Article
Chemistry, Inorganic & Nuclear
Anton S. Pozdeev, Wei-Jia Chen, Maksim Kulichenko, Hyun Wook Choi, Alexander I. Boldyrev, Lai-Sheng Wang
Summary: Researchers have discovered that copper-boron binary clusters have unique covalent bonding structures, which are determined by the high stability of the appropriate-sized boron chain structures in this range. In larger boron chain structures, it is expected that ionic bonding between copper and boron will occur.
SOLID STATE SCIENCES
(2023)
Review
Chemistry, Physical
Teng-Teng Chen, Ling Fung Cheung, Lai-Sheng Wang
Summary: Photoelectron spectroscopy combined with quantum chemistry is a powerful method to study the structures and bonding of size-selected boron clusters. Metal-doped boron clusters not only exhibit novel structures, but also provide insights into the metal-boron bonds critical for understanding boride materials. Recent advances in transition metal-doped boron clusters include the discovery of metal-boron multiple bonds and novel aromatic boron clusters.
ANNUAL REVIEW OF PHYSICAL CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Hyun Wook Choi, Wei-Jia Chen, G. Stephen Kocheril, Dao-Fu Yuan, Lai-Sheng Wang
Summary: In this study, the structures and chemical bonding of two Bi-doped boron clusters were investigated using experimental and theoretical methods. It was found that both clusters adopt a planar structure with the Bi atom bonded to the periphery of the cluster. Chemical bonding analysis revealed the presence of sigma and pi double-aromaticity in the boron clusters.
Article
Multidisciplinary Sciences
Wan-Lu Li, Teng-Teng Chen, Wei-Jia Chen, Jun Li, Lai-Sheng Wang
Summary: In this study, the researchers investigated lanthanide-doped octa-boron clusters with the rare +I oxidation state using photoelectron spectroscopy and theoretical calculations. The results showed a significant change in the oxidation state of lanthanides from +III to +I, leading to the formation of clusters similar to aromatic hydrocarbon molecules with monovalent lanthanide ligands.
NATURE COMMUNICATIONS
(2021)
Article
Biochemistry & Molecular Biology
Peng-Fei Han, Qiang Sun, Hua-Jin Zhai
Summary: We predict a new example of boron-based inverse sandwich alloy clusters, V2B7-, through computational global-minimum structure searches and quantum chemical calculations. Chemical bonding analysis reveals that the inverse sandwich cluster is governed by globally delocalized 6p and 6s frameworks, following the (4n + 2) Huckel rule. The skeleton B-B s bonding is shown to be quasi-Lewis-type, roof-like 4c-2e V-B-2-V s bonds, covering the whole surface of the inverse sandwich cluster in a truly three-dimensional manner.
Review
Chemistry, Inorganic & Nuclear
Sourav Kar, Alaka Nanda Pradhan, Sundargopal Ghosh
Summary: Metal-rich metallaborane clusters with triply and tetra bridging borylenes, and multicentred boride units have attracted renewed interest due to their diverse reactivity and unique structural features. Recent advancements in synthetic strategies utilizing transition metals have enabled the isolation of borylene species and the encapsulation of boride inside different clusters. The bonding ability of borylene and boride with multiple transition metals has led to the formation of a series of metal-rich metallaboranes.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Multidisciplinary Sciences
Ruofei Cheng, Jie Zhang, Huifang Zhang, Zaozao Qiu, Zuowei Xie
Summary: The study presents a new method for enantioselective synthesis of chiral-at-cage o-carboranes using iridium catalysis, allowing for efficient synthesis of new skeletons under mild conditions. The results demonstrate that the use of chiral phosphoramidite ligand is crucial for achieving asymmetric o-carborane B-H alkenylation.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Gai-ru Yan, Yu-qian Liu, Xin-bo Liu, Meng-hui Wang, Zhong-hua Cui, Sudip Pan
Summary: Planar hexacoordination (ph) has been rarely reported in the literature. Recent electronic structure calculations predict the existence of anionic planar hexacoordinate beryllium and magnesium clusters, phBe/Mg, which have high kinetic stability and could be confirmed experimentally. These clusters are covalently bonded with six carbon centers and contain bridging positions occupied by M (Al, Ga for phBe and Ga, In, Tl for phMg). The bonding between Be/Mg and the carbon centers in phBe/Mg is double aromatic (s + p) in nature, involving 7c-2e delocalized s bonds and p bonds.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Wenhao Sun, Melanie Schnell
Summary: Broadband rotational spectroscopy was used to investigate the geometries of 3-methyl-3-oxetanemethanol and its complexes with water molecules. The study found that the conformation of 3-methyl-3-oxetanemethanol is influenced by microsolvation effects, and the hydrogen-bond arrangements in the hydrate complexes evolve with increasing water molecules.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Stephen A. Miller
Summary: This study investigates the structure, stability, and cooperative bonding of alpha-quartz silica (SiO2) through computational molecular orbital analysis.The results show that despite the geminal oxygen-oxygen distances of 2.61-2.64 angstrom, silica model complexes exhibit anomalously large O-O bond orders that increase with increasing cluster size. The long covalent bond theory (LCBT) proposed in this study suggests that non-canonical O-O bonds play a subtle but crucial role in the structure and stability of Earth's most abundant material.
FRONTIERS IN CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Chandan Nandi, Arindam Roy, Ketaki Kar, Marie Cordier, Sundargopal Ghosh
Summary: A variety of cobalt-rich metallaheteroboranes were synthesized by treating compounds such as nido-[(Cp*Co)(2)B6H6E2] (E = Se, Te) and [Ru-3(CO)(12)] under thermolytic conditions. These metal-rich clusters have different core structures and were characterized using NMR, IR, ESI-MS, and X-ray diffraction analysis techniques.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Maksim Kulichenko, Wei-Jia Chen, Yang-Yang Zhang, Cong-Qiao Xu, Jun Li, Lai-Sheng Wang
Summary: The strong relativistic effects in gold and gold compounds lead to interesting chemical and physical properties. Small gold clusters prefer planar structures, and dopants can be used to tune their properties. The stability of Zn-doped Au9Zn- is demonstrated by its electronic configuration and chemical bonding properties.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Multidisciplinary
Caiyun Chen, Haifeng Lv, Ping Zhang, Zhiwen Zhuo, Yu Wang, Chen Ma, Wenbin Li, Xuguang Wang, Baojie Feng, Peng Cheng, Xiaojun Wu, Kehui Wu, Lan Chen
Summary: Borophene, a novel material composed of boron atoms, has been successfully synthesized as large-size, single-crystalline bilayer on a copper substrate. The bilayer borophene exhibits metallic character and increased resistance to oxidation compared to its monolayer counterparts.
Article
Chemistry, Multidisciplinary
Chao-Jiang Zhang, Filiberto Ortiz-Chi, Xi-Ling Xu, Hong-Guang Xu, Gabriel Merino, Wei-Jun Zheng
Summary: The study explored the structures of C2Al4-/0 and C(2)Al(5)(-/0) using different techniques. It was found that C2Al4- has a boat-like structure consisting of a C-2 unit surrounded by four aluminum atoms. In contrast, the neutral C2Al4 species has a planar structure with two ptC units. The most stable isomer of C2Al5- adopts a D-3h symmetry with the C(2) unit interacting with five aluminum atoms.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Sergey A. Tikhonov, Andrey E. Sidorin, Alexander A. Ksenofontov, Denis Yu. Kosyanov, Ilya S. Samoilov, Anna D. Skitnevskaya, Alexander B. Trofimov, Elena V. Antina, Mikhail B. Berezin, Vitaliy I. Vovna
Summary: The electronic structure, cationic and excited states of a series of 1,3,5,7-tetramethyl-substituted BODIPYs were studied using X-ray photoelectron spectroscopy (XPS) and steady-state absorption spectroscopy. Computational methods including ADC(2), OVGF, DFT, and TD-DFT were used to interpret the experimental data. The substitution effects on the XPS and absorption spectra for the 2,6-positions of 4Me,2R-BODIPY pyrrole nuclei were determined.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Dao-Fu Yuan, Tarek Trabelsi, Yue-Rou Zhang, Joseph S. Francisco, Lai-Sheng Wang
Summary: This study accurately determines the electron affinity and bond dissociation energy of SO3 and its radical anion SO3- using cryogenically cooled anions and high-level ab initio calculations. The excited states of SO3- are also calculated, providing valuable information for interpreting autodetachment processes.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Review
Chemistry, Multidisciplinary
Nikita Fedik, Roman Zubatyuk, Maksim Kulichenko, Nicholas Lubbers, Justin S. Smith, Benjamin Nebgen, Richard Messerly, Ying Wai Li, Alexander Boldyrev, Kipton Barros, Olexandr Isayev, Sergei Tretiak
Summary: Machine learning is becoming the preferred method for modeling complex chemical processes and materials. It provides a surrogate model trained on reference data to establish a relationship between molecular structures and chemical properties. This Review highlights the developments in using machine learning to evaluate chemical properties and obtain simplified quantum-mechanical descriptions, as well as the challenges and future outlook in this field.
NATURE REVIEWS CHEMISTRY
(2022)
Article
Biochemistry & Molecular Biology
Anton S. Pozdeev, Pavel Rublev, Steve Scheiner, Alexander I. Boldyrev
Summary: Boron hydrides have unique bonding patterns and have been extensively studied. In this work, indium hydrides of In2Hx (x = 0-4,6) and In3Hy (y = 0-5) series were investigated using DFT and ab initio quantum chemistry methods. The bonding pattern of indium hydrides differs from classical structures and boron hydrides of the BnHn+2 series. The studied stoichiometries exhibit multi-center bonds, aromaticity, and the tendency for indium to preserve the 1c-2e lone pair.
Correction
Chemistry, Multidisciplinary
Nikita Fedik, Roman Zubatyuk, Maksim Kulichenko, Nicholas Lubbers, Justin S. Smith, Benjamin Nebgen, Richard Messerly, Ying Wai Li, Alexander I. Boldyrev, Kipton Barros, Olexandr Isayev, Sergei Tretiak
NATURE REVIEWS CHEMISTRY
(2022)
Editorial Material
Chemistry, Physical
Michele Ceriotti, Lasse Jensen, David E. Manolopoulos, Todd Martinez, David R. Reichman, Francesco Sciortino, C. David Sherrill, Qiang Shi, Carlos Vega, Lai-Sheng Wang, Emily A. Weiss, Xiaoyang Zhu, Jenny Stein, Tianquan Lian
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
G. Stephen Kocheril, Han-Wen Gao, Lai-Sheng Wang
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Maksim Kulichenko, Kipton Barros, Nicholas Lubbers, Nikita Fedik, Guoqing Zhou, Sergei Tretiak, Benjamin Nebgen, Anders M. N. Niklasson
Summary: The most recent shadow potential energy version of Extended Lagrangian Born-Oppenheimer molecular dynamics (XL-BOMD) has been implemented in the semiempirical PyTorch-based software PySeQM. The implementation includes finite electronic temperatures, canonical density matrix perturbation theory, and an adaptive Krylov subspace approximation. The PyTorch implementation utilizes GPU and machine learning hardware accelerators for simulations. The new XL-BOMD formulation allows for the study of challenging chemical systems with charge instabilities and low electronic energy gaps. In a simulation of 840 carbon atoms, one integration time step executes in 4 s on a single Nvidia RTX A6000 GPU.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Anton S. Pozdeev, Wei-Jia Chen, Hyun Wook Choi, Maksim Kulichenko, Dao-Fu Yuan, Alexander I. Boldyrev, Lai-Sheng Wang
Summary: Copper is capable of mediating the formation of bilayer borophenes. Copper-boron binary clusters are used to investigate the interactions between copper and boron, which are crucial for understanding the growth mechanisms of borophenes on copper substrates. In this study, joint photoelectron spectroscopy and theoretical calculations were conducted on two di-copper-doped boron clusters, Cu2B3 (-) and Cu2B4 (-). Well-resolved photoelectron spectra were obtained, revealing the presence of low-lying isomers in both cases. Theoretical calculations showed that the global minimum structures of Cu2B3 (-) and Cu2B4 (-) have different arrangements of copper and boron atoms.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Dao-Fu Yuan, Yuan Liu, Yue-Rou Zhang, Lai-Sheng Wang
Summary: The first observation of a polarization-assisted dipole-bound state (DBS) for a molecule with a dipole moment below 2.5 debye is reported. Photoelectron and photodetachment spectroscopies are conducted and a DBS is found only 6 cm-1 below the detachment threshold along with sharp vibrational Feshbach resonances. The observed DBS has pi-symmetry stabilized by the strong anisotropic polarizability of indolyl.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
G. Stephen Kocheril, Han-Wen Gao, Lai-Sheng Wang
Summary: We conducted a temperature-controlled photoelectron imaging study on SbO2-, which was produced from a laser vaporisation source and cooled in a cryogenic 3D Paul trap. We obtained vibrationally resolved photoelectron spectra for the ground state detachment transition and determined the bending frequencies for both SbO2 and SbO2-. Franck-Condon simulations allowed us to estimate the vibrational temperature of the trapped SbO2- anion. We also obtained a near-threshold spectrum of SbO2- at a photon energy of 3.4958 eV, revealing partially resolved rotational structure and providing an accurate measurement of the electron affinity of SbO2.
Article
Chemistry, Physical
Yue-Rou Zhang, Dao-Fu Yuan, Lai-Sheng Wang
Summary: Molecular anions with polar neutral cores can support highly diffused dipole-bound states below their detachment thresholds. Recent experimental advances have allowed the investigation of dipole-bound excited states at a new level. This Perspective describes recent progress in the investigation of dipole-bound states using an electrospray photoelectron spectroscopy apparatus equipped with a cryogenically cooled Paul trap.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Yue-Rou Zhang, Dao-Fu Yuan, Chen-Hui Qian, Guo-Zhu Zhu, Lai-Sheng Wang
Summary: Although the influence of molecular polarizability on the formation of dipole-bound states (DBSs) is not well understood, this study investigates the role of polarization interactions in the formation of DBSs using carbazolide as a model compound. The study utilizes cryogenic photodetachment spectroscopy and high-resolution photoelectron spectroscopy and reveals the presence of a polarization-assisted DBS, despite the carbazolyl neutral core having a dipole moment smaller than the critical value. The study also provides valuable information about the vibrational modes and electronic states of carbazolide.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Inorganic & Nuclear
Anton S. Pozdeev, Wei-Jia Chen, Maksim Kulichenko, Hyun Wook Choi, Alexander I. Boldyrev, Lai-Sheng Wang
Summary: Researchers have discovered that copper-boron binary clusters have unique covalent bonding structures, which are determined by the high stability of the appropriate-sized boron chain structures in this range. In larger boron chain structures, it is expected that ionic bonding between copper and boron will occur.
SOLID STATE SCIENCES
(2023)
Article
Computer Science, Interdisciplinary Applications
Maksim Kulichenko, Kipton Barros, Nicholas Lubbers, Ying Wai Li, Richard Messerly, Sergei Tretiak, Justin S. Smith, Benjamin Nebgen
Summary: A strategy called uncertainty-driven dynamics for active learning (UDD-AL) is developed to modify the potential energy surface in molecular dynamics simulations based on the uncertainty of a neural network ensemble. It efficiently discovers configurations that meaningfully augment the training data set. The method is demonstrated to explore chemically relevant configuration space that is otherwise inaccessible.
NATURE COMPUTATIONAL SCIENCE
(2023)
