Monolithic integration of MoS2-based visible detectors and GaN-based UV detectors
You Wu1,2, Zhiwen Li1,2, Kah-Wee Ang3, Yuping Jia1,2, Zhiming Shi1,2, Zhi Huang4, Wenjie Yu5, Xiaojuan Sun1,2, Xinke Liu1,2,6,*, and Dabing Li1,2,7,*
- 1State Key Laboratory of Luminescence and Applications, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun 130033, China
- 2Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China
- 3Department of Electrical and Computer Engineering, National University of Singapore, Singapore 117583, Singapore
- 4Shenzhen Castle Security Technology Co., Ltd., Shenzhen 518000, China
- 5State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, China
- 6e-mail: email@example.com
- 7e-mail: firstname.lastname@example.org
With the increasing demand for high integration and multi-color photodetection for both military and civilian applications, the research of multi-wavelength detectors has become a new research hotspot. However, current research has been mainly in visible dual- or multi-wavelength detectors, while integration of both visible light and ultraviolet (UV) dual-wavelength detectors has rarely been studied. In this work, large-scale and high-quality monolayer was grown by the chemical vapor deposition method on transparent free-standing GaN substrate. Monolithic integration of -based visible detectors and GaN-based UV detectors was demonstrated using common semiconductor fabrication technologies such as photolithography, argon plasma etching, and metal deposition. High performance of a 280 nm and 405 nm dual-wavelength photodetector was realized. The responsivity of the UV detector reached 172.12 A/W, while that of the visible detector reached 17.5 A/W. Meanwhile, both photodetectors achieved high photocurrent gain, high external quantum efficiency, high normalized detection rate, and low noise equivalent power. Our study extends the future application of dual-wavelength detectors for image sensing and optical communication.
Two-dimensional (2D) layered materials have received extensive attention due to their unique optical and electronic properties [1–10]. Molybdenum disulfide (), a typical member of the 2D transition-metal dichalcogenide materials family, has been the most investigated because of its potential applications in high-performance next-generation electrical and optoelectronic devices such as wearable flexible devices, image sensors, and communication devices [11–14]. Compared to the earliest studied graphene (zero bandgap), has a stable band gap associated with the number of material layers varying from 1.2 to 1.8 eV; moreover, the monolayer is a direct band gap () . The -based photodetectors (PDs) have achieved significant progress due to their high carrier mobility (), high thermal stability (), and high absorbance of . Various methods for 2D material preparation have been investigated such as mechanical exfoliation , electrochemical exfoliation [17,18], thermal decomposition , magnetron sputtering , and chemical vapor deposition (CVD) [21–23]. In 2012, an exfoliated single-layer phototransistor was obtained for the first time, and the photoresponsivity was at 750 nm . Ultrasensitive exfoliated monolayer photodetectors were also demonstrated, showing a distinct photoresponse in the range of 400–680 nm, and the peak photoresponsivity was 880 A/W at a wavelength of 561 nm . The 2D obtained by mechanical exfoliation has a better material quality, but it is uncontrollable and small in size (micrometer scale). Electrochemical exfoliation is also a method of obtaining 2D from top to bottom that can be used to produce larger-scale 2D , but with poor quality and problems like interfacial defects also occur when transferring to a target substrate. The CVD growth method has been the most widely investigated because of its excellent repeatability and large size.
substrates were used for CVD growth initially because they are perfectly compatible with Si-based optoelectronics [25,26]. However, it was found that it is easier to obtain high-quality on crystalline substrates like sapphire and GaN [27,28]. These crystal substrates having excellent thermal and chemical stability can be utilized for the preparation of transparent devices. GaN is significantly superior to and sapphire substrates because of its nearly perfect lattice matching [29,30] (0.8%, , ) and the small discrepancy on the thermal expansion coefficients between ()  and GaN ( ). The almost perfect lattice matching and small difference in thermal expansion coefficient make it possible to grow a higher quality single-layer (SL) on GaN. In addition, it has been demonstrated that the quasiparticle interaction will happen between the 2D and GaN substrate, resulting in the modulation of the intrinsic valley carriers in SL , or strong electron-phonon coupling between and GaN can lead to an increasing absorption coefficient of the layer . Figure 1 shows the calculated absorption coefficient of SL in the visible region, in which the value of SL is significantly increased. As a typical representative of the third generation semiconductor, GaN-based materials own the advantages of a wide and direct band gap, good thermal stability, and chemical stability , making it one of the best choices for UV photodetector fabrication. High-quality 2D grown on a lattice-matched GaN substrate has the potential to realize new concept high-performance photodetectors with the typical 2D/3D hybrid structure.
Figure 1. (a) Illustration of the SL -on-GaN structure. (b) Due to the electron-phonon coupling between and GaN, the calculated absorption coefficient of the SL layer is increased significantly in the visible region.
With the increasing demand for miniaturization, high integration, and multi-function photodetection, the investigation of 2D/3D multi-wavelength detectors has become a new focus. A hybrid 2D GaN heterostructure for dual-functional (405 nm and 532 nm) detection was realized with photoresponsivity on the order of . Similarly, multilayer grown on a free-standing GaN substrate also showed a multiple-wavelength photoresponse corresponding to 405, 532, and 638 nm, respectively . Two-dimensional -based dual-wavelength or multi-wavelength photodetectors have promising applications in future optical communication and image sensors. However, previous research has mainly focused on visible light detection, and this work achieved dual-wavelength detection of the -based visible range and the GaN-based UV range. Monolithic integration of UV and visible dual-wavelength detection in this work could broaden optical communications by reducing the signal error rate.
In this work, large-scale SL was grown on a lattice-matched and transparent free-standing (FS) GaN wafer by the CVD method. Common but efficient semiconductor fabrication processes were utilized to obtain monolithic integration of -based visible and GaN-based UV detectors. Both the materials and devices were fully characterized. Raman spectroscopy, transmission electron microscopy (TEM), and absorption spectroscopy were used to characterize the as-grown material, proving that a high-quality SL material was obtained. The photoresponsive properties of -based visible and GaN-based UV detectors under different incident light power conditions have been investigated. The photoresponsivity , photoconductive gain , external quantum efficiency (EQE), noise equivalent power (NEP), normalized detectivity , and the switching characteristics of the monolithic integration dual-wavelength detector were systematically studied in this work.
A. Sample Preparation and Device Fabrication
A (0001)-oriented Ga face FS-GaN substrate with thickness of was grown by the hydride vapor phase epitaxy (HVPE) method. Ammonia () and metal Ga/HCl were used as the nitrogen source and gallium source, respectively, and mixed gas was used as the carrier gas. After HVPE growth, it was further polished by chemical mechanical polishing (CMP) to obtain a surface with a surface roughness of 0.2 nm. A two-inch FS-GaN substrate was cut into pieces (1 cm by 1 cm) for the growth process, which is limited by the CVD chamber. The GaN substrate was ultrasonically cleaned with acetone, isopropanol, and deionized water for 10 min each time before being placed in the CVD chamber. 20 mg of molybdenum oxide () was located in an alumina crucible with an FS-GaN substrate upside down on the center of the crucible. 8 g of sulfur (S) powder was laid upstream, and the alumina crucible was located near the center in 100 sccm of argon (Ar) gas flow. The tube was thoroughly cleaned by Ar gas flow to remove air before the growth process. The SL was grown at 750°C for 10 min. The growth temperature has a significant effect on the thickness and shape of the layer. The optimized growth conditions were selected in this study. After the SL was grown on the GaN sample, a photolithography process was performed, and then part of the was etched by the Ar plasma without the protection of the photoresist. Standard photolithography and electron beam evaporation (EBE) for Au electrode (50 nm) preparation were used to define the electrode.
B. Materials and Device Characterizations
The incident laser wavelength of the Raman spectra was 514 nm from an Ar ion laser with laser power of 0.025 mW to avoid laser-induced heat. The absorbance spectra were tested by a UV-visible spectrometer (Shimadzu-2450) from 350 to 800 nm. Current-voltage (I-V) characteristics of the devices were measured by a Keithley 4200-SCS semiconductor analyzer. All measurements of materials and devices were carried out at room temperature.
3. RESULTS AND DISCUSSION
Figure 2(a) schematically illustrates the growth process by CVD. powder and were used as precursors, while a Ga-face FS-GaN substrate () was placed upside down on the center of the alumina crucible. The growth was completed in an Ar atmosphere with a growth temperature of 750°C for 10 min. The detailed growth process was described in the previous work . The grown on GaN was characterized, and the Raman spectrum was shown in Fig. 2(b). Raman spectrum measurement is based on the Raman scattering effect of the laser passing through the sample, reflecting the interlaminar vibration and intralayer vibration of the material, which is an important means for structural characterization of 2D layered materials . For the Raman spectrum of 2D , only and optical modes can be observed, which represent the in-plane vibration modes of and Mo atoms and the out-of-plane vibration modes of atoms. In addition, the full width at half-maximum (FWHM) of the peak characterizes the crystalline quality of 2D . The value of FWHM for peak here is about , which indicates the high quality of . Although the FWHM here is slightly larger than that of mechanical exfoliated , large-scale continuous on GaN was obtained by the CVD method in this work. The frequency difference () between the and Raman peaks is also important information for analyzing the thickness of . The positions of the and peaks are at 384.5 and , respectively, and the frequency difference is about , corresponding to monolayer which is consistent with other literatures [29,37,38]. An additional strong peak centered at around was observed, which is in accord with the high-order harmonic frequency of an acoustic phonon of GaN, and is not a Raman active mode [39,40]. Figure 2(c) is the cross-sectional transmission electron microscopy (TEM) image of the grown on GaN substrate. The measured film thickness is , indicating a single layer of , which is consistent with the Raman measurement result. Figure 2(d) shows the absorbance of the SL- grown on GaN as a function of incident wavelength. There are several absorption peaks in the visible region for SL : 430.9, 611.8, and 658.12 nm, respectively, and the absorption at 430.9 nm is the strongest, which is the exciton peak associated with the band edge. The excitonic absorption peaks between 600 and 700 nm observed for arise from the point of the Brillouin zone [41,42]. The spin-orbit splitting of the valence band of results in an energy difference between the two exciton peaks. Absorbance is the quantification of the absorption intensity, which is defined as , where is the intensity of original light and is the intensity of transmitted light . According to the Beer–Lambert law, the relationship between and is described as , where is the thickness of material and is the absorption coefficient. The absorption coefficient is calculated using the formula: . is 0.15 at 405 nm, indicating 29.2% of incident light intensity is absorbed. The thickness of SL is about 0.617 nm. The value of absorption coefficient calculated in this work is , which is similar to the absorption coefficient of the multilayer we studied before . The obtained absorption coefficient of the grown on FS-GaN is about one order of magnitude higher than that of the 2D grown on substrate, which may result in a highly responsive photodetector. The high absorption coefficient in this work could be due to growth on a nearly lattice-matched and a small thermal expansion mismatch FS-GaN substrate, resulting in a high quality of .
Figure 2. (a) Illustration of SL growth process by CVD under Ar atmosphere. The FS-GaN substrate was placed upside down on the center of the crucible, and the SL- was grown on the Ga-face. The growth condition was 750°C lasting for 10 min. (b) Raman spectrum of SL- on FS-GaN. (c) Cross-sectional transmission electron microscopy (TEM) image of the grown on the GaN substrate. The measured film thickness is , indicating a single layer of . (d) Absorbance of SL on the FS-GaN substrate as a function of incident wavelength. The strongest absorption is at around 430 nm.
The schematic diagram of the experimental process for monolithic integration of GaN-based UV detectors and -based visible detectors is shown in Fig. 3(a). A large-scale SL was grown on the pre-cleaned FS-GaN substrate by CVD. Then the SL on the FS-GaN sample was etched by Ar plasma to remove part of the that was not protected by photoresist. After the photoresist was removed, an interdigitated Au electrode (50 nm) was prepared on the entire sample to obtain the monolithic integrated GaN PDs and PDs by standard photolithography and metal evaporation. Figure 3(b) is the optical microscope image of monolithic integration of -based and GaN-based detectors, and the reference scale in the image is 100 μm. Each photodetector owns an active area of 47,376. Figure 3(c) is the 3D schematic view of monolithic integration device. The top view photo image of the fabricated detector is shown in the inset. In this work, monolithic integration of GaN-based detectors and -based detectors was achieved in a feasible and low-cost way.
Figure 3. (a) Schematic diagram of the preparation steps of monolithic integration of GaN-based UV detectors and -based visible detectors. Photoresist was used for mask, and part of the SL was etched by Ar plasma. Standard photolithography was applied, and a 50 nm Au electrode was fabricated by electron beam evaporation for the whole wafer. (b) Optical microscope image of monolithic integration of GaN-based and MoS2-based detectors. The reference scale in the image is 100 μm. (c) 3D schematic view of the monolithic integration device. Top view photo image of size sample fabricated is shown in the inset.
Figure 4(a) shows dark current and light current under 280 nm incident light with different incident power of GaN PDs as a function of voltage, while Fig. 4(b) shows that of PDs under 405 nm laser illumination. Our study before has compared the three different laser wavelengths, 405, 532, and 638 nm. It was found that the PD under the incident light of 405 nm has the best photodetector performance, which is because of a high-photocurrent gain mechanism and high absorption ratio . For 280 nm UV light, it can be absorbed by GaN and then generate photo-generated carriers to achieve UV detection. Thereby, dual-color detection was achieved in this study. The ratio of for GaN PDs is about – at a bias voltage of 20 V. It shows as good response to UV light, which is comparable to the results of previous studies [44,45]. As for PDs, the ratio of here is – at a bias voltage of 3 V.
Figure 4. (a) Dark current and light current for 280 nm incident light under different powers of the GaN PD. (b) Dark current and light current for a 405 nm laser under different incident powers of the PD.
The photoelectric characteristics of both the GaN-based UV detector and visible detector are calculated as shown in Fig. 5. The responsivity (), the quantification of the photosensitivity of PDs under certain wavelength light, is described as , where photocurrent is calculated by , is the active area of PD, and is the power density of incident light. Figures 5(a) and 5(d) are photocurrent and responsivity of the GaN PD and PD at 20 V and 3 V, respectively. The peak photoresponsivity of the GaN PD is 172.12 A/W under incident light power of 15 nW, while that of PD is 17.5 A/W under 2 mW laser illumination. This rather high photoresponsivity may be associated with longer carrier lifetime and less carrier recombination in the 2D material under weaker illumination. As shown in Fig. 5(d), as the incident laser power decreases, the of PD increases slightly, which is in accord with previous reports in and other 2D-based devices [46,47]. When the light power density increased enough, the trap states would be saturated, resulting in the photoresponsivity decrease .
Figure 5. (a) Responsivity (A/W) and photocurrent (μA), (b) photoconductive gain and external quantum efficiency (EQE), and (c) noise equivalent power (NEP) and normalized detectivity of the GaN PD as functions of incident power under a fixed voltage of 20 V. (d) Responsivity (A/W) and photocurrent (mA), (e) photoconductive gain and external quantum efficiency (EQE), and (f) noise equivalent power (NEP) and normalized detectivity of the PD as functions of incident power under a fixed voltage of 3 V.
Photoconductive gain () and EQE of the GaN-based PDs and -based PDs were also calculated as shown in Fig. 5(b) and Fig. 5(e), respectively. Photoconductive gain indicates the number of photocurrent carriers generated by absorbing each photon, which can be calculated by the formula , where is the elementary charge, is the frequency of the incident light, is the Planck constant, and is the absorption percentage. has been calculated in Figs. 5(a) and 5(d). In theory, GaN can absorb light with energy higher than its band gap, so for 280 nm light, . The absorption percentage of SL at 405 nm is 29.2%, which has been discussed before. The trend of photoconductive gain under different incident power is consistent with that of responsivity. For a GaN UV detector, the maximum photoconductive gain of 763.71 was obtained at a voltage of 20 V and an incident light power of 15 nW. The visible detector achieved a of 183.88 at 3 V and an incident light power of 2 mW. EQE is the percentage of collected electrons to the total number of incident photons, which can be described as . The maximum EQE of GaN UV detectors reached 76,370.1%, and for visible detectors the maximum EQE is 5369%. Both the GaN-based UV detector and -based visible detector exhibit high photoelectric conversion efficiency.
To further evaluate the detectivity and detection limit of our devices, normalized detectivity () and noise equivalent power (NEP) were calculated as shown in Figs. 5(c) and 5(f) for the GaN UV PD and the visible PD. NEP can evaluate the signal-to-noise ratio more quantitatively, which is defined as the incident optical power at unit signal-to-noise ratio, described as , where is signal power and is noise power . In this work, we can assume that the signal current is the illumination current and the noise current is the dark current (). Therefore, NEP can be calculated by the formula , in which is the elementary charge amount and is the amplifier bandwidth. A small NEP means that the noise is small, indicating the better performance of the device. The normalized detectivity (), indicating the detection limit to detect the minimum optical signal, is calculated by the equation . The larger means the stronger detection capability of the detector. For a GaN UV detector under 280 nm illumination, NEP is , and is Jones. For a visible detector, NEP is , and is Jones. The performance of the -based PD in this work is much lower than that of Si-based PDs ( of and of Jones) [50,51], but it is better than the SL -based PD ( of 7.5 mA/W) . This work achieved monolithic integration of GaN-based UV PD and -based visible PD for the first time to our knowledge in a simple process; however, the performance of the detectors is still not ideal, and further optimization of CVD growth details and device fabrication optimization are necessary.
Photo-switching characteristics have also been investigated for both GaN-based and -based PDs at a fixed voltage under 280 nm and 405 nm wavelength of incident light illumination, respectively. Figures 6(a) and 6(c) show the photocurrent of the GaN PD and PD under periodic changes in dark and illumination conditions. When under-illuminated, the current rises to the on state and then falls to the off state under the dark condition. The switch ratio of devices is described as . For GaN-based UV PD, the ratio of photocurrent versus dark is about 27.4, while that of -based visible PD is about 13.5. The switching behavior is quite stable through multiple times of changing the illumination conditions. The rise time () of the photodetectors is usually defined as the time it takes for the current to increase from 10% to 90% of the maximum, and the fall time () is the time for current decreasing from 90% to 10%. For a GaN UV detector, is 0.21 s and is 0.22 s as shown in Fig. 6(b); for visible detector, is 1.36 s and is 8.31 s as shown in Fig. 6(d). and obtained in this work are shorter than that of graphene-based devices , but are comparable to the reported SL -based PDs . For -based PD, when the laser turns off, the photocurrent decays to the dark level exponentially. It is observed that the sustained photocurrent is because of the long-range Coulomb potential captured, which may be related to the charged impurities in the interface of or inside , therefore greatly affecting the recombination of electron-hole pairs. The proper device passivation or packaging technology can further improve the photocurrent switching performance of the device, which is also the next step for us to improve the performance.
Figure 6. Photocurrent as a function of time under alternative dark and illumination. (a) Photocurrent-time curve of GaN illuminated by a 280 nm light source with the incident power of 15.01 nW at 20 V. (b) The rise time (from 10% to 90% of maximum photocurrent) and the fall time (from 90% to 10% of maximum photocurrent) of the GaN PD. (c) Photocurrent-time curve of illuminated by a 405 nm laser with the incident power of 10 mW at 3 V. (d) The rise and fall time of the PD.
In this work, the CVD growth method was used to obtain a high-quality and large-scale monolayer on a nearly lattice matched free-standing GaN substrate. And by a low-cost and feasible process, monolithic integration of -based visible detectors and GaN-based UV detectors was realized. The responsivity of the UV detector reached 172.12 A/W under 280 nm illumination, while that of the visible detector reached 17.5 A/W under 405 nm laser. Meanwhile, high-photocurrent gain , high external quantum efficiency, high normalized detectivity, and low noise equivalent power have been achieved for both two kinds of photodetectors. This study provides a low-cost, easy-to-process method for the preparation of dual-wavelength detectors with monolithic integrated UV and visible light, which has promising applications in image sensing and optical communication devices.
Acknowledgment. We thank Prof. Ke Xu from Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, for useful discussion and Prof. Hao-Chung Kuo from Taiwan Chiao Tung University. You Wu and Zhiwen Li contributed equally to this work.
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