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The research presented in the paper concerns the elastic properties of struvite. The article combines theoretical and experimental research. Experimental studies were carried out on struvite single crystals grown in sodium metasilicate gel by single diffusion. This unique method leads to obtaining crystals of sufficiently large size to conduct, for the first time, experimental measurement of elastic properties of monocrystalline struvite. Using the nanoindentation method, the Ez = 29.1 ± 0.7 GPa value of the component of Young's modulus was determined for a struvite single crystal. In addition, the elastic constants C11, C22, and C33 were determined using micro-Brillouin spectroscopy. Theoretical calculations of the abovementioned properties have been carried out by employing density functional theory methods. Scaling of the theoretical elastic constants leads to obtaining good agreement with the experimental values. Values of the Ex and Ey components of the Young's modulus, not available from the experimental nanoindentation technique, have been determined theoretically as 23 GPa and 27 GPa, respectively. Differences in the values of elastic components and Young's modulus components are related to the layered crystal structure of struvite and directional character of the hydrogen-bonding pattern. [ABSTRACT FROM AUTHOR]

With increasing demand and environmental concerns, researchers are exploring new materials that can perform as well or better than traditional materials while reducing environmental impact. The BAMline, a real-life sample materials research beamline, provides unique insights into materials' electronic and chemical structure at different time and length scales. The beamline specializes in x-ray absorption spectroscopy, x-ray fluorescence spectroscopy, and tomography experiments. This enables real-time optimization of material properties and performance for various applications, such as energy transfer, energy storage, catalysis, and corrosion resistance. This paper gives an overview of the analytical methods and sample environments of the BAMline, which cover non-destructive testing experiments in materials science, chemistry, biology, medicine, and cultural heritage. We also present our own synthesis methods, processes, and equipment developed specifically for the BAMline, and we give examples of synthesized materials and their potential applications. Finally, this article discusses the future perspectives of the BAMline and its potential for further advances in sustainable materials research. [ABSTRACT FROM AUTHOR]

We present the computational methodology, which for the first time allows rigorous twelve-dimensional (12D) quantum calculations of the coupled intramolecular and intermolecular vibrational states of hydrogen-bonded trimers of flexible diatomic molecules. Its starting point is the approach that we introduced recently for fully coupled 9D quantum calculations of the intermolecular vibrational states of noncovalently bound trimers comprised of diatomics treated as rigid. In this paper, it is extended to include the intramolecular stretching coordinates of the three diatomic monomers. The cornerstone of our 12D methodology is the partitioning of the full vibrational Hamiltonian of the trimer into two reduced-dimension Hamiltonians, one in 9D for the intermolecular degrees of freedom (DOFs) and another in 3D for the intramolecular vibrations of the trimer, and a remainder term. These two Hamiltonians are diagonalized separately, and a fraction of their respective 9D and 3D eigenstates is included in the 12D product contracted basis for both the intra- and intermolecular DOFs, in which the matrix of the full 12D vibrational Hamiltonian of the trimer is diagonalized. This methodology is implemented in the 12D quantum calculations of the coupled intra- and intermolecular vibrational states of the hydrogen-bonded HF trimer on an ab initio calculated potential energy surface (PES). The calculations encompass the one- and two-quanta intramolecular HF-stretch excited vibrational states of the trimer and low-energy intermolecular vibrational states in the intramolecular vibrational manifolds of interest. They reveal several interesting manifestations of significant coupling between the intra- and intermolecular vibrational modes of (HF)3. The 12D calculations also show that the frequencies of the v = 1, 2 HF stretching states of the HF trimer are strongly redshifted in comparison to those of the isolated HF monomer. Moreover, the magnitudes of these trimer redshifts are much larger than that of the redshift for the stretching fundamental of the donor-HF moiety in (HF)2, most likely due to the cooperative hydrogen bonding in (HF)3. The agreement between the 12D results and the limited spectroscopic data for the HF trimer, while satisfactory, leaves room for improvement and points to the need for a more accurate PES. [ABSTRACT FROM AUTHOR]

This paper reports the release of PathSum, a new software suite of state-of-the-art path integral methods for studying the dynamics of single or extended systems coupled to harmonic environments. The package includes two modules, suitable for system–bath problems and extended systems comprising many coupled system–bath units, and is offered in C++ and Fortran implementations. The system–bath module offers the recently developed small matrix path integral (SMatPI) and the well-established iterative quasi-adiabatic propagator path integral (i-QuAPI) method for iteration of the reduced density matrix of the system. In the SMatPI module, the dynamics within the entanglement interval can be computed using QuAPI, the blip sum, time evolving matrix product operators, or the quantum–classical path integral method. These methods have distinct convergence characteristics and their combination allows a user to access a variety of regimes. The extended system module provides the user with two algorithms of the modular path integral method, applicable to quantum spin chains or excitonic molecular aggregates. An overview of the methods and code structure is provided, along with guidance on method selection and representative examples. [ABSTRACT FROM AUTHOR]

With the development of modern industry, the discharge of dye wastewater is increasing year by year, and the damage caused by this wastewater to the ecosystem is often irreversible. Therefore, the research on the harmless treatment of dyes has attracted much attention in recent years. In this paper, commercial titanium dioxide (anatase nanometer titanium dioxide) was heat treated with anhydrous ethanol to synthesize titanium carbide (C/TiO2). Its maximum adsorption capacity for cationic dyes methylene blue (MB) and Rhodamine B is 27.3 and 124.6 mg g−1, respectively, which is much higher than that of pure TiO2. The adsorption kinetics and isotherm model of C/TiO2 were studied and characterized by Brunauer–Emmett–Teller, x-ray photoelectron spectroscopy, x-ray diffraction, Fourier transform infrared spectroscopy, and other methods. The results show that the carbon layer on the surface of C/TiO2 promotes the increase in surface hydroxyl groups, which is the main reason for the increase in MB adsorption. Compared with other adsorbents, C/TiO2 showed excellent reusability. The experimental results of adsorbent regeneration showed that the adsorption rate R% of MB was almost unchanged after three cycles. During the recovery of C/TiO2, the dyes adsorbed on its surface are removed, which solves the problem that the adsorbent cannot degrade dyes simply by adsorption. Additionally, C/TiO2 has a stable adsorption effect, is insensitive to the pH value, has a simple preparation process, and has relatively low raw material prices, making it suitable for large-scale operation. Therefore, it has good commercial prospects in the organic dye industry wastewater treatment. [ABSTRACT FROM AUTHOR]

Some chemical reactions proceed on multiple potential energy surfaces and are often accompanied by a change in spin multiplicity, being called spin-forbidden reactions, where the spin–orbit coupling (SOC) effects play a crucial role. In order to efficiently investigate spin-forbidden reactions with two spin states, Yang et al. [Phys. Chem. Chem. Phys. 20, 4129–4136 (2018)] proposed a two-state spin-mixing (TSSM) model, where the SOC effects between the two spin states are simulated by a geometry-independent constant. Inspired by the TSSM model, we suggest a multiple-state spin-mixing (MSSM) model in this paper for the general case with any number of spin states, and its analytic first and second derivatives have been developed for locating stationary points on the mixed-spin potential energy surface and estimating thermochemical energies. To demonstrate the performance of the MSSM model, some spin-forbidden reactions involving 5d transition elements are calculated using the density functional theory (DFT), and the results are compared with the two-component relativistic ones. It is found that MSSM DFT and two-component DFT calculations may provide very similar stationary-point information on the lowest mixed-spin/spinor energy surface, including structures, vibrational frequencies, and zero-point energies. For the reactions containing saturated 5d elements, the reaction energies by MSSM DFT and two-component DFT agree very well within 3 kcal/mol. As for the two reactions OsO+ + CH4 → OOs(CH2)+ + H2 and W + CH4 → WCH2 + H2 involving unsaturated 5d elements, MSSM DFT may also yield good reaction energies of similar accuracy but with some counterexamples. Nevertheless, the energies may be remarkably improved by a posteriori single point energy calculations using two-component DFT at the MSSM DFT optimized geometries, and the maximum error of about 1 kcal/mol is almost independent of the SOC constant used. The MSSM method as well as the developed computer program provides an effective utility for studying spin-forbidden reactions. [ABSTRACT FROM AUTHOR]

In modern electronics and power systems, good-performance dielectric capacitors have an essential function. Polymer-based dielectrics are widely used in the field of dielectric capacitors because of their large dielectric constant, flexibility, low density, and ease of processing. At present, ferroelectric polymers suffer from low breakdown field strength and high dielectric losses. How to improve the performance of dielectric materials in capacitors is still a promising research. This paper chooses the ferroelectric polymer poly(vinylidene fluoride) (PVDF) that worked as the matrix, and the linear polymers polyimide, cyanoethyl pullulan (CR-S), polyethersulfone, and cyanoethylated cellulose served as fillers. This all-organic dielectric composite produced as films working in electrostatic energy storage devices is prepared by using a casting method. Analyzing the test results, the composite film exhibited excellent electrical properties when the CR-S doping content was 5 wt. %. The organic composite dielectric based on CR-S/PVDF has a breakdown field strength of 450 MV/m, a discharge energy storage density (Ue) of 10.3 J/cm3, a high dielectric constant of 10.9, and a low dielectric loss of 0.004 at 1 kHz, which is a significant improvement compared with other dielectric composites. This all-organic dielectric composite strategy offers a new approach to achieve better-performance dielectric energy storage materials. [ABSTRACT FROM AUTHOR]

Observations of a high spin selectivity in various helical structures, which is called the chirality-induced spin selectivity, suggest a common mechanism originating from the helical geometry. In this paper, we consider a helical chain of atomic p± orbitals having the tangential angular momentum l = ±1. We show in this model that the coupling of l and the spin gives rise to spin-velocity locking, i.e., directions of spin and group velocity are parallel or antiparallel depending on the chirality of the helix, and consequently, an almost perfect spin selectivity in a specific energy region in a wide range of the curvature and the torsion of the helix. We find that the present spin-velocity locking originates from the helical symmetry in which the Hamiltonian is invariant with respect to a combined operation of the rotation around the helix axis and the translation along the helix axis. Therefore, we expect that spin-velocity locking occurs in a wide variety of helical structures. [ABSTRACT FROM AUTHOR]

Transient bonds between fast linkers and slower particles are widespread in physical and biological systems. Despite their diverse structure and function, a commonality is that the linkers diffuse on timescales much faster compared to the overall motion of the particles they bind to. This limits numerical and theoretical approaches that need to resolve these diverse timescales with high accuracy. Many models, therefore, resort to effective, yet ad hoc, dynamics, where linker motion is only accounted for when bound. This paper provides a mathematical justification for such coarse-grained dynamics that preserves detailed balance at equilibrium. Our derivation is based on multiscale averaging techniques and is broadly applicable. We verify our results with simulations on a minimal model of fast linker binding to a slow particle. We show how our framework can be applied to various systems, including those with multiple linkers, stiffening linkers upon binding, or slip bonds with force-dependent unbinding. Importantly, the preservation of detailed balance only sets the ratio of the binding to the unbinding rates, but it does not constrain the detailed expression of binding kinetics. We conclude by discussing how various choices of binding kinetics may affect macroscopic dynamics. [ABSTRACT FROM AUTHOR]

In this paper, we use the previously introduced Canonical Polyadic (CP)-Multiple Shift Block Inverse Iteration (MSBII) eigensolver [S. D. Kallullathil and T. Carrington, J. Chem. Phys. 155, 234105 (2021)] in conjunction with a contraction tree to compute vibrational spectra. The CP-MSBII eigensolver uses the CP format. The memory cost scales linearly with the number of coordinates. A tensor in CP format represents a wavefunction constrained to be a sum of products (SOP). An SOP wavefunction can be made more accurate by increasing the number of terms, the rank. When the required rank is large, the runtime of a calculation in CP format is long, although the memory cost is small. To make the method more efficient, we break the full problem into pieces using a contraction tree. The required rank for each of the sub-problems is small. To demonstrate the effectiveness of the ideas, we computed vibrational energy levels of acetonitrile (12-D) and ethylene oxide (15-D). [ABSTRACT FROM AUTHOR]

A photovoltaic device fabricated with conventional zincblende materials can use the Type-II quantum well structure, which spatially separates electrons and holes, to reduce their recombination rate. In order to obtain higher power conversion efficiency, it is desirable to preserve more energetic carriers by engineering a phonon "bottleneck," a mismatch between the gaps in the well and barrier phonon structure. Such a mismatch leads to poor phonon transport and therefore prevents energy from leaving the system in the form of heat. In this paper, we perform a superlattice phonon calculation to verify the "bottleneck" effect and build on this a model to predict the steady state of the hot electrons under photoexcitation. We describe the electrons and phonons with a coupled Boltzmann equation system and numerically integrate it to get the steady state. We find that inhibited phonon relaxation does lead to a more out-of-equilibrium electron distribution and discuss how this might be enhanced. We examine the different behaviors obtained for various combinations of recombination and relaxation rates and their experimental signatures. [ABSTRACT FROM AUTHOR]

Simulations of exciton and charge hopping in amorphous organic materials involve numerous physical parameters. Each of these parameters must be computed from costly ab initio calculations before the simulation can commence, resulting in a significant computational overhead for studying exciton diffusion, especially in large and complex material datasets. While the idea of using machine learning to quickly predict these parameters has been explored previously, typical machine learning models require long training times, which ultimately contribute to simulation overheads. In this paper, we present a new machine learning architecture for building predictive models for intermolecular exciton coupling parameters. Our architecture is designed in such a way that the total training time is reduced compared to ordinary Gaussian process regression or kernel ridge regression models. Based on this architecture, we build a predictive model and use it to estimate the coupling parameters which enter into an exciton hopping simulation in amorphous pentacene. We show that this hopping simulation is able to achieve excellent predictions for exciton diffusion tensor elements and other properties as compared to a simulation using coupling parameters computed entirely from density functional theory. This result, along with the short training times afforded by our architecture, shows how machine learning can be used to reduce the high computational overheads associated with exciton and charge diffusion simulations in amorphous organic materials. [ABSTRACT FROM AUTHOR]

In this paper, we outline a physically motivated framework for describing spin-selective recombination processes in chiral systems, from which we derive spin-selective reaction operators for recombination reactions of donor–bridge–acceptor molecules, where the electron transfer is mediated by chirality and spin–orbit coupling. In general, the recombination process is selective only for spin-coherence between singlet and triplet states, and it is not, in general, selective for spin polarization. We find that spin polarization selectivity only arises in hopping-mediated electron transfer. We describe how this effective spin-polarization selectivity is a consequence of spin-polarization generated transiently in the intermediate state. The recombination process also augments the coherent spin dynamics of the charge separated state, which is found to have a significant effect on the recombination dynamics and to destroy any long-lived spin polarization. Although we only consider a simple donor–bridge–acceptor system, the framework we present here can be straightforwardly extended to describe spin-selective recombination processes in more complex systems. [ABSTRACT FROM AUTHOR]

The self-consistent phonon (SCP) method allows one to include anharmonic effects when treating a many-body quantum system at thermal equilibrium. The system is then described by an effective temperature-dependent harmonic Hamiltonian, which can be used to estimate its various dynamic and static properties. In this paper, we combine SCP with ab initio (AI) potential energy evaluation in which case the numerical bottleneck of AI-SCP is the evaluation of Gaussian averages of the AI potential energy and its derivatives. These averages are computed efficiently by the quasi-Monte Carlo method utilizing low-discrepancy sequences leading to a fast convergence with respect to the number, S, of the AI energy evaluations. Moreover, a further substantial (an-order-of-magnitude) improvement in efficiency is achieved once a numerically cheap approximation of the AI potential is available. This is based on using a perturbation theory-like (the two-grid) approach in which it is the average of the difference between the AI and the approximate potential that is computed. The corresponding codes and scripts are provided. [ABSTRACT FROM AUTHOR]

A large number of force fields have been proposed for describing the behavior of liquid water within classical atomistic simulations, particularly molecular dynamics. In the past two decades, models that incorporate molecular polarizability and even charge transfer have become more prevalent, in attempts to develop more accurate descriptions. These are frequently parameterized to reproduce the measured thermodynamics, phase behavior, and structure of water. On the other hand, the dynamics of water is rarely considered in the construction of these models, despite its importance in their ultimate applications. In this paper, we explore the structure and dynamics of polarizable and charge-transfer water models, with a focus on timescales that directly or indirectly relate to hydrogen bond (H-bond) making and breaking. Moreover, we use the recently developed fluctuation theory for dynamics to determine the temperature dependence of these properties to shed light on the driving forces. This approach provides key insight into the timescale activation energies through a rigorous decomposition into contributions from the different interactions, including polarization and charge transfer. The results show that charge transfer effects have a negligible effect on the activation energies. Furthermore, the same tension between electrostatic and van der Waals interactions that is found in fixed-charge water models also governs the behavior of polarizable models. The models are found to involve significant energy–entropy compensation, pointing to the importance of developing water models that accurately describe the temperature dependence of water structure and dynamics. [ABSTRACT FROM AUTHOR]

Multiple ERI (Electron Repulsion Integral) tensor contractions (METC) with several matrices are ubiquitous in quantum chemistry. In response theories, the contraction operation, rather than ERI computations, can be the major bottleneck, as its computational demands are proportional to the multiplicatively combined contributions of the number of excited states and the kernel pre-factors. This paper presents several high-performance strategies for METC. Optimal approaches involve either the data layout reformations of interim density and Fock matrices, the introduction of intermediate ERI quartet buffer, and loop-reordering optimization for a higher cache hit rate. The combined strategies remarkably improve the performance of the MRSF (mixed reference spin flip)-TDDFT (time-dependent density functional theory) by nearly 300%. The results of this study are not limited to the MRSF-TDDFT method and can be applied to other METC scenarios. [ABSTRACT FROM AUTHOR]

In this paper, the solubility of carbon dioxide (CO2) in water along the isobar of 400 bar is determined by computer simulations using the well-known TIP4P/Ice force field for water and the TraPPE model for CO2. In particular, the solubility of CO2 in water when in contact with the CO2 liquid phase and the solubility of CO2 in water when in contact with the hydrate have been determined. The solubility of CO2 in a liquid–liquid system decreases as the temperature increases. The solubility of CO2 in a hydrate–liquid system increases with temperature. The two curves intersect at a certain temperature that determines the dissociation temperature of the hydrate at 400 bar (T3). We compare the predictions with T3 obtained using the direct coexistence technique in a previous work. The results of both methods agree, and we suggest 290(2) K as the value of T3 for this system using the same cutoff distance for dispersive interactions. We also propose a novel and alternative route to evaluate the change in chemical potential for the formation of hydrates along the isobar. The new approach is based on the use of the solubility curve of CO2 when the aqueous solution is in contact with the hydrate phase. It considers rigorously the non-ideality of the aqueous solution of CO2, providing reliable values for the driving force for nucleation of hydrates in good agreement with other thermodynamic routes used. It is shown that the driving force for hydrate nucleation at 400 bar is larger for the methane hydrate than for the carbon dioxide hydrate when compared at the same supercooling. We have also analyzed and discussed the effect of the cutoff distance of dispersive interactions and the occupancy of CO2 on the driving force for nucleation of the hydrate. [ABSTRACT FROM AUTHOR]

The development of multireference coupled cluster (MRCC) techniques has remained an open area of study in electronic structure theory for decades due to the inherent complexity of expressing a multiconfigurational wavefunction in the fundamentally single-reference coupled cluster framework. The recently developed multireference-coupled cluster Monte Carlo (mrCCMC) technique uses the formal simplicity of the Monte Carlo approach to Hilbert space quantum chemistry to avoid some of the complexities of conventional MRCC, but there is room for improvement in terms of accuracy and, particularly, computational cost. In this paper, we explore the potential of incorporating ideas from conventional MRCC—namely, the treatment of the strongly correlated space in a configuration interaction formalism—to the mrCCMC framework, leading to a series of methods with increasing relaxation of the reference space in the presence of external amplitudes. These techniques offer new balances of stability and cost against accuracy, as well as a means to better explore and better understand the structure of solutions to the mrCCMC equations. [ABSTRACT FROM AUTHOR]

In this paper, we present dyadic adaptive HOPS (DadHOPS), a new method for calculating linear absorption spectra for large molecular aggregates. This method combines the adaptive HOPS (adHOPS) framework, which uses locality to improve computational scaling, with the dyadic HOPS method previously developed to calculate linear and nonlinear spectroscopic signals. To construct a local representation of dyadic HOPS, we introduce an initial state decomposition that reconstructs the linear absorption spectra from a sum over locally excited initial conditions. We demonstrate the sum over initial conditions can be efficiently Monte Carlo sampled and that the corresponding calculations achieve size-invariant [i.e., O (1) ] scaling for sufficiently large aggregates while trivially incorporating static disorder in the Hamiltonian. We present calculations on the photosystem I core complex to explore the behavior of the initial state decomposition in complex molecular aggregates as well as proof-of-concept DadHOPS calculations on an artificial molecular aggregate inspired by perylene bis-imide to demonstrate the size-invariance of the method. [ABSTRACT FROM AUTHOR]

In this paper, we present a covariant approach that utilizes Noether's second theorem to derive a symmetric stress tensor from the grand thermodynamic potential functional. We focus on the practical case where the density of the grand thermodynamic potential is dependent on the first and second coordinate derivatives of the scalar order parameters. Our approach is applied to several models of inhomogeneous ionic liquids that consider electrostatic correlations of ions or short-range correlations related to packing effects. Specifically, we derive analytical expressions for the symmetric stress tensors of the Cahn–Hilliard-like model, Bazant–Storey–Kornyshev model, and Maggs–Podgornik–Blossey model. All of these expressions are found to be consistent with respective self-consistent field equations. [ABSTRACT FROM AUTHOR]

In this paper, we present a new module to predict the potential surface reconstruction configurations of given surface structures in the framework of our machine learning and graph theory assisted universal structure searcher. In addition to random structures generated with specific lattice symmetry, we made full use of bulk materials to obtain a better distribution of population energy, namely, randomly appending atoms to a surface cleaved from bulk structures or moving/removing some of the atoms on the surface, which is inspired by natural surface reconstruction processes. In addition, we borrowed ideas from cluster predictions to spread structures better between different compositions, considering that surface models of different atom numbers usually have some building blocks in common. To validate this newly developed module, we tested it with studies on the surface reconstructions of Si (100), Si (111), and 4H–SiC (1 1 ̄ 02) − c (2 × 2) , respectively. We successfully gave the known ground states, as well as a new SiC surface model, in an extremely Si-rich environment. [ABSTRACT FROM AUTHOR]

Semiflexible slender filaments are ubiquitous in nature and cell biology, including in the cytoskeleton, where reorganization of actin filaments allows the cell to move and divide. Most methods for simulating semiflexible inextensible fibers/polymers are based on discrete (bead-link or blob-link) models, which become prohibitively expensive in the slender limit when hydrodynamics is accounted for. In this paper, we develop a novel coarse-grained approach for simulating fluctuating slender filaments with hydrodynamic interactions. Our approach is tailored to relatively stiff fibers whose persistence length is comparable to or larger than their length and is based on three major contributions. First, we discretize the filament centerline using a coarse non-uniform Chebyshev grid, on which we formulate a discrete constrained Gibbs–Boltzmann (GB) equilibrium distribution and overdamped Langevin equation for the evolution of unit-length tangent vectors. Second, we define the hydrodynamic mobility at each point on the filament as an integral of the Rotne–Prager–Yamakawa kernel along the centerline and apply a spectrally accurate "slender-body" quadrature to accurately resolve the hydrodynamics. Third, we propose a novel midpoint temporal integrator, which can correctly capture the Ito drift terms that arise in the overdamped Langevin equation. For two separate examples, we verify that the equilibrium distribution for the Chebyshev grid is a good approximation of the blob-link one and that our temporal integrator for overdamped Langevin dynamics samples the equilibrium GB distribution for sufficiently small time step sizes. We also study the dynamics of relaxation of an initially straight filament and find that as few as 12 Chebyshev nodes provide a good approximation to the dynamics while allowing a time step size two orders of magnitude larger than a resolved blob-link simulation. We conclude by applying our approach to a suspension of cross-linked semiflexible fibers (neglecting hydrodynamic interactions between fibers), where we study how semiflexible fluctuations affect bundling dynamics. We find that semiflexible filaments bundle faster than rigid filaments even when the persistence length is large, but show that semiflexible bending fluctuations only further accelerate agglomeration when the persistence length and fiber length are of the same order. [ABSTRACT FROM AUTHOR]

Second-order N-electron valence state perturbation theory (NEVPT2) is an exactly size-consistent and intruder-state-free multi-reference theory. To accelerate the NEVPT2 computation, Guo and Neese combined it with the local pair-natural orbital (PNO) method using the projected atomic orbitals (PAOs) as the underlying local basis [Guo et al., J. Chem. Phys. 144, 094111 (2016)]. In this paper, we report the further development of the PNO-NEVPT2 method using the orthonormal and non-redundant localized virtual molecular orbitals (LVMOs) instead of PAOs. The LVMOs were previously considered to perform relatively poor compared to PAOs because the resulting orbital domains were unacceptably large. Our prior work, however, showed that this drawback can be remedied by re-forming the domain construction scheme using differential overlap integrals [Saitow et al., J. Chem. Phys. 157, 084101 (2022)]. In this work, we develop further refinements to enhance the feasibility of using LVMOs. We first developed a two-level semi-local approach for screening out so-called weak-pairs to select or truncate the pairs for PNO constructions more flexibly. As a refinement specific to the Pipek–Mezey localization for LVMOs, we introduced an iterative scheme to truncate the Givens rotations using varying thresholds. We assessed the LVMO-based PNO-NEVPT2 method through benchmark calculations for linear phenyl alkanes, which demonstrate that it performs comparably well relative to the PAO-based approach. In addition, we evaluated the Co–C bond dissociation energies for the cobalamin derivatives composed of 200 or more atoms, which confirms that the LVMO-based method can recover more than 99.85% of the canonical NEVPT2 correlation energy. [ABSTRACT FROM AUTHOR]

In two recent papers [A. D. Becke, J. Chem. Phys. 156, 214101 (2022) and A. D. Becke, J. Chem. Phys. 157, 234102 (2022)], we compared two Kohn–Sham density functionals based on physical modeling and theory with the best density-functional power-series fits in the literature. The best error statistics reported to date for a hybrid functional on the general main-group thermochemistry, kinetics, and noncovalent interactions (GMTKN55) chemical database of Goerigk et al. [Phys. Chem. Chem. Phys. 19, 32184 (2017)] were obtained. In the present work, additional second-order perturbation-theory terms are considered. The result is a 12-parameter double-hybrid density functional with the lowest GMTKN55 WTMAD2 "weighted total mean absolute deviation" error (1.76 kcal/mol) yet seen for any hybrid or double-hybrid density-functional approximation. We call it "DH23." [ABSTRACT FROM AUTHOR]

Metal oxide nanoparticle (NP) supports of both good conductivity and stability have the potential to enhance both the reaction activity and stability of the loaded electrocatalysts. In this paper, a facile two-step approach to disperse Pt nanoparticles on the surface of an IrO2 NP support (Pt/IrO2) was developed. Physical characterization by x-ray diffraction spectroscopy and transmission/scanning electron microscopy suggests a good dispersion of the Pt NPs. The temperature effect (from 293 to 353 K) of oxygen reduction reaction on Pt/IrO2 was studied by using a rotating ring disk electrode The results show that although the kinetic current density on Pt/IrO2 is close to that on commercial Pt/C at room temperature, the apparent activation energy (Ea,app) in the former case is much lower, suggesting a much higher activity at elevated temperatures. The superiority in Ea,app is attributed to the electron interaction between Pt and the IrO2 support, as supported by the change of surface chemical state given by x-ray photo-electron spectroscopy. [ABSTRACT FROM AUTHOR]

This paper aims at the theoretical study of the CO2 magnetic-dipole ν2 + ν3 rovibrational absorption band that was recently detected in the Martian atmosphere. Specific characteristics of the magnetic dipole operator are carefully examined. Our evaluation of the magnetic-dipole line intensities is based on the variational calculations and the use of molecular properties is determined through specially performed ab initio quantum chemical calculations. The comparison of our simulated magnetic-dipole spectrum with available laboratory taken data also requires the knowledge of line intensities in the quadrupole band, which partially overlaps with that magnetic-dipole. Quadrupole intensities, once reconsidered, are permitted to correct previously reported values of the integrated intensity as well as the intensity of selected branches. The sum of our calculated magnetic-dipole and quadrupole rovibrational lines is shown to be in good agreement with both sets of presently available data from FTIR and OFCEAS laboratory observations. [ABSTRACT FROM AUTHOR]

In Paper I [J. R. Elliott, A. J. Schultz, and D. A. Kofke, J. Chem. Phys. 143, 114110 (2015)] of this series, a methodology was presented for computing the coefficients of a power series of the Helmholtz energy in reciprocal temperature, β, through density series based on cluster integral expansions. Previously, power series in β were evaluated by thermodynamic perturbation theory (TPT) using molecular simulation of a reference fluid. The present methodology uses cluster integrals to evaluate coefficients of the density expansion at each individual order of temperature. While Paper I [J. R. Elliott, A. J. Schultz, and D. A. Kofke, J. Chem. Phys. 143, 114110 (2015)] developed this methodology for square well (SW) spheres, the present work extends the methodology to Lennard-Jones (LJ) spheres, where the reference fluid is the Weeks-Chandler-Andersen potential. Comparisons of TPT coefficients computed from cluster integrals to those from molecular simulation show good agreement through third order in β when coefficients are expressed with effective approximants. Notably, the agreement for LJ spheres is much better than for SW spheres although fewer coefficients of the density series (B2–B5) are available than for SW spheres (B2–B6). The coefficients for Bi(β) of the reference fluid are shown to follow a simple relationship to the virial coefficients of hard sphere fluids, corrected for the temperature dependency of the equivalent hard sphere diameter. This lays the foundation for a correlation of the second virial coefficient of LJ spheres B2(β) that extrapolates to infinite order in temperature. This correlation of B2(β) provides a basis for estimating the low density limit of TPT coefficients at all orders in temperature, facilitating a recursive extrapolation formula to estimate TPT coefficients of fourth order and higher over the entire density range. The applicability of the resulting equation of state is demonstrated by computing the thermodynamic properties for LJ spheres and comparing to standard simulation results. [ABSTRACT FROM AUTHOR]

The present paper is the second part of a series of papers aimed at assessing the accuracy of alchemical computational approaches based on nonequilibrium techniques for solvation free energy of organic molecules in the context of molecular dynamics simulations. In Paper I [Procacci, J. Chem. Phys. 151, 144113 (2019)], we dealt with bidirectional estimates of solvation free energies using nonequilibrium approaches. Here, we assess accuracy and precision of unidirectional estimates with the focus on the Gaussian and Jarzynski estimators. We present a very simple methodology to increase the statistics in the work distribution, hence boosting the accuracy and precision of the Jarzynski unidirectional estimates at no extra cost, exploiting the observed decorrelation between the random variables represented by the Lennard-Jones solute-solvent recoupling or decoupling work and by the electrostatic work due to the charging/discharging of the solute in the solvent. [ABSTRACT FROM AUTHOR]

The polymeric Langmuir theory, developed in Paper I [J. Dudowicz et al., J. Chem. Phys. 151, 124706 (2019)], is employed to investigate the influence of van der Waals interactions and chain rigidity on the thermodynamics of the reversible molecular binding to interfaces in one component polymer fluids (polymer melts). Both van der Waals interactions and chain stiffness are found to influence the temperature variation of the surface coverage Θ, the binding transition itself, and the cooperativity of molecular binding. Re-entrancy of the surface coverage Θ(T) is found to arise when the intermolecular interactions are sufficiently attractive to cause a liquid-vapor like phase separation in the interfacial region, a phenomenon that can occur in the binding of both small molecules and polymer chains to surfaces. [ABSTRACT FROM AUTHOR]

We report the vacuum-ultraviolet threshold-photoelectron spectrum of HC5N recorded over a wide spectral range, from 84 000 to 120 000 cm−1, with a 120 cm−1 spectral resolution, better than what was achieved in previous photoelectron studies, and with mass selectivity. The adiabatic ionization potential of cyanobutadiyne is measured at 85 366 (±40) cm−1. Assignment of the vibrational bands of the four lowest electronic states X+2Π, A+2Π, B+2Σ+, and C+2Π are performed, supported by high level ab initio calculations which are fully detailed in Paper II [B. Gans et al., J. Chem. Phys. 150, 244303 (2019)] and by Franck-Condon simulations. Only vibrational stretching modes are observed in the threshold-photoelectron spectra. The ground state of HC5N+ exhibits a vibrational progression in the ν2 stretching mode involving mainly the elongation of the C≡C triple bonds, whereas the A+ and C+ excited electronic states show a progression in the stretching mode mainly associated with the elongation of the C≡N bond, i.e., ν4 and ν3, respectively. The B+ state appears almost as a vibrationless structure in close vicinity to the A+ state. [ABSTRACT FROM AUTHOR]

Exact nonadiabatic quantum evolution preserves many geometric properties of the molecular Hilbert space. In the first paper of this series ["Paper I," S. Choi and J. Vaníček, J. Chem. Phys. 150, 204112 (2019)], we presented numerical integrators of arbitrary-order of accuracy that preserve these geometric properties exactly even in the adiabatic representation, in which the molecular Hamiltonian is not separable into kinetic and potential terms. Here, we focus on the separable Hamiltonian in diabatic representation, where the split-operator algorithm provides a popular alternative because it is explicit and easy to implement, while preserving most geometric invariants. Whereas the standard version has only second-order accuracy, we implemented, in an automated fashion, its recursive symmetric compositions, using the same schemes as in Paper I, and obtained integrators of arbitrary even order that still preserve the geometric properties exactly. Because the automatically generated splitting coefficients are redundant, we reduce the computational cost by pruning these coefficients and lower memory requirements by identifying unique coefficients. The order of convergence and preservation of geometric properties are justified analytically and confirmed numerically on a one-dimensional two-surface model of NaI and a three-dimensional three-surface model of pyrazine. As for efficiency, we find that to reach a convergence error of 10−10, a 600-fold speedup in the case of NaI and a 900-fold speedup in the case of pyrazine are obtained with the higher-order compositions instead of the second-order split-operator algorithm. The pyrazine results suggest that the efficiency gain survives in higher dimensions. [ABSTRACT FROM AUTHOR]

In this paper, the Hessian matrix of valence bond (VB) self-consistent field (VBSCF) energy with respect to orbitals are evaluated by applying the nonorthogonal orbital based N-body reduced density matrices, which was presented in Paper I. To this end, an automatic formula/code generator (AFCG) is developed; with which the matrix elements between internally contracted excited configurations of VB wave function and the corresponding codes are generated automatically. Compared to the tedious manual formula deducing and implementing, AFCG is much more convenient and efficient, and enables us to avoid troublesome debugging. With the help of AFCG, the Hessian-based Newton-Raphson algorithm is implemented for the VBSCF orbital optimization. Test calculations indicate that the Newton-Raphson algorithm converges quadratically and has much better convergence behavior than the gradient-based LBFGS algorithms. Furthermore, a combined approach with LBFGS and Newton-Raphson algorithms is applied to reduce the total CPU time of the calculation. [ABSTRACT FROM AUTHOR]

The process of quasi-isothermal dehydration of thin films of pure water and aqueous sugar solutions is investigated with a dual experimental and theoretical approach. A nanoporous paper disk with a homogeneous internal structure was used as a substrate. This experimental set-up makes it possible to gather thermodynamic data under well-defined conditions, develop a numerical model, and extract needed information about the dehydration process, in particular the water activity. It is found that the temperature evolution of the pure water film is not strictly isothermal during the drying process, possibly due to the influence of water diffusion through the cellulose web of the substrate. The role of sugar is clearly detectable and its influence on the dehydration process can be identified. At the end of the drying process, trehalose molecules slow down the diffusion of water molecules through the substrate in a more pronounced way than do the glucose molecules. [ABSTRACT FROM AUTHOR]

This document is an erratum for a paper titled "Unusual dynamics of tetrahedral liquids caused by the competition between dynamic heterogeneity and structural heterogeneity" published in the Journal of Chemical Physics. The erratum points out several typographical errors in Figure 5 of the original paper, including incorrect labels and missing information. The corrections provided in the erratum do not impact the results or conclusions of the original paper. The erratum also clarifies a reference to a figure in the Results and Discussions section. [Extracted from the article]

In this paper, we have studied the vibrational spectral features for the collagen triple helix using a dispersion corrected hybrid density functional theory (DFT-D) approach. The protein is simulated by an infinite extended polymer both in the gas phase and in a water micro-solvated environment. We have adopted proline-rich collagen models in line with the high content of proline in natural collagens. Our scaled harmonic vibrational spectra are in very good agreement with the experiments and allow for the peak assignment of the collagen amide I and III bands, supporting or questioning the experimental interpretation by means of vibrational normal modes analysis. Furthermore, we demonstrated that IR spectroscopy in the THz region can detect the small variations inherent to the triple helix helicity (10/3 over 7/2), thus elucidating the packing state of the collagen. So far, identifying the collagen helicity is only possible by means of crystal x-ray diffraction. [ABSTRACT FROM AUTHOR]

Both the reweighting factor and the modified T-move algorithm proposed in this work contribute to reducing the time-step errors. Both the reweighting factor and the modified T-move algorithm proposed in this work contribute to reducing the time-step errors. We discovered a programming error and an error in some of the input files, which led us to recommend a reweighting factor that gives a positive and far from optimal time-step error. [Extracted from the article]

This paper presents further development of the new semi-classical trajectory-based formalism described in Paper I [Chistikov et al., J. Chem. Phys. 151, 194106 (2019)]. We report the results of simulation and analysis of the low-frequency collision-induced absorption (CIA) in CO2–Ar, including its true dimer component. Our consideration relies on the use of ab initio intermolecular potential energy and induced dipole surfaces for CO2–Ar calculated in an assumption of a rigid CO2 structure using the CCSD(T) method. The theory, the details of which are reported in Paper I [Chistikov et al., J. Chem. Phys. 151, 194106 (2019)], permits taking into account the effect of unbound and quasi-bound classical trajectories on the CIA in the range of a rototranslational band. This theory is largely extended by trajectory-based simulation of the true bound dimer absorption in the present paper. The spectra are obtained from a statistical average over a vast ensemble of classical trajectories restricted by properly chosen domains in the phase space. Rigorous classical theory is developed for two low-order spectral moments interpreted as the Boltzmann-weighted average of the respective dipole functions. These spectral moments were then used to check the accuracy of our trajectory-based spectra, for which both spectral moments can be evaluated independently in terms of specific integrals over the trajectory-based calculated spectral profiles. Good agreement between the spectral moments calculated as integrals over the frequency domain or the phase space largely supports the reliability of our simulated CIA spectra, which conform with the available microwave and far-infrared observations. [ABSTRACT FROM AUTHOR]

Often, a single correlation function is used to measure the kinetics of a complex system. In contrast, a large set of k-vector modes and their correlation functions are commonly defined for motion in free space. This set can be transformed to the van Hove correlation function, which is the Green's function for molecular diffusion. Here, these ideas are generalized to other observables. A set of correlation functions of nonlinear functions of an observable is used to extract the corresponding Green's function. Although this paper focuses on nonlinear correlation functions of an equilibrium time series, the results are directly connected to other types of nonlinear kinetics, including perturbation–response experiments with strong fields. Generalized modes are defined as the orthogonal polynomials associated with the equilibrium distribution. A matrix of mode-correlation functions can be transformed to the complete, single-time-interval (1D) Green's function. Diagonalizing this matrix finds the eigendecays. To understand the advantages and limitation of this approach, Green's functions are calculated for a number of models of complex dynamics within a Gaussian probability distribution. Examples of non-diffusive motion, rate heterogeneity, and range heterogeneity are examined. General arguments are made that a full set of nonlinear 1D measurements is necessary to extract all the information available in a time series. However, when a process is neither dynamically Gaussian nor Markovian, they are not sufficient. In those cases, additional multidimensional measurements are needed. [ABSTRACT FROM AUTHOR]

This paper makes an extensive comparison of a dynamical model for a mechanism of direct dissociation to the detailed molecular beam experiments of CH4 dissociation on a Ni(100) surface reported in the previous paper. When a PES incorporating an ‘‘exit channel’’ barrier is used in the model and steric (multidimensional) aspects are included approximately via a ‘‘hole’’ approximation, excellent agreement is achieved between the model and experiments. This strengthens the qualitative mechanistic conclusions of Holmblad, Wambach, and Chorkendorff [J. Chem. Phys. 102, 8255 (1995)]. © 1995 American Institute of Physics. [ABSTRACT FROM AUTHOR]

Two-dimensional (2D) Janus transition metal dichalcogenides MXY manifest novel physical properties owing to the breaking of out-of-plane mirror symmetry. Recently, the 2H phase of MoSH has been demonstrated to possess intrinsic superconductivity, whereas the 1T phase exhibits a charge density waves state. In this paper, we have systematically studied the stability and electron–phonon interaction characteristics of MoSLi. Our results have shown that both the 2H and 1T phases of MoSLi are stable, as indicated by the phonon spectrum and the ab initio molecular dynamics. However, the 1T phase exhibits an electron–phonon coupling constant that is twice as large as that of the 2H phase. In contrast to MoSH, the 1T phase of MoSLi exhibits intrinsic superconductivity. By employing the ab initio anisotropic Migdal-Eliashberg formalism, we have revealed the two-gap superconducting nature of 1T-MoSLi, with a transition temperature (Tc) of 14.8 K. The detailed analysis indicates that the superconductivity in 1T-MoSLi primarily originates from the interplay between the vibration of the phonon modes in the low-frequency region and the dz2 orbital. These findings provide a fresh perspective on superconductivity within Janus structures. [ABSTRACT FROM AUTHOR]

Endohedrally doped clusters form a large category of cage clusters, with unique structures, diverse elemental compositions, and highly tunable electronic structures and physisochemical properties. They have been widely achieved in laboratory and may serve as functional building blocks for assembling new supermolecular structures and devices. In this paper, for the first time, we disclosed the luminescence properties of endohedrally doped group-IV clusters by time-dependent density functional theory calculations. A total of 64 cage clusters have been explored in terms of stability, emission wavelength, and the energy difference between the first excited singlet and triplet states. The key geometric and electronic factors governing the photophysical properties of these cage clusters were unveiled, to provide crucial insights for crafting atomically precise nanoclusters for optical and optoelectronic applications. [ABSTRACT FROM AUTHOR]

It is significant to investigate the calcium carbonate (CaCO3) precipitation mechanism during the carbon capture process; nevertheless, CaCO3 precipitation is not clearly understood yet. Understanding the carbonation mechanism at the atomic level can contribute to the mineralization capture and utilization of carbon dioxide, as well as the development of new cementitious materials with high-performance. There are many factors, such as temperature and CO2 concentration, that can influence the carbonation reaction. In order to achieve better carbonation efficiency, the reaction conditions of carbonation should be fully verified. Therefore, based on molecular dynamics simulations, this paper investigates the atomic-scale mechanism of carbonation. We investigate the effect of carbonation factors, including temperature and concentration, on the kinetics of carbonation (polymerization rate and activation energy), the early nucleation of calcium carbonate, etc. Then, we analyze the local stresses of atoms to reveal the driving force of early stage carbonate nucleation and the reasons for the evolution of polymerization rate and activation energy. Results show that the higher the calcium concentration or temperature, the higher the polymerization rate of calcium carbonate. In addition, the activation energies of the carbonation reaction increase with the decrease in calcium concentrations. [ABSTRACT FROM AUTHOR]

Vibrational coherences in ultrafast pump–probe (PP) and 2D electronic spectroscopy (2DES) provide insights into the excited state dynamics of molecules. Femtosecond coherence spectra and 2D beat maps yield information about displacements of excited state surfaces for key vibrational modes. Half-broadband 2DES uses a PP configuration with a white light continuum probe to extend the detection range and resolve vibrational coherences in the excited state absorption (ESA). However, the interpretation of these spectra is difficult as they are strongly dependent on the spectrum of the pump laser and the relative displacement of the excited states along the vibrational coordinates. We demonstrate the impact of these convoluting factors for a model based upon cresyl violet. A careful consideration of the position of the pump spectrum can be a powerful tool in resolving the ESA coherences to gain insights into excited state displacements. This paper also highlights the need for caution in considering the spectral window of the pulse when interpreting these spectra. [ABSTRACT FROM AUTHOR]

This paper evaluates the accuracy of the Hermitian form of the downfolding procedure using the double unitary coupled cluster (DUCC) ansatz on the benchmark systems of linear chains of hydrogen atoms, H6 and H8. The computational infrastructure employs the occupation-number-representation codes to construct the matrix representation of arbitrary second-quantized operators, allowing for the exact representation of exponentials of various operators. The tests demonstrate that external amplitudes from standard single-reference coupled cluster methods that sufficiently describe external (out-of-active-space) correlations reliably parameterize the Hermitian downfolded effective Hamiltonians in the DUCC formalism. The results show that this approach can overcome the problems associated with losing the variational character of corresponding energies in the corresponding SR-CC theories. [ABSTRACT FROM AUTHOR]

Quantum Dot Cellular Automata (QCA) is an emerging trend in the field of nanoelectronics, and computing can be regarded as an alternative to the traditional complementary metal–oxide–semiconductor technology. The paper is devoted to the study of the key functional properties of the cells for molecular QCA based on mixed valence molecules. The theoretical results for the heat dissipation under the conditions of the fast nonadiabatic switching event and cell–cell response function are obtained in the framework of the quantum-mechanical vibronic approach. These results are parameterized using the previous reliable ab initio calculations performed for oxidized norbornadiene and its polycyclic derivatives with variable lengths of the bridge. The comparative analysis of the dimeric and bidimeric molecular cells composed of these compounds is given. It is underlined that the conditions of a strong non-linear response and a low heat release are contradictory. However, despite this problem, a parametric regime is proposed, which provides a low heat release in combination with a strong nonlinear response of the working cell to the electric field induced by the polarized driver cell. [ABSTRACT FROM AUTHOR]

In the previous paper [C. W. Kim and I. Franco, J. Chem. Phys. 160, 214111-1–214111-13 (2024)], we developed a theory called MQME-D, which allows us to decompose the overall energy dissipation process in open quantum system dynamics into contributions by individual components of the bath when the subsystem dynamics is governed by a Markovian quantum master equation (MQME). Here, we contrast the predictions of MQME-D against the numerically exact results obtained by combining hierarchical equations of motion (HEOM) with a recently reported protocol for monitoring the statistics of the bath. Overall, MQME-D accurately captures the contributions of specific bath components to the overall dissipation while greatly reducing the computational cost compared to exact computations using HEOM. The computations show that MQME-D exhibits errors originating from its inherent Markov approximation. We demonstrate that its accuracy can be significantly increased by incorporating non-Markovianity by exploiting time scale separations (TSS) in different components of the bath. Our work demonstrates that MQME-D combined with TSS can be reliably used to understand how energy is dissipated in realistic open quantum system dynamics. [ABSTRACT FROM AUTHOR]

The superadiabatic dynamical density functional theory (superadiabatic-DDFT) is a promising new method for the study of colloidal systems out-of-equilibrium. Within this approach, the viscous forces arising from interparticle interactions are accounted for in a natural way by explicitly treating the dynamics of the two-body correlations. For bulk systems subject to spatially homogeneous shear, we use the superadiabatic-DDFT framework to calculate the steady-state pair distribution function and the corresponding viscosity for low values of the shear-rate. We then consider a variant of the central approximation underlying this superadiabatic theory and obtain an inhomogeneous generalization of a rheological bulk theory due to Russel and Gast. This paper thus establishes for the first time a connection between DDFT approaches, formulated to treat inhomogeneous systems, and existing work addressing nonequilibrium microstructure and rheology in bulk colloidal suspensions. [ABSTRACT FROM AUTHOR]

We propose a new collocation multi-configuration time-dependent Hartree (MCTDH) method. It reduces point-set error by using more points than basis functions. Collocation makes it possible to use MCTDH with a general potential energy surface without computing any integrals. The collocation points are associated with a basis larger than the basis used to represent wavefunctions. Both bases are obtained from a direct product basis built from single-particle functions by imposing a pruning condition. The collocation points are those on a sparse grid. Heretofore, collocation MCTDH calculations with more points than basis functions have only been possible if both the collocation grid and the basis set are direct products. In this paper, we exploit a new pseudo-inverse to use both more points than basis functions and a pruned basis and grid. We demonstrate that, for a calculation of the lowest 50 vibrational states (energy levels and wavefunctions) of CH2NH, errors can be reduced by two orders of magnitude by increasing the number of points, without increasing the basis size. This is true also when unrefined time-independent points are used. [ABSTRACT FROM AUTHOR]

In this paper, we introduce the Floquet mean-field dynamics and Floquet surface hopping approaches to study the nonadiabatic dynamics in periodically driven solid systems. We demonstrate that these two approaches can be formulated in both real and reciprocal spaces. Using the two approaches, we are able to simulate the interaction between electronic carriers and phonons under periodic drivings, such as strong light–matter interactions. Employing the Holstein and Peierls models, we show that strong light–matter interactions can effectively modulate the dynamics of electronic population and mobility. Notably, our study demonstrates the feasibility and effectiveness of modeling low-momentum carriers' interactions with phonons using a truncated reciprocal space basis, an approach impractical in real space frameworks. Moreover, we reveal that even with a significant truncation, carrier populations derived from surface hopping maintain greater accuracy compared to those obtained via mean-field dynamics. These results underscore the potential of our proposed methods in advancing the understanding of carrier–phonon interactions in various periodically driven materials. [ABSTRACT FROM AUTHOR]