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Ehrl, Benno ; Liebherr, Raphaela ; Gorris, H. H.

Single molecule kinetics of horseradish peroxidase exposed in large arrays of femtoliter-sized fused silica chambers

Article

Ehrl, Benno, Liebherr, Raphaela and Gorris, H. H. (2013) Single molecule kinetics of horseradish peroxidase exposed in large arrays of femtoliter-sized fused silica chambers. Analyst 138, 4260- 4265.

DOI to cite this document: 10.5283/epub.34240


Abstract

Large arrays of femtoliter-sized chambers were etched into the surface of fused silica slides to enclose and observe hundreds of single horseradish peroxidase (HRP) molecules in parallel. Individual molecules of HRP oxidize the fluorogenic substrate Amplex Red to fluorescent resorufin in separate chambers, which was monitored by fluorescence microscopy. Photooxidation of Amplex Red and ...

Large arrays of femtoliter-sized chambers were etched into the surface of fused silica slides to enclose and observe hundreds of single horseradish peroxidase (HRP) molecules in parallel. Individual molecules of HRP oxidize the fluorogenic substrate Amplex Red to fluorescent resorufin in separate chambers, which was monitored by fluorescence microscopy. Photooxidation of Amplex Red and photobleaching of resorufin have previously limited the analysis of HRP in femtoliter arrays. We have strongly reduced these effects by optimizing the fluorescence excitation and detection scheme to yield accurate single molecule substrate turnover rates. We demonstrate the presence of long-lived kinetic states of single HRP molecules that are individually different for each molecule in the array. The large number of molecules investigated in parallel provides excellent statistics on the activity distribution in the enzyme population, which is similar to that reported for other enzymes such as β-galactosidase. We have further confirmed that the product formation of HRP in femtoliter chambers is 10-fold lower than that in the bulk solution due to the particular two-step redox reaction mechanism of HRP.



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Details

Item typeArticle
Journal or Publication TitleAnalyst
PublisherRoyal Society of Chemistry (RSC)
Open Access TypeAlliance-/National licence
Volume138
Page Range4260- 4265
Date2013
Date of publication04 Aug 2016 08:31
InstitutionsChemistry and Pharmacy > Institut für Analytische Chemie, Chemo- und Biosensorik
Identification Number
ValueType
10.1039/C3AN00809FDOI
Dewey Decimal Classification500 Science > 540 Chemistry & allied sciences
StatusPublished
RefereedYes, this version has been refereed
Created at the University of RegensburgYes
URN of the UB Regensburgurn:nbn:de:bvb:355-epub-342403
Item ID34240

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