All-inorganic cesium lead halide (CsPbX3, X = Br(-), I(-)) perovskites could potentially provide comparable photovoltaic performance with enhanced stability compared to organic-inorganic lead halide species. However, small-bandgap cubic CsPbI3 has been difficult to study due to challenges forming CsPbI3 in the cubic phase. Here, a low-temperature procedure to form cubic CsPbI3 has been developed through a halide exchange reaction using films of sintered CsPbBr3 nanocrystals. The reaction was found to be strongly dependent upon temperature, featuring an Arrhenius relationship. Additionally, film thickness played a significant role in determining internal film structure at intermediate reaction times. Thin films (50 nm) showed only a small distribution of CsPbBrxI3-x species, while thicker films (350 nm) exhibited much broader distributions. Furthermore, internal film structure was ordered, featuring a compositional gradient within film. Transient absorption spectroscopy showed the influence of halide exchange on the excited state of the material. In thicker films, charge carriers were rapidly transferred to iodide-rich regions near the film surface within the first several picoseconds after excitation. This ultrafast vectorial charge-transfer process illustrates the potential of utilizing compositional gradients to direct charge flow in perovskite-based photovoltaics.
All
inorganic cesium lead bromide (CsPbBr3) perovskite
is a more stable alternative to methylammonium lead bromide (MAPbBr3) for designing high open-circuit voltage solar cells and
display devices. Poor solubility of CsBr in organic solvents makes
typical solution deposition methods difficult to adapt for constructing
CsPbBr3 devices. Our layer-by-layer methodology, which
makes use of CsPbBr3 quantum dot (QD) deposition followed
by annealing, provides a convenient way to cast stable films of desired
thickness. The transformation from QDs into bulk during thermal annealing
arises from the resumption of nanoparticle growth and not from sintering
as generally assumed. Additionally, a large loss of organic material
during the annealing process is mainly from 1-octadecene left during
the QD synthesis. Utilizing this deposition approach for perovskite
photovoltaics is examined using typical planar architecture devices.
Devices optimized to both QD spin-casting concentration and overall
CsPbBr3 thickness produce champion devices that reach power
conversion efficiencies of 5.5% with a V
oc value of 1.4 V. The layered QD deposition demonstrates a controlled
perovskite film architecture for developing efficient, high open-circuit
photovoltaic devices.
Multipole strength distributions for isoscalar L ≤ 2 transitions in 28 Si have been extracted using 386-MeV inelastic α scattering at extremely forward angles, including 0• . Observed strength distributions are in good agreement with microscopic calculations for an oblate-deformed ground-state. In particular, a large peak at an excitation energy of 17.7 MeV in the isoscalar giant monopole resonance (ISGMR) strength is consistent with the calculations.
The isoscalar giant monopole resonance (ISGMR) strength distribution in 24 Mg has been determined from background-free inelastic scattering of 386-MeV α particles at extreme forward angles, including 0 • .
Energy transfer coupled with electron
transfer is a convenient
approach to mimic photosynthesis in light energy conversion. Better
understanding of mechanistic details of energy transfer processes
is important to enhance the performance of dye or quantum dot-sensitized
solar cells. Energy transfer through both long-range dipole-based
Förster resonance energy transfer (FRET) and short-range Dexter
energy transfer (DET) mechanisms have been identified to occur between
CdSe quantum dots (QDs) linked to a red-infrared-absorbing squaraine
dye through a short thiol functional group (SQSH). Solutions of SQSH
linked to CdSe were investigated through steady-state and time-resolved
spectroscopy experiments to explore both mechanisms. Photoluminescence
studies revealed that smaller QDs had higher energy transfer efficiencies
than predicted by FRET, and femtosecond transient absorption experiments
revealed faster energy transfer rates in smaller donor QD sizes. These
findings supported a DET process dominating at small donor sizes.
The presence of both processes illustrates multiple strategies for
utilizing energy transfer in light-harvesting assemblies and the required
considerations in device design to maximize energy transfer gains
through either mechanism.
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