Silver Nanoclusters Serve as Fluorescent Rivets Linking Hoogsteen Triplex DNA and DNA Structures
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Silver Nanoclusters Serve as Fluorescent Rivets Linking Hoogsteen Triplex DNA and DNA Structures. / Nagda, Riddhi; Park, Sooyeon; Jung, Il Lae; Nam, Keonwook; Yadavalli, Hari Chandana; Kim, Young Min; Yang, Kyungjik; Kang, Jooyoun; Thulstrup, Peter Waaben; Bjerrum, Morten Jannik; Cho, Minhaeng; Kim, Tae-Hwan; Roh, Young Hoon; Shah, Pratik; Yang, Seong Wook.
I: ACS Nano, Bind 16, Nr. 8, 2022, s. 13211-13222.Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt
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TY - JOUR
T1 - Silver Nanoclusters Serve as Fluorescent Rivets Linking Hoogsteen Triplex DNA and DNA Structures
AU - Nagda, Riddhi
AU - Park, Sooyeon
AU - Jung, Il Lae
AU - Nam, Keonwook
AU - Yadavalli, Hari Chandana
AU - Kim, Young Min
AU - Yang, Kyungjik
AU - Kang, Jooyoun
AU - Thulstrup, Peter Waaben
AU - Bjerrum, Morten Jannik
AU - Cho, Minhaeng
AU - Kim, Tae-Hwan
AU - Roh, Young Hoon
AU - Shah, Pratik
AU - Yang, Seong Wook
PY - 2022
Y1 - 2022
N2 - Greater understanding of the mutual influence between DNA and the associated nanomaterial on the properties of each other can provide alternative strategies for designing and developing DNA nanomachines. DNA secondary structures are essential for encapsulating highly emissive silver nanoclusters (DNA/AgNCs). Likewise, AgNCs stabilize secondary DNA structures, such as hairpin DNA, duplex DNA, and parallel-motif DNA triplex. In this study, we found that the fluorescence of AgNCs encapsulated within a Hoogsteen triplex DNA structure can be turned on and off in response to pH changes. We also show that AgNCs can act as nanoscale rivets, linking two functionally distinctive DNA nanostructures. For instance, we found that a Hoogsteen triplex DNA structure with a seven-cytosine loop encapsulates red fluorescent AgNCs. The red fluorescence faded under alkaline conditions, whereas the fluorescence was restored in a near-neutral environment. Hairpin DNA and random DNA structures did not exhibit this pH dependent AgNCs fluorescence. A fluorescence lifetime measurement and a small-angle X-ray scattering analysis showed that the triplex DNA-encapsulated AgNCs were photophysically convertible between bright and dark states. An in-gel electrophoresis analysis indicated that bright and dark convertibility depended on the AgNCs-riveted dimerization of the triplex DNAs. Moreover, we found that AgNCs rivet the triplex DNA and hairpin DNA to form a heterodimer, emitting orange fluorescence. Our findings suggest that AgNCs between two cytosine-rich loops can be used as nanorivets in designing noncanonical DNA origami beyond Watson-Crick base pairing.
AB - Greater understanding of the mutual influence between DNA and the associated nanomaterial on the properties of each other can provide alternative strategies for designing and developing DNA nanomachines. DNA secondary structures are essential for encapsulating highly emissive silver nanoclusters (DNA/AgNCs). Likewise, AgNCs stabilize secondary DNA structures, such as hairpin DNA, duplex DNA, and parallel-motif DNA triplex. In this study, we found that the fluorescence of AgNCs encapsulated within a Hoogsteen triplex DNA structure can be turned on and off in response to pH changes. We also show that AgNCs can act as nanoscale rivets, linking two functionally distinctive DNA nanostructures. For instance, we found that a Hoogsteen triplex DNA structure with a seven-cytosine loop encapsulates red fluorescent AgNCs. The red fluorescence faded under alkaline conditions, whereas the fluorescence was restored in a near-neutral environment. Hairpin DNA and random DNA structures did not exhibit this pH dependent AgNCs fluorescence. A fluorescence lifetime measurement and a small-angle X-ray scattering analysis showed that the triplex DNA-encapsulated AgNCs were photophysically convertible between bright and dark states. An in-gel electrophoresis analysis indicated that bright and dark convertibility depended on the AgNCs-riveted dimerization of the triplex DNAs. Moreover, we found that AgNCs rivet the triplex DNA and hairpin DNA to form a heterodimer, emitting orange fluorescence. Our findings suggest that AgNCs between two cytosine-rich loops can be used as nanorivets in designing noncanonical DNA origami beyond Watson-Crick base pairing.
KW - Hoogsteen triplex DNA
KW - Nanorivets
KW - Silver nanoclusters
KW - Head-to-head dimerization, and Noncanonical DNA origami
KW - CLUSTERS
KW - NUMBERS
U2 - 10.1021/acsnano.2c06631
DO - 10.1021/acsnano.2c06631
M3 - Journal article
C2 - 35952305
VL - 16
SP - 13211
EP - 13222
JO - A C S Nano
JF - A C S Nano
SN - 1936-0851
IS - 8
ER -
ID: 318529728