Direct probe of spectral inhomogeneity reveals synthetic tunability of single-nanocrystal spectral linewidths
The spectral linewidth of an ensemble of fluorescent emitters is dictated by the combination of single-emitter linewidths and sample inhomogeneity. For semiconductor nanocrystals, efforts to tune ensemble linewidths for optical applications have focused primarily on eliminating sample inhomogeneitie...
| Main Authors: | , , , , , , , |
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| Format: | Article |
| Language: | en_US |
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Nature Publishing Group
2014
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| Online Access: | http://hdl.handle.net/1721.1/84988 https://orcid.org/0000-0003-2220-4365 https://orcid.org/0000-0002-5613-8928 |
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| author | Cui, Jian Marshall, Lisa F. Chen, Ou Brokmann, Xavier Bawendi, Moungi G. Beyler, Andrew Paul Harris, Daniel Kelly Wanger, Darcy Deborah |
| author2 | Massachusetts Institute of Technology. Department of Chemistry |
| author_facet | Massachusetts Institute of Technology. Department of Chemistry Cui, Jian Marshall, Lisa F. Chen, Ou Brokmann, Xavier Bawendi, Moungi G. Beyler, Andrew Paul Harris, Daniel Kelly Wanger, Darcy Deborah |
| author_sort | Cui, Jian |
| collection | MIT |
| description | The spectral linewidth of an ensemble of fluorescent emitters is dictated by the combination of single-emitter linewidths and sample inhomogeneity. For semiconductor nanocrystals, efforts to tune ensemble linewidths for optical applications have focused primarily on eliminating sample inhomogeneities, because conventional single-molecule methods cannot reliably build accurate ensemble-level statistics for single-particle linewidths. Photon-correlation Fourier spectroscopy in solution (S-PCFS) offers a unique approach to investigating single-nanocrystal spectra with large sample statistics and high signal-to-noise ratios, without user selection bias and at fast timescales. With S-PCFS, we directly and quantitatively deconstruct the ensemble linewidth into contributions from the average single-particle linewidth and from sample inhomogeneity. We demonstrate that single-particle linewidths vary significantly from batch to batch and can be synthetically controlled. These findings delineate the synthetic challenges facing underdeveloped nanomaterials such as InP and InAs core–shell particles and introduce new avenues for the synthetic optimization of fluorescent nanoparticles. |
| first_indexed | 2024-09-23T08:02:21Z |
| format | Article |
| id | mit-1721.1/84988 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T08:02:21Z |
| publishDate | 2014 |
| publisher | Nature Publishing Group |
| record_format | dspace |
| spelling | mit-1721.1/849882022-09-23T10:28:18Z Direct probe of spectral inhomogeneity reveals synthetic tunability of single-nanocrystal spectral linewidths Cui, Jian Marshall, Lisa F. Chen, Ou Brokmann, Xavier Bawendi, Moungi G. Beyler, Andrew Paul Harris, Daniel Kelly Wanger, Darcy Deborah Massachusetts Institute of Technology. Department of Chemistry Massachusetts Institute of Technology. Department of Materials Science and Engineering Bawendi, Moungi G. Cui, Jian Beyler, Andrew Paul Marshall, Lisa F. Chen, Ou Harris, Daniel Kelly Wanger, Darcy Deborah Brokmann, Xavier Bawendi, Moungi G. The spectral linewidth of an ensemble of fluorescent emitters is dictated by the combination of single-emitter linewidths and sample inhomogeneity. For semiconductor nanocrystals, efforts to tune ensemble linewidths for optical applications have focused primarily on eliminating sample inhomogeneities, because conventional single-molecule methods cannot reliably build accurate ensemble-level statistics for single-particle linewidths. Photon-correlation Fourier spectroscopy in solution (S-PCFS) offers a unique approach to investigating single-nanocrystal spectra with large sample statistics and high signal-to-noise ratios, without user selection bias and at fast timescales. With S-PCFS, we directly and quantitatively deconstruct the ensemble linewidth into contributions from the average single-particle linewidth and from sample inhomogeneity. We demonstrate that single-particle linewidths vary significantly from batch to batch and can be synthetically controlled. These findings delineate the synthetic challenges facing underdeveloped nanomaterials such as InP and InAs core–shell particles and introduce new avenues for the synthetic optimization of fluorescent nanoparticles. United States. Dept. of Energy. Office of Basic Energy Sciences (Division of Materials Sciences and Engineering Grant DE-FG02-07ER46454) National Institutes of Health (U.S.) (Award P41EB015871-26A1) National Science Foundation (U.S.). Graduate Research Fellowship Program Hertz Foundation 2014-02-18T20:05:05Z 2014-02-18T20:05:05Z 2013-06 2013-01 Article http://purl.org/eprint/type/JournalArticle 1755-4330 1755-4349 http://hdl.handle.net/1721.1/84988 Cui, Jian, Andrew P. Beyler, Lisa F. Marshall, Ou Chen, Daniel K. Harris, Darcy D. Wanger, Xavier Brokmann, and Moungi G. Bawendi. “Direct probe of spectral inhomogeneity reveals synthetic tunability of single-nanocrystal spectral linewidths.” Nature Chemistry 5, no. 7 (June 2, 2013): 602-606. https://orcid.org/0000-0003-2220-4365 https://orcid.org/0000-0002-5613-8928 en_US http://dx.doi.org/10.1038/nchem.1654 Nature Chemistry 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 Nature Publishing Group Prof. Bawendi via Erja Kajosalo |
| spellingShingle | Cui, Jian Marshall, Lisa F. Chen, Ou Brokmann, Xavier Bawendi, Moungi G. Beyler, Andrew Paul Harris, Daniel Kelly Wanger, Darcy Deborah Direct probe of spectral inhomogeneity reveals synthetic tunability of single-nanocrystal spectral linewidths |
| title | Direct probe of spectral inhomogeneity reveals synthetic tunability of single-nanocrystal spectral linewidths |
| title_full | Direct probe of spectral inhomogeneity reveals synthetic tunability of single-nanocrystal spectral linewidths |
| title_fullStr | Direct probe of spectral inhomogeneity reveals synthetic tunability of single-nanocrystal spectral linewidths |
| title_full_unstemmed | Direct probe of spectral inhomogeneity reveals synthetic tunability of single-nanocrystal spectral linewidths |
| title_short | Direct probe of spectral inhomogeneity reveals synthetic tunability of single-nanocrystal spectral linewidths |
| title_sort | direct probe of spectral inhomogeneity reveals synthetic tunability of single nanocrystal spectral linewidths |
| url | http://hdl.handle.net/1721.1/84988 https://orcid.org/0000-0003-2220-4365 https://orcid.org/0000-0002-5613-8928 |
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