Coulomb Coupling Research Articles

Magic-Angle Exciton Coupling in a Molecular Solid: Optical Consequence of Null-Coulombic Coupling.

Instances of magic angle excitonic coupling and its optical consequences are infrequently documented in the literature, yet they hold fundamental significance in understanding excited state electronic processes within molecular aggregates. Weak/null long-range dipolar Coulombic coupling is the characteristic of chromophore arrays positioned in a magic angle configuration. This study presents a rare example of such phenomena in CF3DPT solids, resulting in a high fluorescence quantum efficiency of 62 ± 3% in the aggregated solid state. Supported by computational calculations, we validate our experimental findings of null-Coulombic coupling and significant charge transfer (CT) coupling within the solid state.

Study the Characteristic of the Coupling Parameter ( ? ) in Dusty Plasma by Computer modeling

Computer modeling has been used to investing the Coulomb coupling parameter ?. The effects of the structure parameter K, grain charge Z, plasma density N, temperature dust grain Td, on the Coulomb coupling parameter had been studied. It was seen that the ? was increasing with increasing Z and N, and decrease with increasing K and T. Also the critical value of ? that the phase transfer of the plasma state from liquid to solid was studied.

Interplay of coulomb and exciton-phonon coupling controls singlet fission dynamics in two pentacene polymorphs.

Pentacene is an important model organic semiconductor in both the singlet exciton fission (SF) and organic electronics communities. We have investigated the effect of changing crystal structure on the SF process, generating multiple triplet excitons from an initial singlet exciton, and subsequent triplet recombination. Unlike for similar organic semiconductors that have strong SF sensitive to polymorphism, we find almost no quantitative difference between the kinetics of triplet pair (TT) formation in the two dominant polymorphs of pentacene. Both pairwise dimer coupling and momentum-space crystal models predict much faster TT formation from the bright singlet excited state of the Bulk vs ThinFilm polymorph, contrasting with the experiment. GW and Bethe-Salpeter equation calculations, including exciton-phonon coupling, reveal that ultrafast phonon-driven transitions in the ThinFilm polymorph compensate the intrinsically slower purely Coulomb-mediated TT formation channel, rationalizing the similarity in observed rates. Taking into account the influence of subtle structural distinctions on both the direct and phonon-mediated SF pathways reveals a predictive capability to these methods, expected to be applicable to a wide variety of molecular crystals.

A Simple Expression for the Screening of Excitonic Couplings between Chlorophylls as Inferred for Photosystem I Trimers.

The Coulomb coupling between transition densities of the pigments in photosynthetic pigment-protein complexes, termed excitonic coupling, is a key factor for the description of optical spectra and energy transfer. A challenging question is the quantification of the screening of the excitonic coupling by the optical polarizability of the environment. We use the equivalence between the sophisticated quantum chemical polarizable continuum (PCM) model and the simple electrostatic Poisson-TrEsp approach to analyze the distance and orientation dependence of the dielectric screening between chlorophylls in photosystem I trimers. On the basis of these calculations we find that the vacuum couplings Vmn(0) and the couplings in the dielectric medium Vmn=fmnVmn(0) are related by the empirical screening factor fmn=0.60+39.6θ(|κmn|-1.17)exp(-0.56Rmn/Å), where κmn is the usual orientational factor of the dipole-dipole coupling between the pigments, Rmn is the center-to-center distance, and the Heaviside-function θ(|κmn|-1.17) ensures that the exponential distance dependence only contributes for in-line type dipole geometries. We are confident that the present expression can be applied also to other pigment-protein complexes with chlorophyll or related pigments of similar shape. The variance between the Poisson-TrEsp and the approximate coupling values is found to decrease by a factor of 8 and 3-4 using the present expression, instead of an exponential distance dependent or constant screening factor, respectively, assumed previously in the literature.

Compressibility effects on Rayleigh-Taylor instability in magnetized strongly coupled dusty plasma

The compressibility effects have been studied on the internal wave modes and Rayleigh-Taylor (R-T) instability in a magnetized strongly coupled dusty plasma (SCDP). A dusty fluid model is constructed considering the effects of weakly coupled electrons/ions and strongly coupled dust grains under the influence of the gravitational field. The effects of the magnetic field and viscoelastic coefficients have been incorporated under the generalized hydrodynamic (GH) fluid description in a quasineutral dusty plasma. The dispersion relation of R-T instability is derived analytically and discussed in the strongly coupled limit. The compressibility effects have appeared in the internal wave modes, significantly modifying the R-T instability criterion and growth rates. The Coulomb coupling parameter and dust magnetosonic speed suppress the growth rate of the R-T instability in a compressible SCDP.

Bulk viscosity of the rigid rotor one-component plasma.

Bulk viscosity of a plasma consisting of strongly coupled diatomic ions is computed using molecular dynamics simulations. The simulations are based on the rigid rotor one-component plasma, which is introduced as a model system that adds two degrees of molecular rotation to the traditional one-component plasma. It is characterized by two parameters: the Coulomb coupling parameter, Γ, and the bond length parameter, Ω. Results show that the long-range nature of the Coulomb potential can lead to long rotational relaxation times, which in turn yield large values for bulk viscosity. The bulk-to-shear viscosity ratio is found to span from small to large values depending on the values of Γ and Ω. Although bulk viscosity is often neglected in plasma modeling, these results motivate that it can be large in molecular plasmas with rotational degrees of freedom.

Energy-Conserving Surface Hopping for Auger Processes.

Auger-type processes are ubiquitous in nanoscale materials because quantum confinement enhances Coulomb interactions, and there exist large densities of states. Modeling Auger processes requires the modification of nonadiabatic (NA) molecular dynamics algorithms to include transitions caused by both NA and Coulomb couplings. The system is split into quantum and classical subsystems, e.g., electrons and vibrations, and as a result, energy conservation becomes nontrivial. In surface hopping, an electronic transition induced by NA coupling is accompanied by a classical velocity readjustment to ensure conservation of the total quantum-classical energy. A different treatment is needed for Auger transitions driven by Coulomb interactions. We develop a nonadiabatic molecular dynamics methodology that meticulously differentiates the energy redistribution accompanying hops induced by the NA coupling and the Coulomb interaction and correctly conserves the total energy at each transition. If the transition is driven by a Coulomb interaction, the hop energy is redistributed within the quantum electronic subsystem only. If the transition is NA, the energy is redistributed between the quantum and classical subsystems. Properly maintaining energy conservation for both types of transitions is crucial to generate a correct order of events, obtain accurate transition times, maintain a proper statistical distribution of state populations, and reach thermodynamic equilibrium. We test the method with biexciton annihilation and Auger-assisted hot electron relaxation in a CdSe quantum dot. The sequence of Auger and phonon-driven processes and the calculated time scales are in excellent agreement with the experimental results. The developed approach can be coupled with any surface-hopping method and provides a crucial practical advance to study charge-carrier dynamics in the nanoscale and condensed matter systems.

Photoionization process of the hydrogenlike carbon ion embedded in warm and hot dense plasmas.

Complicated many-body interactions between ions and surrounding particles exist in warm and hot dense plasmas. It will significantly alter the atomic structures and dynamic properties of the embedded ions. Recently, the atomic-state-dependent (ASD) screening model has been proposed and shown to be valid for investigating the screening effect in warm and hot dense plasmas over a wide range of electron densities and temperatures. By employing the ASD model, we investigate the photoionization process for the hydrogenlike carbon ion embedded in warm and hot dense plasmas with corresponding Coulomb coupling parameter ranges of 0.05 ≤ Γ ≤ 1.16, where Γ characterizes the ratio of the average potential to thermal energy. It is found that there are stronger plasma screening effects on the ionization energy and photoionization cross section due to the negative-energy electron distributions considered in the ASD model compared to those considering only free electrons. The present results from the ASD model show reasonable agreement with the classical Debye-Hückel (DH) model in weakly coupled plasmas. However, significant deviations of the ionization energy and cross section between these two models are observed in moderately and strongly coupled plasmas, due to the approximate treatment of the plasma-electron density distribution of the DH model. In the region of low photoelectron energies, the positions of the shape resonance peaks of the cross sections obtained from the ASD model differ significantly from those of the DH model due to the different screening effects.

Tunable Photocarrier Dynamics in CuS Nanoflakes under Pressure Modulation.

Two-dimensional materials with a unique layered structure have attracted intense attention all around the world due to their extraordinary physical properties. Most importantly, the internal Coulomb coupling can be regulated, and thus electronic transition can be realized by manipulating the interlayer interaction effectively through adding external fields. At present, the properties of two-dimensional materials can be tuned through a variety of methods, such as adding pressure, strain, and electromagnetic fields. For optoelectronic applications, the lifetime of the photogenerated carriers is one of the most crucial parameters for the materials. Here, we demonstrate effective modulation of the optical band gap structure and photocarrier dynamics in CuS nanoflakes by applying hydrostatic pressure via a diamond anvil cell. The peak differential reflection signal shows a linear blueshift with the pressure, suggesting effective tuning of interlayer interaction inside CuS by pressure engineering. The results of transient absorption show that the photocarrier lifetime decreases significantly with pressure, suggesting that the dissociation process of the photogenerated carriers accelerates. It could be contributed to the phase transition or the decrease of the phonon vibration frequency caused by the pressure. Further, Raman spectra reveal the change of Cu-S and S-S bonds after adding pressure, indicating the possible occurrence of structural phase transition. Interestingly, all of the variation modes are reversible after releasing pressure. This work has provided an excellent sight to show the regulation of pressure on the photoelectric properties of CuS, exploring CuS to wider applications that can lead toward the realization of future excitonic and photoelectric devices modulated by high pressure.

Mean force emission theory for classical bremsstrahlung in strongly coupled plasmas

This work presents mean force emission theory, which extends the classical theory of bremsstrahlung emission to strongly coupled plasmas. In the high-frequency limit, the theory reduces to solving for the electron trajectory during a binary collision, but where the electron–ion interactions occur through the potential of mean force. In the low-frequency limit, it uses an autocorrelation formalism that captures effects of multiple collisions and strongly correlated motion. The predictions are benchmarked by comparison with first-principles classical molecular dynamics simulations of a fully ionized hydrogen plasma in which all interactions are repulsive. The comparison shows good agreement up to Coulomb coupling strengths of Γ∼30. The theory improves upon traditional models by including strong coupling effects and systematically including the effect of multiple collisions. Furthermore, mean force emission theory provides evidence that the Drude correction factor commonly used in quantum calculations of optical quantities may not be adequate at strong coupling.

Suppressing electron disorder-induced heating of ultracold neutral plasma via optical lattice

Disorder-induced heating (DIH) prevents ultracold neutral plasma into the electron strong coupling regime. Here, we propose a scheme to suppress electronic DIH via optical lattice. We simulate the evolution dynamics of ultracold neutral plasma constrained by three-dimensional optical lattice using the classical molecular dynamics method. The results show that for experimentally achievable conditions, electronic DIH is suppressed by a factor of 1.3, and the Coulomb coupling strength can reach 0.8, which is approaching the strong coupling regime. Suppressing electronic DIH via optical lattice may pave a way for the research of electronic strongly coupled plasma.

Phase separations of strongly coupled fine particles and fine particle mixtures in plasmas

AbstractPhase separations in strongly coupled fine particles in plasmas are discussed and two‐component mixtures are simulated by molecular dynamics with the background plasma being treated as continuum. The system size of laboratory experiments is assumed and separations into phases with a common electron density of the background plasma are analyzed. Since the charge on fine particles increases approximately in proportion to the size, we expect the larger component with stronger coupling condensates from the mixture. Results expressed in terms of strengths of Coulomb coupling and screening of the larger component seem to be mostly similar to the one‐component case, at least in cases where the ratio of fine particle sizes is 2, and the mixing ratio is in the range from 0.25 to 0.75.

Analysis of Interference Effect in Double Optomechanically Induced Transparency System

We propose a scheme to investigate the interference properties of a double optomechanically induced transparency system, which involves two charged nanomechanical resonators, coupled via Coulomb interaction. The results show that the opening of transparency windows is caused by a destructive interference effect only in the weak optical coupling region. For strong optical coupling, normal mode splitting dominates the transparency phenomenon. In the intermediate region, both destructive interference and normal mode splitting contribute to the transparency windows. When the Coulomb coupling is much weaker than the optical coupling, the Coulomb interaction strength linearly determines the distance between the two transparency windows, and has nearly no influence on the destructive interference effect. Otherwise, the system will work in a nonlinear region.

Optomechanically induced transparency in a hybrid system containing two-level atomic ensemble and optical parametric amplifier

We investigate the physical properties of multiple optomechanically induced transparency in a system. The system consists of two charged mechanical resonators and an optical cavity. An optical parametric amplifier (OPA) and a two-level atom ensemble are filled into the optical cavity. Some physical phenomena appear in the system driven by the probe field and the pump field. The width of transparent windows can be manipulated by the coupling strengths of the system. Specifically, the width of the transparency window increases with an increase in the parametric gain of the optical parametric amplifier (OPA). Furthermore, the number of transparent windows and the location of transparent points are also affected by the system parameters. The presence of two-level atomic ensemble causes the double transparent windows to be split three transparent windows. The Coulomb coupling between the two charged mechanical resonators causes the transparent points to move. Our approach provides a great flexibility for manipulating multiple induced transparency. It is helpful to study the quantum properties of nonlinear optical systems.

When should PIC simulations be applied to atmospheric pressure plasmas? Impact of correlation heating

Molecular dynamics simulations are used to test when the particle-in-cell (PIC) method applies to atmospheric pressure plasmas. It is found that PIC applies only when the plasma density and macroparticle weight are sufficiently small because of two effects associated with correlation heating. The first is the physical effect of disorder-induced heating (DIH). This occurs if the plasma density is large enough that a species (typically ions) is strongly correlated in the sense that the Coulomb coupling parameter exceeds one. In this situation, DIH causes ions to rapidly heat following ionization. PIC is not well suited to capture DIH because doing so requires using a macroparticle weight of one and a grid that well resolves the physical interparticle spacing. These criteria render PIC intractable for macroscale domains. The second effect is a numerical error due to artificial correlation heating (ACH). ACH is like DIH in that it is caused by the Coulomb repulsion between particles, but differs in that it is a numerical effect caused by a macroparticle weight larger than one. Like DIH, it is associated with strong correlations. However, here the macroparticle coupling strength is found to scale as Γw2/3 , where Γ is the physical coupling strength and w is the macroparticle weight. So even if the physical coupling strength of a species is small, as is expected for electrons in atmospheric pressure plasmas, a sufficiently large macroparticle weight can cause the macroparticles to be strongly coupled and therefore heat due to ACH. Furthermore, it is shown that simulations in reduced dimensions exacerbate these issues.

New Theoretical Model to Describe Carrier Multiplication in Semiconductors: Explanation of Disparate Efficiency in MoTe2 versus PbS and PbSe.

We present a theoretical model to compute the efficiency of the generation of two or more electron-hole pairs in a semiconductor by the absorption of one photon via the process of carrier multiplication (CM). The photogeneration quantum yield of electron-hole pairs is calculated from the number of possible CM decay pathways of the electron and the hole. We apply our model to investigate the underlying cause of the high efficiency of CM in bulk 2H-MoTe2, as compared to bulk PbS and PbSe. Electronic band structures were calculated with density functional theory, from which the number of possible CM decay pathways was calculated for all initial electron and hole states that can be produced at a given photon energy. The variation of the number of CM pathways with photon energy reflects the dependence of experimental CM quantum yields on the photon energy and material composition. We quantitatively reproduce experimental CM quantum yields for MoTe2, PbS, and PbSe from the calculated number of CM pathways and one adjustable fit parameter. This parameter is related to the ratio of Coulomb coupling matrix elements and the cooling rate of the electrons and holes. Large variations of this fit parameter result in small changes in the modeled quantum yield for MoTe2, which confirms that its high CM efficiency can be mainly attributed to its extraordinary large number of CM pathways. The methodology of this work can be applied to analyze or predict the CM efficiency of other materials.

Block-matching and 3D filtering-based denoising of acoustic images obtained through point contact excitation and detection method

A novel experimental method based on the Coulomb coupling technique is used for visualizing the interaction of ultrasonic waves in PZT (Lead Zirconate Titanate - (Pb[ZrxTi1-x]O3 (0 ≤ x ≤ 1)) ceramic materials. The method of excitation and detection through a point contact produces representations of propagating wave vectors in the time domain as a series of images. In the acoustic image, several types of noises from different types of sources corrupt the signal as well as the image. As a result, the resolution and quality of the images are reduced. Block matching and 3D filtering (BM3D) algorithm is implemented for the reduction of noises from ultrasonic signals that are in the form of 2D images. Here, we also implemented a custom-designed hybrid filter and conventional total variation (TV-L1) filter on the noisy images to compare the final denoised outputs from the BM3D filter. Comparison metrics like PSNR (peak signal-to-noise ratio) and SSIM (structural similarity index measure) are used for quantitative analysis of those denoised ultrasonic images with respect to their ground truth or almost noise-free counterparts. Based upon those parameter values, the BM3D filter demonstrated the best results for the denoising of the acoustic images acquired from the sample PZT material. This paper discusses and explains the results and proves the successful application of the BM3D algorithm on acoustic image data.

Non-adiabatic molecular dynamics simulations provide new insights into the exciton transfer in the Fenna-Matthews-Olson complex.

A trajectory surface hopping approach, which uses machine learning to speed up the most time-consuming steps, has been adopted to investigate the exciton transfer in light-harvesting systems. The present neural networks achieve high accuracy in predicting both Coulomb couplings and excitation energies. The latter are predicted taking into account the environment of the pigments. Direct simulation of exciton dynamics through light-harvesting complexes on significant time scales is usually challenging due to the coupled motion of nuclear and electronic degrees of freedom in these rather large systems containing several relatively large pigments. In the present approach, however, we are able to evaluate a statistically significant number of non-adiabatic molecular dynamics trajectories with respect to exciton delocalization and exciton paths. The formalism is applied to the Fenna-Matthews-Olson complex of green sulfur bacteria, which transfers energy from the light-harvesting chlorosome to the reaction center with astonishing efficiency. The system has been studied experimentally and theoretically for decades. In total, we were able to simulate non-adiabatically more than 30 ns, sampling also the relevant space of parameters within their uncertainty. Our simulations show that the driving force supplied by the energy landscape resulting from electrostatic tuning is sufficient to funnel the energy towards site 3, from where it can be transferred to the reaction center. However, the high efficiency of transfer within a picosecond timescale can be attributed to the rather unusual properties of the BChl a molecules, resulting in very low inner and outer-sphere reorganization energies, not matched by any other organic molecule, e.g., used in organic electronics. A comparison with electron and exciton transfer in organic materials is particularly illuminating, suggesting a mechanism to explain the comparably high transfer efficiency.

Effects of disorder on electron heating in ultracold plasmas

Starting from the beginning of their research in the early 2000s, the ultracold plasmas were considered as a promising tool to achieve considerable values of the Coulomb coupling parameter for electrons. Unfortunately, this was found to be precluded by a sharp spontaneous increase in temperature, which was often attributed to the so-called disorder-induced heating. It is the aim of the present paper to quantify the effect of spontaneous heating as a function of the initial ionic disorder and, thereby, to estimate the efficiency of its mitigation, e.g., by the Rydberg blockade. As a result of the performed simulations, we found that the dynamics of electrons exhibited a well-expressed transition from the case of the quasi-regular arrangement of ions to the disordered one; the magnitude of the effect being about 30%. Thereby, we can conclude that the two-step formation of ultracold plasmas—involving the intermediate stage of the blockaded Rydberg gas—can really serve as a tool to increase the degree of Coulomb coupling, but the efficiency of this method is moderate.

Quantum dense coding and teleportation based on two coupled quantum dot molecules influenced by intrinsic decoherence, tunneling rates, and Coulomb coupling interaction

Quantum dense coding and teleportation based on two coupled quantum dot molecules influenced by intrinsic decoherence, tunneling rates, and Coulomb coupling interaction