Piezoelectric Yield of Single Electrospun Poly(acrylonitrile) Ultrafine Fibers Studied by Piezoresponse Force Microscopy and Numerical Simulations.

Quantitative converse piezoelectric coefficient (d33) mapping of polymer ultrafine fibers of poly(acrylonitrile) (PAN), as well as of poly(vinylidene fluoride) (PVDF) as a reference material, obtained by rotating electrospinning, was carried out by piezoresponse force microscopy in the constant-excitation frequency-modulation mode (CE-FM-PFM). PFM mapping of single fibers reveals their piezoelectric activity and provides information on its distribution along the fiber length. Uniform behavior is typically observed on a length scale of a few micrometers. In some cases, variations with sinusoidal dependence along the fiber are reported, compatibly with a possible twisting around the fiber axis. The observed features of the piezoelectric yield have motivated numerical simulations of the surface displacement in a piezoelectric ultrafine fiber concerned by the electric field generated by biasing of the PFM probe. Uniform alignment of the piezoelectric axis along the fiber would comply with the uniform but strongly variable values observed, and sinusoidal variations were occasionally found on the fibers laying on the conductive substrate. Furthermore, in the latter case, numerical simulations show that the piezoelectric tensor's shear terms should be carefully considered in estimations since they may provide a remarkably different contribution to the overall deformation profile.

Exciton Dephasing by Phonon-Induced Scattering between Bright Exciton States in InP/ZnSe Colloidal Quantum Dots.

Decoherence or dephasing of the exciton is a central characteristic of a quantum dot (QD) that determines the minimum width of the exciton emission line and the purity of indistinguishable photon emission during exciton recombination. Here, we analyze exciton dephasing in colloidal InP/ZnSe QDs using transient four-wave mixing spectroscopy. We obtain a dephasing time of 23 ps at a temperature of 5 K, which agrees with the smallest line width of 50 µeV we measure for the exciton emission of single InP/ZnSe QDs at 5 K. By determining the dephasing time as a function of temperature, we find that exciton decoherence can be described as a phonon-induced, thermally activated process. The deduced activation energy of 0.32 meV corresponds to the small splitting within the nearly isotropic bright exciton triplet of InP/ZnSe QDs, suggesting that the dephasing is dominated by phonon-induced scattering within the bright exciton triplet.

Fine Structure of Nearly Isotropic Bright Excitons in InP/ZnSe Colloidal Quantum Dots.

The fine structure of exciton states in colloidal quantum dots (QDs) results from the compound effect of anisotropy and electron-hole exchange. By means of single-dot photoluminescence spectroscopy, we show that the emission of photoexcited InP/ZnSe QDs originates from radiative recombination of such fine structure exciton states. Depending on the excitation power, we identify a bright exciton doublet, a trion singlet, and a biexciton doublet line that all show pronounced polarization. Fluorescence line narrowing spectra of an ensemble of InP/ZnSe QDs in magnetic fields demonstrate that the bright exciton effectively consists of three states. The Zeeman splitting of these states is well described by an isotropic exciton model, where the fine structure is dominated by electron-hole exchange and shape anisotropy leads to only a minor splitting of the F = 1 triplet. We argue that excitons in InP-based QDs are nearly isotropic because the particular ratio of light and heavy hole masses in InP makes the exciton fine structure insensitive to shape anisotropy.

Coherence and Density Dynamics of Excitons in a Single-Layer MoS2 Reaching the Homogeneous Limit.

We measure the coherent nonlinear response of excitons in a single layer of molybdenum disulfide embedded in hexagonal boron nitride, forming a h-BN/MoS2/ h-BN heterostructure. Using four-wave mixing microscopy and imaging, we correlate the exciton inhomogeneous broadening with the homogeneous one and population lifetime. We find that the exciton dynamics is governed by microscopic disorder on top of the ideal crystal properties. Analyzing the exciton ultrafast density dynamics using amplitude and phase of the response, we investigate the relaxation pathways of the resonantly driven exciton population. The surface protection via encapsulation provides stable monolayer samples with low disorder, avoiding surface contaminations and the resulting exciton broadening and modifications of the dynamics. We identify areas localized to a few microns where the optical response is totally dominated by homogeneous broadening. Across the sample of tens of micrometers, weak inhomogeneous broadening and strain effects are observed, attributed to the remaining interaction with the h-BN and imperfections in the encapsulation process.

Long Exciton Dephasing Time and Coherent Phonon Coupling in CsPbBr2Cl Perovskite Nanocrystals.

Fully inorganic cesium lead halide perovskite nanocrystals (NCs) have shown to exhibit outstanding optical properties such as wide spectral tunability, high quantum yield, high oscillator strength as well as blinking-free single photon emission, and low spectral diffusion. Here, we report measurements of the coherent and incoherent exciton dynamics on the 100 fs to 10 ns time scale, determining dephasing and density decay rates in these NCs. The experiments are performed on CsPbBr2Cl NCs using transient resonant three-pulse four-wave mixing (FWM) in heterodyne detection at temperatures ranging from 5 to 50 K. We found a low-temperature exciton dephasing time of 24.5 ± 1.0 ps, inferred from the decay of the photon-echo amplitude at 5 K, corresponding to a homogeneous line width (fwhm) of 54 ± 5 µeV. Furthermore, oscillations in the photon-echo signal on a picosecond time scale are observed and attributed to coherent coupling of the exciton to a quantized phonon mode with 3.45 meV energy.