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铁电薄膜异质结的光伏效应因具有重要的应用前景而备受关注, 而且其中多种光伏效应机制的共存带来了丰富而复杂的物理内涵. 为了研究界面对光伏效应的重要作用, 制备了基于BiFeO3铁电薄膜的具有“金属/铁电体/半导体”非对称电极结构的Pt/BiFeO3/Nb:SrTiO3异质结, 并系统研究了其在不同波长(365和445 nm)激光照射下的光伏效应. 在365 nm, 74 mW/cm2光照下, 异质结的光伏开路电压高达0.55 V. 而且, 由于光激发和光吸收过程的不同, 365 nm激光照射下该异质结的开路电压和短路电流比445 nm激光照射下的结果显著提高. 随着温度降低, 开路电压单调上升, 而不同波长下的短路电流则表现出不同的变化规律. 另外, 随着光强的提高, 异质结整流效应获得增强, 通过分析, 空间电荷限制电流传导机制对异质结输运有重要贡献, 而光生载流子将通过填充缺陷影响输运特性.The photovoltaic effect of ferroelectric BiFeO3 (BFO)-based heterojunction has been one of hot subjects of theoretical and experimental studies due to its important application prospects, and the coexistence of varieties of photovoltaic effect mechanisms (bulk photovoltaic effect, domain wall effect, interfacial barrier effect, etc.) can bright rich and complicated physics nature. In order to investigate the important role that the interface plays in the photovoltaic effect, we prepare the Pt/BFO(60 nm)/Nb:SrTiO3 (NSTO) heterojunction with an asymmetric metal/ferroelectric/semiconductor structure, and systematically investigate the photovoltaic effect under laser irradiation with different wavelengths (365 nm and 445 nm). The heterojunction exhibits much stronger open-circuit voltage (Voc, ～0.55 V at 74 mW/cm2) and short-circuit current density (Jsc, ～ 208 μA/cm2 at 74 mW/cm2) for the laser irradiation with 365 nm wavelength than those for the laser irradiation with 445 nm wavelength, and the Voc and Jsc are both strengthened with the increase of light intensity. This is because the 365 nm light with the photon energy ～3.4 eV can stimulate photon-induced carriers in both BFO (band gap ～2.7 eV) and NSTO (band gap ～3.2 eV) at both the Pt/BFO interface and the BFO/NSTO interface, while the 445 nm light with the photon energy ～2.8 eV can only generate carriers in BFO. Thus the photovoltaic voltage is much bigger for the 365 nm light. Furthermore, the laser absorption process is much more efficient for the 365 nm light (79% absorbed in BFO and 21% absorbed in NSTO) than for the 445 nm light (21% absorbed in BFO). In addition, the temperature dependent Voc and Jsc are also investigated. It is found that for the 365 nm and 445 nm laser irradiation, the Voc increases with temperature decreasing, which is possibly due to the variations of the built-in potential, concentration of thermal charge carriers, and/or electron-phonon scatterings. The sharper variation of Voc above ～ 200 K may suggest the more significant role of thermal charge carriers at high temperatures. Interestingly, the temperature dependent Jsc behaves differently for the 365 nm and 445 nm light. Under the 365 nm laser irradiation, the Jsc remains almost unchanged below 170 K and increases sharply with temperature increasing above 170 K, which may be related to the dominant role of thermal excitation for the 365 nm light. While for the 445 nm light, the Jsc decreases with temperature increasing, which follows the variation trend of its Voc. What is more, the conduction mechanism of Pt/BFO/NSTO heterojunction under laser irradiation is also studied. It is found that the conduction for the 445 nm light can be nicely described by the space-charge-limited bulk conduction (SCLC) model and the photon-generated carriers may fill the traps and thus leading the transition voltage to decrease. While for the 365 nm light, the conduction is more complicated and cannot be described by the SCLC model. Our findings may be helpful in understanding the photovoltaic effect in transition-metal oxide based heterojunctions and designing photovoltaic devices.
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Keywords:
- photovoltaic effect /
- heterojunction /
- rectification characteristics
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图 1 Pt/BFO/NSTO异质结 (a)样品结构示意图; (b)能带结构示意图
Fig. 1. Pt/BFO/NSTO heterojunction: (a) Schematic illustration; (b) energy band structure diagram.
图 2 (a) BFO/NSTO异质结的XRD测试结果; (b)在2 kHz下测量BFO (200 nm)薄膜的P-E铁电回滞曲线
Fig. 2. (a) XRD pattern of BFO/NSTO heterojunction; (b) P-E hysteresis loop of BFO (200 nm) film measured under 2 kHz.
图 3 室温下, 黑暗及不同光强的光照射下Pt/BFO(60 nm)/NSTO异质结的J-V曲线 (a)波长365 nm光照下的结果; (b)波长445 nm光照下的结果, 插图为低电压区域的放大图像
Fig. 3. J-V curves of Pt/BFO(60 nm)/NSTO heterojunction in the dark and under the laser irradiation with various irradiation intensities at room temperature: (a) λ ～ 365 nm; (b) λ ～ 445 nm. The inset of panel (b) shows the magnified image at low voltages.
图 4 不同波长光照下的(a)开路电压和(b)短路电流密度随着光照强度的变化
Fig. 4. Light intensity dependent (a) open-circuit voltage and (b) short-circuit current density under laser irradiation with different wavelengths.
图 5 (a), (c)不同温度下Pt/BFO/NSTO异质结的J-V曲线; (b), (d)开路电压和短路电流密度随温度的变化; (a), (b) λ ～ 365 nm, 74 mW/cm2; (c), (d) λ ～ 445 nm, 1.56 W/cm2
Fig. 5. (a), (c) Temperature dependent J-V curves of Pt/BFO/NSTO heterojunction under laser irradiation; (b), (d) corresponding temperature dependent open-circuit voltage and short-circuit current density. In (a) and (b), λ ～ 365 nm, 74 mW/cm2; in (c) and (d), λ ～ 445 nm, 1.56 W/cm2.
图 6 Jsc随1000/T的变化及Arrhenius公式拟合
Fig. 6. Jsc vs. 1000/T and the fitting result by Arrhenius model.
图 7 肖特基势垒高度和理想因子随温度的变化 (a) λ ～ 365 nm, 74 mW/cm2; (b) λ ～ 445 nm, 1.56 W/cm2
Fig. 7. Temperature dependent Schottky barrier height and ideal factor: (a) λ ～ 365 nm, 74 mW/cm2; (b) λ ～ 445 nm, 1.56 W/cm2.
图 8 (a)在445 nm光照和不加光时Pt/BFO/NSTO异质结的J-V曲线, 黑色实线是根据SCLC模型拟合的结果; (b) Vtran和
${V'_{{\rm{tran}}}}$ 随光强的变化关系Fig. 8. (a) J-V curves of Pt/BFO/NSTO heterojunction in the dark and under the laser irradiation with different irradiation intensities for 445 nm wavelength. The black solid lines are fitting results by SCLC model. (b) Light intensity dependent Vtran and
${V'_{{\rm{tran}}}}$ . -
[1] Tan Z W, Hong L Q, Fan Z, Tian J J, Zhang L Y, Jiang Y, Hou Z P, Chen D Y, Qin M H, Zeng M, Gao J W, Lu X B, Zhou G F, Gao X S, Liu J M 2019 NPG Asia Mater. 11 20
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Google Scholar
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Google Scholar
[4] Chakrabartty J, Harnagea C, Celikin M, Rosei F, Nechache R 2018 Nat. Photonics 12 271
Google Scholar
[5] Wang J, Ma J, Yang Y B, Chen M F, Zhang J X, Ma J, Nan C W 2019 ACS Appl. Electron. Mater. 1 862
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[14] Fan Z, Yao K, Wang J 2014 Appl. Phys. Lett. 105 162903
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
[27] Feng L, Yang S W, Lin Y, Zhang D L, Huang W C, Zhao W B, Yin Y W, Dong S N, Li X G 2015 ACS Appl. Mater. Interfaces 7 26036
Google Scholar
[28] Huang W C, Liu Y K, Luo Z, Hou C M, Zhao W B, Yin Y W, Li X G 2018 J. Phys. D: Appl. Phys. 51 234005
Google Scholar
[29] Wang X J, Zhou Q, Li H, Hu C, Zhang L L, Zhang Y, Zhang Y H, Sui Y, Song B 2018 Appl. Phys. Lett. 112 122103
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Google Scholar
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Google Scholar
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Google Scholar
[38] Snaith H J, Mende S L, Grätzel M, Chiesa M 2006 Phys. Rev. B 74 045306
Google Scholar
[39] Elumalai N K, Uddin A 2016 Energy Environ. Sci. 9 391
Google Scholar
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Liu E K, Zhu B S, Luo J S 2008 The Physics of Semiconductors (7th Ed.) (Beijing: Publishing House of Electronics Industry) p183 (in Chinese)
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[48] Steiner M A, Geisz J F, Friedman D J, Olavarria W J, Duda A, Moriarty T E 2011 37th IEEE Photovoltaic Specialists Conference (PVSC) Seattle, WA, USA, June 19–24, 2011 p002527
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Google Scholar
[50] Kabulov R R, Matchanov N A, Umarov B R 2018 Appl. Sol. Energy 53 297
Google Scholar
[51] Wu C Y, Chen J F 1982 J. Appl. Phys. 53 3852
Google Scholar
[52] Mihailetchi V D, Koster L J A, Hummelen J C, Blom P W M 2004 Phys. Rev. Lett. 93 216601
Google Scholar
[53] Lee D, Baek S H, Kim T H, Yoon J G, Folkman C M, Eom C B, Noh T W 2011 Phys. Rev. B 84 125305
Google Scholar
[54] Janardhanam V, Lee H K, Shim K H, Hong H B, Lee S H, Ahn K S, Choi C J 2010 J. Alloys Compd. 504 146
Google Scholar
[55] Chang S T, Lee J Y M 2002 Appl. Phys. Lett. 80 655
Google Scholar
[56] Nana R, Gnanachchelvi P, Awaah M A, Gowda M H, Kamto A M, Wang Y, Park M, Das K 2010 Phys. Status Solidi A 207 1489
Google Scholar
[57] Guo Y P, Guo B, Dong W, Li H, Liu H Z 2013 Nanotechnology 24 275201
Google Scholar
[58] Choi T, Lee S, Choi Y J, Kiryukhin V, Cheong S W 2009 Science 324 63
Google Scholar
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