Direct single-molecule dynamic detection of chemical reactions
Guan, J., Jia, C., Li, Y., Liu, Z., Wang, J., Yang, Z., Gu, C., Su, D., Houk, K. N., Zhang, D., Guo, X.
American Association for the Advancement of Science (AAAS)
Published 2018
American Association for the Advancement of Science (AAAS)
Published 2018
| Publication Date: |
2018-02-10
|
|---|---|
| Publisher: |
American Association for the Advancement of Science (AAAS)
|
| Electronic ISSN: |
2375-2548
|
| Topics: |
Natural Sciences in General
|
| Published by: |
| _version_ | 1836398788563959810 |
|---|---|
| autor | Guan, J., Jia, C., Li, Y., Liu, Z., Wang, J., Yang, Z., Gu, C., Su, D., Houk, K. N., Zhang, D., Guo, X. |
| beschreibung | Single-molecule detection can reveal time trajectories and reaction pathways of individual intermediates/transition states in chemical reactions and biological processes, which is of fundamental importance to elucidate their intrinsic mechanisms. We present a reliable, label-free single-molecule approach that allows us to directly explore the dynamic process of basic chemical reactions at the single-event level by using stable graphene-molecule single-molecule junctions. These junctions are constructed by covalently connecting a single molecule with a 9-fluorenone center to nanogapped graphene electrodes. For the first time, real-time single-molecule electrical measurements unambiguously show reproducible large-amplitude two-level fluctuations that are highly dependent on solvent environments in a nucleophilic addition reaction of hydroxylamine to a carbonyl group. Both theoretical simulations and ensemble experiments prove that this observation originates from the reversible transition between the reactant and a new intermediate state within a time scale of a few microseconds. These investigations open up a new route that is able to be immediately applied to probe fast single-molecule physics or biophysics with high time resolution, making an important contribution to broad fields beyond reaction chemistry. |
| citation_standardnr | 6161772 |
| datenlieferant | ipn_articles |
| feed_id | 228416 |
| feed_publisher | American Association for the Advancement of Science (AAAS) |
| feed_publisher_url | http://www.aaas.org/ |
| insertion_date | 2018-02-10 |
| journaleissn | 2375-2548 |
| publikationsjahr_anzeige | 2018 |
| publikationsjahr_facette | 2018 |
| publikationsjahr_intervall | 7984:2015-2019 |
| publikationsjahr_sort | 2018 |
| publisher | American Association for the Advancement of Science (AAAS) |
| quelle | Science Advances |
| relation | http://advances.sciencemag.org/cgi/content/short/4/2/eaar2177?rss=1 |
| search_space | articles |
| shingle_author_1 | Guan, J., Jia, C., Li, Y., Liu, Z., Wang, J., Yang, Z., Gu, C., Su, D., Houk, K. N., Zhang, D., Guo, X. |
| shingle_author_2 | Guan, J., Jia, C., Li, Y., Liu, Z., Wang, J., Yang, Z., Gu, C., Su, D., Houk, K. N., Zhang, D., Guo, X. |
| shingle_author_3 | Guan, J., Jia, C., Li, Y., Liu, Z., Wang, J., Yang, Z., Gu, C., Su, D., Houk, K. N., Zhang, D., Guo, X. |
| shingle_author_4 | Guan, J., Jia, C., Li, Y., Liu, Z., Wang, J., Yang, Z., Gu, C., Su, D., Houk, K. N., Zhang, D., Guo, X. |
| shingle_catch_all_1 | Direct single-molecule dynamic detection of chemical reactions Single-molecule detection can reveal time trajectories and reaction pathways of individual intermediates/transition states in chemical reactions and biological processes, which is of fundamental importance to elucidate their intrinsic mechanisms. We present a reliable, label-free single-molecule approach that allows us to directly explore the dynamic process of basic chemical reactions at the single-event level by using stable graphene-molecule single-molecule junctions. These junctions are constructed by covalently connecting a single molecule with a 9-fluorenone center to nanogapped graphene electrodes. For the first time, real-time single-molecule electrical measurements unambiguously show reproducible large-amplitude two-level fluctuations that are highly dependent on solvent environments in a nucleophilic addition reaction of hydroxylamine to a carbonyl group. Both theoretical simulations and ensemble experiments prove that this observation originates from the reversible transition between the reactant and a new intermediate state within a time scale of a few microseconds. These investigations open up a new route that is able to be immediately applied to probe fast single-molecule physics or biophysics with high time resolution, making an important contribution to broad fields beyond reaction chemistry. Guan, J., Jia, C., Li, Y., Liu, Z., Wang, J., Yang, Z., Gu, C., Su, D., Houk, K. N., Zhang, D., Guo, X. American Association for the Advancement of Science (AAAS) 2375-2548 23752548 |
| shingle_catch_all_2 | Direct single-molecule dynamic detection of chemical reactions Single-molecule detection can reveal time trajectories and reaction pathways of individual intermediates/transition states in chemical reactions and biological processes, which is of fundamental importance to elucidate their intrinsic mechanisms. We present a reliable, label-free single-molecule approach that allows us to directly explore the dynamic process of basic chemical reactions at the single-event level by using stable graphene-molecule single-molecule junctions. These junctions are constructed by covalently connecting a single molecule with a 9-fluorenone center to nanogapped graphene electrodes. For the first time, real-time single-molecule electrical measurements unambiguously show reproducible large-amplitude two-level fluctuations that are highly dependent on solvent environments in a nucleophilic addition reaction of hydroxylamine to a carbonyl group. Both theoretical simulations and ensemble experiments prove that this observation originates from the reversible transition between the reactant and a new intermediate state within a time scale of a few microseconds. These investigations open up a new route that is able to be immediately applied to probe fast single-molecule physics or biophysics with high time resolution, making an important contribution to broad fields beyond reaction chemistry. Guan, J., Jia, C., Li, Y., Liu, Z., Wang, J., Yang, Z., Gu, C., Su, D., Houk, K. N., Zhang, D., Guo, X. American Association for the Advancement of Science (AAAS) 2375-2548 23752548 |
| shingle_catch_all_3 | Direct single-molecule dynamic detection of chemical reactions Single-molecule detection can reveal time trajectories and reaction pathways of individual intermediates/transition states in chemical reactions and biological processes, which is of fundamental importance to elucidate their intrinsic mechanisms. We present a reliable, label-free single-molecule approach that allows us to directly explore the dynamic process of basic chemical reactions at the single-event level by using stable graphene-molecule single-molecule junctions. These junctions are constructed by covalently connecting a single molecule with a 9-fluorenone center to nanogapped graphene electrodes. For the first time, real-time single-molecule electrical measurements unambiguously show reproducible large-amplitude two-level fluctuations that are highly dependent on solvent environments in a nucleophilic addition reaction of hydroxylamine to a carbonyl group. Both theoretical simulations and ensemble experiments prove that this observation originates from the reversible transition between the reactant and a new intermediate state within a time scale of a few microseconds. These investigations open up a new route that is able to be immediately applied to probe fast single-molecule physics or biophysics with high time resolution, making an important contribution to broad fields beyond reaction chemistry. Guan, J., Jia, C., Li, Y., Liu, Z., Wang, J., Yang, Z., Gu, C., Su, D., Houk, K. N., Zhang, D., Guo, X. American Association for the Advancement of Science (AAAS) 2375-2548 23752548 |
| shingle_catch_all_4 | Direct single-molecule dynamic detection of chemical reactions Single-molecule detection can reveal time trajectories and reaction pathways of individual intermediates/transition states in chemical reactions and biological processes, which is of fundamental importance to elucidate their intrinsic mechanisms. We present a reliable, label-free single-molecule approach that allows us to directly explore the dynamic process of basic chemical reactions at the single-event level by using stable graphene-molecule single-molecule junctions. These junctions are constructed by covalently connecting a single molecule with a 9-fluorenone center to nanogapped graphene electrodes. For the first time, real-time single-molecule electrical measurements unambiguously show reproducible large-amplitude two-level fluctuations that are highly dependent on solvent environments in a nucleophilic addition reaction of hydroxylamine to a carbonyl group. Both theoretical simulations and ensemble experiments prove that this observation originates from the reversible transition between the reactant and a new intermediate state within a time scale of a few microseconds. These investigations open up a new route that is able to be immediately applied to probe fast single-molecule physics or biophysics with high time resolution, making an important contribution to broad fields beyond reaction chemistry. Guan, J., Jia, C., Li, Y., Liu, Z., Wang, J., Yang, Z., Gu, C., Su, D., Houk, K. N., Zhang, D., Guo, X. American Association for the Advancement of Science (AAAS) 2375-2548 23752548 |
| shingle_title_1 | Direct single-molecule dynamic detection of chemical reactions |
| shingle_title_2 | Direct single-molecule dynamic detection of chemical reactions |
| shingle_title_3 | Direct single-molecule dynamic detection of chemical reactions |
| shingle_title_4 | Direct single-molecule dynamic detection of chemical reactions |
| timestamp | 2025-06-30T23:32:39.277Z |
| titel | Direct single-molecule dynamic detection of chemical reactions |
| titel_suche | Direct single-molecule dynamic detection of chemical reactions |
| topic | TA-TD |
| uid | ipn_articles_6161772 |