化学物理
Light-induced molecular dynamics often involve the excitation of several electronic, vibrational, and rotational states. Since the ensuing electronic and nuclear motion determines the pathways and outcomes of photoinduced reactions, our…
Water at solid surfaces is key for many processes ranging from biological signal transduction to membrane separation and renewable energy conversion. However, under realistic conditions, which often include environmental and surface charge…
Monoterpene ketones are frequently studied compounds that enjoy great popularity both in chemistry and in physics due to comparatively high volatility, stability, conformational rigidity and commercial availability. Herein, we explore the…
In this paper, we present results obtained using QMCTorch, a modular framework for real-space Quantum Monte Carlo (QMC) simulations of small molecular systems. Built on the popular deep learning library PyTorch, QMCTorch is GPU-native and…
Strongly correlated systems are well described as a configuration interaction of Slater determinants classified by their number of unpaired electrons. This treatment is however unfeasible. In this manuscript, it is demonstrated that single…
Machine learning models often require large datasets and struggle to generalize beyond their training distribution. These limitations pose significant challenges in scientific and engineering contexts, where generating exhaustive datasets…
Accurate simulation of atomic systems has the potential to revolutionize the design of molecules and materials. Unfortunately, exact solutions of the Schr\"odinger equation scale as O(N!) and remain inaccessible for systems with more than a…
We present a fully numerical framework for the optimization of molecule-specific quantum chemical basis functions within the quantics tensor train format using a finite-difference scheme. The optimization is driven by solving the…
Water contamination by arsenic(V) constitutes a major public-health concern, underscoring the need for models that capture both equilibrium and transient adsorption behaviour. A framework that can do so is the steepest-entropy-ascent…
Zero and ultralow-field nuclear magnetic resonance (ZULF NMR) is an NMR modality where experiments are performed in fields at which spin-spin interactions within molecules and materials are stronger than Zeeman interactions. This typically…
In recent years, there has been a push to go beyond Born-Oppenheimer theory and build electronic states from a phase space perspective, i.e. parameterize electronic states by both nuclear position(R) and nuclear momentum(P). Previous…
Atomistic simulations are essential tools in chemistry and materials science, accelerating the discovery of novel catalysts, energy storage materials, and pharmaceuticals. However, running these simulations remains challenging due to the…
Multireference systems are usually challenging to investigate using ab initio methods as they require an accurate description of static electron correlation. The urgency of developing similar approaches is even more pressing when molecules…
Ligand strain energy, the energy difference between the bound and unbound conformations of a ligand, is an important component of structure-based small molecule drug design. A large majority of observed ligands in protein-small molecule…
A pillar of our current understanding of the photoluminescence of Ir(III) complexes is the assumption that the population of triplet metal-centered states determines an efficient non-radiative decay to the ground state minimum. Based on…
Variational optimization of neural-network quantum state representations has achieved FCI-level accuracy for ground state calculations, yet computing optical properties involving excited states remains challenging. In this work, we present…
Quantifying correlation and complexity in quantum many-body states is central to advancing theoretical and computational chemistry, physics, and quantum information science. This work introduces a novel framework, mutual correlation, based…
Static disorder plays a crucial role in the electronic dynamics and spectroscopy of complex molecular systems. Traditionally, obtaining observables averaged over static disorder requires thousands of realizations via direct sampling of the…
We report an efficient implementation of the ionization potential (IP) variant of the equation-of-motion coupled cluster (IP-EOM-CC) method based on the exact two-component atomic mean field (X2CAMF) framework, utilizing Cholesky…
The PySCF package has emerged as a powerful and flexible open-source platform for quantum chemistry simulations. However, the efficiency of electronic structure calculations can vary significantly depending on the choice of computational…