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Register a new userPitfalls and prospects of optical spectroscopy to characterize perovskite-transport layer interfaces
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Perovskite photovoltaics has witnessed an unprecedented increase in power conversion efficiency over the last decade. The choice of transport layers, through which photo-generated electrons and holes are transported to the electrodes, is a crucial factor for further improving both the device performance and stability. In this perspective, we critically examine the application of optical spectroscopy to characterize the quality of the transport layer-perovskite interface. We highlight the power of complementary studies that use both continuous wave (cw) and time-resolved photoluminescence (PL) to understand non-radiative losses, and additional transient spectroscopies for characterizing the potential for loss-less carrier extraction at the solar cell interfaces. Based on this discussion, we make recommendations on how to extrapolate results from optical measurements to assess the quality of a transport layer, and its impact on solar cell efficiency.
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Charge transport layers (CTLs) are key components of diffusion controlled perovskite solar cells, however, they can induce additional non-radiative recombination pathways which limit the open circuit voltage (V_OC) of the cell. In order to realize the full thermodynamic potential of the perovskite absorber, both the electron and hole transport layer (ETL/HTL) need to be as selective as possible. By measuring the quasi-Fermi level splitting (QFLS) of perovskite/CTL heterojunctions, we quantify the non-radiative interfacial recombination current for a wide range of commonly used CTLs, including various hole-transporting polymers, spiro-OMeTAD, metal oxides and fullerenes. We find that all studied CTLs limit the V_OC by inducing an additional non-radiative recombination current that is significantly larger than the loss in the neat perovskite and that the least-selective interface sets the upper limit for the V_OC of the device. The results also show that the V_OC equals the internal QFLS in the absorber layer of (pin, nip) cells with selective CTLs and power conversion efficiencies of up to 21.4%. However, in case of less selective CTLs, the V_OC is substantially lower than the QFLS which indicates additional losses at the contacts and/or interfaces. The findings are corroborated by rigorous device simulations which outline several important considerations to maximize the V_OC. This work shows that the real challenge to supress non-radiative recombination losses in perovskite cells on their way to the radiative limit lies in the suppression of carrier recombination at the perovskite/CTL interfaces.
Among the n-type metal oxide materials used in the planar perovskite solar cells, zinc oxide (ZnO) is a promising candidate to replace titanium dioxide (TiO2) due to its relatively high electron mobility, high transparency, and versatile nanostructures. Here, we present the application of low temperature solution processed ZnO/Al-doped ZnO (AZO) bilayer thin film as electron transport layers (ETLs) in the inverted perovskite solar cells, which provide a stair-case band profile. Experimental results revealed that the power conversion efficiency (PCE) of perovskite solar cells were significantly increased from 12.25 to 16.07% by employing the AZO thin film as the buffer layer. Meanwhile, the short-circuit current density (Jsc), open-circuit voltage (Voc), and fill factor (FF) were improved to 20.58 mA/cm2, 1.09V, and 71.6%, respectively. The enhancement in performance is attributed to the modified interface in ETL with stair-case band alignment of ZnO/AZO/CH3NH3PbI3, which allows more efficient extraction of photogenerated electrons in the CH3NH3PbI3 active layer. Thus, it is demonstrated that the ZnO/AZO bilayer ETLs would benefit the electron extraction and contribute in enhancing the performance of perovskite solar cells.
Transparent conductors-nearly an oxymoron-are in pressing demand, as ultra-thin-film technologies become ubiquitous commodities. As current solutions rely on non-abundant elements, perovskites such as SrVO3 and SrNbO3 have been suggested as next generation transparent conductors. Our ab-initio calculations and analytical insights show, however, that reducing the plasma frequency below the visible spectrum by strong electronic correlations-a recently proposed strategy-unavoidably comes at a price: an enhanced scattering and thus a substantial optical absorption above the plasma edge. As a way out of this dilemma we identify several perovskite transparent conductors, relying on hole doping, somewhat larger bandwidths and separations to other bands.
Although the structural phase transitions in single-crystal hybrid methyl-ammonium (MA) lead halide perovskites (MAPbX3, X = Cl, Br, I) are common phenomena, they have never been observed in the corresponding nanocrystals. Here we demonstrate that two-photon-excited photoluminescence (PL) spectroscopy is capable of monitoring the structural phase transitions in MAPbX3 nanocrystals because nonlinear susceptibilities govern the light absorption rates. We provide experimental evidence that the orthorhombic-to-tetragonal structural phase transition in a single layer of 20-nm-sized 3D MAPbBr3 nanocrystals is spread out within the 70 - 140 K range. This structural phase instability range arises because, unlike in single-crystal MAPbX3, free rotations of MA ions in the corresponding nanocrystals are no longer restricted by a long-range MA dipole order. The resulting configurational entropy loss can be even enhanced by the interfacial electric field arising due to charge separation at the MAPbBr3/ZnO heterointerface, extending the orthorhombic-to-tetragonal structural phase instability range from 70 to 230 K. We conclude that the weak sensitivity of conventional one-photon-excited PL spectroscopy to the structural phase transitions in 3D MAPbX3 nanocrystals results from the structural phase instability providing negligible distortions of PbX6 octahedra. In contrast, the intensity of two-photon-excited PL and electric-field-induced one-photon-excited PL still remains sensitive enough to weak structural distortions due to the higher rank tensor nature of nonlinear susceptibilities involved. We also show that room-temperature PL originates from the radiative recombination of the optical-phonon vibrationally excited polaronic quasiparticles with energies might exceed the ground-state Frohlich polaron and Rashba energies due to optical-phonon bottleneck.
Spin backflow and spin-memory loss have been well established to considerably lower the interfacial spin transmissivity of metallic magnetic interfaces and thus the energy efficiency of spin-orbit torque technologies. Here we report that spin backflow and spin-memory loss at Pt-based heavy metal/ferromagnet interfaces can be effectively eliminated by inserting an insulating paramagnetic NiO layer of optimum thickness. The latter enables the thermal magnon-mediated essentially unity spin-current transmission at room temperature due to considerably enhanced effective spin-mixing conductance of the interface. As a result, we obtain dampinglike spin-orbit torque efficiency per unit current density of up to 0.8 as detected by the standard technology ferromagnet FeCoB and others, which reaches the expected upper-limit spin Hall ratio of Pt. We establish that Pt/NiO and Pt-Hf/NiO are two energy-efficient, integration-friendly, and high-endurance spin-current generators that provide >100 times greater energy efficiency than sputter-deposited topological insulators BiSb and BiSe. Our finding will benefit spin-orbitronic research and advance spin-torque technologies.
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