This study uses density functional theory (DFT) based calculations to understand the water oxidation process using a copper–porphyrin complex. Three possible reaction pathways (mechanisms) are explored. Through a series of steps involving the proton‐coupled electron transfers (PCETs), the complex changes its oxidation state from II to IV, forming high‐valent copper–oxo species ([LCu IV = O], L = porphyrin). The metal oxo species then allows another water molecule to attack, eventually forming an oxygen–oxygen (O─O) bond – the important step in oxygen generation. In general, the rest of the electrocatalysis mechanism involves the formation of a peroxo linkage, followed by oxidation to molecular oxygen (O═O). The key differences in Mechanisms I‐III involve the formation of [LCu IV = O]. In Mechanism I, [LCu IV = OH] + is formed at E = 1.26 V vs. SHE, followed by deprotonation. In Mechanism II, the formation of [LCu IV = O] involves PCET from the [LCu III ‐OH] at E = 1.71 V vs. SHE, and the rest of the steps remain the same. In Mechanism III, [LCu III ‐OH] is directly formed from [LCu II = OH 2 ] via PCET at E = 1.56 V. It should be noted that the bottleneck involves the formation of high‐valent copper oxo species.
本研究使用基于密度泛函理论（DFT）的计算来理解使用铜-卟啉络合物的水氧化过程。探讨了三种可能的反应途径（机制）。通过一系列涉及质子耦合电子转移（PCETs）的步骤，配合物将其氧化态从II变为IV，形成高价铜氧（[LCu IV = O], L =卟啉）。然后，金属氧允许另一个水分子攻击，最终形成氧-氧（O─O）键——这是氧气生成的重要步骤。一般来说，电催化机制的其余部分包括形成过氧键，然后氧化成分子氧（O = O）。机制I - III的关键差异涉及[LCu IV = O]的形成。在机制1中，[LCu IV = OH] +在E = 1.26 V vs. SHE下形成，然后进行去质子化。在机制II中，[LCu IV = O]在E = 1.71 V vs. SHE下由[LCu III‐OH]形成PCET，其余步骤保持不变。在机制III中，[LCu II = OH 2]在E = 1.56 V下经PCET直接生成[LCu III‐OH]。应该指出的是，瓶颈涉及到高价铜氧的形成。
{"title":"Computational Investigation on the Mechanism of Electrocatalytic Water Oxidation by Copper(II) Porphyrin","authors":"Shanti Gopal Patra, Chhanda Paul, Aritra Saha, Pratim Kumar Chattaraj","doi":"10.1002/adts.202501442","DOIUrl":"https://doi.org/10.1002/adts.202501442","url":null,"abstract":"This study uses density functional theory (DFT) based calculations to understand the water oxidation process using a copper–porphyrin complex. Three possible reaction pathways (mechanisms) are explored. Through a series of steps involving the proton‐coupled electron transfers (PCETs), the complex changes its oxidation state from II to IV, forming high‐valent copper–oxo species ([LCu <jats:sup>IV</jats:sup> = O], L = porphyrin). The metal oxo species then allows another water molecule to attack, eventually forming an oxygen–oxygen (O─O) bond – the important step in oxygen generation. In general, the rest of the electrocatalysis mechanism involves the formation of a peroxo linkage, followed by oxidation to molecular oxygen (O═O). The key differences in Mechanisms I‐III involve the formation of [LCu <jats:sup>IV</jats:sup> = O]. In Mechanism I, [LCu <jats:sup>IV</jats:sup> = OH] <jats:sup>+</jats:sup> is formed at <jats:italic>E</jats:italic> = 1.26 V vs. SHE, followed by deprotonation. In Mechanism II, the formation of [LCu <jats:sup>IV</jats:sup> = O] involves PCET from the [LCu <jats:sup>III</jats:sup> ‐OH] at <jats:italic>E</jats:italic> = 1.71 V vs. SHE, and the rest of the steps remain the same. In Mechanism III, [LCu <jats:sup>III</jats:sup> ‐OH] is directly formed from [LCu <jats:sup>II</jats:sup> = OH <jats:sub>2</jats:sub> ] via PCET at <jats:italic>E</jats:italic> = 1.56 V. It should be noted that the bottleneck involves the formation of high‐valent copper oxo species.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"168 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145582906","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Parkinson's disease (PD) is a progressive neurodegenerative disorder marked by the pathological aggregation of α‐synuclein (α‐syn) and the degeneration of dopaminergic neurons. The interaction between α‐syn and 14‐3‐3ζ has been implicated in modulating α‐syn's stability, localization, and aggregation behavior, rendering it a promising target for therapeutic intervention. In this study, we employed a comprehensive computational pipeline to identify small‐molecule inhibitors capable of disrupting the 14‐3‐3ζ/α‐syn interaction. Structure‐ and ligand‐based virtual screening, followed by toxicity filtering and molecular dynamics simulations, led to the identification of Var84 (orthosteric, ORT) and DB11581 (allosteric, ALO) as candidate inhibitors. A dual‐site inhibition (DUO) approach involving simultaneous binding of both ligands is also investigated. Absolute binding free energy (ABFE) and residence time (RAMD) analyses revealed cooperative binding effects: ALO maintained strong binding across systems, while ORT binding weakened in the DUO system, likely due to increased inter‐protein separation. UMAP clustering and secondary structure analysis indicated that the DUO system preserved helical α‐syn conformations while reducing aggregation‐prone β‐structures. Additionally, supervised machine learning models trained on inter‐protein contact features identified key residue pairs perturbed by ligand binding, corroborating findings from communication network analyses, thereby offering mechanistic insight and a transferable framework for targeting PPIs in neurodegenerative diseases.
{"title":"Dual Allosteric and Orthosteric Inhibition of 14‐3‐3ζ–α‐Synuclein Interaction: A Multiscale Simulation and Machine Learning Approach","authors":"Gourav Chakraborty, Aditi Chaudhary, Niladri Patra","doi":"10.1002/adts.202501455","DOIUrl":"https://doi.org/10.1002/adts.202501455","url":null,"abstract":"Parkinson's disease (PD) is a progressive neurodegenerative disorder marked by the pathological aggregation of α‐synuclein (α‐syn) and the degeneration of dopaminergic neurons. The interaction between α‐syn and 14‐3‐3ζ has been implicated in modulating α‐syn's stability, localization, and aggregation behavior, rendering it a promising target for therapeutic intervention. In this study, we employed a comprehensive computational pipeline to identify small‐molecule inhibitors capable of disrupting the 14‐3‐3ζ/α‐syn interaction. Structure‐ and ligand‐based virtual screening, followed by toxicity filtering and molecular dynamics simulations, led to the identification of Var84 (orthosteric, ORT) and DB11581 (allosteric, ALO) as candidate inhibitors. A dual‐site inhibition (DUO) approach involving simultaneous binding of both ligands is also investigated. Absolute binding free energy (ABFE) and residence time (RAMD) analyses revealed cooperative binding effects: ALO maintained strong binding across systems, while ORT binding weakened in the DUO system, likely due to increased inter‐protein separation. UMAP clustering and secondary structure analysis indicated that the DUO system preserved helical α‐syn conformations while reducing aggregation‐prone β‐structures. Additionally, supervised machine learning models trained on inter‐protein contact features identified key residue pairs perturbed by ligand binding, corroborating findings from communication network analyses, thereby offering mechanistic insight and a transferable framework for targeting PPIs in neurodegenerative diseases.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"28 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145567140","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhaodi Yang, Yujie Jia, Yaohong Yan, Si‐Dian Li, Yuewen Mu
The study on the transport properties of borophenes is scarce, which is important for their potential applications in electronic and sensing devices. The study suggests the holes tend to suppress the conductance of borophenes in zigzag direction, though they all behave much better than graphene. Surprisingly, inserting a row of borophene into borophene will abnormally enhance the conductance up to three times under certain bias. The charge transfer between and subunits leads to the shift of bands, as a result, the Fermi level is dominated by the bands from subunit with more anisotropic Fermi surface and higher Fermi velocities. Furthermore, Fermi surface analysis suggests the bands across the interface is scarce or absent. Combined with high electrostatic potential on subunit and small fluctuation of electron transfer in subunits, quasi‐1D transport appears, accounting for the abnormal enhancement in conductance. Given many nearly degenerate allotropes for borophene, the abnormal enhancement is likely observable in other family of lateral heterostructures as well. This study not only elucidates an anomalous conductance enhancement in specific borophene heterostructures, but also proposes a way to enhance the conductance in lateral heterostructures via band tailoring.
{"title":"Abnormal Enhancement for the Conductance of Borophene Lateral Heterostructures","authors":"Zhaodi Yang, Yujie Jia, Yaohong Yan, Si‐Dian Li, Yuewen Mu","doi":"10.1002/adts.202501457","DOIUrl":"https://doi.org/10.1002/adts.202501457","url":null,"abstract":"The study on the transport properties of borophenes is scarce, which is important for their potential applications in electronic and sensing devices. The study suggests the holes tend to suppress the conductance of borophenes in zigzag direction, though they all behave much better than graphene. Surprisingly, inserting a row of borophene into borophene will abnormally enhance the conductance up to three times under certain bias. The charge transfer between and subunits leads to the shift of bands, as a result, the Fermi level is dominated by the bands from subunit with more anisotropic Fermi surface and higher Fermi velocities. Furthermore, Fermi surface analysis suggests the bands across the interface is scarce or absent. Combined with high electrostatic potential on subunit and small fluctuation of electron transfer in subunits, quasi‐1D transport appears, accounting for the abnormal enhancement in conductance. Given many nearly degenerate allotropes for borophene, the abnormal enhancement is likely observable in other family of lateral heterostructures as well. This study not only elucidates an anomalous conductance enhancement in specific borophene heterostructures, but also proposes a way to enhance the conductance in lateral heterostructures via band tailoring.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"1 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145559409","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
One of the key challenges in the large‐scale application of perovskite solar cells is stability. Researchers have found that passivation molecules play a crucial role in mitigating interface defects, thereby enhancing stability. Traditionally, the design of passivation molecules has relied on the expertise of chemists and materials scientists. In this study, we introduce a novel approach driven by a language model and dipole‐moment‐knowledge‐based strategy for passivation molecule design. Specifically, we employ the open‐source Gemma model, which is pre‐trained and fine‐tuned on the PubChem and QM9 datasets. This fine‐tuning enables Gemma to generate passivation molecules with higher dipole moments. Further density functional theory (DFT) validation reveals that molecules designed by Gemma improve the stability of perovskite structures with surface defects by approximately 27.75%. Additionally, electronic density of states and charge distribution analysis further support these findings. This study highlights the potential of language models in the design of next‐generation photovoltaic device materials, particularly in passivation molecule development.
{"title":"Dipole‐Moment‐Knowledge‐Guided Molecular Design for Perovskite Surface Passivation: A Gemma‐Language‐Model and DFT‐Driven Framework","authors":"Tianhui Jiang, Yifeng Gao, Guozhen Liu, Guoxiang Zhao, Junjie Hu, Rongjian Sa, Peng Gao","doi":"10.1002/adts.202501318","DOIUrl":"https://doi.org/10.1002/adts.202501318","url":null,"abstract":"One of the key challenges in the large‐scale application of perovskite solar cells is stability. Researchers have found that passivation molecules play a crucial role in mitigating interface defects, thereby enhancing stability. Traditionally, the design of passivation molecules has relied on the expertise of chemists and materials scientists. In this study, we introduce a novel approach driven by a language model and dipole‐moment‐knowledge‐based strategy for passivation molecule design. Specifically, we employ the open‐source Gemma model, which is pre‐trained and fine‐tuned on the PubChem and QM9 datasets. This fine‐tuning enables Gemma to generate passivation molecules with higher dipole moments. Further density functional theory (DFT) validation reveals that molecules designed by Gemma improve the stability of perovskite structures with surface defects by approximately 27.75%. Additionally, electronic density of states and charge distribution analysis further support these findings. This study highlights the potential of language models in the design of next‐generation photovoltaic device materials, particularly in passivation molecule development.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"75 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145559563","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Natthapong Jampaiboon, Chayanon Atthapak, Thiti Bovornratanaraks, Björn Alling, Annop Ektarawong
This study presents a comprehensive first‐principles investigation of and , focusing on their thermodynamic stability and mechanical behavior. The results reveal that, at absolute zero, Hf‐rich with , is thermodynamically stable, whereas Y‐rich with and with are unstable against decomposition into relevant competing phases, i.e., solid solution and for Y‐rich and , and ‐rhombohedral B for . However, near‐stability of Y‐rich , where , with formation energies within 4 meV per atom above the Hf−Y−B convex hull implies its potential entropy‐driven thermodynamic stabilization at elevated temperatures. Both and are mechanically stable, according to the Born stability criteria, and Vegard's law is largely obeyed for their structural parameters and elastic moduli. Hf‐rich exhibits superhard behavior with a maximum Vickers hardness of 43.9 GPa at = 0.167, while that of ranges between 33 and 39 GPa and peaks at 38.2 GPa for = 0.875. The maximum Vickers hardness values of and surpass those of their constituent compounds. These findings offer fundamental insights into stabilities and mechanical performance of the − and − mixtures, providing theoretical guidance for future development of advanced metal boride‐based hard‐coating materials.
{"title":"Thermodynamic Consideration and Mechanical Behavior of Boride‐Containing Solid Solutions of Hafnium−Yttrium−Boron System Revealed by a First‐Principles Analysis","authors":"Natthapong Jampaiboon, Chayanon Atthapak, Thiti Bovornratanaraks, Björn Alling, Annop Ektarawong","doi":"10.1002/adts.202501517","DOIUrl":"https://doi.org/10.1002/adts.202501517","url":null,"abstract":"This study presents a comprehensive first‐principles investigation of and , focusing on their thermodynamic stability and mechanical behavior. The results reveal that, at absolute zero, Hf‐rich with , is thermodynamically stable, whereas Y‐rich with and with are unstable against decomposition into relevant competing phases, i.e., solid solution and for Y‐rich and , and ‐rhombohedral B for . However, near‐stability of Y‐rich , where , with formation energies within 4 meV per atom above the Hf−Y−B convex hull implies its potential entropy‐driven thermodynamic stabilization at elevated temperatures. Both and are mechanically stable, according to the Born stability criteria, and Vegard's law is largely obeyed for their structural parameters and elastic moduli. Hf‐rich exhibits superhard behavior with a maximum Vickers hardness of 43.9 GPa at = 0.167, while that of ranges between 33 and 39 GPa and peaks at 38.2 GPa for = 0.875. The maximum Vickers hardness values of and surpass those of their constituent compounds. These findings offer fundamental insights into stabilities and mechanical performance of the − and − mixtures, providing theoretical guidance for future development of advanced metal boride‐based hard‐coating materials.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"28 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145535429","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Technology Computer-Aided Design (TCAD) modeling is a vital tool for the design of complex optoelectronic devices such as III-V multijunction solar cells. In this work, Bayesian optimization is proposed as a robust framework that is able to tackle difficulties that arise in the optimization of expensive to evaluate black-box functions, such as TCAD solvers. This method is applied to a lattice-matched GaInP/Ga(In)As/Ge triple junction solar cell, which incorporates a distributed Bragg reflector for space applications. The results show a path to increase the efficiency of current commercial space triple junction solar cells.
{"title":"Using Bayesian Optimization to Increase the Efficiency of III-V Multijunction Solar Cells","authors":"Pablo F. Palacios, Carlos Algora","doi":"10.1002/adts.202500821","DOIUrl":"https://doi.org/10.1002/adts.202500821","url":null,"abstract":"Technology Computer-Aided Design (TCAD) modeling is a vital tool for the design of complex optoelectronic devices such as III-V multijunction solar cells. In this work, Bayesian optimization is proposed as a robust framework that is able to tackle difficulties that arise in the optimization of expensive to evaluate black-box functions, such as TCAD solvers. This method is applied to a lattice-matched GaInP/Ga(In)As/Ge triple junction solar cell, which incorporates a distributed Bragg reflector for space applications. The results show a path to increase the efficiency of current commercial space triple junction solar cells.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"127 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145531882","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The proposed perovskite device structure considers several factors to realize their significance on device performance. Initially, the PCE variation between the two absorber halides is investigated, yielding a maximum PCE of 24.31% for CH3NH3SnBr3 and 27.37% for CH3NH3SnI3. Additionally, the SCAPS‐1D simulation assesses the contribution of distinct HTMs and ETMs. By further optimizing these layers along with diverse intrinsic parameters, the device's PCE increased from 27.37% to 40.17%. To improve predictive capabilities, a dataset of 29565 is generated utilizing the SCAPS‐1D simulator for CH3NH3SnI3‐based solar cells. Data preprocessing in Python applied leakage‐safe Pearson correlation filtering: within each highly collinear group (|r| ≥ 0.90), one representative predictor is retained and the remainder are excluded to reduce multicollinearity and improve interpretability. Six machine learning models are tested, and Random Forest is validated to be the most credible performer with an R2 of 96% and an RMSE of 0.210. The optimized configuration — FTO/WS 2 (ETL)/CH 3 NH 3 SnI 3 (absorber)/V 2 O 5 (HTL)/Pt (back contact) — achieves a record simulated efficiency of 40.17%, surpassing prior reports. This performance is attributed to WS 2 ’s favorable band alignment, CH 3 NH 3 SnI 3 ’s strong absorption, and V 2 O 5 ’s stability. The combined SCAPS–ML framework not only accelerates optimization but also provides actionable design rules for environmentally sustainable, lead‐free PSCs.
{"title":"Optimization of Lead‐Free Perovskite Solar Cell Architecture Using Machine Learning and Numerical Simulations","authors":"Md. Arifur Rahman, Mohammad Jahangir Alam","doi":"10.1002/adts.202501590","DOIUrl":"https://doi.org/10.1002/adts.202501590","url":null,"abstract":"The proposed perovskite device structure considers several factors to realize their significance on device performance. Initially, the PCE variation between the two absorber halides is investigated, yielding a maximum PCE of 24.31% for CH3NH3SnBr3 and 27.37% for CH3NH3SnI3. Additionally, the SCAPS‐1D simulation assesses the contribution of distinct HTMs and ETMs. By further optimizing these layers along with diverse intrinsic parameters, the device's PCE increased from 27.37% to 40.17%. To improve predictive capabilities, a dataset of 29565 is generated utilizing the SCAPS‐1D simulator for CH3NH3SnI3‐based solar cells. Data preprocessing in Python applied leakage‐safe Pearson correlation filtering: within each highly collinear group (|r| ≥ 0.90), one representative predictor is retained and the remainder are excluded to reduce multicollinearity and improve interpretability. Six machine learning models are tested, and Random Forest is validated to be the most credible performer with an R2 of 96% and an RMSE of 0.210. The optimized configuration — FTO/WS <jats:sub>2</jats:sub> (ETL)/CH <jats:sub>3</jats:sub> NH <jats:sub>3</jats:sub> SnI <jats:sub>3</jats:sub> (absorber)/V <jats:sub>2</jats:sub> O <jats:sub>5</jats:sub> (HTL)/Pt (back contact) — achieves a record simulated efficiency of 40.17%, surpassing prior reports. This performance is attributed to WS <jats:sub>2</jats:sub> ’s favorable band alignment, CH <jats:sub>3</jats:sub> NH <jats:sub>3</jats:sub> SnI <jats:sub>3</jats:sub> ’s strong absorption, and V <jats:sub>2</jats:sub> O <jats:sub>5</jats:sub> ’s stability. The combined SCAPS–ML framework not only accelerates optimization but also provides actionable design rules for environmentally sustainable, lead‐free PSCs.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"171 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145509681","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chandon Sarker, Sushmita Sadhu Pakhi, M. N. H. Liton, M. R. Islam, Mst. H. Khatun, Mohammad Kamal Hossain, M. Shahjahan, Arpon Chakraborty
This study compiles the structural, mechanical, bonding, and dynamical characteristics of the recently synthesized rare earth metallic compounds MC 2 B 2 (M = Lu, La) by means of density functional theory (DFT). Both LuC 2 B 2 and LaC 2 B 2 crystallize in tetragonal symmetry. The negative cohesive energy of LuC 2 B 2 (−7.824 eV atom −1 ) and LaC 2 B 2 (−7.692 eV atom −1 ) ensured the stability of both compounds. The compounds exhibit mechanical stability with significant elastic anisotropy, ductility, and high hardness (22.84 and 21.84 GPa for LuC 2 B 2 and LaC 2 B 2 , respectively). The electronic band structures and density of states (DOS) indicate metallic behavior, predominantly influenced by Lu/La‐5d, B‐2p, and C‐2p states, showing mixed bonding characteristics with ionic and covalent contributions. Both compounds are hard and brittle in nature. Possessing a high melting point (2183.06 K for LuC 2 B 2 and 1873.82 K for LaC 2 B 2 ), the compounds are suitable for applications in thermally harsh conditions. Through Drude‐like low‐energy behavior, optical properties also confirmed metallic nature and showed significant reflection and absorption with a specific directional dependence, especially LuC 2 B 2 shows exceptional reflectivity (≈80%) in the infrared (IR) to lower upper ultraviolet (UV) regions. The findings collectively demonstrate that LuC 2 B 2 and LaC 2 B 2 are viable options for cutting‐edge technological applications that demand superior optoelectronic, thermophysical, and mechanical performance.
{"title":"Exploring the Multifunctional Properties of MC 2 B 2 (M = Lu, La) Structures Using Density Functional Theory","authors":"Chandon Sarker, Sushmita Sadhu Pakhi, M. N. H. Liton, M. R. Islam, Mst. H. Khatun, Mohammad Kamal Hossain, M. Shahjahan, Arpon Chakraborty","doi":"10.1002/adts.202501440","DOIUrl":"https://doi.org/10.1002/adts.202501440","url":null,"abstract":"This study compiles the structural, mechanical, bonding, and dynamical characteristics of the recently synthesized rare earth metallic compounds MC <jats:sub>2</jats:sub> B <jats:sub>2</jats:sub> (M = Lu, La) by means of density functional theory (DFT). Both LuC <jats:sub>2</jats:sub> B <jats:sub>2</jats:sub> and LaC <jats:sub>2</jats:sub> B <jats:sub>2</jats:sub> crystallize in tetragonal symmetry. The negative cohesive energy of LuC <jats:sub>2</jats:sub> B <jats:sub>2</jats:sub> (−7.824 eV atom <jats:sup>−1</jats:sup> ) and LaC <jats:sub>2</jats:sub> B <jats:sub>2</jats:sub> (−7.692 eV atom <jats:sup>−1</jats:sup> ) ensured the stability of both compounds. The compounds exhibit mechanical stability with significant elastic anisotropy, ductility, and high hardness (22.84 and 21.84 GPa for LuC <jats:sub>2</jats:sub> B <jats:sub>2</jats:sub> and LaC <jats:sub>2</jats:sub> B <jats:sub>2</jats:sub> , respectively). The electronic band structures and density of states (DOS) indicate metallic behavior, predominantly influenced by Lu/La‐5d, B‐2p, and C‐2p states, showing mixed bonding characteristics with ionic and covalent contributions. Both compounds are hard and brittle in nature. Possessing a high melting point (2183.06 K for LuC <jats:sub>2</jats:sub> B <jats:sub>2</jats:sub> and 1873.82 K for LaC <jats:sub>2</jats:sub> B <jats:sub>2</jats:sub> ), the compounds are suitable for applications in thermally harsh conditions. Through Drude‐like low‐energy behavior, optical properties also confirmed metallic nature and showed significant reflection and absorption with a specific directional dependence, especially LuC <jats:sub>2</jats:sub> B <jats:sub>2</jats:sub> shows exceptional reflectivity (≈80%) in the infrared (IR) to lower upper ultraviolet (UV) regions. The findings collectively demonstrate that LuC <jats:sub>2</jats:sub> B <jats:sub>2</jats:sub> and LaC <jats:sub>2</jats:sub> B <jats:sub>2</jats:sub> are viable options for cutting‐edge technological applications that demand superior optoelectronic, thermophysical, and mechanical performance.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"184 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145509679","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
I. Ouadha, M. H. Elahmar, H. Rached, M. Caid, D. Rached, Y. Rached, S. Al‐Qaisi, A. Boutramine, N. Hacini
MAX phases, which combine metallic and ceramic characteristics, are promising candidates for operation in extreme environments owing to their exceptional structural and functional versatility. This study employs first principles density functional theory (DFT) to investigate the stability, mechanical anisotropy, and optical response of the novel M 4 GaC 3 (M = V, Nb, and Ta) MAX‐phases. All three compounds are confirmed to be thermodynamically and mechanically stable. A key finding is their outstanding performance, exhibiting ultra‐high stiffness and strong thermal resilience, which establishes their suitability for extreme thermomechanical conditions. Electronic structure analysis confirms metallic conductivity, while the optical spectra reveal high reflectivity in the visible and infrared ranges. These first‐principles predictions provide critical design insights, identifying the M 4 GaC 3 family as promising multifunctional materials for structural and functional roles in aerospace and high‐performance energy systems.
{"title":"Computational Design of M 4 GaC 3 (M = V, Nb, Ta) MAX‐Phases: Stability, Mechanical Strength, and Optical Response Under High Pressure and Temperature","authors":"I. Ouadha, M. H. Elahmar, H. Rached, M. Caid, D. Rached, Y. Rached, S. Al‐Qaisi, A. Boutramine, N. Hacini","doi":"10.1002/adts.202501514","DOIUrl":"https://doi.org/10.1002/adts.202501514","url":null,"abstract":"MAX phases, which combine metallic and ceramic characteristics, are promising candidates for operation in extreme environments owing to their exceptional structural and functional versatility. This study employs first principles density functional theory (DFT) to investigate the stability, mechanical anisotropy, and optical response of the novel M <jats:sub>4</jats:sub> GaC <jats:sub>3</jats:sub> (M = V, Nb, and Ta) MAX‐phases. All three compounds are confirmed to be thermodynamically and mechanically stable. A key finding is their outstanding performance, exhibiting ultra‐high stiffness and strong thermal resilience, which establishes their suitability for extreme thermomechanical conditions. Electronic structure analysis confirms metallic conductivity, while the optical spectra reveal high reflectivity in the visible and infrared ranges. These first‐principles predictions provide critical design insights, identifying the M <jats:sub>4</jats:sub> GaC <jats:sub>3</jats:sub> family as promising multifunctional materials for structural and functional roles in aerospace and high‐performance energy systems.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"21 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145499106","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuxuan Cao, Wei Zhou, Guangxiong Luo, Chenxi Zhang, C. P. Liang
This study employs semiempirical molecular orbital methods to evaluate the electronic and solvation characteristics of five common molecules as electrolyte additives and co‐solvents for alkali metal batteries. The highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) suggest that 1,2‐dimethoxyethane (DME), 1,2‐diethoxyethanes (DEE) and 1,3‐dioxolane (DOL) exhibit suitable redox activity for electrochemical process. However, after binding with one Li ion, DME distinguishes itself as a more promising solvent for alkali metal batteries. The solvation structure of DME with alkali metal ions is investigated. The geometric relaxation and electronic transfer imply that partial crystallization happens as the number of DME reaches the saturation point (maximum three DMEs). This crystallization improves the electrochemical stability and mediates the redox activity. In addition, fluorination of DME enhance DME's oxidation resistance and chemical stability, and partial fluorination with 4 F atoms (F4DME) displays the optimum properties. On the other hand, fluorination destabilizes the solvation structures with alkali metal ions, and reduces the saturated DMEs from three to two. The desolvation tendency and enhanced binding energy provide a viable way to tune the electrochemical performance of solvent, and thus enable a balance between chemical stability and electrochemical kinetics.
{"title":"Theoretical Screening for Electronic and Solvation Characteristics of Common Molecules as Electrolyte Additives and Co‐Solvents for Alkali Metal Batteries","authors":"Yuxuan Cao, Wei Zhou, Guangxiong Luo, Chenxi Zhang, C. P. Liang","doi":"10.1002/adts.202500767","DOIUrl":"https://doi.org/10.1002/adts.202500767","url":null,"abstract":"This study employs semiempirical molecular orbital methods to evaluate the electronic and solvation characteristics of five common molecules as electrolyte additives and co‐solvents for alkali metal batteries. The highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) suggest that 1,2‐dimethoxyethane (DME), 1,2‐diethoxyethanes (DEE) and 1,3‐dioxolane (DOL) exhibit suitable redox activity for electrochemical process. However, after binding with one Li ion, DME distinguishes itself as a more promising solvent for alkali metal batteries. The solvation structure of DME with alkali metal ions is investigated. The geometric relaxation and electronic transfer imply that partial crystallization happens as the number of DME reaches the saturation point (maximum three DMEs). This crystallization improves the electrochemical stability and mediates the redox activity. In addition, fluorination of DME enhance DME's oxidation resistance and chemical stability, and partial fluorination with 4 F atoms (F4DME) displays the optimum properties. On the other hand, fluorination destabilizes the solvation structures with alkali metal ions, and reduces the saturated DMEs from three to two. The desolvation tendency and enhanced binding energy provide a viable way to tune the electrochemical performance of solvent, and thus enable a balance between chemical stability and electrochemical kinetics.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"368 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145491953","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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