Semiconductors group

Abstract:

Characterisation of materials often requires the use of a substrate to support the sample being investigated. For optical characterisation at terahertz frequencies, quartz is commonly used owing to its high transmission and low absorption at these frequencies. Knowledge of the complex refractive index of quartz is required for analysis of time-domain terahertz spectroscopy and optical pump terahertz probe spectroscopy for samples on a quartz substrate. Here, we present the refractive index and extinction coefficient for α-quartz between 0.5 THz and 5.5 THz (17–183 cm^−1) taken at 10, 40, 80, 120, 160, 200 and 300 K. Quartz shows excellent transmission and is thus an ideal optical substrate over the THz band, apart from the region 3.9 ± 0.1 THz owing to a spectral feature originating from the lowest energy optical phonon modes. We also present the experimentally measured polariton dispersion of α-quartz over this frequency range.

Abstract:

We investigate the Raman spectrum of the low-temperature orthorhombic phase of the organic-inorganic halide perovskite CH3NH3PbI3, by combining first-principles calculations with high-resolution low-temperature Raman measurements. We find good agreement between theory and experiment and successfully assign each of the Raman peaks to the underlying vibrational modes. In the low-frequency spectral range (below 60 cm-1), we assign the prominent Raman signals at 26, 32, 42, and 49 cm-1to the Pb-I-Pb bending modes with either Agor B2gsymmetry and the signal at 58 cm-1to the librational mode of the organic cation. Owing to their significant intensity, we propose that these peaks can serve as clear markers of the vibrations of the [PbI3]-network and of the CH3NH3+ cations in this perovskite, respectively. In particular, the ratios of the intensities of these peaks might be used to monitor possible deviations from the ideal stoichiometry of CH3NH3PbI3.

Abstract:

To date, the most efficient hybrid metal halide peroskite solar cells employ TiO2 as electron-transporting material (ETM), making these devices unstable under UV light exposure. Replacing TiO2 with fullerene derivatives has been shown to result in improved electronic contact and increased device lifetime, making it of interest to assess whether similar improvements can be achieved by using other organic semiconductors as ETMs. In this work, we investigate perylene-3,4:9,10-tetracarboxylic bis(benzimidazole) as a vacuum-processable ETM, and we minimize electron-collection losses at the electron-selective contact by depositing pentamethylcyclopentadienyl cyclopentadienyl rhodium dimer, (RhCp*Cp)2, on fluorinated tin oxide. With (RhCp*Cp)2 as an interlayer, ohmic contacts can be formed, there is interfacial doping of the ETM, and stabilized power conversion efficiencies of up to 14.2% are obtained.

Abstract:

Traditionally, III–V multi-junction cells have been used in concentrator photovoltaic (CPV) applications, which deliver extremely high efficiencies but have failed to compete with ‘flat-plate’ silicon technologies owing to cost. Here, we assess the feasibility of using metal halide perovskites for CPVs, and we evaluate their device performance and stability under concentrated light. Under simulated sunlight, we achieve a peak efficiency of 23.6% under 14 Suns (that is, 14 times the standard solar irradiance), as compared to 21.1% under 1 Sun, and measure 1.26 V open-circuit voltage under 53 Suns, for a material with a bandgap of 1.63 eV. Importantly, our encapsulated devices maintain over 90% of their original efficiency after 150 h aging under 10 Suns at maximum power point. Our work reveals the potential of perovskite CPVs, and may lead to new PV deployment strategies combining perovskites with low-concentration factor and lower-accuracy solar tracking systems.

Abstract:

Metal halide perovskites have proven to be excellent light-harvesting materials in photovoltaic devices whose efficiencies are rapidly improving. Here, we examine the temperature-dependent photon absorption, exciton binding energy, and band gap of FAPbI3 (thin film) and find remarkably different behavior across the β–γ phase transition compared with MAPbI3. While MAPbI3 has shown abrupt changes in the band gap and exciton binding energy, values for FAPbI3 vary smoothly over a range of 100–160 K in accordance with a more gradual transition. In addition, we find that the charge-carrier mobility in FAPbI3 exhibits a clear T–0.5 trend with temperature, in excellent agreement with theoretical predictions that assume electron–phonon interactions to be governed by the Fröhlich mechanism but in contrast to the T–1.5 dependence previously observed for MAPbI3. Finally, we directly observe intraexcitonic transitions in FAPbI3 at low temperature, from which we determine a low exciton binding energy of only 5.3 meV at 10 K.