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The ability to characterise perovskite phases non-destructively is key on the route to ensuring their long-term stability in operando. Raman spectroscopy holds the promise to play an important role in this task. Among all perovskites, formamidinium lead iodide (FAPbI3) has emerged as one of the most promising candidates for single-junction photovoltaic cells. However, Raman spectroscopy of FAPbI3 remains challenging as is evidenced by conflicting reports in the literature. Here, we demonstrate that due to the vulnerability of FAPbI3 to laser-induced degradation, the detected Raman spectrum depends strongly on the experimental conditions. This can lead to conflicting results and is revealed as the origin of discrepancies in the literature. We overcome this issue by deploying defocused Raman spectroscopy, preventing laser-induced damage to the sample and simultaneously improving the signal-to-noise ratio, allowing us to furthermore resolve much weaker Raman modes than was previously possible. We offer step-by-step instructions on how to apply this technique to a given spectrometer. Non-destructive characterisation of the FAPbI3 phases further enables us to quantify the phase stability of pristine FAPbI3 crystals and FAPbI3 grown with the high-performance additive methylenediammonium chloride (MDACl2). This shows that the neat crystals fully degrade within two weeks, whereas in samples grown with the additive only about 2% of the crystal bulk is in the δ-phase after 400 days. This establishes defocused Raman spectroscopy as a powerful tool for the characterisation of FAPbI3 and other perovskite materials. [ABSTRACT FROM AUTHOR]

We introduce 2,3,8,9,14,15-hexachloro-5,6,11,12,17,18-hexaazatrinaphthylene (HATNA-Cl6) as n-dopable electron transport material (ETM) for small molecule organic solar cells. Because of its large optical energy gap of 2.7 eV and its well suited energy level positions, the material can be implemented as a semitransparent spacer layer between the reflecting metal contact and the photoactive C60 acceptor layer in p-i-n type solar cells. By varying the ETM thickness, it is possible to shift the position of the photoactive area with respect to the interference maximum of the optical field distribution. Applying n-HATNA-Cl6 instead of the parasitically absorbing reference ETM n-C60 results in a considerably improved photocurrent density and accordingly in a higher efficiency. At dETM=100 nm the power conversion efficiency is more than doubled as it increases from (100 nm n-C60) = 0.5% to (100 nm n-HATNA-Cl6) = 1.1%. [ABSTRACT FROM AUTHOR]

A key feature of stacked organic solar cells is an efficient recombination contact at the interface between the solar cells in the stack. Here, an electron current has to be converted into a hole current without loss of energy. Furthermore, the recombination contact has to be highly transparent. We present a new approach for small molecule organic solar cells using highly doped organic layers. Our approach adapts the use of tunnel diodes known from inorganic tandem solar cells. We compare a metal cluster based recombination contact reported in literature to the new approach using different organic tandem solar cell structures. For this purpose, current-voltage characteristics of adequate solar cells are measured. The experiments show that highly doped layers as recombination contacts in tandem organic solar cells are superior to the metal cluster based approach. The proposed concept allows an addition of the open circuit voltages of the subcells of a tandem solar cell, without absorption or reflection at the recombination contact. The results further show that our concept does not depend on the specific choice of materials as it is seen for metal cluster based recombination contacts. It therefore represents a general approach which is compatible to mass manufacturing. [ABSTRACT FROM AUTHOR]

We present metal multilayers consisting of aluminum and silver in different combinations serving as semitransparent top contacts for organic solar cells. Scanning electron microscopy, atomic force microscopy, and optical spectroscopy are used to illustrate how ultrathin Al interlayers influence the morphology of Ag layers evaporated on top of organic materials and how closed layers with good conductivity can be achieved. Multilayer metal contacts are used to fabricate top-illuminated small-molecule organic solar cells (SM-OSCs) which reach efficiencies comparable to conventional SM-OSCs that employ tin-doped indium oxide as electrode. It is shown that combinations of Al and Au lead to similar results, suggesting a similar mechanism for the influence on morphological development of both Ag and Au. [ABSTRACT FROM AUTHOR]

The aim of this article is to investigate the origin of the open circuit voltage (Voc) in organic heterojunction solar cells. The studied devices consist of buckminsterfullerene C60 as acceptor material and an oligophenyl-derivative 4,4′-bis-(N,N-diphenylamino)quaterphenyl (4P-TPD) as donor material. These photoactive materials are sandwiched between indium tin oxide and p-doped hole transport layers. Using two different p-doped hole transport layers, the built-in voltage of the solar cells is independently changed from the metal contacts. The influence of the built-in voltage on the Voc is investigated in bulk and planar heterojunctions. In bulk heterojunctions, in which doped transport layers border directly on the photoactive blend layer, Voc cannot exceed the built-in voltage significantly. Though, in planar heterojunctions, Voc is identical with the splitting of quasi-Fermi levels at the donor-acceptor interface and is thus primarily determined by the difference of the lowest unoccupied molecular orbital of C60 and the highest occupied molecular orbital of 4P-TPD. In planar heterojunctions, the open circuit voltage can exceed the built-in voltage. Furthermore, the investigations show that the efficiency of organic solar cells can be improved by using p-doped charge transport layers with optimized energy level alignment to the active materials. The optimized planar heterojunction shows a fill factor of up to 65.5% and a Voc of 0.95 V. For solar cells with insufficient energy level alignment between the photoactive layer system and the hole transport layer, a reduced Voc in bulk heterojunction cells and a characteristic S shape of the I-V characteristics in planar heterojunction cells are observed. [ABSTRACT FROM AUTHOR]

The implementation of proper charge carrier transport materials in p-i-n type organic solar cells strongly influences the device performance. Our investigation focuses on the substitution of the standard layer sequence used at the side of electron transport, usually consisting of either C60/exciton blocking layer/metal or n-C60/metal by a layer sequence including a window layer. Here, we evaluate the transparent electron transport material 1,4,5,8-naphthalenetetracarboxylic dianhydride (NTCDA), which guarantees a loss free charge extraction from the active materials due to a good energy level alignment as well as exciton blocking due to its wide bandgap. It is demonstrated that upon the exchange of the electron transport layer n-C60 for n-NTCDA, the solar power conversion efficiency of a p-i-n device can be increased by 10%. [ABSTRACT FROM AUTHOR]

A nondestructive method for assessing the thickness of the photoactive layer in poly(3-hexyl-thiophene):1-(3-methoxy-carbonyl)propyl-1-phenyl-(6,6)C61 (P3HT:PCBM) solar cells is reported. In the approach the absorption spectrum of the solar cell as derived by optical simulations is fitted to the corresponding measured spectrum, varying only the P3HT:PCBM layer thickness. Within the 50–250 nm thickness range, a linear correlation between the position of a certain spectral minimum and the P3HT:PCBM layer thickness is shown, based on simulated absorption spectra. As an initial application, absorption spectra for 240 P3HT:PCBM solar cells prepared at four different spin-coating speeds were recorded, and the average P3HT:PCBM layer thickness estimated for each spin-coating speed. The simulated fraction of light absorbed in the P3HT:PCBM layer of the solar cells is compared with the P3HT:PCBM absorption spectra measured for films spin coated on simpler substrate types. The latter spectra cannot account for the light harvested in the photoactive layer of P3HT:PCBM solar cells because of substantial optical interference in the solar cells. The measured short circuit current densities Jsc for the solar cells vary with the spin-coating speed in a manner confirmed by optical simulations of the maximal short circuit current densities. The measured efficiencies follow the same pattern. On average the measured Jsc is 1–2 mA/cm2 below the simulated maximal short circuit current densities. Based on the resemblance of the measured and simulated absorption spectra such difference can be attributed to recombination exclusively. [ABSTRACT FROM AUTHOR]

A nondestructive method is described for assessing the thickness of the photoactive layer in poly(3-hexyl-thiophene):1-(3-methoxy-carbonyl)propyl-1-phenyl-(6,6)[C.sub.61] (P3HT:PCBM) solar cells. The studies have showed that the blend layer thickness of a P3HT:PCBM solar cell can be deduced from its absorption spectrum.

Interfaces between organic electron-donating (D) and electron-accepting (A) materials have the ability to generate charge carriers on illumination. Efficient organic solar cells require a high yield for this process, combined with a minimum of energy losses. Here, we investigate the role of the lowest energy emissive interfacial charge-transfer state (CT1) in the charge generation process. We measure the quantum yield and the electric field dependence of charge generation on excitation of the charge-transfer (CT) state manifold via weakly allowed, low-energy optical transitions. For a wide range of photovoltaic devices based on polymer:fullerene, small-molecule:C60 and polymer:polymer blends, our study reveals that the internal quantum efficiency (IQE) is essentially independent of whether or not D, A or CT states with an energy higher than that of CT1 are excited. The best materials systems show an IQE higher than 90% without the need for excess electronic or vibrational energy. [ABSTRACT FROM AUTHOR]