Ab Initio Level Research Articles

Quantifying the Structure of Water and Hydrated Monovalent Ions by Density Functional Theory-Based Molecular Dynamics.

The accurate description of the structures of water and hydrated ions is important in electrochemical desalination, ion separation, and supercapacitors. In this work, we present an ab initio atomistic simulation-based study to explore the structure of water and hydrated monovalent ions (Li+, Na+, K+, Rb+, F-, and Cl-) at ambient conditions using generalized gradient approximation (GGA)-based methods with and without van der Waals correction (PBE, PBE + D3, and revPBE + D3) and recently developed strongly constrained and appropriately normed (SCAN) meta-GGA. We find that both revPBE + D3 and SCAN can well capture the structure of bulk water with +30 K artificial high temperature in contrast to overstructuring water using PBE and PBE + D3. However, being the same as PBE + D3, revPBE + D3 overestimates the structure of the hydration shell, especially for monovalent cations. Surprisingly, SCAN can well match the experimental results of hydrated monovalent ions. Detailed structure analyzes of entropy reveal that the hydration shell under the level of PBE + D3 and revPBE + D3 is more disordered and looser than SCAN. The successful prediction of the flexible SCAN functional could facilitate the exploration of complex ionic processes in the aqueous phase, the interactions of hydrated ions with surfaces, and solvation states in nanopores at an accurate, efficient, predictive, and ab initio level.

A systematic review of computer-mediated communications in Chinese as a foreign language from 2008 to 2022: Research contexts, theoretical foundations and methodology, affordances and limitations

The Covid-19 pandemic has demonstrated how ubiquitous and pervasive technology to support communication and collaboration has become in people’s lives. This article seeks to provide an overview of the use of computer-mediated communication (CMC) in learning Chinese as a foreign language (CFL). The authors systematically reviewed 68 empirical research articles and 3 review articles published between 2008 and 2022 (early April). This in-depth review aims to investigate: (1) the characteristics of CMC-facilitated CFL learning in the worldwide context; (2) common theoretical foundations and methodological approaches; (3) CFL learners’ linguistic and intercultural communicative competence development through CMC; (4) affordances and limitations of CMC in the field of CFL research. Findings from this review suggest that the majority of studies were in formal education contexts within Anglosphere countries. The most commonly acknowledged theoretical foundations in CFL were well aligned with the wider second language acquisition (SLA) domain. A mixed-methods approach was the predominant methodological approach undertaken in the selected papers, with a small number of experimental or quasi-experimental studies between 2008 and 2022. The analysis also identified a clear research gap in relation to young CFL learners in the literature. The predominance of studies at ab initio level would suggest that more research is needed on younger CFL learners and on intermediate and advanced CFL learners using CMC. Additionally, the synthesized affordances of applying CMC technologies in CFL practice from this review were: (1) active engagement; (2) authentic communication; (3) learner centeredness; and (4) opportunities for practice and discovery. By addressing technological and individual CMC implementation limitations in a CFL context, suggestions and recommendations about further research and teaching practice are highlighted in the conclusion section.

Ultrahigh strength and negative thermal expansion and low thermal conductivity in graphyne nanosheets confirmed by machine-learning interatomic potentials

After several decades of experimental endeavors, most recently large-area γ-graphyne layered materials have been synthesized via a reversible dynamic alkyne metathesis approach (Nature Synthesis (2022) 1, 449–454). Motivated by the aforementioned accomplishment and highly appealing physics of the nanoporous sp–sp2-hybridized carbon allotropes, herein we explore the thermal and mechanical properties of six different graphyne lattices, via machine-learning interatomic potentials (MLIPs). To this aim, by employing a computationally efficient passive-training approach, the thermal and mechanical properties are evaluated with ab-initio level of accuracy using the classical molecular dynamics simulations. Analysis of mechanical properties at room temperature reveal that graphyne nanosheets depending on the atomic structure and loading direction can show remarkably high ultimate tensile strengths up to around 90 GPa. The graphyne nanomembranes are however predicted to show by around two orders of magnitude suppressed lattice thermal conductivity than graphene. Graphyne nanoporous networks are also predicted to show ultrahigh negative thermal expansion coefficients, one order of magnitude higher than that of the graphene. The presented MLIP-based results provide a critical vision on the structure and thermo-mechanical property relationships in sp–sp2-hybridized graphyne allotropes, which can be useful for the design of novel nanodevices using this important class of nanomaterials.

Multireference Generalization of the Weighted Thermodynamic Perturbation Method.

We describe the generalized weighted thermodynamic perturbation (gwTP) method for estimating the free energy surface of an expensive "high-level" potential energy function from the umbrella sampling performed with multiple inexpensive "low-level" reference potentials. The gwTP method is a generalization of the weighted thermodynamic perturbation (wTP) method developed by Li and co-workers [J. Chem. Theory Comput. 2018, 14, 5583-5596] that uses a single "low-level" reference potential. The gwTP method offers new possibilities in model design whereby the sampling generated from several low-level potentials may be combined (e.g., specific reaction parameter models that might have variable accuracy at different stages of a multistep reaction). The gwTP method is especially well suited for use with machine learning potentials (MLPs) that are trained against computationally expensive ab initio quantum mechanical/molecular mechanical (QM/MM) energies and forces using active learning procedures that naturally produce multiple distinct neural network potentials. Simulations can be performed with greater sampling using the fast MLPs and then corrected to the ab initio level using gwTP. The capabilities of the gwTP method are demonstrated by creating reference potentials based on the MNDO/d and DFTB2/MIO semiempirical models supplemented with the "range-corrected deep potential" (DPRc). The DPRc parameters are trained to ab initio QM/MM data, and the potentials are used to calculate the free energy surface of stepwise mechanisms for nonenzymatic RNA 2'-O-transesterification model reactions. The extended sampling made possible by the reference potentials allows one to identify unequilibrated portions of the simulations that are not always evident from the short time scale commonly used with ab initio QM/MM potentials. We show that the reference potential approach can yield more accurate ab initio free energy predictions than the wTP method or what can be reasonably afforded from explicit ab initio QM/MM sampling.

Computational discovery of new modifications in scandium oxychloride (ScOCl) using a multi‐methodological approach

AbstractScandium oxychloride (ScOCl) has recently become of interest as an advanced material with possible applications in solid oxide fuel cells, photocatalysis, and electronic devices, as are oxyhalides of various transition metals. In the present study, crystal structure prediction has been utilized to fully investigate the energy landscape of ScOCl. A multi‐methodological approach has been used consisting of a combination of two search methods, where the final structure optimization has been performed on ab initio level using DFT‐LDA and hybrid PBE0 functionals. The experimentally observed α‐ScOCl phase has been found as well as several additional structure candidates at high pressures and/or temperatures. A successful synthesis of these novel ScOCl modifications would have the potential for extending the scientific, technological and industrial applications of ScOCl.

Ab initio computations of BaZrO3, CaTiO3, SrTiO3 perovskite as well as WO3 and ReO3 (001) surfaces

We computed, at the ab initio level, BaZrO3, CaTiO3, SrTiO3 as well as WO3 and ReO3 (001) surfaces and analyzed systematic tendencies therein. As obtained by our ab initio hybrid DFT-HF computations, at BO2-terminated (001) surfaces of investigated ABO3 perovskites as well as WO3 and ReO3 oxides, all top-layer ions shift in the direction of the crystal bulk. The single-deviation from this tendency is upward shift of the WO2-terminated WO3 (001) surface top layer O ion by the magnitude of +0.42% of the bulk lattice constant a0. In contrary, all second layer ions, with the single exception of ReO2-terminated ReO3 (001) surface O ion, shifts upwards. Our computed BO2-terminated SrTiO3, CaTiO3, BaZrO3, WO3 and ReO3 (001) surface Γ–Γ band gaps always are smaller than their respective bulk Γ–Γ band gaps. The B–O ion chemical bond populations in the SrTiO3, CaTiO3 and BaZrO3 perovskite bulk are always smaller than at their nearby BO2-terminated (001) surfaces. On the contrary, the W–O and Re–O ion chemical bond populations in the WO3 (0.142e) and ReO3 (0.212e) bulk are slightly larger than at nearby the WO2- and ReO2-terminated WO3 and ReO3 (001) surfaces (0.108e and 0.170e). Nonetheless, the W–O and Re–O chemical bond populations between the W and Re ions located in the upper layer and the O ions located in the second layer of the WO2- and ReO2-terminated (001) surfaces (0.278e and 0.262e) are the absolutely largest bond populations in the WO3 and ReO3 crystals.

Systematic electronic structure in the cuprate parent state from quantum many-body simulations.

The quantitative description of correlated electron materials remains a modern computational challenge. We demonstrate a numerical strategy to simulate correlated materials at the fully ab initio level beyond the solution of effective low-energy models and apply it to gain a detailed microscopic understanding across a family of cuprate superconducting materials in their parent undoped states. We uncover microscopic trends in the electron correlations and reveal the link between the material composition and magnetic energy scales through a many-body picture of excitation processes involving the buffer layers. Our work illustrates a path toward a quantitative and reliable understanding of more complex states of correlated materials at the ab initio many-body level.

An examination of the reaction pathways of XO + O → X + O2 (X = Br and I)

Kinetics and mechanism of potentially important atmospheric ozone depletion reactions XO + O → X + O2 (X = Br and I) have been explored at the ab initio level. Several minimum energy geometries and transition states are identified at the MP2 level using correlation consistent triple zeta and effective core potential basis sets and energetics are obtained at the QCISD(T)//MP2 level of theory. Possible reaction pathways are discussed on the basis of IRC calculations and changes of geometries along the reaction paths. A direct reaction mechanism as well as reaction path via transition states and equilibrium geometries are identified. For both the reactions, early transition states have been detected just after the reactions start. In case of BrO + O reaction, we obtained a transition state of Br.OO type before the product formation, whereas in case of IO + O reaction, an equilibrium geometry of I.OO type has been detected leading to the product formation. Similar to I.OO, for ClO + O reaction an equilibrium geometry of Cl.OO type was reported in literature for product formation. This anomaly for TS-Br.OO may be due the artifact of MP2 optimization method. A multi-reference approach is expected to reveal the correct picture. A detailed dynamical study of this transition state may lead to clear bond-breaking and bond-forming information, which may be helpful to predict the true reaction pathway. Heats of reaction are found to be consistent with experimental data. Bond dissociation energies of the ground state intermediate isomers to various dissociation asymptotes are also reported. This is the first theoretical report for the possible reaction pathways and may be served as a reference for future investigation using higher methodology.

Ro-vibrational levels and their (e-f) splitting of acetylene molecule calculated from new potential energy surfaces

Ro-vibrational energy levels of acetylene are reported using variational nuclear motion calculations from new ab initio and empirically optimized full six-dimensional potential energy surfaces in the ground electronic state of the acetylene molecule. The calculations account for the triple, quadruple and quintuple excitations as well as relativistic and diagonal Born-Oppenheimer corrections. Variational nuclear motion calculations were performed using the exact kinetic energy operator in orthogonal coordinates. The convergence of energy levels calculations versus the size of the vibrational basis set functions was verified. Our best ab initio potential energy surface that includes the above-mentioned contributions provides the RMS (obs.-calc.) errors of 0.95 cm−1 for five fundamental energy levels. The largest contribution to the RMS error is caused primarily by a significant deviation of the ν4 fundamental frequency. Experimental values of 120 vibrational band origins were used to empirically adjust few lower-order parameters of the potential energy surface. The average error drops down to 0.45 cm−1 or 0.25 cm−1 for empirically optimized potential energy function with two or seven adjusted parameters corresponding to quadratic force field terms and one third order term. The splitting of (e – f) rovibrational doublets and their J dependence were calculated with high accuracy due to the full account of Coriolis interactions. Computed (e – f) splittings allow one to check the correctness of the assignment of empirical energy levels. The estimation of the accuracy for the calculated vibrational levels in an extended range up to 9500 cm−1 shows that the set of ab initio vibrational levels can be used for future assignments of empirically not observed ro-vibrational energy levels. The comparison of the calculated and experimental ro-vibrational energy levels of the C2D2 and 13C2H2 isotopologues is also reported.

Low and Anisotropic Tensile Strength and Thermal Conductivity in the Single-Layer Fullerene Network Predicted by Machine-Learning Interatomic Potentials

In the latest ground-breaking experimental advancement (Nature (2022), 606, 507), zero-dimensional fullerenes (C60) have been covalently bonded to form single-layer two-dimensional (2D) fullerene network, namely quasi-hexagonal-phase fullerene (qHPC60). Motivated by the aforementioned accomplishment, in this communication, for the first time, we explore the phononic and mechanical properties of the qHPC60 monolayer, employing state-of-the-art machine-learning interatomic potentials. By employing an efficient passive-training methodology, the thermal and mechanical properties were examined with an ab-initio level of accuracy using the classical molecular dynamics simulations. Predicted phonon dispersion confirmed the desirable dynamical stability of the qHPC60 monolayer. Room temperature lattice thermal conductivity is predicted to be ultralow and around 2.9 (5.7) W/m·K along the x(y) directions, which are by three orders of magnitude lower than that of the graphene. Close to the ground state and at room temperature, the ultimate tensile strength of the qHPC60 monolayer along the x(y) directions is predicted to be 7.0 (8.8) and 3.3 (4.2) GPa, respectively, occurring at corresponding strains of around 0.07 and 0.029, respectively. The presented computationally accelerated first-principles results confirm highly anisotropic and remarkably low tensile strength and phononic thermal conductivity of the qHPC60 fullerene network nanosheets.

Beryllium ion coordination in Ammonia, methanol and water solvents

• Be is a key component of materials indispensable in today’s industries and its solvation behavior is a topic of interest. • The study highlight the coordination behavior of beryllium ion with water, ammonia and methanol solvents. • Fitting procedure to obtain Binding energy convergence. • Temperature effects on the isomeric distribution for each cluster size. • MP2 method as reliable method to describe the solvation process around cations. The solvation of B e 2 + [ M g N H 3 n = 1 - 10 ] 2 + cation in ammonia, methanol and water has been studied at Ab initio MP2 level using cluster models in which the solvent molecules have been distributed between the first and second solvation shells. In all cases, the first solvation sphere results to be saturated with four solvent molecules in a tetrahedral arrangement. The second shell contains instead up to 8,12 and 16 ligands in the case of methanol, water and ammonia, respectively. Solvent molecules in the second solvation shell serve to stabilizes the structures through the formation of a number of hydrogen bonds and improves the agreement with the available experimental data. From obtained distances values it can be deduced that beryllium ion establishes with the solvent molecules, inside the first coordination shell, bonds of covalent nature (less than1.8Å) which are longer than those with the magnesium ion. Using a fitting procedure, binding energy values of 29.2, 46.9 and 68.6 kcal/mol, for ammonia, water and methanol clusters, have been obtained, respectively. The clustering enthalpies and free energies have been also evaluated. Temperature effects on the isomeric distribution for each cluster and for all considered solvents, have been calculated in the range of 25–40 K and results show that only the tetracoordinated systems are populate.

The Electrostatic Gating of Carbon Nanotube Field-Effect Biosensors Characterized at the Molecular Scale Using Simulations

Carbon nanotube field-effect biosensors (CNT-bioFETs) are ultraminiaturized devices that can be used to measure single-molecule kinetics of biomolecules on time scales going from a few microseconds to several minutes, as demonstrated for nucleic acid hybridization [1] and folding [2] as well as for enzyme function [3]. Experiments indicate that the sensitivity of CNT-bioFETs originates from the interplay between the nanotube’s conductance, which is monitored by the device, and the electrostatic potential generated by the biomolecule under investigation, which is localized on the nanotube [4,5]. The measured conductance exhibits characteristic transitions between two levels (or more) as a function of time, as the biomolecule folds or performs its function. Yet, the origin of this electrostatic gating of the carbon nanotube by a single biomolecule is not well understood at the molecular scale.To bridge this gap, we employ molecular dynamics (MD) and Hamiltonian replica exchange (HREX) simulations to unveil: (1) the interactions between the biomolecule and the nanotube to which it is attached in the device and (2) the electrostatic potential on the nanotube as the state of the biomolecule changes. We address these questions by considering three prototypical cases: the function of the Lysozyme protein, the hybridization of 10-nt DNA sequence and the folding of a DNA G-quadruplex, which were previously characterized using CNT-bioFETs [1-5].Our simulations show that the lysozyme, the 10-nt DNA sequence and the DNA G-quadruplex interact differently with the nanotube to which they are attached. Consequently, the electrostatic potential (ESP) that they generate on the nanotube is very sensitive to the type and state of the biomolecule. When compared to experiment, the ESP distribution for the with-ligand and without-ligand states of the Lysozyme protein are in line with the measured two-level conductance by CNT-bioFETs. For the DNAs, however, the ESP distribution for their different states does not agree with the measured two-level conductance. Experiments imply that the DNA strand is not interacting with the nanotube, which is not what our simulations suggest. The reason for this apparent conflict could arise from the impact of the external electric field imposed by the gate electrode in CNT-bioFETs on highly charged systems such as DNAs, as supported by our recent simulations.The significance of this work is twofold. First, it contributes to a better understanding of the inner working of carbon nanotube field-effect biosensors, which is crucially needed to support the development of these promising devices in the lab. Second, it provides the structural ensemble of the biomolecules and their interactions with the nanotube in these devices, which can serve as a starting point for a finer characterization of their effect on the carbon nanotube’s conductance at the ab initio level.[1] S. Sorgenfrei et al. Nat Nanotechnol, 2011, 6, 126-132.[2] D. Bouilly et al. Nano Lett, 2016, 16, 4679-4685.[3] Y. Choi et al. Science, 2012, 335, 319-324.[4] S. Sorgenfrei et al. Nano Lett, 2011, 11, 3739-3743.[5] Y. Choi et al. Nano Lett, 2013, 13, 625-631.

Ultrafast charge transfer coupled to quantum proton motion at molecule/metal oxide interface.

Understanding how the nuclear quantum effects (NQEs) in the hydrogen bond (H-bond) network influence the photoexcited charge transfer at semiconductor/molecule interface is a challenging problem. By combining two kinds of emerging molecular dynamics methods at the ab initio level, the path integral-based molecular dynamics and time-dependent nonadiabatic molecular dynamics, and choosing CH3OH/TiO2 as a prototypical system to study, we find that the quantum proton motion in the H-bond network is strongly coupled with the ultrafast photoexcited charge dynamics at the interface. The hole trapping ability of the adsorbed methanol molecule is notably enhanced by the NQEs, and thus, it behaves as a hole scavenger on titanium dioxide. The critical role of the H-bond network is confirmed by in situ scanning tunneling microscope measurements with ultraviolet light illumination. It is concluded the quantum proton motion in the H-bond network plays a critical role in influencing the energy conversion efficiency based on photoexcitation.

Ultrafast photo-induced processes in complex environments: The role of accuracy in excited-state energy potentials and initial conditions

Light induces non-equilibrium time evolving molecular phenomena. The computational modeling of photo-induced processes in large systems, embedded in complex environments (i.e., solutions, proteins, materials), demands for a quantum and statistical mechanic treatment to achieve the required accuracy in the description of both the excited-state energy potentials and the choice of the initial conditions for dynamical simulations. On the other hand, the theoretical investigation on the atomistic scale of times and sizes of the ultrafast photo-induced reactivity and non-equilibrium relaxation dynamics right upon excitation requests tailored computational protocols. These methods often exploit hierarchic computation schemes, where a large part of the degrees of freedom are required to be treated explicitly to achieve the right accuracy. Additionally, part of the explicit system needs to be treated at ab initio level, where density functional theory, using hybrid functionals, represents a good compromise between accuracy and computational cost, when proton transfers, non-covalent interactions, and hydrogen bond dynamics play important roles. Thus, the modeling strategies presented in this review stress the importance of hierarchical quantum/molecular mechanics with effective non-periodic boundary conditions and efficient phase-sampling schemes to achieve chemical accuracy in ultrafast time-resolved spectroscopy and photo-induced phenomena. These approaches can allow explicit and accurate treatment of molecule/environment interactions, including also the electrostatic and dispersion forces of the bulk. At the same time, the specificities of the different case studies of photo-induced phenomena in solutions and biological environments are highlighted and discussed, with special attention to the computational and modeling challenges.

Exploring Complex Reaction Networks Using Neural Network-Based Molecular Dynamics Simulation.

Ab initio molecular dynamics (AIMD) is an established method for revealing the reactive dynamics of complex systems. However, the high computational cost of AIMD restricts the explorable length and time scales. Here, we develop a fundamentally different approach using molecular dynamics simulations powered by a neural network potential to investigate complex reaction networks. This potential is trained via a workflow combining AIMD and interactive molecular dynamics in virtual reality to accelerate the sampling of rare reactive processes. A panoramic visualization of the complex reaction networks for decomposition of a novel high explosive (ICM-102) is achieved without any predefined reaction coordinates. The study leads to the discovery of new pathways that would be difficult to uncover if established methods were employed. These results highlight the power of neural network-based molecular dynamics simulations in exploring complex reaction mechanisms under extreme conditions at the ab initio level, pushing the limit of theoretical and computational chemistry toward the realism and fidelity of experiments.

(3-(4-klorofenil)-4,5-dihidroizoksazol-4,5-diil)dimetanol Bileşiği: Antibakteriyel Aktivite, Antifungal Aktivite ve Hesaplanmış Yapısal Parametreler

We intended to quantify the antibacterial and antifungal activity results of 4,5-dihydroisoxazole dimethanol compound (1a) against several bacteria and fungi and also calculate some structural parameters (theoretical descriptors) of compound (1a) with this work. Microdilution broth procedures were studied using microdilution wells for the minimal inhibitory concentrations (MICs) test. Compound (1a) exhibited fair activities against all the bacteria and fungi. Compound (1a) has been a good result (MIC = 50 µg/ml) against particularly P. aeruginosa. The structure of compound (1a) was drawn, and geometrical optimization was done using the Ab initio (RHF/3-21G) level.

Chemistry without the Born-Oppenheimer approximation.

Chemistry without the Born-Oppenheimer approximation.

Excited electron and spin dynamics in topological insulator: A perspective from ab initio non-adiabatic molecular dynamics

We perform an ab initio non-adiabatic molecular dynamics simulation to investigate the non-equilibrium spin and electron dynamics in a prototypical topological insulator (TI) Bi2Se3. Different from the ground state, we reveal that backscattering can happen in an oscillating manner between time-reversal pair topological surface states (TSSs) in the non-equilibrium dynamics. Analysis shows the phonon excitation induces orbital composition change by electron-phonon interaction, which further stimulates spin canting through spin-orbit coupling. The spin canting of time-reversal pair TSSs leads to the non-zero non-adiabatic coupling between them and then issues in backscattering. Both the spin canting and backscattering result in ultrafast spin relaxation with a timescale around 100 fs. This study provides critical insights into the non-equilibrium electron and spin dynamics in TI at the ab initio level and paves a way for the design of ultrafast spintronic materials.

Stable Carbenes as Structural Components of Partially Saturated Sulfur-Containing Heterocycles.

Recently, an unusual elongation of the C-S bond was observed experimentally for some sulfur-containing heterocycles. Using a superior ab initio (SCS-MP2/cc-pVTZ) level of theory, we showed that the phenomenon can be explained by a contribution of a donor–acceptor adduct of a carbene with an unsaturated ligand. One may achieve further elongation of the C-S bond, eventually turning it to a coordinate one, by increasing the stability of each part of the system as, e.g., in the utmost case of spiro adducts with Arduengo carbenes. The effect of carbene stability was quantified by employing the isodesmic reactions of carbene exchange.

Pressure-induced dimerization and collapse of antiferromagnetism in the Kitaev material α−Li2IrO3

We present magnetization measurements carried out on polycrystalline and single-crystalline samples of $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ under hydrostatic pressures up to 2 GPa and establish the temperature-pressure phase diagram of this material. The N\'eel temperature (${T}_{\mathrm{N}}$) of $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ is slightly enhanced upon compression with $d{T}_{\mathrm{N}}/dp$ = 1.5 K/GPa. Above 1.2 GPa, $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ undergoes a first-order phase transition toward a nonmagnetic dimerized phase, with no traces of the magnetic phase observed above 1.8 GPa at low temperatures. The critical pressure of the structural dimerization is strongly temperature dependent. This temperature dependence is well reproduced on the ab initio level by taking into account lower phonon entropy in the nonmagnetic phase. We further show that the initial increase in ${T}_{\mathrm{N}}$ of the magnetic phase is due to a weakening of the Kitaev interaction $K$ along with the enhancement of the Heisenberg term $J$ and off-diagonal anisotropy $\mathrm{\ensuremath{\Gamma}}$. Our study reveals a common thread in the interplay of magnetism and dimerization in pressured Kitaev materials.