Energy Transfer Between i-Motif DNA Encapsulated Silver Nanoclusters and Fluorescein Amidite Efficiently Visualizes the Redox State of Live Cells

Hari Chandana Yadavalli; Yeolhoe Kim; Il Lae Jung; Sooyeon Park; Tae Hwan Kim; Jin Young Shin; Riddhi Nagda; Peter Waaben Thulstrup; Morten Jannik Bjerrum; Yong Joo Bhang; Phil Hyu Lee; Won Ho Yang; Pratik Shah; Seong Wook Yang

doi:10.1002/smll.202401629

Energy Transfer Between i-Motif DNA Encapsulated Silver Nanoclusters and Fluorescein Amidite Efficiently Visualizes the Redox State of Live Cells

Hari Chandana Yadavalli
, Yeolhoe Kim
, Il Lae Jung
, Sooyeon Park
, Tae Hwan Kim
, Jin Young Shin
, Riddhi Nagda
, Peter Waaben Thulstrup
, Morten Jannik Bjerrum
, Yong Joo Bhang
, Phil Hyu Lee
, Won Ho Yang^*
, Pratik Shah^*
, Seong Wook Yang^*

^*Corresponding author

Research output: Contribution to journal › Journal article › Research › peer-review

4 Citations (Scopus)

174 Downloads (Pure)

Abstract

The redox regulation, maintaining a balance between oxidation and reduction in living cells, is vital for cellular homeostasis, intricate signaling networks, and appropriate responses to physiological and environmental cues. Here, a novel redox sensor, based on DNA-encapsulated silver nanoclusters (DNA/AgNCs) and well-defined chemical fluorophores, effectively illustrating cellular redox states in live cells is introduced. Among various i-motif DNAs, the photophysical property of poly-cytosines (C20)-encapsulated AgNCs that sense reactive oxygen species (ROS) is adopted. However, the sensitivity of C20/AgNCs is insufficient for evaluating ROS levels in live cells. To overcome this drawback, the ROS sensing mechanism of C20/AgNCs through gel electrophoresis, mass spectrometry, and small-angle X-ray scattering is primarily defined. Then, by tethering fluorescein amidite (FAM) and Cyanine 5 (Cy5) dyes to each end of the C20/AgNCs sensor, an Energy Transfer (ET) between AgNCs and FAM is achieved, resulting in intensified green fluorescence upon ROS detection. Taken together, the FAM-C20/AgNCs-Cy5 redox sensor enables dynamic visualization of intracellular redox states, yielding insights into oxidative stress-related processes in live cells.

Original language	English
Article number	2401629
Journal	Small
Volume	20
Issue number	40
Number of pages	13
ISSN	1613-6810
DOIs	https://doi.org/10.1002/smll.202401629
Publication status	Published - 3 Oct 2024

Funding

Funding Information: This work was supported by the Korea Medical Device Development Fund (KMDF) (RS\u20102022\u201000141618), the Korea Health Technology R&D Project through the Korea Health Industry Development Institute (KHIDI), funded by the Ministry of Health & Welfare, Republic of Korea (HU21C0053), the Basic Science Research Program through the National Research Foundation (NRF) (NRF\u20102018R1A6A1A03025607, 2018R1D1A1B07051125, 2021R1A6A3A13044758, 2022R1F1A1073998, 2022R1A2C10915076, and 2023R1A2C3004112). This research was also supported in part by the Brain Korea 21 (BK21) FOUR (Fostering Outstanding Universities for Research) program from the Ministry of Education (MOE, Korea). H.C.Y. is a recipient of a fellowship awarded by the BK21 FOUR program.

Keywords

DNA
energy transfer
imaging
redox sensing
silver nanoclusters

Access to Document

10.1002/smll.202401629Licence: CC BY-NC-ND

Energy Transfer Between i-Motif DNA Encapsulated Silver Nanoclusters and Fluorescein Amidite Efficiently Visualizes the Redox State of Live CellsFinal published version, 5.35 MBLicence: CC BY-NC-ND

Citation Styles

Yadavalli, H. C., Kim, Y., Jung, I. L., Park, S., Kim, T. H., Shin, J. Y., Nagda, R., Thulstrup, P. W., Bjerrum, M. J., Bhang, Y. J., Lee, P. H., Yang, W. H., Shah, P., & Yang, S. W. (2024). Energy Transfer Between i-Motif DNA Encapsulated Silver Nanoclusters and Fluorescein Amidite Efficiently Visualizes the Redox State of Live Cells. Small, 20(40), Article 2401629. https://doi.org/10.1002/smll.202401629

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title = "Energy Transfer Between i-Motif DNA Encapsulated Silver Nanoclusters and Fluorescein Amidite Efficiently Visualizes the Redox State of Live Cells",

abstract = "The redox regulation, maintaining a balance between oxidation and reduction in living cells, is vital for cellular homeostasis, intricate signaling networks, and appropriate responses to physiological and environmental cues. Here, a novel redox sensor, based on DNA-encapsulated silver nanoclusters (DNA/AgNCs) and well-defined chemical fluorophores, effectively illustrating cellular redox states in live cells is introduced. Among various i-motif DNAs, the photophysical property of poly-cytosines (C20)-encapsulated AgNCs that sense reactive oxygen species (ROS) is adopted. However, the sensitivity of C20/AgNCs is insufficient for evaluating ROS levels in live cells. To overcome this drawback, the ROS sensing mechanism of C20/AgNCs through gel electrophoresis, mass spectrometry, and small-angle X-ray scattering is primarily defined. Then, by tethering fluorescein amidite (FAM) and Cyanine 5 (Cy5) dyes to each end of the C20/AgNCs sensor, an Energy Transfer (ET) between AgNCs and FAM is achieved, resulting in intensified green fluorescence upon ROS detection. Taken together, the FAM-C20/AgNCs-Cy5 redox sensor enables dynamic visualization of intracellular redox states, yielding insights into oxidative stress-related processes in live cells.",

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author = "Yadavalli, \{Hari Chandana\} and Yeolhoe Kim and Jung, \{Il Lae\} and Sooyeon Park and Kim, \{Tae Hwan\} and Shin, \{Jin Young\} and Riddhi Nagda and Thulstrup, \{Peter Waaben\} and Bjerrum, \{Morten Jannik\} and Bhang, \{Yong Joo\} and Lee, \{Phil Hyu\} and Yang, \{Won Ho\} and Pratik Shah and Yang, \{Seong Wook\}",

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year = "2024",

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Yadavalli, HC, Kim, Y, Jung, IL, Park, S, Kim, TH, Shin, JY, Nagda, R, Thulstrup, PW, Bjerrum, MJ, Bhang, YJ, Lee, PH, Yang, WH, Shah, P & Yang, SW 2024, 'Energy Transfer Between i-Motif DNA Encapsulated Silver Nanoclusters and Fluorescein Amidite Efficiently Visualizes the Redox State of Live Cells', Small, vol. 20, no. 40, 2401629. https://doi.org/10.1002/smll.202401629

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AU - Yadavalli, Hari Chandana

AU - Kim, Yeolhoe

AU - Jung, Il Lae

AU - Park, Sooyeon

AU - Kim, Tae Hwan

AU - Shin, Jin Young

AU - Nagda, Riddhi

AU - Thulstrup, Peter Waaben

AU - Bjerrum, Morten Jannik

AU - Bhang, Yong Joo

AU - Lee, Phil Hyu

AU - Yang, Won Ho

AU - Shah, Pratik

AU - Yang, Seong Wook

N1 - .

PY - 2024/10/3

Y1 - 2024/10/3

N2 - The redox regulation, maintaining a balance between oxidation and reduction in living cells, is vital for cellular homeostasis, intricate signaling networks, and appropriate responses to physiological and environmental cues. Here, a novel redox sensor, based on DNA-encapsulated silver nanoclusters (DNA/AgNCs) and well-defined chemical fluorophores, effectively illustrating cellular redox states in live cells is introduced. Among various i-motif DNAs, the photophysical property of poly-cytosines (C20)-encapsulated AgNCs that sense reactive oxygen species (ROS) is adopted. However, the sensitivity of C20/AgNCs is insufficient for evaluating ROS levels in live cells. To overcome this drawback, the ROS sensing mechanism of C20/AgNCs through gel electrophoresis, mass spectrometry, and small-angle X-ray scattering is primarily defined. Then, by tethering fluorescein amidite (FAM) and Cyanine 5 (Cy5) dyes to each end of the C20/AgNCs sensor, an Energy Transfer (ET) between AgNCs and FAM is achieved, resulting in intensified green fluorescence upon ROS detection. Taken together, the FAM-C20/AgNCs-Cy5 redox sensor enables dynamic visualization of intracellular redox states, yielding insights into oxidative stress-related processes in live cells.

AB - The redox regulation, maintaining a balance between oxidation and reduction in living cells, is vital for cellular homeostasis, intricate signaling networks, and appropriate responses to physiological and environmental cues. Here, a novel redox sensor, based on DNA-encapsulated silver nanoclusters (DNA/AgNCs) and well-defined chemical fluorophores, effectively illustrating cellular redox states in live cells is introduced. Among various i-motif DNAs, the photophysical property of poly-cytosines (C20)-encapsulated AgNCs that sense reactive oxygen species (ROS) is adopted. However, the sensitivity of C20/AgNCs is insufficient for evaluating ROS levels in live cells. To overcome this drawback, the ROS sensing mechanism of C20/AgNCs through gel electrophoresis, mass spectrometry, and small-angle X-ray scattering is primarily defined. Then, by tethering fluorescein amidite (FAM) and Cyanine 5 (Cy5) dyes to each end of the C20/AgNCs sensor, an Energy Transfer (ET) between AgNCs and FAM is achieved, resulting in intensified green fluorescence upon ROS detection. Taken together, the FAM-C20/AgNCs-Cy5 redox sensor enables dynamic visualization of intracellular redox states, yielding insights into oxidative stress-related processes in live cells.

KW - DNA

KW - energy transfer

KW - imaging

KW - redox sensing

KW - silver nanoclusters

KW - DNA

KW - energy transfer

KW - imaging

KW - redox sensing

KW - silver nanoclusters

U2 - 10.1002/smll.202401629

DO - 10.1002/smll.202401629

M3 - Journal article

AN - SCOPUS:85194696700

SN - 1613-6810

VL - 20

JO - Small

JF - Small

IS - 40

M1 - 2401629

ER -