Crosscutting Recombination Metrology for Expediting VOC Engineering

Abstract

Work carried out under this grant addressed the need for improved materials and device characterization of solar cell designs. This experimental program aimed to develop joint electrical and optical studies of solar cells based on the group-II-VI semiconductor CdTe and the chalcogenide semiconductor Cu(InGa)Se2. Electrical measurements focused on temperature (T) and illumination intensity (I) dependence of the open-circuit voltage (VOC), a quantity that plays an important role in conversion efficiency. The VOC depends on temperature and illumination intensity through the energy gap and positions of the quasiFermi levels (QFLs). Optical measurements exploited the illumination and temperature dependence of absolute photoluminescence (PL) intensity (PL-I), a quantity that also depends on the QFL positions. The QFL splitting is a quantity that also depends on recombination rates within the solar cell, including radiative and non-radiative processes. Other factors affect the electrical and optical properties. These include band offsets at both the front and back interfaces of the device active region where electrical contacts are formed. Understanding, locating, and quantifying the recombination properties of the solar cells was the principal goal of this research. Custom simulations were developed to solve continuity and Poisson equations selfconsistently to obtain free-electron and free-hole concentrations. The measurements of temperature and intensity dependent VOC and PL-I allowed the extraction of a number of physical parameters including the conduction band offset, the shunt constant, and the effective capture coefficient for recombination centers, both within the absorber and at the absorber-buffer interface. In addition, the back-contact barrier height is determined from electrical properties. Each of these is discussed in the report. The illumination intensity dependence of VOC and PL-I do not overlap in experiments primarily because PL is not observed in the low-intensity regime where VOC is studied. Absolute PL-I measurements enabled development of an approach directly comparing it with VOC. This in turn allowed development of a simulation capability that would consistently use both measurements, as functions of T and I, for producing a minimization scheme using a differential evolution algorithm. The approach was applied to both CdTe and Cu(InGa)Se2 solar cells each prepared under various conditions. Shunt conductivity, QFL splitting, recombination were measured. Also extensively studied are current-voltage and frequency-dependent capacitance voltage. Work completed under this grant included studies of magnesium zinc oxide (MZO) buffered CdTe solar cells including the effects of hydroiodic acid (HI) treatment. From these studies the recombination rates were quantified at the buffer/absorber (front) interface. The effect of back-contact barrier height was investigated. CdTe solar cells were prepared with CdSe and CdS buffer layers. Lower grain-boundary potential fluctuation, higher back-contact barrier height, and greater bulk recombination were observed in early devices with CdSe buffer layer. Investigations were also carried out into CdS/Cu(InGa)Se2 solar cells. A metal-insulatorsemiconductor capacitance-voltage technique was developed to extract recombinationrelevant properties of the absorber interface. From this work the density of interface states Dit, their capture cross-section σ, fixed charge at the interface Qf, and surface recombination velocity were all extracted.