Accurate prediction of inverted singlet-triplet excited states using self-consistent spin-opposite perturbation theory
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arXiv
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| Natura: | Preprint |
| Pubblicazione: |
2026
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| _version_ | 1866915857255366656 |
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| author | Tran, Nhan Tri Nguyen, Hoang Thanh Tran, Lan Nguyen |
| author_facet | Tran, Nhan Tri Nguyen, Hoang Thanh Tran, Lan Nguyen |
| contents | The violation of Hund's rule, resulting in an inverted singlet-triplet (INVEST) gap, represents a paradigm shift in photophysics with major implications for OLED technology. INVEST molecules facilitate barrierless reverse intersystem crossing, theoretically permitting 100\% internal quantum efficiency without thermal activation. However, accurately predicting negative singlet-triplet energy gaps typically demands prohibitive computational costs. In this study, we evaluate the efficacy of our recently developed one-body Møller-Plesset perturbation theory (OBMP2) and its spin-opposite variant (O2BMP2) as efficient alternatives. Benchmarking against 30 INVEST molecules reveals that O2BMP2, with appropriate spin-opposite scaling, achieves the accuracy of ADC(3) and EOM-CCSD. Furthermore, with the possibility of reducing computational complexity to $N^4$, O2BMP2 provides a robust balance of accuracy and efficiency, making it suitable for the high-throughput screening of next-generation INVEST materials. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2603_11891 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Accurate prediction of inverted singlet-triplet excited states using self-consistent spin-opposite perturbation theory Tran, Nhan Tri Nguyen, Hoang Thanh Tran, Lan Nguyen Chemical Physics The violation of Hund's rule, resulting in an inverted singlet-triplet (INVEST) gap, represents a paradigm shift in photophysics with major implications for OLED technology. INVEST molecules facilitate barrierless reverse intersystem crossing, theoretically permitting 100\% internal quantum efficiency without thermal activation. However, accurately predicting negative singlet-triplet energy gaps typically demands prohibitive computational costs. In this study, we evaluate the efficacy of our recently developed one-body Møller-Plesset perturbation theory (OBMP2) and its spin-opposite variant (O2BMP2) as efficient alternatives. Benchmarking against 30 INVEST molecules reveals that O2BMP2, with appropriate spin-opposite scaling, achieves the accuracy of ADC(3) and EOM-CCSD. Furthermore, with the possibility of reducing computational complexity to $N^4$, O2BMP2 provides a robust balance of accuracy and efficiency, making it suitable for the high-throughput screening of next-generation INVEST materials. |
| title | Accurate prediction of inverted singlet-triplet excited states using self-consistent spin-opposite perturbation theory |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2603.11891 |