Fabrication and Characterization of Silicon nanowire/PEDOT: PSS Hybrid Hetrojunction Photosensor

doi:10.21203/rs.3.rs-2491165/v1

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Fabrication and Characterization of Silicon nanowire/PEDOT: PSS Hybrid Hetrojunction Photosensor

https://doi.org/10.21203/rs.3.rs-2491165/v1

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Silicon nanowire (SiNW) samples arrays are prepared by the metal-assisted chemical etching method using Ag as a catalyst and different etching durations of 15, 30 and 60 min. The structural, morphological and optical properties of the prepared SiNWs are investigated. The diameter of the prepared SiNWs ranges from 20 nm to 280 nm whilst the reflectance is less than 1% in the visible region wavelengths for all prepared samples. Hybrid heterojunction photosensors based on n-SiNWs/ PEDOT: PSS are fabricated by directly spin casting SiNWs by PEDOT: PSS thin films. The photosensor fabricated based on the SiNWs prepared for 60 min of duration exhibit excellent spectral responsivity of 23.231 mA W^− 1 and high sensitivity of 43.948% at 0 V bias under 622 nm light. Furthermore, the sensor shows high specific detectivity reaching 0.3×10¹¹ Jones with the bias voltage of 1 V and T_rice/T_fall of 20/23 ms with the bias voltage of 0.5 V.

The remarkable multifunctional features of nanocrystalline semiconductors with just one dimension, such as nanotubes, nanorods and nanowires, have elicited the interest of researchers. Some properties are high crystallinity, surface-to-volume ratio, quantum confinement effects and long lifespan electron-hole recombination[1], [2]. Silicon nanowires (SiNW) are amongst the most remarkable 1D nanostructures known today. Depending on the surface morphology, SiNWs have a variety of stunning qualities, such as diameter, length, growth direction and crystallization. Furthermore, the density of the generated NWs influences features such as optical and electrical properties. Owing to the quantum confinement effect, the optical band gap of SiNWs changes from indirect to direct, and the band gap grows as the wire diameter decreases [3],[4]. These nanostructures have a wide range of potential applications, which are biochemical sensors[5], gas sensors [6],lithium-ion batteries [7], field-effect transistors[8], catalysis[9], and solar cells [4],[10] . On the one hand, numerous methods for fabricating top–down and bottom–up techniques were used to create SiNWs, including vapour–liquid–solid[11], thermal evaporation[12], plasma-enhanced CVD[13], lithography[14] and laser ablation[15]. However, these processes have considerable downsides in that they often need costly, intricate equipment, toxic Si precursors, and high vacuum and temperature. Owing to these qualities, synthesis is costly and time consuming, limiting its commercialisation potential. On the other hand, the metal-assisted chemical etching (MACE) method has been proposed as a successful, promising synthetic approach[16]–[18]. This procedure is simple, quick and low cost. Furthermore, the MACE technique enables excellent crystalline NW quality and simple control of numerous factors such as orientation, doping type, length and diameter. The MACE technique consists of two steps: developing metal catalysts and the following etching procedure. Based on their wavelength response, photodetectors are classified as selective or wideband. Broadband photodetectors with high detection efficiency, fast response time, excellent operational stability, compact size and cheap cost offer enormous commercialisation potential. Aside from the many semiconducting materials used for photodetection, hybrid organic–inorganic structures are gaining popularity owing to their attractive optical and electrical properties [19]–[23]. PEDOT: PSS is one of the most effective conducting polymers. Extensive research has been carried out on photodetectors based on hybrid PEDOT: PSS/n-type inorganic semiconductor designs that show promising photo response[24], [25] .

2.1 Silicon nanowire array fabrication

SiNWs were fabricated by the MACE method using Ag as a catalyst and HF/H₂O₂ solution on single-sided polished n-type Si (100) wafer substrates (525 ± 25) µm thick, one side polished, phosphorus-doped, with resistivity of 5–10 Ohm.cm. They were ultrasonically cleaned using acetone followed by ethanol for 5 min at room temperature to eliminate organic contaminates. The substrate was treated with Piranha solution H₂SO₄/H₂O₂(3:1) at 70 c for 30 min to eliminate organic residues from the surface. After each cleaning step, deionized water was used to clean the wafers. The wafers were then immersed in diluted hydrofluoric (HF) acid for 5 min. For Ag nanoparticle deposition, cleaned wafers were dipped in HF acid (4.8 M) and AgNO₃ with concentration of 0.005 M for 1 min, and washed with deionized water. The prepared Ag/Si(100) samples were etched for different durations of 15, 30 and 60 min by HF/H₂O₂ to prepare SiNWs. The prepared SiNW samples were immersed in HNO₃ solution for 1 min to remove Ag nanoparticles from the surface of the SiNWs. Finally, the prepared SiNW samples were immersed in diluted HF acid (10%) for 1 min to remove SiO₂ native oxide from the surface[17], [26] .

2.2 Device fabrication

Figures 1(a–c) show how organic and inorganic nanostructures are made. After SiNW fabrication, Al was gun-deposited on the Si wafer’s back to act as a cathode contact. The SiNW was coated with highly conductive PEDOT: PSS (Clevis PH1000) on the FTO glass substrate to act as an anode contact. Highly conductive PEDOT: PSS contains 7% EG and 1% Triton X-100, by spin-speed at 2000 rpm for 40 s, as shown in Fig. 1(d). Owing to the capillary effect, blended PEDOT: PSS easily filled SiNW gaps to form core–sheath heterojunctions. The SiNW substrate can stick well onto the ITO/glass. The samples were annealed at 140 c for 20 min to remove the solvent. Each device had an active area of 1 cm².

3.1 Optical properties

Figure 2 illustrates the reflectance spectra of the Si(100) wafer and SiNWs prepared with different etching times. Frequently, the surface reflectance of Si exceeds 44% in the visible region (500–700 nm). Figure 1(b) shows the SiNW reflection decreases substantially as the length of the nanowires increases. The surface reflectance decreases to as low as 0.9%, 0.1% and 0.4% for etching times of 15, 30 and 60 min, respectively. This drop in reflectance may be attributed to subwavelength light harvesting and light scattering interactions between densely packed SiNWs[27]–[29] .

The energy gap of Si and SiNW films was determined from the reflectance spectrum for various etching times based on the Tauc relation [30]. The reflectivity decreased from the maximum value R_max to the minimum value R_min owing to light absorption by the substance. A line graph was drawn between [ln (R_max−R_min/(R − R_min]² and hυ as the ordinate to find the semiconductor’s band gap. Figure 3 shows the energy band gap of Si(100) wafer and SiNWs prepared for different durations. The energy gap of Si(100) wafer is 1.28 eV, as depicted in Fig. 3(a), and increases to 1.78, 1.8 and 1.82 eV for SiNWs prepared using various etching times of 15, 30 and 60 min, respectively, as shown in Figs. 2(b–c). The Si bulk is an indirect band-gap semiconductor with a band-gap energy of about 1.1 eV. However, when the size of Si is reduced to less than that of the free exciton, the band gap increases and causes a direct band gap [31]. SiNWs show greater direct bandgaps when the diameter is reduced whilst the length is increased [32].

3.2 Surface morphology

Figures 4(a–f ) show the FE-SEM images of the SiNWs prepared by the MACE method using different etching times with diameter distribution. The diameter of the NWs was measured using Image J software. The diameters of the SiNWs prepared with etching time of 15 min in the range of 20–300 nm decreases to the range of 20–280 nm for SiNWs prepared with etching time of 30 min, whereas that using etching time of 60 min decreases to the range of 20–240 nm. A similar trend was observed in previous studies by other researchers [33]. With the increase in etching time, the diameter of the nanowires is reduced. The direct energy gaps also increase with reducing SiNW diameter. The increase of etching time leads to an appreciable increase of the number density of nanowires. This result could be explained by the greater flexibility of the NW when increasing the etching time. Therefore, more often join to form beams due to van der Waals attractive forces. Similar trends were seen in earlier studies conducted by other researchers [34], [35].

3.3 Crystalline structure

Figure 5 shows the XRD spectra of the Si planar and SiNWs prepared at various etching times. The XRD peak for Si(100) corresponds to the lattice planes of (400) at 68.77° [39]. However, the intensity of XRD decreases with increasing the etching time that could be due to reducing the wire diameter when the etching time increases, and as result, the coverage area decreases. No other XRD peaks are seen in the XRD patterns, indicating no formation for SiO₂ layer on the surface of the prepared SiNWs. Furthermore, the appearance of the XRD peak at the same location as the Si wafer and SiNWs despite using different etching time indicates that the MACE method does not affect the value of the lattice parameter of the samples [36].

4.1 I-V (Current–Voltage Characteristics)

The electrical properties of SiNW samples prepared with different etching durations of 15, 30 and 60 min were investigated using current-voltage (I-V) measurements at room temperature and in the dark. Metal and semiconductors (Al/SiNWs) created a Schottky contact. The FTO/PEDO-PSS/SiNWs/Al device structure was subjected to I–V measurements ranging from − 1 V to 1 V. The I-V characteristics of the FTO/PEDO-PSS/SiNWs/Al hybrid photosensors made with an etching duration of 15 min are shown in Fig. 6(a). The photocurrents measured as a function of the applied reverse bias are extremely sensitive to light intensity under 506 nm illuminations with light intensities 20 mW/cm². The dark current of about 25.32 µA increases up to 182.75 µA with the bias voltage of 0.5 V. The measured photocurrent shows a remarkable increase with an increase in the incident light at 535 nm, with light intensities of 26.6 mW/cm². The dark current of about 28.43 µA increases to 234.63 µA at the bias voltage of 0.5 V. Importantly, the device reveals excellent photovoltaic characteristics under light illuminations of 622 nm with light intensities of 35 mW/cm². At the bias voltage of 1 V, the dark current of around 36.3 µA can be increased to 505.43 µA. A considerable increase is observed in the current value as the applied voltage increases. Figures 6(b–c) illustrate the I-V characteristics of the FTO/PEDO-PSS\SiNWs\Al hybrid photosensor prepared using etching times of 15, 30 and 60 min. When the etching period is 60 min. The reason for this is that the electron flows into the SiNW layers from Al, where it recombines with holes, leaving negatively charged electrons, which leads to the n-type role of SiNWs concerning Si. The electron demonstrates an increase in current intensity in the forward bias with an increase in etching time or with the length of the SiNWs. At the bias voltage of 1 V, the dark current of around 65 µA rises to 3.402 µA and flows into the SiNW layers from Al, where it recombines with holes. Therefore, in the forward bias, the current increases with an increase in the applied voltage because the forward bias voltage reduces the voltage barrier, consequently decreasing the width of the depletion region. As for the reverse bias, the width of the depletion region increases, which leads to impeding the movement of electrons. Therefore, the formation of a large voltage barrier at the interface rectifies the behaviour of the current [37]–[39].

4.2 Photo response characteristics

One of the most important factors in determining a photosensor’s capability is response speed. Figures 7(a–c), 8(a–b) and 9(a–b) demonstrate the photocurrent measurement at various biases for 0, 0.5 and 1 V for heterojunction devices to different light illumination values of 506, 535 and 622 nm for etching times of 15, 30 and 60 min, respectively. When the light is turned ON and OFF, heterojunction devices show a minimum dark current and a maximum light current. Various performance parameters of the fabricated photosensors. The sensitivity (S), responsivity (R), and detectivity (D) are calculated as follows[40] :

$$\text{S}= \frac{\text{I}\text{l}\text{i}\text{g}\text{h}\text{t}- \text{I}\text{d}\text{a}\text{r}\text{k}}{\text{I}\text{d}\text{a}\text{r}\text{k}} \times 100\%$$

$$R= \frac{\text{I}\text{l}\text{i}\text{g}\text{h}\text{t}- \text{I}\text{d}\text{a}\text{r}\text{k}}{Pin*A}$$

$$\text{D} = \text{R} \sqrt{\frac{A}{2\text{e}\text{I}\text{d}\text{a}\text{r}\text{k}}}$$

Where Pin is the incident optical power in mW, e is the electronic charge and A is the active area of the respected devices (0.785 cm² in this work). The sensitivity to light decreases as the bias voltage increases from 0 V to 1 V. This finding demonstrates that the apparatus can produce electron–hole pairs and successfully separate them, which enables the exhibition of a high current at 0 V. A tremendous enhancement is observed in the photocurrent for devices with increased bias voltage, where I_light/Idark ratios reach their highest value at the bias voltage of 1 V. Furthermore, the responsivity increases with the device’s bias voltage[41]. The heterojunction device with 622 nm illumination and 60 min etching time exhibits excellent spectral responsivity of 159.86 mA W^− 1 and high specific detectivity reaching 0.3×10¹¹ Jones with the bias voltage of 1 V, high sensitivity of 43.948%, and T_rice/T_fall of 20/23 ms with the bias voltage 0.5 V with 539 nm illumination. Table 1 compares the summary of the main findings in this work and previous studies. A higher responsivity of heterojunction device with 622 nm for etching time of 30 min is 70.787 mA\W at 1 V. At the bias voltage of 0 V43.948 highest sensitivity of about 23.371% is obtained at 622 nm illumination. The best specific detectivity of the device at etching time of 30 min reaches 0.2×1011 Jones, with high I_light/I_dark ratio of 18/24 ms at the bias voltage of 1 V under illumination by 506 nm. The fabricated SiNWs/PEDOT:PSS photosensor at 15 min etching time shows the highest sensitivity of 5.327% at 622 nm at 0 V. At the bias voltage of 1 V, the greater responsivity of ~ 17 mA\W and highest detectivity of 0.44×1010 Jones are obtained. The I_light/I_dark ratio is 26\28 ms at the bias voltage 0.5 V for 506 nm light

Table 1

Photoresponse parameters of fabricated SiNWs/PEDOT:PSS photosensors
Device structure	T_rise/T_dec. (ms)	Sensitivity %	Responsivity (A/mW)	Detectivity (Jones)	Ref.
FTO/PEDOT:PSS/SiNWs/Al (λ = 622nm) at 0V (etching time 60min)	35/36	43,948	13.794	0.24x10¹¹	Present work
FTO/PEDOT:PSS/SiNWs/Al (λ = 535nm) at 0 V (etching time 60min)	20/23	6,250	95.785	0.265×10¹¹	Present work
FTO/PEDOT:PSS/SiNWs/Al (λ = 535nm) at 1V(etching time 60min)	26/34	5,135	159.86	0.31×10¹¹	Present work
PEDOT:PSS/SiNWs (λ = 650 nm)	-	-	20	4 × 10¹¹	[42]
PEDOT:PSS/Si (λ = 656 nm)	129/146(µs)		137	2 × 10⁹	[43]
Perovskite thin film/SiNWs array	22.2/17.6		130	1×10¹³	[44]
Al/SiNWs/P2O5/Ag (50mW/cm2)	0.7/0.75	3578	-	-	[45]
n-SnO2/SiNWs (656nm)	47/11	0.64 × 10²		1.8 × 10¹⁰	[17]
PEDOT:PSS(Si + Psi micro-arrays)	396/412(µs)	-	1172.8 (White light)	5.81×10¹³	[41]

SiNWs are prepared by the MACE method using different etching times of 15, 30 and 60 min. The paper shows the effect of different etching times on the photosensor’s reflectance, electrical conduction and photo response. The produced SiNWs show a remarkable drop in reflectance from 0.9% and 0.7% to as low as 0.4% for varying etching times of 15, 30 and 60 minutes, respectively, compared with the Si planar. Moreover, device analysis shows that FTO/PEDO-PSS\SiNWs\Al at 60 min can work with a high responsivity of 159.86 mA\W and a very high sensitivity of 5135% at the expense of the devices at etching times of 15 and 30 min. This considerable reduction in reflectance confirms SiNWs are ideal candidates for solar cells. The I-V characteristics demonstrate the uniform-reproducible junctions’ rectifying behaviour. Our findings show that SiNWs at an etching time of 60 min are substantially more optically and electrically active, paving the way for their use in optoelectronic devices and solar cells.

We declare that the Submitted Research Paper is our original work and no part of it has been published anywhere else in the past. We take full responsibility, that if in future, the paper is found invalid according to basic rules, the last decision will be of the Authorities concerned. Any form of plagiarism will lead to disqualification of the paper.

Acknowledgement

We would like to express our profound gratitude to department of Physics/College os Science/University of Basrah for supporting the work.

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11) Authors' contributions: H.H. Inaya done the preparation and characterization of samples, analysis the obtained results and wrote the main manuscript. M A Mahdi read the obtained results and help to analyze it. Further, Mahdi read the manuscript as well as correct the mistakes.

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Fabrication and Characterization of Silicon nanowire/PEDOT: PSS Hybrid Hetrojunction Photosensor

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Abstract

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1. Introduction

2. Experimental Details

2.1 Silicon nanowire array fabrication

2.2 Device fabrication

3. Results And Discussions

3.1 Optical properties

3.2 Surface morphology

3.3 Crystalline structure

4. Electrical Characteristics

4.1 I-V (Current–Voltage Characteristics)

4.2 Photo response characteristics

Conclusions

Declarations

References

Additional Declarations

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