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A Study Regarding Dielectric Response and ac Electrical Conductivity of Schottky Structures (SSs) Interlaid with (Fe3O4-PVA) by Using Dielectric Spectroscopy Method

A Study Regarding Dielectric Response and ac Electrical Conductivity of Schottky Structures (SSs)... This study aims to reveal the complex-dielectric permittivity, complex electric modulus, complex impedance, and ac elec- trical conductivity of the SS interlaid with Fe O -PVA. For this intent, impedance measurements were actualized in the 3 4 frequency range of 0.1–1000 kHz and the voltage range of (– 5) – 7 V. The computed dielectric parameters via impedance measurements were presented as functions of both frequency and voltage to uncover their impacts on dielectric response, polarization, and conductivity. The dielectric parameters presented as a function of voltage showcase discernible zenith demeanor amid (– 1) and 0 V, and this behavior becomes more noticeable for low frequencies. These corollaries indicate that the source of zeniths is the surface states and their distribution in the forbidden band gap of the semiconductor. On the ′ ′′ other hand, ϵ , ϵ , tanδ values presented as a function of frequency exhibit a decrement trend with frequency increment, and frequency independency at higher frequencies. This frequency-related behavior of the dielectric parameters signifies the dominance of the Maxwell-Wagner and space charge polarization in the material. Further, the Nyquist diagrams of the SS confer one single semicircular arc corresponding to a Debye-type single relaxation process. Additionally, the conduc- tion mechanism of the structure was scrutinized via the slope of the lnσ -lnω plot. The slope values smaller than the ac unit signify that the hopping of mobile charges dominates the conduction. All these experimental ramifications denote the preponderant effects of frequency and voltage on the dielectric response of the structure. Keywords Fe O -PVA organic interface · Impedance spectroscopy · Complex dielectric and electric modulus · Ac 3 4 electrical conductivity 1 Introduction In recent years, it has been a priority to optimize the perfor- mances of Schottky structures since they immensely come into play in assorted implementations thanks to their apt- ness to integrated circuits. The wide implementation area Esra Erbilen Tanrıkulu of these structures has been spread from radiation detectors [email protected] [1], temperature sensors [2–4], and optoelectronic devices 1 [5, 6], to solar cells [7]. The most common approach to Graduate School of Natural and Applied Sciences, achieve Schottky structures with better performance and a Department of Advanced Technologies, Gazi University, Ankara, Turkey low cost is to try various materials as an interfacial layer [6, 8–14]. One of the most plausible materials to use as an inter- Department of Physics, Faculty of Science, Gazi University, Ankara, Turkey layer is organic polymer materials [2, 15–19]. Polyvinyl alcohol (PVA), in particular, provides advantages due to its Department of Chemistry and Chemical Processing Technologies, Vocational Highschool of Technical Sciences, salient features, primarily its easy production and low-cost Gazi University, Ankara, Turkey requirement [20–23]. Additionally, its adjustable features The General Directorate of State Hydraulic Works, Ankara, with some dopants make them congruous for multitudinous Turkey 1 3 Journal of Inorganic and Organometallic Polymers and Materials application areas. Since doping PVA, especially with metal dielectric properties. In another study performed on the or metal oxide increases its conductivity, it also increases dielectric characterization of MIS structure with PVAc-Si the possibility of usage of it in the electrical industry [22, insulator layer, it is concluded that the usage of PVAc-Si as 23]. Moreover, the doping process of PVA advances also an interfacial layer is proper, and the resultant MIS structure mechanical, thermal, and dielectric features [24–28]. Like- can be used in the floating gate memory devices [ 21]. Addi- wise, iron oxide (Fe O ) nanostructures are prominent in tionally, it is also noted in the literature that Schottky diodes 3 4 the literature by their unique magnetic properties, high ther- with PVC and doped-PVC interfacial layers have increased mal resistance, nontoxicity, and requirement for effortless dielectric constant, and in turn more energy capability com- production process [29–35]. Moreover, the usage of both pared to the traditional MS structure [39]. Considering the these materials together (PVA and Fe O ), investigations of literature outcomes epitomized above and considering the 3 4 their mechanical, thermal, and dielectric characteristics, and supreme dielectric peculiarities of the Fe O -PVA struc- 3 4 implementations spread from magnetic resonance imaging ture, it is believed that the usage of the Fe O -PVA structure 3 4 (MRI) to nanocatalyst and so far are supplanted in the lit- instead of traditional interlayers would change and enhance erature [24, 29, 36]. Considering the literature epitomized the dielectric characteristics of SSs. above, interposing of Fe O -PVA structure between metal The current study is the continuation of our previous 3 4 and semiconductor is foreseen congruous as an interfacial studies including temperature-reliant [40] and frequency- layer and may boost the performance of SSs. Especially, the reliant [41] electrical characteristics of SSs interlaid with underscored dielectric peculiarities of the Fe O -PVA struc- Fe O -PVA. The ref [40] verifies the formation of Fe O 3 4 3 4 3 4 ture motivate scrutinizing the dielectric characteristics of nanostructure, and dominant current transport mechanism the SS interlaid with it. (CTM) as thermionic-emission (TE) theory with Double- When another material such as dielectric or polymer Gaussian-distribution (DGD) of the BHs. In the other study materials is interposed between metal and semiconductor, [41], the evaluation of the main electrical characteristics is the metal-semiconductor (MS) structure is converted to the performed and the dependence on the frequency and volt- metal-oxide/insulator/polymer-semiconductor (MIS, MOS, age of them are revealed. Moreover, the region in which the or MPS) and may gain condenser characteristics. The pres- dominant effects of the surface states are observed is deter - ence of this layer intercepts the coaction between metal and mined as the depletion region. When it comes to this study, semiconductor, bringing in charge and energy storage capa- the scope is to investigate the dielectric properties, electric bility to the structure. Therefore, scrutinizing the dielectric modulus, and ac electrical conductivity, and designate the characteristics of these structures gains more importance. relaxation process, dominant conductance mechanism, and To comprehend the dielectric characteristics, they can be their frequency and voltage dependence. These experimen- parametrized in terms of complex dielectric permittivity tal corollaries reveal that the dielectric features of the fab- ∗ ′ ′′ ( ϵ ) including real ( ϵ ) and imaginer ( ϵ ) components, ricated SSs interlaid with Fe O -PVA strongly depend on 3 4 and loss factor (tand). Therewithal, calculation of complex voltage and frequency. Additionally, the frequency reliant ∗ ′ ′′ electric modulus (M ) and ac electrical conductivity ( σ variations of ϵ and ϵ validate that the structure has ac ) would be beneficial to be informed about the relaxation Maxwell-Wagner polarization, along with the Nyquist dia- process and transmission mechanism. Additionally, occur- gram shows that the structure has the Debye type single ring polarization in the material with the external electric relaxation. field manages all these dielectric parameters, and polariza - tion mechanisms called electronic, ionic, orientation and surface-charge polarizations show high dependency on 2 Experimental Procedure the frequency of the electric field [ 37, 38]. Therefore, fre- quency-reliant impedance analyses (covering capacitance The production of the Au/Fe O -PVA/n-Si SSs were based 3 4 (C), and conductance(G/ω) analyses) are prevalently used on an n-type Si wafer whose rudimental traits are its 350 to parametrize these dielectric features and delve into fre- µm thickness, 2” diameter, 1–10 Ω.cm resistivity, and quency and voltage reliant variations of them [37, 38]. < 100 > float-zone. After the first step as a chemical clean - The dielectric characterization of the SS with various ing process of the wafer, the coating of 99.999% pure Au interfacial layers is prevalent in the literature [16, 21]. For in the vacuum chamber was applied to achieve ∼150 nm instance, Yürekli et al. [16] reported a study comparing the thickness ohmic contact onto the rear side of the wafer. Fol- dielectric characteristics of SSs with three different inter - lowing that, the spin-coating method was utilized to grow facial layers. They demonstrated that the interfacial layer PVA: Fe O solution onto the fore side of the wafer. After- 3 4 has a changer effect on the dielectric trails and they noted ward, the production of the mentioned SSs was completed 3% graphene doped PVA interfacial layer shows better by evaporating high purity Au to become rectifier contacts 1 3 Journal of Inorganic and Organometallic Polymers and Materials –3 2 with a thickness of 150 nm and an area of 7.85 × 10 cm . following equations using impedance measurement results Figure 1 depicts the schematic representation of the pro- [38, 43–45]; duced Au/Fe O -PVA/n-Si SS. Refs [40] and [41] involve 3 4 more detailed articulation of the production process and ϵ = (1a) some structural analysis pertaining to Fe O -PVA nano- 3 4 structure. The XRD spectra presented in [40] reveal the spi- ′′ nel cubic crystal structure of the Fe O nanostructure with 3 4 ϵ = (1b) ω C an almost 13 nm crystallite size. Additionally, the reported SEM images in [40] give the uniform distribution of the ′′ ϵ G spherical-shaped Fe O nanostructure with a size less than 3 4 tanδ = = (1c) ϵ ω C 20 nm, while UV-Vis absorption spectra reveal the direct and indirect transitions with band gaps of 2.2 eV and 1.4 eV respectively. Prior to impedance measurements, the samples In these equations, C, G, and ω(= 2πf) are the measured were prepared by pasting it to a thin Cu holder utilizing a capacitance, conductance, and angular frequency, respec- silver paste to perform impedance measurements with an tively, while C is the geometric capacitance. The computed HP 4192 A LF impedance analyzer for various frequencies. ϵ values were demonstrated in Fig. 2a–c depending on frequency and voltage. Figure 2a presents the ϵ vs. V plot from – 5 to 7 V in a wide frequency range (0.1 kHz–1 MHz). 3 Results and Discussion Figure 2a also includes the peak between – 1.5 and 0 V cor- responding to the depletion region, especially for low fre- 3.1 Dielectric Permittivity quencies. Peak occurrence at the depletion region at which surface states exhibit the effects dominantly along with peak When a dielectric material undergoes an external electric nonoccurrence for high frequencies signify that surface field, the field entails keeping positive and negative charges states are responsible for this behavior. When a material is apart and inducing an electric dipole moment. Tackling the exposed to an ac external electric field with low frequencies, dielectric response of the material is crucial concerning the the charges at the surface states have adequate time to align materials’ applicability in electronic applications. These themselves with the same direction of the external field, so characterizations can be identified in terms of the complex their contributions can be detected. For high frequencies of dielectric permittivity ( ϵ ), and loss tangent (tand) parame- the external field, these charges cannot have adequate time, ′ ′′ ters. The real ( ϵ ) and imaginer ( ϵ ) portions of dielectric so their contributions become insufficient compared to the permittivity, and loss tangent (tanδ) denote energy absorp- low frequencies. To put it another way, the detectable contri- tion, energy release in the material, and loss factor, respec- butions of the charges at the surface states vicariously lead tively [42, 43]. These parameters were computed via the to greater values of ϵ at low frequencies compared to the Fig. 1 A schematic representation of the produced Au/Fe O -PVA/n-Si SSs 3 4 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 2 a Real dielectric vs. V for the entire frequency range, Real dielectric vs. ln f b for the negative bias region, and c for the positive bias region high frequencies. The ϵ vs. lnf plots drawn for both nega- permittivity [50, 51]. According to Maxwell-Wagner polar- tive and positive bias regions separately and presented in ization based on Koop theory, the conduction electrons are Fig. 2b and c support these surface state effects with high mobile in the high resistive grain boundary region at low values at low frequencies compared to the values at high frequencies and low resistive grains at high frequencies. frequencies. This behavior of ϵ reliant on frequency is Encountered resistance at the low frequencies leads to accu- anticipated considering the Maxwell-Wagner polariza- mulation of the space charges, in turn, high ϵ values [42, tion [4, 44, 46–49]. Maxwell-Wagner, also referred to as 43, 52, 53]. From a cursory overview, the effectiveness of space charge polarization is effective at low and medium all possible polarization mechanisms as electronic, ionic, frequencies, and generally supplanted in the structure con- orientation, and space-charge polarization at low frequen- sisting of materials with different conductivity or dielectric cies leads to obtaining high ϵ values for these frequencies 1 3 Journal of Inorganic and Organometallic Polymers and Materials thanks to contributions of overall mechanisms. Albeit, due depending on frequency and voltage. Figure 3a exhibits ′′ to the varying effectiveness of these mechanisms depend - the drop of the computed ϵ values from 81.2 to 8.47 for ing on frequency, their contributions to the whole polariza- 0.1 kHz, and 1.02 to 0.03 for 1 MHz, additionally, a peak tion also vary. Electronic and ionic polarization while being behavior similar to the one observed in the depletion region dominant at very high frequencies, contributions are insuf- of the ϵ -V plot. Peak existence in the depletion region, ficient compared to the low frequencies [ 54–56]. especially at low frequencies, emanates from the domination ′′ The imaginer portion of the dielectric permittivity ( ϵ of surface states in these regions. To prominence the visu- ′′ ) corresponds to the energy loss during the alignment of the ality of frequency dependence, ϵ values were presented ′′ dipoles according to the external electric field, and the com - as ϵ -lnf plots for both reverse and forward bias regions puted values via Eq. (1b) were demonstrated in Fig. 3a–c separately in Fig. 3b and c. Figure 3b and c display that for Fig. 3 a Imaginer dielectric vs. V for the entire frequency range, Imaginer dielectric vs. ln f b for the negative bias region, and c for the positive bias region 1 3 Journal of Inorganic and Organometallic Polymers and Materials ′′ both voltage regions ϵ drops with frequency, congruous also shifts higher voltage values, with augmentation with Maxwell-Wagner polarization, and for further frequen- in frequency. The second peak becomes expeditiously cies reaches a nearly constant value regardless of voltage. disapperent with frequency augmentation, proving the source of this peak is as the surface states which loses 3.2 Tangent loss its dominant impacts for higher frequencies and these voltages. Additionally, tanδ-lnf plots for both reverse and forward bias regions were drawn separately and The tanδ value corresponds to the amount of energy demonstrated in Fig. 4c and d. loss during the alignment of the dipoles reliant on the external field direction. Figure 4a and b present the Both these figures indicate the sudden drop of tand tanδ-V plots for low and high frequencies, respec- values with increment in frequency for both voltage tively. Two distinct peaks come into view in Fig. 4a regions, and for high frequencies tanδ values become for low frequencies whereas just one peak comes into independent of frequency and voltage. The high view for high frequencies (Fig. 4b). Figure 4b confirms dielectric loss at low frequencies may be caused by that the height of the first peak in Fig. 4a drops and the high impact of the surface states caused by several Fig. 4 Tangent loss vs. Va between 0.1 to 7 kHz, and b between 10 to 1000 kHz, Tangent loss vs. ln f c for the negative bias region, and d for the positive bias region 1 3 Journal of Inorganic and Organometallic Polymers and Materials reasons in this region [42]. In conclusion, these fre- location of the arc centers on the real axis signifies the domi - ′ ′′ quency reliant behaviors of ϵ , ϵ , and tanδ are nant relaxation as Debye-type relaxation [57]. anticipated behaviors consistent with similar struc- tures reported in the literature [16, 37, 57–59]. 3.4 Impedance Analysis 3.3 Electric modulus The dielectric characteristics can be detailed by applying the impedance spectroscopy method. The real ( Z ) and imag- ∗ ′′ The complex electric modulus (M ) is a parameter that can iner ( Z ) portions of impedance can be computed via the provide information regarding relaxation phenomena and following relation; polarization process. M is defined as the inverse of the ′′ ′ 1 ϵ ϵ ∗ ′ ′′ ϵ , and the real (M ) and imaginer (M ) portions can be Z = = ( ) − j ( ) ∗ 2 2 2 2 (3) ′ ′′ ′ ′′ iω C ϵ o ωC ϵ + ϵ ωC ϵ + ϵ o o computed applying the following relation [47, 48, 57, 60]; ′ ′′ 1 ϵ ϵ ∗ The computed Z values were demonstrated in Fig. 8a M = = + j (2) 2 2 2 2 ∗ ′ ′′ ′ ′′ ′ ′ ϵ + ϵ ϵ + ϵ and b as Z -V plots and in Fig. 8c and d as Z -ln(f) plots. Figure 8a–d presents the peak behavior at the depletion ′ ′′ The M and M were given in Figs. 5a–c and 6a–d region regardless of frequency and peak height drops with depending on frequency and voltage. According to Fig. 5a, augmented frequency. The voltage region where the peak M values give a peak at the depletion region for each occurs and attenuated peak height at high frequencies vali- frequency. Additionally, Fig. 5b and c display rising M date the peak source as surface states and stable charges [45, values with frequency and applied voltage for both voltage 65]. For both voltage regions, Z values drop with rising regions. In the negative bias region displayed in Fig. 5b, frequency, saturate, and reach almost constant values at high voltage dispersion is more prominent compared to the for- frequencies, as demonstrated in Fig. 8c and d. The high Z ward bias region in Fig. 5c. values at low frequencies and the frequency independence ′′ The computed M values were demonstrated depend- at high frequencies are due to the space charge polarization ing on voltage and frequency in Fig. 6a–d. Figure 6a and b occurring at low frequencies [23, 45, 57, 66]. Additionally, depict the peak at the region corresponding to the depletion the high Z values at low frequencies indicate that resistive region along with varying peak height and position depend- grain boundaries are the source of the high resistivity at this ing on frequency value. The peak height rises with rising frequency region [67–69]. ′′ frequency and the peak’s position shifts toward the lower The computed Z values via Eq. (3) were depicted in ′′ ′′ ′′ voltage values. Peak behaviors also exist in the M -lnf Fig. 9a and b as Z -V plots and in Fig. 9c and d as Z ′′ plots depicted in Fig. 6c and d. Figure 6c clearly depicts -ln(f) plots. The Z -V plots demonstrated in Fig. 9a and that the peak occurrence comes into play at approximately b show the same peak behavior as seen in Fig. 8a and b 0 V. Figure 6d validates the peak occurrence corresponds to and the peak has the same variations with voltage and fre- ′′ the depletion region and displays the augmentation of M quency. The plots versus frequency drawn for reverse and values with frequency. forward bias regions with 0.15 V steps were demonstrated ′′ ′ The M -M plots were demonstrated in Fig. 7a and in Fig. 9c and d, respectively. As depicted in Fig. 9c, the ′′ b for reverse and forward bias regions, respectively, and Z values show an increase, reaching its maximum value these plots can impart more knowledge about the relaxation and with ongoing frequency increment dropping. Figure 9d process. Figure 7a indicates a distinct semicircle at low and shows the same attitudes for all forward bias voltages. The ′′ medium frequencies, whereas a deviation from the semi- frequency value at which Z reaches its maximum value circle at high frequencies. The presence of semicircles in corresponds to the relaxation frequency (f ) and it is clear Fig. 7a marks that the polarization in these regions emanates from the figures that this frequency is contingent on the from the grain actions [61, 62]. In contrast, the distortion of applied voltage [64, 70]. In conclusion, the diminution of ′ ′′ the semicircle is the result of grain boundaries dominating Z and Z values for higher frequency emanates from the polarization [17, 63]. For the forward bias region, Fig. 7b elevated number of hopping electrons with increment fre- indicates a semicircular arc varying radius with applied volt- quency [16, 66, 71, 72]. ages. Additionally, the small semicircular arc that occurred To gain more knowledge about relaxation phenomena, ′ ′′ at low frequencies can be seen inset plot of Fig. 7b. These Z and Z values were arranged as a Nyquist diagram small arcs are the results of weak grain boundary effects, demonstrated in Fig. 10a and b for reverse and forward bias in spite of the arc at the high frequencies corresponding to region, respectively. For both voltage regions, the plots pres- the grain effects [ 62, 64]. Moreover, for both figures, the ent overlapping semicircle-like geometrical shapes localized 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 5 a Real electric modulus vs. V for the entire frequency range, Real electric modulus vs. ln f b for the negative bias region, and c for the positive bias region at the center of the real axis origin verifying the Debye-type 70, 72, 73]. To put it another way, since the point where the single relaxation process occurring in the material [70]. In semicircle intersects the x-axis is related to the bulk resis- the reverse bias region, the radii of the semicircles show tance, Fig. 10b validates the increased bulk resistance of the almost independence on voltage as depicted in Fig. 10a, sample with voltage [74, 75]. while in the forward bias region, one small semicircle arc As a final step of impedance analysis, the phase angle corresponding to the low frequencies accompanies semi- (θ) amid resistive and capacitive currents is computed by ′ ′′ circles with radii varying reliant on voltage corresponding substituting Z and Z values in the following expression; to the high frequencies (Fig. 10b). Figure 10b presents the ( ) ′′ rising trend of semicircles’ radii with rising voltages, and −1 θ = tan (4) this behavior marks in essence a decrease in dc conductivity and an increase in the impedance with rising voltage [66, 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 6 Imaginer electric modulus vs. V a between 0.1 to 7 kHz, and b between 10 to 1000 kHz, Imaginer electric modulus vs. ln f c for negative bias region, and d for positive bias region The θ vs. V plots for reverse and forward bias regions were regardless of frequency and its shift with elevated frequency demonstrated in Fig. 11a and b, respectively, and they indi- pertains to a preponderant surface state effect in this region cate the clear variation of θ reliant on frequency. For low [37]. frequencies as presented in Fig. 11a, the θ varies approxi- mately between 0° to 60° in the reverse bias region depend- 3.5 Ac Conductivity ing on the frequency with an abrupt peak around (– 1) – 0 V. To put it another way, in the reverse bias region the θ aug- The real portion of the complex electrical conductivity ( σ ments with frequency and this behavior pursue until reach- ) corresponds to the ac conductivity ( σ ) and it can pro- ac ing 200 kHz validating in Fig. 11b. After that, the θ has a vide knowledge pertaining to probable conduction mecha- declining trend with augmented frequencies. Since the 90° nism for the material. The σ can be defined in terms of ac θ value in the reverse bias region corresponds to the prevail- dielectric loss or tangent loss as depicted in the following ing capacitive currents, it can be evaluated that the produced expression [58, 76–78]; Schottky structure showcases capacitive traits for 50 kHz, ′′ σ = ωϵ ϵ =(d /A) ωCtanδ (5) ac o i 70 kHz, and 100 kHz frequency values rather than resis- tive traits [16, 45, 71]. Additionally, the peak occurrence 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 7 Real electric modulus vs. imaginer electric modulus a for negative bias region, and b for positive bias region The computed σ values were illustrated versus voltage prevail the conduction. These results accommodate with the ac in Fig. 12a and b for low and high frequencies, in order. literature for similar structures [37, 39, 48, 58, 76, 77, 81]. Figure 12a and b indicate the evident increase of σ with In conclusion, we can say that the growth of a conven- ac elevated frequency, and a steep decrease of σ at around tional insulator/oxide layer at the M/S interface by tra- ac 0 V for each frequency. The elevated σ values for high ditional techniques cannot entirely passivate the active ac frequencies are explicable by hopping of charge carriers and dangling bonds at the semiconductor surface. In recent trapping or releasing of charges from the surface state levels times, scientists have focused on improving the perfor- [37, 58, 77]. Additionally, the drop of the series resistance mance of Schottky structures like diodes, photodiodes, at high frequencies can be acceptable as another source of solar cells, capacitors, and transistors by utilizing a high- frequency-reliant behavior of σ [48, 76]. On the other permittivity interlayer such as metal or metal-oxide doped ac hand, the σ can be defined as a function of angular fre - polymer due to their high surface-area, low-weight, good ac quency ( ω ) as depicted in the following expression [45, 48, mechanical-strength, electron storage capacity, flexibility, 78–80]; and easy growing methods like electrospinning, solid-liq- uid phase separation and template synthesis. In this study, σ = σ + Bω (6) ac dc the dielectric value of (Fe O -doped PVA) was achieved as 2 3 7.5 even at 100 Hz which is two times the SiO insulator In Eq. (6), B and s represent the pre-factor and frequency layer. Therefore, we can also say that these can be success- exponent. To evaluate σ values according to Eq. 6, fully used instead of conventional insulators in electronic ac these values were rearranged as the double logarithmic devices. σ -ω plots for three different dc voltages, as depicted in ac Fig. 13. Figure 13 depicts two discrete linear regions reliant on frequency regardless of dc voltage values. These linear 4 Conclusions occurred at different frequency areas validate the depen - dency of the conduction mechanism on frequency. Further, This study scrutinized the complex dielectric permittivity, the fitting of these linear ensures to computation of s val - complex electric modulus, complex impedance, and ac elec- ues which assures the knowledge pertaining to the prepon- trical conductivity of the Schottky structure and their varia- derant conduction mechanism. The s values correspond to tions reliant on the voltage and frequency. The impedance the slope of linear and vary between 0.14 and 0.34 for low measurements involving capacitance/conductance-voltage frequency area, whereas it is 0.40 for high frequency area data sets in the frequency range of 0.1 to 1000 kHz and the regardless of the voltage value. These s values mark the voltage range of (-5) to 7 V were used for this evaluation. ′ ′′ independence of the conduction mechanism on voltage and The computed ϵ , ϵ , and tanδ values presented depend- their values ranging between 0 and 1 validate that the trap- ing on voltage depict peak behavior between – 1 and 0 V cor- ping and releasing of the mobile charges amid surface states responding to the depletion region. Additionally, this peak 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 8 Reel impedance vs. V a between 0.1 to 7 kHz, and b between 10 to 1000 kHz, Reel impedance vs. ln f c for negative bias region, and (d) for positive bias region behavior is more prominent at low frequencies compared to then releasing of charges amid surface states. In epitome, high frequencies. The voltage and frequency region where the dielectric response of the Au/Fe O -PVA/n-Si Schottky 3 4 the peak occurred corresponds to the region where surface structure is sensitive to frequency and applied dc voltage state effects are dominant, and this corollary validates the tremendously, and salient effects of surface states on these ′ ′′ peak source as surface states. On the other hand, ϵ , ϵ dielectric characteristics come into play at low frequencies , and tanδ values presented depending on frequency exhibit and depletion layer. decrement behavior with frequency which denotes the exis- tence of Maxwell-Wagner and space charge polarization in the material. Furthermore, the Nyquist diagrams of the Schottky structure have one single semicircular arc local- ized at the center of the real axis origin. One peak in these diagrams corresponds to the single relaxation process, while localization of them at the center of the real axis corresponds to a Debye-type relaxation. The exhaustive evaluation of σ ac reliant on frequency and voltage gives a corollary that the prevail conduction in the material occurs via trapping, and 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 9 Imaginer impedance vs. Va between 0.1 to 7 kHz, and b between 10 to 1000 kHz, Imaginer impedance vs. ln f c for the negative bias region, and (d) for the positive bias region 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 10 Imaginer impedance vs. real impedance a for negative bias region, and b for positive bias region Fig. 11 Phase angle vs. Va between 0.1 to 7 kHz, and b between 10 to 1000 kHz 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 12 Ac conductivity vs. V a between 0.1 to 7 kHz, and b between 10 to 1000 kHz, Ac conductivity vs. ln f c for the negative bias region, and d for the positive bias region Fig. 13 The double logarithmic σ -ω graphs for three forward biases ac 1 3 Journal of Inorganic and Organometallic Polymers and Materials Acknowledgements This study was supported by the Gazi University structures. J. Mater. Sci.: Mater. Electron. 35, 227 (2024). h t t p s : / / Scientific Research Project (BAP) with FYL-2024-9859.d o i . o r g / 1 0 . 1 0 0 7 / s 1 0 8 5 4 - 0 2 4 - 1 2 0 0 7 - 7 5. G. Özel, S. Demirezen, Investigation of hybrid CuPc-doped ZnO/p-silicon photodiodes for photonic and electronic applica- Author Contributions All authors contributed to the study’s concep- tions. J. Mater. Sci.: Mater. Electron. 35, 946 (2024). h t t p s : / / d o i . o tion and design. Material preparation, data collection and analysis r g / 1 0 . 1 0 0 7 / s 1 0 8 5 4 - 0 2 4 - 1 2 6 7 7 - 3 were performed by Arezou Khalkhali, Esra Erbilen Tanrıkulu, Seçkin 6. M. Raj, C. Joseph, M. Subramanian, V. Perumalsamy, V. Elayap- Altındal Yerişkin, Aysun Arslan Alsaç, and Kevser Yıldız. The first pan, Superior photoresponse MIS Schottky barrier diodes with draft of the manuscript was written by Esra Erbilen Tanrıkulu, and nanoporous:Sn-WO films for ultraviolet photodetector applica - Seçkin Altındal Yerişkin and all authors commented on previous 3 tion. New J. Chem. 44, 7708–7718 (2020). h t t p s : / / d o i . o r g / 1 0 . 1 0 3 versions of the manuscript. All authors read and approved the final 9 / d 0 n j 0 0 1 0 1 e manuscript.All authors contributed to the study’s conception and 7. R. Ramadan, R.J. Martín-Palma, Electrical characterization of design. Material preparation, data collection and analysis were per- MIS schottky barrier diodes based on nanostructured porous sili- formed by Arezou Khalkhali, Esra Erbilen Tanrıkulu, Seçkin Altındal con and silver nanoparticles with applications in solar cells. Ener- Yerişkin, Aysun Arslan Alsaç, and Kevser Yıldız. The first draft of the gies. 13, 2165 (2020). h t t p s : / / d o i . o r g / 1 0 . 3 3 9 0 / e n 1 3 0 9 2 1 6 5 manuscript was written by Esra Erbilen Tanrıkulu, and Seçkin Altındal 8. G. Henry Thomas, A. Ashok Kumar, S. Kaleemulla, V. Rajago- Yerişkin and all authors commented on previous versions of the manu- pal Reddy, Electrical, structural, morphological and photovoltaic script. All authors read and approved the final manuscript. properties of Au/n-Ge heterojunctions using V O interfacial 2 5 layer. J. Mater. Sci.: Mater. Electron. 35, 1345 (2024). h t t p s : / / d o i Funding Open access funding provided by the Scientific and Techno - . o r g / 1 0 . 1 0 0 7 / s 1 0 8 5 4 - 0 2 4 - 1 3 0 3 8 - w logical Research Council of Türkiye (TÜBİTAK). 9. D.S. Reddy, V. Rajagopal Reddy, C.J. Choi, Dysprosium oxide (Dy O ) layer effect on the interface possessions of Au/n-GaN 2 3 Data Availability No datasets were generated or analysed during the Schottky diode as an interlayer and its chemical and microstruc- current study. tural features. Mater. Sci. Semiconduct. Process. 173, 108133 (2024). h t t p s : / / d o i . o r g / 1 0 . 1 0 1 6 / j . m s s p . 2 0 2 4 . 1 0 8 1 3 3 10. A. Usha Rani, D. Surya Reddy, A. Ashok Kumar, V. Rajagopal Declarations Reddy, Structural, chemical, optical, electrical and photodiode properties of Au/ZnPc/undoped-InP MPS-type diode using a Conflict of Interest The authors declare no competing interests. ZnPc interlayer. Mater. Sci. Eng.: B 305, 117436 (2024). h t t p s : / / d o i . o r g / 1 0 . 1 0 1 6 / j . m s e b . 2 0 2 4 . 1 1 7 4 3 6 Open Access This article is licensed under a Creative Commons 11. D. Mallikarjuna, A.A. Kumar, V.R. Reddy, S. Kaleemulla, V. Attribution 4.0 International License, which permits use, sharing, Janardhanam, C.J. Choi, Photovoltaic and barrier properties of adaptation, distribution and reproduction in any medium or format, Au/n-Ge Schottky junction modified by Methylene Blue Organic as long as you give appropriate credit to the original author(s) and the Dye Interlayer. J. Inorg. Organomet. Polym Mater. (2024). h t t p s : / source, provide a link to the Creative Commons licence, and indicate / d o i . o r g / 1 0 . 1 0 0 7 / s 1 0 9 0 4 - 0 2 4 - 0 3 3 5 2 - 5 if changes were made. The images or other third party material in this 12. S. Hlali, F. Bourguiba, N. Hizem, A. Kalboussi, R. Dhahri, A.M. article are included in the article’s Creative Commons licence, unless Al-Syadi, E. Brens Elkenany, S. Kossi, Investigation of electri- indicated otherwise in a credit line to the material. If material is not cal properties at ambient and high temperature of Al O based 2 3 included in the article’s Creative Commons licence and your intended Schottky barrier diodes structure using I-V, C-V and G/ω-V mea- use is not permitted by statutory regulation or exceeds the permitted surements, (2024). h t t p s : / / d o i . o r g / 1 0 . 2 1 2 0 3 / r s . 3 . r s - 4 8 6 3 7 6 7 / v 1 use, you will need to obtain permission directly from the copyright 13. P. Vivek, J. Chandrasekaran, V. Balasubramani, Fabrication of holder. To view a copy of this licence, visit h t t p : / / c r e a t i v e c o m m o n s . o Cu/Y-MoO /p-Si type Schottky barrier diodes by facile spray r g / l i c e n s e s / b y / 4 . 0 /. pyrolysis technique for photodetection application. Sens. Actua- tors: Phys. 335, 113361 (2022). h t t p s : / / d o i . o r g / 1 0 . 1 0 1 6 / j . s n a . 2 0 2 1 . 1 1 3 3 6 1 14. B. Akın, S.A. Hameed, S. Altındal Yerişkin, M. Ulusoy, H. 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Fukami, Impedance spec- 657, 414791 (2023). h t t p s : / / d o i . o r g / 1 0 . 1 0 1 6 / j . p h y s b . 2 0 2 3 . 4 1 4 7 9 troscopy and dielectric analysis in KH PO single crystal. Solid 2 4 1 State Ionics. 177, 2857–2864 (2006). h t t p s : / / d o i . o r g / 1 0 . 1 0 1 6 / j . s s i 77. B. Kınacı, C. Bairam, Y. Yalçın, E. Çokduygulular, Ç. Çetinkaya, . 2 0 0 6 . 0 5 . 0 5 3 H.İ. Efkere, S. Özçelik, Evaluation of dielectric properties of Au/TZO/n–Si structure depending on frequency and voltage. J. Publisher’s Note Springer Nature remains neutral with regard to juris- Mater. Sci.: Mater. Electron. 33, 10516–10523 (2022). h t t p s : / / d o i dictional claims in published maps and institutional affiliations. . o r g / 1 0 . 1 0 0 7 / s 1 0 8 5 4 - 0 2 2 - 0 8 0 3 8 - 7 1 3 http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Journal of Inorganic and Organometallic Polymers and Materials Springer Journals

A Study Regarding Dielectric Response and ac Electrical Conductivity of Schottky Structures (SSs) Interlaid with (Fe3O4-PVA) by Using Dielectric Spectroscopy Method

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Springer Journals
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1574-1443
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10.1007/s10904-025-03667-x
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Abstract

This study aims to reveal the complex-dielectric permittivity, complex electric modulus, complex impedance, and ac elec- trical conductivity of the SS interlaid with Fe O -PVA. For this intent, impedance measurements were actualized in the 3 4 frequency range of 0.1–1000 kHz and the voltage range of (– 5) – 7 V. The computed dielectric parameters via impedance measurements were presented as functions of both frequency and voltage to uncover their impacts on dielectric response, polarization, and conductivity. The dielectric parameters presented as a function of voltage showcase discernible zenith demeanor amid (– 1) and 0 V, and this behavior becomes more noticeable for low frequencies. These corollaries indicate that the source of zeniths is the surface states and their distribution in the forbidden band gap of the semiconductor. On the ′ ′′ other hand, ϵ , ϵ , tanδ values presented as a function of frequency exhibit a decrement trend with frequency increment, and frequency independency at higher frequencies. This frequency-related behavior of the dielectric parameters signifies the dominance of the Maxwell-Wagner and space charge polarization in the material. Further, the Nyquist diagrams of the SS confer one single semicircular arc corresponding to a Debye-type single relaxation process. Additionally, the conduc- tion mechanism of the structure was scrutinized via the slope of the lnσ -lnω plot. The slope values smaller than the ac unit signify that the hopping of mobile charges dominates the conduction. All these experimental ramifications denote the preponderant effects of frequency and voltage on the dielectric response of the structure. Keywords Fe O -PVA organic interface · Impedance spectroscopy · Complex dielectric and electric modulus · Ac 3 4 electrical conductivity 1 Introduction In recent years, it has been a priority to optimize the perfor- mances of Schottky structures since they immensely come into play in assorted implementations thanks to their apt- ness to integrated circuits. The wide implementation area Esra Erbilen Tanrıkulu of these structures has been spread from radiation detectors [email protected] [1], temperature sensors [2–4], and optoelectronic devices 1 [5, 6], to solar cells [7]. The most common approach to Graduate School of Natural and Applied Sciences, achieve Schottky structures with better performance and a Department of Advanced Technologies, Gazi University, Ankara, Turkey low cost is to try various materials as an interfacial layer [6, 8–14]. One of the most plausible materials to use as an inter- Department of Physics, Faculty of Science, Gazi University, Ankara, Turkey layer is organic polymer materials [2, 15–19]. Polyvinyl alcohol (PVA), in particular, provides advantages due to its Department of Chemistry and Chemical Processing Technologies, Vocational Highschool of Technical Sciences, salient features, primarily its easy production and low-cost Gazi University, Ankara, Turkey requirement [20–23]. Additionally, its adjustable features The General Directorate of State Hydraulic Works, Ankara, with some dopants make them congruous for multitudinous Turkey 1 3 Journal of Inorganic and Organometallic Polymers and Materials application areas. Since doping PVA, especially with metal dielectric properties. In another study performed on the or metal oxide increases its conductivity, it also increases dielectric characterization of MIS structure with PVAc-Si the possibility of usage of it in the electrical industry [22, insulator layer, it is concluded that the usage of PVAc-Si as 23]. Moreover, the doping process of PVA advances also an interfacial layer is proper, and the resultant MIS structure mechanical, thermal, and dielectric features [24–28]. Like- can be used in the floating gate memory devices [ 21]. Addi- wise, iron oxide (Fe O ) nanostructures are prominent in tionally, it is also noted in the literature that Schottky diodes 3 4 the literature by their unique magnetic properties, high ther- with PVC and doped-PVC interfacial layers have increased mal resistance, nontoxicity, and requirement for effortless dielectric constant, and in turn more energy capability com- production process [29–35]. Moreover, the usage of both pared to the traditional MS structure [39]. Considering the these materials together (PVA and Fe O ), investigations of literature outcomes epitomized above and considering the 3 4 their mechanical, thermal, and dielectric characteristics, and supreme dielectric peculiarities of the Fe O -PVA struc- 3 4 implementations spread from magnetic resonance imaging ture, it is believed that the usage of the Fe O -PVA structure 3 4 (MRI) to nanocatalyst and so far are supplanted in the lit- instead of traditional interlayers would change and enhance erature [24, 29, 36]. Considering the literature epitomized the dielectric characteristics of SSs. above, interposing of Fe O -PVA structure between metal The current study is the continuation of our previous 3 4 and semiconductor is foreseen congruous as an interfacial studies including temperature-reliant [40] and frequency- layer and may boost the performance of SSs. Especially, the reliant [41] electrical characteristics of SSs interlaid with underscored dielectric peculiarities of the Fe O -PVA struc- Fe O -PVA. The ref [40] verifies the formation of Fe O 3 4 3 4 3 4 ture motivate scrutinizing the dielectric characteristics of nanostructure, and dominant current transport mechanism the SS interlaid with it. (CTM) as thermionic-emission (TE) theory with Double- When another material such as dielectric or polymer Gaussian-distribution (DGD) of the BHs. In the other study materials is interposed between metal and semiconductor, [41], the evaluation of the main electrical characteristics is the metal-semiconductor (MS) structure is converted to the performed and the dependence on the frequency and volt- metal-oxide/insulator/polymer-semiconductor (MIS, MOS, age of them are revealed. Moreover, the region in which the or MPS) and may gain condenser characteristics. The pres- dominant effects of the surface states are observed is deter - ence of this layer intercepts the coaction between metal and mined as the depletion region. When it comes to this study, semiconductor, bringing in charge and energy storage capa- the scope is to investigate the dielectric properties, electric bility to the structure. Therefore, scrutinizing the dielectric modulus, and ac electrical conductivity, and designate the characteristics of these structures gains more importance. relaxation process, dominant conductance mechanism, and To comprehend the dielectric characteristics, they can be their frequency and voltage dependence. These experimen- parametrized in terms of complex dielectric permittivity tal corollaries reveal that the dielectric features of the fab- ∗ ′ ′′ ( ϵ ) including real ( ϵ ) and imaginer ( ϵ ) components, ricated SSs interlaid with Fe O -PVA strongly depend on 3 4 and loss factor (tand). Therewithal, calculation of complex voltage and frequency. Additionally, the frequency reliant ∗ ′ ′′ electric modulus (M ) and ac electrical conductivity ( σ variations of ϵ and ϵ validate that the structure has ac ) would be beneficial to be informed about the relaxation Maxwell-Wagner polarization, along with the Nyquist dia- process and transmission mechanism. Additionally, occur- gram shows that the structure has the Debye type single ring polarization in the material with the external electric relaxation. field manages all these dielectric parameters, and polariza - tion mechanisms called electronic, ionic, orientation and surface-charge polarizations show high dependency on 2 Experimental Procedure the frequency of the electric field [ 37, 38]. Therefore, fre- quency-reliant impedance analyses (covering capacitance The production of the Au/Fe O -PVA/n-Si SSs were based 3 4 (C), and conductance(G/ω) analyses) are prevalently used on an n-type Si wafer whose rudimental traits are its 350 to parametrize these dielectric features and delve into fre- µm thickness, 2” diameter, 1–10 Ω.cm resistivity, and quency and voltage reliant variations of them [37, 38]. < 100 > float-zone. After the first step as a chemical clean - The dielectric characterization of the SS with various ing process of the wafer, the coating of 99.999% pure Au interfacial layers is prevalent in the literature [16, 21]. For in the vacuum chamber was applied to achieve ∼150 nm instance, Yürekli et al. [16] reported a study comparing the thickness ohmic contact onto the rear side of the wafer. Fol- dielectric characteristics of SSs with three different inter - lowing that, the spin-coating method was utilized to grow facial layers. They demonstrated that the interfacial layer PVA: Fe O solution onto the fore side of the wafer. After- 3 4 has a changer effect on the dielectric trails and they noted ward, the production of the mentioned SSs was completed 3% graphene doped PVA interfacial layer shows better by evaporating high purity Au to become rectifier contacts 1 3 Journal of Inorganic and Organometallic Polymers and Materials –3 2 with a thickness of 150 nm and an area of 7.85 × 10 cm . following equations using impedance measurement results Figure 1 depicts the schematic representation of the pro- [38, 43–45]; duced Au/Fe O -PVA/n-Si SS. Refs [40] and [41] involve 3 4 more detailed articulation of the production process and ϵ = (1a) some structural analysis pertaining to Fe O -PVA nano- 3 4 structure. The XRD spectra presented in [40] reveal the spi- ′′ nel cubic crystal structure of the Fe O nanostructure with 3 4 ϵ = (1b) ω C an almost 13 nm crystallite size. Additionally, the reported SEM images in [40] give the uniform distribution of the ′′ ϵ G spherical-shaped Fe O nanostructure with a size less than 3 4 tanδ = = (1c) ϵ ω C 20 nm, while UV-Vis absorption spectra reveal the direct and indirect transitions with band gaps of 2.2 eV and 1.4 eV respectively. Prior to impedance measurements, the samples In these equations, C, G, and ω(= 2πf) are the measured were prepared by pasting it to a thin Cu holder utilizing a capacitance, conductance, and angular frequency, respec- silver paste to perform impedance measurements with an tively, while C is the geometric capacitance. The computed HP 4192 A LF impedance analyzer for various frequencies. ϵ values were demonstrated in Fig. 2a–c depending on frequency and voltage. Figure 2a presents the ϵ vs. V plot from – 5 to 7 V in a wide frequency range (0.1 kHz–1 MHz). 3 Results and Discussion Figure 2a also includes the peak between – 1.5 and 0 V cor- responding to the depletion region, especially for low fre- 3.1 Dielectric Permittivity quencies. Peak occurrence at the depletion region at which surface states exhibit the effects dominantly along with peak When a dielectric material undergoes an external electric nonoccurrence for high frequencies signify that surface field, the field entails keeping positive and negative charges states are responsible for this behavior. When a material is apart and inducing an electric dipole moment. Tackling the exposed to an ac external electric field with low frequencies, dielectric response of the material is crucial concerning the the charges at the surface states have adequate time to align materials’ applicability in electronic applications. These themselves with the same direction of the external field, so characterizations can be identified in terms of the complex their contributions can be detected. For high frequencies of dielectric permittivity ( ϵ ), and loss tangent (tand) parame- the external field, these charges cannot have adequate time, ′ ′′ ters. The real ( ϵ ) and imaginer ( ϵ ) portions of dielectric so their contributions become insufficient compared to the permittivity, and loss tangent (tanδ) denote energy absorp- low frequencies. To put it another way, the detectable contri- tion, energy release in the material, and loss factor, respec- butions of the charges at the surface states vicariously lead tively [42, 43]. These parameters were computed via the to greater values of ϵ at low frequencies compared to the Fig. 1 A schematic representation of the produced Au/Fe O -PVA/n-Si SSs 3 4 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 2 a Real dielectric vs. V for the entire frequency range, Real dielectric vs. ln f b for the negative bias region, and c for the positive bias region high frequencies. The ϵ vs. lnf plots drawn for both nega- permittivity [50, 51]. According to Maxwell-Wagner polar- tive and positive bias regions separately and presented in ization based on Koop theory, the conduction electrons are Fig. 2b and c support these surface state effects with high mobile in the high resistive grain boundary region at low values at low frequencies compared to the values at high frequencies and low resistive grains at high frequencies. frequencies. This behavior of ϵ reliant on frequency is Encountered resistance at the low frequencies leads to accu- anticipated considering the Maxwell-Wagner polariza- mulation of the space charges, in turn, high ϵ values [42, tion [4, 44, 46–49]. Maxwell-Wagner, also referred to as 43, 52, 53]. From a cursory overview, the effectiveness of space charge polarization is effective at low and medium all possible polarization mechanisms as electronic, ionic, frequencies, and generally supplanted in the structure con- orientation, and space-charge polarization at low frequen- sisting of materials with different conductivity or dielectric cies leads to obtaining high ϵ values for these frequencies 1 3 Journal of Inorganic and Organometallic Polymers and Materials thanks to contributions of overall mechanisms. Albeit, due depending on frequency and voltage. Figure 3a exhibits ′′ to the varying effectiveness of these mechanisms depend - the drop of the computed ϵ values from 81.2 to 8.47 for ing on frequency, their contributions to the whole polariza- 0.1 kHz, and 1.02 to 0.03 for 1 MHz, additionally, a peak tion also vary. Electronic and ionic polarization while being behavior similar to the one observed in the depletion region dominant at very high frequencies, contributions are insuf- of the ϵ -V plot. Peak existence in the depletion region, ficient compared to the low frequencies [ 54–56]. especially at low frequencies, emanates from the domination ′′ The imaginer portion of the dielectric permittivity ( ϵ of surface states in these regions. To prominence the visu- ′′ ) corresponds to the energy loss during the alignment of the ality of frequency dependence, ϵ values were presented ′′ dipoles according to the external electric field, and the com - as ϵ -lnf plots for both reverse and forward bias regions puted values via Eq. (1b) were demonstrated in Fig. 3a–c separately in Fig. 3b and c. Figure 3b and c display that for Fig. 3 a Imaginer dielectric vs. V for the entire frequency range, Imaginer dielectric vs. ln f b for the negative bias region, and c for the positive bias region 1 3 Journal of Inorganic and Organometallic Polymers and Materials ′′ both voltage regions ϵ drops with frequency, congruous also shifts higher voltage values, with augmentation with Maxwell-Wagner polarization, and for further frequen- in frequency. The second peak becomes expeditiously cies reaches a nearly constant value regardless of voltage. disapperent with frequency augmentation, proving the source of this peak is as the surface states which loses 3.2 Tangent loss its dominant impacts for higher frequencies and these voltages. Additionally, tanδ-lnf plots for both reverse and forward bias regions were drawn separately and The tanδ value corresponds to the amount of energy demonstrated in Fig. 4c and d. loss during the alignment of the dipoles reliant on the external field direction. Figure 4a and b present the Both these figures indicate the sudden drop of tand tanδ-V plots for low and high frequencies, respec- values with increment in frequency for both voltage tively. Two distinct peaks come into view in Fig. 4a regions, and for high frequencies tanδ values become for low frequencies whereas just one peak comes into independent of frequency and voltage. The high view for high frequencies (Fig. 4b). Figure 4b confirms dielectric loss at low frequencies may be caused by that the height of the first peak in Fig. 4a drops and the high impact of the surface states caused by several Fig. 4 Tangent loss vs. Va between 0.1 to 7 kHz, and b between 10 to 1000 kHz, Tangent loss vs. ln f c for the negative bias region, and d for the positive bias region 1 3 Journal of Inorganic and Organometallic Polymers and Materials reasons in this region [42]. In conclusion, these fre- location of the arc centers on the real axis signifies the domi - ′ ′′ quency reliant behaviors of ϵ , ϵ , and tanδ are nant relaxation as Debye-type relaxation [57]. anticipated behaviors consistent with similar struc- tures reported in the literature [16, 37, 57–59]. 3.4 Impedance Analysis 3.3 Electric modulus The dielectric characteristics can be detailed by applying the impedance spectroscopy method. The real ( Z ) and imag- ∗ ′′ The complex electric modulus (M ) is a parameter that can iner ( Z ) portions of impedance can be computed via the provide information regarding relaxation phenomena and following relation; polarization process. M is defined as the inverse of the ′′ ′ 1 ϵ ϵ ∗ ′ ′′ ϵ , and the real (M ) and imaginer (M ) portions can be Z = = ( ) − j ( ) ∗ 2 2 2 2 (3) ′ ′′ ′ ′′ iω C ϵ o ωC ϵ + ϵ ωC ϵ + ϵ o o computed applying the following relation [47, 48, 57, 60]; ′ ′′ 1 ϵ ϵ ∗ The computed Z values were demonstrated in Fig. 8a M = = + j (2) 2 2 2 2 ∗ ′ ′′ ′ ′′ ′ ′ ϵ + ϵ ϵ + ϵ and b as Z -V plots and in Fig. 8c and d as Z -ln(f) plots. Figure 8a–d presents the peak behavior at the depletion ′ ′′ The M and M were given in Figs. 5a–c and 6a–d region regardless of frequency and peak height drops with depending on frequency and voltage. According to Fig. 5a, augmented frequency. The voltage region where the peak M values give a peak at the depletion region for each occurs and attenuated peak height at high frequencies vali- frequency. Additionally, Fig. 5b and c display rising M date the peak source as surface states and stable charges [45, values with frequency and applied voltage for both voltage 65]. For both voltage regions, Z values drop with rising regions. In the negative bias region displayed in Fig. 5b, frequency, saturate, and reach almost constant values at high voltage dispersion is more prominent compared to the for- frequencies, as demonstrated in Fig. 8c and d. The high Z ward bias region in Fig. 5c. values at low frequencies and the frequency independence ′′ The computed M values were demonstrated depend- at high frequencies are due to the space charge polarization ing on voltage and frequency in Fig. 6a–d. Figure 6a and b occurring at low frequencies [23, 45, 57, 66]. Additionally, depict the peak at the region corresponding to the depletion the high Z values at low frequencies indicate that resistive region along with varying peak height and position depend- grain boundaries are the source of the high resistivity at this ing on frequency value. The peak height rises with rising frequency region [67–69]. ′′ frequency and the peak’s position shifts toward the lower The computed Z values via Eq. (3) were depicted in ′′ ′′ ′′ voltage values. Peak behaviors also exist in the M -lnf Fig. 9a and b as Z -V plots and in Fig. 9c and d as Z ′′ plots depicted in Fig. 6c and d. Figure 6c clearly depicts -ln(f) plots. The Z -V plots demonstrated in Fig. 9a and that the peak occurrence comes into play at approximately b show the same peak behavior as seen in Fig. 8a and b 0 V. Figure 6d validates the peak occurrence corresponds to and the peak has the same variations with voltage and fre- ′′ the depletion region and displays the augmentation of M quency. The plots versus frequency drawn for reverse and values with frequency. forward bias regions with 0.15 V steps were demonstrated ′′ ′ The M -M plots were demonstrated in Fig. 7a and in Fig. 9c and d, respectively. As depicted in Fig. 9c, the ′′ b for reverse and forward bias regions, respectively, and Z values show an increase, reaching its maximum value these plots can impart more knowledge about the relaxation and with ongoing frequency increment dropping. Figure 9d process. Figure 7a indicates a distinct semicircle at low and shows the same attitudes for all forward bias voltages. The ′′ medium frequencies, whereas a deviation from the semi- frequency value at which Z reaches its maximum value circle at high frequencies. The presence of semicircles in corresponds to the relaxation frequency (f ) and it is clear Fig. 7a marks that the polarization in these regions emanates from the figures that this frequency is contingent on the from the grain actions [61, 62]. In contrast, the distortion of applied voltage [64, 70]. In conclusion, the diminution of ′ ′′ the semicircle is the result of grain boundaries dominating Z and Z values for higher frequency emanates from the polarization [17, 63]. For the forward bias region, Fig. 7b elevated number of hopping electrons with increment fre- indicates a semicircular arc varying radius with applied volt- quency [16, 66, 71, 72]. ages. Additionally, the small semicircular arc that occurred To gain more knowledge about relaxation phenomena, ′ ′′ at low frequencies can be seen inset plot of Fig. 7b. These Z and Z values were arranged as a Nyquist diagram small arcs are the results of weak grain boundary effects, demonstrated in Fig. 10a and b for reverse and forward bias in spite of the arc at the high frequencies corresponding to region, respectively. For both voltage regions, the plots pres- the grain effects [ 62, 64]. Moreover, for both figures, the ent overlapping semicircle-like geometrical shapes localized 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 5 a Real electric modulus vs. V for the entire frequency range, Real electric modulus vs. ln f b for the negative bias region, and c for the positive bias region at the center of the real axis origin verifying the Debye-type 70, 72, 73]. To put it another way, since the point where the single relaxation process occurring in the material [70]. In semicircle intersects the x-axis is related to the bulk resis- the reverse bias region, the radii of the semicircles show tance, Fig. 10b validates the increased bulk resistance of the almost independence on voltage as depicted in Fig. 10a, sample with voltage [74, 75]. while in the forward bias region, one small semicircle arc As a final step of impedance analysis, the phase angle corresponding to the low frequencies accompanies semi- (θ) amid resistive and capacitive currents is computed by ′ ′′ circles with radii varying reliant on voltage corresponding substituting Z and Z values in the following expression; to the high frequencies (Fig. 10b). Figure 10b presents the ( ) ′′ rising trend of semicircles’ radii with rising voltages, and −1 θ = tan (4) this behavior marks in essence a decrease in dc conductivity and an increase in the impedance with rising voltage [66, 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 6 Imaginer electric modulus vs. V a between 0.1 to 7 kHz, and b between 10 to 1000 kHz, Imaginer electric modulus vs. ln f c for negative bias region, and d for positive bias region The θ vs. V plots for reverse and forward bias regions were regardless of frequency and its shift with elevated frequency demonstrated in Fig. 11a and b, respectively, and they indi- pertains to a preponderant surface state effect in this region cate the clear variation of θ reliant on frequency. For low [37]. frequencies as presented in Fig. 11a, the θ varies approxi- mately between 0° to 60° in the reverse bias region depend- 3.5 Ac Conductivity ing on the frequency with an abrupt peak around (– 1) – 0 V. To put it another way, in the reverse bias region the θ aug- The real portion of the complex electrical conductivity ( σ ments with frequency and this behavior pursue until reach- ) corresponds to the ac conductivity ( σ ) and it can pro- ac ing 200 kHz validating in Fig. 11b. After that, the θ has a vide knowledge pertaining to probable conduction mecha- declining trend with augmented frequencies. Since the 90° nism for the material. The σ can be defined in terms of ac θ value in the reverse bias region corresponds to the prevail- dielectric loss or tangent loss as depicted in the following ing capacitive currents, it can be evaluated that the produced expression [58, 76–78]; Schottky structure showcases capacitive traits for 50 kHz, ′′ σ = ωϵ ϵ =(d /A) ωCtanδ (5) ac o i 70 kHz, and 100 kHz frequency values rather than resis- tive traits [16, 45, 71]. Additionally, the peak occurrence 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 7 Real electric modulus vs. imaginer electric modulus a for negative bias region, and b for positive bias region The computed σ values were illustrated versus voltage prevail the conduction. These results accommodate with the ac in Fig. 12a and b for low and high frequencies, in order. literature for similar structures [37, 39, 48, 58, 76, 77, 81]. Figure 12a and b indicate the evident increase of σ with In conclusion, we can say that the growth of a conven- ac elevated frequency, and a steep decrease of σ at around tional insulator/oxide layer at the M/S interface by tra- ac 0 V for each frequency. The elevated σ values for high ditional techniques cannot entirely passivate the active ac frequencies are explicable by hopping of charge carriers and dangling bonds at the semiconductor surface. In recent trapping or releasing of charges from the surface state levels times, scientists have focused on improving the perfor- [37, 58, 77]. Additionally, the drop of the series resistance mance of Schottky structures like diodes, photodiodes, at high frequencies can be acceptable as another source of solar cells, capacitors, and transistors by utilizing a high- frequency-reliant behavior of σ [48, 76]. On the other permittivity interlayer such as metal or metal-oxide doped ac hand, the σ can be defined as a function of angular fre - polymer due to their high surface-area, low-weight, good ac quency ( ω ) as depicted in the following expression [45, 48, mechanical-strength, electron storage capacity, flexibility, 78–80]; and easy growing methods like electrospinning, solid-liq- uid phase separation and template synthesis. In this study, σ = σ + Bω (6) ac dc the dielectric value of (Fe O -doped PVA) was achieved as 2 3 7.5 even at 100 Hz which is two times the SiO insulator In Eq. (6), B and s represent the pre-factor and frequency layer. Therefore, we can also say that these can be success- exponent. To evaluate σ values according to Eq. 6, fully used instead of conventional insulators in electronic ac these values were rearranged as the double logarithmic devices. σ -ω plots for three different dc voltages, as depicted in ac Fig. 13. Figure 13 depicts two discrete linear regions reliant on frequency regardless of dc voltage values. These linear 4 Conclusions occurred at different frequency areas validate the depen - dency of the conduction mechanism on frequency. Further, This study scrutinized the complex dielectric permittivity, the fitting of these linear ensures to computation of s val - complex electric modulus, complex impedance, and ac elec- ues which assures the knowledge pertaining to the prepon- trical conductivity of the Schottky structure and their varia- derant conduction mechanism. The s values correspond to tions reliant on the voltage and frequency. The impedance the slope of linear and vary between 0.14 and 0.34 for low measurements involving capacitance/conductance-voltage frequency area, whereas it is 0.40 for high frequency area data sets in the frequency range of 0.1 to 1000 kHz and the regardless of the voltage value. These s values mark the voltage range of (-5) to 7 V were used for this evaluation. ′ ′′ independence of the conduction mechanism on voltage and The computed ϵ , ϵ , and tanδ values presented depend- their values ranging between 0 and 1 validate that the trap- ing on voltage depict peak behavior between – 1 and 0 V cor- ping and releasing of the mobile charges amid surface states responding to the depletion region. Additionally, this peak 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 8 Reel impedance vs. V a between 0.1 to 7 kHz, and b between 10 to 1000 kHz, Reel impedance vs. ln f c for negative bias region, and (d) for positive bias region behavior is more prominent at low frequencies compared to then releasing of charges amid surface states. In epitome, high frequencies. The voltage and frequency region where the dielectric response of the Au/Fe O -PVA/n-Si Schottky 3 4 the peak occurred corresponds to the region where surface structure is sensitive to frequency and applied dc voltage state effects are dominant, and this corollary validates the tremendously, and salient effects of surface states on these ′ ′′ peak source as surface states. On the other hand, ϵ , ϵ dielectric characteristics come into play at low frequencies , and tanδ values presented depending on frequency exhibit and depletion layer. decrement behavior with frequency which denotes the exis- tence of Maxwell-Wagner and space charge polarization in the material. Furthermore, the Nyquist diagrams of the Schottky structure have one single semicircular arc local- ized at the center of the real axis origin. One peak in these diagrams corresponds to the single relaxation process, while localization of them at the center of the real axis corresponds to a Debye-type relaxation. The exhaustive evaluation of σ ac reliant on frequency and voltage gives a corollary that the prevail conduction in the material occurs via trapping, and 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 9 Imaginer impedance vs. Va between 0.1 to 7 kHz, and b between 10 to 1000 kHz, Imaginer impedance vs. ln f c for the negative bias region, and (d) for the positive bias region 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 10 Imaginer impedance vs. real impedance a for negative bias region, and b for positive bias region Fig. 11 Phase angle vs. Va between 0.1 to 7 kHz, and b between 10 to 1000 kHz 1 3 Journal of Inorganic and Organometallic Polymers and Materials Fig. 12 Ac conductivity vs. V a between 0.1 to 7 kHz, and b between 10 to 1000 kHz, Ac conductivity vs. ln f c for the negative bias region, and d for the positive bias region Fig. 13 The double logarithmic σ -ω graphs for three forward biases ac 1 3 Journal of Inorganic and Organometallic Polymers and Materials Acknowledgements This study was supported by the Gazi University structures. J. Mater. Sci.: Mater. Electron. 35, 227 (2024). h t t p s : / / Scientific Research Project (BAP) with FYL-2024-9859.d o i . o r g / 1 0 . 1 0 0 7 / s 1 0 8 5 4 - 0 2 4 - 1 2 0 0 7 - 7 5. G. Özel, S. Demirezen, Investigation of hybrid CuPc-doped ZnO/p-silicon photodiodes for photonic and electronic applica- Author Contributions All authors contributed to the study’s concep- tions. J. Mater. Sci.: Mater. Electron. 35, 946 (2024). h t t p s : / / d o i . o tion and design. Material preparation, data collection and analysis r g / 1 0 . 1 0 0 7 / s 1 0 8 5 4 - 0 2 4 - 1 2 6 7 7 - 3 were performed by Arezou Khalkhali, Esra Erbilen Tanrıkulu, Seçkin 6. M. Raj, C. Joseph, M. Subramanian, V. Perumalsamy, V. Elayap- Altındal Yerişkin, Aysun Arslan Alsaç, and Kevser Yıldız. The first pan, Superior photoresponse MIS Schottky barrier diodes with draft of the manuscript was written by Esra Erbilen Tanrıkulu, and nanoporous:Sn-WO films for ultraviolet photodetector applica - Seçkin Altındal Yerişkin and all authors commented on previous 3 tion. New J. Chem. 44, 7708–7718 (2020). h t t p s : / / d o i . o r g / 1 0 . 1 0 3 versions of the manuscript. All authors read and approved the final 9 / d 0 n j 0 0 1 0 1 e manuscript.All authors contributed to the study’s conception and 7. R. Ramadan, R.J. Martín-Palma, Electrical characterization of design. Material preparation, data collection and analysis were per- MIS schottky barrier diodes based on nanostructured porous sili- formed by Arezou Khalkhali, Esra Erbilen Tanrıkulu, Seçkin Altındal con and silver nanoparticles with applications in solar cells. Ener- Yerişkin, Aysun Arslan Alsaç, and Kevser Yıldız. The first draft of the gies. 13, 2165 (2020). h t t p s : / / d o i . o r g / 1 0 . 3 3 9 0 / e n 1 3 0 9 2 1 6 5 manuscript was written by Esra Erbilen Tanrıkulu, and Seçkin Altındal 8. G. Henry Thomas, A. Ashok Kumar, S. Kaleemulla, V. Rajago- Yerişkin and all authors commented on previous versions of the manu- pal Reddy, Electrical, structural, morphological and photovoltaic script. All authors read and approved the final manuscript. properties of Au/n-Ge heterojunctions using V O interfacial 2 5 layer. J. Mater. Sci.: Mater. Electron. 35, 1345 (2024). h t t p s : / / d o i Funding Open access funding provided by the Scientific and Techno - . o r g / 1 0 . 1 0 0 7 / s 1 0 8 5 4 - 0 2 4 - 1 3 0 3 8 - w logical Research Council of Türkiye (TÜBİTAK). 9. D.S. Reddy, V. Rajagopal Reddy, C.J. Choi, Dysprosium oxide (Dy O ) layer effect on the interface possessions of Au/n-GaN 2 3 Data Availability No datasets were generated or analysed during the Schottky diode as an interlayer and its chemical and microstruc- current study. tural features. Mater. Sci. Semiconduct. Process. 173, 108133 (2024). h t t p s : / / d o i . o r g / 1 0 . 1 0 1 6 / j . m s s p . 2 0 2 4 . 1 0 8 1 3 3 10. A. Usha Rani, D. Surya Reddy, A. Ashok Kumar, V. Rajagopal Declarations Reddy, Structural, chemical, optical, electrical and photodiode properties of Au/ZnPc/undoped-InP MPS-type diode using a Conflict of Interest The authors declare no competing interests. ZnPc interlayer. Mater. Sci. Eng.: B 305, 117436 (2024). h t t p s : / / d o i . o r g / 1 0 . 1 0 1 6 / j . m s e b . 2 0 2 4 . 1 1 7 4 3 6 Open Access This article is licensed under a Creative Commons 11. D. Mallikarjuna, A.A. Kumar, V.R. Reddy, S. Kaleemulla, V. Attribution 4.0 International License, which permits use, sharing, Janardhanam, C.J. Choi, Photovoltaic and barrier properties of adaptation, distribution and reproduction in any medium or format, Au/n-Ge Schottky junction modified by Methylene Blue Organic as long as you give appropriate credit to the original author(s) and the Dye Interlayer. J. Inorg. Organomet. Polym Mater. (2024). h t t p s : / source, provide a link to the Creative Commons licence, and indicate / d o i . o r g / 1 0 . 1 0 0 7 / s 1 0 9 0 4 - 0 2 4 - 0 3 3 5 2 - 5 if changes were made. The images or other third party material in this 12. S. Hlali, F. Bourguiba, N. Hizem, A. Kalboussi, R. Dhahri, A.M. article are included in the article’s Creative Commons licence, unless Al-Syadi, E. Brens Elkenany, S. Kossi, Investigation of electri- indicated otherwise in a credit line to the material. If material is not cal properties at ambient and high temperature of Al O based 2 3 included in the article’s Creative Commons licence and your intended Schottky barrier diodes structure using I-V, C-V and G/ω-V mea- use is not permitted by statutory regulation or exceeds the permitted surements, (2024). h t t p s : / / d o i . o r g / 1 0 . 2 1 2 0 3 / r s . 3 . r s - 4 8 6 3 7 6 7 / v 1 use, you will need to obtain permission directly from the copyright 13. P. Vivek, J. Chandrasekaran, V. Balasubramani, Fabrication of holder. To view a copy of this licence, visit h t t p : / / c r e a t i v e c o m m o n s . o Cu/Y-MoO /p-Si type Schottky barrier diodes by facile spray r g / l i c e n s e s / b y / 4 . 0 /. pyrolysis technique for photodetection application. Sens. Actua- tors: Phys. 335, 113361 (2022). h t t p s : / / d o i . o r g / 1 0 . 1 0 1 6 / j . s n a . 2 0 2 1 . 1 1 3 3 6 1 14. B. Akın, S.A. Hameed, S. Altındal Yerişkin, M. Ulusoy, H. 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Journal of Inorganic and Organometallic Polymers and Materials – Springer Journals

Published: Mar 11, 2025

Keywords: Fe3O4-PVA organic interface; Impedance spectroscopy; Complex dielectric and electric modulus; Ac electrical conductivity

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