To gain insight into the properties of photovoltaic and light-emitting materials, detailed information about their optical absorption spectra is essential. Here, we elucidate the temperature dependence of such spectra for methylammonium lead iodide (CH 3 NH 3 PbI 3 ), with specific attention to its sub-band gap absorption edge (often termed Urbach energy). On the basis of these data, we first find clear further evidence for the universality of the correlation between the Urbach energy and open-circuit voltage losses of solar cells. Second, we find that for CH 3 NH 3 PbI 3 the static, temperature-independent, contribution of the Urbach energy is 3.8 ± 0.7 meV, which is smaller than that of crystalline silicon (Si), gallium arsenide (GaAs), indium phosphide (InP), or gallium nitride (GaN), underlining the remarkable optoelectronic properties of perovskites.
Metal-halide perovskites feature very low deep-defect densities, enabling thereby high operating voltages on solar cell level. Here, by precise extraction of their absorption spectra, we find that the low deep-defect density is unaffected when Cs + and Rb + are added during the perovskite synthesis. By comparing single-crystals and polycrystalline thin-films of methyl ammonium lead iodide/bromide, we find these defects to be predominantly localized at surfaces and grain boundaries. Furthermore, for the most important photovoltaic materials, we demonstrate a strong correlation between their Urbach energy and open-circuit voltage deficiency on the solar cell level. Via external quantum yield photoluminescence efficiency measurements, we explain these results as a consequence of non-radiative open-circuit voltage losses in the solar cell.Finally, we define practical power conversion efficiency limits of solar cells by taking into account the Urbach energy.
Morphological and gel-to-liquid phase transitions of lipid membranes are generally
considered to primarily depend on the structural motifs in the hydrophobic core of the
bilayer. Structural changes in the aqueous headgroup phase are typically not considered,
primarily because they are difficult to quantify. Here, we investigate structural
changes of the hydration shells around large unilamellar vesicles (LUVs) in aqueous
solution, using differential scanning calorimetry (DSC), and temperature-dependent
ζ-potential and high-throughput angle-resolved second harmonic scattering
measurements (AR-SHS). Varying the lipid composition from
1,2-dimyristoyl-
sn
-glycero-3-phosphocholine(DMPC) to
1,2-dimyristoyl-
sn
-glycero-3-phosphate (DMPA), to
1,2-dimyristoyl-
sn
-glycero-3-phospho-
l
-serine (DMPS), we
observe surprisingly distinct behavior for the different systems that depend on the
chemical composition of the hydrated headgroups. These differences involve changes in
hydration following temperature-induced counterion redistribution, or changes in
hydration following headgroup reorientation and Stern layer compression.
Water is the matrix of life and serves as a solvent for
numerous
physical and chemical processes. The origins of the nature of inhomogeneities
that exist in liquid water and the time scales over which they occur
remains an open question. Here, we report femtosecond elastic second
harmonic scattering (fs-ESHS) of liquid water in comparison to an
isotropic liquid (CCl4) and show that water is indeed a
nonuniform liquid. The coherent fs-ESHS intensity was interpreted,
using molecular dynamics simulations, as arising from charge density
fluctuations with enhanced nanoscale polarizabilities around transient
voids having an average lifetime of 300 fs. Although voids were also
present in CCl4, they were not characterized by hydrogen
bond defects and did not show strong polarizability fluctuations,
leading to fs-ESHS of an isotropic liquid. The voids increased in
number at higher temperatures above room temperature, in agreement
with the fs-ESHS results.
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