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1.  Field Evaluation of Polymer Capacitive Humidity Sensors for Bowen Ratio Energy Balance Flux Measurements 
Sensors (Basel, Switzerland)  2010;10(8):7748-7771.
The possibility of reliable, reasonably accurate and relatively inexpensive estimates of sensible heat and latent energy fluxes was investigated using a commercial combination thin-film polymer capacitive relative humidity and adjacent temperature sensor instrument. Long-term and unattended water vapour pressure profile difference measurements using low-power combination instruments were compared with those from a cooled dewpoint mirror hygrometer, the latter often used with Bowen ratio energy balance (BREB) systems. An error analysis, based on instrument relative humidity and temperature errors, was applied for various capacitive humidity instrument models. The main disadvantage of a combination capacitive humidity instrument is that two measurements, relative humidity and temperature, are required for estimation of water vapour pressure as opposed to one for a dewpoint hygrometer. In a laboratory experiment using an automated procedure, water vapour pressure differences generated using a reference dewpoint generator were measured using a commercial model (Dew-10) dewpoint hygrometer and a combination capacitive humidity instrument. The laboratory measurement comparisons showed that, potentially, an inexpensive model combination capacitive humidity instrument (CS500 or HMP50), or for improved results a slightly more expensive model (HMP35C or HMP45C), could substitute for the more expensive dewpoint hygrometer. In a field study, in a mesic grassland, the water vapour pressure measurement noise for the combination capacitive humidity instruments was greater than that for the dewpoint hygrometer. The average water vapour pressure profile difference measured using a HMP45C was highly correlated with that from a dewpoint hygrometer with a slope less than unity. Water vapour pressure measurements using the capacitive humidity instruments were not as accurate, compared to those obtained using a dewpoint hygrometer, but the resolution magnitudes for the profile difference measurements were less than the minimum of 0.01 kPa required for BREB measurements when averaged over 20 min. Furthermore, the longer-term capacitive humidity measurements are more reliable and not dependent on a sensor bias adjustment as is the case for the dewpoint hygrometer. A field comparison of CS500 and HMP45C profile water vapour pressure differences yielded a slope of close to unity. However, the CS500 exhibited more variable water vapour pressure measurements mainly due to its increased variation in temperature measurements compared to the HMP45C. Comparisons between 20-min BREB sensible heat fluxes obtained using a HMP45C and a dewpoint hygrometer yielded a slope of almost unity. BREB sensible heat fluxes measured using a HMP45C were reasonably well correlated with those obtained using a surface-layer scintillometer and eddy covariance (slope of 0.9629 and 0.9198 respectively). This reasonable agreement showed that a combination capacitive humidity instrument, with similar relative humidity (RH) and temperature error magnitudes of at most 2% RH and 0.3 °C respectively, and similar measurement time response, would be an adequate and less expensive substitute for a dewpoint hygrometer. Furthermore, a combination capacitive humidity instrument requires no servicing compared to a dewpoint hygrometer which requires a bias adjustment and mirror cleaning each week. These findings make unattended BREB measurements of sensible heat flux and evaporation cheaper and more reliable with the system easier to assemble and service and with reduced instrument power.
doi:10.3390/s100807748
PMCID: PMC3231178  PMID: 22163625
humidity resolution; energy balance fluxes; humidity measurement; surface-layer scintillometer; eddy covariance
2.  Free-solution electrophoretic separations of DNA–drag-tag conjugates on glass microchips with no polymer network and no loss of resolution at increased electric field strength 
Electrophoresis  2011;32(10):1201-1208.
Here, we demonstrate the potential for high-resolution electrophoretic separations of ssDNA-protein conjugates in borosilicate glass microfluidic chips, with no sieving media and excellent repeatability. Using polynucleotides of two different lengths conjugated to moderately cationic protein polymer drag-tags, we measured separation efficiency as a function of applied electric field. In excellent agreement with prior theoretical predictions of Slater et al., resolution is found to remain constant as applied field is increased up to 700 V/cm, the highest field we were able to apply. This remarkable result illustrates the fundamentally different physical limitations of Free-Solution Conjugate Electrophoresis (FSCE)-based DNA separations relative to matrix-based DNA electrophoresis. Single-stranded DNA separations in “gels” have always shown rapidly declining resolution as the field strength is increased; this is especially true for ssDNA > 400 bases in length. FSCE’s ability to decouple DNA peak resolution from applied electric field suggests the future possibility of ultra-rapid FSCE sequencing on chips. We investigated sources of peak broadening for FSCE separations on borosilicate glass microchips, using six different protein polymer drag-tags. For drag-tags with four or more positive charges, electrostatic and adsorptive interactions with pHEA-coated microchannel walls led to appreciable band-broadening, while much sharper peaks were seen for bioconjugates with nearly charge-neutral protein drag-tags.
doi:10.1002/elps.201000574
PMCID: PMC3416026  PMID: 21500207
Drag-tag; ELFSE; FSCE; Free-solution microchip electrophoresis; Band broadening
3.  Introduction to power-frequency electric and magnetic fields. 
Environmental Health Perspectives  1993;101(Suppl 4):73-81.
This paper introduces the reader to electric and magnetic fields, particularly those fields produced by electric power systems and other sources using frequencies in the power-frequency range. Electric fields are produced by electric charges; a magnetic field also is produced if these charges are in motion. Electric fields exert forces on other charges; if in motion, these charges will experience magnetic forces. Power-frequency electric and magnetic fields induce electric currents in conducting bodies such as living organisms. The current density vector is used to describe the distribution of current within a body. The surface of the human body is an excellent shield for power-frequency electric fields, but power-frequency magnetic fields penetrate without significant attenuation; the electric fields induced inside the body by either exposure are comparable in magnitude. Electric fields induced inside a human by most environmental electric and magnetic fields appear to be small in magnitude compared to levels naturally occurring in living tissues. Detection of such fields thus would seem to require the existence of unknown biological mechanisms. Complete characterization of a power-frequency field requires measurement of the magnitudes and electrical phases of the fundamental and harmonic amplitudes of its three vector components. Most available instrumentation measures only a small subset, or some weighted average, of these quantities. Hand-held survey meters have been used widely to measure power-frequency electric and magnetic fields. Automated data-acquisition systems have come into use more recently to make electric- and magnetic-field recordings, covering periods of hours to days, in residences and other environments.(ABSTRACT TRUNCATED AT 250 WORDS)
PMCID: PMC1519708  PMID: 8206045
4.  Citrate-capped gold nanoparticle electrophoretic heat production in response to a time-varying radiofrequency electric-field 
The evaluation of heat production from gold nanoparticles (AuNPs) irradiated with radiofrequency (RF) energy has been problematic due to Joule heating of their background ionic buffer suspensions. Insights into the physical heating mechanism of nanomaterials under RF excitations must be obtained if they are to have applications in fields such as nanoparticle-targeted hyperthermia for cancer therapy. By developing a purification protocol which allows for highly-stable and concentrated solutions of citrate-capped AuNPs to be suspended in high-resistivity water, we show herein, for the first time, that heat production is only evident for AuNPs of diameters ≤ 10 nm, indicating a unique size-dependent heating behavior not previously observed. Heat production has also shown to be linearly dependent on both AuNP concentration and total surface area, and severely attenuated upon AuNP aggregation. These relationships have been further validated using permittivity analysis across a frequency range of 10 MHz to 3 GHz, as well as static conductivity measurements. Theoretical evaluations suggest that the heating mechanism can be modeled by the electrophoretic oscillation of charged AuNPs across finite length scales in response to a time-varying electric field. It is anticipated these results will assist future development of nanoparticle-assisted heat production by RF fields for applications such as targeted cancer hyperthermia.
doi:10.1021/jp309053z
PMCID: PMC3686525  PMID: 23795228
Radiofrequency; Gold; Nanoparticles; Heating; Permittivity
5.  Monitoring Scanning Electrochemical Microscopy Approach Curves with Mid-Infrared Spectroscopy – Towards a Novel Current-Independent Positioning Mode 
Analytical chemistry  2010;82(8):3132-3138.
Single-bounce attenuated total reflection infrared spectroscopy in the 3–20 µm range (MIR) has been combined with scanning electrochemical microscopy (SECM) for in situ spectroscopic detection of electrochemically induced localized surface modifications using an ultramicroelectrode (UME). In this study, a novel current-independent approach for positioning the UME in aqueous electrolyte solution is presented using either changes of IR absorption intensity associated with borosilicate glass (BSG), which is used as shielding material of the UME wire, or by monitoring IR changes of the water spectrum within the penetration depth of the evanescent field due to displacement of water molecules in the volume between the sample surface and the UME within the evanescent field. The experimental results show that the UME penetrates into the exponentially decaying evanescent field in close vicinity (a few µm) to the ATR crystal surface. Hence, the resulting intensity changes of the IR absorption spectra for borosilicate glass (increase) and for water (decrease), can be used to determine the position of the UME relative to the ATR crystal surface independent of the current measured at the UME.
doi:10.1021/ac902781h
PMCID: PMC2862910  PMID: 20329757
6.  ON THE LOCATION OF THE FORCES WHICH DETERMINE THE ELECTRICAL DOUBLE LAYER BETWEEN COLLODION PARTICLES AND WATER 
1. The cataphoretic P.D. of suspended particles is assumed to be due to an excess in the concentration of one kind of a pair of oppositely charged ions in the film of water enveloping the particles and this excess is generally ascribed to a preferential adsorption of this kind of ions by the particle. The term adsorption fails, however, to distinguish between the two kinds of forces which can bring about such an unequal distribution of ions between the enveloping film and the opposite film of the electrical double layer, namely, forces inherent in the water itself and forces inherent in the particle (e.g. chemical attraction between particle and adsorbed ions). 2. It had been shown in a preceding paper that collodion particles suspended in an aqueous solution of an ordinary electrolyte like NaCl, Na2SO4, Na4Fe(CN)6, CaCl2, HCl, H2SO4, or NaOH are always negatively charged, and that the addition of these electrolytes increases the negative charge as long as their concentration is below M/1,000 until a certain maximal P.D. is reached. Hence no matter whether acid, alkali, or a neutral salt is added, the concentration of anions must always be greater in the film enveloping the collodion particles than in the opposite film of the electrical double layer, and the reverse is true for the concentration of cations. This might suggest that the collodion particles, on account of their chemical constitution, attract anions with a greater force than cations, but such an assumption is rendered difficult in view of the following facts. 3. Experiments with dyes show that at pH 5.8 collodion particles are stained by basic dyes (i.e. dye cations) but not by acid dyes (i.e. dye anions), and that solutions of basic dyes are at pH 5.8 more readily decolorized by particles of collodion than acid dyes. It is also shown in this paper that crystalline egg albumin, gelatin, and Witte's peptone form durable films on collodion only when the protein exists in the form of a cation or when it is isoelectric, but not when it exists in the form of an anion (i.e. on the alkaline side of its isoelectric point). Hence if any ions of dyes or proteins are permanently bound at the surface of collodion particles through forces inherent in the collodion they are cations but not anions. The fact that isoelectric proteins form durable films on collodion particles suggests, that the forces responsible for this combination are not ionic. 4. It is shown that salts of dyes or proteins, the cations of which are capable of forming durable films on the surface of the collodion, influence the cataphoretic P.D. of the collodion particles in a way entirely different from that of any other salts inasmuch as surprisingly low concentrations of salts, the cation of which is a dye or a protein, render the negatively charged collodion particles positive. Crystalline egg albumin and gelatin have such an effect even in concentrations of 1/130,000 or 1/65,000 of 1 per cent, i.e. in a probable molar concentration of about 10–9. 5. Salts in which the dye or protein is an anion have no such effect but act like salts of the type of NaCl or Na2SO4 on the cataphoretic P.D. of collodion particles. 6. Amino-acids do not form durable films on the surface of collodion particles at any pH and the salts of amino-acids influence their cataphoretic P.D. in the same way as NaCl but not in the same way as proteins or dyes, regardless of whether the amino-acid ion is a cation or an anion. 7. Ordinary salts like LaCl3 also fail to form a durable film on the surface of collodion particles. 8. Until evidence to the contrary is furnished, these facts seem to suggest that the increase of the negative charge of the collodion particles caused by the addition of low concentrations of ordinary electrolytes is chiefly if not entirely due to forces inherent in the aqueous solution but to a less extent, if at all, due to an attraction of the anions of the electrolyte by forces inherent in the collodion particles.
PMCID: PMC2140615  PMID: 19872044
7.  Plasmonic and photonic scattering and near fields of nanoparticles 
We theoretically compare the scattering and near field of nanoparticles from different types of materials, each characterized by specific optical properties that determine the interaction with light: metals with their free charge carriers giving rise to plasmon resonances, dielectrics showing zero absorption in wide wavelength ranges, and semiconductors combining the two beforehand mentioned properties plus a band gap. Our simulations are based on Mie theory and on full 3D calculations of Maxwell’s equations with the finite element method. Scattering and absorption cross sections, their division into the different order electric and magnetic modes, electromagnetic near field distributions around the nanoparticles at various wavelengths as well as angular distributions of the scattered light were investigated. The combined information from these calculations will give guidelines for choosing adequate nanoparticles when aiming at certain scattering properties. With a special focus on the integration into thin film solar cells, we will evaluate our results.
doi:10.1186/1556-276X-9-50
PMCID: PMC3915561  PMID: 24475923
Nanoparticles; Plasmonics; Photonics; Scattering; Near field; Mie theory; FEM simulations; Solar cells; 42.70.-a; 78.67.Bf; 73.20.Mf
8.  THE PENETRATION OF VESICANT VAPORS INTO HUMAN SKIN 
The Journal of General Physiology  1946;29(6):441-469.
Analytical methods which are accurate to about 1 per cent have been developed for the determination of small amounts (ca. 500 γ) of bis(β-chloroethyl)-sulfide (H), ethyl-bis(β-chloroethyl)amine (EBA), tris(β-chloroethyl)amine (TBA), β-chloroethyl-benzylsulfide (benzyl-H), and β-chloroethyl-ethylsulfide (ethyl-H). The determinations are made by micro titration of the HCl liberated upon complete hydrolysis of the vesicants. A description is given of an apparatus suitable for applying vapors of vesicants to unit areas of skin. A very precise and reproducible micropipetting technique is described for the introduction of the vesicants into the penetration apparatus. By means of this penetration apparatus studies have been made of several factors which may influence the rate at which vesicant vapors penetrate into skin. Model experiments have been performed in which H was allowed to vaporize and the vapor was absorbed on a surface such as that of diethylene glycol or vaseline. It has been found that if the surface of liquid H is increased by spreading the agent on filter paper, the rate of evaporation is markedly increased. Furthermore, if the vapor is agitated by means of a magnetically driven fan, the rate of absorption by diethylene glycol is greatly accelerated. With vaseline as the absorbing surface it has been found that the area of the absorbing surface has an effect on the rate of absorption of H vapor. More H is absorbed by vaseline spread on filter paper to give a rough surface than is absorbed by a smooth film of vaseline. Measurements of the rate of penetration into human skin of H, EBA, TBA, benzyl-H, and ethyl-H vapors have been performed at 21–23°C. and 30–31°C. by means of the penetration apparatus described in this paper. The measurements were carred out on human volunteers under conditions of controlled temperature and humidity. When human skin is exposed to air saturated with H vapor, the H penetrates the skin of the forearm at a rate of about 1.4 γ per cm.2 per minute (temperature 21–23°C.; relative humidity 46 per cent). This value was found to hold in experiments in which H vapor was applied for 3 to 30 minute intervals, thus indicating that the permeability of the skin to H vapor is not altered during a 30 minute exposure. Agitation of the H vapor by fanning did not result in any measurable increase in the rate of penetration. Two of the volunteers were Negroes; the permeability of their skin to H vapor did not differ appreciably from that found for the other subjects. When human skin is exposed to air saturated with EBA vapor, the vesicant penetrates at the rate of 2.8 γ per cm.2 per minute (temperature 22°C., relative humidity 50 to 52 per cent). The amount of EBA penetrated is linear with exposure time for exposure periods of 5 to 20 minutes. Under similar conditions, it was found that TBA penetrates at a rate of about 0.18 γ per cm.2 per minute (temperature 22–23°C.; relative humidity 45 to 48 per cent). This value was found to hold in experiments in which TBA vapor was applied for 30 to 60 minute intervals. The amount of TBA penetrated is linear with exposure time. In the case of benzyl-H, a linear relationship between the amount lost from the penetration cup and exposure time was also observed but the plot did not pass through the origin. It is suggested that this anomaly is due to retention on the skin surface of an appreciable quantity of benzyl-H as a result of rapid physical adsorption or chemical combination with a constituent of the skin. The rate of penetration of benzyl-H may be calculated from the slope of the plot and is found to be 0.35 γ per cm.2 per minute (temperature 22°C., relative humidity 55 to 60 per cent). The results with ethyl-H showed great variation among individual subjects and no satisfactory value for the rate of penetration can be given as yet. Measurements were also made of the rate of penetration of H, EBA, and TBA vapors at 30–31°C. (relative humidity 47 to 49 per cent). At this temperature, a linear relationship was observed between the amount penetrated and the time of exposure. H vapor penetrated at a rate of 2.7 γ per cm.2 per minute, EBA vapor at 5.1 γ per cm.2 per minute, and TBA vapor at 0.29 γ per cm.2 per minute. Three of the subjects in the EBA measurements were Negroes. The permeability of their skin to EBA vapor did not differ from that found for the white subjects. Despite this fact, their skin failed to vesicate after an exposure period twice that which caused 50 per cent vesication in the white subjects. Calculation of the precision of the data showed that the average deviation, standard deviation, and standard error were not appreciably different for the data obtained with human subjects as compared with data for control experiments in which human skin was not involved. Consequently, no significant differences in the rate of penetration into the skin of individual subjects can be discerned from the data presented in this communication. The increase in the rate of penetration of H, EBA, and TBA vapors from 21–23°C. to 30–31°C. is approximately proportional to the increase in volatility of each agent. These results indicate that at the same gas concentration in milligrams per liter, H, EBA, and TBA vapors would all penetrate at about the same rate. The data presented above permit a determination of the approximate amount of each vesicant which must penetrate to cause vesication in about 50 per cent of the exposed sites. This amount has been designated by the symbol V50. The V50 for H and TBA at 21–23°C. is the same, being about 6γ; at 30–31°C., the V50 is 4 to 5 γ. On the other hand, the V50 for EBA at 22°C. and 30–31°C. is about 26 to 28 γ. Thus, per gamma penetrated, H and TBA vapors are about equally effective in producing vesication while EBA vapor is only ⅕ to ⅛ as effective.
PMCID: PMC2142809  PMID: 19873472
9.  Electrohydrodynamics of Charge Separation in Droplet-Based Ion Sources with Time-Varying Electrical and Mechanical Actuation 
Charge transport and separation in mechanically-driven, droplet-based ion sources are investigated using computational analysis and supporting experiments. A first-principles model of electrohydrodynamics (EHD) and charge migration is formulated and implemented using FLUENT CFD software for jet/droplet formation. For validation, classical experiments of electrospraying from a thin capillary are simulated, specifically, the transient EHD cone-jet formation of a fluid with finite electrical conductivity, and the Taylor cone formation in a perfectly electrically-conducting fluid. The model is also used to investigate the microscopic physics of droplet charging in mechanically-driven droplet-based ion sources, such as AMUSE (Array of Micromachined UltraSonic Electrospray). Here, AMUSE is subject to DC and AC electric fields of varying amplitude and phase, with respect to a time-varying mechanical force driving the droplet formation. For the DC-charging case, a linear relationship is demonstrated between the charge carried by each droplet and an applied electric field magnitude, in agreement with previously reported experiments. For the AC-charging case, a judiciously-chosen phase-shift in the time-varying mechanical (driving ejection) and electrical (driving charge transport) signals allows for a significantly increased amount of charge, of desired polarity, to be pumped into a droplet upon ejection. Complementary experimental measurements of electrospray electrical current and charge-per-droplet, produced by the AMUSE ion source, are performed and support theoretical predictions for both DC and AC-charging cases. The theoretical model and simulation tools provide a versatile and general analytical framework for fundamental investigations of coupled electrohydrodynamics and charge transport. The model also allows for the exploration of different configurations and operating modes to optimize charge separation in atmospheric pressure electrohydrodynamic ion sources under static and dynamic electrical and mechanical fields.
doi:10.1016/j.jasms.2009.12.022
PMCID: PMC2847640  PMID: 20149681
10.  The effect of ambient humidity on the electrical properties of graphene oxide films 
Nanoscale Research Letters  2012;7(1):363.
We investigate the effect of water adsorption on the electrical properties of graphene oxide (GO) films using the direct current (DC) measurement and alternating current (AC) complex impedance spectroscopy. GO suspension synthesized by a modified Hummer's method is deposited on Au interdigitated electrodes. The strong electrical interaction of water molecules with GO films was observed through electrical characterizations. The DC measurement results show that the electrical properties of GO films are humidity- and applied voltage amplitude-dependent. The AC complex impedance spectroscopy method is used to analyze the mechanism of electrical interaction between water molecules and GO films in detail. At low humidity, GO films exhibit poor conductivity and can be seen as an insulator. However, at high humidity, the conductivity of GO films increases due to the enhancement of ion conduction. Our systematic research on this effect provides the fundamental supports for the development of graphene devices originating from solution-processed graphene oxide.
doi:10.1186/1556-276X-7-363
PMCID: PMC3467191  PMID: 22748079
Graphene oxide; Humidity sensing; Complex impedance spectroscopy; Nano device
11.  Spatial variation of permittivity of an electrolyte solution in contact with a charged metal surface: a mini review 
Contact between a charged metal surface and an electrolyte implies a particular ion distribution near the charged surface, i.e. the electrical double layer. In this mini review, different mean-field models of relative (effective) permittivity are described within a simple lattice model, where the orientational ordering of water dipoles in the saturation regime is taken into account. The Langevin-Poisson-Boltzmann (LPB) model of spatial variation of the relative permittivity for point-like ions is described and compared to a more general Langevin-Bikerman (LB) model of spatial variation of permittivity for finite-sized ions. The Bikerman model and the Poisson-Boltzmann model are derived as limiting cases. It is shown that near the charged surface, the relative permittivity decreases due to depletion of water molecules (volume-excluded effect) and orientational ordering of water dipoles (saturation effect). At the end, the LPB and LB models are generalised by also taking into account the cavity field.
doi:10.1080/10255842.2011.624769
PMCID: PMC3664910  PMID: 22263808
charged metal surface; relative permittivity; electric double layer; finite element method; metallic electrode; water ordering; finite-sized ions; saturation effect; excluded volume effect
12.  Theoretical Treatment and Numerical Simulation of Potential and Concentration Profiles in Extremely Thin Non-Electroneutral Membranes Used for Ion-Selective Electrodes 
The applicability of extremely thin non-electroneutral membranes for ion-selective electrodes (ISEs) is investigated. A theoretical treatment of potential and concentration profiles in space-charge membranes of << 1 μm thickness is presented. The theory is based on the Nernst-Planck equation for ion fluxes, which reduces to Boltzmann’s formula at equilibrium, and on the Poisson relationship between space-charge density and electric field gradient. A general solution in integral form is obtained for the potential function and the corresponding ion profiles at equilibrium. A series of explicit sub-solutions is derived for particular cases. Membrane systems with up to three different ion species are discussed, including trapped ionic sites and co-extracted ions. Solid-contacted thin membranes (without formation of aqueous films at the inner interface) are shown to exhibit a sub-Nernstian response. The theoretical results are confirmed by numerical simulations using a simplified finite-difference procedure based on the Nernst-Planck-Poisson model, which are shown to be in excellent agreement.
doi:10.1016/j.jelechem.2010.01.001
PMCID: PMC3523753  PMID: 23255874
Ion-selective electrodes; Thin membranes; Space charge; Potential; Concentration profiles; Theory; Numerical simulation; Nernst-Planck-Poisson model
13.  Fabrication and Characterization of Polyaniline/PVA Humidity Microsensors 
Sensors (Basel, Switzerland)  2011;11(8):8143-8151.
This study presents the fabrication and characterization of a humidity microsensor that consists of interdigitated electrodes and a sensitive film. The area of the humidity microsensor is about 2 mm2. The sensitive film is polyaniline doping polyvinyl alcohol (PVA) that is prepared by the sol-gel method, and the film has nanofiber and porous structures that help increase the sensing reaction. The commercial 0.35 μm Complimentary Metal Oxide Semiconductor (CMOS) process is used to fabricate the humidity microsensor. The sensor needs a post-CMOS process to etch the sacrificial layer and to coat the sensitive film on the interdigitated electrodes. The sensor produces a change in resistance as the polyaniline/PVA film absorbs or desorbs vapor. Experimental results show that the sensitivity of the humidity sensor is about 12.6 kΩ/%RH at 25 °C.
doi:10.3390/s110808143
PMCID: PMC3231745  PMID: 22164067
humidity microsensors; polyaniline; polyvinyl alcohol; MEMS
14.  Incorporating Phase-Dependent Polarizability in Non-Additive Electrostatic Models for Molecular Dynamics Simulations of the Aqueous Liquid-Vapor Interface 
We discuss a new classical water force field that explicitly accounts for differences in polarizability between liquid and vapor phases. The TIP4P-QDP (4-point transferable intermolecular potential with charge dependent-polarizability) force field is a modification of the original TIP4P-FQ fluctuating charge water force field of Rick et al.1 that self-consistently adjusts its atomic hardness parameters via a scaling function dependent on the M-site charge. The electronegativity (χ) parameters are also scaled in order to reproduce condensed-phase dipole moments of comparable magnitude to TIP4P-FQ. TIP4P-QDP is parameterized to reproduce experimental gas-phase and select condensed-phase properties. The TIP4P-QDP water model possesses a gas phase polarizability of 1.40 Å3 and gas-phase dipole moment of 1.85 Debye, in excellent agreement with experiment and high-level ab initio predictions. The liquid density of TIP4P-QDP is 0.9954(±0.0002) g/cm3 at 298 K and 1 atmosphere, and the enthalpy of vaporization is 10.55(±0.12) kcal/mol. Other condensed-phase properties such as the isobaric heat capacity, isothermal compressibility, and diffusion constant are also calculated within reasonable accuracy of experiment and consistent with predictions of other current state-of-the-art water force fields. The average molecular dipole moment of TIP4P-QDP in the condensed phase is 2.641(±0.001) Debye, approximately 0.02 Debye higher than TIP4P-FQ and within the range of values currently surmised for the bulk liquid. The dielectric constant, ε = 85.8 ± 1.0, is 10% higher than experiment. This is reasoned to be due to the increase in the condensed phase dipole moment over TIP4P-FQ, which estimates ε remarkably well. Radial distribution functions for TIP4P-QDP and TIP4P-FQ show similar features, with TIP4P-QDP showing slightly reduced peak heights and subtle shifts towards larger distance interactions. Since the greatest effects of the phase-dependent polarizability are anticipated in regions with both liquid and vapor character, interfacial simulations of TIP4P-QDP were performed and compared to TIP4P-FQ, a static polarizability analog. Despite similar features in density profiles such as the position of the GDS and interfacial width, enhanced dipole moments are observed for the TIP4P-QDP interface and onset of the vapor phase. Water orientational profiles show an increased preference (over TIP4P-FQ) in the orientation of the permanent dipole vector of the molecule within the interface; an enhanced z-induced dipole moment directly results from this preference. Hydrogen bond formation is lower, on average, in the bulk for TIP4P-QDP than TIP4P-FQ. However, the average number of hydrogen bonds formed by TIP4P-QDP in the interface exceeds that of TIP4P-FQ, and observed hydrogen bond networks extend further into the gaseous region. The TIP4P-QDP interfacial potential, calculated to be -11.98(±0.08) kcal/mol, is less favorable than that for TIP4P-FQ by approximately 2% as a result of a diminished quadrupole contribution. Surface tension is calculated within a 1.3% reduction from the experimental value. Results reported demonstrate TIP4P-QDP as a model comparable to the popular TIP4P-FQ while accounting for a physical effect previously neglected by other water models. Further refinements to this model, as well as future applications are discussed.
doi:10.1021/ct800320f
PMCID: PMC3488353  PMID: 23133341
Phase Dependent Polarizability; Molecular Dynamics; Charge Equilibration; Polarizable Force Field; Liquid-Vapor Interface; TIP4P-QDP
15.  Three-Dimensional Microstructural Properties of Nanofibrillated Cellulose Films 
Nanofibrillated cellulose (NFC) films have potential as oxygen barriers for, e.g., food packaging applications, but their use is limited by their hygroscopic characteristics. The three-dimensional microstructure of NFC films made of Pinus radiata (Radiata Pine) kraft pulp fibres has been assessed in this study, considering the structural development as a function of relative humidity (RH). The surface roughness, micro-porosity, thickness and their correlations were analyzed using X-ray microtomography (X–μCT) and computerized image analysis. The results are compared to those from scanning electron microscopy and laser profilometry. Based on a series of films having varying amounts of 2,2,6,6-tetramethylpiperidinyl-1-oxyl (TEMPO)-mediated oxidated nanofibrils, it was demonstrated that X–μCT is suitable for assessing the surface and bulk 3D microstructure of the cellulose films. Additionally, one of the series was assessed at varying humidity levels, using the non-destructive capabilities of X–μCT and a newly developed humidity chamber for in-situ characterization. The oxygen transmission rate (OTR) of the films (20 g/m2) was below 3.7mLm−2 day−1 at humidity levels below 60% RH. However, the OTR increased considerably to 12.4mLm−2 day−1 when the humidity level increased to 80% RH. The increase in OTR was attributed to a change of the film porosity, which was reflected as an increase in local thickness. Hence, the characterization techniques applied in this study shed more light on the structures of NFC films and how they are affected by varying humidity levels. It was demonstrated that in increasing relative humidity the films swelled and the oxygen barrier properties decreased.
doi:10.3390/ijms15046423
PMCID: PMC4013638  PMID: 24743887
nanofibrillated cellulose; NFC; oxygen transmission rate; OTR; tomography; humidity
16.  Electric field depth–focality tradeoff in transcranial magnetic stimulation: simulation comparison of 50 coil designs 
Brain stimulation  2012;6(1):1-13.
Background
Various transcranial magnetic stimulation (TMS) coil designs are available or have been proposed. However, key coil characteristics such as electric field focality and attenuation in depth have not been adequately compared. Knowledge of the coil focality and depth characteristics can help TMS researchers and clinicians with coil selection and interpretation of TMS studies.
Objective
To quantify the electric field focality and depth of penetration of various TMS coils.
Methods
The electric field distributions induced by 50 TMS coils were simulated in a spherical human head model using the finite element method. For each coil design, we quantified the electric field penetration by the half-value depth, d1/2, and focality by the tangential spread, S1/2, defined as the half-value volume (V1/2) divided by the half-value depth, S1/2 = V1/2/d1/2.
Results
The 50 TMS coils exhibit a wide range of electric field focality and depth, but all followed a depth–focality tradeoff: coils with larger half-value depth cannot be as focal as more superficial coils. The ranges of achievable d1/2 are similar between coils producing circular and figure-8 electric field patterns, ranging 1.0–3.5 cm and 0.9–3.4 cm, respectively. However, figure-8 field coils are more focal, having S1/2 as low as 5 cm2 compared to 34 cm2 for circular field coils.
Conclusions
For any coil design, the ability to directly stimulate deeper brain structures is obtained at the expense of inducing wider electrical field spread. Novel coil designs should be benchmarked against comparison coils with consistent metrics such as d1/2 and S1/2.
doi:10.1016/j.brs.2012.02.005
PMCID: PMC3568257  PMID: 22483681
transcranial magnetic stimulation; electric field; depth; focality; simulation
17.  A Humidity Sensing Organic-Inorganic Composite for Environmental Monitoring 
Sensors (Basel, Switzerland)  2013;13(3):3615-3624.
In this paper, we present the effect of varying humidity levels on the electrical parameters and the multi frequency response of the electrical parameters of an organic-inorganic composite (PEPC+NiPc+Cu2O)-based humidity sensor. Silver thin films (thickness ∼200 nm) were primarily deposited on plasma cleaned glass substrates by the physical vapor deposition (PVD) technique. A pair of rectangular silver electrodes was formed by patterning silver film through standard optical lithography technique. An active layer of organic-inorganic composite for humidity sensing was later spun coated to cover the separation between the silver electrodes. The electrical characterization of the sensor was performed as a function of relative humidity levels and frequency of the AC input signal. The sensor showed reversible changes in its capacitance with variations in humidity level. The maximum sensitivity ∼31.6 pF/%RH at 100 Hz in capacitive mode of operation has been attained. The aim of this study was to increase the sensitivity of the previously reported humidity sensors using PEPC and NiPc, which has been successfully achieved.
doi:10.3390/s130303615
PMCID: PMC3658764  PMID: 23493124
composite film; humidity sensor; physical vapor deposition; scanning electron micrograph
18.  Magnetic Behavior of Surface Nanostructured 50-nm Nickel Thin Films 
Nanoscale Research Letters  2010;5(10):1596-1602.
Thermally evaporated 50-nm nickel thin films coated on borosilicate glass substrates were nanostructured by excimer laser (0.5 J/cm2, single shot), DC electric field (up to 2 kV/cm) and trench-template assisted technique. Nanoparticle arrays (anisotropic growth features) have been observed to form in the direction of electric field for DC electric field treatment case and ruptured thin film (isotropic growth features) growth for excimer laser treatment case. For trench-template assisted technique; nanowires (70–150 nm diameters) have grown along the length of trench template. Coercive field and saturation magnetization are observed to be strongly dependent on nanostructuring techniques.
doi:10.1007/s11671-010-9682-2
PMCID: PMC2956046  PMID: 21076670
Magnetic nanostructures; Magnetic properties; Surface treatment
19.  Magnetic Behavior of Surface Nanostructured 50-nm Nickel Thin Films 
Nanoscale Research Letters  2010;5(10):1596-1602.
Thermally evaporated 50-nm nickel thin films coated on borosilicate glass substrates were nanostructured by excimer laser (0.5 J/cm2, single shot), DC electric field (up to 2 kV/cm) and trench-template assisted technique. Nanoparticle arrays (anisotropic growth features) have been observed to form in the direction of electric field for DC electric field treatment case and ruptured thin film (isotropic growth features) growth for excimer laser treatment case. For trench-template assisted technique; nanowires (70–150 nm diameters) have grown along the length of trench template. Coercive field and saturation magnetization are observed to be strongly dependent on nanostructuring techniques.
doi:10.1007/s11671-010-9682-2
PMCID: PMC2956046  PMID: 21076670
Magnetic nanostructures; Magnetic properties; Surface treatment
20.  Ultrahigh humidity sensitivity of graphene oxide 
Scientific Reports  2013;3:2714.
Humidity sensors have been extensively used in various fields, and numerous problems are encountered when using humidity sensors, including low sensitivity, long response and recovery times, and narrow humidity detection ranges. Using graphene oxide (G-O) films as humidity sensing materials, we fabricate here a microscale capacitive humidity sensor. Compared with conventional capacitive humidity sensors, the G-O based humidity sensor has a sensitivity of up to 37800% which is more than 10 times higher than that of the best one among conventional sensors at 15%–95% relative humidity. Moreover, our humidity sensor shows a fast response time (less than 1/4 of that of the conventional one) and recovery time (less than 1/2 of that of the conventional one). Therefore, G-O appears to be an ideal material for constructing humidity sensors with ultrahigh sensitivity for widespread applications.
doi:10.1038/srep02714
PMCID: PMC3776968  PMID: 24048093
21.  Optimal sensitometric curves of Kodak EDR2 film for dynamic intensity modulated radiation therapy verification 
Purpose:
To investigate the optimal sensitometric curves of extended dose range (EDR2) radiographic film in terms of depth, field size, dose range and processing conditions for dynamic intensity modulated radiation therapy (IMRT) dosimetry verification with 6 MV X-ray beams.
Materials and methods:
A Varian Clinac 23 EX linear accelerator with 6 MV X-ray beam was used to study the response of Kodak EDR2 film. Measurements were performed at depths of 5, 10 and 15 cm in MedTec virtual water phantom and with field sizes of 2x2, 3x3, 10x10 and 15x15 cm2. Doses ranging from 20 to 450 cGy were used. The film was developed with the Kodak RP X-OMAT Model M6B automatic film processor. Film response was measured with the Vidar model VXR-16 scanner. Sensitometric curves were applied to the dose profiles measured with film at 5 cm in the virtual water phantom with field sizes of 2x2 and 10x10 cm2 and compared with ion chamber data. Scanditronix/Wellhofer OmniProTM IMRT software was used for the evaluation of the IMRT plan calculated by Eclipse treatment planning.
Results:
Investigation of the reproducibility and accuracy of the film responses, which depend mainly on the film processor, was carried out by irradiating one film nine times with doses of 20 to 450 cGy. A maximum standard deviation of 4.9% was found which decreased to 1.9% for doses between 20 and 200 cGy. The sensitometric curves for various field sizes at fixed depth showed a maximum difference of 4.2% between 2x2 and 15x15 cm2 at 5 cm depth with a dose of 450 cGy. The shallow depth tended to show a greater effect of field size responses than the deeper depths. The sensitometric curves for various depths at fixed field size showed slightly different film responses; the difference due to depth was within 1.8% for all field sizes studied. Both field size and depth effect were reduced when the doses were lower than 450 cGy. The difference was within 2.5% in the dose range from 20 to 300 cGy for all field sizes and depths studied. Dose profiles measured with EDR2 film were consistent with those measured with an ion chamber. The optimal sensitometric curve was acquired by irradiating film at a depth of 5 cm with doses ranging from 20 to 450 cGy with a 3×3 cm2 multileaf collimator. The optimal sensitometric curve allowed accurate determination of the absolute dose distribution. In almost 200 cases of dynamic IMRT plan verification with EDR2 film, the difference between measured and calculated dose was generally less than 3% and with 3 mm distance to agreement when using gamma value verification.
Conclusion:
EDR2 film can be used for accurate verification of composite isodose distributions of dynamic IMRT when the optimal sensitometric curve has been established.
doi:10.2349/biij.4.1.e4
PMCID: PMC3097693  PMID: 21614315
IMRT treatment plan verification; EDR2 film; sensitometric curves
22.  Metal-Enhanced Fluorescence from Nanoparticulate Zinc Films 
A detailed study of metal-enhanced fluorescence (MEF) from fluorophores in the blue-to- red spectral region placed in close proximity to thermally evaporated zinc nanostructured films is reported. The zinc nanostructured films were deposited onto glass microscope slides as individual particles and were 1–10 nm in height and 20–100 nm in width, as characterized by Atomic Force Microscopy. The surface plasmon resonance peak of the zinc nanostructured films was ≈ 400 nm. Finite-difference time-domain calculations for single and multiple nanostructures organized in a staggered fashion on a solid support predict, as expected, that the electric fields are concentrated both around and between the nanostructures. Additionally, Mie scattering calculations show that the absorption and scattering components of the extinction spectrum are dominant in the UV and visible spectral ranges, respectively. Enhanced fluorescence emission accompanied by no significant changes in excited state lifetimes of fluorophores with emission wavelengths in the visible blue-to-red spectral range near-to zinc nanostructured films were observed, implying that MEF from zinc nanostructured films is mostly due to an electric field enhancement effect.
doi:10.1021/jp806790u
PMCID: PMC2676115  PMID: 19946356
Metal-Enhanced Fluorescence; Plasmon-Enhanced Fluorescence; Surface-Enhanced Fluorescence; Plasmonics; Radiative Decay Engineering; Zinc Oxide Nanostructures; Silver Island Films; Metallic Nanostructures; Plasmonic Nanostructures; Aluminum Nanostructures; Fluorophores
23.  Interface traps and quantum size effects on the retention time in nanoscale memory devices 
Nanoscale Research Letters  2013;8(1):369.
Based on the analysis of Poisson equation, an analytical surface potential model including interface charge density for nanocrystalline (NC) germanium (Ge) memory devices with p-type silicon substrate has been proposed. Thus, the effects of Pb defects at Si(110)/SiO2, Si(111)/SiO2, and Si(100)/SiO2 interfaces on the retention time have been calculated after quantum size effects have been considered. The results show that the interface trap density has a large effect on the electric field across the tunneling oxide layer and leakage current. This letter demonstrates that the retention time firstly increases with the decrease in diameter of NC Ge and then rapidly decreases with the diameter when it is a few nanometers. This implies that the interface defects, its energy distribution, and the NC size should be seriously considered in the aim to improve the retention time from different technological processes. The experimental data reported in the literature support the theoretical expectation.
doi:10.1186/1556-276X-8-369
PMCID: PMC3847579  PMID: 23984827
Interface trap; Nanocrystalline; Quantum-size effect; Memory; Retention time; 85.30.Tv; 85.35.-p; 73.63.-b
24.  Structural responses of DNA-DDAB films to varying hydration and temperature 
The structure of a DNA-dimethyldidodecylammonium bromide (DDAB) film was recently described to undergo a distinctive transition in response to the water content in the surrounding environment.1 The existence, preparation, and basic properties of DNA-surfactant films have been known in the literature for some time.2,3 Here, we describe the structural response of DNA-DDAB films to environmental changes, particularly temperature and humidity, in greater detail revealing new structural states. We can direct the lamellar structure of the film into three distinct states – double-stranded DNA (dsDNA) paired with an interdigitated bilayer of DDAB (bDDAB), single-stranded DNA (ssDNA) with monolayer of DDAB (mDDAB), and ssDNA with bDDAB. Both temperature and humidity cause the molecules composing the lamellar structure to change reversibly from ssDNA to dsDNA and/or from mDDAB to bDDAB. We found that the structural transition from dsDNA to ssDNA and bDDAB to mDDAB is concerted and follows apparent first order kinetics. We also found that the double-stranded conformation of DNA in the film can be stabilized with the inclusion of cholesterol even while the DDAB in the film is able to form either a monolayer or bilayer depending on the environmental conditions. Films treated with ethidium bromide prompt switching of dsDNA to ssDNA before bDDAB transitions to mDDAB. Swelling experiments have determined that there is a direct proportionality between the macroscopic increase in volume and the nanoscopic increase in lamellar spacing when a film is allowed to swell in water. Finally, experiments with phosphate-buffered saline (PBS) indicate that the films can disassemble in a simulated biological environment due to screening of their charges by buffer salt. We conclude that the structure of DNA in the film depends on the water content (as measured by the relative humidity) and temperature of the environment, while the state of DDAB depends essentially only on the water content. The structure of the film is quite flexible, and can be altered by changing environmental conditions as well as the chemical ingredients. These films will have useful, new applications as responsive materials, e.g. in drug and gene delivery.
doi:10.1021/ja909514j
PMCID: PMC2895560  PMID: 20438082
nucleic acid-surfactant films; biomaterials; responsive materials; DNA
25.  Biocompatibility Implications of Polypyrrole Synthesis Techniques 
Polypyrrole (PPy) is an inherently conducting polymer that has shown great promise for biomedical applications within the nervous system. However, to effectively use PPy as a biomaterial implant, it is important to understand and reproducibly control the electrical properties, physical topography, and surface chemistry of the polymer. Although there is much research published on the use of PPy in various applications, there is no systematic study linking the methodologies used for PPy synthesis to PPy’s basic polymeric properties (e.g., hydrophilicity, surface roughness), and to the biological effects these properties have on cells. Electrochemically synthesized PPy films differ greatly in their characteristics depending on synthesis parameters such as dopant, substrate, and thickness, among other parameters. In these studies, we have used three dopants (chloride (Cl), tosylate (ToS), polystyrene sulfonate (PSS)), two substrates (gold and indium tin oxide-coated glass), and a range of thicknesses, to measure and compare the biomedically-important characteristics of surface roughness, contact angle, conductivity, dopant stability, and cell adhesion (using PC-12 cells and Schwann cells). As predicted, we discovered large differences in roughness depending on the dopant used and the thickness of the film, while substrate choice had little effect. From contact angle measurements, PSS was found to yield the most hydrophilic material, most likely because of free charges from the long PSS chains exposed on the surface of the PPy. ToS-doped PPy films were tenfold more conductive than Cl- or PSS-doped films. X-ray photoelectron spectroscopy studies were used to evaluate dopant concentrations of PPy films stored in water and phosphate buffered saline over 14 days, and conductance studies over the same timeframe measured electrical stability. PSS proved to be the most stable dopant, though all films experienced significant decay in conductivity and dopant concentration. Cell adhesion studies demonstrated the dependence of cell outcome on film thickness and dopant choice. The strengths and weaknesses of different synthesis parameters, as demonstrated by these experiments, are critical design factors that must be leveraged when designing biomedical implants. The results of these studies should provide practical insight to researchers working with conducting polymers, and particularly PPy, on the relationships between synthesis parameters, polymeric properties, and biological compatibility.
doi:10.1088/1748-6041/3/3/034124
PMCID: PMC2562301  PMID: 18765899
polypyrrole; conducting polymers; electrochemical synthesis; characterization; biocompatibility; conductivity

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