The chemical dynamics of nanosensors capable of single-molecule detection
Recent advances in nanotechnology have produced the first sensor transducers capable of resolving the adsorption and desorption of single molecules. Examples include near infrared fluorescent single-walled carbon nanotubes that report single-molecule binding via stochastic quenching. A central quest...
| Main Authors: | , , , , , , , , , , |
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| Format: | Article |
| Language: | en_US |
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American Institute of Physics (AIP)
2013
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| Online Access: | http://hdl.handle.net/1721.1/77955 https://orcid.org/0000-0003-2944-808X https://orcid.org/0000-0003-4304-3484 |
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| author | Boghossian, Ardemis A. Zhang, Jingqing Le Floch-Yin, Francois T. Ulissi, Zachary Ward Bojo, Peter Han, Jae-Hee Kim, Jong-Ho Arkalgud, Jyoti R. Reuel, Nigel Forest Braatz, Richard D. Strano, Michael S. |
| author2 | Massachusetts Institute of Technology. Department of Aeronautics and Astronautics |
| author_facet | Massachusetts Institute of Technology. Department of Aeronautics and Astronautics Boghossian, Ardemis A. Zhang, Jingqing Le Floch-Yin, Francois T. Ulissi, Zachary Ward Bojo, Peter Han, Jae-Hee Kim, Jong-Ho Arkalgud, Jyoti R. Reuel, Nigel Forest Braatz, Richard D. Strano, Michael S. |
| author_sort | Boghossian, Ardemis A. |
| collection | MIT |
| description | Recent advances in nanotechnology have produced the first sensor transducers capable of resolving the adsorption and desorption of single molecules. Examples include near infrared fluorescent single-walled carbon nanotubes that report single-molecule binding via stochastic quenching. A central question for the theory of such sensors is how to analyze stochastic adsorption events and extract the local concentration or flux of the analyte near the sensor. In this work, we compare algorithms of varying complexity for accomplishing this by first constructing a kinetic Monte Carlo model of molecular binding and unbinding to the sensor substrate and simulating the dynamics over wide ranges of forward and reverse rate constants. Methods involving single-site probability calculations, first and second moment analysis, and birth-and-death population modeling are compared for their accuracy in reconstructing model parameters in the presence and absence of noise over a large dynamic range. Overall, birth-and-death population modeling was the most robust in recovering the forward rate constants, with the first and second order moment analysis very efficient when the forward rate is large (>10[superscript −3] s[superscript −1]). The precision decreases with increasing noise, which we show masks the existence of underlying states. Precision is also diminished with very large forward rate constants, since the sensor surface quickly and persistently saturates. |
| first_indexed | 2024-09-23T11:45:50Z |
| format | Article |
| id | mit-1721.1/77955 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T11:45:50Z |
| publishDate | 2013 |
| publisher | American Institute of Physics (AIP) |
| record_format | dspace |
| spelling | mit-1721.1/779552022-09-27T21:45:08Z The chemical dynamics of nanosensors capable of single-molecule detection Boghossian, Ardemis A. Zhang, Jingqing Le Floch-Yin, Francois T. Ulissi, Zachary Ward Bojo, Peter Han, Jae-Hee Kim, Jong-Ho Arkalgud, Jyoti R. Reuel, Nigel Forest Braatz, Richard D. Strano, Michael S. Massachusetts Institute of Technology. Department of Aeronautics and Astronautics Massachusetts Institute of Technology. Department of Biological Engineering Massachusetts Institute of Technology. Department of Chemical Engineering Boghossian, Ardemis A. Zhang, Jingqing Le Floch-Yin, Francois T. Ulissi, Zachary Ward Bojo, Peter Arkalgud, Jyoti R. Reuel, Nigel Forest Braatz, Richard D. Strano, Michael S. Recent advances in nanotechnology have produced the first sensor transducers capable of resolving the adsorption and desorption of single molecules. Examples include near infrared fluorescent single-walled carbon nanotubes that report single-molecule binding via stochastic quenching. A central question for the theory of such sensors is how to analyze stochastic adsorption events and extract the local concentration or flux of the analyte near the sensor. In this work, we compare algorithms of varying complexity for accomplishing this by first constructing a kinetic Monte Carlo model of molecular binding and unbinding to the sensor substrate and simulating the dynamics over wide ranges of forward and reverse rate constants. Methods involving single-site probability calculations, first and second moment analysis, and birth-and-death population modeling are compared for their accuracy in reconstructing model parameters in the presence and absence of noise over a large dynamic range. Overall, birth-and-death population modeling was the most robust in recovering the forward rate constants, with the first and second order moment analysis very efficient when the forward rate is large (>10[superscript −3] s[superscript −1]). The precision decreases with increasing noise, which we show masks the existence of underlying states. Precision is also diminished with very large forward rate constants, since the sensor surface quickly and persistently saturates. American Society for Engineering Education. National Defense Science and Engineering Graduate Fellowship United States. Dept. of Energy (Fellowship) National Science Foundation (U.S.) (Fellowship) 2013-03-20T20:58:31Z 2013-03-20T20:58:31Z 2011-08 2011-04 Article http://purl.org/eprint/type/JournalArticle 0021-9606 1089-7690 http://hdl.handle.net/1721.1/77955 Boghossian, Ardemis A. et al. “The Chemical Dynamics of Nanosensors Capable of Single-molecule Detection.” The Journal of Chemical Physics 135.8 (2011): 084124. ©2011 American Institute of Physics https://orcid.org/0000-0003-2944-808X https://orcid.org/0000-0003-4304-3484 en_US http://dx.doi.org/10.1063/1.3606496 Journal of Chemical Physics 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 Institute of Physics (AIP) MIT Web Domain |
| spellingShingle | Boghossian, Ardemis A. Zhang, Jingqing Le Floch-Yin, Francois T. Ulissi, Zachary Ward Bojo, Peter Han, Jae-Hee Kim, Jong-Ho Arkalgud, Jyoti R. Reuel, Nigel Forest Braatz, Richard D. Strano, Michael S. The chemical dynamics of nanosensors capable of single-molecule detection |
| title | The chemical dynamics of nanosensors capable of single-molecule detection |
| title_full | The chemical dynamics of nanosensors capable of single-molecule detection |
| title_fullStr | The chemical dynamics of nanosensors capable of single-molecule detection |
| title_full_unstemmed | The chemical dynamics of nanosensors capable of single-molecule detection |
| title_short | The chemical dynamics of nanosensors capable of single-molecule detection |
| title_sort | chemical dynamics of nanosensors capable of single molecule detection |
| url | http://hdl.handle.net/1721.1/77955 https://orcid.org/0000-0003-2944-808X https://orcid.org/0000-0003-4304-3484 |
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