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Abstract
This paper presents a novel tunable narrowband photodetector based on Ag-MgF2-Ag (metal-dielectric-metal: MDM) Fabry-Perot (FP) microcavity structure. The tunability is achieved through precise adjustment of the thickness of the metal and intermediate dielectric layers of the FP microcavity, taking into account the response spectral range of planar perovskite. After optimizing the parameters mentioned above, the prototype devices were prepared by combining the perovskite layer and MDM layer. The center wavelength of the planar detector can be tuned from 430 nm to 680 nm within the detection band of 400-800 nm, with a narrow FWHM about 30 nm and a relatively high response of 0.05 A/W @ 5 V bias voltage for 500 nm. Meanwhile the rise and fall times of the detector are 375 ms and 550 ms, respectively. The experimental results are corroborated by the theory. Our design is highly beneficial to such applications as hyperspectral photography and color-related active optical devices, which paves the way to design this kind of triple structure.
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1. Introduction
With advancements in areas such as machine vision, biological detection, auto-driving, multi- or hyperspectral sensing, narrowband photodetectors have demonstrated promising applications [1–3]. In response to the increasing demand for narrowband photodetectors, several strategies have been suggested, including those based on narrowband absorption materials [4,5], charge collection narrowing effect [6–8], plasma resonance effect [9,10], utilization of optical microcavities [11]. However, most of these strategies can only achieve narrowband detection for specific wavelengths. For instance, the narrowband absorption (NBA) and charge collection narrowing (CCN) methods depend on the absorption properties of specific semiconductors, while the plasma resonance effect primarily relies on nanoparticles [12]. These limitations pose challenges in adjusting the central wavelength of the photodetector.
Among the strategies explored, the perovskite narrowband optoelectronic device based on optical microcavities has emerged as a new class of revolutionary optoelectronic devices with the potential for various practical applications, which incorporates the optical microcavities into the excellent optoelectronic properties of perovskite (high absorption coefficient, long carrier separation distance, high carrier mobility, adjustable optical broadband [13–15], etc.). Various coupled microcavities schemes based on FP cavities [16–19], photonic crystals [20,21], and whispering-gallery cavities [22,23] have been extensively studied for their remarkable ability to discriminate wavelengths [24,25]. For example, Xu et al. proposed to equip one-dimensional photonic crystal microcavity inspired by the compound eye of a butterfly on top of inorganic perovskite, and designed narrowband photodetectors with three central wavelengths of 800 nm, 850 nm, and 900 nm by controlling the structural parameters of the optical microcavity, achieving a narrowband detection effect with a half-height width lower than 60 nm [26]. Zhang Fujun et al. achieved narrowband detection in the ultraviolet region by utilizing Fabry-Perot (FP) resonant structures and photomultiplier photodetectors composed of PEDOT: PSS and P3HT:PC71BM.The devices exhibited an external quantum efficiency of 9300% and a half-height width of 33 nm at the central wavelength of 350 nm [11].
To date, achieving tunable narrowband detection over a wide spectral range remains a significant challenge. Despite the fact that the Fabry-Perot (FP) structure of optical microcavities is commonly employed to manipulate light with a predetermined wavelength and has a significant effect on the physical properties, to our knowledge, modulating the spectral response range of perovskite based on FP microcavities has not been reported up to now. The coupling of perovskite with an optical microcavity represents an intelligent approach for achieving a highly narrowband response. Compared to the commercially available dye molecular filters, FP cavity features better stability, higher color purity and allows for adjustment of its center wavelength and FHWM by modifying its structure, which is more significant to realize hyperspectral detection. The FP cavity comprises two layers of high reflectivity structures separated by an intermediate dielectric layer. Based on the high-reflectivity structure, the FP cavity is typically divided into all-dielectric and metal-dielectric-metal (MDM [27,28]) FP microcavities. The all-dielectric FP microcavity utilizes a distributed Bragg reflector (DBR [29]) as the high reflectivity structure, which can achieve a high Q factor since the all-dielectric microcavity has no absorption loss. However, they encounter limitations in their ability to operate across a wide range of bandwidths, particularly in the visible region, mainly due to their constrained stop-bandwidth [24]. Additionally, they exhibit rapid dispersion of reflection phase within the Bragg-mirror stopband, which is in contrast to the behavior observed in MDM FP cavities. In this work, we propose the use of MDM FP microcavities to modulate the spectral response range of perovskite. The device performance can be improved by optimizing the perovskite and FP microcavities.
2. Experiment
Figure 1 illustrates a series of device fabrication processes. First, the substrates are placed in a beaker containing a polytetrafluoroethylene cleaning rack. Then, an appropriate amount of acetone is poured in and ultrasonically cleaned for 20 minutes. Subsequently, the substrate is sequentially ultrasonically cleaned with ethanol, deionized water, and ethanol for 20 minutes each. After drying, the glass substrate is placed in a drying oven and kept at 150°C for 30 minutes. The dried glass substrates are then treated with UV ozone for 30 minutes to decompose organic matter on the surface, making the surface hydrophilic and improving substrate wettability.
The perovskite precursor solution was prepared by the way of Ref. [30]., PbI2, MAI, and FAI were mixed with the molar ratio1:x:(1-x), and 3% (by mass) of Pb (SCN)2 was added to increase the grain size of the perovskite film. Then, 2000 µL of DMF and 240 µL of DMSO were added, and the solution was filtered through a funnel to prepare the perovskite precursor solution. The pre-treated glass substrate was transferred to a glove box for perovskite spin-coating. The coating onto the substrate was done in two stages, with a spin speed of 500 rpm and an acceleration of 5000 rpm/s for 3 s in the first stage, and a spin speed of 2000-6000 rpm and an acceleration of 12000rpm/s for 60 s in the second stage. Ethyl ether was quickly dropped as an anti-solvent around 10 s during the spin-coating process [31,32]. The perovskite film was placed on a heating stage at 70°C for 2 min and annealed at a higher temperature for 10 min. The higher annealing temperature depended on the ratio of MAI and FAI [33], with 100°C used for pure MAPbI3 and 150°C used for pure FAPbI3. The annealed sample was then transferred into the physical vapor deposition system. The metal-dielectric-metal (MDM) FP microcavity, made of metallic Ag and dielectric MgF2, was evaporated on the glass substrates. The evaporation rates of the Ag and MgF2 were controlled by a thickness monitor at a rate of 0.05 nm/s. The silver electrode was deposited on the perovskite film side by evaporating at a rate of 0.1 nm/s with a thickness of 100 nm (see Fig. 1).
3. Results and discussion
Figure 2(a) shows the schematic diagram of the proposed MDM FP microcavity, and Fig. 2(b) displays the cross section SEM images of the MDM cavity, the partition interface between Ag and MgF2 can be clearly observed. When the light beam is normal incident, the transmittance of the FP is given by
Fig. 2. (a) Schematic diagram of MDM FP optical microcavity structure. (b) Cross-section SEM image of the MDM optical microcavity.
The central wavelength of the narrowband transmission peak is primarily governed by the MgF2 layer’s thickness d, the transmission peak’s linewidth is mainly dependent on the reflectance of the Ag layer R[35]. Hence, the FP optical microcavity is critical in determining the narrowband effect of the overall device. Here we design the structural parameters by simulation.
The Ag/MgF2/Ag microcavity structure of Fig. 2 is simulated, the thickness of the metal layer is set to 40 nm, and the thickness of the dielectric layer is changed from 90 nm to 220 nm in the steps of 10 nm. Figure 3(a) shows the transmittance spectrum as a function of MgF2 thickness and the wavelength calculated by the TMM (transfer matrix method) and FEM (finite element method). The results from the TMM and FEM are basically the same, and the small differences may be due to the accuracy settings in the calculation process. Figure 3(b) displays the relationship between the central wavelength and the thickness of the MgF2 layer, which is an almost linear relationship, giving the inspiration to design tunable filter structures. Wavelength-selective photo-detection is necessary for narrowband photodetectors to achieve color discrimination, which is crucial for many applications, including color photography, machine vision, gaming and intelligent surveillance. Three representative central wavelengths were selected as optical trichromes to represent the entire spectrum. Figure 3(c) plots the transmittance spectrum of the central wavelengths of around 430 nm, 500 nm, and 680 nm for different metal layer thicknesses. As we can see, the low intensity and the narrower bandwidth of the transmission peak appear when the thickness of the metal layer increases, the reason is that compared with the single Ag layer, the MDM triple layer structure exhibits obviously resonant absorption. In addition, the center wavelength of the transmission peak exhibits a blue-shift along with the increase of the Ag layer thickness.
Fig. 3. (a) Simulated transmittance spectra obtained using different methods. (b) Simulated relationship between resonance wavelength and MgF2 thickness. The color map represents the transmittance values. (c) Simulated transmittance spectra at specific center wavelengths with varying Ag layer thickness. (d) The blue, green, and red scatter plots are the transmission spectra of the simulated center wavelengths corresponding to 430 nm, 500 nm, and 680 nm, respectively, and the solid lines represent the corresponding experimental measurements. The insets are samples of the experiment.
According to Fig. 3(c) and the device fabrication method, we prepare three samples with the central wavelengths of 430 nm, 500 nm, and 680 nm, the corresponding thicknesses of the Ag layer are 50 nm, 50 nm and 40 nm, respectively, shown as insert in Fig. 3(d). Because the lower transmittance at 680 nm leads to bad performance PD (photodetector) due to thick Ag layer, the thickness of Ag thickness is decreased to 40 nm at the center wavelength of 680 nm to ensure the good performance of PD. We performed further optimization to accurately determine the thickness of MgF2 at the central wavelength as shown by the scatter plots in Fig. 3(d). The Ag/MgF2/Ag structure exhibits varying parameter values at different center wavelengths: 50 nm/102.96 nm/50 nm at 430 nm, 50 nm/131.48 nm/50 nm at 500 nm, and 40 nm/198.36 nm/40 nm at 680 nm. The corresponding solid line is the experimental result. The design center wavelength 430 nm, 500 nm, and 680 nm corresponds to the experimental peak wavelengths of 432 nm, 499 nm, and 678 nm respectively. The transmittance curve is in good accordance with the simulated results. The slight difference is due to fabricating error during film deposition. The prepared films have a high color purity and uniformity over the entire range.
Next, we optimize the detection property of the perovskite. A schematic diagram of the photoactive layer and electrode configuration is exhibited in Fig. 4(a), the incident light window is located at the bottom. The effect of the component of the photoactive layer on the photocurrent properties is discussed firstly. The ratio of MA:FA = 4:6 perovskite is used to obtain the largest grain size for better detection performance according to Ref. [30]. Figure 4(b) displays the photocurrent of pure MA, pure FA, and the ratio of MA:FA = 4:6 perovskite. Obviously, you can see that the MA0.4FA0.6PbI3 demonstrates the best photocurrent under the same conditions. Figure 4(c) and (d) show the transmittance curve and the photocurrent curve under different rotation speeds during the spin coating process for the best component MA0.4FA0.6PbI3 film. The rotation speed determines the thickness of the photoactive layer, and the thickness of the prepared perovskite affects the performance of the perovskite. The faster the rotation speed is, the more the precursor is thrown out, which leads to a thinner film. For the thicker film, the photo-generated carriers need to move a long distance to be collected by the electrode, resulting in a low collection rate of photocarriers. For the thinner photoactive film with a fast rotation speed, the density of photocarriers in the electrode increases, but the utilization of light is not high. As shown in Fig. 4(d), the maximum photocurrent response appears at the speed of 3000 rmp, confirming this conclusion. Figures 4(e) and (f) are the SEM images of the optimized MA0.4FA0.6PbI3 perovskite (the spin speed of 3000 rmp). We find that the MA0.4FA0.6PbI3 perovskite film has large crystals about several micrometers in size from Fig. 4(e) and 650 nm of the thickness from Fig. 4(d), no layered grain boundary at the whole cross-sectional interface.
Fig. 4. (a) Schematic diagram of light illumination. (b) Photocurrent corresponding to different proportions of MA and FA. (c) Transmittance spectra under different spin coating speed. (d) Photocurrent corresponding to different spin coating speed. The optimal ratio and speed SEM planar image (e) and cross section (f).
Figure 5(a) exhibits the schematic diagram of the overall configuration of the perovskite detector coupled with the FP microcavity. The normalized optical field distribution based on the structure of Fig. 5(a) is simulated by the FEM method with 50 nm Ag layer, 130 nm MgF2 layer, and the optimized thickness of 650 nm perovskite layer, the result is shown in Fig. 5(b). The evidence indicates that only one resonant wavelength at 500 nm is observed within the spectral range of 400-800 nm, and the electric field is predominantly localized in the middle MgF2 layer. Figure 5(c) depicts the normalized electric field intensity distribution of the device at the resonant wavelength of 500 nm and non-resonant wavelengths of 450 nm and 550 nm. We can observe that the E-field is mainly concentrated between the two metal layers at the resonance wavelength of 500 nm, and the E-field enhancement band is narrow leading to a narrow transmission because of FP resonance. And the perovskite layer displays the maximum electric field intensity, which is expected to facilitate the generation of photo-generated carriers. Figure 5(d) is the electromagnetic wave loss spectra in the different positions of the perovskite, the 500 nm center wavelength absorption loss is the largest, and as the electromagnetic wave propagates from the surface of the perovskite layer to the interior, the energy of the electromagnetic wave gets lower and lower until completely absorbed.
Fig. 5. (a) Schematic diagram of the device configuration. (b) Simulated E-field amplitude distributions as a function of wavelength in the visible region. (c) Normalized electric field amplitude at the resonant and non-resonant wavelengths. (d) Loss spectrum of electromagnetic waves in perovskite layer.
Responsivity (R) and external quantum efficiency (EQE) are commonly used parameters to describe photodetectors and can be calculated from the following equations [36,37]:
where Iph is the difference between the light current and dark current, the average dark current measurements at 2 V, 5 V, and 10 V bias are 0.324 nA, 0.755 nA, 1.64 nA, P and λ is the power and wavelength of the incident light, q is the elementary charge, h is the Planck constant, and c is the speed of light. Figure 6(a) shows the responsivity curves of the prepared narrowband photodetector centered at 500 nm for different bias voltages. For planar detectors, higher applied voltages lead to improved responsivity but also result in increased noise current and broadening of the full-width half maximum (FWHM). After considering these factors, a bias voltage of 5 V is chosen as the operating voltage for the device. Figure 6(b) illustrates the responsivity curves of three narrowband detectors prepared with center wavelengths of 430 nm, 500 nm, and 680 nm, and the corresponding responsivities are 0.036 A/W, 0.052 A/W, and 0.027 A/W, respectively. PD1, PD2 and PD3 are used to represent photodetectors with the central wavelength of 430 nm, 500 nm and 680 nm, correspondingly. Figure 6(c) plots the normalized EQE curve, with the FWHMs of PD1, PD2, and PD3 being 22 nm, 25 nm, and 32 nm, respectively, which is much narrower compared to the reported papers [3,38]. The absolute values of EQE are presented in Fig. S1 in the Supplement 1. The D* is widely used to indicate the sensitivity of the photodetector, which can be calculated from the following equation [39]: where R is the responsivity, q is the elementary charge, A is the active area which equals 3.78 mm2 in our experiment, Id is the dark current. The detectivity curves are obtained from the responsivity curves and are shown in Fig. 6(d). To characterize the transient current response of the narrowband perovskite, a monochromator is used to adjust the test wavelength to the detector’s corresponding center wavelength and the I-t curves of detectors with different center wavelengths at 5 V bias are tested in Fig. 6(e). The rise and fall time of PD1, PD2, PD3 are 386/548 ms, 375/550 ms, 398/612 ms respectively. Figure 6(f) shows the I-V curves at 430 nm for different incident light intensities. The I-V curves indicate that the slope of the curve increases with increasing incident light power, and the zero-crossing point of the IV curve indicates good ohmic contact between the electrode and semiconductor material.Fig. 6. Responsivity spectra of the device (a) under different applied voltage and (b) with different transmission peaks. (c) Normalized EQE of the device with different transmission peaks. (d) Typical detectivity with different transmission peaks. (e) TPC curves of the designed PD. (f) IV curves of the PD1 with different light intensity.
4. Conclusion
This work is based on planar perovskite detector coupled with FP microcavity to achieve narrow-band detection with tunable center wavelength. The structural parameters of the FP microcavity are optimized in terms of transmittance and half-height width, and the optimal responsivity curves of the perovskite layer at different ratios and different spin coating speeds are investigated. Under the guidance of simulation, three photodetectors with center wavelengths of 430 nm, 500 nm, and 680 nm are fabricated, and the optical responses at center wavelengths were 0.036 A/W, 0.052 A/W, and 0.027 A/W, with half-height widths of 22 nm, 25 nm, and 32 nm, respectively. The devised detector encompasses the primary spectral range of visible trichromatic colors, exhibiting a relatively narrow half-height width, indicating superior color purity. These characteristics hold potential for various applications, including the development of hyperspectral cameras and monochromatic single-pixel imaging systems.
Funding
National Defense Basic Scientific Research Program of China (173, 2019-JCJQ-ZD-282-00); National Natural Science Foundation of China (62275192); National Natural Science Foundation of China (61975148).
Disclosures
The authors declare no conflicts of interest.
Data availability
Data underlying the results presented in this paper are not publicly available at this time but may be obtained from the authors upon reasonable request.
Supplemental document
See Supplement 1 for supporting content.
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