التفاصيل البيبلوغرافية
| العنوان: |
Pure State v-Representability of Density Matrix Embedding Theory |
| المؤلفون: |
Faulstich, Fabian M., Kim, Raehyun, Cui, Zhi-Hao, Wen, Zaiwen, Chan, Garnet Kin-Lic, Lin, Lin |
| المصدر: |
Journal of Chemical Theory and Computation, 18(2), 851-864, (2022-02-08) |
| بيانات النشر: |
American Chemical Society |
| سنة النشر: |
2022 |
| المجموعة: |
Caltech Authors (California Institute of Technology) |
| مصطلحات موضوعية: |
Impurities, Algorithms, Optimization, Lagrangians, Energy, Physical and Theoretical Chemistry, Computer Science Applications |
| الوصف: |
Density matrix embedding theory (DMET) formally requires the matching of density matrix blocks obtained from high-level and low-level theories, but this is sometimes not achievable in practical calculations. In such a case, the global band gap of the low-level theory vanishes, and this can require additional numerical considerations. We find that both the violation of the exact matching condition and the vanishing low-level gap are related to the assumption that the high-level density matrix blocks are noninteracting pure-state v-representable (NI-PS-V), which assumes that the low-level density matrix is constructed following the Aufbau principle. To relax the NI-PS-V condition, we develop an augmented Lagrangian method to match the density matrix blocks without referring to the Aufbau principle. Numerical results for the 2D Hubbard and hydrogen model systems indicate that, in some challenging scenarios, the relaxation of the Aufbau principle directly leads to exact matching of the density matrix blocks, which also yields improved accuracy. ; © 2022 American Chemical Society. Received 21 October 2021. Published online 27 January 2022. This work was partially supported by the Air Force Office of Scientific Research under award number FA9550-18-1-0095 (G.K.-L.C. and L.L.), and by the Department of Energy under grant no. DE-SC0017867 (F.M.F. and R.K.) and under grant no. DE-SC0018140 (Z.-H.C.). Z.-H.C. acknowledges support from the Eddleman Quantum Institute through a graduate research fellowship. G.K.-L.C. and L.L. are Simons Investigators. Author Contributions: F.M.F. and R.K. contributed equally. The authors declare no competing financial interest. |
| نوع الوثيقة: |
article in journal/newspaper |
| اللغة: |
unknown |
| العلاقة: |
https://doi.org/10.1021/acs.jctc.1c01061Test; oai:authors.library.caltech.edu:n9dda-zzj89; eprintid:113233; resolverid:CaltechAUTHORS:20220202-544261000 |
| DOI: |
10.1021/acs.jctc.1c01061 |
| الإتاحة: |
https://doi.org/10.1021/acs.jctc.1c01061Test |
| حقوق: |
info:eu-repo/semantics/closedAccess ; Other |
| رقم الانضمام: |
edsbas.269EAF91 |
| قاعدة البيانات: |
BASE |
