Admittance spectra and drive-level-capacitance profiles of several high performance Cu2ZnSn(Se,S)4 (CZTSSe) solar cells with bandgap ∼1.0–1.5 eV are reported. In contrast to the case for Cu(In,Ga)(S,Se)2, the CZTSSe capacitance spectra exhibit a dielectric freeze out to the geometric capacitance plateau at moderately low frequencies and intermediate temperatures (120–200 K). These spectra reveal important information regarding the bulk properties of the CZTSSe films, such as the dielectric constant and a dominant acceptor with energy level of 0.13–0.2 eV depending on the bandgap. This deep acceptor leads to a carrier freeze out effect that quenches the CZTSSe fill factor and efficiency at low temperatures.
External quantum efficiency and transient photocapacitance (TPC) spectra were obtained for perovskite solar cells with methylammonium lead triiodide perovskite absorbers formed by either dip or vapor conversion. These measurements reveal an extended band of sub-gap states in all of the devices studied. The defect band is best fit by a pair of defects, and the appearance of the defect signal in the transient photocapacitance spectra indicates that at least one of the observed defects is in the perovskite absorber. The cells with the largest density of defect states show the lowest short-circuit current density and open-circuit voltage for slow, quasi-steady-state, current density-voltage sweeps and the largest hysteresis in short-circuit current density for fast sweeps. This suggests that defect states in the perovskite absorber limit steady-state device performance, and that these defects or associated mobile charges play a role in the hysteresis observed in current density-voltage measurements.
Back contacts can significantly limit CdTe solar cell performance, reducing both open circuit voltage (V oc) and fill factor (FF). Copper is an essential component of effective back contacts, but its presence in the CdTe absorber creates detrimental recombination centers. Rapid thermal processing (RTP) is demonstrated as a highly effective approach for reducing back contact barriers in CdTe solar cells contacted with ZnTe:Cu buffer layers, substantially improving both FF (>73%) and V oc (>850 mV). Current density and quantum efficiency remain essentially unchanged, but a five-fold increase in minority carrier lifetime is observed which is attributed to passivation of recombination sites in the back contact region. Quantitative analysis of secondary ion mass spectrometry shows that the majority of Cu segregates to the Au metallization layer and that the ZnTe buffer appears to inhibit the Cu diffusion into CdTe. 3D imaging of the back contact region using atom probe tomography shows that optimized devices are characterized by preferential segregation of copper to both the Au|ZnTe and CdTe|ZnTe interfaces, perhaps in the form of Cu x Te. With its low thermal budget the RTP process has been successfully applied to multiple device architectures. including devices with certified efficiencies in excess of 16%.
Transient photocapacitance (TPC) spectra were obtained on a series of Cu2ZnSn(Se,S)4 absorber devices with varying Se:S ratios, providing bandgaps (Eg) between 1 eV and 1.5 eV. Efficiencies varied between 8.3% and 9.3% for devices with Eg ≤ 1.2 eV and were near 6.5% for devices with Eg ≥ 1.4 eV. The TPC spectra revealed a band-tail region with Urbach energies at or below 18 meV for the first group, but in the 25-30 meV range for the higher band-gap samples. A deeper defect band centered near 0.8 eV was also observed in most samples. We identified a correlation between the Urbach energies and the voltage deficit in these devices.
Oxygenated cadmium sulfide (CdS:O) produced by reactive sputtering has emerged as a promising alternative to conventional CdS for use as the n-type window layer in CdTe solar cells. Here, complementary techniques are used to expose the window layer (CdS or CdS:O) in completed superstrate devices and combined with a suite of materials characterization to elucidate its evolution during high temperature device processing. During device fabrication amorphous CdS:O undergoes significant interdiffusion with CdTe and recrystallization, forming CdS 1-y Te y nanocrystals whose Te fraction approaches solubility limits. Significant oxygen remains after processing, concentrated in sulfate clusters dispersed among the CdS 1-y Te y alloy phase, accounting for ~30% of the post-processed window layer based on cross-sectional microscopy. Interdiffusion and recrystallization are observed in devices with un-oxygenated CdS, but to a much lesser extent. Etching experiments suggest that the CdS thickness is minimally changed during processing, but the CdS:O window layer is reduced from 100 nm to 60-80 nm, which is confirmed by microscopy. Alloying reduces the band gap of the CdS:O window layer to 2.15 eV, but reductions in thickness and areal density improve its transmission spectrum, which is well matched to device quantum efficiency. The changes to the window layer
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