Mathias Mews

Monolithic perovskite/silicon-heterojunction tandem solar cells processed at low temperature

Tandem solar cells combining silicon and perovskite absorbers have the potential to outperform state-of-the-art high efficiency silicon single junction devices. However, the practical fabrication of monolithic silicon/perovskite tandem solar cells is challenging as material properties and processing requirements such as temperature restrict the device design. Here, we fabricate an 18% efficient monolithic tandem cell formed by a silicon heterojunction bottom- and a perovskite top-cell enabling a very high open circuit voltage of 1.78 V. The monolithic integration was realized via low temperature processing of the semitransparent perovskite sub-cell where an energetically aligned electron selective contact was fabricated by atomic layer deposition of tin oxide. The hole selective, transparent top contact was formed by a stack of the organic hole transport material spiro-OMeTAD, molybdenum oxide and sputtered indium tin oxide. The tandem cell design is currently limited by the photocurrent generated in the silicon bottom cell that is reduced due to reflectance losses. Based on optical modelling and first experiments, we show that these losses can be significantly reduced by combining optical optimization of the device architecture including light trapping approaches.

Hydrogen plasma treatments for passivation of amorphous-crystalline silicon-heterojunctions on surfaces promoting epitaxy

The impact of post-deposition hydrogen plasma treatment (HPT) on passivation in amorphous/crystalline silicon (a-Si:H/c-Si) interfaces is investigated. Combining low temperature a-Si:H deposition and successive HPT, a high minority carrier lifetime >8 ms is achieved on c-Si 〈100〉, which is otherwise prone to epitaxial growth and thus inferior passivation. It is shown that the passivation improvement stems from diffusion of hydrogen atoms to the heterointerface and subsequent dangling bond passivation. Concomitantly, the a-Si:H hydrogen density increases, leading to band gap widening and void formation, while the film disorder is not increased. Thus, HPT allows for a-Si:H band gap and a-Si:H/c-Si band offset engineering.The impact of post-deposition hydrogen plasma treatment (HPT) on passivation in amorphous/crystalline silicon (a-Si:H/c-Si) interfaces is investigated. Combining low temperature a-Si:H deposition and successive HPT, a high minority carrier lifetime >8 ms is achieved on c-Si 〈100〉, which is otherwise prone to epitaxial growth and thus inferior passivation. It is shown that the passivation improvement stems from diffusion of hydrogen atoms to the heterointerface and subsequent dangling bond passivation. Concomitantly, the a-Si:H hydrogen density increases, leading to band gap widening and void formation, while the film disorder is not increased. Thus, HPT allows for a-Si:H band gap and a-Si:H/c-Si band offset engineering.

Valence band alignment and hole transport in amorphous/crystalline silicon heterojunction solar cells

To investigate the hole transport across amorphous/crystalline silicon heterojunctions, solar cells with varying band offsets were fabricated using amorphous silicon suboxide films. The suboxides enable good passivation if covered by a doped amorphous silicon layer. Increasing valence band offsets yield rising hole transport barriers and reduced device efficiencies. Carrier transport by thermal emission is reduced and tunnel hopping through valence band tail states increases for larger barriers. Nevertheless, stacks of films with different band gaps, forming a band offset staircase at the heterojunction, could allow the application of these layers in silicon heterojunction solar cells.

Valence band offset in heterojunctions between crystalline silicon and amorphous silicon (sub)oxides (a-SiOx:H, 0 < x < 2)

The heterojunction between amorphous silicon (sub)oxides (a-SiOx:H, 0  4 eV for the a-SiO2/c-Si interface, while the electronic quality of the heterointerface deteriorates. High-bandgap a-SiOx:H is therefore unsuitable for the hole contact in heterojunction solar cells, due to electronic transport hindrance resulting from the large ΔEV. Our method is readily applicable to other heterojunctions.

Potential of PEDOT:PSS as a hole selective front contact for silicon heterojunction solar cells

We show that the highly conductive polymer poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS) can successfully be applied as a hole selective front contact in silicon heterojunction (SHJ) solar cells. In combination with a superior electron selective heterojunction back contact based on amorphous silicon (a-Si), mono-crystalline n-type silicon (c-Si) solar cells reach power conversion efficiencies up to 14.8% and high open-circuit voltages exceeding 660 mV. Since in the PEDOT:PSS/c-Si/a-Si solar cell the inferior hybrid junction is determining the electrical device performance we are capable of assessing the recombination velocity (vI) at the PEDOT:PSS/c-Si interface. An estimated vI of ~400 cm/s demonstrates, that while PEDOT:PSS shows an excellent selectivity on n-type c-Si, the passivation quality provided by the formation of a native oxide at the c-Si surface restricts the performance of the hybrid junction. Furthermore, by comparing the measured external quantum efficiency with optical simulations, we quantify the losses due to parasitic absorption of PEDOT:PSS and reflection of the device layer stack. By pointing out ways to better passivate the hybrid interface and to increase the photocurrent we discuss the full potential of PEDOT:PSS as a front contact in SHJ solar cells.

Solution-processed amorphous silicon surface passivation layers

Amorphous silicon thin films, fabricated by thermal conversion of neopentasilane, were used to passivate crystalline silicon surfaces. The conversion is investigated using X-ray and constant-final-state-yield photoelectron spectroscopy, and minority charge carrier lifetime spectroscopy. Liquid processed amorphous silicon exhibits high Urbach energies from 90 to 120 meV and 200 meV lower optical band gaps than material prepared by plasma enhanced chemical vapor deposition. Applying a hydrogen plasma treatment, a minority charge carrier lifetime of 1.37 ms at an injection level of 1015/cm3 enabling an implied open circuit voltage of 724 mV was achieved, demonstrating excellent silicon surface passivation.

In-system photoelectron spectroscopy study of tin oxide layers produced from tetrakis(dimethylamino)tin by plasma enhanced atomic layer deposition

Tin oxide (SnO2) layers were deposited using plasma enhanced atomic layer deposition with tetrakis(dimethylamino)tin precursor and oxygen plasma. The deposited layers were analyzed by spectral ellipsometry, conductivity measurements, and in-system photoelectron spectroscopy. Within a deposition temperature range of 90–210 °C, the resistivity of the SnO2 layers decreases by 5 orders of magnitude with increasing deposition temperature. At the same time, the refractive index at 632.8 nm increases from 1.7 to 1.9. These changes in bulk layer properties are connected to results from photoelectron spectroscopy. It is found that decreasing carbon and nitrogen contaminations in the tin oxide layers lead to decreasing optical band gaps and increasing refractive index. Additionally, for the deposited SnO2 layers, a shoulder in the O 1s core level spectrum is observed that decreases with the deposition temperature and thus is proposed to be related to hydroxyl groups.

Electronic structure of indium-tungsten-oxide alloys and their energy band alignment at the heterojunction to crystalline silicon

The electronic structure of thermally co-evaporated indium-tungsten-oxide films is investigated. The stoichiometry is varied from pure tungsten oxide to pure indium oxide, and the band alignment at the indium-tungsten-oxide/crystalline silicon heterointerface is monitored. Using in-system photoelectron spectroscopy, optical spectroscopy, and surface photovoltage measurements, we show that the work function of indium-tungsten-oxide continuously decreases from 6.3 eV for tungsten oxide to 4.3 eV for indium oxide, with a concomitant decrease in the band bending at the hetero interface to crystalline silicon than indium oxide.

Aluminium metallisation for interdigitated back-contact silicon heterojunction solar cells

Back-contact silicon heterojunction solar cells with an efficiency of 22% were manufactured, featuring a simple aluminium metallisation directly on the doped amorphous silicon films. Both the open-circuit voltage and the fill factor heavily depend on the parameters of the annealing step after aluminium layer deposition. Using numerical device simulations and in accordance with the literature, we demonstrate that the changes in solar cell parameters with annealing can be explained by the formation of an aluminium silicide layer at temperatures as low as 150 degrees C, improving the contact resistance and thus enhancing the fill factor. Further annealing at higher temperatures initialises the crystallisation of the amorphous silicon layers, yielding even lower contact resistances, but also introduces more defects, diminishing the open-circuit voltage.

Interdigitated back contact silicon heterojunction solar cells: Towards an industrially applicable structuring method

We report on the investigation and comparison of two different processing approaches for interdigitated back contacted silicon heterojunction solar cells: our photolithography-based reference procedure and our newly developed shadow mask process. To this end, we analyse fill factor losses in different stages of the fabrication process. We find that although comparably high minority carrier lifetimes of about 4 ms can be observed for both concepts, the shadow masked solar cells suffer yet from poorly passivated emitter regions and significantly higher series resistance. Approaches for addressing the observed issues are outlined and first solar cell results with efficiencies of about 17 % and 23 % for shadow masked and photolithographically structured solar cells, respectively, are presented.