Public Abstract

DE-SC0017889: Light-Induced Spin Trapping in Transition Metal Compounds

Award Status: Inactive

Institution: Michigan State University, East Lansing, MI
UEI: R28EKN92ZTZ9
DUNS: 193247145

Most Recent Award Date: 08/13/2021
Number of Support Periods: 3
PM: Holder, Aaron

Current Budget Period: 09/01/2019 - 08/31/2022
Current Project Period: 09/01/2017 - 08/31/2022
PI: Wilson, Angela

Supplement Budget Period: N/A

Public Abstract

Light-Induced Spin Trapping in Transition Metal Compounds Angela K. Wilson and Inga S. Ulusoy Department of Chemistry, Michigan State University Transition metal complexes are used in a large variety of applications in areas such as energy conversion and information technology. They are used in dye-sensitized solar cells (DSSCs) where a number of their unique properties, including their ability to absorb light enable their light harvesting efficiency, are important. As well, transition metal species have many applications in green chemistry due to their photocatalytic behavior - their ability to accelerate photochemical reactions. To improve upon these applications such as in identifying promising candidates to replace expensive transition metal compounds currently used in DSSCs, the ability to tune electronic properties and light-matter interactions of transition metal compounds, specifically, a class of transition metal compounds called spin-crossover (SCO) compounds, to their targeted use is essential. In this work, theoretical methods will be developed to enable insights into the electronic excitation pathways of transition metal species when irradiated by light. This will enable an effective and efficient tailoring and development of SCO compounds to their targeted applications. The theoretical methods that will be developed, extended, and employed include both time-independent and time dependent quantum mechanical approaches using both configuration interaction (CI) and time-dependent configuration interaction (TDCI) methods, enabling the progress of a reaction over time and subjected to an electric field, to be examined. Accurate and detailed information about the coupling of the electronic states, their interaction with electromagnetic fields, and influencing factors such as pressure, temperature, or ligand type, in spin-transition and spin-trapping processes will be gained. Factors that govern the excitation and de-excitation mechanisms in the compounds will be discerned, thus helping intelligent design of SCO compounds for future applications.

Light-Induced Spin Trapping in Transition Metal Compounds

Angela K. Wilson and Inga S. Ulusoy

Department of Chemistry, Michigan State University

Transition metal complexes are used in a large variety of applications in areas such as energy conversion and information technology. They are used in dye-sensitized solar cells (DSSCs) where a number of their unique properties, including their ability to absorb light enable their light harvesting efficiency, are important. As well, transition metal species have many applications in green chemistry due to their photocatalytic behavior - their ability to accelerate photochemical reactions. To improve upon these applications such as in identifying promising candidates to replace expensive transition metal compounds currently used in DSSCs, the ability to tune electronic properties and light-matter interactions of transition metal compounds, specifically, a class of transition metal compounds called spin-crossover (SCO) compounds, to their targeted use is essential. In this work, theoretical methods will be developed to enable insights into the electronic excitation pathways of transition metal species when irradiated by light. This will enable an effective and efficient tailoring and development of SCO compounds to their targeted applications.

The theoretical methods that will be developed, extended, and employed include both time-independent and time dependent quantum mechanical approaches using both configuration interaction (CI) and time-dependent configuration interaction (TDCI) methods, enabling the progress of a reaction over time and subjected to an electric field, to be examined. Accurate and detailed information about the coupling of the electronic states, their interaction with electromagnetic fields, and influencing factors such as pressure, temperature, or ligand type, in spin-transition and spin-trapping processes will be gained. Factors that govern the excitation and de-excitation mechanisms in the compounds will be discerned, thus helping intelligent design of SCO compounds for future applications.