Accurate and efficient DFT-based diabatization for hole and electron transfer using absolutely localized molecular orbitals.

  title={Accurate and efficient DFT-based diabatization for hole and electron transfer using absolutely localized molecular orbitals.},
  author={Yuezhi Mao and Andr{\'e}s Montoya-Castillo and Thomas E. Markland},
  journal={The Journal of chemical physics},
  volume={151 16},
Diabatic states and the couplings between them are important for quantifying, elucidating, and predicting the rates and mechanisms of many chemical and biochemical processes. Here, we propose and investigate approaches to accurately compute diabatic couplings from density functional theory (DFT) using absolutely localized molecular orbitals (ALMOs). ALMOs provide an appealing approach to generate variationally optimized diabatic states and obtain their associated forces, which allows for the… 
10 Citations

Improved Projection-Operator Diabatization Schemes for the Calculation of Electronic Coupling Values.

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Path Integral Quantum Mechanics: from the basics to the latest developments

This work is part of a joint doctoral program in condensed matter physics and theoretical chemistry that aims at simulating the quantum dynamics of light nuclei in materials and molecular systems.


Professor Tom Markland focuses on problems at the interface of quantum mechanics and statistical mechanics, with applications ranging from chemistry and biology to geology and materials science, and quantum mechanical effects.



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An analytic expression for the forces in constrained DFT and their implementation in geometry optimization is presented, a prerequisite for the calculation of electron transfer parameters.

Electronic Couplings for Charge Transfer across Molecule/Metal and Molecule/Semiconductor Interfaces: Performance of the Projector Operator-Based Diabatization Approach

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