Nonadiabatic Dynamics with Spin-orbit Coupling / Nicole I Bellonzi.

Format:

Book

Thesis/Dissertation

Author/Creator:

Bellonzi, Nicole I., author.

Contributor:

Subotnik, Joseph E., degree supervisor.

University of Pennsylvania. Department of Chemistry, degree granting institution.

Language:

English

Subjects (All):

Physical chemistry.

Chemistry.

Computational chemistry.

Chemistry--Penn dissertations.

Penn dissertations--Chemistry.

Local Subjects:

Physical chemistry.

Chemistry.

Computational chemistry.

Chemistry--Penn dissertations.

Penn dissertations--Chemistry.

Genre:

Academic theses.

Physical Description:

1 online resource (172 pages)

Contained In:

Dissertations Abstracts International 81-04B.

Place of Publication:

[Philadelphia, Pennsylvania] : University of Pennsylvania ; Ann Arbor : ProQuest Dissertations & Theses, 2019.

Language Note:

English

System Details:

Mode of access: World Wide Web.

text file

Summary:

After photoexcitation, molecules can follow many different paths for electronic relaxation. Of these paths, electronic transitions between states of different spin-multiplicities, intersystem crossings, have largely been ignored in many systems because of their spin-forbidden nature, but recent work has shown that intersystem crossings can occur at short times and compete with other relaxation pathways. Understanding these complicated excited state processes requires both advanced excited state dynamics algorithms and excited state electronic structure. In the first part of the work presented here, we investigate a variety of inexpensive, mixed quantum-classical approaches for nonadiabatic dynamics. We find that modern approaches have made great advances but may lead to instabilities when unphysical trajectories are included. In the second part of this work, methods are developed for the requisite electronic structure for nonadiabatic dynamics with spin-orbit coupling. We present a computationally efficient algorithm for computing the energies, analytic gradients and nonadiabatic derivative couplings of spin-adiabatic states corresponding to configuration interaction singles or time-dependent density functional theory incorporating spin-orbit couplings. We expect this algorithm will be useful for future exploration of intersystem crossings in real molecular systems.

Notes:

Source: Dissertations Abstracts International, Volume: 81-04, Section: B.

Advisors: Subotnik, Joseph E.; Committee members: Abraham Nitzan; Jessica Anna; Andrew Rappe.

Department: Chemistry.

Ph.D. University of Pennsylvania 2019.

Local Notes:

School code: 0175

ISBN:

9781088336830

Access Restriction:

Restricted for use by site license.

This item is not available from ProQuest Dissertations & Theses.

This item must not be sold to any third party vendors.