Solar energy storage and conversion is a key technology for the future realization of a sustainable energy production worldwide. The utilization of low-energy photons by means of upconversion (UC) processes has the main advantage of the upconversion process and solar energy-harvesting devices being considered and optimized independently, without affecting the particular physical characteristics of the operating sunlight excited material or device architectures. The UC-device must function efficiently with noncoherent light excitation, under light intensities comparable with those obtainable from moderate concentrated sunlight (1 to 20 suns, AM1.5); such a low degree of concentration allows usage of Fresnel-type focusing systems. We report chemical synthesis and efficient functioning of a triplet–triplet annihilation upconversion-based device, harvesting the entire deep-red spectral range of the sun irradiation (Δλ∼142  nm) in a gap-free manner.

Improving efficiency of triplet–triplet annihilation-based photon upconversion (TTA-UC) in crystalline media is challenging because it usually suffers from the severe aggregation of the donor (sensitizer) molecules in acceptor (emitter) crystals. We show a kinetically controlled crystal growth approach to improve donor dispersibility in acceptor crystals. As the donor–acceptor combination, a benchmark pair of platinum(II) octaethylporphyrin (PtOEP) and 9,10-diphenylanthracene (DPA) is employed. A surfactant-assisted reprecipitation technique is employed, where the concentration of the injected PtOEP–DPA solution holds the key to control dispersibility; at a higher PtOEP–DPA concentration, a rapid crystal growth results in better dispersibility of PtOEP molecules in DPA crystals. The improvement of donor dispersibility significantly enhances the TTA-UC quantum yield. Thus, the inherent function of donor-doped acceptor crystals can be maximized by controlling the crystallization kinetics.

It is well known that the rate and efficiency of photon upconversion via triplet–triplet annihilation (TTA-UC) are strongly dependent on the energetics of the sensitizer and acceptor molecules. In rigid scaffoldings, where the dyes are fixed in position, the structure and orientation of the molecules also presumably play an important role. We investigate how the variation in the position of the phosphonate surface binding group on 9,10-diphenylanthracene influences TTA-UC in self-assembled bilayers on ZrO2. Interestingly, meta- or para-substitution of the anthracene dye with phosphonate groups had minimal influence on their energetics, surface loadings, or sensitizer to acceptor triplet energy transfer efficiency. However, the TTA-UC efficiency is three times lower with the meta-substituted dye, which is attributed to its threefold decrease in its triplet excited state lifetime relative to the para-substituted dye.

Upconversion (UC) of low-energy photons into high-energy light can in principle increase the efficiency of solar devices by converting photons with energies below the energy absorption threshold into radiation that can be utilized. Among UC mechanisms, the sensitized triplet–triplet annihilation-based upconversion (sTTA-UC) is the most recent that would be applied in solar technologies. sTTA-UC was demonstrated using sunlight in 2006, and due to its high efficiency at low excitation intensities with noncoherent light, it is considered a promising strategy for the recovering of subbandgap photons. Here, we describe briefly the working principle of the sTTA-UC, and we review the most recent advances of its use in solar applications.

Triisopropylsilylethynyl-substituted acenes (TIPS-acenes) have received prominent attention in the field of singlet fission, the pentacene derivative being an exothermic singlet fission material, and the tetracene being a prototypical endothermic material. Little attention has been given to TIPS-anthracene, which is expected to exhibit exothermic triplet–triplet annihilation, despite literature reports to the contrary. We show that there is some evidence for singlet fission in TIPS-anthracene solutions, and that it does exhibit triplet–triplet annihilation. We apply anti-Stokes action spectroscopy to determine the upconversion efficiency of a composition of TIPS-anthracene and platinum octaethylporphyrin. At a bias equivalent to 0.86 suns, the composition exhibited an annihilation efficiency of 3.2%, which may be compared to diphenylanthracene, which yielded 9.2% under the same conditions. We attribute the low efficiency to a combination of a shorter triplet lifetime and low lying T2 and T3 states. The results are supported by ab initio quantum chemical calculations.

The limiting efficiency of a solar cell enhanced by both up- and downconversion is calculated to be 44.6% under one sun illumination using a detailed balance formalism. We show that solar cells are enhanced by both spectral conversion and photon recycling. This device architecture has the advantage of being able to enhance existing technologies after relatively few modifications. Importantly, we show that this device architecture’s limiting efficiency peaks close to the band gap of silicon, unlike other spectral converters with three absorbing thresholds.

An approach to enhance the ultimate efficiency of the silicon nanowires (Si NWs) solar cell is proposed based on a hybrid population-based algorithm. The suggested technique integrates the ability of exploration in a gravitational search algorithm (GSA) with the exploitation capability of particle swarm optimization (PSO) to synthesize both algorithms’ strengths. The hybrid GSA-PSO algorithm in MATLAB® code is linked to finite-difference time-domain solution technique based on Lumerical-software to simulate and optimize the Si NWs’ geometrical parameters. The suggested GSA-PSO algorithm has advantages in terms of better convergence and final fitness values than that of the PSO algorithm. Further, the Si NWs lattice with optimized diameters and heights shows a high ultimate efficiency of 42.5% with an improvement of 42.8% over the Si NWs lattice with the same diameters and heights. This enhancement is attributed to the different generated optical modes combined with multiple scattering and reduced reflection due to the different heights and different diameters, respectively.

An innovative approach to improve the performance of photovoltaic solar cells is presented. Until recently, the fabrication of grating layers has been well proven using bulk micromachining techniques, but lately low-cost dip-pen nanolithography (DPN) has been proposed as a method for printing nanostructures on different substrates and has matured to become one of the most versatile patterning techniques available at the nanoscale. However, this technique has scarcely been studied and tested for fabricating grating layers. In this research, submicron grating patterns from high refractive index polymers are fabricated on a few types of solar cells, significantly improving their efficiency. The appropriate geometries and materials for the grating patterns are obtained via numerical optimization using rigorous coupled wave analysis for electromagnetic simulations of the grating multilayer. Possible light-confinement schemes are analyzed, and their figures of merit are assessed. The simulation of the electrical characteristics is integrated with postdesign electromagnetic simulation. The corresponding theoretical and experimental studies shed light on the impact of the merger of the grating structure with the light harvester on the device’s optical and electrical properties. Success in using DPN paves pathways to low-cost fabrication of light harvesting devices with improved performance.

Currently, perovskite–silicon tandem solar cells are one of the most investigated concepts for overcoming the theoretical limit for the power conversion efficiency of silicon solar cells. For monolithic tandem solar cells, the available light must be distributed equally between the two subcells, which is known as current matching. For a planar device design, a global optimization of the layer thicknesses in the perovskite top cell allows current matching to be reached and reflective losses of the solar cell to be minimized at the same time. However, even after this optimization, the reflection and parasitic absorption losses add up to 7  mA  /  cm2. In this contribution, we use numerical simulations to study how well hexagonal sinusoidal nanotextures in the perovskite top-cell can reduce the reflective losses of the combined tandem device. We investigate three configurations. The current density utilization can be increased from 91% for the optimized planar reference to 98% for the best nanotextured device (period 500 nm and peak-to-valley height 500 nm), where 100% refers to the Tiedje–Yablonovitch limit. In a first attempt to experimentally realize such nanophotonically structured perovskite solar cells for monolithic tandems, we investigate the morphology of perovskite layers deposited onto sinusoidally structured substrates.