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Atomic-Scale Dynamics Probed by Photon Correlations.

ABSTRACT: Light absorption and emission have their origins in fast atomic-scale phenomena. To characterize these basic steps (e.g., in photosynthesis, luminescence, and quantum optics), it is necessary to access picosecond temporal and picometer spatial scales simultaneously. In this Perspective, we describe how state-of-the-art picosecond photon correlation spectroscopy combined with luminescence induced at the atomic scale with a scanning tunneling microscope (STM) enables such studies. We outline recent STM-induced luminescence work on single-photon emitters and the dynamics of excitons, charges, molecules, and atoms as well as several prospective experiments concerning light-matter interactions at the nanoscale. We also describe future strategies for measuring and rationalizing ultrafast phenomena at the nanoscale.

SUBMITTER: Roslawska A

PROVIDER: S-EPMC7315641 | biostudies-literature | 2020 Jun

REPOSITORIES: biostudies-literature

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Atomic-Scale Dynamics Probed by Photon Correlations.

Rosławska Anna A Leon Christopher C CC Grewal Abhishek A Merino Pablo P Kuhnke Klaus K Kern Klaus K

ACS nano 20200601 6

Light absorption and emission have their origins in fast atomic-scale phenomena. To characterize these basic steps (<i>e</i>.<i>g</i>., in photosynthesis, luminescence, and quantum optics), it is necessary to access picosecond temporal and picometer spatial scales simultaneously. In this Perspective, we describe how state-of-the-art picosecond photon correlation spectroscopy combined with luminescence induced at the atomic scale with a scanning tunneling microscope (STM) enables such studies. We ...[more]

PMID: 32479059

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Project description:Exchange dynamics between molecules free in solution and bound to the surface of a large supramolecular structure, a polymer, a membrane or solid support are important in many phenomena in biology and materials science. Here we present a novel and generally applicable solution NMR technique, known as dark-state exchange saturation transfer (DEST), to probe such exchange phenomena with atomic resolution. This is illustrated by the exchange reaction between amyloid-? (A?) monomers and polydisperse, NMR-invisible ('dark') protofibrils, a process of significant interest because the accumulation of toxic, aggregated forms of A?, from small oligomers to very large assemblies, has been implicated in the aetiology of Alzheimer's disease. The (15)N-DEST experiment imprints with single-residue-resolution dynamic information on the protofibril-bound species in the form of (15)N transverse relaxation rates ((15)N-R(2)) and exchange kinetics between monomers and protofibrils onto the easily observed two-dimensional (1)H-(15)N correlation spectrum of the monomer. The exchanging species on the protofibril surface comprise an ensemble of sparsely populated states where each residue is either tethered to (through other residues) or in direct contact with the surface. The first eight residues exist predominantly in a mobile tethered state, whereas the largely hydrophobic central region and part of the carboxy (C)-terminal hydrophobic region are in direct contact with the protofibril surface for a significant proportion of the time. The C-terminal residues of both A?40 and A?42 display lower affinity for the protofibril surface, indicating that they are likely to be surface exposed rather than buried as in structures of A? fibrils, and might therefore comprise the critical nucleus for fibril formation. The values, however, are significantly larger for the C-terminal residues of A?42 than A?40, which might explain the former's higher propensity for rapid aggregation and fibril formation.

Dataset Information

Atomic-Scale Dynamics Probed by Photon Correlations.

Publications

Atomic-Scale Dynamics Probed by Photon Correlations.

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