dc.contributor.author | Hsieh, Chang Yu | |
dc.contributor.author | Cao, Jianshu | |
dc.date.accessioned | 2018-01-22T14:58:55Z | |
dc.date.available | 2018-01-22T14:58:55Z | |
dc.date.issued | 2018-01 | |
dc.date.submitted | 2017-01 | |
dc.identifier.issn | 0021-9606 | |
dc.identifier.issn | 1089-7690 | |
dc.identifier.uri | http://hdl.handle.net/1721.1/113246 | |
dc.description.abstract | We use the "generalized hierarchical equation of motion" proposed in Paper I [C.-Y. Hsieh and J. Cao, J. Chem. Phys. 148, 014103 (2018)] to study decoherence in a system coupled to a spin bath. The present methodology allows a systematic incorporation of higher-order anharmonic effects of the bath in dynamical calculations. We investigate the leading order corrections to the linear response approximations for spin bath models. Two kinds of spin-based environments are considered: (1) a bath of spins discretized from a continuous spectral density and (2) a bath of localized nuclear or electron spins. The main difference resides with how the bath frequency and the system-bath coupling parameters are distributed in an environment. When discretized from a continuous spectral density, the system-bath coupling typically scales as ∼1/NB where N B is the number of bath spins. This scaling suppresses the non-Gaussian characteristics of the spin bath and justifies the linear response approximations in the thermodynamic limit. For the nuclear/electron spin bath models, system-bath couplings are directly deduced from spin-spin interactions and do not necessarily obey the 1/NB scaling. It is not always possible to justify the linear response approximations in this case. Furthermore, if the spin-spin Hamiltonian is highly symmetrical, there exist additional constraints that generate highly non-Markovian and persistent dynamics that is beyond the linear response treatments. | en_US |
dc.description.sponsorship | National Science Foundation (U.S.) (Grant CHE-1112825) | en_US |
dc.publisher | American Institute of Physics (AIP) | en_US |
dc.relation.isversionof | http://dx.doi.org/10.1063/1.5018726 | en_US |
dc.rights | Creative Commons Attribution-Noncommercial-Share Alike | en_US |
dc.rights.uri | http://creativecommons.org/licenses/by-nc-sa/4.0/ | en_US |
dc.source | arXiv | en_US |
dc.title | A unified stochastic formulation of dissipative quantum dynamics. II. Beyond linear response of spin baths | en_US |
dc.type | Article | en_US |
dc.identifier.citation | Hsieh, Chang-Yu, and Cao, Jianshu. “A Unified Stochastic Formulation of Dissipative Quantum Dynamics. II. Beyond Linear Response of Spin Baths.” The Journal of Chemical Physics 148, 1 (January 2018): 014104 © 2018 Author(s) | en_US |
dc.contributor.department | Massachusetts Institute of Technology. Department of Chemistry | en_US |
dc.contributor.mitauthor | Hsieh, Chang Yu | |
dc.contributor.mitauthor | Cao, Jianshu | |
dc.relation.journal | Journal of Chemical Physics | en_US |
dc.eprint.version | Original manuscript | en_US |
dc.type.uri | http://purl.org/eprint/type/JournalArticle | en_US |
eprint.status | http://purl.org/eprint/status/NonPeerReviewed | en_US |
dc.date.updated | 2018-01-17T17:19:53Z | |
dspace.orderedauthors | Hsieh, Chang-Yu; Cao, Jianshu | en_US |
dspace.embargo.terms | N | en_US |
dc.identifier.orcid | https://orcid.org/0000-0002-3931-001X | |
dc.identifier.orcid | https://orcid.org/0000-0001-7616-7809 | |
mit.license | OPEN_ACCESS_POLICY | en_US |