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Ultrafast Coherent Control Spectroscopy

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dc.contributor.advisor Weinacht, Thomas C en_US
dc.contributor.author Tseng, Chien-hung en_US
dc.contributor.other Department of Physics en_US
dc.date.accessioned 2013-05-22T17:35:43Z
dc.date.accessioned 2015-04-24T14:47:35Z
dc.date.available 2013-05-22T17:35:43Z
dc.date.available 2015-04-24T14:47:35Z
dc.date.issued 2012-05-01 en_US
dc.identifier Tseng_grad.sunysb_0771E_10841 en_US
dc.identifier.uri http://hdl.handle.net/1951/59896 en_US
dc.identifier.uri http://hdl.handle.net/11401/71444 en_US
dc.description 110 pg. en_US
dc.description.abstract Coherent control of quantum systems is currently a very active area of research in physics and chemistry. The goal of coherent control is to prepare molecules in specic quantum states that can lead to different chemical reactions, e.g. fragmentation and isomerization. One approach is the control of interference between multiple quantum pathways via their phases from the initial to the final state which consequently excites one molecular state or molecule over another with shaped pulses. The other approach is to generate different reaction products with pulses that match specic transient Franck Condon windows and transfer the wavepacket in a precise phase of vibrational motion to a new electronic state. Recently, there are increasing applications of coherent control towards cellular imaging. It is especially benecial for distinguishing broadband fluorophores with similar two-photon absorption crosssections, e.g. for free and enzyme-bound nicotinamide adenine dinucleotide (NADH). In this thesis, we discriminate between samples containing either free NADH or enzyme-bound NADH solutions with pulses that have a phase jump at a given frequency within the excitation bandwidth. This parameter scan is sensitive to as low as 3% of binding. The same idea can be generalized to other two-photon fluorescence systems, and a closed-loop feedback control approach should allow even wider application. We also develop two-dimensional (2D) Fourier transform spectroscopy in the deep UV (262 nm) to study DNA bases excited state relaxation dynamics. We compare 2D spectroscopy measurements in the deep UV for monomeric adenine and uracil in aqueous solutions. Both molecules show excited state absorption on short timescales and ground state bleach extending for over 1 ps. While the 2D spectrum for uracil shows changes in the center of gravity during the first few hundred femtoseconds, the center of gravity of the 2D spectrum for adenine does not show similar changes. We discuss our results in light of ab initio electronic structure calculations. en_US
dc.description.sponsorship This work is sponsored by the Stony Brook University Graduate School in compliance with the requirements for completion of degree. en_US
dc.format Monograph en_US
dc.format.medium Electronic Resource en_US
dc.language.iso en_US en_US
dc.publisher The Graduate School, Stony Brook University: Stony Brook, NY. en_US
dc.subject.lcsh Physics--Optics--Atomic physics en_US
dc.title Ultrafast Coherent Control Spectroscopy en_US
dc.type Dissertation en_US
dc.mimetype Application/PDF en_US
dc.contributor.committeemember Schneble, Dominik en_US
dc.contributor.committeemember Fernandez-Serra, Maria V en_US
dc.contributor.committeemember Ruhman, Sanford. en_US

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