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Abstract
Antimony selenide (Sb2Se3) is a suitable candidate for a broadband photodetector owing to its remarkable optoelectronic properties. Achieving a high-performance self-powered photodetector through a desirable heterojunction still needs more efforts to explore. In this work, we demonstrate a broadband photodetector based on the hybrid heterostructure of Sb2Se3 nanorod arrays (NRAs) absorber and polymer acceptor (P(NDI2OD-T2), N2200). Owing to the well-matched energy levels between N2200 and Sb2Se3, the recombination of photogenerated electrons and holes in N2200/Sb2Se3 hybrid heterostructure is greatly inhibited. The photodetector can detect the wavelength from 405 to 980 nm, and exhibit high responsivity of 0.39 A/W and specific detectivity of 1.84 × 1011 Jones at 780 nm without bias voltage. Meanwhile, ultrafast response rise time (0.25 ms) and fall time (0.35 ms) are obtained. Moreover, the time-dependent photocurrent of this heterostructure-based photodetector keeps almost the same value after the storge for 40 days, indicating the excellent stability and reproducibility. These results demonstrate the potential application of a N2200/Sb2Se3 NRAs heterojunction in visible−near-infrared photodetectors.
© 2023 Optica Publishing Group under the terms of the Optica Open Access Publishing Agreement
1. Introduction
Antimony selenide (Sb2Se3) has emerged as a promising photoelectric material due to its excellent properties, such as low cost, non-toxicity, earth-abundant constituents, decent carrier mobility (∼10 cm2 V-1 S-1), and board spectral response from ultraviolet (UV) to near-infrared region [1,2]. Furthermore, Sb2Se3 possesses a stable orthorhombic phase with quasi-one-dimensional (1D) crystal structure, in which (Sb4Se6)n ribbons stack along the [001] direction through strong covalent Sb-Se bond, making carrier transport in the [001] direction is much easier than that in other directions [3–7], whereas in the [100] and [010] directions, (Sb4Se6)n ribbons are held together by van der Waals forces [6,7]. Consequently, Sb2Se3 demonstrates an extensive application prospect in photovoltaic, photodetector and flexible photoelectron. The power conversion efficiency of Sb2Se3 solar cells increased from < 3% to >10% in the past years [8].
Photodetectors based on Sb2Se3 have been reported recently and applied in many fields, such as heart-rate detection, underwater multispectral computational imaging system, and artificial visual perception nervous system [9–11]. The special 1D crystal structure produces high performance when combing with other materials. For instance, the mixed-dimensional integration of 1D Sb2Se3 with two-dimensional (2D) materials, such as WS2 and β-In2S3, exhibits the remarkably increased photocurrent density and a photoresponsivity as high as 1.51 A/W [12,13]. The formation of heterojunction enables the operation of self-powered photodetectors without an external bias voltage, where the photogenerated carriers are efficiently separated by the built-in field in the junction. Zhao et al. demonstrates a Ga2O3/Sb2Se3 heterojunction photodetector, giving the responsivity and detectivity as high as 9.28 mA/W and 1.23 × 1011 Jones at 0 V bias voltage, respectively, along with the excellent photoresponse speed (the rise/decay time of 834 µs/822 µs) [14]. A boron-doped ZnO/Sb2Se3 NRAs heterojunction based photodetector exhibited outstanding optoelectronic performance in the wavelength range of 460−930 nm at 0 V bias voltage, as well as reached a responsivity of 172.8 mA/W and a specific detectivity of 2.25 × 1011 Jones [15]. Very recently, the detection wavelength was extended to 1650 nm by extrinsic photoconduction, though the extrinsic photoresponse is much lower than the intrinsic photoresponse [16].
On the other hand, the organic-inorganic heterostructure, composed of organic and inorganic material, provides a unique possibility to combine high-performance device with low fabrication cost [17,18]. For example, a visible−blind UV photodetector was designed based on PEDOT: PSS/SnOX/IGZO heterostructure, which exhibited a photoresponsivity of 984 A/W at 320 nm, and a specific detectivity up to 3.3 × 1014 Jones [19]. A self-powered solar-blind photodetector based on PEDOT:PSS/Ga2O3 p-n junction with an ultrahigh responsibility of 2.6 A/W was fabricated [20]. High-performance phenyl-C61-butyric acid methyl easter/Cd3P2 nanowire photodetectors was achieved, covering UV−visible to near-infrared wavelength with high stability and reproductivity [21].
In this work, unlike traditional inorganic heterostructures, we first introduced organic materials (poly{[N, N′-bis(2-octyldodecyl)-naphthalene-1,4,5,8-bis(dicarboximide)-2,6-dyl]-alt-5,5′-(2,2′-dithiophene)}, P(NDI2OD-T2), N2200]) as a n-type material into the p-type Sb2Se3, fabricating a self-powered N2200/Sb2Se3 NRAs heterojunction photodetector. N2200 exhibits a wide absorption behavior even in the near-infrared region, good solubility in organic solvents, excellent chemical stability and high electron mobility [22,23]. In addition, the band alignment between N2200 and Sb2Se3 can effectively separate photogenerated carriers. The formation of N2200/Sb2Se3 organic-inorganic hybrid heterostructure make the self-powered photodetector exhibit an excellent responsivity of 0.39 A/W and a specific detectivity of 1.84 × 1011 Jones at 780 nm, along with the ultrafast response speed at both rise (0.25 ms) and decay (0.35 ms) processes. Thus, this work offers a feasible way to achieve organic-inorganic heterojunction photodetectors with high responsivity, ultrafast response speed and good stability.
2. Experimental section
2.1 Device fabrication
Sb2Se3 NRAs were fabricated in a substrate configuration (window layer/N2200/Sb2Se3 NRAs/MoSe2/Mo/glass). Mo with a thickness of ∼1 µm was prepared by 1200 W direct current magnetron sputtering in 0.3 Pa Ar atmosphere. Subsequently, Mo-coated glass was selenized at 600 °C under Se-containing vacuum chamber to form a very thin MoSe2 layer. Sb2Se3 NRAs were deposited by a closed sublimation technique (CSS) process reported in our previous work [24]. N2200 was dissolved in chlorobenzene at a concentration of 10 mg/mL, spin-coated on Sb2Se3 NRAs at a low speed of 500 rpm for 10 s and a high speed of 3000 rpm for 40 s, respectively, and then placed on a hot plate to dry at 70 °C for 5 mins. A ∼70 nm thick intrinsic zinc oxide (IZO) and a ∼300 nm thick aluminum-doped zinc oxide (AZO) were deposited by radiofrequency magnetron sputtering at room temperature, respectively.
2.2 Characterizations
The surface morphology of the samples was obtained using scanning electron microscopy (SEM) (Nova Nano SEM 450, FEI). Capacitance−voltage (C−V) measurement was performed on Agilent B1500A device in the dark at room temperature. For the measurement of external quantum efficiency (EQE), we used Enlitech QER3011 device equipped with a 150 W xenon lamp (QE-R3018). Atomic force microscope (AFM) and scanning Kelvin probe force microscopy (KPFM) were carried out by using MFP-3D oxford instrument. Energy level information was measured by ultraviolet photoemission spectroscopy (UPS, ESCALAB 250Xi, Thermo Scientific). The photoelectric characteristic of the device was performed on a semiconductor parameter analyzer (Keithley 2400 source meter) and a C-995 optical chopper combined with the semiconductor lasers with different wavelengths (405, 532, 638, 780, 830 and 980 nm). The time-resolved response result was recorded by an oscilloscope (Agilent Technologies DSO-X4022A).
3. Results and discussion
Figure 1(a) illustrates the preparation process of N2200 capped Sb2Se3 NRAs hybrid heterostructure. Firstly, Sb2Se3 nanorod array was grown on Mo-coated glass substrate via a CSS technique, where the Mo layer was deposited by the magnetron sputtering process. N2200 organic layer was deposited on Sb2Se3 nanorod array through spin coating. The thickness of N2200 could be controlled by the concentration of precursor solution and the revolutions per minute (RPM) in the spin coating process. Top transparent conductive oxide (TCO) layer was then deposited by the magnetron sputtering process. Figures 1(b)−d show the cross-sectional SEM images of the as-fabricated Sb2Se3 NRAs, N2200-coated Sb2Se3 NRAs, and the completed TCO/N2200/Sb2Se3 NRAs organic-inorganic hybrid heterostructure device, respectively. As shown in Fig. 1(b), the high-density Sb2Se3 NRAs are distinguishable, uniform, and vertically grown on the Mo-coated glass substrate. The diameter of Sb2Se3 nanorods is in a range of 200−400 nm and the average length of the nanorod is about 2 µm. After the coating of N2200, the surface of Sb2Se3 NRAs was covered with a thin shell (the thickness is ∼15 nm). The magnified SEM image as an inset in Fig. 1(c) reveals that N2200 shell is only on the top end of the nanorod, forming a cap-like coverage, which could provide a high surface area for the p-n interface. From SEM image of the device shown in Fig. 1(d), we can also see that the spaces between Sb2Se3 NRAs are not completely filled by the window layer, which can only be deposited on the top of the nanorod due to the wrapping of N2200.
Fig. 1. (a) Schematic illustration of the preparation process of N2200/Sb2Se3 NRAs heterostructure-based photodetector. Cross-sectional SEM images of (b) Sb2Se3 NRAs fabricated by close-space sublimation, (c) N2200/Sb2Se3 NRAs heterostructure (the inset is an enlarged morphology of the selected area), and (d) the completed device.
The effect of N2200 capping layer on the surface morphology and potential of Sb2Se3 NRAs was investigated by AFM and KPFM measurements. As shown in Figs. 2(a) and 2(b), the root-mean-square (RMS) roughness is estimated to be 161 and 151 nm for the surface of Sb2Se3 NRA before and after the spin-coating of N2200, respectively. It suggests that the coverage of N2200 has a slight effect on the NRAs surface roughness. As shown in Fig. 2(c), the line profiles exhibit very similar evolution for the NRAs surface before and after coating of N2200. As shown in Figs. 2(d) and 2(e), the corresponding surface potential contrast for the N2200-capped Sb2Se3 NRAs is smaller than that of the as-prepared NRAs. The line profiles in Fig. 2(f) reveal that the as-prepared Sb2Se3 NRAs shows a larger potential difference of -1.09 V with a deviation of 80 mV, while the corresponding values for the N2200-capped sample are -0.807 V and 50 mV, respectively. This potential variation indicates that the capping of N2200 could shift up the surface Fermi level, suggesting a formation of N2200/Sb2Se3 NRA heterojunction. UPS measurement was performed to characterize the band structure at N2200/Sb2Se3 interface, and the result is shown in Figure S1 (Supplement 1).
Fig. 2. AFM and scanning KPFM images of (a and d) the as-prepared and (b and e) the N2200-capped Sb2Se3 NRAs. (c) Line profiles of the height measured along the white lines drawn in a and b. (f) Line profiles of the contact potential difference measured along the white lines drawn in d and e.
Figure 3(a) illustrates the energy band diagram of N2200/Sb2Se3 organic-inorganic hybrid heterostructure. The photogenerated carrier can be effectively extracted without any transport barrier. The lowest unoccupied molecular orbital (LUMO) of N2200 is lower than the conduction band (CB) of Sb2Se3, the electrons in CB of Sb2Se3 can be directly transferred to the LUMO of N2200 when visible light is absorbed to generate electron-hole pairs in Sb2Se3. On the other hand, because the highest occupied molecular orbital (HOMO) of N2200 is lower than the valence band (VB) of Sb2Se3, the photoexcited holes in the former can be easily injected into the latter. Capacitance−voltage (C−V) (Figure S2) measurement was applied to explore the built-in potential (Vbi) for the device. Vbi, obtained from the horizontal intercepts, is estimated to be 0.32 V, which enables an effective separation of photogenerated carriers and then reduces the charge accumulation at the N2200/Sb2Se3 interface. Thus, the heterojunction is expected to exhibit a pronounced photoresponse without bias voltage.
Fig. 3. (a) Schematic diagram of energy band of N2200/Sb2Se3 NRAs heterojunction. (b) Schematic illustration of the configuration for photoelectric property measurement. (c) Dark I−V characteristic curve of N2200/Sb2Se3 NRAs heterojunction photodetector. (d) I−V characteristics of the photodetector measured under light illumination of different wavelengths. (e) Time-dependent photocurrent response of the photodetector under different wavelengths with a power intensity of 12.74 mW/cm2 at 0 V bias voltage.
Figure 3(c) exhibits a typical current−voltage (I−V) characteristic curve of N2200/Sb2Se3 NRAs heterojunction photodetector in the dark. The device displays the obvious diode characteristics with a rectification ratio of 8.7 at ±1 V and a leakage current of 9 nA, which may be attributed to the cap-like interface. We infer that it could avoid the contact between TCO and back electrode, and result in less leakage current for the device. Dark I−V curve is fitted by using the following standard diode equation:
I−V characteristics of the photodetector in the visible to near-infrared region were investigated under the laser illumination of different wavelengths, as shown in Fig. 3(d). The curves under light illumination could not pass the zero point, which verifies that the device can function as a self-driven photodetector without an external bias. It is well-known that EQE response is mainly due to the sufficient generation and collection of carriers, and the transport and recombination of carriers generated in the absorber layer are significantly influenced by the rear surface and interface properties [27]. Thus, as compared with the previous report [9], the lower EQE shown in Supplement 1, Fig. S3 is probably due to the defects at N2200/Sb2Se3 interface. It would lead to carrier recombination and suppress carrier transport and collection, which is the main obstacle for the performance of organic-inorganic heterojunction devices.
Figure 3(e) demonstrates the photocurrent switching behavior of N2200/Sb2Se3 NRAs heterojunction photodetector under light illumination of different wavelengths, where the pulsed light was generated by a mechanical chopper (Fig. 3(b)). It is clearly seen that the photocurrent first increases with increasing the wavelength from 405 to 780 nm, and then decreases at the longer wavelength (780−980 nm), which is consistent with the tendency of the spectral response shown in Figure S3. It indicates that the N2200/Sb2Se3 NRA heterojunction can be operated in a wide wavelength range.
To further characterize the photoelectric performance of N2200/Sb2Se3 NRA heterostructure-based photodetector, 780 nm laser was chosen to explore the photosensitivity dependence on light intensity. Figure 4(a) displays the I−V characteristics under 780 nm laser illumination with an incident light intensity varying from 0.06 to 51.21 mW/cm2. It is found that the photocurrent increases with increasing the light intensity within the measurement range. This notable dependence suggests a high sensitivity of the device to the red light. Figure 4(b) shows the photocurrent (Jphoto) versus light intensity (P) without bias voltage. The relationship between Jphoto and P can be described by the power law:
where A is a constant at the specific wavelength, and θ is a parameter related to the carrier trapping and recombination process in the photodetector. Fitting the plot of Fig. 4(b) by using Eq. (2), θ of 0.76 is obtained. Additionally, θ is determined to be 0.71−0.92 in Supplement 1, Fig. S4. The deviation from the ideal slope of θ = 1 is attributed to the carrier generation, trapping, and recombination processes in the N2200/Sb2Se3 NRA heterostructure [28]. Responsivity (R) and specific detectivity (D*) are calculated by the following equations:Fig. 4. (a) I−V characteristics curves of the heterojunction photodetector measured under dark and 780 nm laser illumination with different light intensities. (b) Light intensity-dependent photocurrent of the photodetector under 780 nm laser illumination, fitted by a power law. (c) Light intensity-dependent responsivity (black curve) and detectivity (blue curve) of the photodetector. (d−e) Time-dependent photovoltage of the photodetector under different pulsed light illumination. (f) Rise and decay time curve of the photodetector.
The response speed is also one of the key figures of merits for a photodetector. In this work, the response speed of N2200/Sb2Se3 NRAs organic-inorganic heterojunction was investigated by monitoring the variation of photovoltage under the pulsed incident light, which was generated by using an optical chopper with the varied frequency from 4 to 800 Hz. As shown in Figs. 4(d) and 4(e), the photodetector exhibits a fast response speed with excellent repeatability and stability in the frequency range of 4−800 Hz. Moreover, the rise and decay times which can be defined as the times required to reach 90% and drop to 10% of the maximum photovoltage [5,35,36], are determined to be 0.25 and 0.35 ms, respectively, as shown in Fig. 4(f).
The operational stability is crucial to the practical application of a photodetector. We further investigate the photocurrent switching performance of the photodetector after storage in ambient conditions (∼25 °C, 55% relative humidity) for 40 days, as demonstrated in Fig. 5. It is noteworthy that the photodetector based on N2200/Sb2Se3 heterojunction exhibits an excellent stability and reproducibility in air, without the dominant degradation. For an organic-inorganic hybrid device, its stability is mainly dependent on the organic material. The hydrophobic and entangling aliphatic side chains of N2200 ensure a sufficient resistance to moisture. Hence N2200 has been widely used in fabricating various optoelectronic devices [37–39], which exhibited good ambient stability. In this work, Sb2Se3 with the narrow band gap and high carrier mobility is combined with N2200 with the wide absorption range to construct a visible−near-infrared photodetector. The proper energy level alignment between Sb2Se3 and N2200 is favorable for the transport of photogenerated carriers without an external bias. Meanwhile, the built-in potential of the hybrid heterostructure can effectively separate the photogenerated carriers, reduce the charge accumulation at the interface, and further improve the photoelectric characteristics. In view of the above results, it can be inferred that N2200/Sb2Se3 NRAs is an efficient multipurpose heterojunction for photodetector in the future.
Fig. 5. Time-dependent photocurrent of the photodetector with on/off switching under 780 nm laser illumination with a power intensity of 3.83 mW/cm2 after storage for 40 days.
4. Conclusion
In summary, we designed and fabricated a self-powered photodetector based on N2200/Sb2Se3 NRAs organic-inorganic heterostructure. The photodetector exhibits excellent photoresponse behavior in a wide wavelength range from 405−980 nm without an external bias voltage. Benefiting from the strong absorption and the appropriate band alignment of high-quality heterostructure between Sb2Se3 and N2200, the photodetector achieves the extremely high responsivity and detectivity (0.39 A/W and 1.84 × 1011 Jones), and ultrafast response speed (τrise = 0.25 ms, and τfall = 0.35 ms). Furthermore, a good operation stability and reproducibility of this heterojunction photodetector is demonstrated. Our findings in this work afford a feasible pathway to develop the device with impressive broadband photodetection performance.
Funding
Natural Science Foundation of Hebei Province (A2021201038); Scientific Research Foundation of Hebei Province for the Returned Overseas Chinese Scholars (C20220308); Project for the Cultivation of Scientific and Technological Innovation Ability of College and Middle School Students (22E50035D).
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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