Single-atom “surgery” on chiral all-dialkynyl-protected superatomic silver nanoclusters DOI
Chengkai Zhang,

Wei‐Dan Si,

Wei-Dong Tian

и другие.

Science Bulletin, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 1, 2024

Язык: Английский

DNA-AgNC Loaded Liposomes for Measuring Cerebral Blood Flow Using Two-Photon Fluorescence Correlation Spectroscopy DOI
Xiaojin Wang, Mikkel B. Liisberg,

Georgia L. Nolt

и другие.

ACS Nano, Год журнала: 2023, Номер 17(13), С. 12862 - 12874

Опубликована: Июнь 21, 2023

Unraveling the transport of drugs and nanocarriers in cerebrovascular networks is important for pharmacokinetic hemodynamic studies but challenging due to complexity sensing individual particles within circulatory system a live animal. Here, we demonstrate that DNA-stabilized silver nanocluster (DNA-Ag16NC) emits first near-infrared window upon two-photon excitation second NIR can be used multiphoton vivo fluorescence correlation spectroscopy measurement cerebral blood flow rates mice with high spatial temporal resolution. To ensure bright stable emission during experiments, loaded DNA-Ag16NCs into liposomes, which served dual purposes concentrating fluorescent label protecting it from degradation. DNA-Ag16NC-loaded liposomes enabled quantification velocities vessels living mouse.

Язык: Английский

Процитировано

16

Total Structure, Structural Transformation and Catalytic Hydrogenation of [Cu41(SC6H3F2)15Cl3(P(PhF)3)6(H)25]2− Constructed from Twisted Cu13 Units DOI Creative Commons
Huimin Zhou,

Tengfei Duan,

Zidong Lin

и другие.

Advanced Science, Год журнала: 2023, Номер 11(7)

Опубликована: Дек. 8, 2023

Abstract Herein, a remarkable achievement in the synthesis and characterization of an atomically precise copper‐hydride nanocluster, [Cu 41 (SC 6 H 3 F 2 ) 15 Cl (P(PhF) (H) 25 ] 2− via mild one‐pot reaction is presented. Through X‐ray crystallography analysis, it revealed that exhibits unique shell–core–shell structure. The inner Cu 29 kernel composed three twisted 13 units, connected through 4 face sharing. Surrounding metal core, two shells, resembling protective sandwich structure are observed. This arrangement, along with intracluster π ··· interactions intercluster C─H···F─C interactions, contributes to enhanced stability . presence, number, location hydrides within nanocluster established combination experimental density functional theory investigations. Notably, addition phosphine ligand triggers fascinating nanocluster‐to‐nanocluster transformation , resulting generation nanoclusters, 14 (PPh 8 10 + 7 0 Furthermore, demonstrated catalytic activity hydrogenation nitroarenes. intriguing provides opportunity explore assembly M similar other coinage investigate thiol co‐protected copper nanoclusters.

Язык: Английский

Процитировано

16

Theoretical Analysis of the Electronic Structure and Optical Properties of DNA-Stabilized Silver Cluster Ag16Cl2 in Aqueous Solvent DOI Creative Commons

Sami Malola,

María Francisca Matus, Hannu Häkkinen

и другие.

The Journal of Physical Chemistry C, Год журнала: 2023, Номер 127(33), С. 16553 - 16559

Опубликована: Авг. 9, 2023

DNA-stabilized silver nanoclusters with 10–30 atoms are by construction ideal candidates for biocompatible bright fluorescent emitters, but their electronic structure is not well understood. Here, using density functional theory (DFT), we analyze the ground-state and optical absorption of a NIR-emitting cluster Ag16Cl2, which stabilized two DNA strands 9-base sequence 5′-CACCTAGCG-3′ whose atomic was very recently confirmed to have chlorides bound core. We able (i) unambiguously assign charge this in aqueous solvent, (ii) details silver–DNA interactions effect on charge, (iii) character low-energy peaks involved electron orbitals make first assessment circular dichroism, (iv) evaluate suitability various DFT exchange–correlation functionals via benchmarking experimental data. This work lays out baseline all future theoretical understand electronic, chiroptical, fluorescence properties these fascinating nanostructures.

Язык: Английский

Процитировано

15

Hydration Sensitive Orthogonal Dual Emission of a DNA‐Stabilized Silver Nanocluster DOI
Mikkel B. Liisberg, Vanessa Rück, Giacomo Romolini

и другие.

Advanced Optical Materials, Год журнала: 2024, Номер 12(19)

Опубликована: Май 11, 2024

Abstract DNA‐stabilized silver nanoclusters (DNA‐AgNCs) are a class of emitters that have primarily been studied for their molecular‐like photophysical properties with ns‐lived fluorescence. However, µs‐lived luminescence has recently reported an increasing number DNA‐AgNCs, but little is still known about the origin long‐lived emission. To deepen understanding state, (DNA) 2 ‐[Ag 11 ] 7+ , emitter short‐ and dual emission, studied. By examining crystals it found fluorescence transitions orthogonal to each other, which implies components long axis AgNC, such as nucleobases, contribute significantly polarization character luminescent state. The effect hydration level on emission dried droplets also investigated, water drastically reduces from state causes redshift Finally, unusual excitation intensity‐dependent response noticed. This ascribed heterogeneous local environment amorphous solid resulting in different conformations optically activated delayed probabilities. presented results provide new key insights into nature DNA‐AgNCs.

Язык: Английский

Процитировано

6

Analytical method for the determination of the absorption coefficient of DNA-stabilized silver nanoclusters DOI Creative Commons
Giacomo Romolini, Cecilia Cerretani, Vanessa Rück

и другие.

Nanoscale, Год журнала: 2024, Номер 16(26), С. 12559 - 12566

Опубликована: Янв. 1, 2024

DNA-stabilized silver nanoclusters (DNA-AgNCs) are biocompatible emitters formed by atoms and cations encapsulated in DNA oligomers. Here, we present an analytical approach to calculate the molar absorption coefficient (ε) of these systems, which consists combining UV-Vis spectroscopy, electrospray ionization-mass spectrometry (ESI-MS), inductively coupled plasma-optical emission (ICP-OES). ESI-MS enables determination number silvers bound strands, whereas ICP-OES allows measurement total amount solution. The data is used concentration DNA-AgNCs together with absorbance, for calculation ε. We compare obtained ε experimental values previously determined through fluorescence correlation spectroscopy (FCS) theoretical estimates based on itself. Finally, radiative decay rates (kf) evaluated compared those typically found organic fluorophores, highlighting molecular-like nature DNA-AgNC emission.

Язык: Английский

Процитировано

5

A bivariate fluorescence biosensor based on Janus DNA nanoarchitecture-loaded dual-emissive Ag nanoclusters as bi-responsive signaling reporters DOI
Chunli Yang,

Yanan Shi,

Yuqing Zhang

и другие.

Biosensors and Bioelectronics, Год журнала: 2024, Номер 263, С. 116621 - 116621

Опубликована: Июль 31, 2024

Язык: Английский

Процитировано

5

Beyond nature's base pairs: machine learning-enabled design of DNA-stabilized silver nanoclusters DOI
Peter Mastracco, Stacy M. Copp

Chemical Communications, Год журнала: 2023, Номер 59(69), С. 10360 - 10375

Опубликована: Янв. 1, 2023

Data mining and machine learning are powerful tools for investigation design of DNA-based nanomaterials.

Язык: Английский

Процитировано

13

Multi-Objective Design of DNA-Stabilized Nanoclusters Using Variational Autoencoders With Automatic Feature Extraction DOI Creative Commons
Elham Sadeghi, Peter Mastracco, Anna Gonzàlez‐Rosell

и другие.

ACS Nano, Год журнала: 2024, Номер unknown

Опубликована: Сен. 17, 2024

DNA-stabilized silver nanoclusters (Ag

Язык: Английский

Процитировано

5

A DNA‐Stabilized Ag1812+ Cluster with Excitation‐Intensity‐Dependent Dual Emission DOI Creative Commons
Vanessa Rück, Mikkel B. Liisberg, Christian Brinch Mollerup

и другие.

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(39)

Опубликована: Авг. 14, 2023

DNA-stabilized silver nanoclusters (DNA-AgNCs) are easily tunable emitters with intriguing photophysical properties. Here, a DNA-AgNC dual emission in the red and near-infrared (NIR) regions is presented. Mass spectrometry data showed that two DNA strands stabilize 18 atoms nanocluster charge of 12+. Besides determining composition DNA2 [Ag18 ]12+ , steady-state time-resolved methods were applied to characterize picosecond fluorescence relatively intense microsecond-lived NIR luminescence. During this process, luminescence-to-fluorescence ratio was found be excitation-intensity-dependent. This peculiar feature very rare for molecular allows use as nanoscale excitation intensity probe. For purpose, calibration curves constructed using three different approaches based either on or measurements. The results processes like thermally activated delayed (TADF) photon upconversion through triplet-triplet annihilation (TTA) could excluded . We, therefore, speculate ratiometric response result optically fluorescence.

Язык: Английский

Процитировано

11

Atomic Structure of a DNA‐Stabilized Ag11 Nanocluster with Four Valence Electrons DOI Creative Commons
Vanessa Rück, Vlad Andrei Neacșu, Mikkel B. Liisberg

и другие.

Advanced Optical Materials, Год журнала: 2023, Номер 12(7)

Опубликована: Ноя. 8, 2023

Abstract The combination of mass spectrometry and single crystal X‐ray diffraction HPLC‐purified DNA‐stabilized silver nanoclusters (DNA‐AgNCs) is a powerful tool to determine the charge structure encapsulated AgNC. Such information not only relevant design new DNA‐AgNCs with tailored properties, but it also important for bio‐conjugation experiments essential electronic calculations. Here, efforts green emissive DNA‐AgNC are presented. Unfortunately, original DNA‐AgNC, known have four valence electrons, could be crystallized. By modifying stabilizing DNA sequence, while maintaining spectroscopic several mutants successfully crystallized, one them, data provided insight into positions. While conformation resolved, described approach provides valuable class dual electrons. These results constitute roadmap on how improve crystallization quality measurements.

Язык: Английский

Процитировано

11