Polarization-resolved single-molecule tracking reveal strange dynamics of individual fluorescent tracers through a deep rubbery polymer network

2021 ◽  
Author(s):  
Jaladhar Mahato ◽  
Sukanya Bhattacharya ◽  
Dharmendar Kumar Sharma ◽  
Arindam Chowdhury
Keyword(s):  
Single Molecule ◽  
Local Structure ◽  
Biological Systems ◽  
Polymer Network ◽  
Soft Materials ◽  
Complex Environments ◽  
Fluorescent Tracers ◽  
Single Molecule Tracking ◽  
Structure And Dynamics

Tracking the movement of fluorescent single-molecule (SM) tracers has provided several new insights on the local structure and dynamics in complex environments such as soft materials and biological systems. However,...

scholarly journals Polarization-resolved single-molecule tracking reveals strange dynamics of individual fluorescent tracers through a plasticized (rubbery) polymer network

2020 ◽  
Author(s):  
Jaladhar Mahato ◽  
Sukanya Bhattacharya ◽  
Dharmendar K. Sharma ◽  
Arindam Chowdhury
Keyword(s):  
Single Molecule ◽  
Heterogeneous Media ◽  
Polymer Network ◽  
Soft Materials ◽  
Wide Distribution ◽  
Anomalous Transport ◽  
Emission Anisotropy ◽  
Rigid Polymer ◽  
Network Analyses ◽  
Passive Tracers

<div>Tracking the movement of fluorescent single-molecule (SM) tracers has provided several new insights on the local structure and dynamics in complex environments such as soft materials and biological systems. However, SM tracking (SMT) remains unreliable at molecular length scales, as the localization-error (LE) of SM trajectories (~30-50 nm) is considerably larger than size of molecular tracers (~1-3 nm). Thus, instances of tracer (im)mobility in heterogeneous media, which provide indicator for underlying anomalous-transport mechanisms, remains obscured within the realms of SMT. Since translation of passive tracers in an isotropic network is associated with fast dipolar rotation, we propose authentic pauses within LE can be revealed upon probing SM reorientational dynamics. Here, we demonstrate how polarization-resolved SMT (PR-SMT) can provide emission-anisotropy at each super-localized position, thereby revealing tumbling propensity of SMs during random walk. For Rhodamine 6G tracers undergoing heterogeneous transport in a hydrated polyvinylpyrrolidone (PVP) network, analyses of PR-SMT trajectories enabled us to discern instances of genuine immobility and localized motion within the LE. Our investigations on 100 SMs in hydrated (plasticized) PVP films reveal a wide distribution of dwell-times and pause-frequencies, which demonstrate that majority of probes intermittently experience complete translational and rotational immobilization. This indicates tracers serendipitously encounter compact, rigid polymer cavities during transport, implying the existence of nanoscale glass-like domains sparsely distributed in a redominantly deep-rubbery polymer network far above the glass transition. PR-SMT is simple to implement and opens up alternate avenues to interrogate transient (bio)molecular interactions leading to anomalous transport in inhomogeneous media.</div>

scholarly journals Polarization-resolved single-molecule tracking reveals strange dynamics of individual fluorescent tracers through a plasticized (rubbery) polymer network

2020 ◽  
Author(s):  
Jaladhar Mahato ◽  
Sukanya Bhattacharya ◽  
Dharmendar K. Sharma ◽  
Arindam Chowdhury
Keyword(s):  
Single Molecule ◽  
Heterogeneous Media ◽  
Polymer Network ◽  
Soft Materials ◽  
Wide Distribution ◽  
Anomalous Transport ◽  
Emission Anisotropy ◽  
Rigid Polymer ◽  
Network Analyses ◽  
Passive Tracers

<div>Tracking the movement of fluorescent single-molecule (SM) tracers has provided several new insights on the local structure and dynamics in complex environments such as soft materials and biological systems. However, SM tracking (SMT) remains unreliable at molecular length scales, as the localization-error (LE) of SM trajectories (~30-50 nm) is considerably larger than size of molecular tracers (~1-3 nm). Thus, instances of tracer (im)mobility in heterogeneous media, which provide indicator for underlying anomalous-transport mechanisms, remains obscured within the realms of SMT. Since translation of passive tracers in an isotropic network is associated with fast dipolar rotation, we propose authentic pauses within LE can be revealed upon probing SM reorientational dynamics. Here, we demonstrate how polarization-resolved SMT (PR-SMT) can provide emission-anisotropy at each super-localized position, thereby revealing tumbling propensity of SMs during random walk. For Rhodamine 6G tracers undergoing heterogeneous transport in a hydrated polyvinylpyrrolidone (PVP) network, analyses of PR-SMT trajectories enabled us to discern instances of genuine immobility and localized motion within the LE. Our investigations on 100 SMs in hydrated (plasticized) PVP films reveal a wide distribution of dwell-times and pause-frequencies, which demonstrate that majority of probes intermittently experience complete translational and rotational immobilization. This indicates tracers serendipitously encounter compact, rigid polymer cavities during transport, implying the existence of nanoscale glass-like domains sparsely distributed in a redominantly deep-rubbery polymer network far above the glass transition. PR-SMT is simple to implement and opens up alternate avenues to interrogate transient (bio)molecular interactions leading to anomalous transport in inhomogeneous media.</div>

Development of Synchrotron Footprinting at NSLS and NSLS-II

2019 ◽  
Vol 26 (1) ◽  
pp. 55-60 ◽  
Author(s):  
Jen Bohon
Keyword(s):  
Solvent Accessibility ◽  
Biological Systems ◽  
In Vivo Studies ◽  
Aqueous Samples ◽  
Biological Mechanisms ◽  
Macromolecular Assembly ◽  
Structure And Dynamics ◽  
Synchrotron Light ◽  
Ideal Technique

Background: First developed in the 1990’s at the National Synchrotron Light Source, xray synchrotron footprinting is an ideal technique for the analysis of solution-state structure and dynamics of macromolecules. Hydroxyl radicals generated in aqueous samples by intense x-ray beams serve as fine probes of solvent accessibility, rapidly and irreversibly reacting with solvent exposed residues to provide a “snapshot” of the sample state at the time of exposure. Over the last few decades, improvements in instrumentation to expand the technology have continuously pushed the boundaries of biological systems that can be studied using the technique. Conclusion: Dedicated synchrotron beamlines provide important resources for examining fundamental biological mechanisms of folding, ligand binding, catalysis, transcription, translation, and macromolecular assembly. The legacy of synchrotron footprinting at NSLS has led to significant improvement in our understanding of many biological systems, from identifying key structural components in enzymes and transporters to in vivo studies of ribosome assembly. This work continues at the XFP (17-BM) beamline at NSLS-II and facilities at ALS, which are currently accepting proposals for use.

scholarly journals Local Structure and Dynamics of Functional Materials Studied by X-ray Absorption Fine Structure

Symmetry ◽  
2021 ◽  
Vol 13 (8) ◽  
pp. 1315
Author(s):  
Takafumi Miyanaga
Keyword(s):  
Fine Structure ◽  
Local Structure ◽  
Chemical Reactivity ◽  
Functional Materials ◽  
X Ray ◽  
Structure And Dynamics ◽  
Absorption Fine ◽  
Structure Phase Transition ◽  
Local Electronic Structure ◽  
X Ray Absorption

X-ray absorption fine structure (XAFS) is a powerful technique used to analyze a local electronic structure, local atomic structure, and structural dynamics. In this review, I present examples of XAFS that apply to the local structure and dynamics of functional materials: (1) structure phase transition in perovskite PbTiO3 and magnetic FeRhPd alloys; (2) nano-scaled fluctuations related to their magnetic properties in Ni–Mn alloys and Fe/Cr thin films; and (3) the Debye–Waller factors related to the chemical reactivity for catalysis in polyanions and ligand exchange reaction. This study shows that the local structure and dynamics are related to the characteristic function of the materials.

scholarly journals Synthesis and Photostability of Unimolecular Submersible Nanomachines: Toward Single-Molecule Tracking in Solution

2016 ◽  
Vol 18 (10) ◽  
pp. 2343-2346 ◽  
Author(s):  
Víctor García-López ◽  
Jonathan Jeffet ◽  
Shunsuke Kuwahara ◽  
Angel A. Martí ◽  
Yuval Ebenstein ◽  
...  
Keyword(s):  
Single Molecule ◽  
Single Molecule Tracking
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