Complex potential energy surfaces: gradients with projected CAP technique

The complex absorbing potential (CAP) technique is one of the commonly used Non-Hermitian quantum mechanics approaches for characterizing electronic resonances. CAP combined with various electronic structure methods has shown promising results in quantifying the energies and widths of electronic resonances in molecular systems. While CAP-based methods can be used to map complex potential energy surfaces for resonance states, efficient exploration of these surfaces, e.g. geometry optimization or dynamical simulations, require information on the nuclear gradient. Currently, the only nuclear gradients available for CAP-based methods are for Hartree-Fock and Equation-of-Motion Coupled-Cluster method with single and double excitations (J. Chem. Phys. 146, 031101 (2017)). Here we provide a general approach that relies on projected CAP formulation and extends gradients and non-adiabatic couplings formulations developed for bound-state electronic structure methods to resonances. The approach is not limited to a specific electron structure method and is generally applicable to any electronic structure methods, provided the information on the gradients and non-adiabatic couplings is available for bound states. Here, we focus on the State-Averaged Complete Active Space Self-Consistent Field (SA-CASSCF) and Multi-Reference Configurational Interaction with Single excitation (MR-CIS) as our methods of choice. We establish the accuracy of the developed gradients and report equilibrium geometries for several representative temporary anion species ($\mathrm{N_2^-}$, $\mathrm{H_2CO^-}$, $\mathrm{H_2CO_2^-}$ and $\mathrm{C_2H_4^-}$).

Publication Details

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ArXiv.org
Published
2025-03-06
Primary Topic
Advanced Chemical Physics Studies
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article
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article

Complex potential energy surfaces: gradients with projected CAP technique

ArXiv.org
Advanced Chemical Physics Studies
article

Complex potential energy surfaces: gradients with projected CAP technique

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Abstract

The complex absorbing potential (CAP) technique is one of the commonly used Non-Hermitian quantum mechanics approaches for characterizing electronic resonances. CAP combined with various electronic structure methods has shown promising results in quantifying the energies and widths of electronic resonances in molecular systems. While CAP-based methods can be used to map complex potential energy surfaces for resonance states, efficient exploration of these surfaces, e.g. geometry optimization or dynamical simulations, require information on the nuclear gradient. Currently, the only nuclear gradients available for CAP-based methods are for Hartree-Fock and Equation-of-Motion Coupled-Cluster method with single and double excitations (J. Chem. Phys. 146, 031101 (2017)). Here we provide a general approach that relies on projected CAP formulation and extends gradients and non-adiabatic couplings formulations developed for bound-state electronic structure methods to resonances. The approach is not limited to a specific electron structure method and is generally applicable to any electronic structure methods, provided the information on the gradients and non-adiabatic couplings is available for bound states. Here, we focus on the State-Averaged Complete Active Space Self-Consistent Field (SA-CASSCF) and Multi-Reference Configurational Interaction with Single excitation (MR-CIS) as our methods of choice. We establish the accuracy of the developed gradients and report equilibrium geometries for several representative temporary anion species ($\mathrm{N_2^-}$, $\mathrm{H_2CO^-}$, $\mathrm{H_2CO_2^-}$ and $\mathrm{C_2H_4^-}$).

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Complex potential energy surfaces: gradients with projected CAP technique · ArXiv.org (2025) | TGRS Research Map | TGRS