Nonlinear Ultrafast Spectroscopy of Electron and Energy Transfer in Molecule Complexes
The proposed research program will focus on the development of a unified dynamical theoretical framework for calculating the optical response of molecular assemblies and applying it towards studying the interplay of energy and charge transfer in artificial chromophore-aggregate complexes. Applications will be made to poly (p phenylene vinylene), (PPV) oligomers, several families of stilbenoid aggregates with stacking through a cyclophane group, coupled porphyrin arrays, and energy funneling in phenylacetylene dendrimers. The approach is based on formulating the problem using the density- matrix and developing Liouville-space techniques which provide physical insight and are particularly suitable for computing both coherent and incoherent transport. A physical picture based on collective electronic normal modes which represent the dynamics of the optically-driven reduced single electron density matrix will be established. Femtosecond signals and optical properties will be directly related to the motions of electron-hole pairs in real space, completely avoiding the calculation of many-electron excited-state wavefunctions, thus, considerably reducing computational effort. Vibrational and solvent effects will be incorporated. Guidelines for the synthesis of new donor/bridge/acceptor molecules with desired properties such as carrier transport, optical response time scales and fluorescence quantum yields will be developed. The analogy with Thz emission spectroscopy which probes charge carrier dynamic is in semiconductor superlattices will be explored. A systematic procedure for identifying the electronic coherence sizes which control the transport and optical properties will be developed. Localization of electronic transition density matrices of large molecules will be used to break the description of their optical response into coupled chromophores. The proposal is divided into four parts: (i) Collective-Oscillator Representation of Electronic Excitations in Molecular Assemblies; (ii) Nonlinear Optical Spectroscopy of Coupled Chromophores; (iii) Long-Range Electron Transfer and Transport in Solvents with Complex Spectral Densities; (iv) Probing Exciton-Migration by Coherent Femtosecond Spectroscopies.
- Research Organization:
- University of Rochester, NY (US)
- Sponsoring Organization:
- USDOE Office of Science (SC)
- DOE Contract Number:
- FG02-01ER15155
- OSTI ID:
- 875998
- Report Number(s):
- DOE/ER/15155-3; TRN: US200711%%246
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
36 MATERIALS SCIENCE
75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
CHARGE CARRIERS
ELECTRON DENSITY
ELECTRON TRANSFER
ELECTRONS
EMISSION SPECTROSCOPY
ENERGY TRANSFER
FLUORESCENCE
MATRICES
OPTICAL PROPERTIES
PORPHYRINS
PROBES
RESEARCH PROGRAMS
SOLVENTS
SPECTROSCOPY
SUPERLATTICES
SYNTHESIS
TOLAN
TRANSPORT
Energy transfer
Chromophore aggreates
Electron transfer
Non-linear optical properties