A UVC photodetector based on Mg-doped ZnO film

doi:10.21203/rs.3.rs-4347208/v1

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A UVC photodetector based on Mg-doped ZnO film

https://doi.org/10.21203/rs.3.rs-4347208/v1

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The solar-blind ultraviolet (UV) photodetector (PD) can find extensive applications in fire prevention, ozone hole monitoring, navigation, and more, for the advantage of no solar background radiation in the UVC band (200-280 nm) at the earth's surface. However, most of the UVC PDs reported in recent years, including gallium oxide PDs, zinc oxide-based PDs, and aluminum nitride PDs, suffer from the complex and costive fabrication process, which requires high-temperature material fabrication and high fabrication costs. Here, we report a UVC PD composed of magnesium-doped zinc oxide (MgZnO) photosensitive functional material via a simple low-temperature sol-gel fabrication method. In the study, firstly, the synthesizing method of the MgZnO photosensitive functional layer is systematically investigated. Then, the optical bandgap change of MgZnO with the doped Mg concentrations is explored. The physical model of the relationship between the Mg-doped concentrations and the optical bandgap of the MgZnO photosensitive functional layer is established by spectroscopic methods. Based on the doping study, a highly responsive MgZnO UVC PD has been designed and fabricated. The MgZnO UVC PD shows a response bandwidth of 200 nm-280 nm, a high responsivity of 108 mA/W, and rise and fall times as low as 0.4 s and 2.4 s, respectively. The work reported here may open an easy, low-cost route for developing UVC PDs.

MgZnO

UVC

Sol-gel

Solar-blind

Photodetector

Solar-blind ultraviolet (UV) photodetector (PD) can find extensive applications in fire prevention, ozone hole monitoring, navigation, and more, for the UVC (200–280 nm) PD is interference-free in low UVC radiation zones in the near-earth environment [1–8]. Because detecting UVC requires wide bandgap semiconductors as the photosensitive layer, UVC PDs are mainly made from ultra-wide bandgap semiconductors (UWBG), such as gallium oxide (Ga₂O₃), aluminum nitride (AlN), boron nitride (BN), and magnesium-doped zinc oxide (MgZnO) [1, 9–12]. However, the fabrications of UVC PDs using the above UWBG materials all require complex fabrication processes with a high temperature, such as chemical vapor deposition (CVD) [11, 13] and molecular beam epitaxy (MBE) [14]. Thus, a UWBG functional material based on a low-temperature process is highly required.

In this study, we report the synthesis of MgZnO photosensitive functional material based on a simple sol-gel (S-G) method with a low-temperature process. Firstly, the MgZnO functional material doped with Mg concentrations is fabricated using the low-temperature sol-gel method. Based on the synthesized MgZnO, a UVC PD with high responsivity is built. During the doping study, the relationship between the Mg doping concentrations and the modulation of E_g is systematically investigated. Based on the 1%Mg-doped concentration of MgZnO, a UVC PD is built, which exhibits selective sensitization to the UVC band. The MgZnO UVC PD achieves high responsivity up to 108 mA/W at UV light of 254 nm. In addition, the MgZnO UVC PD’s rise time under UV light illumination is significantly reduced to 0.4 s (28 s, MgZnO UVC PD reported in the literature [15]). The study provides a new way to build high-responsivity MgZnO UVC PD via a simple low-temperature method.

2.1 Synthesis of MgZnO functional materials

The six groups of MgZnO functional materials with Mg mass fractions of 0%, 1%, 5%, 10%, 20%, and 30% are synthesized by the sol-gel method, with zinc acetate dihydrate (Zn(CH₃COO)₂·2H₂O) as the primary precursor, magnesium acetate tetrahydrate (C₄H₆O₄Mg·4H₂O) as dopant precursor, ethylene glycol methyl ether as a solvent, and ethanolamine (DEA) as a stabilizer. The detailed synthesis process is as follows: firstly, 0.1756 g, 0.1739 g, 0.1668 g, 0.1580 g, 0.1405 g, and 0.1229 g zinc acetate are mixed with 0 g, 0.0017 g, 0.0086 g, 0.0172 g, 0.0343 g, and 0.0515 g magnesium acetate, respectively. Then, each of the six mixtures above is added to 4 ml ethylene glycol methyl ether together with 0.0489 g ethanolamine stabilizer in six beakers, respectively. Next, six beakers are placed on a magnetic stirrer at 60°C for 3 h and then left for 24 h to obtain six clarified MgZnO colloidal solutions.

2.2 Fabrication of the MgZnO UVC PD

Glass substrates are cleaned using deionized water, acetone, and ethanol, respectively. Then, the cleaned glass substrates are blown dry with N₂. Later, the as-synthesized six MgZnO colloid solutions are spin-coated on the glass substrates at 3000 rpm for 30 s and then heated onto a heating platform at 95°C for 15 min to evaporate the solvent. The above spin-coating and heating process is repeated 6 times to form MgZnO functional materials. Next, the material product is annealed at 450°C for 1 h to minimize defects. Finally, MgZnO functional layers are obtained on glass substrates. After the 100 nm Al film is deposited onto the MgZnO functional layer by photolithography to form interdigital electrodes, the MgZnO PDs are finally fabricated.

2.3 Characterization and Photoelectric Measurement

The surface morphology and the doped Mg distribution of the synthesized MgZnO functional materials are investigated by scanning electron microscope (SEM, JEOL JSM-7900F, Japan) and energy dispersive spectrometer (EDS, JEOL JSM-7900F, Japan). The transmission and absorption spectra of the MgZnO functional materials are analyzed using a UV-visible spectrometer (UV-vis spectrometer, Ocean Optics QE65 Pro, USA) in the range of 200–850 nm.

Then, the electrical properties and responses of the MgZnO PDs, such as I-V, I-t curves, and interfacial resistance under UV (310 nm) and UV (200–390 nm) light illumination, are investigated using a source meter (Keithley 2450, USA) and a semiconductor parameter analyzer (Keithley 4200, USA). The responsivity of MgZnO PDs is measured by a source meter and UV light sources (254 nm, 310 nm, 365 nm, 395 nm).

The schematic structure of the MgZnO PD is shown in Fig. 1a. The MgZnO PD adopts a simple planar metal-semiconductor-metal (MSM) structure, including a 100 nm Al interdigital electrode, a MgZnO functional layer, and a glass substrate. A photograph of the MgZnO PD is shown in Fig. 1b, and the fabrication process of the MgZnO PD is shown in Fig. 1d. The SEM image of the device is shown in Fig. 1c. It can be found that the surface structure of the MgZnO functional layer is homogeneous without bubbles or other obvious defects. The EDS image of the MgZnO functional layer is shown in Fig. 1e. The elemental composition of MgZnO indicates that Mg content is successfully doped. The existence of the Mg dopant is consistent with the reported study, indicating that the atomic radii of Mg and Zn are close to each other, and the stable existence of the MgZnO structure can be realized by replacing Zn atoms with Mg atoms [16]. Figure 1f shows the typical I-t curve under UV illumination (200–390 nm) at 13.05 mW/cm² and a bias of 5 V of the device. The rise and fall times of the MgZnO PD are measured as low as 0.4 s and 2.4 s, which are faster than the ZnO-based PD. Figure 1g shows the switching ratio of the device for 6 switching operation cycles. The device has a uniform response curve with a stable switching ratio of 4000.

Figure 2a shows the current-voltage (I-V) characteristics curves at light intensities of 5.3, 1.8, 1, and 0.5 mW/cm², respectively. The I-V characterization curves indicate that the MgZnO PD can perceive the UV light at different intensities. The obvious symmetrical rectifying behavior indicates that the classic Schottky contacts between Al and MgZnO are achieved. The stabilized photo-response curves of the MgZnO PD at 5.325 mW/cm² are shown in Fig. 2b, indicating the photo-response will be improved by enhanced bias. Figure 2c shows the MgZnO PD response curves under different bias voltages. The left vertical axis is the responsivity, and the right vertical axis is the photocurrent. The stable photocurrent response of MgZnO PD under 5.325 mW/cm² illumination is shown in Fig. 2d, and the stable response over a long time is shown in the enlarged inset. The dark current of MgZnO PD is measured to only 10 pA under 5.325 mW/cm² illumination. Thus, the low dark current indicates the device’s ability to detect weak UV light. The measured variation of photocurrent with light intensity and the fitting curve of photocurrent with light intensity for the MgZnO PD are shown in Fig. 2e. The photocurrent increases with the increased light intensity in the range of 0 to 5.325 mW/cm², indicating that the MgZnO PD has good linearity over a wide range of light intensities. Figure 2f shows the responsivity change of the device with the light intensity illumination. The responsivity gradually decreases to a limiting value as the light intensity increases in the range of 0–2 mW/cm². When the light intensity exceeds 2 mW/cm², the responsivity hardly changes anymore, which means the photocurrent of the device saturates.

To investigate the Mg-doping concentration on the bandgap change of MgZnO to further tune the as-fabricated PD to work in the UVC band, the optical bandgap of MgZnO with different Mg-doping concentrations is analyzed and quantitatively calculated. The six MgZnO materials with different Mg-doping concentrations are named as follows: 0MgZnO (ZnO), 1%MgZnO, 5%MgZnO, 10%MgZnO, 20%MgZnO, and 30%MgZnO for Mg-doing concentrations of 0, 1%, 5%, 10%, 20%, and 30% in mass ratio, respectively.

Firstly, the spectra of MgZnO functional materials are analyzed in the UV-vis band (200–850 nm). Figure 3a shows the absorption spectra of ZnO, 20%MgZnO, and 30%MgZnO. The inset in the upper right corner of Fig. 3a shows the transmittance spectra of the three functional materials: 1%MgZnO, 5%MgZnO, and 10%MgZnO. As the Mg-doping concentration increases, both the transmittance and absorbance spectra are blue-shifted towards the short-wave direction. From the measured spectra, the E_g of MgZnO functional materials could be derived by the Tauc-plot method [17–19]:

$${\left(\alpha h\nu \right)}^{2}=A\left(h\nu -{E}_{g}\right)$$

Where $\alpha$ is the absorption coefficient, $A$ is a proportionality constant, h is Planck's constant. ν is photon frequency. Then, the curves of ${\left(\alpha h\nu \right)}^{2}$ versus $h\nu$ are plotted in Fig. 3b and Fig. 3c. From those curves, the intersections of their tangent lines and the X-axis is E_g. As shown in Fig. 3b, E_g of MgZnO functional materials increases from 3.36 eV to 3.92 eV (corresponding cut-off wavelengths decrease from 369 nm to 316 nm) as the concentration of doped Mg content increases from 0 to 10%, which agrees with reported literature (MgZnO functional materials varies from 3.38 eV to 3.84 eV as the concentration of Mg increases from 0–40%) [16]. From the analytical results, the E_g of MgZnO functional materials doped with more than 1% Mg mass fraction increases significantly, indicating a substantial blue shift of the cut-off wavelength. An Mg-doping concentration of over 10% of the MgZnO functional material is studied to achieve a shorter cut-off wavelength of the MgZnO functional material. However, single-phase segregation occurs when the Mg concentration rises to 25% [20–23]. To achieve higher doping concentration (> 10%MgZnO) thermal treatment could be utilized. 20%MgZnO and 30%MgZnO are successfully synthesized based on a 95°C preheating process during spin-coating. It is found that the key to the transition from inorganic mixture-amorphous-crystalline is combining the effects of the preheating temperature above 90°C and the annealing treatment above 300°C on the structure of the MgZnO functional materials. Compared to the high temperature of 1200°C by laser treatment [24–26], a relatively low-temperature treatment process for synthesizing 20%MgZnO and 30%MgZnO functional materials is achieved. Figure 3c illustrates that the E_g of the as-synthesized 20%MgZnO and 30%MgZnO is 4.24 eV and 4.27 eV. To be noticed, the E_g of the 20%MgZnO and 30%MgZnO is very close, which indicates that the limit of doping caused the blue-shift. From the slope of the 30%MgZnO curve in Fig. 3c, the cut-off wavelength of the 30%MgZnO is around 280 nm, blue-shifted to around 280 nm, reaching the UVC range.

Figure 3d shows the measured E_g of six MgZnO functional materials doped with different Mg concentrations and the simulated E_g based on Silvaco. Clearly, the experimental values match the simulated E_g well. The horizontal trend of the curve at Mg-doping is larger than 30%, which indicates that the E_g tuned by the doped Mg is reaching the limit. For 30%MgZnO, the E_g (4.27 eV, corresponding to 285nm) is suitable for UVC detection. Figure 3e shows the mechanism of the doped Mg on increasing the E_g of MgZnO functional materials. According to the reported Moss-Burstein shift [27, 28, 28–30], when the element Mg is doped, the MgZnO functional materials show the change of the Fermi energy level towards the conduction band, which causes an increase in the measured E_g. The Fermi energy level increases with increasing Mg-doping concentration. The more the Mg-doping concentration increases, the more the Fermi energy level shifts. Figure 3f-3h shows the working mechanism of MgZnO PD. As shown in Fig. 3f, Φ_m is the energy required for the electron to jump to the conduction band, and Φ_Al is the energy needed for the electron to reach the vacuum energy level. E_c, E_f, and E_v are the positions of the conduction band, the Fermi energy level, and the valence band, respectively. The MgZnO materials form two crystalline states, w-MgZnO, and c-MgZnO, which are similar to ZnO and MgO, respectively. The traveling of thermal-induced free electrons in the MgZnO materials is hindered by crystalline barriers. The electrons can hardly flow through the interface state, which effectively reduces the dark current. Figure 3g shows that under an applied bias voltage, a few electrons jump through the potential barrier and flow across the interfacial state to produce a dark current with a total electron current density of J_n. Under an external bias voltage and UV illumination, the photon energy excites many electrons to jump across the potential barrier and form an induced photocurrent with a total electron current density of J_p, as shown in Fig. 3h.

To verify that the E_g of MgZnO materials could be modulated by Mg-doping concentration, UV PDs built from 0%MgZnO, 1%MgZnO, 5%MgZnO, 10%MgZnO, 20%MgZnO, and 30%MgZnO materials are tested. As shown in Fig. 4a, the responsivity of MgZnO PDs changes with the wavelength of UV illumination. The simulated responsivity curves for three typical 1%MgZnO, 5%MgZnO, and 10%MgZnO PDs are well agreed with the measured results. For all PDs, as the incident light wavelength increases, the responsivity of the devices decreases. There are cut-off wavelengths for the devices with different Mg-doping concentrations, and the cut-off wavelength decreases with the increase of Mg-doping concentration. Clearly, the cut-off wavelengths of 1%MgZnO, 5%MgZnO, and 10%MgZnO PDs change from 336 nm to 316 nm, which is in good agreement with the calculated E_g (Fig. 3d). Specially, from Fig. 4a, the 1%MgZnO PD achieves a measured responsivity of up to 108 mA/W under UVC illumination (254 nm) and a bias of 5 V. The suppression ratio of UVC (254 nm) and non-UVC (310, 365, and 395 nm) signals (UVC responsivity vs. non-UVC responsivity) can be as high as 50 times. The inset of Fig. 4a shows that when the Mg-doping concentration increases from 1–10%, the responsivity of non-UVC decays gradually.

The responsivity of MgZnO PDs changes with Mg-doping concentration is further verified as shown in Fig. 4b. For 0%-30%MgZnO PDs, when under 254nm UV illumination, the responsivity first increases then decreases with Mg-doping concentration, and 1%MgZnO PD has the highest responsivity. Under 310nm, 365nm, and 395nm illumination, the responsivity of the PDs all decreases and keeps a constant small value for all PDs. To see the doping-caused wavelength cut-off effect, the PDs with 1%MgZnO, 5%MgZnO, and 10%MgZnO are tested in 254nm and 310nm UV illuminations. As in Fig. 4c, for 254nm illumination, the PDs with 1%, 5%, and 10% Mg-doping concentration all have high responsivity, which means 254 nm is within the devices’ UV detection spectra. Under 310nm illumination, 1%MgZnO PD has a large responsivity of 2 mA/W, while 5%MgZnO and 10%MgZnO PDs have a much smaller responsivity of 0.2 mA/W, which means the 310 nm beyond 5%MgZnO’s and 10%MgZnO’s UV detection range.

Figure 4d shows the responsivity of the devices with three different Mg-doping concentrations under 365nm and 395nm illumination. Clearly, the responsivity of the devices under the two non-UVC illuminations (365, 395 nm) is low because the wavelength cut-off values of those Mg-doped devices are shorter than the illumination wavelengths. This further confirms that the MgZnO functional materials fabricated from the low-temperature sol-gel method could effectively turn cut-off wavelengths to form UVC detectors.

In this study, we report the synthesis of MgZnO photosensitive functional material based on a simple S-G with a low-temperature process. The photo-response cut-off wavelength of the MgZnO can be effectively turned by Mg-doping concentration. Based on the synthesized MgZnO materials, UV PDs are successfully built. The 1%MgZnO PD exhibits high responsivity of up to 108 mA/W in the UVC band (254 nm). In addition, the MgZnO PD’s rise and fall times under UV light illumination are reduced to 0.4 s and 2.4 s (both about 28 s, MgZnO UVC PD reported in the literature [15]). The study might lead to a new strategy to build a high-responsivity MgZnO UVC PD using a simple low-temperature method.

Author contributions

Bowen Ren: Conceptualization, Methodology, Data curation, Writing-original draft & editing. Jiawei Zhai: Writing-editing. Jinhui Song: Supervision, Funding acquisition, Writing-review & editing.

Acknowledgments

This project is financially supported by the National Key R&D Program of China (2018YFA0703200).

Data availability

The original data supporting the present study's findings are available from the author upon reasonable request.

Conflict of interest

The authors declare that they have no conflict of interest.

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A UVC photodetector based on Mg-doped ZnO film

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Abstract

Figures

1 Introduction

2 Experimental details

2.1 Synthesis of MgZnO functional materials

2.2 Fabrication of the MgZnO UVC PD

2.3 Characterization and Photoelectric Measurement

3 Result and Discussion

4 Conclusion

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References

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