Watching Orientational Ordering at the Nanoscale with Coherent Anti‐Stokes Raman Microscopy

Parekh, Sapun H.; Domke, Katrin F.

doi:10.1002/chem.201301394

Cited by 14 publications

(13 citation statements)

References 66 publications

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“…Raman spectroscopy is widely used to study the orientation of guest species at various temperature/pressure conditions (see, e. g., examples in Sections 6 and 8). Coherent anti‐Stokes Raman scattering spectromicroscopy (CARS), is particularly sensitive: for example, it revealed the formation of head‐to‐tail chains of adsorbate molecules inside the pores of ZSM‐5 zeolite …”

Section: Characterization Techniquesmentioning

confidence: 99%

Supramolecular Organization in Confined Nanospaces

Tabacchi

2018

ChemPhysChem

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Empty spaces are abhorred by nature, which immediately rushes in to fill the void. Humans have learnt pretty well how to make ordered empty nanocontainers, and to get useful products out of them. When such an order is imparted to molecules, new properties may appear, often yielding advanced applications. This review illustrates how the organized void space inherently present in various materials: zeolites, clathrates, mesoporous silica/organosilica, and metal organic frameworks (MOF), for example, can be exploited to create confined, organized, and self-assembled supramolecular structures of low dimensionality. Features of the confining matrices relevant to organization are presented with special focus on molecular-level aspects. Selected examples of confined supramolecular assemblies - from small molecules to quantum dots or luminescent species - are aimed to show the complexity and potential of this approach. Natural confinement (minerals) and hyperconfinement (high pressure) provide further opportunities to understand and master the atomistic-level interactions governing supramolecular organization under nanospace restrictions.

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Section: Characterization Techniquesmentioning

confidence: 99%

Supramolecular Organization in Confined Nanospaces

Tabacchi

2018

ChemPhysChem

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“…The anisotropy of materials plays a key role in opto-electronic, 1–7 polymer, 8–11 and bio-related research issues, 12–25 investigating their physical and chemical properties as well as their functions. 1–34 Notably, anisotropy is an important parameter for health and medical research because the material anisotropy is an inherent feature in the research and diagnostics of, for example, neuro-related or cardiovascular diseases. 14,16,22 For the analysis of such anisotropic material properties on the nanoscale, powerful characterization methods such as polarization-dependent techniques have to be selected and further developed.…”

Section: Introductionmentioning

confidence: 99%

Polarization-Dependent Atomic Force Microscopy–Infrared Spectroscopy (AFM-IR): Infrared Nanopolarimetric Analysis of Structure and Anisotropy of Thin Films and Surfaces

Hinrichs

Shaykhutdinov

2018

Appl Spectrosc

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Infrared techniques enable nondestructive and label-free studies of thin films with high chemical and structural contrast. In this work, we review recent progress and perspectives in the nanoscale analysis of anisotropic materials using an extended version of the atomic force microscopy-infrared (AFM-IR) technique. This advanced photothermal technique, includes polarization control of the incoming light and bridges the gap in IR spectroscopic analysis of local anisotropic material properties. Such local anisotropy occurs in a wide range of materials during molecular nucleation, aggregation, and crystallization processes. However, analysis of the anisotropy in morphology and structure can be experimentally and theoretically demanding as it is related to order and disorder processes in ranges from nanoscopic to macroscopic length scales, depending on preparation and environmental conditions. In this context IR techniques can significantly assist as IR spectra can be interpreted in the framework of optical models and numerical calculations with respect to both, the present chemical conditions as well as the micro- and nanostructure. With these extraordinary analytic possibilities, the advanced AFM-IR approach is an essential puzzle piece in direction to connect nanoscale and macroscale anisotropic thin film properties experimentally. In this review, we highlight the analytic possibilities of AFM-IR for studies on nanoscale anisotropy with a set of examples for polymer, plasmonic, and polaritonic films, as well as aggregates of large molecules and proteins.

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“… 44 Furthermore, the location and orientation of molecules inside zeolite channels was observed by multiplex coherent anti-Stokes Raman scattering (mCARS). 29 , 51 2-D slices of 2-chlorothiophene inside large coffin-shaped ZSM-5 crystals were recorded, in which the intensity pattern of these head-to-tail oriented probe molecules revealed the subunit structure of such crystals in detail. 29 Such MFI-type zeolite materials were employed by Seebacher et al to visualize mesostructures and, hence, crystalline defects 52 and spatial distribution of probe molecules inside these pores.…”

Section: Introductionmentioning

confidence: 99%

Differences in the Location of Guest Molecules within Zeolite Pores As Revealed by Multilaser Excitation Confocal Fluorescence Microscopy: Which Molecule Is Where?

Sprung

Weckhuysen

2015

J. Am. Chem. Soc.

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A detailed and systematic polarized confocal fluorescence microscopy investigation is presented on three batches of large coffin-shaped ZSM-5 crystals (i.e., parent, steamed at 500 °C, and steamed at 700 °C). In total, six laser lines of different wavelength in the visible region are employed on two crystal positions and three orientations with respect to the polarization plane of the excitation laser light. A fluorescent probe molecule is generated inside the zeolite pores, originating from the acid-catalyzed oligomerization of 4-fluorostyrene. A thorough analysis of the polarization plane of emitting fluorescent light reveals insight into the orientation of the fluorescent probe molecule restricted by the highly ordered zeolite channel framework, thereby visualizing pore accessibility and clearly distinguishing the occupation of straight and sinusoidal channels by the probe molecule. Spectral features are, furthermore, observed to tell apart molecules situated in one or the other pore. Special focus was given on the rim and tip regions of the zeolite ZSM-5 crystals. On the basis of the confocal approach of the investigation, the aforementioned features are evaluated in three dimensions, while the degradation of the zeolite framework upon postsynthesis steam treatment could be visualized by occupation of the sinusoidal pores.

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Watching Orientational Ordering at the Nanoscale with Coherent Anti‐Stokes Raman Microscopy

Cited by 14 publications

References 66 publications

Supramolecular Organization in Confined Nanospaces

Supramolecular Organization in Confined Nanospaces

Polarization-Dependent Atomic Force Microscopy–Infrared Spectroscopy (AFM-IR): Infrared Nanopolarimetric Analysis of Structure and Anisotropy of Thin Films and Surfaces

Differences in the Location of Guest Molecules within Zeolite Pores As Revealed by Multilaser Excitation Confocal Fluorescence Microscopy: Which Molecule Is Where?

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