<i>In situ</i> non-invasive Raman spectroscopic characterisation of succinic acid polymorphism during segmented flow crystallisation

Pallipurath, Anuradha; Flandrin, Pierre Baptiste; Wayment, Lois E; Wilson, Chick C.; Robertson, Karen

doi:10.1039/c9me00103d

Cited by 7 publications

(7 citation statements)

References 25 publications

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“…The line arrangement shows that the crystal is in its more stable β form. [ 32 ] The vibrations in the C–H stretch range are the symmetric (2924 cm −1 ) and asymmetric (2967 cm −1 ) stretch. [ 32 , 33 ] We are not aware of a detailed line assignment for D4‐SA.…”

Section: Resultsmentioning

confidence: 99%

Quantification of the nonlinear susceptibility of the hydrogen and deuterium stretch vibration for biomolecules in coherent Raman micro‐spectroscopy

Boorman

Pope

Masia

et al. 2021

J Raman Spectroscopy

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Deuterium labelling is increasingly used in coherent Raman imaging of complex systems, such as biological cells and tissues, to improve chemical specificity. Nevertheless, quantitative coherent Raman susceptibility spectra for deuterated compounds have not been previously reported. Interestingly, it is expected theoretically that -D stretch vibrations have a Raman susceptibility lower than -H stretch vibrations, with the area of their imaginary part scaling with their wavenumber, which is shifted from around 2900 cm À1 for C-H into the silent region around 2100 cm À1 for C-D. Here, we report quantitative measurements of the nonlinear susceptibility of water, succinic acid, oleic acid, linoleic acid and deuterated isoforms. We show that the -D stretch vibration has indeed a lower area, consistent with the frequency reduction due to the doubling of atomic mass from hydrogen to deuterium. This finding elucidates an important trade-off between chemical specificity and signal strength in the adoption of deuterium labelling as an imaging strategy for coherent Raman microscopy.

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Section: Resultsmentioning

confidence: 99%

Quantification of the nonlinear susceptibility of the hydrogen and deuterium stretch vibration for biomolecules in coherent Raman micro‐spectroscopy

Boorman

Pope

Masia

et al. 2021

J Raman Spectroscopy

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“…However, hydrophobic interfaces, such as oils or polymers, are frequently present in nucleation experiments, including microfluidics, , millifluidics, microwells, polymer tubings, and stirrer coatings . Therefore, it is important to understand how such interfaces can facilitate heterogeneous nucleation of highly polar, hydrophilic molecules from solution.…”

Section: Introductionmentioning

confidence: 99%

Tuning Interfacial Concentration Enhancement through Dispersion Interactions to Facilitate Heterogeneous Nucleation

et al. 2022

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Classical molecular dynamics simulations were used to investigate how dispersion (van der Waals) interactions between non-polar, hydrophobic surfaces and aqueous glycine solutions affect the solution composition, molecular orientation, and dynamics at the interface. Simulations revealed that dispersion interactions lead to a major increase in the concentration of glycine at the interface in comparison with the bulk solution, resulting from a competition between solute and solvent molecules to be or not to be near the interface. This can then lead to kinetic and/or structural effects facilitating heterogeneous nucleation of glycine at non-polar surfaces, in agreement with recent observations for tridecane, graphene, and polytetrafluoroethylene. A novel parameterization process was developed to map a model surface with tunable dispersion interactions to heptane, tridecane, and graphite materials. The model surface was capable of reproducing the solution structure observed in fully atomistic simulations with excellent agreement and also provided good agreement for dynamic properties, at a significantly reduced computational cost. This approach can be used as an effective tool for screening materials for heterogeneous nucleation enhancement or suppression, based on non-specific dispersion interactions based on bulk material molecular properties, rather than interfacial functional groups, templating or confinement effects.

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“…6,8,9 However, experimental unravelling of the molecular basis of these nucleation processes (and indeed also of more recently alternative molecular pathways 2,3,8,10,11 ) faces a fundamental challenge, namely that nucleation events are rare and stochastic in time and space. To an extent, localization of homogeneous events by, e.g, use of liquid-liquid interfaces 9 and droplets [12][13][14] has been used to overcome the spatial challenge, enabling time-resolved monitoring of structure and composition by X-ray absorption, 9,15,16 Raman 14,17 and UV/Vis spectroscopy, 17,18 SAXS 18,19 and XRD/WAXS. 13,18 However, localization is associated with confinement in small volumes, and is often introducing some degree of heterogeneity, which influences observable nucleation behavior.…”

Section: Introductionmentioning

confidence: 99%

Time-Resolved X-ray Phase-Contrast Imaging (XPCI) of Nucleation and Crystal Growth in the Anti-Solvent Crystallization of Lovastatin

Das¹,

Pallipurath

Leng³

et al. 2020

Preprint

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<p>X-ray phase contrast imaging (XPCI) of anti-solvent crystallization of lovastatin from an acetone/water solution was carried out in a concentric flow mixing device, using water as the anti-solvent. Spinodal decomposition of the solution is observed to give rise to ‘oiled out’ phases that undergo heterogeneous nucleation at the interface with the flowing solution. Heterogeneous nucleation is also observed on the walls of the reactor walls in the form of what appears to be Stranski–Krastanov growth of plate-like crystals. XPCI together with Eulerian video magnification forms a powerful tool for the spatio-temporal analysis, revealing mechanistic details of a non-equilibrium process such as anti-solvent crystallization.</p>

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In situ non-invasive Raman spectroscopic characterisation of succinic acid polymorphism during segmented flow crystallisation

Abstract: Non-invasive confocal Raman spectroscopy has been integrated into a highly controllable tri-segmented flow crystallisation environment to uncover the crystallisation pathway from nucleation to crystal growth of the polymorphic compound succinic acid.

Cited by 7 publications

References 25 publications

Quantification of the nonlinear susceptibility of the hydrogen and deuterium stretch vibration for biomolecules in coherent Raman micro‐spectroscopy

Quantification of the nonlinear susceptibility of the hydrogen and deuterium stretch vibration for biomolecules in coherent Raman micro‐spectroscopy

Tuning Interfacial Concentration Enhancement through Dispersion Interactions to Facilitate Heterogeneous Nucleation

Time-Resolved X-ray Phase-Contrast Imaging (XPCI) of Nucleation and Crystal Growth in the Anti-Solvent Crystallization of Lovastatin

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