Related papers: Absolute free energies estimated by combining pre-…
Kinetic energy of individual fission fragment for actinide nuclei is, for example, important for evaluating the prompt-neutron spectrum in the laboratory system. It is experimentally known that kinetic energy for each fragment is constant…
In the first order of perturbation theory, the total energy of a diatomic molecule in the ground state is calculated taking into account the Pauli principle and plasma oscillations of atomic electrons. The Fourier component of the potential…
We generalise the two-sided Bogoliubov inequality for classical particles from [L. Delle Site et al., J.Stat.Mech.Th.Exp. 083201 (2017)] to systems of quantum particles. As in the classical set-up, the inequality leads to upper and lower…
We compute analytically the probability distribution of large deviations in the spin-glass free energy for the Sherrington-Kirkpatrick mean field model, i.e. we compute the exponentially small probability of finding a system with intensive…
In this PhD thesis, we explore and apply methods inspired by the free energy principle to two important areas in machine learning and neuroscience. The free energy principle is a general mathematical theory of the necessary…
We have developed a new simulation algorithm for free-energy calculations. The method is a multidimensional extension of the replica-exchange method. While pairs of replicas with different temperatures are exchanged during the simulation in…
A novel thermodynamic integration (TI) scheme is presented that allows computing the free energy of grain boundaries (GBs) in crystals from atomistic computer simulation. Unlike previous approaches, the method can be applied at arbitrary…
We provide an exact expression of the moment of the partition function for random energy models of finite system size, generalizing an earlier expression for a grand canonical version of the discrete random energy model presented by the…
Free energy sampling methods allow studying the full dynamics of activated processes. Unfortunately, the affordable accuracy of the potential describing the energy and forces of the system is usually rather low. Here we introduce a new…
Free energy calculations based on atomistic Hamiltonians and sampling are key to a first principles understanding of biomolecular processes, material properties, and macromolecular chemistry. Here, we generalize the Free Energy Perturbation…
The partition function and free energy of a quantum many-body system determine its physical properties in thermal equilibrium. Here we study the computational complexity of approximating these quantities for $n$-qubit local Hamiltonians.…
The solvation free energy (SFE) of molecules and ions is a fundamental property governing their solvation behavior and solubility. Molecular simulations offer a route to compute SFEs using alchemical free energy methods, such as…
Recent progress in simulation methodologies and in computer power allow first principle simulations of condensed systems with Born-Oppenheimer electronic energies obtained by Quantum Monte Carlo methods. Computing free energies and…
The hydration free energy of a macromolecule is the central property of interest for understanding its distribution over conformations and its state of aggregation. Calculating the hydration free energy of a macromolecule in all-atom…
Solvation free energy is an important quantity in Computational Chemistry with a variety of applications, especially in drug discovery and design. The accurate prediction of solvation free energies of small molecules in water is still a…
Calculating free energies is an important and notoriously difficult task for molecular simulations. The rapid increase in computational power has made it possible to probe increasingly complex systems, yet extracting accurate free energies…
Energy-based models (EBMs) offer a flexible framework for parameterizing probability distributions using neural networks. However, learning EBMs by exact maximum likelihood estimation (MLE) is generally intractable, due to the need to…
The recently proposed Einstein molecule approach is extended to compute the free energy of molecular solids. This method is a variant of the Einstein crystal method of Frenkel and Ladd[J. Chem. Phys. 81,3188 (1984)]. In order to show its…
Employing a local formula for the electron-electron interaction energy, we derive a self-consistent approximation for the total energy of a general $N$-electron system. Our scheme works as a local variant of the Thomas-Fermi approximation…
We develop an efficient sampling and free energy calculation technique within the adaptive biasing potential (ABP) framework. By mollifying the density of states we obtain an approximate free energy and an adaptive bias potential that is…