Chemical Physics最新文献

{"title":"First principle investigation of essential physical properties of stable Lead-free double perovskites Cs2AgAuX6 (X = cl, Br) for green energy applications","authors":"Abdul Shakoor ,&nbsp;Waqas Raza ,&nbsp;Muhammad Jawad ,&nbsp;Sikander Azam ,&nbsp;Amin Ur Rahman ,&nbsp;Salman Ali ,&nbsp;Noor Ul Amin","doi":"10.1016/j.chemphys.2025.112706","DOIUrl":"10.1016/j.chemphys.2025.112706","url":null,"abstract":"<div><div>In this research, we have utilized density functional theory (DFT) simulations using the full potential linear augmented plane-wave (FPLAPW) approach to estimate the properties of double perovskites. We utilized the PBE-GGA, to calculate structural properties. To calculate the optical and electronic properties of our understudy compounds, we have used the modified Becke and Johnson (mBJ) potential functional. Our findings reveal that these perovskites exhibit band gaps of 1.24 eV and 0.54 eV for X = Br and Cl, respectively. The optical characteristics have been studied using dielectric constants, absorption, refractive index, and reflectivity, which suggest that these double perovskites could be used in solar cells, with the highest transition values in the visible region of photon energy. Furthermore, our transport property calculations using the Boltzmann transport equation indicate that our understudy compounds are best for thermoelectric applications. This research aims to explore and open new doors to experimental and theoretical scientists in the field of optoelectronic and thermoelectric devices.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"595 ","pages":"Article 112706"},"PeriodicalIF":2.0,"publicationDate":"2025-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143641642","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Catalytic mechanisms and metal ion specificity of class II fructose-1,6-bisphosphatases: A QM/MM study","authors":"Jian Wang,&nbsp;Lu Wang,&nbsp;Yinsi Ma,&nbsp;Xue-Ju Lv","doi":"10.1016/j.chemphys.2025.112704","DOIUrl":"10.1016/j.chemphys.2025.112704","url":null,"abstract":"<div><div>Class II Fructose-1,6-bisphosphatases (FBPaseII) play an essential role in gluconeogenesis of bacteria and exhibit conserved catalytic ability with their crucial threonine residue. The activity of FBPaseII is affected when the native metal ion cofactor is replaced. In this study, we developed the FBPaseII catalytic complex models for different species <em>Francisella tularensis</em> and <em>Mycobacterium tuberculosis,</em> with different divalent metal cation Mn²⁺ and Mg²⁺. We simulated the two-step reaction using the Quantum Mechanics/Molecular Mechanics (QM/MM) molecular dynamics (MD) method. The results suggest that the Mg²⁺ in FtFBPase and Mn²⁺ in MtFBPase significantly increase the reaction barrier of FBPaseII, especially in the first step of the reaction. Additionally, we analyzed the stability of the metal ion and the behavior of the water molecules in the active site during the reaction. We propose that the metal ion in the active site plays a role in recruiting water molecules to the reaction center.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"595 ","pages":"Article 112704"},"PeriodicalIF":2.0,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143643935","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Mechanism, kinetics and product nucleation of gas-phase ozonolysis of 3-methyl-3-buten-1-ol in the atmosphere","authors":"Jiaxin Li ,&nbsp;Yanhui Sun ,&nbsp;Yunfeng Li","doi":"10.1016/j.chemphys.2025.112705","DOIUrl":"10.1016/j.chemphys.2025.112705","url":null,"abstract":"<div><div>The unsaturated alcohol 3-methyl-3-buten-1-ol (MBO331) is a typical biogenic volatile organic compound in the atmosphere. The mechanism and kinetics of the MBO331 degradation initiated by O₃ molecules were investigated at the M06-2X/6-311+G(3df,2p)//M06-2X/6-311+G(d,p) level. 4-Hydroxy-2-butanone (P1) is the main product. Molecular dynamics (MD) simulation showed that P1 can form large clusters with SA within 20 ns. The total constant is 8.28 × 10⁻¹⁸ cm³ molecule⁻¹ s⁻¹ at 298 K and 1 atm, and the corresponding lifetime is 2.0 days. This work provides theoretical guidance for the degradation of MBO331 by O₃ molecules and serves as a reference for future experimental studies.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"595 ","pages":"Article 112705"},"PeriodicalIF":2.0,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143682474","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"First-principle calculations to investigate structural, electronic, optical, elastic, and phonon properties of carbon-based IV compounds (Ge, Sn) with hybrids","authors":"Geoffrey Tse","doi":"10.1016/j.chemphys.2025.112702","DOIUrl":"10.1016/j.chemphys.2025.112702","url":null,"abstract":"<div><div>We investigated the electronic, optical and mechanical properties of cubic Germanium Carbide (GeC) and Tin Carbide (SnC) using Density Functional Theory (DFT). Our calculations yielded a lattice length of a = 3.27 Å (3.47 Å) and a bond angle of α = 60° for the primitive cell lattice. The bulk GeC and SnC exhibited indirect bandgaps of 2.33 eV and 1.74 Ev, respectively. Analysis of the density of states plot revealed hybridization between C 2p² and Sn 5p² (Ge 4p²) orbital states. Mechanical property calculations indicated that these carbon-based compounds are brittle and covalent in nature, as suggested by Pugh's ratio. The isotropic nature of the material was confirmed by the identical Young's modulus (E) values in all three directions. We also calculated the group velocity for bulk carbon-based materials and compared these values with their monolayer counterparts. Finally, dynamical stability was verified since all phonon branches exhibited positive frequencies.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"595 ","pages":"Article 112702"},"PeriodicalIF":2.0,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143682411","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"First-principles study of the heavy metals adsorption on SnS2 and Janus monolayers","authors":"Xiaoyu Zhu ,&nbsp;Chi Liu ,&nbsp;Tao Shen ,&nbsp;Xin Liu ,&nbsp;Feifei Sun ,&nbsp;Yue Feng","doi":"10.1016/j.chemphys.2025.112701","DOIUrl":"10.1016/j.chemphys.2025.112701","url":null,"abstract":"<div><div>Heavy metal contamination in water bodies caused serious threats to health and ecosystems, necessitating adsorbing materials for rapid decrease in heavy metals. Therefore, we have conducted a first-principles study on the rapid decrease of heavy metals (Hg, As, Pb) by SnXS (X = S, O, Se) monolayer. Compared with SnS₂, Janus structure SnXS (X = O, Se) narrows the band gap, and increases the electronic interactions between SnXS (X = O, Se) and heavy metals (Hg, As, Pb), thus exhibiting excellent adsorption capacity. In detail, the minimum increase in adsorption capabilities for SnOS and SnSeS are 67.6 % and 27.2 %, respectively. Moreover, the optical properties indicate that at the wavelength of 1550 nm, the refractive indexes of SnSeS reduced after adsorbing As and Pb. Similarly, at the wavelength of 1310 nm, the refractive index of SnOS reduced after adsorbing Hg. Hence, SnXS (X = O, Se) shows a prominent refractive index change characteristic, which has the potential as a functional nanomaterial in the field of optical fiber heavy metal ion detection.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"595 ","pages":"Article 112701"},"PeriodicalIF":2.0,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143643937","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Explanations of the changes of dynamics at the liquid-liquid transition in phosphonium ionic liquids","authors":"K.L. Ngai","doi":"10.1016/j.chemphys.2025.112699","DOIUrl":"10.1016/j.chemphys.2025.112699","url":null,"abstract":"<div><div>Novel properties of ionic conductivity relaxation and structural relaxation were found in experiments on liquid-liquid transition (LLT) in phosphonium ionic liquids with the cation [P_666,14]⁺ and different anions. Structural reorganization at LLT causes the isobaric (isothermal) conductivity relaxation time <em>τ</em>_<em>σ</em>(<em>T,P</em>) to abruptly increase in its temperature (pressure) dependence, which is accompanied by the corresponding decrease of the exponent <em>β</em>_{<em>σKWW</em>}(<em>T,P</em>) in the Kohlrausch-Williams-Watts time correlation function. The correlation between <em>τ</em>_<em>σ</em>(<em>T,P</em>) and <em>β</em>_{<em>σKWW</em>}(<em>T,P</em>) indicates the former is related to or determined by the latter. This inference leads to the explanation by the Coupling Model (CM) with its signature equation predicting exactly that quantitatively. The explanation is justified by the absence of abrupt increase of the relaxation time <em>τ</em>_0<em>σ</em>(<em>T,P</em>) of the local primitive relaxation in the CM at LLT, as expected from its insensitivity to the structural reorganization in LLT. In addition, the CM equation also explained two other properties found in the phosphonium ionic liquids. (1) The <em>β</em>_{<em>σKWW</em>}(<em>T,P</em>) is invariant to variations of <em>T</em> and <em>P</em> while keeping <em>τ</em>_<em>σ</em>(<em>T,P</em>) constant. (2) The structural α-relaxation times <span><math><mrow><msub><mi>τ</mi><mi>α</mi></msub><mrow><mfenced><mi>T</mi></mfenced></mrow></mrow></math></span> in some ionic liquids are longer with a larger activation energy than <em>τ</em>_<em>σ</em>(<em>T</em>) of ion conductivity relaxation, and correspondingly the frequency dispersion of the former is much broader than the latter.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"595 ","pages":"Article 112699"},"PeriodicalIF":2.0,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143643936","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tailoring the electronic and optical properties of CsAuCl₃ via rare-earth doping: A GGA + U + SOC DFT study for phosphor-converted LEDs and advanced optoelectronic applications","authors":"Salman Ahmad ,&nbsp;Muhammad Jawad ,&nbsp;Amin Ur Rahman ,&nbsp;Sikandar Azam ,&nbsp;Asiya Zaman Khan","doi":"10.1016/j.chemphys.2025.112696","DOIUrl":"10.1016/j.chemphys.2025.112696","url":null,"abstract":"<div><div>This study presents aninclusive first-principles investigation of pristine CsAuCl₃ and its rare-earth doped variants (Eu, Tb) using density functional theory (DFT) with the Wien2k implementation of the Full Potential Linearized Augmented Plane Wave (FP-LAPW) method. The calculations incorporate Generalized Gradient Approximation (GGA) with Hubbard U correction and Spin-Orbit Coupling (SOC) to accurately model the strongly correlated f-electrons of the rare-earth dopants. The electronic structure calculations reveal that pristine CsAuCl₃ exhibits semiconducting behavior with an indirect bandgap of 0.672 eV. Upon doping, significant modifications occur: Eu-doped CsAuCl₃ maintains semiconducting character but with a substantially reduced bandgap of 0.034 eV, while Tb-doping induces a transition to metallic behavior. Density of States (DOS) analysis demonstrates pronounced spin polarization in Eu-doped samples, suggesting potential magnetic properties arising from the interaction between Eu 4f states and the host electronic structure. Formation energy calculations confirm the thermodynamic stability of both pristine and doped configurations. Optical property calculations show that rare-earth doping significantly enhances the material's optical response. Doping of Eu and Tb enhances the absorption in infrared, visible, and ultraviolet spectral regions. Notably, Eu-doped CsAuCl₃ exhibits a dramatic enhancement in its static dielectric constant (ε₁(0) = 26.41) compared to the pristine material (ε₁(0) = 2.26). This systematic investigation demonstrates the potential of rare-earth doping for tailoring the electronic and optical properties of CsAuCl₃, suggesting promising applications in phosphor-converted LEDs, photovoltaics, and advanced optoelectronic devices. The results provide fundamental insights into the quantum mechanical mechanisms underlying the observed property modifications while establishing a theoretical framework for future materials engineering in this class of compounds.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"595 ","pages":"Article 112696"},"PeriodicalIF":2.0,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143636530","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Investigation on evolution of surface tension of low reactivity mold flux: Molecular dynamics simulation","authors":"Aihua Zhao ,&nbsp;Min Tan ,&nbsp;Wei Liu ,&nbsp;Guangbei Zhu ,&nbsp;Yuhong Xu ,&nbsp;Tao Li ,&nbsp;Shaopeng Gu ,&nbsp;Liying Ju","doi":"10.1016/j.chemphys.2025.112692","DOIUrl":"10.1016/j.chemphys.2025.112692","url":null,"abstract":"<div><div>The microstructure and surface tension of mold flux are crucial for the stable operation of continuous casting process. The surface tension of CaO-SiO₂-Al₂O₃ based slags with different Al₂O₃ additions was calculated by molecular dynamics simulation. The microstructure of the slag was analyzed to reveal the mechanism of surface tension transition. Furthermore, the pulling cylinder method was employed to verify the accuracy of the molecular dynamics simulation. The results showed that the surface tension increased with Al₂O₃. Nevertheless, when at 15 % to 20 %, due to the formation of anion AlO²⁻ with weak electrostatic potential, the surface tension shows a downward trend.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"595 ","pages":"Article 112692"},"PeriodicalIF":2.0,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143682415","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Two-dimensional Lorandite with high-efficiency photocatalytic water splitting: Insights from ab initio calculations","authors":"Wenyu Fang,&nbsp;Sheng-an Chen,&nbsp;Kai Jin","doi":"10.1016/j.chemphys.2025.112681","DOIUrl":"10.1016/j.chemphys.2025.112681","url":null,"abstract":"<div><div>Photocatalytic water splitting (PWS) plays a crucial role in clean energy generation and environmental protection. In this study, we identified that single-layer Lorandite (TlAsS₂) can be experimentally synthesized due to its low cleavage energy (0.33 J/m²) and high stability. Notably, TlAsS₂ possesses suitable electronegativity (5.06 eV) and a band gap of 2.56 eV, making it a viable candidate for PWS devices. Additionally, single-layer exhibits an electron mobility of 209.83–600.14 cm²/Vs, much higher than the hole mobility of 42.07–52.02 cm²/Vs. Also, it demonstrates a strong absorption coefficient (∼10⁵ cm⁻¹), effectively covering both visible and ultraviolet light, resulting in a desirable light absorption efficiency of 39 %. In conclusion, single-layer TlAsS₂ is a highly promising candidate for optoelectronic and PWS applications due to its favorable electronic properties, light absorption capabilities and overall PWS efficiency.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"595 ","pages":"Article 112681"},"PeriodicalIF":2.0,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143592164","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Chemical insights into the initial thermolysis reactions of [2,2’-bi(1,3,4-oxadiazole)]-5,5’-dinitramide (ICM-101) from quantum chemical modeling","authors":"Shuangfei Zhu,&nbsp;Shufen Zheng,&nbsp;Zixuan Yang,&nbsp;Shuhai Zhang,&nbsp;Ruijun Gou,&nbsp;Yahong Chen","doi":"10.1016/j.chemphys.2025.112684","DOIUrl":"10.1016/j.chemphys.2025.112684","url":null,"abstract":"<div><div>ICM-101 exhibits the density and detonation performance comparable to CL-20, however the atomistic details of its decomposition still remain lacking. Density functional theory and coupled-cluster theory were utilized to study the unimolecular decomposition of ICM-101 in this work. The detailed primary decay reactions map was presented, and results of thermochemistry calculations showed that the preferred decomposition path of ICM-101 is the oxidation of C atom by nitro group, which is a universal decay path in a range of energetic molecules. Furthermore, we found the reversible H transfer and bond rotation reactions for ICM-101 decay, in which bond rotation reaction was proposed as a new sensitivity mechanism. The bond rotation reaction takes place with a low energy barrier, and the product could return back to original molecule with a low barrier. Those findings could contribute to a deep understating of the sensitivity and safety of energetic materials.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"595 ","pages":"Article 112684"},"PeriodicalIF":2.0,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143601555","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}