Predicting Solar Cell Performance from Terahertz and Microwave Spectroscopy

Mobilities and lifetimes of photogenerated charge carriers are core properties of photovoltaic materials and can both be characterized by contactless terahertz or microwave measurements. Here, the expertise from fifteen laboratories is combined to quantitatively model the current voltage characteristics of a solar cell from such measurements. To this end, the impact of measurement conditions, alternate interpretations, and experimental inter laboratory variations are discussed using a Cs,FA,MA Pb I,Br 3 halide perovskite thin film as a case study. At 1 sun equivalent excitation, neither transport nor recombination is significantly affected by exciton formation or trapping. Terahertz, microwave, and photoluminescence transients for the neat material yield consistent effective lifetimes implying a resistance free JV curve with a potential power conversion efficiency of 24.6 . For grainsizes above amp; 8776;20 nm, intra grain charge transport is characterized by terahertz sum mobilities of amp; 8776;32 cm2 V amp; 8722;1 s amp; 8722;1. Drift diffusion simulations indicate that these intra grain mobilities can slightly reduce the fill factor of perovskite solar cells to 0.82, in accordance with the best realized devices in the literature. Beyond perovskites, this work can guide a highly predictive characterization of any emerging semiconductor for photovoltaic or photoelectrochemical energy conversion. A best practice for the interpretation of terahertz and microwave measurements on photovoltaic materials is presente

THz photoconductivity dynamics of semiconductors from sub-nanosecond to millisecond timescales

The pump-probe delay in optical pump, terahertz probe (OPTP) spectroscopy (time-resolved THz spectroscopy) is typically varied using a mechanical delay stage, which limits the delay range to a few nanoseconds. Here we demonstrate an inexpensive modification to typical OPTP setups that extends the range of pump-probe delays to beyond millisecond timescales, whilst retaining the sub-nanosecond resolution required to resolve faster processes that are often present at early times after pulsed optical excitation. We used this new method to investigate the photoconductance dynamics in a range of materials including IIIV semiconductors, metal halide perovskites, germanium and silicon, whose carrier lifetimes range from a few nanoseconds to milliseconds

Terahertz photoconductance dynamics of semiconductors from sub-nanosecond to millisecond timescales

Optical pump terahertz probe spectroscopy (OPTP) is a versatile non-contact technique that measures transient photoconductance decays with femtosecond temporal resolution. However, its maximum temporal range is limited to only a few nanoseconds by the mechanical delay lines used. We extended the temporal range of OPTP to milliseconds and longer while retaining sub-nanosecond resolution. A separate pump laser was electrically synchronized to the probe pulses, allowing the pump–probe delay to be controlled with an electronic delay generator. We demonstrated the capabilities of this technique by examining the photoconductance decays of semiconductors with lifetimes ranging over six orders of magnitude: III-Vs, metal halide perovskites, germanium, and silicon. A direct comparison of results on silicon from OPTP and inductively coupled photoconductance decay highlighted the higher spatial and temporal resolution of OPTP, which allowed in-plane and out-of-plane carrier diffusion to be studied

Approaching the Shockley–Queisser limit for fill factors in lead–tin mixed perovskite photovoltaics

The performance of all solar cells is dictated by charge recombination. A closer to ideal recombination dynamics results in improved performances, with fill factors approaching the limits based on Shockley–Queisser analysis. It is well known that for emerging solar materials such as perovskites, there are several challenges that need to be overcome to achieve high fill factors, particularly for large area lead–tin mixed perovskite solar cells. Here we demonstrate a strategy towards achieving fill factors above 80% through post-treatment of a lead–tin mixed perovskite absorber with guanidinium bromide for devices with an active area of 0.43 cm2. This bromide post-treatment results in a more favorable band alignment at the anode and cathode interfaces, enabling better bipolar extraction. The resulting devices demonstrate an exceptional fill factor of 83%, approaching the Shockley–Queisser limit, resulting in a power conversion efficiency of 14.4% for large area devices