Related papers: Universal Approach for Determining Multi-Dimension…
The very good performance of modern density functional theory for molecular geometries and harmonic vibrational frequencies has been well established. We investigate the performance of density functional theory (DFT) for quartic force…
We present a vibrational dynamical mean-field theory (VDMFT) of the dynamics of atoms in solids with anharmonic interactions. Like other flavors of DMFT, VDMFT maps the dynamics of a periodic anharmonic lattice of atoms onto those of a…
During the noisy intermediate-scale quantum (NISQ) era, quantum computational approaches refined to overcome the challenge of limited quantum resources are highly valuable. However, the accuracy of the molecular properties predicted by most…
High-level vibrational calculations have been used to investigate anharmonicity in a wide variety of materials using density-functional-theory (DFT) methods. We have developed a new and efficient approach for describing strongly-anharmonic…
We developed a general framework for hybrid quantum-classical computing of molecular and periodic embedding approaches based on an orbital space separation of the fragment and environment degrees of freedom. We demonstrate its potential by…
Bosonic quantum devices, which utilize harmonic oscillator modes to encode information, are emerging as a promising alternative to conventional qubit-based quantum devices, especially for the simulation of vibrational dynamics and…
We present a novel formulation of the vibrational density matrix renormalization group (vDMRG) algorithm tailored to strongly anharmonic molecules described by general high-dimensional model representations of potential energy surfaces. For…
We introduce a general approach for the simulation of quantum vibrational states of (symmetric and asymmetric) double-well potentials in molecules and materials for thermodynamic and spectroscopic applications. The method involves solving…
A real-space formalism for density-functional perturbation theory (DFPT) is derived and applied for the computation of harmonic vibrational properties in molecules and solids. The practical implementation using numeric atom-centered…
Determining the vibrational structure of a molecule is central to fundamental applications in several areas, from atmospheric science to catalysis, fuel combustion modeling, biochemical imaging, and astrochemistry. However, when significant…
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…
The quantum quartic anharmonic oscillator with the Hamiltonian $H=\frac{1}{2}\left( p^{2}+x^{2}\right) +\lambda x^{4}$ is a classical and fundamental model that plays a key role in various branches of physics, including quantum mechanics,…
Quantum computation of vibrational properties of molecules is a promising platform to obtain computational advantages for computational chemistry. However, fault-tolerant quantum computations of vibrational properties remain a relatively…
We devise an efficient scheme to determine vibrational properties from Path Integral Molecular Dynamics (PIMD) simulations. The method is based on zero-time Kubo-transformed correlation functions and captures the anharmonicity of the…
In the framework of density functional theory (DFT) simulations of molecules and materials, anharmonic terms of the potential energy surface are commonly computed numerically, with an associated cost that rapidly increases with the size of…
We have developed a formulation of density functional perturbation theory for the calculation of vibrational frequencies in molecules and solids, which uses numerical atomic orbitals as a basis set for the electronic states. The (harmonic)…
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…
We present a first-principles approach for calculating phonon-polariton dispersion relations. In this approach, phonon-photon interaction is described by quantization of a Hamiltonian that describes harmonic lattice vibrations coupled with…
Theoretical predictions of photochemical processes are essential for interpreting and understanding spectral features. Reliable quantum dynamics calculations of vibronic systems require precise modeling of anharmonic effects in the…
We propose a q-deformed model of the anharmonic vibrations in diatomic molecules. We analyse the applicability of the model to the phenomenological Dunham's expansion by comparing with experimental data. Our methodology involves a global…