2025
Edwin C. Johnson; Hayden Robertson; Erica J. Wanless; Grant B. Webber; Ben A. Humphreys
Neutron reflectometry can capture the rapid collapse and swelling of a polymer brush Journal Article
In: Journal of Colloid and Interface Science, vol. 699, pp. 138248, 2025, ISSN: 0021-9797.
@article{Johnson_2025i,
title = {Neutron reflectometry can capture the rapid collapse and swelling of a polymer brush},
author = {Edwin C. Johnson and Hayden Robertson and Erica J. Wanless and Grant B. Webber and Ben A. Humphreys},
url = {http://dx.doi.org/10.1016/j.jcis.2025.138248},
doi = {10.1016/j.jcis.2025.138248},
issn = {0021-9797},
year = {2025},
date = {2025-12-01},
journal = {Journal of Colloid and Interface Science},
volume = {699},
pages = {138248},
publisher = {Elsevier BV},
abstract = {Hypothesis: Measuring dynamic processes in responsive soft matter systems remains a critical frontier in bridging fundamental studies and applied sciences. In particular, determining structural changes of surface-grafted polymers due to the application of stimuli remains poorly examined due to historical instrument limitations. Herein, we exploit the high flux capabilities of the D17 neutron reflectometer (Institut Laue-Langevin, France) to examine kinetic changes in the internal nanostructure of a poly(N-isopropyl-acrylamide) (PNIPAM) brush with temperature or the presence of a common osmolyte (glucose). Experiments: Ellipsometry and neutron reflectometry (NR) was employed to examine changes in brush thickness as a function of temperature in water and aqueous glucose solutions under equilibrium conditions. NR captured the kinetics of brush swelling/collapse triggered by rapid temperature or glucose concentration changes. Findings: Ellipsometry and NR revealed a decrease in the lower critical solution temperature (LCST) of a PNIPAM brush with increasing glucose concentration. Equilibrium NR measurements showed vertical phase separation within the brush when in a near-collapsed state. This stratified structure was expected for the thermally triggered conformation changes, but has not been observed for glucose-triggered collapse/swelling. Excellent statistics were achieved over intervals for the NR kinetic measurements with modelled profiles comparable to longer equilibrium measurements across a wider q range. A small hysteresis was observed in the temperature induced swelling/collapse, while a more pronounced hysteresis was observed in the glucose triggered conformational changes. This hysteresis was equivalent for both swelling and collapse transitions and is attributed to preferential adsorption of the glucose in the brush. Copyright},
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Hayden Robertson; Joshua D. Willott; Andrew R. J. Nelson; Stuart W. Prescott; Erica J. Wanless; B. Grant Webber
Solvent and Ion-Mediated Behavior of a Thermoresponsive Brush: Specific Ion Effects in Methanol-Water Electrolytes Journal Article
In: Macromolecular Rapid Communications, 2025, ISSN: 1521-3927.
@article{Robertson_2025,
title = {Solvent and Ion-Mediated Behavior of a Thermoresponsive Brush: Specific Ion Effects in Methanol-Water Electrolytes},
author = {Hayden Robertson and Joshua D. Willott and Andrew R. J. Nelson and Stuart W. Prescott and Erica J. Wanless and B. Grant Webber},
url = {http://dx.doi.org/10.1002/marc.202500093},
doi = {10.1002/marc.202500093},
issn = {1521-3927},
year = {2025},
date = {2025-05-01},
journal = {Macromolecular Rapid Communications},
publisher = {Wiley},
abstract = {In this study, specific ion effects are explored in methanol-water mixtures, which play a critical role in a diverse range of applications, including protein solubilization and supercapacitors. Spectroscopic ellipsometry and neutron reflectometry are employed to investigate the solvent- and ion-mediated behavior of a poly(N-isopropylacrylamide) (PNIPAM) brush, a well-known thermoresponsive polymer. In the absence of ions and at low methanol mole fractions (xM), PNIPAM displays lower critical solution temperature (LCST) type behavior, with the thermotransition temperature decreasing as xM increased. Upon further increasing xM, a cononsolvency region is identified at approximately xM = 0.15, beyond which re-entrant swelling is observed in conjunction with a suppressed thermoresponse. In the presence of xM = 0.10 electrolytes, the observed specific ion effects adhere to a forward Hofmeister series. Strongly solvated ions, such as Cl- and Br-, decrease the LCST of the brush. In contrast, poorly solvated ions, such as SCN- and I-, lead to more swollen brush profiles and an increase in the LCST. We hypothesize that the stability of water-methanol clusters plays a crucial role in governing polymer solvation, providing insights into the fundamental interactions within mixed solvent systems. Moreover, a theoretical ion that does not impact the swelling or structure of a PNIPAM brush is proposed.},
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Edwin C. Johnson; Kasimir P. Gregory; Hayden Robertson; Isaac J. Gresham; Andrew R. J. Nelson; Vincent S. J. Craig; Stuart W. Prescott; Alister J. Page; Grant B. Webber; Erica J. Wanless
The inductive effect does not explain electron density in haloacetates: are our textbooks wrong? Journal Article
In: Chemical Science, 2025, ISSN: 2041-6539.
@article{Johnson_2025,
title = {The inductive effect does not explain electron density in haloacetates: are our textbooks wrong?},
author = {Edwin C. Johnson and Kasimir P. Gregory and Hayden Robertson and Isaac J. Gresham and Andrew R. J. Nelson and Vincent S. J. Craig and Stuart W. Prescott and Alister J. Page and Grant B. Webber and Erica J. Wanless},
url = {http://dx.doi.org/10.1039/D4SC04832F},
doi = {10.1039/d4sc04832f},
issn = {2041-6539},
year = {2025},
date = {2025-01-01},
journal = {Chemical Science},
publisher = {Royal Society of Chemistry (RSC)},
abstract = {Wave functional theory calculations and experiments reveal that the inductive effect does not explain pKa and charge density trends in haloacetates.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181i,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181ii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiiiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiiiiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
doi = {10.48550/ARXIV.2503.14181},
year = {2025},
date = {2025-01-01},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiiiiiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
doi = {10.48550/ARXIV.2503.14181},
year = {2025},
date = {2025-01-01},
publisher = {arXiv},
abstract = {The paper addresses the vertical and lateral structure of microgels (MGs) layers at the air/water interface and the effect of Langmuir-Blodgett (LB) transfer on solid substrates on the structure. The MGs are based on poly($N$-isopropylacrylamide) networks. For studying the structure at the air/water interface specular and off-specular X-ray reflectivity (OSR/XRR) allows in situ measurements without any labelling techniques. The initial ex situ atomic force microscopy (AFM) scans of LB-transferred MGs at the air/solid interface reveal strong lateral 2D hexagonal ordering across a broad range of lateral surface pressures at the air/water interface before LB-transfer. Notably, for the first time, these results were confirmed by OSR, demonstrating the existence of the long-range hexagonal ordering at low and intermediate surface pressures. For in situ conditions and upon uniaxial compression at the air/water interface, the MG lattice constant decreases non-monotonically. This indicates the formation of domains at low pressures, that approach each other and only compress when the surface isotherm reaches a plateau. Comparing results of in situ and ex situ measurements, our study clearly shows a transfer effect during the LB-deposition on the lateral ordering of the MGs: The distance between the particles decrease during LB-transfer and at high pressures ($Π,>,22,mathrmmNm^-1$) a second distance occurs indicating small domains with hexagonal internal ordering. The novel surface characterisation approaches here highlight the use of both XRR and OSR to probe the vertical and lateral structure of adsorbed MGs, offering in situ, non-invasive insights without the need for doping or transfer-induced artefacts.},
keywords = {},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiiiiiiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
doi = {10.48550/ARXIV.2503.14181},
year = {2025},
date = {2025-01-01},
publisher = {arXiv},
abstract = {The paper addresses the vertical and lateral structure of microgels (MGs) layers at the air/water interface and the effect of Langmuir-Blodgett (LB) transfer on solid substrates on the structure. The MGs are based on poly($N$-isopropylacrylamide) networks. For studying the structure at the air/water interface specular and off-specular X-ray reflectivity (OSR/XRR) allows in situ measurements without any labelling techniques. The initial ex situ atomic force microscopy (AFM) scans of LB-transferred MGs at the air/solid interface reveal strong lateral 2D hexagonal ordering across a broad range of lateral surface pressures at the air/water interface before LB-transfer. Notably, for the first time, these results were confirmed by OSR, demonstrating the existence of the long-range hexagonal ordering at low and intermediate surface pressures. For in situ conditions and upon uniaxial compression at the air/water interface, the MG lattice constant decreases non-monotonically. This indicates the formation of domains at low pressures, that approach each other and only compress when the surface isotherm reaches a plateau. Comparing results of in situ and ex situ measurements, our study clearly shows a transfer effect during the LB-deposition on the lateral ordering of the MGs: The distance between the particles decrease during LB-transfer and at high pressures ($Π,>,22,mathrmmNm^-1$) a second distance occurs indicating small domains with hexagonal internal ordering. The novel surface characterisation approaches here highlight the use of both XRR and OSR to probe the vertical and lateral structure of adsorbed MGs, offering in situ, non-invasive insights without the need for doping or transfer-induced artefacts.},
keywords = {},
pubstate = {published},
tppubtype = {misc}
}
Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiiiiiiiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiiiiiiiiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiiiiiiiiiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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Hayden Robertson; Joanne Zimmer; Anuar Sifuentes Name; Cassia Lux; Sebastian Stock; Regine Klitzing; Olaf Soltwedel
In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces Miscellaneous
2025.
@misc{https://doi.org/10.48550/arxiv.2503.14181iiiiiiiiiiiiiiiiiiiii,
title = {In situ vs ex situ: Comparing the structure of PNIPAM microgels at the air/water and air/solid interfaces},
author = {Hayden Robertson and Joanne Zimmer and Anuar Sifuentes Name and Cassia Lux and Sebastian Stock and Regine Klitzing and Olaf Soltwedel},
url = {https://arxiv.org/abs/2503.14181},
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