Stochastic Models for Non-Linear/Many-Body Dynamics in Molecular Semiconductors

点击翻译按钮获取中文摘要

Professor Eric Bittner of the University of Houston is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry. to model dark background dynamics that contribute to dephasing and spectral diffusion in complex semiconducting systems as revealed in coherent multi-dimensional spectroscopy. This work aims to facilitate the next significant breakthroughs in fundamental aspects of coherent non-linear spectroscopy as applied to condensed-matter physics, materials science, and ultimately, in quantum optoelectronic technologies in a broader context. The optimal choice of materials for such novel technologies relies on a profound understanding of correlated many-body dynamics as manifest in multi-dimensional spectral probes. This project develops key aspects of Quantum Leap by exploiting quantum entanglement of photons to unravel underpinning many-body correlations and hidden-layer dynamics.Spectroscopic line-shapes reveal a wealth of information concerning the underlying background dynamics a system is experiencing. In this project, Bittner proposes the use of quantum stochastic equations and Ito calculus to model dark background dynamics that contribute to dephasing and spectral diffusion in complex semiconducting systems as revealed in coherent multi-dimensional spectroscopy. Theoretical advances include the use of correlated noise and non-commutative noise to model the influence of various background environments on spectroscopic signals. Proposed applications of the work include exciton and bi-exciton dynamics in hybrid organic/inorganic layered semiconductors, semiconducting organic polymers, and DNA-wrapped Carbon nanorods. The work advances the notion that exciton dynamics can be cross-correlated via hidden-layer background processes. Bittner seeks to quantify these as manifest in 2D coherent non-linear spectroscopic signals. The work also advances the use of quantum entangled photons as a probe of many-body dynamics. Previous studies suggest that entanglement can be generated via indirect coupling of emitters to a common or correlated environment. Bittner will explore this idea with the goal developing novel quantum spectroscopies and/or generation of custom entanglements.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.