Chemistry of Materials最新文献_第10页

Investigation of Low-Energy Lattice Dynamics and Their Role in Superionic Na Diffusion and Ultralow Thermal Conductivity of Na3PSe4 as a Solid-State Electrolyte 低能晶格动力学及其在作为固态电解质的 Na3PSe4 的超离子 Na 扩散和超低导热性中的作用研究

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2024-11-25 DOI: 10.1021/acs.chemmater.4c01553

Mayanak K. Gupta, Jingxuan Ding, Hung-Min Lin, Zachary Hood, Naresh C. Osti, Douglas L. Abernathy, Andrey A. Yakovenko, Hui Wang, Olivier Delaire

{"title":"Investigation of Low-Energy Lattice Dynamics and Their Role in Superionic Na Diffusion and Ultralow Thermal Conductivity of Na3PSe4 as a Solid-State Electrolyte","authors":"Mayanak K. Gupta, Jingxuan Ding, Hung-Min Lin, Zachary Hood, Naresh C. Osti, Douglas L. Abernathy, Andrey A. Yakovenko, Hui Wang, Olivier Delaire","doi":"10.1021/acs.chemmater.4c01553","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c01553","url":null,"abstract":"The atomic dynamics of Na3PSe4 were investigated using a combination of neutron scattering experiments and ab initio and machine-learned molecular dynamics simulations to probe the interplay of fast ionic diffusion with atomic vibrations (phonons) of the host lattice. Our results reveal the existence of low-energy vibrational modes, simultaneously involving motions of Na+ ions and framework polyanion subunits, and show that these modes become strongly overdamped in the superionic regime as they couple with the Na+ hopping process. In particular, the Na+ migration energy landscape is strongly impacted by low-energy phonons derived from a soft acoustic branch of the host lattice, which modulates the diameter of the Na+ diffusion channel at the bottleneck. We find that an additional factor for the enhanced Na+ conductivity in Na3PSe4 is the presence of Na-vacancies, which also affect the low-frequency dynamics and thermal vibration amplitudes, pointing to an interplay between Na+ vacancies and host dynamics, jointly enhancing ionic diffusivity. Finally, we investigate the origin of ultralow thermal conductivities in Na3PSe4 and Na3PS4 using Green–Kubo simulations and find that low-energy acoustic phonon modes of the overall crystal framework provide a dominant contribution to the thermal conductivity.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"66 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142696662","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Investigation of Low-Energy Lattice Dynamics and Their Role in Superionic Na Diffusion and Ultralow Thermal Conductivity of Na3PSe4 as a Solid-State Electrolyte

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2024-11-25 DOI: 10.1021/acs.chemmater.4c0155310.1021/acs.chemmater.4c01553

Mayanak K. Gupta*, Jingxuan Ding, Hung-Min Lin, Zachary Hood, Naresh C. Osti, Douglas L. Abernathy, Andrey A. Yakovenko, Hui Wang and Olivier Delaire*,

{"title":"Investigation of Low-Energy Lattice Dynamics and Their Role in Superionic Na Diffusion and Ultralow Thermal Conductivity of Na3PSe4 as a Solid-State Electrolyte","authors":"Mayanak K. Gupta*, Jingxuan Ding, Hung-Min Lin, Zachary Hood, Naresh C. Osti, Douglas L. Abernathy, Andrey A. Yakovenko, Hui Wang and Olivier Delaire*, ","doi":"10.1021/acs.chemmater.4c0155310.1021/acs.chemmater.4c01553","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c01553https://doi.org/10.1021/acs.chemmater.4c01553","url":null,"abstract":"The atomic dynamics of Na3PSe4 were investigated using a combination of neutron scattering experiments and ab initio and machine-learned molecular dynamics simulations to probe the interplay of fast ionic diffusion with atomic vibrations (phonons) of the host lattice. Our results reveal the existence of low-energy vibrational modes, simultaneously involving motions of Na+ ions and framework polyanion subunits, and show that these modes become strongly overdamped in the superionic regime as they couple with the Na+ hopping process. In particular, the Na+ migration energy landscape is strongly impacted by low-energy phonons derived from a soft acoustic branch of the host lattice, which modulates the diameter of the Na+ diffusion channel at the bottleneck. We find that an additional factor for the enhanced Na+ conductivity in Na3PSe4 is the presence of Na-vacancies, which also affect the low-frequency dynamics and thermal vibration amplitudes, pointing to an interplay between Na+ vacancies and host dynamics, jointly enhancing ionic diffusivity. Finally, we investigate the origin of ultralow thermal conductivities in Na3PSe4 and Na3PS4 using Green–Kubo simulations and find that low-energy acoustic phonon modes of the overall crystal framework provide a dominant contribution to the thermal conductivity.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"36 23","pages":"11377–11392 11377–11392"},"PeriodicalIF":7.2,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142851149","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Correction to “Expanded Chemistry and Proton Conductivity in Vanadium-Substituted Variants of γ-Ba4Nb2O9” 对 "γ-Ba4Nb2O9 钒取代变体的扩展化学性质和质子传导性 "的更正

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2024-11-25 DOI: 10.1021/acs.chemmater.4c03167

Alex J Brown, Bettina Schwaighofer, Maxim Avdeev, Bernt Johannessen, Ivana Radosavljevic Evans, Chris D Ling

引用次数: 0

Accelerating Materials Discovery of Novel Europium(II)-Activated Phosphors through Machine Learning Classification of Europium Valences 通过铕价的机器学习分类加速新型铕（II）活化荧光粉的材料发现

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2024-11-25 DOI: 10.1021/acs.chemmater.4c0198110.1021/acs.chemmater.4c01981

Yukinori Koyama*, Yukako Kohriki, Masamichi Harada, Naoto Hirosaki and Takashi Takeda,

{"title":"Accelerating Materials Discovery of Novel Europium(II)-Activated Phosphors through Machine Learning Classification of Europium Valences","authors":"Yukinori Koyama*, Yukako Kohriki, Masamichi Harada, Naoto Hirosaki and Takashi Takeda, ","doi":"10.1021/acs.chemmater.4c0198110.1021/acs.chemmater.4c01981","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c01981https://doi.org/10.1021/acs.chemmater.4c01981","url":null,"abstract":"An approach is presented to accelerate the discovery of host compounds for novel Eu2+-activated phosphor materials by integrating systematic data collection, machine learning, and experimental validation. A data set of Eu2+- and Eu3+-activated phosphors has been constructed using systematic data collection methodology from numerous academic articles. A machine-learning classification model has been developed using the collected data set to predict the oxidation states of Eu ions in potential hosts regarding luminescence. The model considers the nonexclusive nature of the divalent and trivalent oxidation states of Eu ions in phosphor applications. A comprehensive exploration of a materials database was conducted to identify host candidates for novel Eu2+-activated phosphor materials, leading to attempts to synthesize them. Photoluminescence analysis revealed the successful synthesis of 12 new Eu2+-activated phosphors, demonstrating the potential of the proposed approach for accelerating material discovery.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"36 23","pages":"11412–11420 11412–11420"},"PeriodicalIF":7.2,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142843411","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Structural Evolution and Optical Properties of Hydroxyfluorooxoborates MM′2n-1[B3O3F4(OH)]n (M = K, Cs, and Rb; M′ = K, NH4, and Cs; n = 1, 2, and 3)

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2024-11-24 DOI: 10.1021/acs.chemmater.4c0285310.1021/acs.chemmater.4c02853

Huan Pei, Luyong Zhang, Huanhuan Cheng, Shibin Wang, Zhihua Yang, Fangfang Zhang* and Shilie Pan*,

{"title":"Structural Evolution and Optical Properties of Hydroxyfluorooxoborates MM′2n-1[B3O3F4(OH)]n (M = K, Cs, and Rb; M′ = K, NH4, and Cs; n = 1, 2, and 3)","authors":"Huan Pei, Luyong Zhang, Huanhuan Cheng, Shibin Wang, Zhihua Yang, Fangfang Zhang* and Shilie Pan*, ","doi":"10.1021/acs.chemmater.4c0285310.1021/acs.chemmater.4c02853","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02853https://doi.org/10.1021/acs.chemmater.4c02853","url":null,"abstract":"Four hydroxyfluorooxoborates, α-K2[B3O3F4(OH)] (I), β-K2[B3O3F4(OH)] (II), Cs(NH4)3[B3O3F4(OH)]2 (III), and RbCs5[B3O3F4(OH)]3 (IV), with identical fundamental building block (FBB) [B3O3F4(OH)]2–, were obtained successfully and characterized comprehensively. A phase transition between I and II was detected, which led to a space group evolution from centrosymmetric to noncentrosymmetric. The F– and OH– substitution effect was studied based on II and its hydroxyborate derivative K2[B3O3(OH)5], which reveals the corresponding changes in the band gap and the nonlinear optical properties. In addition, the cationic-size effect on the arrangement of the [B3O3F4(OH)]2– FBBs and the birefringent properties were discussed for the title compounds. This study contributes to the advancement of structural chemistry and sheds some light on the structure–property relationship studies of hydroxyfluorooxoborates.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"36 23","pages":"11697–11705 11697–11705"},"PeriodicalIF":7.2,"publicationDate":"2024-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142843869","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Structural Evolution and Optical Properties of Hydroxyfluorooxoborates MM′2n-1[B3O3F4(OH)]n (M = K, Cs, and Rb; M′ = K, NH4, and Cs; n = 1, 2, and 3) 羟基氟氧硼烷 MM′2n-1[B3O3F4(OH)]n（M = K、Cs 和 Rb；M′ = K、NH4 和 Cs；n = 1、2 和 3）的结构演变和光学特性

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2024-11-24 DOI: 10.1021/acs.chemmater.4c02853

Huan Pei, Luyong Zhang, Huanhuan Cheng, Shibin Wang, Zhihua Yang, Fangfang Zhang, Shilie Pan

{"title":"Structural Evolution and Optical Properties of Hydroxyfluorooxoborates MM′2n-1[B3O3F4(OH)]n (M = K, Cs, and Rb; M′ = K, NH4, and Cs; n = 1, 2, and 3)","authors":"Huan Pei, Luyong Zhang, Huanhuan Cheng, Shibin Wang, Zhihua Yang, Fangfang Zhang, Shilie Pan","doi":"10.1021/acs.chemmater.4c02853","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02853","url":null,"abstract":"Four hydroxyfluorooxoborates, α-K2[B3O3F4(OH)] (I), β-K2[B3O3F4(OH)] (II), Cs(NH4)3[B3O3F4(OH)]2 (III), and RbCs5[B3O3F4(OH)]3 (IV), with identical fundamental building block (FBB) [B3O3F4(OH)]2–, were obtained successfully and characterized comprehensively. A phase transition between I and II was detected, which led to a space group evolution from centrosymmetric to noncentrosymmetric. The F– and OH– substitution effect was studied based on II and its hydroxyborate derivative K2[B3O3(OH)5], which reveals the corresponding changes in the band gap and the nonlinear optical properties. In addition, the cationic-size effect on the arrangement of the [B3O3F4(OH)]2– FBBs and the birefringent properties were discussed for the title compounds. This study contributes to the advancement of structural chemistry and sheds some light on the structure–property relationship studies of hydroxyfluorooxoborates.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"183 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142696666","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

High-Pressure/High-Temperature Synthesis of the Lanthanoid Zinc Borates Ln2Zn(B2O5)2 (Ln = Eu, Tb, Yb, Lu) with a Gadolinite-Analogue Crystal Structure and Luminescence Properties of Tb2Zn(B2O5)2:Eu3+ 具有类似钆石榴石晶体结构的镧系锌硼酸盐 Ln2Zn(B2O5)2（Ln = Eu、Tb、Yb、Lu）的高压/高温合成及 Tb2Zn(B2O5)2:Eu3+ 的发光特性

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2024-11-22 DOI: 10.1021/acs.chemmater.4c02134

Tobias A. Teichtmeister, Tom Förster, Alexander Hugo Bernhart, Markus Seibald, Markus Suta, Hubert Huppertz

{"title":"High-Pressure/High-Temperature Synthesis of the Lanthanoid Zinc Borates Ln2Zn(B2O5)2 (Ln = Eu, Tb, Yb, Lu) with a Gadolinite-Analogue Crystal Structure and Luminescence Properties of Tb2Zn(B2O5)2:Eu3+","authors":"Tobias A. Teichtmeister, Tom Förster, Alexander Hugo Bernhart, Markus Seibald, Markus Suta, Hubert Huppertz","doi":"10.1021/acs.chemmater.4c02134","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02134","url":null,"abstract":"Four new lanthanoid zinc borates with the composition Ln2Zn(B2O5)2 (Ln = Eu, Tb, Yb, Lu) were obtained by high-pressure/high-temperature syntheses in a modified Walker-type multianvil device. The layered crystal structures are built up of four- and eight-membered rings of corner-sharing [BO4] tetrahedra. Two adjacent layers are linked by the lanthanoid- and zinc-centered polyhedra. A detailed investigation of the luminescence properties and energy transfer in Eu3+-activated Tb2Zn(B2O5)2 and a thorough characterization of the title compounds by infrared spectroscopy and temperature-dependent powder X-ray diffraction are provided. It turns out that the energy transfer between Tb3+ and Eu3+ is extremely efficient (≥98%), which can be related to the unusually short interlanthanoid distance of around 3.45 Å in this structure. The potential use as a lifetime-based luminescent thermometer relying on a temperature-dependent back energy transfer from Eu3+ to Tb3+ above room temperature with appreciable relative sensitivity (Sr = 0.92% K–1 at 425 K) is indicated.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"15 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685033","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Trions Stimulate Electronic Coupling in Colloidal Quantum Dot Molecules 三离子激发胶体量子点分子中的电子耦合

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2024-11-22 DOI: 10.1021/acs.chemmater.4c02809

Jordi Llusar, Juan I. Climente

引用次数: 0

Trions Stimulate Electronic Coupling in Colloidal Quantum Dot Molecules

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2024-11-22 DOI: 10.1021/acs.chemmater.4c0280910.1021/acs.chemmater.4c02809

Jordi Llusar, and , Juan I. Climente*,

{"title":"Trions Stimulate Electronic Coupling in Colloidal Quantum Dot Molecules","authors":"Jordi Llusar,  and , Juan I. Climente*, ","doi":"10.1021/acs.chemmater.4c0280910.1021/acs.chemmater.4c02809","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02809https://doi.org/10.1021/acs.chemmater.4c02809","url":null,"abstract":"Recent synthetic progress has enabled the controlled fusion of colloidal CdSe/CdS quantum dots in order to form dimers, manifesting electronic coupling in their optical response. While this “artificial H2 molecule” constitutes a milestone toward the development of nanocrystal chemistry, the strength of the coupling has proven to be smaller than intended. The reason is that, when an exciton is photoinduced in the system, the hole localizes inside the CdSe cores and captures the electron, often preventing substantial delocalization across the dimer. Here, we predict, by means of k·p theory and configuration interaction calculations, that using trions instead of neutral excitons or biexcitons restores the electron delocalization. Positive trions are particularly apt because the strong hole–hole repulsion makes electron delocalization robust against moderate asymmetries in the cores, thus maintaining a homodimer-like behavior. The hybridization energies are sufficiently large to preserve the molecular character beyond cryogenic temperatures.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"36 23","pages":"11676–11683 11676–11683"},"PeriodicalIF":7.2,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142843049","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Correction to “P2-Na2/3Mn0.8M0.1M′0.1O2 (M = Zn, Fe and M′ = Cu, Al, Ti): A Detailed Crystal Structure Evolution Investigation”

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2024-11-22 DOI: 10.1021/acs.chemmater.4c0314910.1021/acs.chemmater.4c03149

Jennifer H. Stansby, Neeraj Sharma*, Maxim Avdeev, Helen E A Brand, Bernt Johannessen, Elena Gonzalo, Nicholas E Drewett, Nagore Ortiz-Vitoriano and Teófilo Rojo,

引用次数: 0