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A two-dimensional particle-in-cell code for simulation of low-frequency electromagnetic processes in laboratory plasmas has been developed. The code uses the Darwin method omitting the electromagnetic wave propagation. The Darwin method separates the electric field into solenoidal and irrotational parts. The irrotational electric field is the electrostatic field calculated with the direct implicit algorithm. The solenoidal electric field is calculated with a new algorithm based on the equation for the electric field vorticity. The new algorithm is faster and more reliable than the Streamlined Darwin Field Formulation introduced decades ago. The system of linear equations in the new algorithm is solved using a standard iterative method. The code is applied to simulate an inductively coupled plasma with the driving current flowing around the plasma region.

The effect of a uniform magnetic field on particle transport in low-pressure radio frequency (RF) capacitively coupled plasma (CCP) has been studied using a particle-in-cell (PIC) model. Three distinct regimes of plasma behavior can be identified as a function of the magnetic field. In the first regime at low magnetic fields, asymmetric plasma profiles are observed within the CCP chamber due to the effect of E x B drift. As the magnetic field increases, instabilities develop and form self-organized spoke-shaped structures that are distinctly seen within the bulk plasma closer to the sheath. In this second regime, the spoke-shaped coherent structures rotate inside the plasma chamber in the - E x B direction, where E and B are the DC electric and magnetic field vectors, respectively, and the DC electric field exists in the sheath and pre-sheath regions. The spoke rotation frequency is in the MHz range. As the magnetic field strength increases further, the rotating coherent spokes continue to exist near the sheath. The coherent structures are, however, accompanied by new small-scale incoherent structures originating and moving within the bulk plasma region away from the sheath. This is the third regime of plasma behavior. The threshold values of the magnetic field between these regimes were found not to vary with changing plasma reactor geometry (e.g., area ratio between ground and powered electrodes) or the use of an external capacitor between the RF-powered electrode and the RF source. The threshold values of the magnetic field between these regimes shift toward higher values with increasing gas pressure. This paper provides guidance on the upper limit of the magnetic field for instability-free operation in low-pressure CCP-based semiconductor deposition and etch systems that use the external magnetic field for plasma uniformity control., Comment: Submitted for Review to Physics of Plasmas

Methods of computational quantum chemistry provide accurate approximations of molecular properties crucial for computer-aided drug discovery and other areas of chemical science. However, high computational complexity limits the scalability of their applications. Neural network potentials (NNPs) are a promising alternative to quantum chemistry methods, but they require large and diverse datasets for training. This work presents a new dataset and benchmark called $\nabla^2$DFT that is based on the nablaDFT. It contains twice as much molecular structures, three times more conformations, new data types and tasks, and state-of-the-art models. The dataset includes energies, forces, 17 molecular properties, Hamiltonian and overlap matrices, and a wavefunction object. All calculations were performed at the DFT level ($\omega$B97X-D/def2-SVP) for each conformation. Moreover, $\nabla^2$DFT is the first dataset that contains relaxation trajectories for a substantial number of drug-like molecules. We also introduce a novel benchmark for evaluating NNPs in molecular property prediction, Hamiltonian prediction, and conformational optimization tasks. Finally, we propose an extendable framework for training NNPs and implement 10 models within it.

In this study, we conduct 2D3V Particle-In-Cell simulations of hollow cathodes, encompassing both the channel and plume region, with an emphasis on plasma switch applications. The plasma in the hollow cathode channel can exhibit kinetic effects depending on how fast electrons emitted from the insert are thermalized via Coulomb collisions. The criterion that determines whether the plasma operates in a Duid or kinetic regime is given as follows. When Coulomb collisions occur at a much greater rate than ionization or excitation events, the Electron Energy Distribution Function relaxes to aMaxwellian distribution and the plasmawithin the channel can be describedwith aDuidmodel. In contrast, if inelastic processes are much faster, then the Electron Energy Distribution Function in the channel exhibits a notable high-energy tail, and a kinetic treatment is required. This criterion is applied to other kinds of hollow cathodes from the literature, revealing that a Duid approach is suitable for most electric propulsion applications, whereas a kinetic treatment might be necessary for plasma switches. Additionally, amomentumbalance reveals that a diffusion equation is sufAcient to predict the plasma plume expansion, a crucial input in the design of hollow cathodes for plasma switch applications.

A physical and numerical model of the Townsend discharge in molecular hydrogen and deuterium has been developed to meet the needs of designing a plasma-based switching device for power grid application. The model allows to predict the low-pressure branch of the Paschen curve for applied voltage in the range of several hundred kiloVolts. In the regime of interest, electrons are in a runaway state and ionization by ions and fast neutrals sustains the discharge. It was essential to correctly account for both gas-phase and surface interactions (electron emission and electron back-scattering), especially in terms of their dependence on particle energy. The model yields results consistent with prior data obtained for lower voltage. The three-species (electrons, ions and fast neutrals) model successfully captures the essential physics of the process., Comment: 21 pages, 13 figures

The process of numerical thermalization in particle-in-cell (PIC) simulations has been studied extensively. It is analogous to Coulomb collisions in real plasmas, causing particle velocity distributions (VDFs) to evolve towards a Maxwellian as macroparticles experience polarization drag and resonantly interact with the fluctuation spectrum. This paper presents a practical tutorial on the effects of numerical thermalization in 2D PIC applications. Scenarios of interest include simulations which must be run for many thousands of plasma periods and contain a population of cold electrons that leave the simulation space very slowly. This is particularly relevant to many low temperature plasma discharges and materials processing applications. We present numerical drag and diffusion coefficients and their associated timescales for a variety of grid resolutions, discussing the circumstances under which the electron VDF is modified by numerical thermalization. Though the effects described here have been known for many decades, direct comparison of analytically derived, velocity-dependent numerical relaxation timescales to those of other relevant processes has not often been applied in practice due to complications that arise in calculating thermalization rates in 1D simulations. Using these comparisons, we estimate the impact of numerical thermalization in several example low temperature plasma applications including capacitively coupled plasma (CCP) discharges, inductively coupled plasma (ICP) discharges, beam plasmas, and hollow cathode discharges. Finally, we discuss possible strategies for mitigating numerical relaxation effects in 2D PIC simulations.

Molecular conformation optimization is crucial to computer-aided drug discovery and materials design. Traditional energy minimization techniques rely on iterative optimization methods that use molecular forces calculated by a physical simulator (oracle) as anti-gradients. However, this is a computationally expensive approach that requires many interactions with a physical simulator. One way to accelerate this procedure is to replace the physical simulator with a neural network. Despite recent progress in neural networks for molecular conformation energy prediction, such models are prone to distribution shift, leading to inaccurate energy minimization. We find that the quality of energy minimization with neural networks can be improved by providing optimization trajectories as additional training data. Still, it takes around $5 \times 10^5$ additional conformations to match the physical simulator's optimization quality. In this work, we present the Gradual Optimization Learning Framework (GOLF) for energy minimization with neural networks that significantly reduces the required additional data. The framework consists of an efficient data-collecting scheme and an external optimizer. The external optimizer utilizes gradients from the energy prediction model to generate optimization trajectories, and the data-collecting scheme selects additional training data to be processed by the physical simulator. Our results demonstrate that the neural network trained with GOLF performs on par with the oracle on a benchmark of diverse drug-like molecules using $50$x less additional data., Comment: Published as a conference paper at ICLR2024 (Poster)

The effect of driving frequency in the range of 13.56 MHz to 73 MHz on electron energy distribution and electron heating modes in a 50 mTorr capacitively coupled argon plasma discharge is studied using 1D-3V particle-in-cell simulations. Calculated electron energy probability functions exhibit three distinct ``temperatures'' for low-, mid-, and high-energy electrons. When compared to published experimental data, the calculated probability functions show a reasonable agreement for the energy range resolved in the measurements (about 2 eV to 10 eV). Discrepancies outside this range lead to differences between computational and experimental values of the electron number density determined from the distribution functions, but the predicted effective electron temperature is within 25\% of experimental values. The impedance of the discharge is interpreted in terms of a homogeneous equivalent circuit model and the driving frequency dependence of the inferred combined sheath thickness is found to obey a known, theoretically-derived, power law. The average power transferred from the field to the electrons (electron heating) is computed, and a region of negative heating near the sheath edge, particularly at higher driving frequencies, is identified. Analysis of the electron momentum equation shows that electron inertia, which would average to zero in a linear regime, is responsible for negative values of power deposition near the sheath edge at high driving frequencies due to the highly nonlinear behavior of the discharge., Comment: 18 pages, 20 figures, 57 references

Achieving large-scale kinetic modelling is a crucial task for the development and optimization of modern plasma devices. With the trend of decreasing pressure in applications such as plasma etching, kinetic simulations are necessary to self-consistently capture the particle dynamics. The standard, explicit, electrostatic, momentum-conserving Particle-In-Cell method suffers from restrictive stability constraints on spatial cell size and temporal time step, requiring resolution of the electron Debye length and electron plasma period respectively. This results in a very high computational cost, making the technique prohibitive for large volume device modeling. We investigate the Direct Implicit algorithm and the explicit Energy Conserving algorithm as alternatives to the standard approach, both of which can reduce computational cost with a minimal (or controllable) impact on results. These algorithms are implemented into the well-tested EDIPIC-2D and LTP-PIC codes, and their performance is evaluated via 2D capacitively coupled plasma discharge simulations. The investigation revels that both approaches enable the utilization of cell sizes larger than the Debye length, resulting in reduced runtime, while incurring only minor inaccuracies in plasma parameters. The Direct Implicit method also allows for time steps larger than the electron plasma period, however care must be taken to avoid numerical heating or cooling. It is demonstrated that by appropriately adjusting the ratio of cell size to time step, it is possible to mitigate this effect to an acceptable level.

Low-pressure multi-frequency capacitively coupled plasmas are used for numerous etch and deposition applications in the semiconductor industry. Pulsing of the radio-frequency (RF) sources enables control of neutral and charged species in the plasma on a millisecond timescale. The synchronous (i.e., simultaneous, in-phase) pulsing of both power sources in a dual frequency capacitively coupled plasma is examined in this article. Due to the low gas pressure, modeling has been done using the electrostatic Particle-in-cell/Monte Carlo collision method. The objective of this work is to investigate the sensitivity of the plasma properties to small changes in timing during synchronous pulsing of the 2 RF sources. It is demonstrated that small deviations in the on and off times of the 2 RF sources can lead to major changes in the plasma characteristics. This high sensitivity is of concern for process repeatability but can be utilized to enable better control of the dynamics of plasma-surface interaction. In the simulations, the pulsing parameters (on and off times and ramp rates) are varied and the temporal evolution of plasma characteristics such as electron density (ne), species current at the electrode, and electron temperature are examined. It is demonstrated that if the low-frequency (LF) source is turned off a few {\mu}s before (or after) the high-frequency source, ne during the off-state is significantly higher (or lower) due to the frequency coupling effect. Similarly, turning on the LF source with a small delay results in a sharp increase in the plasma density when the RF sources are turned on., Comment: 19 pages, 17 figures

Plasmas generated using energetic electron beams are well known for their low electron temperature ($T_{e}$) and plasma potential, which makes them attractive for atomic-precision plasma processing applications such as atomic layer etch and deposition. A 2d3v particle-in-cell (PIC) model for an electron beam-generated plasma in argon confined by a constant applied magnetic field is described in this article. Plasma production primarily occurs in the path of the beam electrons in the center of the chamber. The resulting plasma spreads out in the chamber through non-ambipolar diffusion with a short-circuit effect allowing unequal electron and ion fluxes to different regions of the bounding conductive chamber walls. The cross-field transport of the electrons (and thus the steady-state characteristics of the plasma) are strongly impacted by the magnetic field. $T_{e}$ is anisotropic in the electron beam region, but low and isotropic away from the plasma production zone. The plasma density increases, and the plasma becomes more confined near the region of production when the magnetic field strengthens. The magnetic field reduces both electron physical and energy transport perpendicular to the magnetic field. $T_{e}$ is uniform along the magnetic field lines and slowly decreases perpendicular to it. Electrons are less energetic in the sheath regions where the sheath electric field repels and confines the low-energy electrons from the bulk plasma. Even though electron and ion densities are similar in the bulk plasma due to quasi-neutrality, electron and ion fluxes on the grounded chamber walls are unequal at most locations. Electron confinement by the magnetic field weakens with increasing pressure, and the plasma spreads out farther from the electron beam region., Comment: 19 pages and 12 figures on additional 12 pages Submitted to Plasma Sources Science and Technology

We study electron heating in collisionless current-driven turbulence due to the nonlinear interactions between electron- and ion-acoustic waves. PIC simulation results show that due to a large difference between the electron and ion mean velocities the Buneman instability excites large-amplitude ion-acoustic waves, which strongly modifies the electron velocity distribution function, leading to a secondary instability that generates fast electron-acoustic waves; and in this process, a giant electron hole is ultimately created. This giant electron hole is responsible for strong electron heating due to phase mixing. The numerical simulation results are consistent with the previous observations and provide insight into the key processes responsible for electron heating and the generation of nonlinear waves in a collisionless current-driven instability.

With the growing availability of data within various scientific domains, generative models hold enormous potential to accelerate scientific discovery. They harness powerful representations learned from datasets to speed up the formulation of novel hypotheses with the potential to impact material discovery broadly. We present the Generative Toolkit for Scientific Discovery (GT4SD). This extensible open-source library enables scientists, developers, and researchers to train and use state-of-the-art generative models to accelerate scientific discovery focused on material design., Comment: 15 pages, 2 figures

Recently, S Patil et al. have reported the existence of an enhanced operating regime when a low-pressure (5 mTorr) capacitively coupled discharge (CCP) is driven by a very high radio-frequency (60 MHz) source in the presence of a weak external magnetic field applied parallel to its electrodes. Their Particle-in-Cell (PIC) simulations show, that a significantly higher bulk plasma density and ion flux can be achieved at the electrode when the electron cyclotron frequency equals half of the applied RF frequency for a given fixed voltage. In the present work we take a detailed look at this phenomenon and further delineate the effect of this "electron bounce cyclotron resonance (EBCR)" on the electron and ion dynamics of the system. We find that the ionization collision rate and stochastic heating is maximum under resonance condition. The electron energy distribution function also indicates that the population of tail end electrons is highest for the case where EBCR is maximum. Formation of electric field transients in the bulk plasma region are also seen at lower values of applied magnetic field. Finally, we demonstrate that the EBCR induced effect is a low pressure phenomenon and weakens as the neutral gas pressure increases. The potential utility of this effect to advance the operational performance of CCP devices for industrial purposes is discussed., Comment: 34 pages, 13 figures

We study collective processes for an electron beam propagating through a background plasma using simulations and analytical theory. A new regime where the instability of a Langmuir wave packet can grow locally much faster than ion frequency is clearly identified. The key feature of this new regime is an Electron Modulational Instability that rapidly creates a local Langmuir wave packet, which in its turn produces local charge separation and strong ion density perturbations because of the action of the ponderomotive force, such that the beam-plasma wave interaction stops being resonant. Three evolution stages of the process and observed periodic burst features are discussed. Different physical regimes in the plasma and beam parameter space are demonstrated for the first time., Comment: 20 pages, 3 figures

Electron-beam plasma interaction has long been a topic of great interest. Despite the success of Quasi-Linear (QL) theory and Weak Turbulence (WT) theory, their validities are limited by the requirement of sufficiently dense mode spectrum and small wave amplitude. In this paper, we extensively studied the collective processes of a mono-energetic electron beam emitted from a thermionic cathode propagating through a cold plasma by performing a large number of high resolution two-dimensional (2D) particle-in-cell (PIC) simulations and using analytical theories. We confirm that the initial stage of two-stream instability is saturated due to well-known wave-trapping mechanism. Further evolution occurs due to strong wave-wave nonlinear processes. We show that the beam-plasma interaction can be classified into four different physical regimes in the parameter space for the plasma and beam parameters. The differences between the different regimes are analyzed in detail. For the first time, we identified a new regime in strong Langmuir turbulence featured by what we call Electron Modulational Instability (EMI) that could create a local Langmuir wave packet growing faster than the ion plasma frequency. Ions do not have time to respond to EMI in the initial growing stage. On a longer timescale, the action of the ponderomotive force produces very strong ion density perturbations, and eventually the beam-plasma wave interaction stops being resonant due to strong ion density perturbations. Consequently, in this EMI regime, electron beam-plasma interaction occurs in a periodic (intermittent) process. The beams are strongly scattered by waves, and the Langmuir wave spectrum is significantly broadened, which in turn gives rise to strong heating of bulk electrons. A resulting kappa distribution and a wave-energy spectrum, E^2 (k)~k^(-5), are observed in the strong turbulent regime., Comment: 71 pages, 20 figures

We study, by numerical and analytical means, the evolution of a uniform one-dimensional collisionless plasma initiated between plane absorbing walls. The ensuing flow is described by rarefaction waves that propagate symmetrically inward from the boundaries, interact, and eventually vanish after crossing through, leading up to the asymptotic phase., Comment: Submitted to journal

This paper provides perspectives on recent progress in the understanding of the physics of devices where the external magnetic field is applied perpendicularly to the discharge current. This configuration generates a strong electric field, which acts to accelerates ions. The many applications of this set up include generation of thrust for spacecraft propulsion and the separation of species in plasma mass separation devices. These ExB plasmas are subject to plasma-wall interaction effects as well as various micro and macro instabilities, and in many devices, we observe the emergence of anomalous transport. This perspective presents the current understanding of the physics of these phenomena, state-of-the-art computational results, identifies critical questions, and suggests directions for future research, Comment: 59 pages, 25 Figures, submitted to Physics of Plasmas

We study formation of the Vibrational Distribution Function (VDF) in a molecular gas at low pressure, when vibrational levels are excited by electron impact and deactivated in collisions with walls and show that this problem has a convenient analytical solution that can be used to obtain VDF and its dependence on external parameters. The VDF is determined by excitation of vibrational levels by an external source and deactivation in collisions with the wall. Deactivation in wall collisions is little known process. However, we found that the VDF is weakly dependent on the functional form of the actual form of probability gamma_v'->v for a vibrational number v' to transfer into a lower level v at the wall. Because for a given excitation source of vibrational states, the problem is linear the solution for VDF involves solving linear matrix equation. The matrix equation can be easily solved if we approximate probability, in the form: gamma_v'->v=(1/v')theta(v'->v). In this case, the steady-state solution for VDF(v) simply involves a sum of source rates for levels above , with a factor of 1/(v+1). As an example of application, we study the vibrational kinetics in a hydrogen gas and verify the analytical solution by comparing with a full model., Comment: 11 pages, 6 figures, letter

Benchmarking and validation are prerequisite for using simulation codes as predictive tools. In this work, we have developed a Global Model for Negative Hydrogen Ion Source (GMNHIS) and performed benchmarking of GMNHIS against another independently developed code, Global Enhanced Vibrational Kinetic Model (GEVKM). This is the first study to present quite comprehensive benchmarking test of this kind for models of negative hydrogen ion sources (NHIS), and very good agreement has been achieved for electron temperature, vibrational distribution function (VDF) of hydrogen molecules, and n_H^-/n_e ratio. The small discrepancies in number densities of negative hydrogen ions, positive ions, as well as hydrogen atoms can be attributed to the differences in the predicted electron number density for given discharge power. Higher electron number density obtained with GMNHIS is possibly due to fewer dissociation channels accounted for in GMNHIS, leading to smaller energy loss. In addition, we validated GMNHIS against experimental data obtained in an electron cyclotron resonance (ECR) discharge used for H^- production. The model qualitatively (and even quantitatively for certain conditions) reproduces the experimental H^- number density. The H^- number density as a function of pressure first increases at pressures below 12 mTorr, and then saturates for higher pressures. This dependence was analyzed by evaluating contributions from different reaction pathways to the creation and loss of the H^- ions. The developed codes can be used for predicting the H^- production, improving the performance of NHIS, and ultimately optimizing the parameters of negative ion beams for ITER., Comment: 25 pages, 12 figures

An analytical model has been developed to map out the low-pressure (left-hand) branch of the Paschen curve at very high voltage when electrons are in the runaway regime and charge exchange/ionization avalanche by ions and fast neutral atoms becomes important. The model has been applied to helium gas between parallel-plate electrodes, at potentials ranging in magnitude between 10 and 1000 kilovolt. The respective value of reduced electric field E/n varies in the range of 50-6000kTd, with reduced density nd (where n is the gas density and d is the inter-electrode distance) on the order of 10^20 m^-2. For fast neutral atoms produced via charge exchange, the following interactions prove essential to understanding the breakdown mechanism: contribution to impact ionization, strongly anisotropic scattering in collisions with background atoms,and backscattering (of both atoms and ions, which become neutralized) from the cathode. Three regimes of the breakdown have been identified according to relative share of impact ionization by electrons, by ions, and by fast neutrals. In the fast-neutral regime of particular interest here, the ionization avalanche is directed from anode towards cathode. It is initiated by the fast neutral beam backscattered from the cathode, and charge multiplication occurs through multiple successive cycles of ionization and charge exchange. Further, the double-valued shape of the Paschen curve with a branch point near 200 kV is found to be due to heavy species undergoing a transition to runaway regime. The analytical Paschen curve is compared to those obtained with a detailed Particle-In-Cell/Monte Carlo (PIC/MCC) simulation, and also to experimental measurements. The model provides accurate predictions for E/n up to ~ 1000 kTd, constrained by availability and quality of required input data., Comment: 30 pages,14 figures

The two particle-in-cell codes EDIPIC and LSP are benchmarked and validated for a parallel-plate glow discharge in helium, in which the axial electric field had been carefully measured, primarily to investigate and improve the fidelity of their collision models. The scattering anisotropy of electron-impact ionization, as well as the value of the secondary-electron emission yield, are not well known in this case. The experimental uncertainty for the emission yield corresponds to a factor of two variation in the cathode current. If the emission yield is tuned to make the cathode current computed by each code match the experiment, the computed electric fields are in excellent agreement with each other, and within about 10\% of the experimental value. The non-monotonic variation of the width of the cathode fall with the applied voltage seen in the experiment is reproduced by both codes. The electron temperature in the negative glow is within experimental error bars for both codes, but the density of slow trapped electrons is underestimated. A more detailed code comparison done for several synthetic cases of electron-beam injection into helium gas shows that the codes are in excellent agreement for ionization rate, as well as for elastic and excitation collisions with isotropic scattering pattern. The remaining significant discrepancies between the two codes are due to differences in their electron binary-collision models, and for anisotropic scattering due to elastic and excitation collisions.

An independent control of the flux and energy of ions impacting on an object immersed in a plasma is often desirable for many industrial processes such as microelectronics manufacturing. We demonstrate that a simultaneous control of these quantities is possible by a suitable choice of a static magnetic field applied parallel to the plane electrodes in a standard single frequency capacitively coupled plasma device. Our particle-in-cell simulations show a 60% reduction in the sheath width (that improves control of ion energy) and a four fold increase in the ion flux at the electrode as a consequence of the altered ion and electron dynamics due to the ambient magnetic field. A detailed analysis of the particle dynamics is presented and the optimized operating parameters of the device are discussed. The present technique offers a simple and attractive alternative to conventional dual frequency based devices that often suffer from undesirable limitations arising from frequency coupling and electromagnetic effects., Comment: 6 pages, 4 figures

In this survey we consider numerous known and unknown combinatorial realizations of the sequence A079487 and basic facts about it., Comment: 14 pages, 12+ figures

The ballistic population is thought to be responsible for alleviating the electron shading effect and the notching of the photoresist layer. We have performed test-particle simulations where the features in the EVDF of electrons impacting the RF electrode are fully resolved at all energies. An analytic model has been developed to predict existence of peaked and step-like structures in the EVDF., Comment: 29 pages, submitted to Plasma Science and Technology