化学物理
Modeling plasmonic catalysis by applying femtosecond laser pulses of high intensity ($10^{13}-10^{15}$ W cm$^{-2}$), although justified by the time-dependent density functional theory (TDDFT) time-scale limitations, can lead to a…
Accurately and efficiently describing strongly correlated electronic systems is a central challenge in quantum computational chemistry, with classical and quantum computers. The localized active space self-consistent field method (LASSCF)…
Multiply charged actinide molecules provide a unique platform to study fundamental physics and the chemical bond under extreme conditions. Beyond the inherently large relativistic effects associated with a high proton number $Z$, an…
Plasmonic catalysis is a rapidly growing field of research, both from experimental and computational perspectives. Experimental observations demonstrate an enhanced dissociation rate for molecules in the presence of plasmonic nanoparticles…
Iontronics is a burgeoning paradigm that employs ions in solution as information carriers for sensing and computing, e.g., in neuromorphic devices. The fundamentally different working principle as compared to electronics requires novel…
In this work we introduce an effective approach to quantize the electromagnetic response of plasmonic metallic nanostructures. Their shape is arbitrary and they feature a realistic description of the frequency-dependent metal dielectric…
Free energy calculations are widely used tools in computational chemistry, but their dependence on the assignment of partial charges during force field parametrization reduces their accuracy and reproducibility. In this work, we highlight…
In this work, we present the second version of the Donostia Natural Orbital Functional Software, an open-source program for natural orbital functional calculations. The new release incorporates improved optimization algorithms, capabilities…
Modelling the ionic transport in battery cells requires precise parametrization of the involved electrolytes. For carbonate-based electrolytes, however, the evaluation of their parameters suffers from interphase effects between the bulk…
In this work, we develop an extended dissipaton theory that generalizes the environmental couplings beyond the conventional linear and quadratic forms, enabling the treatment of arbitrary order of bath couplings. Applying this theoretical…
Consideration is given to inductively coupled BCl3-plasma (ICP) treatment of the GaN surface, which is a promising technique to get the low resistance ohmic contacts in GaN-based transistors. In some cases, BCl3 plasma treatment results in…
The accurate description of electron correlation and excitation energies remains a fundamental challenge in quantum chemistry. The particle-particle random phase approximation (ppRPA) has emerged as a promising method for capturing a broad…
We present the Plan for Robust and Accurate Potentials (PRAPs), a software package for training and using moment tensor potentials (MTPs) in concert with the Machine Learned Interatomic Potentials (MLIP) software package. PRAPs provides an…
Molecules that violate Hund's rule by exhibiting an inverted singlet-triplet gap (STG), where the first excited singlet (S$_1$) lies below the triplet (T$_1$), are rare but hold great promise as efficient fifth-generation light emitters.…
Molecule generation is advancing rapidly in chemical discovery and drug design. Flow matching methods have recently set the state of the art (SOTA) in unconditional molecule generation, surpassing score-based diffusion models. However,…
The combinatorial scaling of configuration interaction (CI) has long restricted its applicability to only the simplest molecular systems. Here, we report the first numerically exact CI calculation exceeding one quadrillion ($10^{15}$)…
We perform a series of calculations using simulated QPUs, accelerated by the NVIDIA CUDA-Q platform, focusing on a molecular analog of an amine-functionalized metal-organic framework (MOF), a promising class of materials for CO$_2$ capture.…
The density matrix renormalization group (DMRG) is a powerful numerical technique to solve strongly correlated quantum systems: it deals well with systems which are not dominated by a single configuration (unlike Coupled Cluster) and it…
Water behaves very differently at surfaces and under extreme confinement, but the boundary between these two regimes has remained unclear. Despite evidence that interfacial effects persist under sub-nanometre confinement, the…
In this work, we present a proof-of-concept investigation of non-equilibrium chemical reaction dynamics at a molecule-electrode interface, driven out of equilibrium by an applied votage bias and mediated by a confined, enhanced vacuum…