The temporally averaged effective radius demonstrates that the columnar cavity experiences a growth region followed by decay as it progresses away from the tip. Further examination of the characteristics of local breathing mode oscillations in the growth and decay regions indicates the alteration of the cavity's oscillatory behaviour as it travels from the growth region to the decay region, with the oscillations within the growth region being characterized by lower frequencies. For representative cavitation numbers $\sigma \in [1.2,2.6]$ , we find that pressure fluctuations exhibit a shift of the spectrum towards lower frequencies as the cavitation number decreases, similar to its influence on breathing mode oscillations. The results indicate the existence of correlations between the breathing mode oscillations and the pressure fluctuations. While the low-frequency pressure fluctuations are found to be correlated with the growth region, the breathing mode oscillations within the decay region are related to higher-frequency pressure fluctuations. The proposed mechanism can play an important role in developing mitigation strategies for TVC, which can reduce the underwater radiated noise by marine propellers.

Spatiotemporal pattern formation in parametrically driven two-dimensional Bose–Einstein condensates

We investigate spatiotemporal periodic patterns in harmonically trapped Bose–Einstein condensates (BECs) driven by a periodic modulation of the interaction. Resonant with the breathing mode, we show the emergence of a square lattice pattern containing two orthonormal stripes. We study the time evolutions of the lattice patterns for different driving strengths and dissipations. We find that its spatial periodicity and temporal oscillating frequency match the Bogoliubov dispersion, which is the intrinsic property of the system and relevant to the parametric amplification of elementary excitations. In the circumstances of strong driving strength and low dissipation, we further observe the triad interaction and the resulting superlattice state, which are well explained by the nonlinear amplitude equation for superimposed stripes. These results shed light on unexplored nonlinear spatiotemporal dynamics of two-dimensional patterns in harmonically trapped BECs that can pave the way for engineering exotic patterns by state-of-the-art experiments.

Unveiling Structural Variations in Armchair-Edge Coronoids by Spectroscopies.

This study explores the electronic and vibrational properties of armchair coronoids (ACs), a unique class of polycyclic aromatic hydrocarbons with varying molecular and cavity sizes. Through density functional theory simulations, we investigated the X-ray photoelectron spectroscopy (XPS) and Raman spectra of C222, C114, C42, and their derivatives with different cavity sizes. The results reveal that band gaps and electronic properties of ACs can be precisely tuned by adjusting the molecular and cavity dimensions. XPS spectra demonstrated shifts in binding energy correlating with bandgap variations, while Raman spectra exhibited distinct C-C stretching and breathing modes. Notably, the introduction of cavities led to shifts in the breathing mode band, providing insights into the structural identification of ACs through Raman spectroscopy. The findings suggest that combining XPS and Raman spectroscopy can effectively characterize ACs, offering a comprehensive understanding of their structure-property relationships. This research lays the groundwork for future experimental and theoretical studies on the potential applications of ACs in electronic materials.

Sr-Doping-Modulated Metal-Insulator Transition in NdNiO3 Epitaxial Films

Abstract Perovskite-structured nickelates, ReNiO3 (Re = rare earth), have long garnered significant research interest due to their sharp and highly tunable metal-insulator transitions (MITs). Doping the parent compound ReNiO3 with alkaline earth metal can substantially suppress this MIT. Recently, intriguing superconductivity has been discovered in doped infinite-layer nickelates (ReNiO2), while the mechanism behind A-site doping-suppressed MIT in the parent compound ReNiO3 remains unclear. To address this problem, we grew a series of Nd1−x Sr x NiO3 (NSNO, x = 0–0.2) thin films and conducted systematic electrical transport measurements. Our resistivity and Hall measurements suggest that Sr-induced excessive holes are not the primary reason for MIT suppression. Instead, first-principles calculations indicate that Sr cations, with larger ionic radius, suppress breathing mode distortions and promote charge transfer between oxygen and Ni cations. This process weakens Ni–O bond disproportionation and Ni2+/Ni4+ charge disproportionation. Such significant modulations in lattice and electronic structures convert the ground state from a charge-disproportionated antiferromagnetic insulator to a paramagnetic metal, thereby suppressing the MIT. This scenario is further supported by the weakened MIT observed in the tensile-strained NSNO/SrTiO3(001) films. Our work reveals the A-side doping-modulated electrical transport of perovskite nickelate films, providing deeper insights into novel electric phases in these strongly correlated nickelate systems.

All-Optical Control of Bubble and Skyrmion Breathing.

Controlling the dynamics of topologically protected spin objects by all-optical means promises enormous potential for future spintronic applications. Excitation of bubbles and skyrmions in ferrimagnetic [Fe(0.35 nm)/Gd(0.40 nm)]_{160} multilayers by ultrashort laser pulses leads to a periodic modulation of the core diameter of these spin objects, the so-called breathing mode. We demonstrate versatile amplitude and phase control of this breathing using a double excitation scheme, where the observed dynamics is controlled by the excitation delay. We gain insight into both the timescale on which the breathing mode is launched and the role of the spin object size on the dynamics. Our results demonstrate that ultrafast optical excitation allows for precise tuning of the spin dynamics of trivial and nontrivial spin objects, showing a possible control strategy in device applications.

Fate of Boltzmann's breathers: Kinetic theory perspective.

The dynamics of a system composed of elastic hard particles confined by an isotropic harmonic potential are studied. In the low-density limit, the Boltzmann equationprovides an excellent description, and the system does not reach equilibrium except for highly specific initial conditions: it generically evolves toward and stays in a breathing mode. This state is periodic in time, with a Gaussian velocity distribution, an oscillating temperature, and a density profile that oscillates as well. We characterize this breather in terms of initial conditions and constants of the motion. For low but finite densities, the analysis requires taking into account the finite size of the particles. Under well-controlled approximations, a closed description is provided, which shows how equilibrium is reached at long times. The (weak) dissipation at work erodes the breather's amplitude, while concomitantly shifting its oscillation frequency. An excellent agreement is found between molecular dynamics simulation results and the theoretical predictions for the frequency shift. For the damping time, the agreement is not as accurate as for the frequency and the origin of the discrepancies is discussed.

Extended quantum molecular dynamics model predicts new breathing modes in $$^{36}$$Ar bubble nuclei

Extended quantum molecular dynamics model predicts new breathing modes in $$^{36}$$Ar bubble nuclei

The use of 1D carbon nanotube interacting with caffeine molecules for applications in solar cells: structure optimisation, Raman analysis and optoelectronic properties

This study proposes a promising candidate for organic solar cells through the creation of a novel nano-hybrid system composed of caffeine molecules encapsulated within a semiconducting single-walled carbon nanotube known as NT14 (14,0). The stability and optoelectronic properties of this hybrid system, designated as CA@NT14, were thoroughly investigated. We determined the optimal diameter for the NT14 nanotube using molecular mechanics, Density Functional Theory, spectral moment’s method, and bond polarizability model, finding it to be approximately 1.18 nm. The encapsulation’s impact on the Raman-active modes, specifically the radial breathing mode and tangential mode, was analyzed through Raman spectra calculations, revealing structural stability and charge transfer from CA to NT14. Notably, the NT14’s Fermi level position increased upon encapsulation, indicating charge transfer and a type-II band alignment. The study further examined the bandgap characteristics of the hybrid system, finding that the encapsulation of CA within semiconducting NT14 nanotubes minimally impacts the nanotube’s bandgap, thus retaining its excellent visible light absorption properties. Conversely, encapsulating CA within metallic nanotubes significantly reduces their bandgap, limiting their light absorption range. The nonresonant Raman responses of NT14 pre- and post-encapsulation corroborated the charge transfer between CA and NT14. Future research will focus on computing the electronic transport characteristics, transmission spectra, I-V characteristics, and yield of CA@NT14 using DFT and Non-Equilibrium Green’s Function ( formalism. An experimental study will be conducted to validate these theoretical findings. These results indicate the potential of CA@NT14 hybrids as effective active layers in organic solar cells, highlighting their significance in advancing optoelectronic applications.

Theoretical Hints to Optimize Energy Dissipation and Cell–Cell Response in Quantum Cellular Automata Based on Tetrameric and Bidimeric Cells

This article is largely oriented towards the theoretical foundations of the rational design of molecular cells for quantum cellular automata (QCA) devices with optimized properties. We apply the vibronic approach to the analysis of the two key properties of such molecular cells, namely the cell–cell response and energy dissipation in the course of the non-adiabatic switching of the electric field acting on the cell. We consider two kinds of square planar cells, namely cells represented by a two-electron tetrameric mixed valence (MV) cluster and bidimeric cells composed of two one-electron MV dimeric half-cells. The model includes vibronic coupling of the excess electrons with the breathing modes of the redox sites, electron transfer, intracell interelectronic Coulomb repulsion, and also the interaction of the cell with the electric field of polarized neighboring cells. For both kinds of cells, the heat release is shown to be minimal in the case of strong delocalization of excess electrons (weak vibronic coupling and/or strong electron transfer) exposed to a weak electric field. On the other hand, such a parametric regime proves to be incompatible with a strong nonlinear cell–cell response. To reach a compromise between low energy dissipation and a strong cell–cell response, we suggest using weakly interacting MV molecules with weak electron delocalization as cells. From this point of view, bidimeric cells are advantageous over tetrameric ones due to their smaller number of electron transfer pathways, resulting in a lower extent of electron delocalization. The distinct features of bidimeric cells, such as their two possible mutual arrangements (“side-by-side” and “head-to-tail”), are discussed as well. Finally, we briefly discuss some relevant results from a recent ab initio study on electron transfer and vibronic coupling from the perspective of the possibility of controlling the key parameters of molecular QCA cells.

Characterisation Analysis of Sulphur and Phosphorous Doped and Co-doped Graphitic Carbon Nitride (g-C3N4) Materials

Graphitic carbon nitride (g-C3N4) is tailored with doping of different non-metals (Sulphur and Phosphorus). For synthesis through thermal condensation method, the mixtures of urea and dopant with diverse concentrations have been added for preparation of materials. The basic effect of doping and its concentration on the structural morphology and absorption spectra of the samples is investigated in detail. Pure g-C3N4 suffers from high recombination rate of photogenerated electron-hole pairs resulting in low photocatalytic activity. Different techniques like X-ray diffraction (XRD), Scanning electron microscopy (SEM), Fourier transforms infrared (FTIR) spectroscopy, and Photoluminescence spectroscopy (PL) have been used for the characterization. X-ray diffraction studies confirm the formation of the g-C3N4 structure and SEM images reveal crumpled sheets and irregular plate like shapes of the doped graphitic nitride samples. FTIR analysis identify the presence of surface amino (N-H) and water (O-H) groups, cyano terminal group (C≡N), (C≡C), C–N) and (C=N) bonds and breathing mode of the tri-s-triazine units in the samples. PL spectra shows that the sulphur and phosphorus co-doped PSGCN (8 wt.%) sample is better for photocatalytic activity.

Coherent Phonon Dynamics in Plasmonic Gold Tetrahedral Nanoparticle Ensembles.

Coherent phonon modes supported by plasmonic nanoparticles offer prospective applications in chemical and biological sensing. Whereas the characterization of these phonon modes often requires single-particle measurements, synthetic routes to narrow size distributions of nanoparticles permit ensemble investigations. Recently, the synthesis of highly monodisperse gold tetrahedral nanoparticles with tunable edge lengths and corner sharpnesses has been developed. Herein, we characterize a size series of these nanoparticles in colloidal dispersion via transient absorption spectroscopy to examine their mechanical and plasmonic responses upon photoexcitation. Oscillations of transient absorption signals are observed in the plasmon resonance and correspond to the lowest-order radial breathing modes of the nanoparticles, the frequencies of which are affected by the edge length and truncation of the corners. Homogeneous quality factor values ranging from 24 to 34 are observed for the oscillations that convey potential utility in mass-sensing and plasmon-exciton-coupling photonics schemes. Finite-difference time domain and finite element analysis calculations establish specific optically relevant phonon modes.

Trigger mechanism for a singing cavitating tip vortex

The discrete tone radiated from tip vortex cavitation (TVC), known as ‘vortex singing’, was recognized in 1989, but its triggering remains unclear for over thirty years. In this study, the desinent cavitation number and viscous correction are applied to describe the dynamics of cavitation bubbles and the dispersion relation of cavity interfacial waves. The wavenumber-frequency spectrum of the cavity radius from the experiment in CSSRC indicates that singing waves predominantly consist of the stationary double helical modes (kθ = 2- and -2+) and the breathing mode (kθ = 0-), rather than standing waves as assumed in previous literatures. Moreover, two trigger mechanisms, expressed by two triggering lines, are proposed: the twisted TVC, initially at rest, is driven into motion through the corrected natural frequency (fn) due to the step change of the far-field pressure. Subsequently, the frequency associated with the zero-group-velocity point (ῶzgv) at kθ = 0- is excited through ῶi, the frequency at the intersection of dispersion curves at kθ = 0- and -2+, or ῶj, the frequency at the intersection of dispersion curves at kθ = 0- and 2-, corresponding to two types of the vortex singing triggering. These solutions, without empirical parameters, are validated using singing conditions provided by CSSRC and G.T.H., respectively. Furthermore, the coherence and the cross-power spectral density spectrum indicates a large-scale breathing wave propagating along the singing cavity surface and travelling from downstream to hydrofoil tip, providing us a comprehensive understanding for the triggering of vortex singing.

High pressure ferroelectric-like semi-metallic state in Eu-doped BaTiO3.

We have conducted a detailed high-pressure (HP) investigation on Eu-doped BaTiO3 using angle-resolved x-ray diffraction, Raman spectroscopy, and dielectric permittivity measurements. The x-ray diffraction data analysis shows a pressure-induced structural phase transition from the ambient tetragonal to the mixed cubic and tetragonal phases above 1.4GPa. The tetragonality of the sample due to the internal deformation of the TiO6 octahedra caused by the charge difference from Eu doping cannot be lifted by pressure. Softening, weakening, and disappearance of low-frequency Raman modes indicate ferroelectric tetragonal to the paraelectric cubic phase transition. However, the pressure-induced increase in the intensity of [E(LO), A1(LO)] and the octahedral breathing modes indicate that the local structural inhomogeneity remains in the crystal and is responsible for spontaneous polarization in the sample. The low-frequency electronic scattering response suggests pressure-induced carrier delocalization, leading to a semi-metallic state in the system. Our HP dielectric constant data can be explained by the presence of pressure-induced localized clusters of microscopic ferroelectric ordering. Our results suggest that the HP phase coexistence leads to a ferroelectric-like semi-metallic state in Eu-doped BaTiO3 under extreme quantum limits.

Extended Kataura plot of single-walled carbon nanotubes and on-demand fabrication of mixed-dimensional heterostructures

We present a comprehensive optical spectroscopic study on air-suspended single-walled carbon nanotubes (SWNTs) with diameters ranging from 1.7 nm to 3.4 nm and at higher-order optical transitions, a previously inaccessible regime. We establish an atlas of resonant radial breathing modes (RBMs) for more than 100 new SWNTs in this unknown regime, thus significantly extending the RBM dataset in Kataura plot and enhancing our knowledge of SWNTs. Additionally, we develop an innovative transfer technique for manipulating individual SWNTs of known chiralities (determined by optical spectroscopies) by integrating a polarization imaging technique with the conventional van der Waals (vdW) dry transfer. The unprecedented spatial and structural control of this technique enables a deterministic fabrication and integration of a variety of novel mixed-dimensional vdW heterostructures that were considered unachievable before. Our work significantly extends RBM dataset of SWNT Kataura plot and represents a huge advancement towards controlled fabrication and integration of mixed-dimensional vdW heterostructures encompassing one-dimensional vdW materials.

The best whistler: A cavitating tip vortex

The discrete tone radiated from a cavitating tip vortex, known as “vortex singing,” was first recognized in 1989, but its sound generation mechanism has remained a mystery for over 30 years. In this Letter, by means of the correction for the cavitation bubble dynamics and the dispersion relation of cavity interfacial waves, we found that after the far-end disturbances propagate upstream, the whistling vortex should be triggered by near-end sound sources, the breathing mode waves. Further utilizing the theoretical solutions for singing lines and the potential singing cavitation number with frequency, we accurately identified all available tests for seeking the vortex singing over the past three decades, which not only demonstrates that the vortex singing frequency is only determined by the measurable mean cavity radius (rc), cavitation number (σ), and desinent cavitation number (σd) in experiments, but also responses to a long-standing perplexity: why such a best whistler is able to appear only within a narrow range of the cavitation number.

Raman spectroscopy of atomically thin HfX2 (X=S, Se)

Abstract We investigated interlayer modes of few-layer HfX2 (X=S, Se) by using low-frequency micro-Raman spectroscopy with three excitation energies (1.96 eV, 2.33 eV, 2.54 eV) under vacuum condition (10−6 Torr). We observed interlayer modes in HfSe2 when the 2.54-eV excitation energy was used. The low-frequency Raman spectra reveal a series of shear and breathing modes (<50 cm−1) that are helpful for identifying the number of layers. The in-plane Eg and out-of-plane A1g modes of HfSe2 are located at ~150 cm−1 and ~200 cm−1, respectively. In HfS2, in-plane Eg and out-of-plane A1g optical phonons are observed at ~260 cm−1 and ~337 cm−1, respectively. The in-plane and out-of-plane force constants of atomically thin HfSe2 are obtained to be 1.87 ×1019 N/m3 and 6.55×1019 N/m3, respectively, by fitting the observed interlayer modes using the linear chain model. These results provide valuable information on materials parameters for device designs using atomically-thin layered HfX2 (X=S, Se).

Effect of polyelectrolyte (PAA) on the dynamics of weakly charged microemulsion droplets in acidic medium

We use the dynamic light scattering technique (DLS) to study the dynamic behavior of complex constituted by weakly charged microemulsion in the presence of polyelectrolyte. We investigated the impact of adding oppositely charged polyacid (PAA), which is a pH-dependent polyelectrolyte, on the dynamics of charged microemulsion nanodroplets in an acidic medium at pH = 4.5 when the polyacrylic acid are partially charged. In a diluted regime, two diffusive relaxation modes are seen when adding (upon addition) the polyacrylic acid PAA to the microemulsion nanodroplets due to collective diffusion and self-diffusion fluctuations. In the concentrated regime, we observed three diffusive relaxation modes when charged microemulsion nanodroplets complexed with oppositely charged polyacrylic acid. We attribute the two first relaxation modes to the collective diffusion (fluctuation of concentration) and self-diffusion of the microemulsion nanodroplets. The third mode which is a slower relaxation mode; we attribute this relaxation process to the motion of the network formed by the polyacid PAA and microemulsion nanodroplets, or “breathing mode” of the network.