Transformation-Free Generation of a Quasi-Diabatic Representation from the State-Average Orbital-Optimized Variational Quantum Eigensolver DOI
Silvie Illésová, Martin Beseda, Saad Yalouz

et al.

Journal of Chemical Theory and Computation, Journal Year: 2025, Volume and Issue: unknown

Published: May 23, 2025

In the present work, we examine how recent quantum-computing algorithm known as state-average orbital-optimized variational quantum eigensolver (SA-OO-VQE), viewed within context of chemistry a type multiconfiguration self-consistent field (MCSCF) electronic-structure approach, exhibits propensity to produce an ab initio quasi-diabatic representation "for free" if considered least-transformed block-diagonalization procedure, alluded in our previous work (Yalouz, S. et al. J. Chem. Theory Comput. 2022, 18, 776-794) and thoroughly assessed herein. To this end, introduce intrinsic residual descriptors diabaticity re-explore definition linear-algebra properties, well their consequences on vibronic nonadiabatic couplings, optimal diabatic much one may deviate from it. Such considerations are illustrated numerically prototypical case formaldimine, which presents well-known conical intersection between its ground first-excited singlet electronic states.

Language: Английский

Simulating Non-Markovian Quantum Dynamics on NISQ Computers Using the Hierarchical Equations of Motion DOI
Xiaohan Dan, Eitan Geva, Víctor S. Batista

et al.

Journal of Chemical Theory and Computation, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 14, 2025

Quantum computing offers promising new avenues for tackling the long-standing challenge of simulating quantum dynamics complex chemical systems, particularly open systems coupled to external baths. However, such nonunitary on computers is challenging since circuits are specifically designed carry out unitary transformations. Furthermore, often strongly surrounding environment, rendering non-Markovian and beyond scope Markovian master equations like Lindblad or Redfield. In this work, we introduce a algorithm simulate systems. Our approach enables implementation arbitrary noisy intermediate-scale (NISQ) computers. We illustrate method as applied in conjunction with numerically exact hierarchical motion (HEOM) method. The effectiveness resulting HEOM demonstrated simulations non-Lindbladian electronic energy charge transfer models carotenoid-porphyrin-C60 molecular triad dissolved tetrahydrofuran Fenna–Matthews–Olson complex.

Language: Английский

Citations

1
Transformation-Free Generation of a Quasi-Diabatic Representation from the State-Average Orbital-Optimized Variational Quantum Eigensolver DOI
Silvie Illésová, Martin Beseda, Saad Yalouz

et al.

Journal of Chemical Theory and Computation, Journal Year: 2025, Volume and Issue: unknown

Published: May 23, 2025

In the present work, we examine how recent quantum-computing algorithm known as state-average orbital-optimized variational quantum eigensolver (SA-OO-VQE), viewed within context of chemistry a type multiconfiguration self-consistent field (MCSCF) electronic-structure approach, exhibits propensity to produce an ab initio quasi-diabatic representation "for free" if considered least-transformed block-diagonalization procedure, alluded in our previous work (Yalouz, S. et al. J. Chem. Theory Comput. 2022, 18, 776-794) and thoroughly assessed herein. To this end, introduce intrinsic residual descriptors diabaticity re-explore definition linear-algebra properties, well their consequences on vibronic nonadiabatic couplings, optimal diabatic much one may deviate from it. Such considerations are illustrated numerically prototypical case formaldimine, which presents well-known conical intersection between its ground first-excited singlet electronic states.

Language: Английский

Citations

0