Imaging Dynamic Processes in Multiple Dimensions and Length Scales

Filbrun, Seth L.; Zhao, Fei; Chen, Kuangcai; Huang, Teng-Xiang; Yang, Meek; Cheng, Xiaodong; Dong, Bin; Fang, Ning

doi:10.1146/annurev-physchem-090519-034100

Cited by 2 publications

(1 citation statement)

References 200 publications

(232 reference statements)

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“…Future work will be on building circuits [ 87 ] of single molecules organized in diverse configurations, in which orientation control and small dispersion, as demonstrated here or in future studies addressing different molecular structures, are paramount for the performance of applications, including exciton delocalization [ 88 , 89 , 90 , 91 ] for quantum information science [ 11 ]. Another direction can be on optically monitoring the conformational dynamics [ 92 ] of natural and artificial nanostructures, e.g., DNA-based structures for molecular robotics [ 93 , 94 , 95 ]. Moreover, the present insights and methodologies can be useful for understanding molecular interactions.…”

Section: Discussionmentioning

confidence: 99%

Strategies for Controlling the Spatial Orientation of Single Molecules Tethered on DNA Origami Templates Physisorbed on Glass Substrates: Intercalation and Stretching

Cervantes-Salguero

Biaggne

Youngsman

et al. 2022

IJMS

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Nanoarchitectural control of matter is crucial for next-generation technologies. DNA origami templates are harnessed to accurately position single molecules; however, direct single molecule evidence is lacking regarding how well DNA origami can control the orientation of such molecules in three-dimensional space, as well as the factors affecting control. Here, we present two strategies for controlling the polar (θ) and in-plane azimuthal (ϕ) angular orientations of cyanine Cy5 single molecules tethered on rationally-designed DNA origami templates that are physically adsorbed (physisorbed) on glass substrates. By using dipolar imaging to evaluate Cy5′s orientation and super-resolution microscopy, the absolute spatial orientation of Cy5 is calculated relative to the DNA template. The sequence-dependent partial intercalation of Cy5 is discovered and supported theoretically using density functional theory and molecular dynamics simulations, and it is harnessed as our first strategy to achieve θ control for a full revolution with dispersion as small as ±4.5°. In our second strategy, ϕ control is achieved by mechanically stretching the Cy5 from its two tethers, being the dispersion ±10.3° for full stretching. These results can in principle be applied to any single molecule, expanding in this way the capabilities of DNA as a functional templating material for single-molecule orientation control. The experimental and modeling insights provided herein will help engineer similar self-assembling molecular systems based on polymers, such as RNA and proteins.

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Section: Discussionmentioning

confidence: 99%

Strategies for Controlling the Spatial Orientation of Single Molecules Tethered on DNA Origami Templates Physisorbed on Glass Substrates: Intercalation and Stretching

Cervantes-Salguero

Biaggne

Youngsman

et al. 2022

IJMS

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Single–particle rotational microrheology enables pathological staging of macrophage foaming and antiatherosclerotic studies

Shang,

Ma,

Liu

et al. 2024

Proc. Natl. Acad. Sci. U.S.A.

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The formation of macrophage–derived foam cells has been recognized as the pathological hallmark of atherosclerotic diseases. However, the pathological evolution dynamics and underlying regulatory mechanisms remain largely unknown. Herein, we introduce a single–particle rotational microrheology method for pathological staging of macrophage foaming and antiatherosclerotic explorations by probing the dynamic changes of lysosomal viscous feature over the pathological evolution progression. The principle of this method involves continuous monitoring of out–of–plane rotation–caused scattering brightness fluctuations of the gold nanorod (AuNR) probe–based microrheometer and subsequent determination of rotational relaxation time to analyze the viscous feature in macrophage lysosomes. With this method, we demonstrated the lysosomal viscous feature as a robust pathological reporter and uncovered three distinct pathological stages underlying the evolution dynamics, which are highly correlated with a pathological stage–dependent activation of the NLRP3 inflammasome–involved positive feedback loop. We also validated the potential of this positive feedback loop as a promising therapeutic target and revealed the time window–dependent efficacy of NLRP3 inflammasome–targeted drugs against atherosclerotic diseases. To our knowledge, the pathological staging of macrophage foaming and the pathological stage–dependent activation of the NLRP3 inflammasome–involved positive feedback mechanism have not yet been reported. These findings provide insights into in–depth understanding of evolutionary features and regulatory mechanisms of macrophage foaming, which can benefit the analysis of effective therapeutical drugs as well as the time window of drug treatment against atherosclerotic diseases in preclinical studies.

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Imaging Dynamic Processes in Multiple Dimensions and Length Scales

Cited by 2 publications

References 200 publications

Strategies for Controlling the Spatial Orientation of Single Molecules Tethered on DNA Origami Templates Physisorbed on Glass Substrates: Intercalation and Stretching

Strategies for Controlling the Spatial Orientation of Single Molecules Tethered on DNA Origami Templates Physisorbed on Glass Substrates: Intercalation and Stretching

Single–particle rotational microrheology enables pathological staging of macrophage foaming and antiatherosclerotic studies

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