SearcharxivSearch

arXiv subjects

Gabriel J. Man

Publications and source records attributed to Gabriel J. Man.

4 recordsLinked to original sources

Towards a single-junction non-concentrator metal halide perovskite hot carrier solar cell: review of current gaps and opportunities in understanding slow hot carrier cooling

The photovoltaic solar cell is a mature technology, with silicon-based technologies deployed at scale, yet current technologies are limited by the Shockley-Queisser thermodynamic limit, known since the early 1960s. The single-junction non-concentrator hot carrier solar cell operating at ambient temperature - with its theoretically predicted ultimate power conversion efficiency limit of nearly 70% that is twice the Shockley-Queisser limit and is higher than what can be achieved with even n=6 multijunction solar cells - has remained an elusive yet hot research target since the early 1980s. Metal halide perovskite semiconductors were discovered in the late 1970s and photovoltaic applications have been intensively researched and developed since the early 2010s. Current technology development of perovskite solar cells is heavily motivated by their expected cheap processing costs relative to other Shockley-Queisser limited technologies. History has shown that very few absorber materials develop into viable solar cell technologies, and it has been recognized that given the declining costs of silicon-based technologies, a new material must offer potential for both lower cost and higher efficiencies than the Shockley-Queisser limit. Slow cooling of photocarriers with energy in excess of the band edges (hot carriers), which is the first prerequisite of a solar absorbing material for building a hot carrier solar cell technology, has been reported in perovskites since the 2010s. The goal of this review is to illuminate the path towards a single-junction perovskite hot carrier solar cell technology by emphasizing uncertainties in understanding slow hot carrier cooling and recommending approaches to resolve them.

cond-mat.mtrl-sci

Experimentally observed defect tolerance in the electronic structure of lead bromide perovskites

Point defect tolerance in materials, which extends operational lifetime, is essential for societal sustainability, and the creation of a framework to design such properties is a grand challenge in the material sciences. Using three prototypical lead bromide perovskites in single crystal form and high-resolution synchrotron-based X-ray spectroscopy, we reveal the unexpectedly pivotal role of the A-cation in mediating the influence of photoinduced defects. Organic A-cation hydrogen bonding facilitates chemical flexing of the lead-bromide bond that mitigates the self-doping effect of bromide vacancies. The contribution of partially ionic lead-bromide bonding to the electronic band edges, where the bonding becomes more ionic upon the formation of defects, mitigates re-hybridization of the electronic structure upon degradation. These findings reveal two new general design principles for defect tolerance in materials. Our findings uncover the foundations of defect tolerance in halide perovskites and have implications for defect calculations, all beam-based measurements of photophysical properties and perovskite solar cell technology.

cond-mat.mtrl-sci

A-site Cation Influence on the Conduction Band of Lead Bromide Perovskites

Hot carrier solar cells hold promise for exceeding the Shockley-Queisser limit. Slow hot carrier cooling is one of the most intriguing properties of lead halide perovskites and distinguishes this class of materials from competing materials used in solar cells. Here we use the element selectivity of high-resolution X-ray spectroscopy to uncover a previously hidden feature in the conduction band states, the σ-π energy separation, and find that it is strongly influenced by the strength of electronic coupling between the A-cation and bromide-lead sublattice. Our finding provides an alternative mechanism to the commonly discussed polaronic screening and hot phonon bottleneck carrier cooling mechanisms. Our work emphasizes the optoelectronic role of the A-cation, provides a comprehensive view of A-cation effects in the electronic and crystal structures, and outlines a broadly applicable spectroscopic approach for assessing the impact of chemical alterations of the A-cation on halide and potentially non-halide perovskite electronic structure.

cond-mat.mtrl-sci

Electronic Coupling between the Unoccupied States of the Organic and Inorganic Sub-Lattices of Methylammonium Lead Iodide a Hybrid Organic-Inorganic Perovskite Single Crystal

Organic-inorganic halide perovskites have been intensively re-investigated due to their applications, yet the opto-electronic function of the organic cation remains unclear. Through organic-selective resonant Auger electron spectroscopy measurements on well-defined single crystal surfaces, we find evidence for electronic coupling in the unoccupied states between the organic and inorganic sub-lattices of the prototypical hybrid perovskite, which is contrary to the notion based on previous studies that the organic cation is electronically inert. The coupling is relevant for electron dynamics in the material and for understanding opto-electronic functionality.

cond-mat.mtrl-sci