A Further Comparison of MPS and TTNS for Nonadiabatic Dynamics of Exciton Dissociation

Fuente: arXiv
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Main Authors: Li, Weitang, Ren, Jiajun, Yan, Jun
Format: Preprint
Published: 2025
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author Li, Weitang
Ren, Jiajun
Yan, Jun
author_facet Li, Weitang
Ren, Jiajun
Yan, Jun
contents Tensor networks, such as matrix product states (MPS) and tree tensor network states (TTNS), are powerful ansätze for simulating quantum dynamics. While both ansätze are theoretically exact in the limit of large bond dimensions, [J. Chem. Theory Comput. 2024, 20, 8767-8781] reported a non-negligible discrepancy in its calculations for exciton dissociation. To resolve this inconsistency, we conduct a systematic comparison using Renormalizer, a unified software framework for MPS and TTNS. By revisiting the benchmark P3HT:PCBM heterojunction model, we show that the observed discrepancies arise primarily from insufficient bond dimensions. By increasing bond dimensions, we reduce the relative difference in occupancy for weakly populated electronic states from up to 60% towards the end of the simulation to less than 10% and the absolute difference from 0.05 to 0.005. We also discuss the impact of tensor network structures on accuracy and efficiency, with the difference further reduced by an optimized TTNS structure. Our results confirm that both methods converge to numerically exact solutions when bond dimensions are adequately scaled. This work not only validates the reliability of both methods but also provides high-accuracy benchmark data for future developments in quantum dynamics simulations.
format Preprint
id arxiv_https___arxiv_org_abs_2509_00456
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle A Further Comparison of MPS and TTNS for Nonadiabatic Dynamics of Exciton Dissociation
Li, Weitang
Ren, Jiajun
Yan, Jun
Chemical Physics
Materials Science
Quantum Physics
Tensor networks, such as matrix product states (MPS) and tree tensor network states (TTNS), are powerful ansätze for simulating quantum dynamics. While both ansätze are theoretically exact in the limit of large bond dimensions, [J. Chem. Theory Comput. 2024, 20, 8767-8781] reported a non-negligible discrepancy in its calculations for exciton dissociation. To resolve this inconsistency, we conduct a systematic comparison using Renormalizer, a unified software framework for MPS and TTNS. By revisiting the benchmark P3HT:PCBM heterojunction model, we show that the observed discrepancies arise primarily from insufficient bond dimensions. By increasing bond dimensions, we reduce the relative difference in occupancy for weakly populated electronic states from up to 60% towards the end of the simulation to less than 10% and the absolute difference from 0.05 to 0.005. We also discuss the impact of tensor network structures on accuracy and efficiency, with the difference further reduced by an optimized TTNS structure. Our results confirm that both methods converge to numerically exact solutions when bond dimensions are adequately scaled. This work not only validates the reliability of both methods but also provides high-accuracy benchmark data for future developments in quantum dynamics simulations.
title A Further Comparison of MPS and TTNS for Nonadiabatic Dynamics of Exciton Dissociation
topic Chemical Physics
Materials Science
Quantum Physics
url https://arxiv.org/abs/2509.00456