Ultrafast Coherence Transfer in DNA-templated Silver Nanoclusters

Overview

Journal Nat Commun

Specialty Biology

Date 2017 May 27

PMID 28548085

Citations 18

Authors

Erling Thyrhaug

Sidsel Ammitzboll Bogh

Miguel R Carro-Temboury

Charlotte Stahl Madsen

Tom Vosch

Donatas Zigmantas

Affiliations

Soon will be listed here.

Abstract

DNA-templated silver nanoclusters of a few tens of atoms or less have come into prominence over the last several years due to very strong absorption and efficient emission. Applications in microscopy and sensing have already been realized, however little is known about the excited-state structure and dynamics in these clusters. Here we report on a multidimensional spectroscopy investigation of the energy-level structure and the early-time relaxation cascade, which eventually results in the population of an emitting state. We find that the ultrafast intramolecular relaxation is strongly coupled to a specific vibrational mode, resulting in the concerted transfer of population and coherence between excited states on a sub-100 fs timescale.

Citing Articles

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He R, Wang S, Ju F, Huang Z, Gao Y, Zhang J Biosensors (Basel). 2025; 15(2).

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Robust vibrational coherence protected by a core-shell structure in silver nanoclusters.

Kong J, Kuang Z, Zhang W, Song Y, Yao G, Zhang C Chem Sci. 2024; 15(18):6906-6915.

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Role of transition metals in coinage metal nanoclusters for the remediation of toxic dyes in aqueous systems.

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Chloride Ligands on DNA-Stabilized Silver Nanoclusters.

Gonzalez-Rosell A, Malola S, Guha R, Arevalos N, Matus M, Goulet M J Am Chem Soc. 2023; 145(19):10721-10729.

PMID: 37155337 PMC: 10197127. DOI: 10.1021/jacs.3c01366.

Excited-State Dynamics in a DNA-Stabilized Ag Cluster with Near-Infrared Emission.

Chen J, Kumar A, Cerretani C, Vosch T, Zigmantas D, Thyrhaug E J Phys Chem Lett. 2023; 14(17):4078-4083.

PMID: 37120843 PMC: 10166082. DOI: 10.1021/acs.jpclett.3c00764.

References

Bosbach J, Hendrich C, Stietz F, Vartanyan T, Trager F . Ultrafast dephasing of surface plasmon excitation in silver nanoparticles: influence of particle size, shape, and chemical surrounding. Phys Rev Lett. 2002; 89(25):257404. DOI: 10.1103/PhysRevLett.89.257404. View

Jonas D . Two-dimensional femtosecond spectroscopy. Annu Rev Phys Chem. 2003; 54:425-63. DOI: 10.1146/annurev.physchem.54.011002.103907. View

Zheng J, Nicovich P, Dickson R . Highly fluorescent noble-metal quantum dots. Annu Rev Phys Chem. 2006; 58:409-31. PMC: 2735021. DOI: 10.1146/annurev.physchem.58.032806.104546. View

Vosch T, Antoku Y, Hsiang J, Richards C, Gonzalez J, Dickson R . Strongly emissive individual DNA-encapsulated Ag nanoclusters as single-molecule fluorophores. Proc Natl Acad Sci U S A. 2007; 104(31):12616-21. PMC: 1937515. DOI: 10.1073/pnas.0610677104. View

Read E, Engel G, Calhoun T, Mancal T, Ahn T, Blankenship R . Cross-peak-specific two-dimensional electronic spectroscopy. Proc Natl Acad Sci U S A. 2007; 104(36):14203-8. PMC: 1964816. DOI: 10.1073/pnas.0701201104. View

Abramavicius D, Voronine D, Mukamel S . Unravelling coherent dynamics and energy dissipation in photosynthetic complexes by 2D spectroscopy. Biophys J. 2008; 94(9):3613-9. PMC: 2292377. DOI: 10.1529/biophysj.107.123455. View

Heaven M, Dass A, White P, Holt K, Murray R . Crystal structure of the gold nanoparticle [N(C8H17)4][Au25(SCH2CH2Ph)18]. J Am Chem Soc. 2008; 130(12):3754-5. DOI: 10.1021/ja800561b. View

Farrow D, Qian W, Smith E, Ferro A, Jonas D . Polarized pump-probe measurements of electronic motion via a conical intersection. J Chem Phys. 2008; 128(14):144510. DOI: 10.1063/1.2837471. View

Walter M, Akola J, Lopez-Acevedo O, Jadzinsky P, Calero G, Ackerson C . A unified view of ligand-protected gold clusters as superatom complexes. Proc Natl Acad Sci U S A. 2008; 105(27):9157-62. PMC: 2442568. DOI: 10.1073/pnas.0801001105. View

10.

Yu J, Choi S, Richards C, Antoku Y, Dickson R . Live cell surface labeling with fluorescent Ag nanocluster conjugates. Photochem Photobiol. 2008; 84(6):1435-9. PMC: 2600602. DOI: 10.1111/j.1751-1097.2008.00434.x. View

11.

Patel S, Cozzuol M, Hales J, Richards C, Sartin M, Hsiang J . Electron transfer-induced blinking in Ag nanodot fluorescence. J Phys Chem C Nanomater Interfaces. 2010; 113(47):20264-20270. PMC: 2791375. DOI: 10.1021/jp9079537. View

12.

Antoku Y, Hotta J, Mizuno H, Dickson R, Hofkens J, Vosch T . Transfection of living HeLa cells with fluorescent poly-cytosine encapsulated Ag nanoclusters. Photochem Photobiol Sci. 2010; 9(5):716-21. PMC: 2913586. DOI: 10.1039/c0pp00015a. View

13.

Varnavski O, Ramakrishna G, Kim J, Lee D, Goodson T . Optically excited acoustic vibrations in quantum-sized monolayer-protected gold clusters. ACS Nano. 2010; 4(6):3406-12. DOI: 10.1021/nn1003524. View

14.

Petty J, Fan C, Story S, Sengupta B, Iyer A, Prudowsky Z . DNA Encapsulation of Ten Silver Atoms Produces a Bright, Modulatable, Near Infrared-Emitting Cluster. J Phys Chem Lett. 2010; 1(17):2524-2529. PMC: 2992357. DOI: 10.1021/jz100817z. View

15.

Smith E, Jonas D . Alignment, vibronic level splitting, and coherent coupling effects on the pump-probe polarization anisotropy. J Phys Chem A. 2011; 115(16):4101-13. DOI: 10.1021/jp201928s. View

16.

Petty J, Fan C, Story S, Sengupta B, Sartin M, Hsiang J . Optically enhanced, near-IR, silver cluster emission altered by single base changes in the DNA template. J Phys Chem B. 2011; 115(24):7996-8003. PMC: 3176335. DOI: 10.1021/jp202024x. View

17.

Driehorst T, ONeill P, Goodwin P, Pennathur S, Fygenson D . Distinct conformations of DNA-stabilized fluorescent silver nanoclusters revealed by electrophoretic mobility and diffusivity measurements. Langmuir. 2011; 27(14):8923-33. DOI: 10.1021/la200837z. View

18.

Augulis R, Zigmantas D . Two-dimensional electronic spectroscopy with double modulation lock-in detection: enhancement of sensitivity and noise resistance. Opt Express. 2011; 19(14):13126-33. DOI: 10.1364/OE.19.013126. View

19.

Yang S, Vosch T . Rapid detection of microRNA by a silver nanocluster DNA probe. Anal Chem. 2011; 83(18):6935-9. DOI: 10.1021/ac201903n. View

20.

Choi S, Dickson R, Yu J . Developing luminescent silver nanodots for biological applications. Chem Soc Rev. 2011; 41(5):1867-91. DOI: 10.1039/c1cs15226b. View