Graphene Energy Transfer for Single‐Molecule Biophysics, Biosensing, and Super‐Resolution Microscopy

Kamińska, Izabela; Bohlen, Johann; Yaadav, Renukka; Schüler, Patrick; Raab, Mario; Schröder, Tim; Zähringer, Jonas; Zielonka, Karolina; Krause, Stefan; Tinnefeld, Philip

doi:10.1002/adma.202101099

Cited by 50 publications

(53 citation statements)

References 37 publications

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“…Second, the probability of electric short-circuiting of electrons transferred from PSI to electrolyte should be limited. The latter limitation can be overcome through nano-structuring of the PSI complexes within thin films, e.g., through the use of DNA origami [56], the orienting biotic conductive thin layers (made of, e.g., cytochrome c; [14,[57][58][59]) or organic molecular wires [60,61].…”

Section: Discussionmentioning

confidence: 99%

Competition between intra-protein charge recombination and electron transfer outside photosystem I complexes used for photovoltaic applications

Goyal

Szewczyk

Burdziński

et al. 2022

Photochem Photobiol Sci

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Photosystem I (PSI) complexes isolated from three different species were electrodeposited on FTO conducting glass, forming a photoactive multilayer of the photo-electrode, for investigation of intricate electron transfer (ET) properties in such green hybrid nanosystems. The internal quantum efficiency of photo-electrochemical cells (PEC) containing the PSI-based photo-electrodes did not exceed ~ 0.5%. To reveal the reason for such a low efficiency of photocurrent generation, the temporal evolution of the transient concentration of the photo-oxidized primary electron donor, P+, was studied in aqueous suspensions of the PSI complexes by time-resolved absorption spectroscopy. The results of these measurements provided the information on: (1) completeness of charge separation in PSI reaction centers (RCs), (2) dynamics of internal charge recombination, and (3) efficiency of electron transfer from PSI to the electrolyte, which is the reaction competing with the internal charge recombination in the PSI RC. The efficiency of the full charge separation in the PSI complexes used for functionalization of the electrodes was ~ 90%, indicating that incomplete charge separation was not the main reason for the small yield of photocurrents. For the PSI particles isolated from a green alga Chlamydomonas reinhardtii, the probability of ET outside PSI was ~ 30–40%, whereas for their counterparts isolated from a cyanobacterium Synechocystis sp. PCC 6803 and a red alga Cyanidioschyzon merolae, it represented a mere ~ 4%. We conclude from the transient absorption data for the PSI biocatalysts in solution that the observed small photocurrent efficiency of ~ 0.5% for all the PECs analyzed in this study is likely due to: (1) limited efficiency of ET outside PSI, particularly in the case of PECs based on PSI from Synechocystis and C. merolae, and (2) the electrolyte-mediated electric short-circuiting in PSI particles forming the photoactive layer, particularly in the case of the C. reinhardtii PEC. Graphical abstract

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Section: Discussionmentioning

confidence: 99%

Competition between intra-protein charge recombination and electron transfer outside photosystem I complexes used for photovoltaic applications

Goyal

Szewczyk

Burdziński

et al. 2022

Photochem Photobiol Sci

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“…[42][43][44] Some other studies explored the use of graphene oxide (GO) as immobilization matrix to develop OECT enzyme biosensor. [22,45] In fact, graphene and its derivatives also have many other unique properties, for example, high light absorption and fluorescence quenching ability, [46] which nevertheless has not been explored in the field of OECT devices.…”

Section: Introductionmentioning

confidence: 99%

Multifunctional Hydrogel Hybrid‐Gated Organic Photoelectrochemical Transistor for Biosensing

Lü

Chen

et al. 2022

Adv Funct Materials

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Advanced organic bioelectronics enable smooth fusion between modern electronics and biological systems for better physiological monitoring and pathological examinations. Photon-regulated bioelectronics are especially desirable due to the non-contact impact, remote-control, and even selfpowered operation. However, few studies have addressed the advanced photon-enabled organic photoelectrochemical transistor (OPECT) biosensors capable of operation at zero gate bias. Here, on the basis of a hydrogel/graphene oxide hybrid (denoted as HGH), a multifunctional HGH-gated OPECT biosensor is presented, which is exemplified by Ca 2+ -triggered gelation on the CdS quantum dot (QD) photoelectrode linking with a sandwich immunoassay toward human IgG as the model target. Gelation of HGH on the CdS QD gate electrode can not only inhibit the interfacial mass transfer on the gate/ electrolyte interface, but also significantly block the light absorption of CdS QDs, leading to the corresponding change of the channel currents of OPECT device. At zero gate bias, this OPECT biosensor exhibits high gain in response to light and good analytical performance for human IgG with a detection limit of 50 fg mL -1 . Given the numerous intelligent hydrogel materials and their potential interactions with light, this work unveils a general platform for developing a new class of hydrogel-gated OPECT bioelectronics and beyond.

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“…Methods that exploit the distance-dependent energy transfer to a conductive surface, determine the axial position of fluorophores from lifetime measurements (Chizhik et al 2014). Particularly, methods using graphene-covered substrates (graphene energy transfer, GET) reach sub-10 nm localization precision (Ghosh et al 2019;Kaminska et al 2019;Kamińska et al 2021). Finally, the SML-SSI methods described before can also be applied to localize molecules in the axial direction with sub-10 nm resolution, as demonstrated by 3D-MINFLUX (Gwosch et al 2020), ModLoc (Jouchet et al 2021), and ROSE-Z (Gu et al 2021).…”

Section: First-and Second-generation Nanoscopy Methodsmentioning

confidence: 99%

“…Moreover, three-dimensional origamis have also been developed to benchmark the 3D sub-10 nm techniques, such as the combination of graphene energy transfer and DNA-PAINT, as shown in Fig. 1e, where features separated 2.7 nm in the axial direction were resolved (Kamińska et al 2021). DNA origami offer enormous versatility in terms of geometries and functionalities that can be used.…”

Section: Quantifying Spatial Resolutionmentioning

confidence: 99%

Fluorescence nanoscopy at the sub-10 nm scale

et al. 2021

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Fluorescence nanoscopy represented a breakthrough for the life sciences as it delivers 20-30 nm resolution using far-field fluorescence microscopes. This resolution limit is not fundamental but imposed by the limited photostability of fluorophores under ambient conditions. This has motivated the development of a second generation of fluorescence nanoscopy methods that aim to deliver sub-10 nm resolution, reaching the typical size of structural proteins and thus providing true molecular resolution. In this review, we present common fundamental aspects of these nanoscopies, discuss the key experimental factors that are necessary to fully exploit their capabilities, and discuss their current and future challenges.

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Graphene Energy Transfer for Single‐Molecule Biophysics, Biosensing, and Super‐Resolution Microscopy

Cited by 50 publications

References 37 publications

Competition between intra-protein charge recombination and electron transfer outside photosystem I complexes used for photovoltaic applications

Competition between intra-protein charge recombination and electron transfer outside photosystem I complexes used for photovoltaic applications

Multifunctional Hydrogel Hybrid‐Gated Organic Photoelectrochemical Transistor for Biosensing

Fluorescence nanoscopy at the sub-10 nm scale

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