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> REPLACE THIS LINE WITH YOUR PAPER IDENTIFICATION NUMBER (DOUBLE-CLICK HERE TO EDIT) < 1 Low-Frequency Noise in Field-Effect Devices Functionalized with Dendrimer/Carbon- Nanotube Multilayers Ferdinand V. Gasparyan, Arshak Poghossian, Svetlana A. Vitusevich, Mykhaylo V. Petrychuk, Viktor A. Sydoruk, Jose R. Siqueira Jr., Osvaldo N. Oliveira Jr., Andreas Offenhäusser, and Michael J. Schöning Abstract—Low-frequency noise in an electrolyte-insulator- semiconductor (EIS) structure functionalized with multilayers of polyamidoamine (PAMAM) dendrimer and single-walled carbon nanotubes (SWNT) is studied. The noise spectral density exhibits 1/fγ dependence with the power factor of γ ≈ 0.8 and γ = 0.8 - 1.8 for the bare and functionalized EIS sensor, respectively. The gate- voltage noise spectral density is practically independent of the pH value of the solution, and increases with increasing gate voltage or gate-leakage current. It has been revealed that functionalization of an EIS structure with a PAMAM/SWNTs multilayer leads to an essential reduction of the 1/f noise. To interpret the noise behavior in bare and functionalized EIS devices, a gate-current noise model for capacitive EIS structures based on an equivalent flatband-voltage fluctuation concept has been developed. Index Terms—Low-frequency noise, field-effect sensor, carbon nanotube, dendrimer. I. INTRODUCTION The functionalization of electrolyte-gate field-effect devices (FED), like ion-sensitive field-effect transistors (ISFET), capacitive electrolyte-insulator-semiconductor (EIS) structures and light-addressable potentiometric sensors, with nano- and biomaterials is one of the most attractive approaches for the development of (bio-)chemical sensors and biochips. Since FEDs are charge-sensitive devices, each (bio-)chemical reaction leading to chemical or electrical changes at the gate insulator/electrolyte interface can be detected by coupling the gate with respective chemical or biological recognition elements. These devices have been shown to be versatile tools for detecting pH, ion concentrations, enzymatic reactions [1]– [3], charged macromolecules (DNA (deoxyribonucleic acid), proteins, polyelectrolytes) (see e.g., [4]–[6]), cellular metabolisms and action potentials of living cells [7], [8]) as well as for designing biocomputing logic gates [9]. More recently, nanoparticles [10]–[12], silicon nanowires [13], [14] and carbon nanotubes [15] have attracted significant interest as a promising material for novel nanoscale bioelectronic devices, due to their excellent electronic and chemical properties, leading to an enhanced sensor performance. Manuscript received Februar 9, 2010. F. V. Gasparyan is with the Yerevan State University, 1 Alex Manoogian St., 0025 Yerevan, Armenia (e-mail:fgaspar@ysu.am). A. Poghossian and M. J. Schöning are with the Institute of Nano- and Biotechnologies, Aachen University of Applied Sciences, Ginsterweg 1, 52428 Jülich, Germany, and Jülich-Aachen Research Alliance for Future Information Technology (JARA-FIT), Forschungszentrum Jülich, 52425 Jülich, Germany (e-mail: a.poghossian@fz-juelich.de; m.j.schoening@fz- juelich.de). S. A. Vitusevich, V. A. Sydoruk, and A. Offenhäusser are with the Institute of Bio- and Nanosystems, Jülich-Aachen Research Alliance for Future Information Technology (JARA-FIT), Forschungszentrum Jülich, 52425 Jülich, Germany (e-mail: s.vitusevich@fz-juelich.de; v.sydoruk@fz- juelich.de; a.offenhaeusser@fz-juelich.de). M. V. Petrychuk is with the Taras Shevchenko National University, 01033 Kyiv, Ukraine (e-mail: pmichail@mail.ru). J. R. Siqueira Jr. and O. N. Oliveira Jr. are with the Physics Institute of São Carlos, University of São Paulo, 369, São Carlos, Brazil (e-mail: junior@ifsc.usp.br; chu@ifsc.usp.br). The study of noise spectroscopy can give additional insight into the detection mechanism and detection limit of biosensors. An investigation of a signal/noise ratio in FEDs is especially important in case of an application of FEDs for the measurement of low analyte concentrations, for the detection of biomolecules by their intrinsic molecular charge [4]–[6], as well as for the monitoring of action potentials of living cells, where the sensor output signal can be very small [7], [8]. On the other hand, noise measurements could be a very sensitive method for the analysis of the semiconductor/metal interface quality as well as for the quantitative determination of an analyte concentration as it has been shown for H2 gas sensors in [16], [17]. While the noise has been extensively studied in MOSFETs (metal-oxide-semiconductor field-effect transistor) and related devices [18], [19], so far, the noise investigation in electrolyte-gate FEDs has been limited to transistor structures. For instance, low-frequency (LF) noise of a drain current of Al2O3-gate pH-sensitive ISFETs was studied in [20], [21]. More recently, drain current noise in ISFETs modified with DNA molecules [22] and in electrolyte-gate carbon-nanotube transistors [23], [24] as well as Nyquist noise of cell adhesion in a neuron-transistor hybrid [25] has been investigated. In contrast, very little is known about the noise in field-effect capacitive structures [26]. In this work, LF noise in a capacitive field-effect EIS structure functionalized with polyamidoamine (PAMAM) dendrimer/SWNT (single-walled carbon nanotube) multilayers has been investigated and compared with noise in a bare EIS device. In contrast to transistor structures, mailto:a.poghossian@fz-juelich.de mailto:m.j.schoening@fz-juelich.de mailto:m.j.schoening@fz-juelich.de mailto:s.vitusevich@fz-juelich.de mailto:a.offenhaeusser@fz-juelich.de mailto:junior@ifsc.usp.br > REPLACE THIS LINE WITH YOUR PAPER IDENTIFICATION NUMBER (DOUBLE-CLICK HERE TO EDIT) < 2 capacitive EIS sensors are simple in layout and cost-effective in fabrication (usually, no photolithographic process steps or complicated encapsulation procedures are required). In addition, it has been reported that functionalization of FEDs with carbon nanotubes incorporated into layer-by-layer (LbL) prepared dendrimer films enhances their biosensor performance [27], [28]. As it will be demonstrated below, the functionalization of an EIS structure with a PAMAM/SWNT multilayer leads to an essential reduction of LF noise. II. FABRICATION AND FUNCTIONALIZATION OF EIS STRUCTURES Capacitive Al-p-Si-SiO2-Ta2O5 structures with a 30 nm thermally grown SiO2 and a 55 nm Ta2O5 layer were fabricated. The Ta2O5 layer has been prepared via electron- beam evaporation of 30 nm Ta followed by thermal oxidation at 515 °C for about 30 min [29]. As contact layer, a 300 nm Al film was deposited on the rear side of the Si wafer and then, the wafer was cut into single chips of 10 mm x 10 mm size. The EIS sensor was mounted into a home-made measuring cell and sealed by an O-ring to protect the side walls and backside contact of the chip from the electrolyte solution. The contact area of the EIS sensor with the solution was about 0.5 cm2. The LbL assembly technique has been recognized as a very attractive tool for fabricating functional hybrid materials and nanostructured films, because it offers fine control over film thickness and architecture at the nanoscale. The PAMAM/SWNT multilayers were obtained via consecutive dropping of the respective PAMAM (for 5 min) and SWNT (for 10 min) solutions onto the sensor surface, followed by rinsing and drying steps. These procedures were repeated until the required number of bilayers was achieved (in this study 3- bilayers). Fourth generation G4 PAMAM dendrimers and SWNTs functionalized with carboxylic groups were purchased from Aldrich Co. In aqueous solution, carboxylic groups of the SWNTs deprotonate to carboxylate anions (COO-), yielding negatively charged SWNTs. Since at the pH values of the solutions used the surface of aTa2O5 layer is negatively charged, we started the formation of the LbL multilayers with the positively charged PAMAM dendrimers. Fig. 1 shows the schematic of the EIS structure functionalized with a multilayer of PAMAM/SWNT (a) and the chemical structure of the materials employed (b). For the details of LbL formation of PAMAM/SWNT multilayers, see e.g., [27], [28]. The morphology of the prepared PAMAM/SWNT films has been studied with an atomic force microscope (AFM) BioMat Workstation (JPK Instruments, Germany). Fig. 2 illustrates a tapping mode liquid-cell AFM image of the functionalized sensor surface. The scan size was 5 µm x 5 µm. The prepared LbL film represents an interconnected network structure with randomly oriented SWNTs. The presence of deprotonated carboxylic groups on the nanotubes facilitates their electrostatic interaction with the positively charged PAMAM molecules. The film has a high porosity due to the interpenetration of the SWNT network into the dendrimer layers. III. RESULTS AND DISCUSSION A. C-V characteristics and pH sensitivity of bare and functionalized EIS sensors The adsorption of each PAMAM or SWNT layer was monitored by means of capacitance-voltage (C–V) method at a frequency of 120 Hz using an impedance analyser (Zahner Elektrik, Germany). The measurements have been performed in a pH 7 buffer solution in a Faraday cage at room temperature. For experiments, a DC (direct current) polarization voltage is applied via the reference electrode (conventional liquid-junction Ag/AgCl electrode, Metrohm) and a small AC (alternating current) voltage (20 mV) is applied to the system in order to measure the capacitance of the sensor (see Fig. 1a). All potential values are referred to the Ag/AgCl reference electrode. The total capacitance of the EIS structure functionalized with PAMAM/SWNT layers, C, can be described as a series connection of the space-charge capacitance of the semiconductor, Csc, the capacitance of the gate insulator, Ci,, and the effective capacitance of the PAMAM/SWNT multilayer, CML: MLisc CCCC 1111 ++= . (1) Csc, and therefore C, is among others a function of the gate voltage (Vg) applied to EIS structures and the potential at the gate insulator/electrolyte interface after the PAMAM/SWNT adsorption. Fig. 3a shows typical C-V curves for the EIS structure before and after each step of functionalization. Similar to the bare EIS structure, dependent on the magnitude and polarity of the applied gate voltage, three regions in the C- V curves can be distinguished: accumulation (Vg<-1 V), depletion (-0.6 V<Vg<0 V) and inversion (Vg>0.2 V). As it can be seen, after the adsorption of three bilayers of PAMAM/SWNT, the maximum capacitance in the accumulation range of the C-V curves remains nearly unchanged. Taking into account that the maximum capacitance in the accumulation range of the C-V curve is approximately equal to the gate capacitance, i.e., Cmax=Ci and Cmax(PAMAM/SWNT)=CiCML/(Ci+CML) for the bare and PAMAM/SWNT-covered EIS structure, respectively, it can be concluded that the CML is much higher than Ci. On the other hand, relatively large shifts (20 mV after the adsorption of the first PAMAM1 layer, and about 10 mV after the adsorption of further SWNT or PAMAM layers) have been registered along the voltage axis in the depletion range of the C-V curves. These shifts can clearly be recognized from the zoomed graph in the depletion region at ~60% of the maximum capacitance (see Fig. 3b). This indicates that the adsorption of a PAMAM or SWNT layer induces an interfacial potential change at the electrolyte side and/or gate- insulator side of the layer that is in series to the applied gate > REPLACE THIS LINE WITH YOUR PAPER IDENTIFICATION NUMBER (DOUBLE-CLICK HERE TO EDIT) < 3 voltage Vg. The direction of the shift along the voltage axis depends on the sign of the charge of the adsorbed dendrimer molecules or SWNTs. In case of the adsorption of the positively charged PAMAM, the potential shifts in the same direction as for the case of an additional positive charging of the Ta2O5 surface. Consequently, the direction of the potential change after adsorption of negatively charged SWNTs corresponds to the case as if the Ta2O5 surface would have been additionally negatively charged. Similar effects were reported for a polyelectrolyte multilayer formation onto a p- Si-SO2 [30], [31] and a p-Si-SO2-diamond [32] capacitive EIS sensor. Before the noise experiments, the gate-leakage current and the pH sensitivity of bare and functionalized p-Si-SiO2-Ta2O5 sensors have been examined. The gate-leakage current in the accumulation range was higher (~2-6 nA) than in the depletion and inversion range (~0.2-0.4 nA). In addition, in the accumulation region the gate-leakage current for a bare EIS structure was 2-3 times higher than in case of a functionalized EIS sensor. This could be attributed to the blocking of some of the current paths across the gate area covered with the PAMAM/SWNT multilayer. The EIS sensors with a bare Ta2O5 gate insulator show a pH sensitivity of about 56-57 mV/pH in the range from pH 3 to pH 11, which is in good agreement with values typically reported for a Ta2O5 layer [33], [34]. The presence of the PAMAM/SWNT film did not affect significantly the pH sensitivity of the EIS structure (54.5 mV/pH). This behavior could be attributed to the high porosity of the PAMAM/SWNT film allowing the penetration of H+- or OH--ions to the Ta2O5 surface. B. Low-frequency noise in bare and functionalized EIS structures Noise spectra of bare and functionalized EIS sensors were recorded in a frequency range from 0.06 to 100 Hz using the experimental setup shown in Fig. 4. A voltage from battery E was applied to the EIS structure via a load resistance (R=10 MΩ) and an Ag/AgCl liquid-junction reference electrode. The noise signal from the EIS sensor was amplified using a home- made ultra-low-noise preamplifier and a low-noise amplifier (LNA) ITHACO 1201. The LNA output was connected to an HP 35670A dynamic signal analyzer, which records the noise signal and transforms it into a frequency spectrum using the FFT (Fast Fourier Transform). The measuring cell with the EIS sensor, reference electrode and LNA were placed in a shielding box for protection from external electromagnetic influences. Before the noise experiments in EIS structures, the internal noise level in the measuring system (without EIS sensor) was checked. The noise level from the circuits, preamplifier and amplifier were several orders of magnitude lower than noise in EIS structures under test. The LF noise spectra were measured in buffer solutions of pH 3, pH 7, and pH 11 in accumulation, depletion and inversion regions of the C-V curve by applying different gate voltages. We have observed that the pH value of the buffer solution did not significantly influence the noise spectral density. This is in agreement with results obtained on pH ISFETs [20], [21]. It has been reported that the gate-referred 1/f noise of the channel current of pH ISFETs is also independent of the pH, and the origin of LF noise in these ISFETs is the trapping/detrapping of carriers at the Si-SiO2 interface [20], [21]. Moreover, it has been discussed that the ionic strength of the solution does not affect the noise magnitude of liquid-gated SWNT transistors [23]. These results suggest that the interface between the solution and the gate insulator does not or not significantly contribute to the 1/f noise. Fig. 5 depicts the gate-voltage noise-power spectral density (NSD), SV, as a function of frequency for the bare (a) and functionalized EIS structure (b), recorded in a pH 7 buffer solution at applied gate voltages of -1.5, -1.2, -0.4, 0, and 0.5 V, respectively. As can be seen, the measured NSD exhibits an 1/fγ dependence, whereas the amplitude of the NSDdepends on both the applied gate voltage and the frequency range. At frequencies of f<1 Hz, the power factor estimated from Fig. 5 was approximately γ ≈ 0.8 and γ = 0.8 - 1.8 for the bare and functionalized EIS sensors, respectively. The noise in the bare EIS structure shows a strong dependence on the applied gate voltage (see Fig. 5a). Moreover, the LF noise is much higher in the accumulation region of the C-V curve at applied voltages of -1.5 and -1.2 V. Similar effects have been observed for Al-SiO2-n-Si MOS capacitors showing RTS (random telegraphic signals) noise [35]. However, in our structures no RTS noise behavior was registered. In contrast to the bare EIS structure, the gate voltage related effects in the LF noise of the functionalized EIS sensor are suppressed (Fig. 5b) which could be attributed to the presence of the PAMAM/SWNT multilayer. Surprisingly, at frequencies of f <10 Hz and negative applied voltages, the noise-reduction effect has been revealed in the functionalized EIS structure. This effect depends on both the applied gate voltage and the frequency, and is stronger in the accumulation regime. As an example, Fig. 6 shows the noise spectral density for the bare and functionalized EIS structures as a function of the applied gate voltage evaluated from Figs. 5a and 5b at a frequency of 1 Hz. As can be seen from Fig. 6, the presence of the additional PAMAM/SWNT multilayer leads to the essential reduction (by the factor of up to 100 in the accumulation range) of the 1/f noise in comparison to the bare EIS structure. C. Noise model for EIS structures Several different theories have been proposed to explain the physical origin of noise in FEDs. These include the carrier number fluctuation theory originally developed by McWorther, the mobility fluctuation or Hooge model as well as various unified models (see e.g., [18], [19], [36], [37] and references there). In addition, recently, a charge fluctuation model has been proposed to explain the noise behavior of MOS capacitors [26] and carbon nanotubes [23]. Usually, low-frequency noise in FEDs is measured in the channel current of transistor structures. Typically, 1/f noise in MOSFETs has a spectrum with a slope that varies between 0.7 > REPLACE THIS LINE WITH YOUR PAPER IDENTIFICATION NUMBER (DOUBLE-CLICK HERE TO EDIT) < 4 and 1.3 [37]. It has been generally accepted that at low frequencies, 1/f noise is the dominant source of noise in MOSFETs and trap-related processes (due to the trapping/detrapping of carriers in traps located in the gate oxide, near or at the Si/SiO2 interface) are the major cause of 1/f fluctuations. The origin of low-frequency noise in the channel current of ISFETs has been also explained by the trapping/detrapping of carriers at the Si-SiO2 interface in according to the carrier-number fluctuation model [20]–[22]. In addition, it has been reported that the gate-referred 1/f noise (caused by the capacitive coupling between the channel and gate) in ISFETs is independent of the gate bias [20]. A simple adoption of the carrier-number fluctuation model to capacitive EIS structures, however, does not allow to completely explain the experimentally observed effects such as the dependence of the equivalent gate voltage (or gate current) NSD on a gate-voltage or the noise-reduction effect in functionalized EIS structures. The noise investigations in AlGaN/GaN heterostructure field-effect transistors [38] and in MOS devices with ultrathin gate oxides [39]–[42] show that one of the possible reasons for the dependence of low- frequency noise on the gate bias is the contribution of the gate-leakage current noise to the output noise. In leaky dielectrics, besides the channel current noise, gate-leakage current in the gate oxide of MOS devices should be considered as an important low-frequency noise source. To interpret the results of noise experiments for bare and functionalized EIS structures, we describe a gate-current noise model for capacitive EIS structures based on an equivalent flatband-voltage fluctuation concept that is also used in the carrier-number fluctuation noise model for the drain-current noise in transistor structures [42]. In general, the flatband voltage (a voltage by which the energy bands in the semiconductor continue horizontally up to the surface and the net-charge density in the semiconductor is zero) of an EIS system is given by [4], [43], [44]: i iS solreffb C Q q WEV −−+−= χϕ , (2) where Eref is the potential of the reference electrode, ϕ is the electrolyte/gate insulator interfacial potential (which can be a function of the pH, ion or analyte concentration as well as charge of adsorbed molecules), χsol is the surface-dipole potential of the solution, WS is the work function of the electrons in the semiconductor, q is the elementary charge, and Qi is the total insulator charge per unit area including the charges located within the gate oxide as well as trapped in surface and interface states. Similarly, the flatband voltage of the EIS device covered with the dendrimer/SWNT multilayer can be defined as: ML ML i iS solMLreffbML C Q C Q q WEV −−−+−= χϕ , (3) where ϕML is the electrolyte/gate insulator interfacial potential after the multilayer adsorption, the term QML/CML represents the potential drop across the multilayer, and QML is the total charge in the dendrimer/SWNT multilayer per unit area, which is pH-dependent because of protonation/deprotonation of both amino- and carboxylic groups of dendrimers and SWNTs, respectively. The theoretical modeling of the noise in functionalized FEDs is very complicated due to the presence of an organic/inorganic hybrid structure. For uncorrelated noise sources, the total NSD of a system can be considered as the sum of the individual power densities and should include noise caused from the reference electrode, electrolyte, multilayer of PAMAM/SWNT, oxide/electrolyte and multilayer/electrolyte interfaces, and the solid-state device itself. As it has been reported previously, the gate-related 1/f noise in ISFETs [20], [21] and electrolyte-gated carbon nanotube transistors [23] is independent on the pH. Our experiments in different pH buffer solutions also show that the pH value does not affect significantly the NSD of both bare and functionalized EIS structures. Therefore, it can be suggested that the interface between the solution and the gate insulator as well as charge fluctuations in the PAMAM/SWNT multilayer due to the protonation/deprotonation processes do not distinctly contribute to the 1/f noise. Thus, if the fluctuations in ϕ , ϕML, and QML can be ignored, and if the reference electrode and electrolyte solution generate no noise, then the flatband- voltage fluctuations will be associated with the fluctuations of the number of trapped charges in the gate insulator: i i fbfbML C QVV δδδ =~ . (4) The spectral density of the gate-current fluctuations (SIg) is related to the spectral density of the flatband-voltage fluctuations (Sfb) by [42]: )( )( )( 22 22 fSg C fS gSgfS V i Qi fbIg ≡== , (5) where g=δIg/δVg is the gate conductance, Ig is the gate current, SV is the spectral density of the voltage fluctuations, and SQi (f) is the spectral density of the trapped charge fluctuations. The detailed expression for the gate-current (or gate voltage) noise spectral density will be defined by the mechanism of current transport in a capacitive EIS structure (in this work, an electrolyte-Ta2O5-SiO2-Si-Al structure). For a metal-Ta2O5- SiO2-Si-Al structure, the hopping conduction and tunneling were elucidated to be the dominant conduction mechanisms in the SiO2 layer and Poole-Frenkel field-assisted emission in the Ta2O5 layer [45]. It has been observed that the gate current noise in MOS capacitors[39] and MOSFETs [40]–[42] with thin gate oxides is increased with increasing gate voltage or leakage current, similar to the noise behavior of the capacitive EIS structures investigated in this work. This has been attributed to the more slow-trap states available for a trap- assisted tunneling with increasing gate voltage [39]–[42]. Noise investigations in Ta-Ta2O5-MnO2 capacitors also show a clear dependence of the noise spectral density on the leakage current [46]. From the standpoint of gate-leakage current > REPLACE THIS LINE WITH YOUR PAPER IDENTIFICATION NUMBER (DOUBLE-CLICK HERE TO EDIT) < 5 mechanisms and similarities of gate-current noise behavior in MOSFETs and EIS structures, it seems that as in MOSFETs, the trap-related processes are the most likely cause of low- frequency gate-current noise in capacitive EIS devices, because traps or slow states in oxides can result in a low- frequency fluctuation-dissipation in the conductance of gate oxides [39]. Thus, the gate noise will be proportional to the total amount of traps that can be charged/discharged in the dielectric. The gate voltage-dependent changes in the occupancy of the oxide trap levels will result in a modulation of the conductivity of current paths or charge carriers passing through the device, which could explain the experimentally observed gate-voltage dependence of the noise in capacitive EIS structures. In addition, since the EIS devices work in a liquid environment, the possible micro- and nanopores or pinholes in the gate insulator will be filled with electrolyte solution, thus, decreasing the effective thickness of the gate insulator in pore regions and generating new current paths. As a result, the gate current and therefore, the gate-current noise in EIS structures is expected to be higher than in MOS structures with the same gate insulator. The above proposed noise model might allow also to explain the experimentally observed noise-reduction effect in an EIS structure functionalized with a PAMAM/SWNT multilayer. Although the PAMAM/SWNT multilayer can be considered as a porous structure allowing the penetration of solution to the Ta2O5 surface, nevertheless, it will screen or block some of the current paths across the gate area, thus, decreasing the leakage current and the gate-current noise as well as suppressing the gate-voltage dependence of the NSD, that in fact, has been observed in experiments with a functionalized EIS structure. Another possible reason for the observed noise- reduction effect could be electrochemical processes at the Ta2O5/PAMAM and electrolyte/PAMAM/SWNT interface as well as the charge redistribution in the PAMAM/SWNT multilayer itself. As it has been demonstrated in [27], [28], the PAMAM/SWNT multilayer could act as a “stabilizer” providing a smaller drift and a more stable sensor signal. IV. CONCLUSION LF noise in a capacitive field-effect Al-p-Si-SiO2-Ta2O5 EIS structure functionalized with a PAMAM/SWNT multilayer has been investigated and compared with the noise in a bare EIS device. The noise spectral density exhibits an 1/fγ dependence with the power factor of γ ≈ 0.8 and γ = 0.8 - 1.8 for the bare and functionalized EIS sensors, respectively. The gate-voltage noise spectral density was practically independent on the pH value of the solution and is increased with increasing gate voltage or gate-leakage current. It has been revealed that the existence of the PAMAM/SWNTs multilayer leads to considerable reduction of the 1/f noise. The gate-current noise behavior in bare and functionalized EIS devices has been modeled using the flatband-voltage fluctuations concept. The experimentally observed gate- voltage dependence of the noise in capacitive EIS structures can be explained by the gate-voltage-dependent changes in the occupancy of the oxide trap levels resulting in a modulation of the conductivity of current paths or charge carriers passing through the EIS structure. The detailed mechanism of current transport in field-effect capacitive electrolyte- (SWNT/PAMAM)-Ta2O5-SiO2-Si-Al and electrolyte-Ta2O5- SiO2-Si-Al structures as well as the microscopic origin of the noise-reduction effect requires further investigations. ACKNOWLEDGMENT The authors thank M. Bäcker for the AFM image. Financial support from CAPES (Brazil) is gratefully acknowledged. F.V. Gasparyan is grateful to German Academic Exchange Service (DAAD) for financial support. REFERENCES [1] C.-S. Lee, S. K. Kim, and M. Kim, “Ion-sensitive field-effect transistors for biological sensing”, Sensors, vol. 9, pp. 7111-7131, 2009. [2] M. J. Schöning and A. 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Poghossian, “Determination of the pHpzc of insulators surface from capacitance-voltage characteristics of MIS and EIS structures”, Sens. Actuators B, vol. 44, pp. 551-553, 1997. [45] N. Novkovski and E. Atanassova, “A comprehensive model for the I-V characteristics of metal-Ta2O5/SiO2-Si structures”, Appl. Phys. A, vol. 83, pp. 435-445, 2006. [46] J. Sikula, J. Hlavka, J. Pavelka, V. Sedlakova, L. Grmela, M. Tacano, and S. Hashiguchi, “Low frequency noise of tantalum capacitors”, Active and Passive Elec. Comp., vol. 25, pp. 161-167, 2002. Ferdinand V. Gasparyan was born in Yerevan, Armenia, in 1950. He received the MSc degree as physics-engineer from Yerevan Polytechnic Institute, Yerevan, Armenia, in 1972, the PhD degree in 1981, and the Dr. Sci. degree in 1995. He is full professor with the Department of Physics of Semiconductors and Microelectronics, Yerevan State University. He has authored and co-authored more than 120 scientific papers and 6 books. His current research interests include physical properties and internal noises of semiconductors and p-i-n structures, IR and UV photodiodes, and photoelectrical conversion of solar energy. Arshak Poghossian received his PhD degree in solid-state physics from Leningrad Electrotechnic Institute (Russia) in 1978 and the Dr. Sci. (Engineering) degree in solid-state electronics and microelectronics from the State Universtity of Yerevan (Armenia) in 1995. After being an associate professor at State Engineering University of Armenia and director of Microsensor Ltd. (Yerevan) from 1991 to 1996, he has been a professor at the University of Management and Information (Yerevan). Since 1998, he has been with the Institute of Thin Films and Interfaces (now, Institute of Bio- and Nanosystems) at the Research Centre Jülich, and since 2004, he joined the Institute of Nano- and Biotechnologies at Aachen University of Applied Sciences, Germany. In 2008, he has been appointed as Honorary Professor. His research interests are solid-state chemical sensors and biosensors, sensor materials, nano-devices, microsystem technology, nano- and biotechnology. Svetlana A. Vitusevich received the MSc in radiophysics and electronics, Kiev State University, Ukraine, in 1981 and the PhD degree in physics and mathematics from Institute of Semiconductor Physics (ISP), Kyiv, Ukraine, in 1991. From 1981 to 1997, she was with the ISP, Kyiv, Ukraine, as researcher (1981), scientific researcher (1992), and senior scientific researcher (1994). From 1997 to 1999, she was Alexander von Humboldt Research Fellow at theInstitute of Bio- and Nanosystems (former Institute of Thin Films and Interfaces) at Forschungszentrum Jülich (FZJ), Germany. Since 1999, she is senior scientific researcher at FZJ. She received Dr. habil. degree in 2006. Her research interests include transport and noise properties of different materials for advanced electronic devices and circuits. > REPLACE THIS LINE WITH YOUR PAPER IDENTIFICATION NUMBER (DOUBLE-CLICK HERE TO EDIT) < 7 Her achievements include more than 110 papers in scientific journals and 7 patents, among them two for semiconductor functional transformer. Mykhaylo V. Petrychuk received the PhD degree (1993) in semiconductor physics from the Institute of Semiconductor Physics NAS, Ukraine. He is a senior research scientist of the Radio-Engineering Department at the National Taras Shevchenko University of Kyiv, Ukraine. His primary area of expertise is the physics of low-frequency noise in semiconductors and devices. His research interests include studing of fundamental origin of 1/f noise. He has been involved in the investigation of noise in low-dimensional quantum structures since 2002. He has made a significant contribution to the discovery and understanding of non-equilibrium low-frequency noise in GaN- based structures with two-dimensional conducting channels. He has published over 80 journal/conference papers. Viktor A. Sydoruk received the B.S. degree and the MSc degree in radiophysics and electronics from the National Taras Shevchenko University of Kyiv, Ukraine, in 2006 and 2008, respectively. He is currently working towards the PhD degree as a Graduate Research Assistant under the direction of Dr. habil. Svetlana Vitusevich at the Research Centre Jülich, Germany. His research focuses on the design and characterization of nanostructures, understanding the electrical transport in the structures using noise spectroscopy and supporting instrumentation for study of biosensors. José R. Siqueira Jr. received his B.S. degree in Physics at the Universidade Federal de São Carlos in 2004. His MSc and PhD degrees were received in Materials Science and Engineering from the Instituto de Física de São Carlos at the Universidade de São Paulo, Brazil, in 2006 and 2010, respectively. His research focuses on the processing and characterization of nanostructured films using nanomaterials such as carbon nanotubes, nanoparticles and dendrimers to develop specific units for biosensing within a platform exploiting electrochemical measurements in field-effect devices. Prof. Osvaldo N. Oliveira Jr. is a physics professor at the Instituto de Física de São Carlos, Universidade de São Paulo, Brazil. He received his PhD from the University of Wales, Bangor (UK), in 1990. His research interests include nanostructured films, especially for applications in sensing and biosensing, and natural language processing. He has supervised over 30 PhD and MSc. students, authored ca. 330 papers in refereed journals and filed 7 patents. He is currently associate editor for the Journal of Nanoscience and Nanotechnology. In 2006 he received the Elsevier Scopus Award as one of the most productive Brazilian scientists in terms of number of publications and citations. Andreas Offenhäusser graduated in physics (Diplom) from the University of Ulm in 1985 and completed his PhD at the University of Ulm in 1989. From 1990 to 1992 he worked as an engineer at Robert Bosch GmbH, Reutlingen. From 1992 to 1994 he joined the Frontier Research Program, RIKEN, Japan. From 1994 to 2001, he worked at the Max Planck Institute for Polymer Research, Mainz, as a group leader. In 2000, he received his “habilitation“. He moved to the Forschungszentrum Jülich in 2001 where he is presently director at the Institute of Bio- and Nanosystems (IBN- 2). He is professor for experimental physics at the Rheinisch-Westfälische Technische Hochschule (RWTH) Aachen, Germany. The focus of his work is the functional coupling of sensory cells and neurons with microelectronic devices, signal processing in biological neuronal networks, electronic DNA- Chips, and biophysics of lipid bilayers and membrane receptors. Michael J. Schöning received his diploma degree in electrical engineering (1989) and his PhD in the field of semiconductor- based microsensors for the detection of ions in liquids (1993), both from the Karlsruhe University of Technology. In 1989, he jointed the Institute of Radiochemistry at the Research Centre Karlsruhe. Since 1993, he has been with the Institute of Thin Films and Interfaces (now, Institute of Bio- and Nanosystems) at the Research Centre Jülich, and since 1999 he was appointed as full professor at Aachen University of Applied Sciences, Campus Jülich. Since 2006, he serves as a director of the Institute of Nano- and Biotechnologies (INB) at the Aachen University of Applied Sciences. His main research subjects concern silicon-based chemical and biological sensors, thin-film technologies, solid- state physics, microsystem and nano(bio-)technology. SWNT PAMAM a) b) RE Impedance analyzer V=bias Electrolyte V~ Fig. 1. Schematic of the EIS structure functionalized with a multilayer of PAMAM/SWNT (a) and chemical structure of the materials employed (b); RE: reference electrode. Fig. 2. Tapping mode liquid-cell AFM image of the EIS sensor surface functionalized with a PAMAM/SWNT multilayer. > REPLACE THIS LINE WITH YOUR PAPER IDENTIFICATION NUMBER (DOUBLE-CLICK HERE TO EDIT) < 8 Fig. 3. C-V curves for a bare pSi-SiO2-Ta2O5 EIS structure and EIS sensor functionalized with a PAMAM/SWNT multilayer measured in a buffer solution of pH 7 (a), and zoomed C-V curves for the different layers in the depletion range (b). Fig. 5. Voltage noise spectral density (SV) vs. frequency for a bare (a) and functionalized (b) EIS structure measured at various Vg: (1) -1.5 V, (2) -1.2 V, (3) -0.4 V, (4) 0 V, and (5) 0.5 V. Fig. 4. Experimental setup for noise measurements. E: battery; R: load resistance; DUT: device under test; LNA: low-noise current amplifier; FFT- analyzer: Fast Fourier Transform analyzer. Fig. 6. Noise spectral density for bare and functionalized EIS structures as a function of the applied gate voltage evaluated from Figs. 5a and 5b at a frequency of 1 Hz. I. INTRODUCTION II. FABRICATION AND FUNCTIONALIZATION OF EIS STRUCTURES III. RESULTS AND DISCUSSION IV. Conclusion
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