Manganese(II)-doped
cesium–lead–chloride (Mn2+:CsPbCl3) perovskite nanocrystals have recently
been developed as promising luminescent materials and attractive candidates
for white-light generation. One approach to tuning the luminescence
of these materials has involved anion exchange to incorporate Br–, but the effects of anion exchange on Mn2+ speciation in doped metal-halide perovskites is not well understood
at a microscopic level. Here, we use a combination of X-band electron
paramagnetic resonance (EPR) and photoluminescence spectroscopies
to monitor the Mn2+ dopants in Mn2+:CsPbCl3 nanocrystals during Cl– → Br– anion exchange. Analytical measurements show that
the nanocrystals retain their Mn2+ over the course of Cl– → Br– anion exchange and
they continue to show strong Mn2+
d–d luminescence but, surprisingly, the Mn2+ EPR intensities
all but vanish. Further results suggest that Mn2+ ions
migrate during anion exchange to form clusters that are still luminescent
but show no EPR signal due to antiferromagnetic superexchange coupling.
Monte Carlo simulation and analysis of the Mn2+:CsPb(Cl1–x
Br
x
)3 lattice at various halide compositions (x) bolsters this interpretation by indicating a propensity for Mn2+–Cl– units to cluster as the Br– content increases, increasing the probability of the
nearest-neighbor Mn2+–Mn2+ interactions.
The driving force for this clustering is retention of the stronger
Mn–Cl bonds compared to Mn–Br bonds. In addition, modeling
predicts spinodal decomposition to form Mn2+-enriched domains
even at the end point compositions of x = 0 and 1,
with Mn2+ ordering in next-nearest-neighbor positions driven
by Coulomb interactions and lattice-strain minimization. These results
have important implications for both fundamental studies and applications
of doped and alloyed metal-halide perovskites.
We explore static spherically symmetric black hole solutions allowing a bulk U(1) vector field in the khronometric formulation of Hořava gravity by way of EinsteinAEther. We examine analytic solutions and study numerical results in the limit that the khronon does not backreact on the metric.
CsPb(Cl 1−x Br x ) 3 (0 ≤ x ≤ 1) nanocrystals and thin films doped with a series of trivalent rare-earth ions (RE 3+ = Y 3+ , La 3+ , Ce 3+ , Gd 3+ , Er 3+ , Lu 3+ ) have been prepared and studied using variable-temperature and time-resolved photoluminescence spectroscopies. We demonstrate that aliovalent (trivalent) doping of this type universally generates a new and oftenemissive defect state ca. 50 meV inside the perovskite band gap, independent of the specific RE 3+ dopant identity or of the perovskite form (nanocrystals vs thin films). Chloride-to-bromide anion exchange is used to demonstrate that this near-band-edge photoluminescence shifts with changing band-gap energy to remain just below the excitonic luminescence for all compositions of CsPb(Cl 1−x Br x ) 3 (0 ≤ x ≤ 1). Computations show that this shift stems from the effect of the changing lattice dielectric constants on a shallow defect-bound exciton. Microscopic descriptions of this dopant-induced near-band-edge state and its relation to quantum cutting in Yb 3+ -doped CsPb(Cl 1−x Br x ) 3 are discussed.
The simplified two-mass model of human vocal folds, proposed by Steinecke and Herzel [J. Acoust. Soc. Am. 97(3), 1874-1884 (1995)], has seen widespread use throughout the speech community. Herein, an error is corrected in the contact loadings on colliding vocal folds with asymmetric tissue properties, as arises clinically in cases of unilateral paralysis. A revised contact model is proposed that remediates the erroneous asymmetric contact forces. The vibration regime map presented in Steinecke and Herzel illustrating the dynamical behavior of the system is revised using the corrected collision model.
Despite being an indispensable tool for both researchers and clinicians, traditional endoscopic imaging of the human vocal folds is limited in that it cannot capture their inferior-superior motion. A three-dimensional reconstruction technique using high-speed video imaging of the vocal folds in stereo is explored in an effort to estimate the inferior-superior motion of the medial-most edge of the vocal folds under normal muscle activation in vivo. Traditional stereo-matching algorithms from the field of computer vision are considered and modified to suit the specific challenges of the in vivo application. Inferior-superior motion of the medial vocal fold surface of three healthy speakers is reconstructed over one glottal cycle. The inferior-superior amplitude of the mucosal wave is found to be approximately 13 mm for normal modal voice, reducing to approximately 3 mm for strained falsetto voice, with uncertainty estimated at σ ≈ 2 mm and σ ≈ 1 mm, respectively. Sources of error, and their relative effects on the estimation of the inferior-superior motion, are considered and recommendations are made to improve the technique.
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