Coherent multi-exciton dynamics in semiconductor nanostructures via two-dimensional Fourier transform optical spectroscopy
Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Chemistry, 2009.
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| Format: | Thesis |
| Language: | eng |
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Massachusetts Institute of Technology
2009
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| Online Access: | http://hdl.handle.net/1721.1/49554 |
| _version_ | 1826203545172443136 |
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| author | Stone, Katherine Walowicz |
| author2 | Keith A. Nelson. |
| author_facet | Keith A. Nelson. Stone, Katherine Walowicz |
| author_sort | Stone, Katherine Walowicz |
| collection | MIT |
| description | Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Chemistry, 2009. |
| first_indexed | 2024-09-23T12:38:42Z |
| format | Thesis |
| id | mit-1721.1/49554 |
| institution | Massachusetts Institute of Technology |
| language | eng |
| last_indexed | 2024-09-23T12:38:42Z |
| publishDate | 2009 |
| publisher | Massachusetts Institute of Technology |
| record_format | dspace |
| spelling | mit-1721.1/495542019-04-11T06:31:05Z Coherent multi-exciton dynamics in semiconductor nanostructures via two-dimensional Fourier transform optical spectroscopy Stone, Katherine Walowicz Keith A. Nelson. Massachusetts Institute of Technology. Dept. of Chemistry. Massachusetts Institute of Technology. Dept. of Chemistry. Chemistry. Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Chemistry, 2009. This electronic version was submitted by the student author. The certified thesis is available in the Institute Archives and Special Collections. Includes bibliographical references (p. 139-149). The Coulomb correlations between photoexcited charged particles in materials such as photosynthetic complexes, conjugated polymer systems, J-aggregates, and bulk or nanostructured semiconductors produce a hierarchy of collective electronic excitations (i.e. excitons, biexcitons, etc.) which may be harnessed for applications in quantum optics, light-harvesting, or quantum information technologies. These excitations represent correlations among successively greater numbers of electrons and holes, and their associated multiple-quantum coherences could reveal detailed information about complex many-body interactions and dynamics. However, unlike single-quantum coherences involving excitons, multiple-quantum coherences do not radiate and they have largely eluded direct observation and characterization. In this work, I present a novel optical technique, two-quantum two-dimensional Fourier transform optical spectroscopy, which allows direct observation of the dynamics of multiple-exciton states that reflect the correlations of their constituent electrons and holes. The approach is based on closely analogous methods in nuclear magnetic resonance, in which multiple phase-coherent fields are used to drive successive transitions such that multiple-quantum coherences can be accessed and probed. A spatiotemporal femtosecond pulse shaping technique has been used to overcome the challenge of control over multiple, noncollinear phase-coherent optical Fields in the experimental geometries that are used to isolate selected signal contributions through wavevector matching. (cont.) Results from a GaAs quantum well system reveal distinct coherences of biexcitons that are formed from two identical excitons or from two excitons whose holes are in di®erent spin sublevels ("heavy-hole" and "light-hole" excitons). The biexciton binding energies and dephasing dynamics are determined, and changes in the dephasing rates as a function of the excitation density are observed, revealing still higher-order correlations due to exciton-biexciton interactions. Two-quantum coherences due to four-particle correlations that do not involve bound biexciton states but that in°uence the exciton properties are also observed and characterized. I also present one-quantum two-dimensional Fourier transform optical spectroscopy measurements which show that the higher-order correlations isolated by two-quantum techniques are highly convolved with two-particle correlations in the conventional one-quantum measurements. by Katherine Walowicz Stone. Ph.D. 2009-11-06T14:51:09Z 2009-11-06T14:51:09Z 2009 2009 Thesis http://hdl.handle.net/1721.1/49554 456575977 eng M.I.T. theses are protected by copyright. They may be viewed from this source for any purpose, but reproduction or distribution in any format is prohibited without written permission. See provided URL for inquiries about permission. http://dspace.mit.edu/handle/1721.1/7582 149 p. application/pdf Massachusetts Institute of Technology |
| spellingShingle | Chemistry. Stone, Katherine Walowicz Coherent multi-exciton dynamics in semiconductor nanostructures via two-dimensional Fourier transform optical spectroscopy |
| title | Coherent multi-exciton dynamics in semiconductor nanostructures via two-dimensional Fourier transform optical spectroscopy |
| title_full | Coherent multi-exciton dynamics in semiconductor nanostructures via two-dimensional Fourier transform optical spectroscopy |
| title_fullStr | Coherent multi-exciton dynamics in semiconductor nanostructures via two-dimensional Fourier transform optical spectroscopy |
| title_full_unstemmed | Coherent multi-exciton dynamics in semiconductor nanostructures via two-dimensional Fourier transform optical spectroscopy |
| title_short | Coherent multi-exciton dynamics in semiconductor nanostructures via two-dimensional Fourier transform optical spectroscopy |
| title_sort | coherent multi exciton dynamics in semiconductor nanostructures via two dimensional fourier transform optical spectroscopy |
| topic | Chemistry. |
| url | http://hdl.handle.net/1721.1/49554 |
| work_keys_str_mv | AT stonekatherinewalowicz coherentmultiexcitondynamicsinsemiconductornanostructuresviatwodimensionalfouriertransformopticalspectroscopy |