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Dynamics in Geometrical Confinement pp 127–149Cite as

Rotational Diffusion of Guest Molecules Confined in Uni-directional Nanopores

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Part of the book series: Advances in Dielectrics ((ADVDIELECT))

Abstract

Broadband dielectric spectroscopy (BDS) is employed to study the rotational diffusion of Tris(2-ethylhexyl)phosphate (TEHP), a glass-former, and 4-heptyl-4\(^\prime \)-isothiocyanatobiphenyl (7BT), a liquid crystal, both confined in nanoporous silica membranes having uni-directional pores with diameters in the range 4–10.4 nm. It is observed that upon cooling, the glassy dynamics (\(\alpha \)-process) of TEHP is enhanced near the calorimetric glass transition. This confinement effect is attributed to a slight reduction in density of the liquid in the nanopores. The secondary \(\beta \)-relaxation in TEHP is however unaffected by the geometrical confinement. Silanization of the inner pore surfaces has no measurable effect on the mobility of the guest molecules. For the case of liquid crystal 7BT, two relaxation processes originating from librations about the molecule’s short (\(\delta \)-process) and long axes (\(\beta _{\text {LC}}\)-process) are observed. The former becomes suppressed with decreasing pore diameter, while the latter is nearly unaffected with a tendency to become faster with decreasing pore diameter, an effect caused by orientational ordering due to geometrical constraints.

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Abbreviations

BDS:

Broadband dielectric spectroscopy

TEHP:

Tris(2-ethylhexyl)phosphate

7BT:

4-heptyl-4\(^\prime \)-isothiocyanatobiphenyl

NMR:

Nuclear magnetic resonance

DSC:

Differential scanning calorimetry

MWS:

Maxwell–Wagner–Sillars

LCs:

Liquid crystals

SmE:

Smectic E

HF:

Hydrofluoric acid

Si:

Silicon

pSi:

Porous silicon

pSiO\(_{2 }\) :

Porous silica

SEM:

Scanning electron micrograph

h:

Hour(s)

s:

Second(s)

HMDS:

Hexamethyldisilazane

FTIR:

Fourier transform infrared

HP:

Hewlett Packard

HN:

Havriliak–Negami

\(I\) :

Isotropic

N :

Nematic

S :

Smetic

RTD:

Relaxation time distribution

VFT:

Vogel–Fulcher–Tammann

T :

Temperature

\(T_{\text {g}}\) :

Glass transition temperature

DFT:

Density functional theory

NCS:

Isothiocyanate

Hz:

Hertz

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Acknowledgments

Financial support by the DFG (Germany), within IRTG “Diffusion in Porous Materials,” SFB/TRR 102 within the project “Polymers Under Multiple Constrains,” Alexander von Humboldt Foundation and Leipzig School of Natural Sciences, “Building with Molecules and Nano-Objects” (BuildMoNa) is gratefully acknowledged.

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Authors and Affiliations

  1. Institute of Experimental Physics I, University of Leipzig, Linnéstraße 5, 04103, Leipzig, Germany

    Wycliffe K. Kipnusu, Wilhelm Kossack & Friedrich Kremer

  2. Department of Materials Science and Engineering, Penn State University, University Park, PA, 16802, USA

    Ciprian Iacob

  3. NanoBioMedical Centre, Adam Mickiewicz University, Umultowska 85, 61-614, Poznan, Poland

    Malgorzata Jasiurkowska-Delaporte

  4. Department of Chemical and Biomolecular Engineering, University of Tennessee, Knoxville, TN, 37996-1600, USA

    Joshua R. Sangoro

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  1. Wycliffe K. Kipnusu
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  2. Ciprian Iacob
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Correspondence to Wycliffe K. Kipnusu .

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  1. Group of Molecular Physics, University of Leipzig, Leipzig, Germany

    Friedrich Kremer

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Kipnusu, W.K., Iacob, C., Jasiurkowska-Delaporte, M., Kossack, W., Sangoro, J.R., Kremer, F. (2014). Rotational Diffusion of Guest Molecules Confined in Uni-directional Nanopores. In: Kremer, F. (eds) Dynamics in Geometrical Confinement. Advances in Dielectrics. Springer, Cham. https://doi.org/10.1007/978-3-319-06100-9_5

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