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  • 1
    Online Resource
    Online Resource
    AIP Publishing ; 2021
    In:  The Journal of Chemical Physics Vol. 154, No. 15 ( 2021-04-21)
    In: The Journal of Chemical Physics, AIP Publishing, Vol. 154, No. 15 ( 2021-04-21)
    Abstract: Understanding the properties of water under either soft or hard confinement has been an area of great interest, but nanostructured amphiphilic polymers that provide a secondary confinement have garnered significantly less attention. Here, a series of statistical copolymers of 2-hydroxyethyl acrylate (HEA) and 2-(N-ethylperfluorooctane sulfonamido)ethyl methacrylate (FOSM) are swollen to equilibrium in water to form nanostructured physically cross-linked hydrogels to probe the effect of soft confinement on the dynamics of water. Changing the composition of the copolymer from 10 to 21 mol. % FOSM decreases the average size of the assembled FOSM cross-link, but also the spacing between the cross-links in the hydrogels with the mean distance between the FOSM aggregates decreasing from 3.9 to 2.7 nm. The dynamics of water within the hydrogels were assessed with quasielastic neutron scattering. These hydrogels exhibit superior performance for inhibition of water crystallization on supercooling in comparison to analogous hydrogels with different hydrophilic copolymer chemistries. Despite the lower water crystallinity, the self-diffusion coefficient for these hydrogels from the copolymers of HEA and FOSM decreases precipitously below 260 K, which is a counter to the nearly temperature invariant water dynamics reported previously with an analogous hydrogel [Wiener et al., J. Phys. Chem. B 120, 5543 (2016)] that exhibits nearly temperature invariant dynamics to 220 K. These results point to chemistry dependent dynamics of water that is confined within amphiphilic hydrogels, where the interactions of water with the hydrophilic segments can qualitatively alter the temperature dependent dynamics of water in the supercooled state.
    Type of Medium: Online Resource
    ISSN: 0021-9606 , 1089-7690
    Language: English
    Publisher: AIP Publishing
    Publication Date: 2021
    detail.hit.zdb_id: 3113-6
    detail.hit.zdb_id: 1473050-9
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  • 2
    In: Journal of Applied Physics, AIP Publishing, Vol. 114, No. 11 ( 2013-09-21)
    Abstract: Although devices have been fabricated displaying interesting single-electron transport characteristics, there has been limited progress in the development of tools that can simulate such devices based on their physical geometry over a range of bias conditions up to a few volts per junction. In this work, we present the development of a multi-island transport simulator, MITS, a simulator of tunneling transport in multi-island devices that takes into account geometrical and material parameters, and can span low and high source-drain biases. First, the capabilities of MITS are demonstrated by modeling experimental devices described in the literature, and showing that the simulated device characteristics agree well with the experimental observations. Then, the results of studies of charge transport through a long one-dimensional (1D) chain of gold nano-islands on an insulating substrate are presented. Current-voltage (IV) characteristics are investigated as a function of the overall chain-length and temperature. Under high bias conditions, where temperature has a minimal effect, the IV characteristics are non-Ohmic, and do not exhibit any Coulomb staircase (CS) structures. The overall resistance of the device also increases non-linearly with increasing chain-length. For small biases, IV characteristics show clear CS structures that are more pronounced for larger chain-lengths. The Coulomb blockade and the threshold voltage (Vth) required for device switching increase linearly with the increase in chain length. With increasing temperature, the blockade effects are diminished as the abrupt increase in current at Vth is washed out and the apparent blockade decreases. Microscopic investigations demonstrate that the overall IV characteristics are a result of a complex interplay among those factors that affect the tunneling rates that are fixed a priori (island sizes, island separations, temperature, etc.), and the evolving charge state of the system, which changes as the applied source-drain bias (VSD) is changed. In a system of nano-islands with a broad distribution of sizes and inter-island spacings, the applied bias is divided across the junctions as one would expect of a voltage divider, with larger potential drops across the wider junctions and smaller drops across the narrower junctions. As a result, the tunneling resistances across these wider junctions decrease dramatically, relative to the other junctions, at high VSD thereby increasing their electron tunneling rates. IV behavior at high VSD follows a power-law scaling behavior with the exponent dependent on the length of the chain and the degree of disorder in the system.
    Type of Medium: Online Resource
    ISSN: 0021-8979 , 1089-7550
    Language: English
    Publisher: AIP Publishing
    Publication Date: 2013
    detail.hit.zdb_id: 3112-4
    detail.hit.zdb_id: 1476463-5
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  • 3
    In: Journal of Applied Physics, AIP Publishing, Vol. 126, No. 14 ( 2019-10-14)
    Abstract: La3+, Sm3+, and Gd3+ triple-doped ceria Ce1−x(La1/3Sm1/3Gd1/3)xO2−δ (x = 0.06, 0.12, 0.18, 0.24, and 0.30) materials were synthesized by the sol-gel autocombustion method. The selections of dopants were made by an optimized-average atomic number in accordance with the criteria for optimal-doping in ceria. The higher values of relative-density were achieved above 95% by sintering the samples at 1300 °C. The single-phase cubic-fluorite structures, high-density surface-microstructure with uniformly distributed grains, elemental confirmations, and concentration of oxygen vacancies were confirmed using powder x-ray diffraction, scanning electron microscope with energy dispersive spectroscopy, and micro-Raman spectroscopy. Electrical analysis was carried out by impedance spectroscopy, which confirmed the highest value of total-ionic-conductivity, i.e., 0.0381 S/cm at 600 °C with a minimum activation-energy for the Ce0.82La0.06Sm0.06Gd0.06O2−δ (LSG6) composition. Thermal-expansion analyses confirmed the moderate coefficient of thermal-expansion values for all the compositions and were found to be in good agreement with the recently developed materials. The enhanced total-ionic-conductivity and the moderate coefficient of thermal expansion of LSG6 make it as a potential solid-electrolyte for intermediate temperature-solid oxide fuel cell applications.
    Type of Medium: Online Resource
    ISSN: 0021-8979 , 1089-7550
    Language: English
    Publisher: AIP Publishing
    Publication Date: 2019
    detail.hit.zdb_id: 3112-4
    detail.hit.zdb_id: 1476463-5
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  • 4
    Online Resource
    Online Resource
    AIP Publishing ; 2013
    In:  Applied Physics Letters Vol. 103, No. 4 ( 2013-07-22)
    In: Applied Physics Letters, AIP Publishing, Vol. 103, No. 4 ( 2013-07-22)
    Abstract: The effect of confinement of hemoglobin molecules on photoacoustic (PA) signal is studied experimentally. The PA amplitudes for samples with suspended red blood cells (SRBCs) and hemolyzed red blood cells (HRBCs) were found to be comparable at each hematocrit for 532 nm illumination. The difference between the corresponding amplitudes increased with increasing hematocrit for 1064 nm irradiation. For example, the PA amplitude for the SRBCs was about 260% higher than that of the HRBCs at 40% hematocrit. This observation may help to develop a PA method detecting hemolysis noninvasively.
    Type of Medium: Online Resource
    ISSN: 0003-6951 , 1077-3118
    RVK:
    Language: English
    Publisher: AIP Publishing
    Publication Date: 2013
    detail.hit.zdb_id: 211245-0
    detail.hit.zdb_id: 1469436-0
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  • 5
    Online Resource
    Online Resource
    AIP Publishing ; 2002
    In:  The Journal of Chemical Physics Vol. 117, No. 8 ( 2002-08-22), p. 3837-3847
    In: The Journal of Chemical Physics, AIP Publishing, Vol. 117, No. 8 ( 2002-08-22), p. 3837-3847
    Abstract: We have critically examined the possibility of the existence of yet another process (often referred to as process II in the literature) of much smaller magnitude on the high frequency side in the case of 2-ethyl-1-hexanol and 4-methyl-3-heptanol using the dielectric relaxation technique. We have also studied the mixtures of 2-ethyl-1-hexanol with nonpolar methylcyclohexane and a mixture of 1-bromobutane in 4-methyl-3-heptanol for this purpose. In addition, the differential scanning calorimetry (DSC) has been used to study the structural relaxation in the vicinity of the glass transition temperature using the Tool–Narayanaswami–Moynihan procedure as discussed by Sartor et al. [J. Phys. Chem. 100, 6801 (1996)]. Our results show the presence of a clear process II on the higher frequency side whose freezing-out corresponds to the glass transition event at Tg in the DSC studies. It is suggested that process II is associated with free alcohol molecules and is connected to the structural relaxation in alcohols. The dielectric data have been analyzed to understand the thermodynamics of hydrogen bonding using the model of Dannhauser [J. Chem. Phys. 48, 1911 (1968)] . An attempt has been made to correlate the ratio of relaxation rates of processes I and II and the observed deviation from Debye behavior in the case of alcohols.
    Type of Medium: Online Resource
    ISSN: 0021-9606 , 1089-7690
    Language: English
    Publisher: AIP Publishing
    Publication Date: 2002
    detail.hit.zdb_id: 3113-6
    detail.hit.zdb_id: 1473050-9
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  • 6
    Online Resource
    Online Resource
    AIP Publishing ; 2001
    In:  The Journal of Chemical Physics Vol. 114, No. 8 ( 2001-02-22), p. 3640-3652
    In: The Journal of Chemical Physics, AIP Publishing, Vol. 114, No. 8 ( 2001-02-22), p. 3640-3652
    Abstract: Cycloheptanol, cyclo-octanol, cyanoadamantane and cis-1,2-dimethylcyclohexane are known to form plastic crystals which can be supercooled to show a glass transition at a temperature Tg. The molecular dynamics in different plastic phases is studied in their supercooled states using dielectric spectroscopy (frequency range: 106 Hz–10−3 Hz) and differential scanning calorimetry (DSC) over a wide temperature range. The kinetic freezing of the various dielectric processes have been critically examined in relation to the Tg found in the DSC experiments. The plastic phase I of cyclo-octanol shows two Tg’s: one at 148.5 K and the other at 164 K, the former of which is not found in well annealed phase I. The dielectric α-modes correspond to the latter. Cycloheptanol exhibits many Tg’s for the different plastic phases. Unlike the cyclic alcohols, the dielectric spectra of cyanoadamantane and cis-1,2-dimethylcyclohexane is clearly found to follow the Havriliak–Negami equation, both of which interestingly show very little molecular mobility, often referred to as the secondary relaxation in their glassy states. In addition, the temperature dependence of the relaxation rates and the dielectric strengths are critically examined for various supercooled phases to gain an insight into the nature of the molecular mobility in those phases.
    Type of Medium: Online Resource
    ISSN: 0021-9606 , 1089-7690
    Language: English
    Publisher: AIP Publishing
    Publication Date: 2001
    detail.hit.zdb_id: 3113-6
    detail.hit.zdb_id: 1473050-9
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  • 7
    Online Resource
    Online Resource
    AIP Publishing ; 2012
    In:  The Journal of Chemical Physics Vol. 137, No. 22 ( 2012-12-14)
    In: The Journal of Chemical Physics, AIP Publishing, Vol. 137, No. 22 ( 2012-12-14)
    Abstract: The graphite intercalation compound KC24 adsorbs hydrogen gas at low temperatures up to a maximum stoichiometry of KC24(H2)2, with a differential enthalpy of adsorption of approximately −9 kJ mol−1. The hydrogen molecules and potassium atoms form a two-dimensional condensed phase between the graphite layers. Steric barriers and strong adsorption potentials are expected to strongly hinder hydrogen diffusion within the host KC24 structure. In this study, self-diffusion in a KC24(H2)0.5 sample is measured experimentally by quasielastic neutron scattering and compared to values from molecular dynamics simulations. Self-diffusion coefficients are determined by fits of the experimental spectra to a honeycomb net diffusion model and found to agree well with the simulated values. The experimental H2 diffusion coefficients in KC24 vary from 3.6 × 10−9 m2 s−1 at 80 K to 8.5 × 10−9 m2 s−1 at 110 K. The measured diffusivities are roughly an order of magnitude lower that those observed on carbon adsorbents, but compare well with the rate of hydrogen self-diffusion in molecular sieve zeolites.
    Type of Medium: Online Resource
    ISSN: 0021-9606 , 1089-7690
    Language: English
    Publisher: AIP Publishing
    Publication Date: 2012
    detail.hit.zdb_id: 3113-6
    detail.hit.zdb_id: 1473050-9
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  • 8
    Online Resource
    Online Resource
    AIP Publishing ; 2005
    In:  The Journal of Chemical Physics Vol. 122, No. 24 ( 2005-06-22)
    In: The Journal of Chemical Physics, AIP Publishing, Vol. 122, No. 24 ( 2005-06-22)
    Abstract: We have investigated the dynamics of poly(vinly acetate) using broadband dielectric spectroscopy (DS) covering over 14 decades in frequency up to 20GHz and high-resolution quasielastic neutron-scattering (QENS) technique. The dielectric results have been interpreted in terms of the phenomenological Kohlrausch–Williams–Watts [G. Williams and D. C. Watts, Trans. Faraday Soc. 66, 80 (1970); F. Alvarez, A. Alegría, and J. Colmenero, Phys. Rev. B 47, 125 (1993)] description. Because of the wide frequency range covered by DS, it provides a precise determination of dynamics over a wide temperature range and it revealed a crossover in polymer dynamics at 387K through different dielectric parameters, viz., characteristic times, asymmetric shape parameter, and dielectric strength. Moreover, shape parameter is found to be higher in comparison to other typical polymeric systems. The characteristic relaxation times observed by QENS displayed an anomalous dependence of momentum transfer, indicating the possible existence of heterogeneities in the system even at the high temperatures. In addition, spin-lattice relaxation times, T1, were found to be decoupled from dielectric characteristic times. Based on these results, a model was proposed to account for heterogeneities where we consider coexistence of different regions with standard polymeric behavior but with different characteristic times, leading to a distribution of relaxation times. The model is found to account for the anomalous behavior and an inherent sh ape parameter is found to account for the shape of α relaxation. This model is also found to predict the T variation of T1 characteristic time scales at all temperatures. The origin of the heterogeneous domains is believed to lie in the microstructure of polymer chains.
    Type of Medium: Online Resource
    ISSN: 0021-9606 , 1089-7690
    Language: English
    Publisher: AIP Publishing
    Publication Date: 2005
    detail.hit.zdb_id: 3113-6
    detail.hit.zdb_id: 1473050-9
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  • 9
    Online Resource
    Online Resource
    AIP Publishing ; 2002
    In:  Journal of Applied Physics Vol. 91, No. 8 ( 2002-04-15), p. 5442-5448
    In: Journal of Applied Physics, AIP Publishing, Vol. 91, No. 8 ( 2002-04-15), p. 5442-5448
    Abstract: Hydrogenated microcrystalline silicon thin films have been prepared by the rf glow discharge method using argon as a diluent of SiH4 to achieve a high growth rate. μc-Si:H film having conductivity ∼10−5 S cm−1 was achieved at a deposition rate of 36 Å/min at a moderate power density of 90 mW/cm2, without hydrogen dilution. Micrograins were identified with several well defined crystallographic orientations. Inhomogeneity and porosity at the grain boundary zone have a significant effect on the electrical properties of the films due to adsorption when exposed to atmosphere. However, by adding hydrogen to the Ar-diluted SiH4 plasma, a homogeneous and improved network structure without having any effect of adsorption was obtained at a reduced deposition rate. Highly conducting (σD∼10−3 S cm−1) undoped μc-Si:H film was prepared at a deposition rate of 15 Å/min having 90% crystalline volume fraction. The energy released by the de-excitation of Ar* in the plasma initiates rapid nucleation in the Si network and atomic hydrogen in the plasma helps in the defect elimination, structural reorientation, and grain growth.
    Type of Medium: Online Resource
    ISSN: 0021-8979 , 1089-7550
    Language: English
    Publisher: AIP Publishing
    Publication Date: 2002
    detail.hit.zdb_id: 3112-4
    detail.hit.zdb_id: 1476463-5
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  • 10
    Online Resource
    Online Resource
    AIP Publishing ; 2003
    In:  Journal of Applied Physics Vol. 94, No. 4 ( 2003-08-15), p. 2498-2506
    In: Journal of Applied Physics, AIP Publishing, Vol. 94, No. 4 ( 2003-08-15), p. 2498-2506
    Abstract: Field effect transistors based on a GaN/AlGaN system have shown remarkable performance characteristics in a wide range of device applications. However, due to the large effective mass of GaN, the mobility in the channel is small. In this work, we consider a GaN/AlGaN structure with a thin InN channel of the order of a few monolayers. We find that mobility in the channel can improve considerably while breakdown characteristics are not expected to suffer. Mobilities of ≃2500 cm2 (V s)−1 are predicted along with high sheet charges for low interface disorder. Good agreement with experimental results is observed for higher degrees of disorder within the model. At higher electric fields, we find that most electron population transfers to higher valleys or other subbands that lie in AlGaN or GaN. We also compare the low-field mobility-charge product for this structure with the conventional AlGaN/GaN structure and find that the two values are similar.
    Type of Medium: Online Resource
    ISSN: 0021-8979 , 1089-7550
    Language: English
    Publisher: AIP Publishing
    Publication Date: 2003
    detail.hit.zdb_id: 3112-4
    detail.hit.zdb_id: 1476463-5
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