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Accurately modeling photochemical reactions is difficult due to the presence of conical intersections and locally avoided crossings as well as the inherently multiconfigurational character of excited states. As such, one needs a multi-state…

Chemical Physics · Physics 2024-04-26 Matthew R. Hennefarth , Matthew R. Hermes , Donald G. Truhlar , Laura Gagliardi

The second-order multireference driven similarity renormalization group perturbation theory (DSRG-MRPT2) theory provides an efficient means of correcting the dynamical correlation with the multiconfiguration reference function. The…

Chemical Physics · Physics 2022-02-01 Jae Woo Park

We consider the problem of sampling transition paths between two given metastable states of a molecular system, e.g. a folded and unfolded protein or products and reactants of a chemical reaction. Due to the existence of high energy…

Biomolecules · Quantitative Biology 2023-07-19 Lars Holdijk , Yuanqi Du , Ferry Hooft , Priyank Jaini , Bernd Ensing , Max Welling

Multichannel Quantum Defect Theory (MQDT) is shown to be capable of producing quantitatively accurate results for low-energy atom-molecule scattering calculations. With a suitable choice of reference potential and short-range matching…

Atomic Physics · Physics 2015-03-19 James F. E. Croft , Alisdair O. G. Wallis , Jeremy M. Hutson , Paul S. Julienne

Multiconfiguration pair-density functional theory (MC-PFDT) has previously been applied successfully to carry out ground-state and excited-state calculations. However, because it includes no interaction between electronic states, MC-PDFT…

In the realm of photochemistry, the significance of double excitations (also known as doubly-excited states), where two electrons are concurrently elevated to higher energy levels, lies in their involvement in key electronic transitions…

Chemical Physics · Physics 2024-07-15 Fábris Kossoski , Martial Boggio-Pasqua , Pierre-François Loos , Denis Jacquemin

Excitonic couplings between (bacterio)chlorophyll molecules are necessary for simulating energy transport in photosynthetic complexes. Many techniques for calculating the couplings are in use, from the simple (but inaccurate) point-dipole…

Chemical Physics · Physics 2016-02-09 Elise P. Kenny , Ivan Kassal

Multireference electron correlation methods describe static and dynamical electron correlation in a balanced way, and therefore, can yield accurate and predictive results even when single-reference methods or multiconfigurational…

Chemical Physics · Physics 2019-11-19 Jae Woo Park , Rachael Al-Saadon , Matthew K. MacLeod , Toru Shiozaki , Bess Vlaisavljevich

We develop an alternative formulation in the energy-domain to calculate the second order M{\o}ller-Plesset (MP2) perturbation energies. The approach is based on repeatedly choosing four random energies using a non-separable guiding…

Chemical Physics · Physics 2013-10-22 Qinghui Ge , Yi Gao , Roi Baer , Eran Rabani , Daniel Neuhauser

Accurate simulations of transient X-ray photoelectron spectra (XPS) provide unique opportunities to bridge the gap between theory and experiment in understanding the photoactivated dynamics in molecules and materials. However, simulating…

Chemical Physics · Physics 2024-06-19 Nicholas P. Gaba , Carlos E. V. de Moura , Rajat Majumder , Alexander Yu. Sokolov

We present relativistic many-body perturbation theory plus configuration interaction (MBPT+CI) calculations of the lowest four excited states of Ni$^{12+}$, a promising candidate for highly charged ion (HCI) optical clocks. By combining the…

Atomic Physics · Physics 2026-01-01 Shi-cheng Yu , Hua Guan , Lei She , Cheng-Bin Li

Accurately describing strong electron correlation in complex systems remains a prominent challenge in computational chemistry as near-term quantum algorithms treating total correlation often require prohibitively deep circuits. Here we…

Computational Engineering, Finance, and Science · Computer Science 2026-04-21 Zhanou Liu , Yuhao Chen , Yingjin Ma , Xiao He , Yuxin Deng

The computationally expensive evaluation and storage of high-rank reduced density matrices (RDMs) has been the bottleneck in the calculation of dynamic correlation for multireference wave functions in large active spaces. We present a…

Chemical Physics · Physics 2020-01-08 Ankit Mahajan , Nick S. Blunt , Iliya Sabzevari , Sandeep Sharma

We report the development of programs for on-the-fly surface hopping dynamics simulations in the gas and condensed phases on the potential energy surfaces computed by multistate multireference perturbation theory (XMS-CASPT2) with full…

Chemical Physics · Physics 2017-07-13 Jae Woo Park , Toru Shiozaki

Molecule- and particle-based simulations provide the tools to test, in microscopic detail, the validity of classical nucleation theory. In this endeavour, determining nucleation mechanisms and rates for phase separation requires an…

Materials Science · Physics 2023-02-27 Aaron R. Finney , Matteo Salvalaglio

A number of coupling strategies are presented for stochastically modeled biochemical processes with time-dependent parameters. In particular, the stacked coupling is introduced and is shown via a number of examples to provide an…

Numerical Analysis · Mathematics 2018-04-04 David F. Anderson , Chaojie Yuan

Theoretical studies of photochemical processes require a description of the energy surfaces of excited electronic states, especially near degeneracies, where transitions between states are most likely. Systems relevant to photochemical…

Transition metal dichalcogenides (TMDCs) have demonstrated significant potential as versatile quantum materials for light absorption and emission. Their unique properties are primarily governed by exciton-photon interactions, which can be…

An alternative methodology to investigate indirect polyatomic processes with quasi-classical trajectories is proposed, which effectively avoids any binning or weighting procedure while provides rovibrational resolution. Initial classical…

Multi-molecular excited states accompanied by an intra- and inter-molecular geometric relaxation are commonly encountered in optical and electrooptical studies and applications of organic semiconductors as, for example excimers or charge…

Materials Science · Physics 2022-11-14 Sebastian Hammer , Theresa Linderl , Kristofer Tvingstedt , Wolfgang Brütting , Jens Pflaum