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The adsorption and desorption of reactants and products from a solid surface is essential for achieving sustained surface chemical reactions. At a liquid-solid interface, these processes can involve the collective reorganization of interfacial solvent molecules in order to accommodate the adsorbing or desorbing species. Identifying the role of solvent in adsorption and desorption is important for advancing our understanding of surface chemical rates and mechanisms and for enabling the rational design and optimization of surface chemical systems. In this manuscript we use all-atom molecular dynamics simulation and transition path sampling to identify water's role in the desorption of CO from a Pt(100) surface in contact with liquid water. We demonstrate that the solvation of CO, as quantified by the water coordination number, is an essential component of the desorption reaction coordinate. We use meta dynamics to compute the desorption free energy surface and conclude based on its features that desorption proceeds via a two-step mechanism whereby the final detachment of CO from the surface is preceded by the formation of a nascent solvation shell.

While artificial intelligence has the potential to process vast amounts of data, generate new insights, and unlock greater productivity, its widespread adoption may entail unforeseen consequences. We identify conditions under which AI, by reducing the cost of access to certain modes of knowledge, can paradoxically harm public understanding. While large language models are trained on vast amounts of diverse data, they naturally generate output towards the 'center' of the distribution. This is generally useful, but widespread reliance on recursive AI systems could lead to a process we define as "knowledge collapse", and argue this could harm innovation and the richness of human understanding and culture. However, unlike AI models that cannot choose what data they are trained on, humans may strategically seek out diverse forms of knowledge if they perceive them to be worthwhile. To investigate this, we provide a simple model in which a community of learners or innovators choose to use traditional methods or to rely on a discounted AI-assisted process and identify conditions under which knowledge collapse occurs. In our default model, a 20% discount on AI-generated content generates public beliefs 2.3 times further from the truth than when there is no discount. An empirical approach to measuring the distribution of LLM outputs is provided in theoretical terms and illustrated through a specific example comparing the diversity of outputs across different models and prompting styles. Finally, based on the results, we consider further research directions to counteract such outcomes., Comment: 37 pages, 9 figures

We review the GPAW open-source Python package for electronic structure calculations. GPAW is based on the projector-augmented wave method and can solve the self-consistent density functional theory (DFT) equations using three different wave-function representations, namely real-space grids, plane waves, and numerical atomic orbitals. The three representations are complementary and mutually independent and can be connected by transformations via the real-space grid. This multi-basis feature renders GPAW highly versatile and unique among similar codes. By virtue of its modular structure, the GPAW code constitutes an ideal platform for implementation of new features and methodologies. Moreover, it is well integrated with the Atomic Simulation Environment (ASE) providing a flexible and dynamic user interface. In addition to ground-state DFT calculations, GPAW supports many-body GW band structures, optical excitations from the Bethe-Salpeter Equation (BSE), variational calculations of excited states in molecules and solids via direct optimization, and real-time propagation of the Kohn-Sham equations within time-dependent DFT. A range of more advanced methods to describe magnetic excitations and non-collinear magnetism in solids are also now available. In addition, GPAW can calculate non-linear optical tensors of solids, charged crystal point defects, and much more. Recently, support of GPU acceleration has been achieved with minor modifications of the GPAW code thanks to the CuPy library. We end the review with an outlook describing some future plans for GPAW.

Recent advancements in artificial intelligence (AI) are fundamentally reshaping computing, with large language models (LLMs) now effectively being able to generate and interpret source code and natural language instructions. These emergent capabilities have sparked urgent questions in the computing education community around how educators should adapt their pedagogy to address the challenges and to leverage the opportunities presented by this new technology. In this working group report, we undertake a comprehensive exploration of LLMs in the context of computing education and make five significant contributions. First, we provide a detailed review of the literature on LLMs in computing education and synthesise findings from 71 primary articles. Second, we report the findings of a survey of computing students and instructors from across 20 countries, capturing prevailing attitudes towards LLMs and their use in computing education contexts. Third, to understand how pedagogy is already changing, we offer insights collected from in-depth interviews with 22 computing educators from five continents who have already adapted their curricula and assessments. Fourth, we use the ACM Code of Ethics to frame a discussion of ethical issues raised by the use of large language models in computing education, and we provide concrete advice for policy makers, educators, and students. Finally, we benchmark the performance of LLMs on various computing education datasets, and highlight the extent to which the capabilities of current models are rapidly improving. Our aim is that this report will serve as a focal point for both researchers and practitioners who are exploring, adapting, using, and evaluating LLMs and LLM-based tools in computing classrooms., Comment: 39 pages of content + 12 pages of references and appendices

We find that ion creation/destruction dominates the behavior of electrochemical reaction barriers, through grand-canonical electronic structure calculations of proton-deposition on transition metal surfaces. We show that barriers respond to potential in a nonlinear manner and trace this to the continuous degree of electron transfer as an ion is created or destroyed. This explains both Marcus-like curvature and Hammond-like shifts. Across materials, we find the barrier energy to be driven primarily by the charge presented on the surface, which in turn is dictated by the native work function, a fundamentally different driving force than non-electrochemical systems.

CoPt nanoparticle catalysts are integral to commercial fuel cells. Such systems are prohibitive to fully characterize with electronic structure calculations. Machine-learned potentials offer a scalable solution; however, such potentials are only reliable if representative training data can be employed, which typically requires large electronic structure calculations. Here, we use the nearsighted-force training approach to make high-fidelity machine-learned predictions on large nanoparticles with $>$5,000 atoms using only systematically generated small structures ranging from 38-168 atoms. The resulting ensemble model shows good accuracy and transferability in describing relative energetics for CoPt nanoparticles with various shapes, sizes and Co compositions. It is found that the fcc(100) surface is more likely to form a L1$_0$ ordered structure than the fcc(111) surface. The energy convex hull of the icosahedron shows the most stable particles have Pt-rich skins and Co-rich underlayers. Although the truncated octahedron is the most stable shape across all sizes of Pt nanoparticles, a crossover to icosahedron exists due to a large downshift of surface energy for CoPt nanoparticle alloys. The downshift can be attributed to strain release on the icosahedron surface due to Co alloying. We introduced a simple empirical model to describe the role of Co alloying in the crossover for CoPt nanoparticles. With Monte-Carlo simulations we additionally searched for the most stable atomic arrangement for a truncated octahedron with equal Pt and Co compositions, and also we studied its order-disorder phase transition. We validated the most stable configurations with a new highly scalable density functional theory code called SPARC. Lastly, the order-disorder phase transition for a CoPt nanoparticle exhibits a lower transition temperature and a smoother transition, compared to the bulk CoPt alloy.

The atomic vibrations of a solid surface can play a significant role in the reactions of surface-bound molecules, as well as their adsorption and desorption. Relevant phonon modes can involve the collective motion of atoms over a wide array of length scales. In this manuscript, we demonstrate how the generalized Langevin equation can be utilized to describe these collective motions weighted by their coupling to individual sites. Our approach builds upon the generalized Langevin oscillator (GLO) model originally developed by Tully \textit{et al.} We extend the GLO by deriving parameters from atomistic simulation data. We apply this approach to study the memory kernel of a model platinum surface and demonstrate that the memory kernel has a bimodal form due to coupling to both low-energy acoustic modes and high-energy modes near the Debye frequency. The same bimodal form was observed across a wide variety of solids of different elemental compositions, surface structures, and solvation states. By studying how these dominant modes depend on simulation size, we argue that the acoustic modes are frozen in the limit of macroscopic lattices. By simulating periodically replicated slabs of various sizes we quantify the influence of phonon confinement effects in the memory kernel and their concomitant effect on simulated sticking coefficients.