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Long-range light-modulated charge transport across the molecular heterostructure doped protein biopolymers

Biological electron transfer (ET) across proteins is ubiquitous, such as the notable photosynthesis example, where light-induced charge separation takes place within the reaction center, followed by sequential ET via intramolecular cofactors within the protein. Far from biology, carbon dots (C-Dots)...

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Autores principales: Mondal, Somen, Ghorai, Nandan, Bhunia, Soumyadip, Ghosh, Hirendra. N., Amdursky, Nadav
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8246076/
https://www.ncbi.nlm.nih.gov/pubmed/34257872
http://dx.doi.org/10.1039/d1sc00487e
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author Mondal, Somen
Ghorai, Nandan
Bhunia, Soumyadip
Ghosh, Hirendra. N.
Amdursky, Nadav
author_facet Mondal, Somen
Ghorai, Nandan
Bhunia, Soumyadip
Ghosh, Hirendra. N.
Amdursky, Nadav
author_sort Mondal, Somen
collection PubMed
description Biological electron transfer (ET) across proteins is ubiquitous, such as the notable photosynthesis example, where light-induced charge separation takes place within the reaction center, followed by sequential ET via intramolecular cofactors within the protein. Far from biology, carbon dots (C-Dots) with their unique optoelectronic properties can be considered as game-changers for next-generation advanced technologies. Here, we use C-Dots for making heterostructure (HS) configurations by conjugating them to a natural ET mediator, the hemin molecule, thus making an electron donor–acceptor system. We show by transient absorption and emission spectroscopy that the rapid intramolecular charge separation happens following light excitation, which can be ascribed to an ultrafast electron and hole transfer (HT) from the C-Dot donor to the hemin acceptor. Upon integrating the HS into a protein matrix, we show that this HT within the HS configuration is 3.3 times faster compared to the same process in solution, indicating the active role of the protein in supporting the rapid light-induced long-range intermolecular charge separation. We further use impedance, electrochemical, and transient photocurrent measurements to show that the light-induced transient charge separation results in an enhanced ET and HT efficiency across the protein biopolymer. The charge conduction across our protein biopolymers, reaching nearly 0.01 S cm(−1), along with the simplicity and low-cost of their formation promotes their use in a variety of optoelectronic devices, such as artificial photosynthesis, photo-responsive protonic–electronic transistors, and photodetectors.
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spelling pubmed-82460762021-07-12 Long-range light-modulated charge transport across the molecular heterostructure doped protein biopolymers Mondal, Somen Ghorai, Nandan Bhunia, Soumyadip Ghosh, Hirendra. N. Amdursky, Nadav Chem Sci Chemistry Biological electron transfer (ET) across proteins is ubiquitous, such as the notable photosynthesis example, where light-induced charge separation takes place within the reaction center, followed by sequential ET via intramolecular cofactors within the protein. Far from biology, carbon dots (C-Dots) with their unique optoelectronic properties can be considered as game-changers for next-generation advanced technologies. Here, we use C-Dots for making heterostructure (HS) configurations by conjugating them to a natural ET mediator, the hemin molecule, thus making an electron donor–acceptor system. We show by transient absorption and emission spectroscopy that the rapid intramolecular charge separation happens following light excitation, which can be ascribed to an ultrafast electron and hole transfer (HT) from the C-Dot donor to the hemin acceptor. Upon integrating the HS into a protein matrix, we show that this HT within the HS configuration is 3.3 times faster compared to the same process in solution, indicating the active role of the protein in supporting the rapid light-induced long-range intermolecular charge separation. We further use impedance, electrochemical, and transient photocurrent measurements to show that the light-induced transient charge separation results in an enhanced ET and HT efficiency across the protein biopolymer. The charge conduction across our protein biopolymers, reaching nearly 0.01 S cm(−1), along with the simplicity and low-cost of their formation promotes their use in a variety of optoelectronic devices, such as artificial photosynthesis, photo-responsive protonic–electronic transistors, and photodetectors. The Royal Society of Chemistry 2021-05-18 /pmc/articles/PMC8246076/ /pubmed/34257872 http://dx.doi.org/10.1039/d1sc00487e Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/
spellingShingle Chemistry
Mondal, Somen
Ghorai, Nandan
Bhunia, Soumyadip
Ghosh, Hirendra. N.
Amdursky, Nadav
Long-range light-modulated charge transport across the molecular heterostructure doped protein biopolymers
title Long-range light-modulated charge transport across the molecular heterostructure doped protein biopolymers
title_full Long-range light-modulated charge transport across the molecular heterostructure doped protein biopolymers
title_fullStr Long-range light-modulated charge transport across the molecular heterostructure doped protein biopolymers
title_full_unstemmed Long-range light-modulated charge transport across the molecular heterostructure doped protein biopolymers
title_short Long-range light-modulated charge transport across the molecular heterostructure doped protein biopolymers
title_sort long-range light-modulated charge transport across the molecular heterostructure doped protein biopolymers
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8246076/
https://www.ncbi.nlm.nih.gov/pubmed/34257872
http://dx.doi.org/10.1039/d1sc00487e
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