Low-energy Modes Research Articles

Phonons reveal coupled cholesterol-lipid dynamics in ternary membranes.

Experimental studies of collective dynamics in lipid bilayers have been challenging due to the energy resolution required to observe these low-energy phonon-like modes. However, inelastic X-ray scattering (IXS) measurements - a technique for probing vibrations in soft and biological materials - are now possible with sub-meV resolution, permitting direct observation of low energy, phonon-like modes in lipid membranes. Here, IXS measurements with sub-meV energy resolution reveal a low-energy optic-like phonon mode at roughly 3 meV in the liquid-ordered (Lo) and liquid-disordered (Ld) phases of a ternary lipid mixture. This mode is only observed experimentally at momentum transfers greater than 5 nm-1 in the (Lo) system. A similar gapped mode is also observed in all-atom molecular dynamics (MD) simulations of the same mixture, indicating that the simulations accurately represnt the fast, collective dynamics in the (Lo) phase. It's optical nature and the Q range of the gap together suggest that the observed mode is due to the coupled motion of cholesterol-lipid pairs, separated by several hydrocarbon chains within the membrane plane. Analysis of the simulations provide molecular insight into the origin of the mode in transient, nanoscale substructures of hexagonally packed hydrocarbon chains. This nanoscale hexagonal packing was previously reported based on molecular dynamics simulations and later by NMR measurements. Here, however, the integration of IXS and MD simulations identifies a new signature of the L° substructure in the collective lipid dynamics, thanks to the recent confluence of IXS sensitivity and MD simulation capabilities.

Singular Continuous and Nonreciprocal Phonons in Quasicrystal AlPdMn.

In quasicrystals lacking translational symmetry but having highly ordered structures, understanding how phonons propagate in their aperiodic lattices remains an unsolved issue. We present an inelastic neutron scattering study on acoustic phonon modes of icosahedral quasicrystal AlPdMn, revealing hierarchical pseudo-gap structure in low-energy acoustic modes. Additionally, phonon intensities are asymmetric in energy and wave vectors with respect to the Bragg peak, indicating characteristic nonreciprocal phonon propagation in quasicrystals.

Prediction of novel layered indium halide superconductors

Abstract We design two new layered indium halide compounds LaOInF2 and LaOInCl2 by means of first-principles calculations and evolutionary crystal structure prediction. We find both compounds crystallize in a tetragonal structure with P4/nmm space group and have indirect band gaps of 2.58 eV and 3.21 eV, respectively. By substituting O with F, both of them become metallic and superconducting at low temperature. The F-doping leads to strong electron–phonon coupling in the low-energy acoustic phonon modes which is mainly responsible for the induced superconductivity. The total electron–phonon coupling strength are 1.86 and 1.48, while the superconducting transition temperature (T c) are about 7.2 K and 6.5 K with 10% and 5% F doping for LaOInF2 and LaOInCl2, respectively.

Contrasting Ultra-Low Frequency Raman and Infrared Modes in Emerging Metal Halides for Photovoltaics.

Lattice dynamics are critical to photovoltaic material performance, governing dynamic disorder, hot-carrier cooling, charge-carrier recombination, and transport. Soft metal-halide perovskites exhibit particularly intriguing dynamics, with Raman spectra exhibiting an unusually broad low-frequency response whose origin is still much debated. Here, we utilize ultra-low frequency Raman and infrared terahertz time-domain spectroscopies to provide a systematic examination of the vibrational response for a wide range of metal-halide semiconductors: FAPbI3, MAPbI x Br3-x , CsPbBr3, PbI2, Cs2AgBiBr6, Cu2AgBiI6, and AgI. We rule out extrinsic defects, octahedral tilting, cation lone pairs, and "liquid-like" Boson peaks as causes of the debated central Raman peak. Instead, we propose that the central Raman response results from an interplay of the significant broadening of Raman-active, low-energy phonon modes that are strongly amplified by a population component from Bose-Einstein statistics toward low frequency. These findings elucidate the complexities of light interactions with low-energy lattice vibrations in soft metal-halide semiconductors emerging for photovoltaic applications.

Vacuum structure of an eight-dimensional SU(3) gauge theory on a magnetized torus

We analyze the vacuum structure of an eight-dimensional non-Abelian gauge theory with a compactified four-dimensional torus as the extra dimensions. As a nontrivial background configuration of the gauge field of an SU(n) gauge group, we suppose a magnetic flux in two extra dimensions, and continuous Wilson line phases are also involved. We introduce matter fields and calculate the mass spectrum of low-energy modes appearing in a four-dimensional effective theory in an SU(3) model as an explicit example. As expected, potentially tachyonic states in four-dimensional modes appear from extra-dimensional gauge fields that couple to the flux background since the gauge group is simply connected. The Wilson line phases give a nonvanishing contribution to their masses, and we have a low-energy mass spectrum without tachyonic states, given that these phases take an appropriate value. To verify the validity of the values of the Wilson line phases, we examine the one-loop effective potential for these phases and explicitly show the contribution from each type of field present in our model. It is clarified that, although there seems to be no local minimum in the potential for the Wilson line phases in the pure Yang-Mills case, by including matter fields, we could find a vacuum configuration where tachyonic states disappear. Published by the American Physical Society 2024

Direct Observation and Analysis of Low-Energy Magnons with Raman Spectroscopy in Atomically Thin NiPS3.

van der Waals (vdW) magnets have rapidly emerged as a fertile playground for fundamental physics and exciting applications. Despite the impressive developments over the past few years, technical limitations pose a severe challenge to many other potential breakthroughs. High on the list is the lack of suitable experimental tools for studying spin dynamics on atomically thin samples. Here, Raman scattering techniques are employed to directly observe the low-lying magnon (∼1 meV) even in bilayer NiPS3. The advantage is that it offers excellent energy resolutions far better on low-energy sides than most inelastic neutron spectrometers can offer. More importantly, with appropriate theoretical analysis, the polarization dependence of the Raman scattering by those low-lying magnons also provides otherwise hidden information on the dominant spin-exchange scattering paths for different magnons. By comparing with high-resolution inelastic neutron scattering data, these low-energy Raman modes are confirmed to be indeed of magnon origin. Because of the different scattering mechanisms involved in inelastic neutron and Raman scattering, this information is fundamental in pinning down the final spin Hamiltonian. This work demonstrates the capability of Raman spectroscopy to probe the genuine two-dimensional spin dynamics in atomically thin vdW magnets, which can provide insights that are obscured in bulk spin dynamics.

New Lead-free Hybrid Layered Double Perovskite Halides: Synthesis, Structural Transition and Ultralow Thermal Conductivity.

Hybrid layered double perovskites (HLDPs), representing the two-dimensional manifestation of halide double perovskites, have elicited considerable interest owing to their intricate chemical bonding hierarchy and structural diversity. This intensified interest stems from the diverse options available for selecting alternating octahedral coordinated trivalent [M(III)] and monovalent metal centers [M(I)], along with the distinctive nature of the cationic organic amine located between the layers. Here, we have synthesized three new compounds with general formula (R'/R'')4/2M(III)M(I)Cl8; where R'=C3H7NH3 (i.e. 3N) and R''=NH3C4H8NH3 (i.e. 4N4); M(III)=In3+ or Ru3+; M(I)=Cu+ by simple solution-based acid precipitation method. The structural analysis reveals that (4N4)2CuInCl8 and (4N4)2CuRuCl8 adopt the layered Dion Jacobson (DJ) structure, whereas (3N)4CuInCl8 exhibits layered Ruddlesden Popper (RP) structure. The alternative octahedra within the inorganic layer display distortions and tilting. Three compounds show temperature-dependent structural phase transitions where changes in the staking of inorganic layer, extent of octahedral tilting and reorientation of organic spacers with temperature have been noticed. We have achieved ultralow lattice thermal conductivity (κL) in the HLDPs in the 2 to 300 K range, marking a distinctive feature within the realm of HLDP systems. The RP-HLDP compound, (3N)4CuInCl8, demonstrates anisotropy in κL while measured parallel and perpendicular to layer stacking, showcasing ultralow κL of 0.15 Wm-1K-1 at room temperature, which is one of the lowest values obtained among Pb-free metal halide perovskite. The observed ultralow κL in three new HLDPs is attributed to significant lattice anharmonicity arising from the chemical bonding heterogeneity and soft crystal structure, which resulted in low-energy localized optical phonon modes that suppress heat-carrying acoustic phonons.

Heart rate monitoring reveals differential seasonal energetic trade-offs in male noctule bats.

Understanding how animals meet their daily energy requirements is critical in our rapidly changing world. Small organisms with high metabolic rates can conserve stored energy when food availability is low or increase energy intake when energetic requirements are high, but how they balance this in the wild remains largely unknown. Using miniaturized heart rate transmitters, we continuously quantified energy expenditure, torpor use and foraging behaviour of free-ranging male bats (Nyctalus noctula) in spring and summer. In spring, bats used torpor extensively, characterized by lowered heart rates and consequently low energy expenditures. In contrast, in summer, bats consistently avoided torpor, even though they could have used this low-energy mode. As a consequence, daytime heart rates in summer were three times as high compared with the heart rates in spring. Daily energy use increased by 42% during summer, despite lower thermogenesis costs at higher ambient temperatures. Likely, as a consequence, bats nearly doubled their foraging duration. Overall, our results indicate that summer torpor avoidance, beneficial for sperm production and self-maintenance, comes with a high energetic cost. The ability to identify and monitor such vulnerable energetic life-history stages is particularly important to predict how species will deal with increasing temperatures and changes in their resource landscapes.

Improved bridge modal identification from vibration measurements using a hybrid empirical Fourier decomposition

Bridge health monitoring has been a prominent focus within the global engineering community. Bridge owners, stakeholders, and engineers face the formidable tasks of ensuring efficient monitoring, conducting reliable data analysis, interpreting data logically, and making timely decisions. With the increasing global infrastructure deficit, there is an ever-increasing need to develop reliable and economical bridge monitoring solutions. In this paper, a bridge condition assessment technique is proposed that can utilize the vibration data collected from the instrumented sensors and provide reliable system identification results. The proposed method develops a hybrid approach by integrating the Natural Excitation Technique (NExT) and Empirical Fourier Decomposition (EFD) to analyze ambient bridge vibration data and determine the modal parameters of the bridge. First, NExT is formulated to determine the cross-correlation functions of the bridge measurements, and then EFD is explored to decompose the signals into their monocomponents to identify the bridge modal parameters. The proposed methodology can overcome mode mixing and perform modal identification of a system with closely spaced frequencies and low energy modes. The estimated modal parameters such as bridge frequencies, mode shapes, and damping ratio are used for condition assessment of numerical, experimental and full-scale structures, including a short-span steel bridge located in Ontario, Canada. The results demonstrate that the proposed methodology can provide accurate and robust estimates of bridge modal parameters. Future research is reserved for real-time implementation of the proposed methodology for a wide range of civil structures.

Application of Funnel Metadynamics to the Platelet Integrin αIIbβ3 in Complex with an RGD Peptide.

Integrin αIIbβ3 mediates platelet aggregation by binding the Arginyl-Glycyl-Aspartic acid (RGD) sequence of fibrinogen. RGD binding occurs at a site topographically proximal to the αIIb and β3 subunits, promoting the conformational activation of the receptor from bent to extended states. While several experimental approaches have characterized RGD binding to αIIbβ3 integrin, applying computational methods has been significantly more challenging due to limited sampling and the need for a priori information regarding the interactions between the RGD peptide and integrin. In this study, we employed all-atom simulations using funnel metadynamics (FM) to evaluate the interactions of an RGD peptide with the αIIb and β3 subunits of integrin. FM incorporates an external history-dependent potential on selected degrees of freedom while applying a funnel-shaped restraint potential to limit RGD exploration of the unbound state. Furthermore, it does not require a priori information about the interactions, enhancing the sampling at a low computational cost. Our FM simulations reveal significant molecular changes in the β3 subunit of integrin upon RGD binding and provide a free-energy landscape with a low-energy binding mode surrounded by higher-energy prebinding states. The strong agreement between previous experimental and computational data and our results highlights the reliability of FM as a method for studying dynamic interactions of complex systems such as integrin.

Real-time scheduling for parallel tasks with resource reclamation

This paper considers the real-time scheduling of a parallel task with reclaiming computing resources, which can be utilized for soft real-time tasks or switching to low-energy mode to save energy. Existing works allocate a rectangular piece of computing resources based on the worst-case characterizations of the task to guarantee the deadline, which inherently incurs severe resource wasting due to coarse-grained resource allocation. To address this resource-wasting problem, this paper proposes the ladder-like resource allocation (i.e., a series of rectangular pieces of computing resources). To characterize the ladder-like resource allocation, we present two concepts called resource distribution and allocation vector, which serve as the interfaces between hard and soft real-time tasks. For the former, we derive schedulability tests under the given two interfaces; for the latter, we discuss the methods of determining the two interfaces to reclaim computing resources. This paper is the first work to fully explore the concept of ladder-like resource allocation and its potential consequences on computing resources, soft real-time tasks, and energy. Experiments demonstrate that the proposed approach can effectively reclaim more computing resources than existing approaches while maintaining hard real-time guarantees.

Polaronic Mass Enhancement and Polaronic Excitons in Metal Halide Perovskites.

In metal halide perovskites, the complex dielectric screening together with low energy of phonon modes leads to non-negligible Fröhlich coupling. While this feature of perovskites has already been used to explain some of the puzzling aspects of carrier transport in these materials, the possible impact of polaronic effects on the optical response, especially excitonic properties, is much less explored. Here, with the use of magneto-optical spectroscopy, we revealed the non-hydrogenic character of the excitons in metal halide perovskites, resulting from the pronounced Fröhlich coupling. Our results can be well described by the polaronic-exciton picture where electron and hole interactions are no longer described by a Coulomb potential. Furthermore, we show experimental evidence that the carrier-phonon interaction leads to the enhancement of the carrier's effective mass. Notably, our measurements reveal a pronounced temperature dependence of the carrier's effective mass, which we attribute to a band structure renormalization induced by the population of low-energy phonon modes. This interpretation finds support in our first-principles calculations.

Suppressed terahertz dynamics of water confined in nanometer gaps.

Nanoconfined waters exhibit low static permittivity mainly due to interfacial effects that span about one nanometer. The characteristic length scale may be much longer in the terahertz (THz) regime where long-range collective dynamics occur; however, the THz dynamics have been largely unexplored because of the lack of a robust platform. Here, we use metallic loop nanogaps to sharply enhance light-matter interactions and precisely measure real and imaginary THz refractive indices of nanoconfined water at gap widths ranging from 2 to 20 nanometers, spanning mostly interfacial waters all the way to quasi-bulk waters. We find that, in addition to the well-known interfacial effect, the confinement effect also contributes substantially to the decrease in the complex refractive indices of the nanoconfined water by cutting off low-energy vibrational modes, even at gap widths as large as 10 nanometers. Our findings provide valuable insights into the collective dynamics of water molecules which is crucial to understanding water-mediated processes.

Electrically tunable correlated domain wall network in twisted bilayer graphene

We investigate the domain wall network in twisted bilayer graphene (TBG) under the influence of interlayer bias and screening effect from the layered structure. Starting from the continuum model, we analyze the low-energy domain wall modes within the moiré bilayer structure and obtain an analytic form representing charge density distributions of the two-dimensional structure. By computing the screened electron–electron interaction strengths both within and between the domain walls, we develop a bosonized model that describes the correlated domain wall network. We demonstrate that these interaction strengths can be modified through an applied interlayer bias, screening length and dielectric materials, and show how the model can be employed to investigate various properties of the domain wall network and its stability. We compute correlation functions both without and with phonons. Including electron–phonon coupling in the network, we establish phase diagrams from these correlation functions. These diagrams illustrate electrical tunability of the network between various phases, such as density wave states and superconductivity. Our findings reveal the domain wall network as a promising platform for the experimental manipulation of electron–electron interactions in low dimensions and the study of strongly correlated matter. We point out that our investigation not only enhances the understanding of domain wall modes in TBG but also has broader implications for the development of moiré devices.

Electron mobility of SnO2 from first principles

The transparent conducting oxide SnO2 is a wide bandgap semiconductor that is easily n-type doped and widely used in various electronic and optoelectronic applications. Experimental reports of the electron mobility of this material vary widely depending on the growth conditions and doping concentrations. In this work, we calculate the electron mobility of SnO2 from first principles to examine the temperature and doping concentration dependence and to elucidate the scattering mechanisms that limit transport. We include both electron–phonon scattering and electron-ionized impurity scattering to accurately model scattering in a doped semiconductor. We find a strongly anisotropic mobility that favors transport in the direction parallel to the c-axis. At room temperature and intrinsic carrier concentrations, the low-energy polar-optical phonon modes dominate scattering, while ionized-impurity scattering dominates above 1018 cm−3.

Terahertz nanoscopy: Advances, challenges, and the road ahead

Exploring nanoscale material properties through light-matter interactions is essential to unveil new phenomena and manipulate materials at the atomic level, paving the way for ground-breaking advancements in nanotechnology and materials science. Various elementary excitations and low-energy modes of materials reside in the terahertz (THz) range of the electromagnetic spectrum (0.1–10 THz) and occur over various spatial and temporal scales. However, due to the diffraction limit, a slew of THz studies are restricted to drawing conclusions from the spatially varying THz responses around half of the probing wavelengths, i.e., from tens to a couple of hundred micrometers. To address this fundamental challenge, scanning near-field optical microscopy (SNOM), notably scattering-type SNOM (s-SNOM), combined with THz sources has been employed and is fueling growing interest in this technique across multiple disciplines. This review (1) provides an overview of the system developments of SNOM, (2) evaluates current approaches to understand and quantify light-matter interactions, (3) explores advances in THz SNOM applications, especially studies with THz nano-scale spatial responses employing an s-SNOM, and (4) envisions future challenges and potential development avenues for the practical use of THz s-SNOM.

Scaling Law for Kasha's Rule in Photoexcited Molecular Aggregates.

We study the photophysics of molecular aggregates from a quantum optics perspective, with emphasis on deriving scaling laws for the fast nonradiative relaxation of collective electronic excitations, referred to as Kasha's rule. Aggregates exhibit an energetically broad manifold of collective states with delocalized electronic excitations originating from near-field dipole-dipole exchanges between neighboring monomers. Photoexcitation at optical wavelengths, much larger than the monomer-monomer average separation, addresses almost exclusively symmetric collective states, which for an arrangement known as H-aggregate show an upward hypsochromic shift. The extremely fast subsequent nonradiative relaxation via intramolecular vibrational modes populates lower energy, subradiant states, resulting in effective inhibition of fluorescence. Our analytical treatment allows for the derivation of an approximate scaling law of this relaxation process, linear in the number of available low-energy vibrational modes and directly proportional to the dipole-dipole interaction strength between neighboring monomers.

Three-Fold Coordination of Copper in Sulfides: A Blockade for Hole Carrier Delocalization but a Driving Force for Ultralow Thermal Conductivity.

Copper-rich sulfides are very promising for energy conversion applications due to their environmental compatibility, cost effectiveness, and earth abundance. Based on a comparative analysis of the structural and transport properties of Cu3BiS3 with those of tetrahedrite (Cu12Sb4S13) and other Cu-rich sulfides, we highlight the role of the cationic coordination types and networks on the electrical and thermal properties. By precession-assisted 3D electron diffraction analysis, we find very high anisotropic thermal vibration of copper attributed to its 3-fold coordination, with an anisotropic atomic displacement parameter up to 0.09 Å2. Density functional theory calculations reveal that these Cu atoms are weakly bonded and give rise to low-energy Einstein-like vibrational modes that strongly scatter heat-carrying acoustic phonons, leading to ultralow thermal conductivity. Importantly, we demonstrate that the 3-fold coordination of copper in Cu3BiS3 and in other copper-rich sulfides constituted of interconnected CuS3 networks causes a hole blockade. This phenomenon hinders the possibility of optimizing the carrier concentration and electronic properties through mixed valency Cu+/Cu2+, differently from tetrahedrite and most other copper-rich chalcogenides, where the main interconnected Cu-S network is built of CuS4 tetrahedra. The comparison with various copper-rich sulfides demonstrates that seeking for frameworks characterized by the coexistence of tetrahedral and 3-fold coordinated copper is very attractive for the discovery of efficient thermoelectric copper-rich sulfides. Considering that lattice vibrations and carrier concentration are key factors for engineering transport phenomena (electronic, phonon, ionic, etc.) in copper-rich chalcogenides for various types of applications, our findings improve the guidelines for the design of materials enabling sustainable energy solutions with wide-ranging applications.

Features of cluster ion treatment of the surface of KGd(WO<sub>4</sub>)<sub>2</sub>:Nd single crystal

The features of the surface treatment of single crystals of potassium gadolinium tungstate doped with neodymium ions with low- and high-energy cluster argon ions are considered. Two radically different treatment modes were used: low-energy for more efficient surface smoothing and high-energy for more efficient target etching. Using atomic force microscopy, the topography of the target surface was analyzed before and after cluster ion treatment. Treatment in a low-energy mode was shown to smooth out irregularities on the target surface formed by chemical-mechanical polishing at an etching depth of less than 100 nm. The root-mean-square roughness and maximum height difference of the initial and treated surfaces of potassium gadolinium tungstate doped with neodymium ions were compared. Survey X-ray photoelectron spectra of the initial surface of a KGd(WO4)2:Nd single crystal and after the cluster ion treatment in different modes are presented. The intensities of the potassium and gadolinium peaks were shown to decrease after cluster ion treatment in both modes. A significant decrease in the concentration of potassium atoms in the subsurface layer of the target is explained by the predominant sputtering of potassium as a lighter chemical element. The mutual decrease in the concentrations of gadolinium and potassium atoms can be explained by the weak bonds of these atoms in the lattice of the KGd(WO4)2:Nd single crystal.

Dissipation-based proper orthogonal decomposition of turbulent Rayleigh–Bénard convection flow

We present a formulation of proper orthogonal decomposition (POD) producing a velocity–temperature basis optimized with respect to an H1 dissipation norm. This decomposition is applied, along with a conventional POD optimized with respect to an L2 energy norm, to a dataset generated from a direct numerical simulation of Rayleigh–Bénard convection in a cubic cell (Ra=107, Pr=0.707). The dataset is enriched using symmetries of the cell, and we formally link symmetrization to degeneracies and to the separation of the POD bases into subspaces with distinct symmetries. We compare the two decompositions, demonstrating that each of the 20 lowest dissipation modes is analogous to one of the 20 lowest energy modes. Reordering of modes between the decompositions is limited, although a corner mode known to be crucial for reorientations of the large-scale circulation is promoted in the dissipation decomposition, indicating suitability of the dissipation decomposition for capturing dynamically important structures. Dissipation modes are shown to exhibit enhanced activity in boundary layers. Reconstructing kinetic and thermal energy, viscous and thermal dissipation, and convective heat flux, we show that the dissipation decomposition improves overall convergence of each quantity in the boundary layer. Asymptotic convergence rates are nearly constant among the quantities reconstructed globally using the dissipation decomposition, indicating that a range of dynamically relevant scales is efficiently captured. We discuss the implications of the findings for using the dissipation decomposition in modeling and argue that the H1 norm allows for a better modal representation of the flow dynamics.