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We consider non-adiabatic transitions in multiple dimensions, which occur when the Born-Oppenheimer approximation breaks down. We present a general, multi-dimensional algorithm which can be used to accurately and efficiently compute the…

Chemical Physics · Physics 2018-04-16 V. Betz , B. D. Goddard , T. Hurst

We explain the concept of superadiabatic approximations and show how in the context of the Born- Oppenheimer approximation they lead to an explicit formula that can be used to predict transitions at avoided crossings. Based on this formula,…

Chemical Physics · Physics 2016-06-29 Volker Betz , Benjamin D. Goddard , Uwe Manthe

Conical intersections are ubiquitous in polyatomic molecules and responsible for a wide range of phenomena in chemistry and physics. We introduce and implement a local diabatic representation for the correlated electron-nuclear dynamics…

Quantum Physics · Physics 2023-10-18 Bing Gu

While there have been many developments in computational probes of both strongly-correlated molecular systems and machine-learning accelerated molecular dynamics, there remains a significant gap in capabilities in simulating accurate…

Chemical Physics · Physics 2025-04-04 Yannic Rath , George H. Booth

We present a novel "linear combination of atomic orbitals"-type of approximation, enabling accurate electronic structure calculations for systems of up to 20 or more electronically coupled quantum dots. Using realistic single quantum dot…

Mesoscale and Nanoscale Physics · Physics 2021-03-10 Alexander Mittelstädt , Ludwig A. Th. Greif , Stefan T. Jagsch , Andrei Schliwa

In this work we develop a theory of correlated many-electron dynamics dressed by the presence of a finite-temperature harmonic bath. The theory is based on the ab-initio Hamiltonian, and thus well-defined apart from any phenomenological…

Quantum Physics · Physics 2015-06-05 John A. Parkhill , Thomas Markovich , David G. Tempel , Alan Aspuru-Guzik

Starting from the random phase approximation for the weakly coupled multiband tightly-bounded electron systems, we calculate the dielectric matrix in terms of intraband and interband transitions. The advantages of this representation with…

Condensed Matter · Physics 2016-08-31 P. Zupanovic , A. Bjelis , S. Barisic

This report presents a new approach for treating the coupling of electrons and nuclei in quantum mechanical calculations for molecules and condensed matter. It includes the standard "Born-Oppenheimer approximation" as a special case but…

Chemical Physics · Physics 2013-06-28 Gerald I. Kerley

We present a method for the calculation of electronic structure of systems that contain tens of thousands of atoms. The method is based on the division of the system into mutually overlapping fragments and the representation of the…

Materials Science · Physics 2011-03-09 Nenad Vukmirović , Lin-Wang Wang

The screened electron-electron interaction in a multi-band electron system is calculated within the random phase approximation and in the tight-binding representation. The obtained dielectric matrix contains, beside the usual site-site…

Condensed Matter · Physics 2009-10-28 P. Zupanovic , A. Bjelis , S. Barisic

We study low-energy dynamics generated by a two-dimensional two-state Jahn-Teller Hamiltonian in the vicinity of a conical intersection using quantum wavepacket and trajectories dynamics. Recently, these dynamics were studied by comparing…

Chemical Physics · Physics 2024-02-06 Lea M. Ibele , Federica Agostini

Various non-trivial spaces are becoming popular for embedding structured data such as graphs, texts, or images. Following spherical and hyperbolic spaces, more general product spaces have been proposed. However, searching for the best…

Machine Learning · Computer Science 2022-04-11 Kirill Shevkunov , Liudmila Prokhorenkova

Ab initio modeling of conical intersection dynamics is crucial for various photochemical, photophysical, and biological processes. However, adiabatic electronic states obtained from electronic structure computations involve random phases,…

Chemical Physics · Physics 2024-06-13 Xiaotong Zhu , Bing Gu

A novel treatment of non-adiabatic couplings is proposed. The derivation starts from the long-known, but not well-known, fact that the wave function of the complete system of elctrons and nuclei can be written, without approximation, as a…

Materials Science · Physics 2007-05-23 Nikitas I. Gidopoulos , E. K. U. Gross

We present a high-accuracy procedure for electronic structure calculations of strongly correlated materials. To address limitations in current electronic structure methods, we employ density functional theory in combination with the…

The discrete variable local diabatic representation (LDR) provides a divergence-free framework for exact conical intersection dynamics simulation. In this work, we investigate the convergence with respect to the number of "nuclear" grid…

Chemical Physics · Physics 2026-05-25 Mo Sha , Bing Gu

We present an implementation of the GW approximation for the electronic self-energy within the full-potential linearized augmented-plane-wave (FLAPW) method. The algorithm uses an all-electron mixed product basis for the representation of…

Materials Science · Physics 2010-11-15 Christoph Friedrich , Stefan Blügel , Arno Schindlmayr

The theory of correlated electron systems is formulated in a form which allows to use as a reference point an ab initio band structure theory (AIBST). The theory is constructed in two steps. As a first step the total Hamiltonian is…

Strongly Correlated Electrons · Physics 2007-05-23 Igor Sandalov , Borje Johansson , Olle Eriksson

We investigate the construction of approximated exchange-correlation functionals by interpolating locally along the adiabatic connection between the weak- and the strong-coupling regimes, focussing on the effect of using approximate…

Chemical Physics · Physics 2017-04-05 Stefan Vuckovic , Lucas O. Wagner , Andrew M. Teale , Paola Gori-Giorgi

This work introduces a method for preprocessing measurements of electrical impedance tomography to considerably reduce the effect uncertainties in the electrode contacts have on the reconstruction quality, without a need to explicitly…

Numerical Analysis · Mathematics 2024-12-20 Altti Jääskeläinen , Jussi Toivanen , Asko Hänninen , Ville Kolehmainen , Nuutti Hyvönen
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