Y. P. Ortiz, A. F. Jalbout
We propose a mechanism by which chloromethane and dichloromethane decomposition reaction occurs on the surfaces of graphene. To this end we have performed calculations on the graphene surface with metal adsorption on the sheet on the opposite side of reactions to reduce the formation of free-radical intermediates.
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We present a comprehensive benchmark study of the adsorption energy of a single water molecule on the (001) LiH surface using periodic coupled cluster and quantum Monte Carlo theories. We benchmark and compare different implementations of quantum chemical wave function based theories in order to verify the reliability of the predicted adsorption energies and the employed approximations. Furthermore we compare the predicted adsorption energies to those obtained employing widely-used van der Waals density-functionals. Our findings show that quantum chemical approaches are becoming a robust and r…
Simulation of hydrogen adsorption in hierarchical silicalite: Role of electrostatics and surface chemistry
本研究通过巨正则蒙特卡洛模拟，探究了分级沸石中氢吸附受静电和表面化学的影响，发现引入介孔和静电作用可显著增强吸附，为储氢材料优化提供依据。
Orbital-interaction-aware deep learning model for efficient surface chemistry simulations
本文提出DOTA模型，通过捕捉轨道相互作用模式，实现高效且精确的表面化学模拟，解决吸附能预测中的长期挑战。
Adsorption energies and decomposition barrier heights for ethylene carbonate on the surface of lithium from cluster-based quantum chemistry
研究锂(100)表面乙烯碳酸酯的吸附能和分解活化能，通过有限锂簇计算验证热力学极限方案，发现高阶理论与更低成本方法一致，证明ωB97X-V在锂金属负极电解质溶剂界面化学中表现优异。
The design and production of novel 2-dimensional materials has seen great progress in the last decade, prompting further exploration of the chemistry of such materials. Doping and hydrogenating graphene is an experimentally realised method of changing its surface chemistry, but there is still a great deal to be understood on how doping impacts on the adsorption of molecules. Developing this understanding is key to unlocking the potential applications of these materials. High throughput screening methods can provide particularly effective ways to explore vast chemical compositions of materials.…
Compared to common density functionals, ab initio wave function methods can provide greater reliability and accuracy, which could prove useful when modeling adsorbates or defects of otherwise periodic systems. However, the breaking of translational symmetry necessitates large supercells that are often prohibitive for correlated wave function methods. As an alternative, we introduce the regional embedding approach, which enables correlated wave function treatments of only a target fragment of interest through small, fragment-localized orbital spaces constructed using a simple overlap criterion.…
Hydrogen cyanide (HCN) is a critical reactive source of nitrogen for building key biomolecules relevant for the origin of life. Still, many HCN reactions remain uncharacterized by experiments and theory, and the complete picture of HCN production in planetary atmospheres is not fully understood. To improve this situation, we develop a novel technique making use of computational quantum chemistry, experimental data, and atmospheric numerical simulations. First, we use quantum chemistry simulations to explore the entire field of possible reactions for a list of primary species in N2-, CH4-, and …
Optimizing adsorption configurations on alloy surfaces using Tensor Train Optimizer
该研究将合金表面多分子吸附构型搜索建模为 HUBO，并用 TTOpt 结合 MACE-Osaka24 求解，证明三阶相互作用可在化学精度内识别 CO、NO 的最优覆盖构型。
A Fast, Parallelized, GPU-Accelerated Photochemical Model, XODIAC, with Built-in Equilibrium Chemistry and Multiple Chemical Networks for Exoplanetary Atmospheres
XODIAC是一种快速并行化的GPU加速光化学模型，支持多种化学网络，用于研究系外行星大气化学，展示了其在比较性研究中的高效性和准确性。
Investigating CO Adsorption on Cu(111) and Rh(111) Surfaces Using Machine Learning Exchange-Correlation Functionals
针对CO吸附难题中GGA泛函的缺陷及杂化泛函成本高的问题，本研究采用DeePKS方法训练机器学习交换关联泛函，在Cu(111)和Rh(111)表面实现了接近HSE06的吸附预测精度，为低成本高精度催化剂探索提供了新路径。
The expansion of our Universe is accelerating, due to dark energy. But the nature of dark energy has been a mystery since its discovery at the end of the past century. In Research Highlight https://doi.org/10.1002/ntls.20220003 , Justin Albert, Dmitry Budker and Hossein Sadeghpour provide an overview of how a laser photometric ratio star (a novel light source generated by laser excitation of the Earth's upper-atmospheric sodium layer, which will radiate equally brightly at wavelengths of 589 nm and 820 nm) can help us precisely calibrate telescopes in order to understand the nature of dark ene…
The present theoretical study proposes the enhanced interaction of nanostructures with monosaccharides. It has been demonstrated that the interactions with and without metal adsorption do in fact show that the adsorption energies change accordingly. It is important to note that the chemistry of reactions can also be influenced as a result of this change in dynamics.
CH$_4$ and CO$_2$ Adsorption Mechanisms on Monolayer Graphenylene and their Effects on Optical and Electronic Properties
本文利用SCC-DFTB与MD模拟揭示CH$_4$、CO$_2$在单层GPNL上的吸附解离机制，并结合非平衡格林函数分析其光学与电输运影响。
Gel-Chemistry-Controlled Heavy-Metal Transport and Retention in Cementitious Gel Nanopores: A Molecular Dynamics Study
研究通过分子动力学模拟探讨了不同凝胶化学环境下重金属离子在水泥基纳米孔中的传输与固定机制，揭示了凝胶化学对离子固定的影响。
Iron pyrite (FeS$_{2}$) is the most abundant metal sulfide on Earth. Owing to its reactivity and catalytic activity, pyrite has been studied in various research fields such as surface science, geochemistry, and prebiotic chemistry. Importantly, native iron-sulfur clusters are typically coordinated by cysteinyl ligands of iron-sulfur proteins. In the present paper, we study the adsorption of L-cysteine and its oxidized dimer, L-cystine, on the FeS$_{2}$ surface, using electronic structure calculations based density functional theory and Raman spectroscopy measurements. Our calculations suggest …
Adsorption and Vibrational Spectroscopy of CO on the Surface of MgO from Periodic Local Coupled-Cluster Theory
本研究采用周期性局域耦合簇理论CCSD(T)计算了CO在MgO表面的吸附能与振动频率偏移，结果与实验高度吻合，并揭示了DFT方法因自相互作用误差导致的高估吸附能与错误预测负频率偏移的问题。
A recently developed model chemistry (jun-Cheap) has been slightly modified and proposed as an effective, reliable and parameter-free scheme for the computation of accurate reaction rates with special reference to astrochemical and atmospheric processes. Benchmarks with different sets of state-of-the-art energy barriers spanning a wide range of values show that, in the absence of strong multi-reference contributions, the proposed model outperforms the most well-known model chemistries, reaching a sub-chemical accuracy without any empirical parameter and with affordable computer times. Some tes…
Advancing Surface Chemistry with Large-Scale Ab-Initio Quantum Many-Body Simulations
本文利用GPU加速和可改进多尺度技术实现高达392原子的线性标度量子多体模拟，在石墨烯、金属氧化物及MOF表面吸附中达到化学精度，推动表面化学进入后密度泛函时代。
In the course of our investigations of the adsorption of ions to the air-water interface, we previously reported the surprising result that doubly-charged carbonate anions exhibit a stronger surface affinity than do singly-charged bicarbonate anions. In contrast to monovalent, weakly hydrated anions, which generally show enhanced concentrations in the interfacial region, multivalent (and strongly hydrated) anions are expected to show much weaker surface propensity. In the present work, we use resonantly enhanced deep-UV second harmonic generation spectroscopy to measure the Gibbs free energy o…
We present a self-consistent formalism for computing and understanding the atmospheric chemistry of exoplanets from the viewpoint of an astrophysicist. Starting from the first law of thermodynamics, we demonstrate that the van't Hoff equation (which describes the equilibrium constant), Arrhenius equation (which describes the rate coefficients) and procedures associated with the Gibbs free energy (minimisation, rescaling) have a common physical and mathematical origin. We address an ambiguity associated with the equilibrium constant, which is used to relate the forward and reverse rate coeffici…
An accurate and efficient framework for modelling the surface chemistry of ionic materials
本文提出自动化多层级嵌入框架，以接近DFT的成本将准确cWFT用于离子材料表面，复现19个体系的实验吸附焓并解决吸附构型争议。
Discovering Physically Interpretable Mathematical Expression for Predicting CO2 Adsorption in Metal-Organic Frameworks via Machine Learning-Symbolic Regression
本研究通过ML-SR方法，结合关键结构描述符推导得到可物理解释的CO₂吸附公式，在大规模hMOFs数据集上实现70%以上预测准确率，兼具高效性与机制可解释性。
AI for Interpretable Chemistry: Predicting Radical Mechanistic Pathways via Contrastive Learning
针对现有反应预测器可解释性与跨领域泛化不足的问题，本文提出结合对比学习和机理路径的 RMechRP，并基于 RMechDB 建立首个自由基反应预测基准。
Neural Network Emulator for Atmospheric Chemical ODE
针对大气化学建模复杂且计算量大的问题，提出基于注意力机制的ChemNNE神经网络仿真器，结合正弦时间嵌入、傅里叶神经算子与物理信息损失，在自建大规模化学数据集上实现建模精度与速度的SOTA表现。
Surfaces of metal oxides at working conditions are usually electrified due to the acid-base chemistry. The charged interface compensated with counterions forms the so-called electric double layer. The coupling of surface chemistry and electric double layer is considered to be crucial but poorly understood because of lacking the information at the atomistic scale. Here, we used the latest development in density functional theory based finite-field molecular dynamics simulation to investigate pH-dependence of the Helmholtz capacitance at electrified rutile TiO$_2$ (110)-NaCl electrolyte interfac…
Hydrogen cyanide (HCN) and formaldehyde (H2CO) are key precursors to biomolecules such as nucleobases and amino acids in planetary atmospheres; However, many reactions which produce and destroy these species in atmospheres containing CO2 and H2O are still missing from the literature. We use a quantum chemistry approach to find these missing reactions and calculate their rate coefficients using canonical variational transition state theory and Rice-Ramsperger-Kassel-Marcus/master equation theory at the BHandHLYP/aug-cc-pVDZ level of theory. We calculate the rate coefficients for 126 total react…
Dust grains play a central role in the physics and chemistry of cosmic environments. They influence the optical and thermal properties of the medium due to their interaction with stellar radiation; provide surfaces for the chemical reactions that are responsible for the synthesis of a significant fraction of key astronomical molecules; and they are building blocks of pebbles, comets, asteroids, planetesimals, and planets. In this paper, we review experimental studies of physical and chemical processes, such as adsorption, desorption, diffusion, and reactions forming molecules, on the surface o…
Influence of Chemistry and Topography on the Wettability of Copper
研究通过控制地形和表面化学参数，探讨铜表面润湿性的调控机制，发现地形结构和吸附层对接触角、润湿各向异性及水吸附有显著影响。
Protons at the water/vapor interface are relevant for atmospheric and environmental processes, yet to characterize their surface affinity on the quantitative level is still challenging. Here we utilize phase-sensitive sum-frequency vibrational spectroscopy to quantify the surface density of protons (or their hydronium form) at the intrinsic water/vapor interface, through inspecting the surface-field-induced alignment of water molecules in the electrical double layer of ions. With hydrogen halides in water, the surface adsorption of protons is found to be independent of specific proton-halide a…
Formaldehyde (HCHO) is one one of the most important trace gas in the atmosphere, as it is a pollutant causing respiratory and other diseases. It is also a precursor of tropospheric ozone which damages crops and deteriorates human health. Study of HCHO chemistry and long-term monitoring using satellite data is important from the perspective of human health, food security and air pollution. Dynamic atmospheric chemistry models struggle to simulate atmospheric formaldehyde and often overestimate by up to two times relative to satellite observations and reanalysis. Spatial distribution of modelle…
Combined Experimental and Theoretical Studies on Iodine Capture of Zr-based Metal-Organic Frameworks: Effect of N-functionalization and Adsorption Mechanism
本文合成并研究了Zr基MOFs及其N功能化类似物，发现富N配体通过增强亲和力显著提升碘吸附速率和容量，且具备优异循环性能，为放射性碘捕获机制提供了深入指导。
Ab initio surface chemistry with chemical accuracy
本文结合局域关联和周期性关联波函数理论，以化学精度求解表面分子薛定谔方程，并在CCSD(T)水平上确定水在Al2O3和TiO2上的吸附与解离能量，解决实验争议并评估近似理论误差。
Water gas shift (WGS) reaction is a chemical reaction in which carbon monoxide reacts with water vapor to form carbon dioxide and hydrogen. It is an important reaction industrially used in conjunction with steam reforming of hydrocarbons for the production of high purity hydrogen. Grenoble et al examined the roles of both active metals and metal oxide support on the kinetics of the WGS reaction. They found out that the turn over numbers of various Al2O3 supported transition metals decreased in the trend of Cu, Re, Co, Ru, Ni, Pt, Os, Au, Fe, Pd, Rh, and Ir, which corresponds nicely to the obse…
The surface charge of a water interface determines many fundamental processes in physical chemistry and interface science, and it has been intensively studied for over a hundred years. We summarize experimental methods to characterize the surface charge densities developed so far: electrokinetics, double-layer force measurements, potentiometric titration, surface-sensitive nonlinear spectroscopy, and surface-sensitive mass spectrometry. Then, we elucidate physical ion adsorption and chemical electrification as examples of electrification mechanisms. In the end, novel effects on surface electri…
Using infrared spectroscopy combined with ab initio methods we study reactions of H$_2$O and CO inside the confined spaces of Zn-MOF-74 channels. Our results show that, once the water dissociation reaction H$_2$O$\;\rightarrow\;$OH+H takes place at the metal centers, the addition of 40 Torr of CO at 200 $^{\circ}$C starts the production of formic acid via OH+H+CO$\;\rightarrow\;$HCO$_2$H. Our detailed analysis shows that the overall reaction H$_2$O+CO$\;\rightarrow\;$HCO$_2$H takes place in the confinement of MOF-74 without an external catalyst, unlike the same reaction on flat surfaces. This …
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