Electron Dynamics Research Articles

High-order harmonic generation in liquid crystals

Thermotropic liquid crystals are versatile optical materials that exhibit a state of matter intermediate between liquids and solids. Their properties can change significantly with temperature, pressure, or other external factors, leading to different phases. The transport properties within these materials in different phases are still largely unexplored, and their understanding would enable exciting prospects for innovative technological advancements. High-order harmonic spectroscopy proved to be a powerful spectroscopic tool for investigating the electronic and nuclear dynamics in matter. Here, we report the first experimental observation of high-order harmonic generation in thermotropic liquid crystals in two different phase states, nematic and isotropic. We found the harmonic emission in the nematic phase to be strongly dependent on the relative orientation of the driving field polarization with respect to the liquid crystal alignment. Specifically, the harmonic yield has a maximum when the molecules are aligned perpendicularly to the polarization of the incoming radiation. Our results establish the first step for applying high-order harmonic spectroscopy as a tool for resolving ultrafast electron dynamics in liquid crystals with unprecedented temporal and spatial resolution.

Whistler Waves in the Quasi‐Parallel and Quasi‐Perpendicular Magnetosheath

AbstractIn the Earth's magnetosheath (MSH), several processes contribute to energy dissipation and plasma heating, one of which is wave‐particle interactions between whistler waves and electrons. However, the overall impact of whistlers on electron dynamics in the MSH remains to be quantified. We analyze 18 hr of burst‐mode measurements from the Magnetospheric Multiscale (MMS) mission, including data from the unbiased magnetosheath campaign during February‐March 2023. We present a statistical study of 34,409 whistler waves found using automatic detection. We compare wave occurrence in the different MSH geometries and find three times higher occurrence in the quasi‐perpendicular MSH compared to the quasi‐parallel case. We also study the wave properties and find that the waves propagate quasi‐parallel to the background magnetic field, have a median frequency of 0.2 times the electron cyclotron frequency, median amplitude of 0.03–0.06 nT (30–60 pT), and median duration of a few tens of wave periods. The whistler waves are preferentially observed in local magnetic dips and density peaks and are not associated with an increased temperature anisotropy. Also, almost no whistlers are observed in regions with parallel electron plasma beta lower than 0.1. Importantly, when estimating pitch‐angle diffusion times we find that the whistler waves cause significant pitch‐angle scattering of electrons in the MSH.

Influences of Solar Wind Parameters on Energetic Electron Fluxes at Geosynchronous Orbit Revealed by the Deep SHAP Method

AbstractSolar wind is an intermediary in energy transfer from the Sun into the Earth's magnetosphere, and is considered as a decisive driver of energetic electron dynamics at the geosynchronous orbit (GEO). Based on machine learning technology, several models driven by solar wind parameters have been established to predict GEO electron fluxes. However, the relative contributions of different solar wind parameters on GEO electron fluxes are still unclear. Recently, a feature attribution method, Deep SHapley Additive exPlanations (Deep SHAP) is proposed to open black boxes of machine learning models. In this study, we use the Deep SHAP method to quantify contributions of different solar wind parameters with an artificial neural network (ANN) model. Backpropagating the prediction results of this ANN model from 2011 to 2020, SHAP values for four solar wind parameters (interplanetary magnetic field (IMF) BZ, solar wind speed, solar wind dynamic pressure, and proton density) are calculated and comprehensively analyzed. The results suggest that solar wind speed with a lag of 1 day is the most important driver. We further investigate relative roles of different parameters in three specific electron fluxes variation events (corresponding to electron fluxes reaching a local maximum, a local minimum, and unchanged, respectively). The results suggest that high solar wind speed and southward IMF BZ (high dynamic pressures) facilitate increases (decreases) of electron fluxes. These findings help reveal the underlying physical mechanisms of GEO electron dynamics and help develop more accurate prediction models for GEO electron fluxes.

ULF Wave Transport of Relativistic Electrons in the Van Allen Belts: Criteria for Transition to Radial Diffusion

AbstractRelativistic electrons in the radiation belts can be transported as a result of wave‐particle interactions (WPI) with ultra‐low frequency (ULF) waves. Such WPI are often assumed to be diffusive, parametric models for the radial diffusion coefficient often being used to assess the rates of radial transport. However, these WPI transition from initially coherent interactions to the diffusive regime over a finite time, this time depending on the ULF wave power spectral density, and local resonance conditions. Further, in the real system on the timescales of a single storm, interactions with finite discrete modes may be more realistic. Here, we use a particle‐tracing model to simulate the dynamics of outer radiation belt electrons in the presence of a finite number of discrete frequency modes. We characterize the point of the onset of diffusion as a transition from separate discrete interactions in terms of wave parameters by using the “two‐thirds” overlap criterion (Lichtenberg & Lieberman, 1992, https://doi.org/10.1007/978‐1‐4757‐2184‐3), a comparison between the distance between, and the widths of, the electron's primary resonant islands in phase space. Further, we find the particle decorrelation time in our model system with typical parameters to be on the timescale of hours, which only afterward can the system be modeled by one‐dimensional radial diffusion. Direct comparison of particle transport rates in our model with previous analytic diffusion coefficient formulations show good agreement at times beyond the decorrelation time. These results are critical for determining the time periods and conditions under which ULF wave radial diffusion theory can be applied.

Nanoscale thermal imaging of hot electrons by cryogenic terahertz scanning noise microscopy.

Nanoscale thermal imaging and temperature detection are of fundamental importance in diverse scientific and technological realms. Most nanoscale thermometry techniques focus on probing the temperature of lattice or phonons and are insensitive to nonequilibrium electrons, commonly referred to as "hot electrons." While terahertz scanning noise microscopy (SNoiM) has been demonstrated to be powerful in the thermal imaging of hot electrons, prior studies have been limited to room temperature. In this work, we report the development of a cryogenic SNoiM (Cryo-SNoiM) tailored for quantitative hot electron temperature detection at low temperatures. The microscope features a special two-chamber design where the sensitive terahertz detector, housed in a vacuum chamber, is efficiently cooled to ∼5K using a pulse tube cryocooler. In a separate chamber, the atomic force microscope and the sample can be maintained at room temperature under ambient/vacuum conditions or cooled to ∼110K via liquid nitrogen. This unique dual-chamber cooling system design enhances the efficacy of SNoiM measurements at low temperatures. It not only facilitates the pre-selection of tips at room temperature before cooling but also enables the quantitative derivation of local electron temperature without reliance on any adjustable parameters. The performance of Cryo-SNoiM is demonstrated through imaging the distribution of hot electrons in a cold, self-heated narrow metal wire. This instrumental innovation holds great promise for applications in imaging low-temperature hot electron dynamics and nonequilibrium transport phenomena across various material systems.

Numerical study of the influence of electron inertial effects and electron dynamics on tearing mode instability

The tearing mode instabilities were numerically studied in two distinct models: the finite electron inertial magnetohydrodynamics (MHD) and the electron MHD (EMHD). The finite electron inertial MHD model employed a modified Hall-MHD model that incorporated the electron inertial effects in the generalized Ohm’s Law. On the other hand, the electron dynamics were described by the EMHD model. It is found that both electron inertial effects and electron dynamics significantly influence the linear and nonlinear growth of tearing mode instabilities, with electron dynamics playing a more dominant role. The dependence of the linear growth rate of tearing modes on the electron inertial length de was investigated. The results show that electron inertial effects enhance the growth rate but resemble the behavior of resistivity η. Whereas, in the EMHD model, electron inertia plays a dominant role in tearing mode instabilities. Additionally, a study on the nonlinear saturation of (2,1) tearing modes was conducted, demonstrating consistency with relevant analytical theories. The study indicates that, in both models, the magnetic island exhibits faster growth and achieves a larger saturated island width as de increases.

Beam‐Driven Electron Cyclotron Harmonic and Electron Acoustic Waves as Seen in Particle‐In‐Cell Simulations

AbstractRecent study has demonstrated that electron cyclotron harmonic (ECH) waves can be excited by a low energy electron beam. Such waves propagate at moderately oblique wave normal angles (∼70°). The potential effects of beam‐driven ECH waves on electron dynamics in Earth's plasma sheet is not known. Using two‐dimensional Darwin particle‐in‐cell simulations with initial electron distributions that represent typical plasma conditions in the plasma sheet, we explore the excitation and saturation of such beam‐driven ECH waves. Both ECH and electron acoustic waves are excited in the simulation and propagate at oblique wave normal angles. Compared with the electron acoustic waves, ECH waves grow much faster and have more intense saturation amplitudes. Cold, stationary electrons are first accelerated by ECH waves through cyclotron resonance and then accelerated in the parallel direction by both the ECH and electron acoustic waves through Landau resonance. Beam electrons, on the other hand, are decelerated in the parallel direction and scattered to larger pitch angles. The relaxation of the electron beam and the continuous heating of the cold electrons contribute to ECH wave saturation and suppress the excitation of electron acoustic waves. When the ratio of plasma to electron cyclotron frequency ωpe/ωce increases, the ECH wave amplitude increases while the electron acoustic wave amplitude decreases. Our work reveals the importance of ECH and electron acoustic waves in reshaping sub‐thermal electron distributions and improves our understanding on the potential effects of wave‐particle interactions in trapping ionospheric electron outflows and forming anisotropic (field‐aligned) electron distributions in the plasma sheet.

Unveiling the molecular symphony - A DFT exploration of structure, electronic dynamics, and excited state electron transfer in D-π-A systems, enhanced by TeO2@GQD multi-junctions for solar energy conversion in DSSC

Graphene and graphene-derived materials have sparked a lot of interest because of their unique physico-chemical features, that have positioned graphene as a promising material for future opto-electronics, and energy-harvesting devices. Graphene possesses outstanding mechanical characteristics and chemical inertness, as well as great mobility and optical transparency. Single-layer graphene has a high optical transmissivity that allows it to pass through a wide variety of light wavelengths, making it a popular material for optically conducting windows. Graphene-based metal and metal oxide nanocomposites require substantial investigations to understand the fundamental interactions between nanostructures and the graphene surface in DSSC, for understanding the characteristic features of such nanocomposites. In the present study different donor-π-acceptor, systems were used, which are different in the type of the π –spacer units only. This D-π-A system was then decorated on a (TiO2)9 semiconductor leading to shifting of the absorption wavelength, the absorbed wavelength was further shifted upon interaction with tellurium–oxide@graphene, thereby exploring its application in solar energy harvesting devices. The result of such substitution was assessed in terms of various parameters such as highest occupied molecular orbital (HOMO), least unoccupied molecular orbital (LUMO), energy gap (Egap), maximum wavelength (λmax), the free energy of electron injection efficiency (ΔGinject), open-circuit voltage (Voc), reorganization energy (Δreorg), etc by the DFT method with Gaussian 09 set of codes. The study can prove beneficial for understanding the mechanism of high optical absorption over a broad spectrum in such multijunction systems, the feature which makes them promising materials for efficient optical, electronic, and light-harvesting devices.

Impact of nuclear effects on the ultrafast dynamics of an organic/inorganic mixed-dimensional interface

Electron dynamics at weakly bound interfaces of organic/inorganic materials are easily influenced by large-amplitude nuclear motion. In this work, we investigate the effects of different approximations to the equilibrium nuclear distributions on the ultrafast charge-carrier dynamics of a laser-excited hybrid organic/inorganic interface. By considering a prototypical system consisting of pyrene physisorbed on a MoSe2 monolayer, we analyze linear absorption spectra, electronic density currents, and charge-transfer dynamics induced by a femtosecond pulse in resonance with the frontier-orbital transition in the molecule. The calculations are based on ab initio molecular dynamics with classical and quantum thermostats, followed by time-dependent density-functional theory coupled to multi-trajectory Ehrenfest dynamics. We impinge the system with a femtosecond (fs) pulse of a few hundred GW cm−2 intensity and propagate it for 100 fs. We find that the optical spectrum is insensitive to different nuclear distributions in the energy range dominated by the excitations localized on the monolayer. The pyrene resonance, in contrast, shows a small blue shift at finite temperatures, hinting at an electron-phonon-induced vibrational-level renormalization. The electronic current density following the excitation is affected by classical and quantum nuclear sampling through suppression of beating patterns and faster decay times. Interestingly, finite temperature leads to a longer stability of the ultrafast charge transfer after excitation. Overall, the results show that the ultrafast charge-carrier dynamics are dominated by electronic rather than by nuclear effects at the field strengths and time scales considered in this work.

Ultrafast temporal phase-resolved nonlinear optical spectroscopy in the molecular frame

In an ultrafast nonlinear optical interaction, the electric field of the emitted nonlinear signal provides direct access to the induced nonlinear transient polarization or transient currents and thus carries signatures of ultrafast dynamics in a medium. Measurement of the electric field of such signals offers sensitive observables to track ultrafast electron dynamics in various systems. In this work, we resolve the real-time phase of the electric field of a femtosecond third-order nonlinear optical signal in the molecular frame. The electric field emitted from impulsively pre-aligned gas-phase molecules at room temperature, in a degenerate four-wave mixing scheme, is measured using a spectral interferometry technique. The nonlinear signal is measured around a rotational revival to extract its molecular-frame angle dependence from pump-probe time-delay scans. By comparing these measurements for two linear molecules, carbon dioxide and nitrogen, we show that the measured second-order phase parameter (temporal chirp) of the signal is sensitive to the valence electronic symmetry of the molecules, whereas the amplitude of the signal does not show such sensitivity. We compare measurements to theoretical calculations of the chirp observable in the molecular frame. This work is an important step towards using electric field measurements in nonlinear optical spectroscopy to study ultrafast dynamics of electronically excited molecules in the molecular frame.

Real-time observation of two distinctive non-thermalized hot electron dynamics at MXene/molecule interfaces

The photoinduced non-thermalized hot electrons at an interface play a pivotal role in determining plasmonic driven chemical events. However, understanding non-thermalized electron dynamics, which precedes electron thermalization (~125 fs), remains a grand challenge. Herein, we simultaneously captured the dynamics of both molecules and non-thermalized electrons in the MXene/molecule complexes by femtosecond time-resolved spectroscopy. The real-time observation allows for distinguishing non-thermalized and thermalized electron responses. Differing from the thermalized electron/heat transfer, our results reveal two non-thermalized electron dynamical pathways: (i) the non-thermalized electrons directly transfer to attached molecules at an interface within 50 fs; (ii) the non-thermalized electrons scatter at the interface within 125 fs, inducing adsorbed molecules heating. These two distinctive pathways are dependent on the irradiating wavelength and the energy difference between MXene and adsorbed molecules. This research sheds light on the fundamental mechanism and opens opportunities in photocatalysis and interfacial heat transfer theory.

Light-induced electron dynamics of molecules in cavities: comparison of model Hamiltonians

The rapidly expanding field of polaritonic chemistry requires accurate theoretical simulations to understand new phenomena at the atomic scale. Computing the optoelectronic properties of molecules using established electronic structure methods is a careful balance of accuracy and computational expense, and expanding these methods to quantum electrodynamics to describe coupled cavity-molecule systems is an active topic of development. Key to these methods are the Hamiltonian operators representing the photon cavity modes. The recently introduced quantum electrodynamics time-dependent configuration interaction (QED-TDCI) method allows for the combination of electron dynamics simulations with quantum electrodynamics, enabling the simulation of time-dependent optoelectronic properties of cavity-molecule systems. Using this method, a comparison of two many-state QED Hamiltonians—the Pauli-Fierz and quantum Rabi model Hamiltonians—is presented, with a particular focus on time-dependent properties in applied electric fields.

Capturing electron-driven chiral dynamics in UV-excited molecules

Chiral molecules, used in applications such as enantioselective photocatalysis1, circularly polarized light detection2 and emission3 and molecular switches4,5, exist in two geometrical configurations that are non-superimposable mirror images of each other. These so-called (R) and (S) enantiomers exhibit different physical and chemical properties when interacting with other chiral entities. Attosecond technology might enable influence over such interactions, given that it can probe and even direct electron motion within molecules on the intrinsic electronic timescale6 and thereby control reactivity7–9. Electron currents in photoexcited chiral molecules have indeed been predicted to enable enantiosensitive molecular orientation10, but electron-driven chiral dynamics in neutral molecules have not yet been demonstrated owing to the lack of ultrashort, non-ionizing and perturbative light pulses. Here we use time-resolved photoelectron circular dichroism (TR-PECD)11–15 with an unprecedented temporal resolution of 2.9 fs to map the coherent electronic motion initiated by ultraviolet (UV) excitation of neutral chiral molecules. We find that electronic beatings between Rydberg states lead to periodic modulations of the chiroptical response on the few-femtosecond timescale, showing a sign inversion in less than 10 fs. Calculations validate this and also confirm that the combination of the photoinduced chiral current with a circularly polarized probe pulse realizes an enantioselective filter of molecular orientations following photoionization. We anticipate that our approach will enable further investigations of ultrafast electron dynamics in chiral systems and reveal a route towards enantiosensitive charge-directed reactivity.

Electronic Couplings and Conversion Dynamics between Localized and Charge Transfer Excitations from Many-Body Green's Functions Theory.

We investigate the determination of electronic coupling between localized excitations (LEs) and charge-transfer (CT) excitations based on many-body Green's functions theory in the GW approximation with the Bethe-Salpeter equation (GW-BSE). Using a small molecule dimer system, we first study the influence of different diabatization methods, as well as different model choices within GW-BSE, such as the self-energy models or different levels of self-consistency, and find that these choices affect the LE-CT couplings only minimally. We then consider a large-scale low-donor morphology formed from rubrene and fullerene and evaluate the LE-CT couplings based on coupled GW-BSE-molecular mechanics calculations. For these disordered systems of bulky molecules, we observe differences in the couplings based on the Edmiston-Ruedenberg diabatization compared to the more approximate Generalize Mulliken-Hush and fragment charge difference diabatization formalisms. In a kinetic model for the conversion between LE and CT states, these differences affect the details of state populations in an intermediate time scale but not the final populations.

Fluid and kinetic studies of tokamak disruptions using Bayesian optimization

When simulating runaway electron dynamics in tokamak disruptions, fluid models with lower numerical cost are often preferred to more accurate kinetic models. The aim of this work is to compare fluid and kinetic simulations of a large variety of different disruption scenarios in ITER. We consider both non-activated and activated scenarios; for the latter, we derive and implement kinetic sources for the Compton scattering and tritium beta decay runaway electron generation mechanisms in our simulation tool Dream (Hoppe et al., Comput. Phys. Commun., vol. 268, 2021, 108098). To achieve a diverse set of disruption scenarios, Bayesian optimization is used to explore a range of massive material injection densities for deuterium and neon. The cost function is designed to distinguish between successful and unsuccessful disruption mitigation based on the runaway current, current quench time and transported fraction of the heat loss. In the non-activated scenarios, we find that fluid and kinetic disruption simulations can have significantly different runaway electron dynamics, due to an overestimation of the runaway seed by the fluid model. The primary cause of this is that the fluid hot-tail generation model neglects superthermal electron transport losses during the thermal quench. In the activated scenarios, the fluid and kinetic models give similar predictions, which can be explained by the significant influence of the activated sources on the runaway dynamics and the seed.

Introduction to Section of Dynamic Mathematics: Dynamic Sets Theory: Parallel Sprt-Elements and their Applications

There is a need to develop an instrumental mathematical base for new technologies. The task of the work is to create new approaches for this by introducing new concepts and methods. Our mathematics is unusual for a mathematician, because here the fulcrum is the action, and not the result of the action as in classical mathematics. Therefore, our mathematics is adapted not only to obtain results, but also to directly control actions, which will certainly show its benefits on a fundamentally new type of neural networks with directly parallel calculations, for which it was created. Any action has much greater potential than its result. Significance of the article: in a new qualitatively different approach to the study of complex processes through new mathematical hierarchical parallel dynamic structures, in particular those processes that are dealt with by Synergetics. Our approach is not based on deterministic equations that generate self-organization, which is very difficult to study and gives very small results for a very limited class of problems and does not provide the most important thing - the structure of self-organization. We are just starting from the assumed structure of self-organization, since we are interested not so much in the numerical calculation of this as in the structure of self-organization itself, its formation (construction) for the necessary purposes and its management. Although we are also interested in numerical calculations. Nobel laureates in physics 2023 Ferenc Kraus and his colleagues Pierre Agostini and Anna Lhuillier used a short-pulse laser to generate attosecond pulses of light to study the dynamics of electrons in matter. According to our Theory of singularities of the type synthesizing, its action corresponds to singularity ↑I↓ h q , which allows one to reach the upper level of subtle energies to manipulate lower levels. In April 2023, we proposed using a short-pulse laser to achieve the desired goals by a directly parallel neural network [1]. We then proposed the fundamental development of this directly parallel neural network. In the articles new mathematical structures and operators are constructed through one action - “containment” [2-9]. Here, the construction of new mathematical structures and operators is carried out with generalization to any actions. The significance of our articles is in the formation of the presumptive mathematical structure of subtle energies, this is being done for the first time in science, and the presumptive classification of the mathematical structures of subtle energies for the first time. The experiments of the 2022 Nobel laureates Asle Ahlen, John Clauser, Anton Zeilinger and the experiments in chemistry Nazhipa Valitov eloquently demonstrate that we are right and that these studies are necessary. Be that as it may, we created classes of new mathematical structures, new mathematical singularities, i.e., made a contribution to the development of mathematics

Resolving Photoinduced Femtosecond Three-Dimensional Solute-Solvent Dynamics through Surface Hopping Simulations.

Photoinduced dynamics in solution is governed by mutual solute-solvent interactions, which give rise to phenomena like solvatochromism, the Stokes shift, dual fluorescence, or charge transfer. Understanding these phenomena requires simulating the solute's photoinduced dynamics and simultaneously resolving the three-dimensional solvent distribution dynamics. If using trajectory surface hopping (TSH) to this aim, thousands of trajectories are required to adequately sample the time-dependent three-dimensional solvent distribution functions, and thus resolve the solvent dynamics with sub-Ångstrom and femtosecond accuracy and sufficiently low noise levels. Unfortunately, simulating thousands of trajectories with TSH in the framework of hybrid quantum mechanical/molecular mechanical (QM/MM) can be prohibitively expensive when employing ab initio electronic structure methods. To tackle this challenge, we recently introduced a computationally efficient approach that combines efficient linear vibronic coupling models with molecular mechanics (LVC/MM) via electrostatic embedding [Polonius et al., JCTC 2023, 19, 7171-7186]. This method provides solvent-embedded, nonadiabatically coupled potential energy surfaces while scaling similarly to MM force fields. Here, we employ TSH with LVC/MM to unravel the photoinduced dynamics of two small thiocarbonyl compounds solvated in water. We describe how to estimate the number of trajectories required to produce nearly noise-free three-dimensional solvent distribution functions and present an analysis based on approximately 10,000 trajectories propagated for 3 ps. In the electronic ground state, both molecules exhibit in-plane hydrogen bonds to the sulfur atom. Shortly after excitation, these bonds are broken and reform perpendicular to the molecular plane on timescales that differ by an order of magnitude due to steric effects. We also show that the solvent relaxation dynamics is coupled to the electronic dynamics, including intersystem crossing. These findings are relevant to advance the understanding of the coupled solute-solvent dynamics of solvated photoexcited molecules, e.g., biologically relevant thio-nucleobases.

Limitations of mean-field approximations in describing shift-current and injection-current in materials

We theoretically and computationally investigate bulk photovoltaic effects, with a specific focus on shift-current and injection-current. Initially, we perform a numerical analysis of the direct current (dc) induced by a laser pulse with a one-dimensional model, utilizing mean-field theories such as time-dependent Hartree–Fock and time-dependent Hartree methods. Our numerical results, obtained with mean-field theories, reveal that the dc component of the current, as a second-order nonlinear effect, exists even after irradiation with linearly polarized light as a second-order nonlinear effect, indicating the generation of injection-current. Conversely, when we employ the independent-particle approximation, no injection-current is generated by linearly polarized light. To develop the microscopic understanding of injection-current within the mean-field approximation, we further analyze the dc component of the current with the perturbation theory, employing the mean-field approximations, the independent-particle approximation, and the exact solution of the many-body Schrödinger equation. The perturbation analysis clarifies that the injection-current induced by linearly polarized light under the mean-field approximations is an artifact caused by population imbalance, created through quantum interference from unphysical self-excitation pathways. Therefore, investigation of many-body effects on the bulk photovoltaic effects have to be carefully conducted in mean-field schemes due to potential contamination by unphysical dc current. Additionally, we perform the first-principles electron dynamics calculation for BaTiO3 based on the time-dependent density functional theory, and we confirm that the above findings from the one-dimensional model calculation and the perturbation analysis apply to realistic systems. Published by the American Physical Society 2024

Femtosecond pulse train-facilitated periodic nanostructuring on TiN films via laser-oxidation

Laser-induced periodic surface structure is a universal phenomenon observed when solid materials are irradiated with pulsed lasers. Typically, these structures are generated using Gaussian pulses. Here, we investigate the formation of periodic nanostructures on titanium nitride thin films using two different laser sources: Gaussian pulses and femtosecond pulse trains generated through a Fabry-Perot cavity. Our findings indicate that the formation of self-organized nanostructures on the thin films can occur through either laser-induced oxidation or laser ablation processes, depending on laser fluence, scanning speed, and pulse duration. Interestingly, when utilizing femtosecond pulse trains, we observe that the range of laser fluence thresholds for oxidative nanostructure formation is significantly wider compared to Gaussian pulses. To comprehend the underlying mechanisms driving these observations, we employ a two-temperature model to calculate the ultrafast dynamics of hot electrons when exposed to laser irradiation. Our results reveal that the initial sub-pulse generates a substantial population of hot electrons, exciting surface plasmons and resulting in the creation of a periodic energy distribution. Before these hot electrons can dissipate, subsequent sub-pulses reach the thin film, re-exciting a large number of hot electrons. Consequently, the periodic energy distribution persists for an extended duration, creating more favorable conditions for the formation of periodic oxidative nanostructures when using pulse trains. These findings contribute to a comprehensive understanding of the mechanisms involved in the formation of periodic nanostructures under femtosecond laser irradiation.

MISTER-T: An open-source software package for quantum optimal control of multi-electron systems on arbitrary geometries

We present an open-source software package, MISTER-T (Manipulating an Interacting System of Total Electrons in Real-Time), for the quantum optimal control of interacting electrons within a time-dependent Kohn-Sham formalism. In contrast to other implementations restricted to simple models on rectangular domains, our method enables quantum optimal control calculations for multi-electron systems (in the effective mass formulation) on nonuniform meshes with arbitrary two-dimensional cross-sectional geometries. Our approach is enabled by forward and backward propagator integration methods to evolve the Kohn-Sham equations with a pseudoskeleton decomposition algorithm for enhanced computational efficiency. We provide several examples of the versatility and efficiency of the MISTER-T code in handling complex geometries and quantum control mechanisms. The capabilities of the MISTER-T code provide insight into the implications of varying propagation times and local control mechanisms to understand a variety of strategies for manipulating electron dynamics in these complex systems. Program summaryProgram Title: MISTER-TCPC Library link to program files:https://doi.org/10.17632/psymy4ddnw.1Licensing provisions: GNU General Public License 3Programming language: MATLABSupplementary material: animated movies of total electron densities under the influence of optimal control fields for (1) an asymmetric double-well potential for long propagation times, (2) an asymmetric double-well potential for short propagation times, and (3) a triple-well potential with a position-dependent effective mass.Nature of problem: The MISTER-T code solves quantum optimal control problems for interacting electrons within a time-dependent Kohn-Sham formalism. It can handle two-dimensional systems with arbitrary cross-sectional geometries within the effective mass formulation. The user-friendly code uses forward and backward propagator integration methods to evolve the Kohn-Sham equations with a pseudoskeleton decomposition algorithm for enhanced computational efficiency.Solution method: iterative solution of the quantum optimal control equations using finite element methods, effective mass formulation, pseudoskeleton decomposition, sparse matrix linear algebra, and nonuniform fast Fourier transforms.