Article
Chemistry, Multidisciplinary
Mayanak K. Gupta, Jingxuan Ding, Naresh C. Osti, Douglas L. Abernathy, William Arnold, Hui Wang, Zachary Hood, Olivier Delaire
Summary: By investigating the phonons in Na3PS4 and their coupling to fast sodium diffusion, key anharmonic phonon modes controlling the diffusion process were identified at the Brillouin zone boundary of the anharmonically stabilized cubic phase. Detailed insights into the dynamic mechanism of fast sodium diffusion were provided, offering a pathway to search for further sodium solid electrolytes.
ENERGY & ENVIRONMENTAL SCIENCE
(2021)
Article
Chemistry, Physical
Mayanak K. Gupta, Jingxuan Ding, Dipanshu Bansal, Douglas L. Abernathy, Georg Ehlers, Naresh C. Osti, Wolfgang G. Zeier, Olivier Delaire
Summary: This study provides critical insights into the atomistic mechanisms underlying fast ion conduction in the superionic material Cu7PSe6, through inelastic and quasielastic neutron scattering measurements and molecular dynamics simulations. The results reveal that the diffusion of copper ions is limited by intercluster hopping controlled by selective anharmonic phonons. The thermal conductivity is dominated by low-energy acoustic phonon modes of the crystal framework. These findings highlight the importance of strongly anharmonic effects in superionic systems.
ADVANCED ENERGY MATERIALS
(2022)
Article
Multidisciplinary Sciences
Hiram Kwak, Jae-Seung Kim, Daseul Han, Jong Seok Kim, Juhyoun Park, Gihan Kwon, Seong-Min Bak, Unseon Heo, Changhyun Park, Hyun-Wook Lee, Kyung-Wan Nam, Dong-Hwa Seo, Yoon Seok Jung
Summary: Researchers have designed a new type of halide nanocomposite solid electrolyte that significantly improves the ionic conductivity of solid-state batteries and shows good compatibility with sulfide solid electrolytes. Through theoretical calculations and experimental measurements, it was demonstrated that interfacial oxygen-substituted compounds play a role in enhancing the interfacial conduction mechanism.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Jianxing Huang, Linfeng Zhang, Han Wang, Jinbao Zhao, Jun Cheng, E. Weinan
Summary: The study implemented a deep potential generator to automatically generate fast interatomic potentials for solid-state electrolyte materials, expanding the simulation range of diffusion processes and investigating technical aspects in depth. The computed data agreed well with experimental results, laying the foundation for computational screening research on solid-state electrolyte materials.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Materials Science, Multidisciplinary
Lu Gao, Nan Wu, Nanping Deng, Zhenchao Li, Jianxin Li, Yong Che, Bowen Cheng, Weimin Kang, Ruiping Liu, Yutao Li
Summary: Researchers improved the performance of solid-state Li-metal batteries by introducing Gd-doped CeO2 nanowires to the polymer electrolyte. The optimized composite polymer electrolyte has high ion conductivity and transference number, and exhibits good compatibility with the metallic lithium anode and high-voltage cathode.
ENERGY & ENVIRONMENTAL MATERIALS
(2023)
Article
Chemistry, Physical
Kota Suzuki, Michiyo Kamiya, Naoki Matsui, Satoshi Hori, Masaaki Hirayama, Ryoji Kanno
Summary: Considering the concept of compositional complexity, new solid electrolytes based on quaternary and quinary lithium superionic conductor (LISICON) systems were investigated for highly ion-conducting material development. The study found that even in highly complex compositions, it was difficult to achieve high Ti- and Ga-doping contents in the gamma-Li3PO4 framework. The relatively low ionic conductivities and high activation energies of the quaternary and quinary LISICON systems compared to the ternary LISICON systems indicated a negligible positive effect of the compositional complexity.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Pengbo Wang, Sawankumar Patel, Haoyu Liu, Po-Hsiu Chien, Xuyong Feng, Lina Gao, Benjamin Chen, Jue Liu, Yan-Yan Hu
Summary: The correlation between lattice chemistry and cation migration in high-entropy Li+ conductors is investigated using argyrodite family of Li+ conductors. The study reveals the complex structure-property relationships in high-entropy superionic conductors and highlights the significance of heterogeneity in lattice dynamics.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Seamus D. Jones, Howie Nguyen, Peter M. Richardson, Yan-Qiao Chen, Kira E. Wyckoff, Craig J. Hawker, Raphaele J. Clement, Glenn H. Fredrickson, Rachel A. Segalman
Summary: By self-assembling into superionically conductive domains, the ion electrolyte overcomes the limitation of limited conductivity and achieves excellent performance in lithium-ion batteries.
ACS CENTRAL SCIENCE
(2022)
Article
Chemistry, Physical
Mikael S. Andersson, Vitalie Stavila, Alexander Skripov, Mirjana Dimitrievska, Malgorzata T. Psurek, Juscelino B. Leao, Olga A. Babanova, Roman Skoryunov, Alexei Soloninin, Maths Karlsson, Terrence J. Udovic
Summary: The study investigates the unique structural and ion dynamical properties of NaCB11H12 dispersed within high-surface-area silica through salt-solution infiltration, revealing the formation of a nanoconfined phase with superionic properties that persist at subambient temperatures. Fast-cation diffusion promoted by high anion mobilities leads to Na+ superionic conductivities of around 0.3 mS/cm at room temperature, indicating future potential for conductivity enhancement in related polyhedral (carba)borate-based salts as solid-state electrolytes in battery applications.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Physics, Applied
Yinghua Niu, Wenjun Li, Longfei Liu, Modeste Venin Mendieev Nitou, Jinlan Nie, Zongwei Mei, Feng Cao, Weiqiang Lv
Summary: In this study, the researchers investigated a silicate-based solid Li-ion conductor using ab initio molecular dynamics simulations. They found that adjusting the Si/Al ratio greatly improved Li-ion diffusion and conductivity, enabling room-temperature operation of solid-state batteries.
APPLIED PHYSICS LETTERS
(2022)
Article
Chemistry, Physical
Ronghan Chen, Zhenming Xu, Yuechuan Lin, Buyao Lv, Shou-Hang Bo, Hong Zhu
Summary: In this study, the influence of substituting Cl with Br in Li3OCl1-xBrx on the local structure, lattice dynamics, and Li-ion conductivity was investigated through first-principles calculations. The results showed that the incorporation of Br softens the overall lattice stiffness of Li3OCl1-xBrx, but the accompanying local structural distortion is the main factor in altering the activation energy for Li-ion diffusion.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Chemistry, Physical
Gabriel Krenzer, Johan Klarbring, Kasper Tolborg, Hugo Rossignol, Andrew R. McCluskey, Benjamin J. Morgan, Aron Walsh
Summary: In this study, molecular dynamics simulations were used to investigate the type-II superionic phase transition in α-Li3N. The findings suggest that the superionic transition may be driven by a decrease in defect formation energetics rather than changes in Li transport mechanism. This insight may have implications for other type-II superionic materials.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Moinak Dutta, Manisha Samanta, Tanmoy Ghosh, David J. Voneshen, Kanishka Biswas
Summary: In this study, lattice dynamics in the Zintl compound TlInTe2 were investigated, revealing that the intrinsic rattling nature of Tl leads to strong phonon scattering and a remarkably low phonon lifetime, resulting in an ultralow thermal conductivity in TlInTe2.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Yuan Ouyang, Wei Gong, Qi Zhang, Jia Wang, Sijia Guo, Yingbo Xiao, Dixiong Li, Changhong Wang, Xueliang Sun, Chaoyang Wang, Shaoming Huang
Summary: Solid-state batteries (SSBs) offer improved energy density and safety. However, existing solid-state electrolytes (SSEs) face challenges in meeting the operational requirements of SSBs. This study introduces a novel approach using metal-organic frameworks (MOF-BZN) as high-performance SSEs, which exhibit remarkable lithium ion conductivity and high transference number.
ADVANCED MATERIALS
(2023)
Article
Physics, Applied
Zhi W. Hua, Tan Zheng, Jing X. Sang, Xiao F. Xu, Bin H. Wu, Lian F. Wei
Summary: Vanadium dioxide (VO2) undergoes a phase transition from the monoclinic phase to the rutile phase near 340 K at ambient pressure, with potential device applications. The study calculates the phonon properties of the two phases of VO2 using the TDEP method and constructs a resistance-temperature phase diagram, indicating the stability of the rutile phase. The research provides evidence that anharmonicity in the lattice dynamics of VO2 is significant.
JOURNAL OF PHYSICS D-APPLIED PHYSICS
(2021)
Article
Materials Science, Multidisciplinary
Rituraj Sharma, Matan Menahem, Zhenbang Dai, Lingyuan Gao, Thomas M. Brenner, Lena Yadgarov, Jiahao Zhang, Yevgeny Rakita, Roman Korobko, Iddo Pinkas, Andrew M. Rappe, Omer Yaffe
PHYSICAL REVIEW MATERIALS
(2020)
Article
Materials Science, Multidisciplinary
Rituraj Sharma, Zhenbang Dai, Lingyuan Gao, Thomas M. Brenner, Lena Yadgarov, Jiahao Zhang, Yevgeny Rakita, Roman Korobko, Andrew M. Rappe, Omer Yaffe
PHYSICAL REVIEW MATERIALS
(2020)
Article
Chemistry, Multidisciplinary
Matan Menahem, Zhenbang Dai, Sigalit Aharon, Rituraj Sharma, Maor Asher, Yael Diskin-Posner, Roman Korobko, Andrew M. Rappe, Omer Yaffe
Summary: Recent studies have shown that the optical and electronic properties of 2D hybrid organic-inorganic halide perovskites are strongly influenced by thermal fluctuations. By comparing the structural dynamics of 3D and 2D crystals, the impact of organic cations on the inorganic scaffold can be revealed, providing insights into the performance of these materials.
Article
Chemistry, Physical
Guy Reuveni, Yael Diskin-Posner, Christian Gehrmann, Shravan Godse, Giannis G. Gkikas, Isaac Buchine, Sigalit Aharon, Roman Korobko, Constantinos C. Stoumpos, David A. Egger, Omer Yaffe
Summary: We demonstrate that formamidinium-based crystals differ from methyl ammonium-based halide perovskite crystals due to the presence of intrinsic local static disorder in their inorganic sublattice, despite having a well-defined average crystal structure. Our study combines terahertz-range Raman scattering, single-crystal X-ray diffraction, and first-principles calculations to investigate the temperature-dependent dynamics of the inorganic sublattice in the range of 10-300 K. The temperature evolution of the Raman spectra reveals that low-temperature, local static disorder significantly influences the crystal structural dynamics and phase transitions at higher temperatures.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Maor Asher, Marco Bardini, Luca Catalano, Remy Jouclas, Guillaume Schweicher, Jie Liu, Roman Korobko, Adi Cohen, Yves Geerts, David Beljonne, Omer Yaffe
Summary: We use temperature-dependent low-frequency Raman measurements and first-principles calculations to investigate the order-disorder phase transition of ditBu-BTBT crystals. By analyzing the Raman peaks and their dependence on temperature, we identify the lattice normal modes associated with the phase transition and propose a model to explain the observed behaviors. Our findings suggest that side-chain engineering can be used to control polymorphism in amphidynamic crystals by manipulating lattice interactions.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Materials Science, Multidisciplinary
Matan Menahem, Nimrod Benshalom, Maor Asher, Sigalit Aharon, Roman Korobko, Olle Hellman, Omer Yaffe
Summary: The anharmonic lattice dynamics of oxide and halide perovskites have significant influence on their mechanical and optical properties. Raman spectroscopy is used to study the structural dynamics, but existing interpretations cannot explain the temperature dependence of the observed Raman spectra. In this study, we present a model for second-order Raman scattering that accounts for the unique temperature trend and demonstrate its applicability to other dynamically disordered crystal phases.
PHYSICAL REVIEW MATERIALS
(2023)
Article
Chemistry, Physical
Maor Asher, Remy Jouclas, Marco Bardini, Yael Diskin-Posner, Nitzan Kahn, Roman Korobko, Alan R. Kennedy, Lygia Silva de Moraes, Guillaume Schweicher, Jie Liu, David Beljonne, Yves Geerts, Omer Yaffe
Summary: This study investigates the effect of chemical modifications on the lattice dynamics of organic semiconductors. The results show that specific expressions of vibrational anharmonicity can be suppressed by chemical modifications, with p-conjugated modifications being the most effective.
