Coherent two-exciton dynamics measured using two-quantum rephasing two-dimensional electronic spectroscopy
We use fifth-order two-dimensional electronic spectroscopy to measure coherent four-particle dynamics in a semiconductor nanostructure. By using optical polarization control in two-quantum measurements enabled by the COLBERT spectrometer, we separate coherent signals due to bound biexcitons and unbo...
| Main Authors: | , , , |
|---|---|
| Other Authors: | |
| Format: | Article |
| Language: | en_US |
| Published: |
American Physical Society (APS)
2012
|
| Online Access: | http://hdl.handle.net/1721.1/68670 https://orcid.org/0000-0003-2358-6967 https://orcid.org/0000-0001-7804-5418 |
| _version_ | 1826197008643260416 |
|---|---|
| author | Turner, Daniel B. Wen, Patrick Arias, Dylan H. Nelson, Keith Adam |
| author2 | Massachusetts Institute of Technology. Department of Chemistry |
| author_facet | Massachusetts Institute of Technology. Department of Chemistry Turner, Daniel B. Wen, Patrick Arias, Dylan H. Nelson, Keith Adam |
| author_sort | Turner, Daniel B. |
| collection | MIT |
| description | We use fifth-order two-dimensional electronic spectroscopy to measure coherent four-particle dynamics in a semiconductor nanostructure. By using optical polarization control in two-quantum measurements enabled by the COLBERT spectrometer, we separate coherent signals due to bound biexcitons and unbound two-exciton correlations. The rephasing nature of the measurement allows us to separate homogeneous from inhomogeneous contributions to the two-quantum line shapes. We find that, unlike the bound biexciton state, the energy of the unbound pair and its homogeneous linewidth depend on the laser fluence. Simulations using an extended phenomenological model help determine the primary interaction mechanism that leads to the formation of the unbound exciton pair; the model also indicates that seventh-order interactions contribute to the measured spectra under high pulse fluences. |
| first_indexed | 2024-09-23T10:41:19Z |
| format | Article |
| id | mit-1721.1/68670 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T10:41:19Z |
| publishDate | 2012 |
| publisher | American Physical Society (APS) |
| record_format | dspace |
| spelling | mit-1721.1/686702022-09-27T14:15:02Z Coherent two-exciton dynamics measured using two-quantum rephasing two-dimensional electronic spectroscopy Turner, Daniel B. Wen, Patrick Arias, Dylan H. Nelson, Keith Adam Massachusetts Institute of Technology. Department of Chemistry Nelson, Keith Adam Turner, Daniel B. Wen, Patrick Arias, Dylan H. Nelson, Keith Adam We use fifth-order two-dimensional electronic spectroscopy to measure coherent four-particle dynamics in a semiconductor nanostructure. By using optical polarization control in two-quantum measurements enabled by the COLBERT spectrometer, we separate coherent signals due to bound biexcitons and unbound two-exciton correlations. The rephasing nature of the measurement allows us to separate homogeneous from inhomogeneous contributions to the two-quantum line shapes. We find that, unlike the bound biexciton state, the energy of the unbound pair and its homogeneous linewidth depend on the laser fluence. Simulations using an extended phenomenological model help determine the primary interaction mechanism that leads to the formation of the unbound exciton pair; the model also indicates that seventh-order interactions contribute to the measured spectra under high pulse fluences. American Society for Engineering Education. National Defense Science and Engineering Graduate Fellowship National Science Foundation (U.S.) National Science Foundation (U.S.) (Grant CHE-0616939) 2012-01-26T18:41:05Z 2012-01-26T18:41:05Z 2011-10 2011-10 Article http://purl.org/eprint/type/JournalArticle 1098-0121 1550-235X http://hdl.handle.net/1721.1/68670 Turner, Daniel et al. “Coherent two-exciton dynamics measured using two-quantum rephasing two-dimensional electronic spectroscopy.” Physical Review B 84.16 (2011): n. pag. Web. 26 Jan. 2012. © 2011 American Physical Society https://orcid.org/0000-0003-2358-6967 https://orcid.org/0000-0001-7804-5418 en_US http://dx.doi.org/10.1103/PhysRevB.84.165321 Physical Review B Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf American Physical Society (APS) APS |
| spellingShingle | Turner, Daniel B. Wen, Patrick Arias, Dylan H. Nelson, Keith Adam Coherent two-exciton dynamics measured using two-quantum rephasing two-dimensional electronic spectroscopy |
| title | Coherent two-exciton dynamics measured using two-quantum rephasing two-dimensional electronic spectroscopy |
| title_full | Coherent two-exciton dynamics measured using two-quantum rephasing two-dimensional electronic spectroscopy |
| title_fullStr | Coherent two-exciton dynamics measured using two-quantum rephasing two-dimensional electronic spectroscopy |
| title_full_unstemmed | Coherent two-exciton dynamics measured using two-quantum rephasing two-dimensional electronic spectroscopy |
| title_short | Coherent two-exciton dynamics measured using two-quantum rephasing two-dimensional electronic spectroscopy |
| title_sort | coherent two exciton dynamics measured using two quantum rephasing two dimensional electronic spectroscopy |
| url | http://hdl.handle.net/1721.1/68670 https://orcid.org/0000-0003-2358-6967 https://orcid.org/0000-0001-7804-5418 |
| work_keys_str_mv | AT turnerdanielb coherenttwoexcitondynamicsmeasuredusingtwoquantumrephasingtwodimensionalelectronicspectroscopy AT wenpatrick coherenttwoexcitondynamicsmeasuredusingtwoquantumrephasingtwodimensionalelectronicspectroscopy AT ariasdylanh coherenttwoexcitondynamicsmeasuredusingtwoquantumrephasingtwodimensionalelectronicspectroscopy AT nelsonkeithadam coherenttwoexcitondynamicsmeasuredusingtwoquantumrephasingtwodimensionalelectronicspectroscopy |