Related papers: Quantum harmonic free energies for biomolecules an…
Free energies of molecules can be calculated by quantum computations or by normal mode classical calculations. However, the first can be computationally impractical for large molecules and the second is based on the assumption of harmonic…
Free energy calculations are at the heart of physics-based analyses of biochemical processes. They allow us to quantify molecular recognition mechanisms, which determine a wide range of biological phenomena from how cells send and receive…
We present a theoretical first-principles method to calculate the free energy of a magnetic system in its high-temperature paramagnetic phase, including vibrational, electronic, and magnetic contributions. The method for calculating free…
We introduce a framework for the calculation of ground and excited state energies of bosonic systems suitable for near-term quantum devices and apply it to molecular vibrational anharmonic Hamiltonians. Our method supports generic reference…
Accurately computing the free energies of biological processes is a cornerstone of computer-aided drug design but it is a daunting task. The need to sample vast conformational spaces and account for entropic contributions makes the…
Predictions of relative stabilities of (competing) molecular crystals are of great technological relevance, most notably for the pharmaceutical industry. However, they present a long-standing challenge for modeling, as often minuscule free…
Phonon frequency moments and thermodynamic functions (electrostatic and vibrational parts of the free energy, internal energy, and heat capacity) are calculated for bcc and fcc Coulomb crystals in the harmonic approximation with a…
In this paper, we investigate the use of variational quantum algorithms for simulating the thermodynamic properties of dinuclear metal complexes. Our study highlights the potential of quantum computing to transform advanced simulations and…
A density-functional-theory based approach to efficiently compute numerically exact vibrational free energies - including anharmonicity - for chemically complex multicomponent alloys is developed. It is based on a combination of…
We establish an analytical criterion for dynamical thermalization within harmonic systems, applicable to both classical and quantum models. Specifically, we prove that thermalization of various observables, such as particle energies in…
Variational quantum algorithms offer a promising framework for solving eigenvalue problems on near-term quantum hardware, yet their applicability beyond electronic structure calculations remains relatively unexplored. In this work, we…
The absolute free energy -- or partition function, equivalently -- of a molecule can be estimated computationally using a suitable reference system. Here, we demonstrate a practical method for staging such calculations by growing a molecule…
Thermodynamical systems at the nanoscale, such as single molecules interacting with highly structured vibrational environments, typically undergo non-equilibrium physical processes that lack precise microscopic descriptions.…
Obtaining the free energies of condensed phase chemical reactions remains computationally prohibitive for high-level quantum mechanical methods. We introduce a hierarchical machine learning framework that bridges this gap by distilling…
In this work, I propose a statistical mechanical framework, for the evaluation of the free energy in molecular systems, by "deleting" all the molecules in a "single" step. The approach can be considered as the statistical mechanics…
Quantitative evaluations of the free energy of materials must take into account thermal and zero-point energy fluctuations. While these effects can easily be estimated within a harmonic approximation, corrections arising from the anharmonic…
We report model calculations of the time-dependent internal energy and entropy for a single quasi-free massive quantum particle at a constant temperature. We show that the whole process started from a fully coherent quantum state to…
We demonstrate that the discrete character of the vibrational spectrum of a small crystal accounts for size dependence of its thermodynamic properties and melting temperature. Using a self-consistent statistical method [Phys. Rev.B 66,…
We propose a method to continually monitor the energy of a quantum system. We show that by having some previous knowledge of the system's dynamics, but not all of it, one can use the measured energy to determine many other quantities, such…
Quantum thermodynamics is a powerful theoretical tool for assessing the suitability of quantum materials as platforms for novel technologies. In particular, the modeling of quantum cycles allows us to investigate the heat changes and work…