Physical Sciences and Mathematics Commons^™

Designing, Constructing, And Employing Two-Dimensional Ultrafast Spectroscopy To Resolve Complex Kinetics, Jason R. Darvin

Theses and Dissertations

Multiple population-period transient spectroscopy (MUPPETS) is a two dimensional ultrafast time resolved spectroscopy technique. MUPPETS uses three pairs of optical pulses over two time periods to separate homogeneous and heterogeneous causes of rate dispersion. This dissertation details improvements to the MUPPETS optical assembly enabling measurements on systems that previously fell outside of the MUPPETS 2-ns time window. In addition, the theoretical groundwork is laid to unveil the hidden coordinate controlling rate exchange using 2D and 3D correlation functions.

The first project details improvements made to the MUPPETS assembly. A detailed method was developed to eliminate astigmatism, coma, and spherical aberration …

Two-Dimensional Transient Spectroscopy Measuring Heterogeneity In Electronic And Rotational Dynamics, Haorui Wu

Theses and Dissertations

Multiple population-period transient spectroscopy (MUPPETS) is a picosecond, time resolved experiment that uses a sequence of six laser pulses. It was previously known that MUPPETS could measure heterogeneity in electronic-state decay. This dissertation presents two projects that extend MUPPETS to new processes. One process is the extension from 2-level system into 3-level system, another new process extends the kinetics from electronic decay to rotational decay. In addition, a third, ongoing project on rotational dynamics in ionic liquids will also be discussed briefly. The first project consisted of two main parts. The first part focused on the biexciton decay in semiconductor …