Article
Chemistry, Multidisciplinary
Kai Braun, Otto Hauler, Dai Zhang, Xiao Wang, Thomas Chasse, Alfred J. Meixner
Summary: Surface charging effects at metal-molecule interfaces have significant impacts on the performance of organic electronics, especially with the ongoing downsizing of organic components. A spectroscopic approach based on tip-enhanced Raman spectroscopy (TERS) is utilized to study metal-molecule interfaces under applied voltage, revealing how intrinsic inductive effects in molecules can shift electron density distribution when bias voltage is applied. This experiment provides valuable insights into charged metal-molecule interfaces.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Materials Science, Multidisciplinary
Dennis Perchak, Ryan J. McCarty, Kieron Burke
Summary: Conditional-probability density functional theory (CP-DFT) is a formally exact method for finding correlation energies from Kohn-Sham DFT without evaluating an explicit energy functional. In this paper, the authors provide details on how to generate accurate exchange-correlation energies for the ground-state uniform gas using CP-DFT. They also propose using the exchange hole in a CP antiparallel spin calculation to extract the high-density limit. Furthermore, the authors present a highly accurate analytic solution to the Thomas-Fermi model and compare its performance to Kohn-Sham for this problem, highlighting its potential usefulness at high temperatures. Several approximations to the CP potential are explored and compared to accurate parametrizations for both exchange-correlation energies and holes.
Article
Chemistry, Multidisciplinary
Luis Leyva-Parra, Ricardo Pino-Rios
Summary: The electronic structure, changes in aromatic behavior, and stability of the least studied m-quinone in the benzoquinone family were investigated. Unrestricted density functional theory calculations and three aromaticity criteria were used to understand why this isomer prefers the triplet state in its ground state. The answer lies in spin density delocalization and proposed resonance structure contributions.
NEW JOURNAL OF CHEMISTRY
(2023)
Article
Nanoscience & Nanotechnology
Jing Zhou, Kunming Yang, Bihuan Yang, Boan Zhong, Songsong Yao, Youcao Ma, Jian Song, Tongxiang Fan, Dawei Tang, Jie Zhu, Yue Liu
Summary: Graphene has great potential for thermal management applications due to its high thermal conductivity. However, the low interface thermal conductance between graphene and metals limits its effective heat dissipation. In this study, the interfacial electron behaviors were investigated by comparing hydrogenation-treated graphene with pure graphene, and the effect of graphene layer numbers on the interfacial thermal conductance was systematically studied. The results showed that a larger interfacial thermal conductance can be obtained with lower layer numbers.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Nanoscience & Nanotechnology
Jing Zhou, Kunming Yang, Bihuan Yang, Boan Zhong, Songsong Yao, Youcao Ma, Jian Song, Tongxiang Fan, Dawei Tang, Jie Zhu, Yue Liu
Summary: As a typical two-dimensional material, graphene has high in-plane thermal conductivity but low interface thermal conductance with metals, limiting its effectiveness in thermal management. This study investigates the interfacial electron behaviors between hydrogenation-treated graphene and nickel nanofilms. The results show that a larger interface thermal conductance can be obtained when the layer number is low, possibly reaching a peak value at a certain layer number.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Benfang Niu, Haoran Liu, Yanchun Huang, Emely Gu, Minxing Yan, Ziqiu Shen, Kangrong Yan, Buyi Yan, Jizhong Yao, Yanjun Fang, Hongzheng Chen, Chang-Zhi Li
Summary: A simple and scalable interfacial strategy is reported to facilitate the assembly of high-performance inverted perovskite solar cells (PSCs) and scale-up modules. This strategy improves the chemical stability, charge extraction, and energy level alignment of the hole-selective interface, while promoting perovskite crystallization. As a result, the corresponding inverted PSCs and modules achieve remarkable power conversion efficiencies (PCEs) of 24.5% and 20.7% (aperture area of 19.4 cm(2)), respectively. This strategy is also effective for perovskite with various bandgaps, demonstrating the highest PCE of 19.6% for the 1.76-eV bandgap PSCs.
ADVANCED MATERIALS
(2023)
Article
Physics, Multidisciplinary
Shadi Fatayer, Florian Albrecht, Ivano Tavernelli, Mats Persson, Nikolaj Moll, Leo Gross
Summary: By using single charge injections with an atomic force microscope, redox reactions of a molecule on a multilayer insulating film were investigated. Three channels for neutralization were observed and corresponding to transitions to different excited states. Energy differences between these transitions were measured using single-electron tunneling spectroscopy, and compared with density functional theory calculations. The results show that excited states of molecules can be prepared and their optical gap energies can be quantified through controlled single-charge injections.
PHYSICAL REVIEW LETTERS
(2021)
Article
Materials Science, Multidisciplinary
Ayoub Aouina, Matteo Gatti, Siyuan Chen, Shiwei Zhang, Lucia Reining
Summary: In this work, accurate exchange-correlation potentials for Si and NaCl are determined based on the ground-state densities obtained from auxiliary field quantum Monte Carlo calculations. The study shows that these potentials can be rationalized as an ensemble of a few local functions of the density, characterized by the gradient of the density and the local kinetic energy density. By using these accurate potentials, the KS band structure can be obtained with high accuracy. The findings also confirm the stability of the KS system and question the meaning of details of the potentials.
Article
Multidisciplinary Sciences
Philipp Geppert, Max Althoen, Daniel Fichtner, Herwig Ott
Summary: Exploring the dynamics of inelastic and reactive collisions on the quantum level is a fundamental goal in quantum chemistry. Such collisions are of particular importance in connection with Rydberg atoms in dense environments since they may considerably influence both the lifetime and the quantum state of the scattered Rydberg atoms. The authors report on the study of state-changing collisions between Rydberg atoms and ground state atoms, finding that the outcome of such collisions is not limited to a single hydrogenic manifold, and observing a redistribution of population over a wide range of final states. They also find that even the decay to states with the same angular momentum quantum number as the initial state, but different principal quantum number is possible.
NATURE COMMUNICATIONS
(2021)
Review
Chemistry, Physical
Zhuoyu Peng, Ruixuan Wan, Bo Zhang
Summary: Single-molecule fluorescence microscopy is an effective technique for studying redox processes at the electrochemical interface. It allows for high-resolution imaging of individual molecules and the detection of single nanobubbles generated on the electrode surface.
CURRENT OPINION IN ELECTROCHEMISTRY
(2022)
Article
Engineering, Chemical
Wei Chen, Yumiao Lu, Yanlei Wang, Feng Huo, Wei-Lu Ding, Li Wei, Hongyan He
Summary: Tuning the structures and properties of interfacial ionic liquids using electric fields is crucial for modern energy storage technologies. Experimental results show asymmetric structural evolution and enhanced mobility of interfacial ILs during charge injection. Slow and mild charge injection is advantageous for maintaining structural stability and regulating dielectric constants.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
Article
Chemistry, Physical
Muhammad N. Tahir, Tong Zhu, Honghui Shang, Jia Li, Volker Blum, Xinguo Ren
Summary: We present a method based on localized resolution of identity (LRI) for calculating the analytical gradients of RPA ground-state energy with respect to atomic positions within the atomic orbital basis set framework. Our results demonstrate the numerical precision and usefulness of LRI in RPA gradient evaluations.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Nanoscience & Nanotechnology
Kanji Homma, Satoshi Kaneko, Kazuhito Tsukagoshi, Tomoaki Nishino
Summary: Charge transfer at metal-molecule interfaces is crucial in nanomaterials, especially for electronic applications, but its understanding at the single-molecule level is still limited. In this study, a highly conductive adsorption site was discovered in a single-molecule junction (SMJ) of naphthalenedithiol using surface-enhanced Raman scattering (SERS) and current-voltage measurements. The vibrational energy and conductance analysis revealed that the high conductivity is attributed to the adsorption site with significant charge transfer. This research demonstrates that SERS combined with transport measurements can provide insights into both the structures of SMJs and charge transfer at metal-molecule interfaces.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Ettore Bartalucci, Alexander A. A. Malar, Anne Mehnert, Julius B. Kleine B. Buening, Lennart Guenzel, Maik Icker, Martin Boerner, Christian Wiebeler, Beat H. H. Meier, Stefan Grimme, Berthold Kersting, Thomas Wiegand
Summary: In this study, proton-detected solid-state Nuclear Magnetic Resonance (NMR) experiments were used to detect a single water molecule trapped in a lanthanide complex by analyzing three types of non-covalent interactions. The water proton resonances were detected at a chemical-shift value close to zero ppm, which was further confirmed by quantum-chemical calculations. Density Functional Theory calculations revealed the sensitivity of the proton chemical-shift value for hydrogen-pi interactions. This study highlights the importance of proton-detected solid-state NMR in probing weak non-covalent interactions in molecular recognition events in chemistry and biology.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Materials Science, Multidisciplinary
Haoran Zhu, Peixuan Liu, Xu Zuo, Bin Shao
Summary: This paper reveals that the antiferromagnetic ground state of CrOCl is determined by the competition of magnetic exchange interactions, and the adjustment of parameters can lead to the experimentally observed ground state.
