Particle Picture Research Articles

Aerosol fluidized bed coating: Exploring the impact of process conditions on process yield, coating coverage and thickness

Aerosol droplets are used to coat fluidized particles in this work. Coating experiments utilizing aerosol droplets (with a mean diameter of around 1μm) were performed under different process conditions to explore their impact on process yield, as well as on coating coverage. Core materials were glass and porous γ-Al2O3, which had mean diameters of 653μm and 610μm, respectively. Sodium benzoate (NaB) solution and silicon dioxide (SiO2) nanosuspension were used as the coating liquid. After sampling, particle pictures were taken by a scanning electron microscope and analyzed using image processing to determine the coating coverage. To simulate the coating process and determine, for each experiment, a factor for preferential deposition on already occupied positions, Monte Carlo simulations were used. Also, some particles were cut in the middle to measure coating layer thickness. Intraparticle coating thickness distribution from Monte Carlo simulations coarsely matches the measured thickness from cut particles. Results show that the process yield, coating coverage, and preference factor are affected by experimental conditions such as expanded bed height, fluidization air temperature, atomizing pressure, the number of aerosol inlets, as well as the surface potential of core particles. This study is first to examine the impact of surface charge of different core materials on droplet deposition. In an experiment with SiO2 nanosuspension, γ-Al2O3 cores could be coated quite uniformly with SiO2 nanoparticles with a layer thickness of ca. 1.1μm. This shows the potential of aerosol droplet deposition as a novel semi-wet method for coating large particles with nanoparticles without using any binders.

Tunable exciton valley-pseudospin orders in moiré superlattices.

Excitons in two-dimensional (2D) semiconductors have offered an attractive platform for optoelectronic and valleytronic devices. Further realizations of correlated phases of excitons promise device concepts not possible in the single particle picture. Here we report tunable exciton "spin" orders in WSe2/WS2 moiré superlattices. We find evidence of an in-plane (xy) order of exciton "spin"-here, valley pseudospin-around exciton filling vex = 1, which strongly suppresses the out-of-plane "spin" polarization. Upon increasing vex or applying a small magnetic field of ~10 mT, it transitions into an out-of-plane ferromagnetic (FM-z) spin order that spontaneously enhances the "spin" polarization, i.e., the circular helicity of emission light is higher than the excitation. The phase diagram is qualitatively captured by a spin-1/2 Bose-Hubbard model and is distinct from the fermion case. Our study paves the way for engineering exotic phases of matter from correlated spinor bosons, opening the door to a host of unconventional quantum devices.

On the particle picture of Emergence

The Emergence Proposal is the idea that all kinetic terms for fields in quantum gravity are emergent in the infrared from integrating out towers of states. It predicts that in a supersymmetric string theory context, the tree-level prepotential terms can be recovered precisely by integrating out a tower of non-perturbative states. In this note we present a new perspective, and associated quantitative evidence, for this proposal. We argue that the tree-level kinetic terms arise from integrating out the ultraviolet physics of each of the states in the tower. This ultraviolet physics is associated to extended objects, and cannot be captured by a standard particle Schwinger integral. Instead, we argue that it should be captured by a Schwinger-like integral where the proper time is analytically continued, and a contour is taken around the origin. This maps to certain integral representations for the moduli space periods, and indeed one recovers the tree-level prepotential exactly. This interpretation suggests that the ultraviolet physics which gives the leading contribution to the prepotential is localised on point intersections of the extended objects. We also argue that over special loci in moduli space there can exist a particle picture of the states, and an associated simple particle Schwinger integral, which leads to the full tree-level prepotential. These are loci with special degenerations, such as the singular limit of the resolved conifold.

Langevin picture of subdiffusive particles under the joint influence of an expanding medium and an external constant force

It has been found that expanding medium has a nonnegligible influence on particle’s diffusion, the physical mechanism of which is quite different from an external force field. To study the joint influence of the expanding medium and the constant force, we start from the Langevin picture of the subdiffusive particles in the expanding medium, and then introduce the effect of the external constant force in two ways, which are sustainedly or intermittently acting on the particle’s motion. Therefore, we get two models with the only difference on the force terms. Then under the framework of the Langevin equation, we conduct detailed analyses and derive the corresponding Fokker–Planck equations and the moments for the two models. In the case with the sustained constant force, the force behaves as a decoupled force, which is called Galilei invariant. While for the intermittent case, the force changes the diffusion behavior, and the specific effects vary according to the expanding rate of the medium. Our detailed theoretical analyses and simulations present a consistent Langevin framework of investigating anomalous diffusion phenomena in the expanding medium together with the external force.

Composition and mixing state of individual aerosol particles from northeast Greenland and Svalbard in the Arctic during spring 2018

The Arctic region is warming about four times faster than the rest of the globe, and thus it is important to understand the processes driving climate change in this region. Aerosols are a significant component of the Arctic climate system as they form ice crystals and liquid droplets that control the dynamics of clouds and also directly interact with solar radiation, depending on the compositions and mixing states of individual particles. Here, we report on the characteristics of submicron-sized aerosol particles using transmission electron microscopy obtained at two high Arctic sites, northeast Greenland (Villum Research Station) and Svalbard (Zeppelin Observatory), during spring 2018. The results showed that a dominant compound in the submicron-sized spring aerosols was sulfate, followed by sea salt particles. Both model simulations and observations at the Zeppelin Observatory showed that sea salt particles became more prevalent when low-pressure systems passed by the station. Model simulations indicate that both sampling sites were affected by diffused and diluted long-range transport of anthropogenic aerosols from lower latitudes with negligible influences of biomass burning emissions during the observation period. Overall, the composition of measured aerosol particles from the two Arctic sites was generally similar and showed no apparent variation except for the sea salt fractions. This study shows a general picture of high Arctic aerosol particles influenced by marine sources and diffused long-range transport of anthropogenic sources during the Arctic spring period. These results will contribute to a better knowledge of the aerosol composition and mixing state during the Arctic spring, which helps to understand the contributions of aerosols to the Arctic climate.

(Invited) Stochasticity in the Number of Quantum Defects in Fluorescent Carbon Nanotubes

Single wall carbon nanotubes (SWCNTs) display chirality dependent near infrared (NIR) fluorescence. Their optoelectronic properties can be further tuned by incorporating quantum defects/organic color centers (OCC) via reactions with diazonium salts. The absolute number of defects per SWCNT determines the properties but is not exactly known. Measuring it is complicated because typical SWCNT samples contain multiple chiralities, that congest the spectra and prevents to distinguish defects from different chiralities. Aqueous two-phase extraction (APTE) is a powerful technique to isolate specific chiralities. Here, we show that quantum defects do not affect APTE, which indicates that the chemical potential is not substantially affected and pinpoints to low numbers of defects. The purity of (6,5)-SWCNTs allows us to image the NIR fluorescence contributions (E11 below 1050 nm, and E11 * above 1050 nm) on the single SWCNT level and defect incorporation itself on the single molecule level. Interestingly, one observes a stochastic distribution of the numbers of defects, which can be explained by a Poisson distribution. We find a mean number of defects of 0-3 per SWCNT. These results indicate the large variance between ensemble and single particle picture. In summary, we show that single quantum defects can be counted by NIR imaging and that stochasticity plays a crucial role for their optical properties.

Emergence of a Bose polaron in a small ring threaded by the Aharonov-Bohm flux

The model of a ring threaded by the Aharonov-Bohm flux underlies our understanding of a coupling between gauge potentials and matter. The typical formulation of the model is based upon a single particle picture, and should be extended when interactions with other particles become relevant. Here, we illustrate such an extension for a particle in an Aharonov-Bohm ring subject to interactions with a weakly interacting Bose gas. We show that the ground state of the system can be described using the Bose-polaron concept—a particle dressed by interactions with a bosonic environment. We connect the energy spectrum to the effective mass of the polaron, and demonstrate how to change currents in the system by tuning boson-particle interactions. Our results suggest the Aharonov-Bohm ring as a platform for studying coherence and few- to many-body crossover of quasi-particles that arise from an impurity immersed in a medium.

Qubit picture of virtual particles

Qubit picture of virtual particles

Molecular Views on Fischer-Tropsch Synthesis.

For nearly a century, the Fischer-Tropsch (FT) reaction has been subject of intense debate. Various molecular views on the active sites and on the reaction mechanism have been presented for both Co- and Fe-based FT reactions. In the last 15 years, the emergence of a surface-science- and molecular-modeling-based bottom-up approach has brought this molecular picture a step closer. Theoretical models provided a structural picture of the Co catalyst particles. Recent surface science experiments and density functional theory (DFT) calculations highlighted the importance of realistic surface coverages, which can induce surface reconstruction and impact the stability of reaction intermediates. For Co-based FTS, detailed microkinetic simulations and mechanistic experiments are moving toward a consensus about the active sites and the reaction mechanism. The dynamic phase evolution of Fe-based catalysts under the reaction conditions complicates identification of the surface structure and the active sites. New techniques can help tackle the combinatorial complexity in these systems. Experimental and DFT studies have addressed the mechanism for Fe-based catalysts; the absence of a clear molecular picture of the active sites, however, limits the development of a molecular view of the mechanism. Finally, direct CO2 hydrogenation to long-chain hydrocarbons could present a sustainable pathway for FT synthesis.

Probing Rashba spin-orbit coupling by subcycle lightwave control of valley polarization

We perform nonperturbative calculations of light-field driven valley-polarization process in monolayer ${\mathrm{MoS}}_{2}$ which has additional Rashba spin-orbit couplings (SOCs). The ultrafast electron dynamics is simulated within the independent particle picture by solving density-matrix equations in the basis of linear combination of atomic orbitals, where tight-binding (TB) models including both intrinsic atomic and Rashba SOCs are used to calculate relevant matrix elements. We demonstrate that the Rashba-type SOCs can be manifested by suboptical-cycle control of valley selectivity excitations, in particular necessary via using few-cycle linearly polarized pulse with controlled carrier-envelope phase (CEP). This procedure will lead to a CEP-dependent valley Hall conductivity (VHC), which exhibits an important phase shift among different Rashba coupling strengths. The additional analysis shows that this phase shift is mainly determined by the ${d}_{z}^{2}$-orbital TB Rashba parameter from Mo atom and originates from contribution of conduction bands to VHC, where the Berry curvature modified by Rashba SOC plays a crucial role. Moreover, we also provide a qualitative interpretation on the Rashba-dependent VHC in terms of suboptical-cycle Landau-Zener-St\"uckelberg interference. Our results suggest a feasible approach for probing Rashba SOCs in hexagonal two-dimensional materials, and might pave the way of achieving more controls in the future valleytronics application.

Effect of four-phonon interaction on phonon thermal conductivity and mean-free-path spectrum of high-temperature phase SnSe

The phonon thermal conductivity and mean-free-path (MFP) spectrum of high-temperature phase SnSe (β-SnSe) are studied using the Boltzmann transport equation and ab initio approaches. The particle picture for phonon transport in β-SnSe is revisited, and the imaginary phonon frequencies caused by the ground-state within conventional density-functional theory are resolved. We show that between 800 and 950 K, the in-plane and cross-plane thermal conductivity has an average decrease of 38% and 19%, respectively, when four-phonon scatterings are considered. This large suppression of phonon transport stems mainly from the strong redistribution scattering process. With both the phonon and electron MFP spectra revealed, a characteristic length of 10 nm is suggested to reduce the in-plane and cross-plane thermal conductivity by 18% and 52%, respectively, via nanostructure engineering without sacrificing the power factor.

Reduced fluctuations for bosons in a double well

We review two recent results on the ground state properties of bosonic systems trapped by a double well external potential. In the limit of a large number of particles and large separation between the wells, we prove that fluctuations in the number of particles occupying each single-well low-energy mode occur at a reduced scale with respect to N, the latter being the typical prediction of the central limit theorem. This signals the breakdown of the independent and uncorrelated particle picture of standard Bose–Einstein condensation and the emergence of an interaction-driven correlated phase in the ground state.

Coherent polaron dynamics of electrons solvated in polar liquids.

An electron solvated in a polar liquid is an elementary quantum system with properties governed by electric interactions with a fluctuating molecular environment. In the prevailing single particle picture, the quantum ground and excited states are determined by a self-consistent potential, as defined by the particular local configuration of the solvation shell. This description neglects collective many-body excitations, which arise from the coupling of electronic degrees of freedom and nuclear motions of the environment. While recent experiments have demonstrated collective nonequilbrium electronic-nuclear motion, i.e. polaron excitations in liquid water, their relevance in the broader context of polar liquids has remained unexplored. Here, we study the nonequilibrium dielectric response of the, compared to water, less polar alcohols isopropanol, and ethylene glycol, that also display a different hydrogen bond pattern. We demonstrate that ultrafast relaxation of photogenerated electrons impulsively induces coherent charge oscillations, which persist for some 10ps. They emit electric waves in a frequency range from 0.1 to 2 THz, depending on electron concentration. Oscillation frequencies and line shapes are reproduced by a unified polaron picture for alcohols and water, which is based on a Clausius-Mossotti local field approach for the THz dielectric function. The analysis suggests a longitudinal character of many-body polaron excitations and a weak coupling to transverse excitations, supported by the underdamped character of charge oscillations. Polaron dynamics are governed by the long-range Coulomb interaction between an excess electron and several thousands of polar solvent molecules, while local electron solvation geometries play a minor role.

Correspondences of matter field fluctuations in semiclassical and classical gravity in the decoherence limit

Abstract A correspondence between fluctuations of non-minimally coupled scalar fields and that of an effective fluid with heat flux and anisotropic stresses, is shown. Though the correspondence between respective stress tensors of scalar fields and fluids is known and widely used in literature, the fluctuations in the two cases still await a formal correspondence and are open to investigation in all details. Using results obtained in the newly established theory of semiclassical stochastic gravity which focuses on the fluctuations of the quantum stress tensor, we show new relations in this regard. This development, apart from its relevance to the field-fluid correspondence, is expected to give insight to the mesoscopic phenomena for gravitating systems, and enable backreaction studies of the fluctuations on the perturbations of astrophysical objects. Such a development is aimed to enhance the perturbative analysis for cosmological spacetimes and astrophysical objects specifically in the decoherence limit. A kinetic theory, which can be based on stochastic fluctuations vs particle picture in curved spacetime may find useful insights from such correspondences in future work.

Charge Transport in Organic Semiconductors: The Perspective from Nonadiabatic Molecular Dynamics.

ConspectusOrganic semiconductors (OSs) are an exciting class of materials that have enabled disruptive technologies in this century including large-area electronics, flexible displays, and inexpensive solar cells. All of these technologies rely on the motion of electrical charges within the material and the diffusivity of these charges critically determines their performance. In this respect, it is remarkable that the nature of the charge transport in these materials has puzzled the community for so many years, even for apparently simple systems such as molecular single crystals: some experiments would better fit an interpretation in terms of a localized particle picture, akin to molecular or biological electron transfer, while others are in better agreement with a wave-like interpretation, more akin to band transport in metals.Exciting recent progress in the theory and simulation of charge carrier transport in OSs has now led to a unified understanding of these disparate findings, and this Account will review one of these tools developed in our laboratory in some detail: direct charge carrier propagation by quantum-classical nonadiabatic molecular dynamics. One finds that even in defect-free crystals the charge carrier can either localize on a single molecule or substantially delocalize over a large number of molecules depending on the relative strength of electronic couplings between the molecules, reorganization, or charge trapping energy of the molecule and thermal fluctuations of electronic couplings and site energies, also known as electron–phonon couplings.Our simulations predict that in molecular OSs exhibiting some of the highest measured charge mobilities to date, the charge carrier forms “flickering” polarons, objects that are delocalized over 10–20 molecules on average and that constantly change their shape and extension under the influence of thermal disorder. The flickering polarons propagate through the OS by short (≈10 fs long) bursts of the wave function that lead to an expansion of the polaron to about twice its size, resulting in spatial displacement, carrier diffusion, charge mobility, and electrical conductivity. Arguably best termed “transient delocalization”, this mechanistic scenario is very similar to the one assumed in transient localization theory and supports its assertions. We also review recent applications of our methodology to charge transport in disordered and nanocrystalline samples, which allows us to understand the influence of defects and grain boundaries on the charge propagation.Unfortunately, the energetically favorable packing structures of typical OSs, whether molecular or polymeric, places fundamental constraints on charge mobilities/electronic conductivity compared to inorganic semiconductors, which limits their range of applications. In this Account, we review the design rules that could pave the way for new very high-mobility OS materials and we argue that 2D covalent organic frameworks are one of the most promising candidates to satisfy them.We conclude that our nonadiabatic dynamics method is a powerful approach for predicting charge carrier transport in crystalline and disordered materials. We close with a brief outlook on extensions of the method to exciton transport, dissociation, and recombination. This will bring us a step closer to an understanding of the birth, survival, and annihiliation of charges at interfaces of optoelectronic devices.

Editorial

Editorial

Structure and magnetism of ultra-small cobalt particles assembled at titania surfaces by ion beam synthesis

Metallic cobalt nanoparticles offer attractive magnetic properties but are vulnerable to oxidation, which suppresses their magnetization. In this article, we report the use of ion beam synthesis to produce ultra-small, oxidation-resistant, cobalt nanoparticles embedded within substoichiometric TiO2-δ thin films. Using high fluence implantation of cobalt at 20–60 keV, the particles were assembled with an average size of 1.5 ± 1 nm. The geometry and structure of the nanoparticles were studied using scanning transmission electron microscopy. Near-edge X-ray fluorescence spectroscopy on the L2,3 Co edges confirms that the majority of the particles beneath the surface are metallic, unoxidised cobalt. Further evidence of the metallic nature of the small particles is provided via their high magnetization and superparamagnetic response between 3 and 300 K with a low blocking temperature of 4.5 K. The magnetic properties were studied using a combination of vibrating sample magnetometry, element-resolved X-ray magnetic circular dichroism, and depth-resolved polarised neutron reflectometry. These techniques provide a unified picture of the magnetic metallic Co particles. We argue, based on these experimental observations and thermodynamic calculations, that the cobalt is protected against oxidation beneath the surface of titania owing to the enthalpic stability of TiO2 over CoO which inhibits solid state reactions.

Mambillikalathil Govind Kumar Menon. 28 August 1928—22 November 2016

M. G. K. Menon, referred to as Goku, was an outstanding particle physicist and an extraordinary statesman of science. He made his major contributions to particle physics during the tortuous years of the unravelling of the full complexity of the families of elementary particles. It was an exciting but perplexing period, and the elucidation of the complexities of the world of elementary particles took the combined efforts of the experimentalists and the theorists. Goku's contributions were central to establishing what was eventually to become the standard picture of elementary particles. He will be remembered for his studies of the two- and three-body decay modes of the charged kaon that gave rise to the ‘τ–θ’ puzzle signalling non-conservation of parity. He coined the evocative phrase ‘associated production’ to describe the creation of kaons and hyperons together in high-energy interactions. He led a team that carried out experiments at great depths underground, and in 1965 they detected an event in which a cosmic-ray neutrino interacted with rock, producing an energetic muon. In the 1980s, with a large detector, also deployed underground, he set a lower bound on the lifetime for the decay of the proton. Menon was a great builder of academic and scientific institutions and a pre-eminent advocate for science. Accordingly, he stimulated and participated actively in building up the scientific and technological infrastructure in independent India, initially as the secretary of the Government of India and subsequently as the minister of state for science and technology. As the president of the International Council of Scientific Unions, he spearheaded its participation in the policymaking body of the United Nations. He was at various times the president of the three leading academies of sciences in India and a founding member and vice-president of the World Academy of Sciences. He was a gentle and loving family man and an energetic and engaged scientific colleague.

Absolutely Continuous Edge Spectrum of Hall Insulators on the Lattice

The presence of chiral modes on the edges of quantum Hall samples is essential to our understanding of the quantum Hall effect. In particular, these edge modes should support ballistic transport and therefore, in a single particle picture, be supported in the absolutely continuous spectrum of the single-particle Hamiltonian. We show in this note that if a free fermion system on the two-dimensional lattice is gapped in the bulk, and has a nonvanishing Hall conductance, then the same system put on a half-space geometry supports edge modes whose spectrum fills the entire bulk gap and is absolutely continuous.

Phonon wave-packet simulations using the quantized definition of energy and a temperature-dependent phonon dispersion relation and phonon density of states.

Wave-packet simulations, regarded as phonon dynamics in the literature, have been used to explore interface conductance problems and to study the frequency-based dynamics of systems of particles. In this work we introduce an extension of the method to improve the postsimulation analysis and to add an energy aspect to the definition of a wave packet. In a wave-packet simulation the most populated frequency activated with the wave packet is known through knowledge of the wave number implemented in the atom displacement equation. The one-to-one correspondence of wave number and frequency is known through the phonon dispersion relation (PDR). We add the temperature dependence of this one-to-one correspondence to the analysis of wave packets through consideration of a temperature-dependent PDR and showed the importance of the temperature-dependent PDR in the wave-packet definition by presenting results considering and neglecting the phenomenon. In addition, the temperature-dependent PDR and the density of states provide us the chance to change the nature of the atomic displacement amplitude as an arbitrary parameter to a tuning knob for the amount of energy it carries and utilize the chance to provide a quantitative measure for the validity of molecular-dynamics simulations considering their classical nature in comparison with the quantum particle picture of phonons.