Journal
NANO LETTERS
Volume 20, Issue 9, Pages 6452-6458Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.0c02146
Keywords
coherent 2D microspectroscopy; optical coherence length; microscopic topography; hierarchical architectures; self-assembly
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Funding
- European Research Council (ERC) [614623, 646737]
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [220404594, PF385/12]
- State of Bavaria within the collaborative research network Solar Technologies go Hybrid (SolTech)
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Many nanotechnology materials rely on a hierarchical structure ranging from the nanometer scale to the micrometer scale. Their interplay determines the nanoscale optical coherence length, which plays a key role in energy transport and radiative decay and, thus, the optoelectronic applications. However, it is challenging to detect optical coherence length in multiscale structures with existing methods. Techniques such as atomic force microscopy and transmission electron microscopy are not sensitive to optical coherence length. Linear absorption and fluorescence spectroscopy methods, on the other hand, were generally limited by inhomogeneous broadening, which often obstructs the determination of nanoscale coherence length. Here, we carry out coherent two-dimensional microspectroscopy to obtain a map of the local optical coherence length within a hierarchically structured molecular film. Interestingly, the nanoscale coherence length is found to correlate with microscale topography, suggesting a perspective for controlling structural coherence on molecular length scales by appropriate microscopic growth conditions.
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