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Register a new userBroadband Ultrafast Dynamics of Refractory Metals: TiN and ZrN
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Transition metal nitrides have recently gained attention in the fields of plasmonics, plasmon-enhanced photocatalysis, photothermal applications, and nonlinear optics because of their suitable optical properties, refractory nature, and large laser damage thresholds. This work reports comparative studies of the transient response of films of titanium nitride, zirconium nitride, and Au under femtosecond excitation. Broadband transient optical characterization helps to adjudicate earlier, somewhat inconsistent reports regarding hot electron lifetimes based upon single wavelength measurements. These pump-probe experiments show sub-picosecond transient dynamics only within the epsilon-near-zero window of the refractory metals. The dynamics are dominated by photoinduced interband transitions resulting from ultrafast electron energy redistribution. The enhanced reflection modulation in the epsilon-near-zero window makes it possible to observe the ultrafast optical response of these films at low pump fluences. These results indicate that electron-phonon coupling in TiN and ZrN is 25-100 times greater than in Au. Strong electron-phonon coupling drives the sub-picosecond optical response and facilitates greater lattice heating compared to Au, making TiN and ZrN promising for photothermal applications. The spectral response and dynamics of TiN and ZrN are only weakly sensitive to pump fluence and pump excitation energy. However, the magnitude of the response is much greater at higher pump photon energies and higher fluences, reaching peak observed values of 15 % in TiN and 50 % in ZrN in the epsilon-near-zero window.
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Understanding the nature and behavior of vacancy-like defects in epitaxial GeSn metastable alloys is crucial to elucidate the structural and optoelectronic properties of these emerging semiconductors. The formation of vacancies and their complexes is expected to be promoted by the relatively low substrate temperature required for the epitaxial growth of GeSn layers with Sn contents significantly above the equilibrium solubility of 1 at.%. These defects can impact both the microstructure and charge carrier lifetime. Herein, to identify the vacancy-related complexes and probe their evolution as a function of Sn content, depth-profiled pulsed low-energy positron annihilation lifetime spectroscopy and Doppler broadening spectroscopy were combined to investigate GeSn epitaxial layers with Sn content in the 6.5-13.0 at.% range. The samples were grown by chemical vapor deposition method at temperatures between 300 and 330 {deg}C. Regardless of the Sn content, all GeSn samples showed the same depth-dependent increase in the positron annihilation line broadening parameters, which confirmed the presence of open volume defects. The measured average positron lifetimes were the highest (380-395 ps) in the region near the surface and monotonically decrease across the analyzed thickness, but remain above 350 ps. All GeSn layers exhibit lifetimes that are 85 to 110 ps higher than the Ge reference layers. Surprisingly, these lifetimes were found to decrease as Sn content increases in GeSn layers. These measurements indicate that divacancies are the dominant defect in the as-grown GeSn layers. However, their corresponding lifetime was found to be shorter than in epitaxial Ge thus suggesting that the presence of Sn may alter the structure of divacancies. Additionally, GeSn layers were found to also contain a small fraction of vacancy clusters, which become less important as Sn content increases.
Here, we study the role of stress state and stress gradient in whisker growth in Sn coatings electrodeposited on brass. The bulk stress in Sn coatings was measured using a laser-optics based curvature setup, whereas glancing angle X-ray diffraction was employed to quantify the surface stress; this also allowed studying role of out-of-plane stress gradient in whisker growth. Both bulk stress and surface stress in Sn coating evolved with time, wherein both were compressive immediately after the deposition, and thereafter while the bulk stress monotonically became more compressive and subsequently saturated with aging at room temperature, the stress near the surface of the Sn coating continually became more tensile with aging. These opposing evolutionary behaviors of bulk and surface stresses readily established a negative out-of-plane stress gradient, required for spontaneous growth of whiskers. The importance of out-of-plane stress gradient was also validated by externally imposing widely different stress states and stress gradients in Sn coatings using a 3-point bending apparatus. It was consistently observed that whisker growth was more in the coatings under external tensile stress, however, with higher negative out-of-plane stress gradient. The results conclusively indicate the critical role of negative out-of-plane stress gradient on whisker growth, as compared to only the nature (i.e., sign and magnitude) of stress.
While metal-halide perovskites have recently revolutionized research in optoelectronics through a unique combination of performance and synthetic simplicity, their low-dimensional counterparts can further expand the field with hitherto unknown and practically useful optical functionalities. In this context, we present the strong temperature dependence of the photoluminescence (PL) lifetime of low-dimensional, perovskite-like tin-halides, and apply this property to thermal imaging with a high precision of 0.05 {deg}C. The PL lifetimes are governed by the heat-assisted de-trapping of self-trapped excitons, and their values can be varied over several orders of magnitude by adjusting the temperature (up to 20 ns {deg}C-1). Typically, this sensitive range spans up to one hundred centigrade, and it is both compound-specific and shown to be compositionally and structurally tunable from -100 to 110 {deg} C going from [C(NH2)3]2SnBr4 to Cs4SnBr6 and (C4N2H14I)4SnI6. Finally, through the innovative implementation of cost-effective hardware for fluorescence lifetime imaging (FLI), based on time-of-flight (ToF) technology, these novel thermoluminophores have been used to record thermographic videos with high spatial and thermal resolution.
Microwave reflectance probed photoconductivity (or $mu$-PCD) measurement represents a contactless and non-invasive method to characterize impurity content in semiconductors. Major drawbacks of the method include a difficult separation of reflectance due to dielectric and conduction effects and that the $mu$-PCD signal is prohibitively weak for highly conducting samples. Both of these limitations could be tackled with the use of microwave resonators due to the well-known sensitivity of resonator parameters to minute changes in the material properties combined with a null measurement. A general misconception is that time resolution of resonator measurements is limited beyond their bandwidth by the readout electronics response time. While it is true for conventional resonator measurements, such as those employing a frequency sweep, we present a time-resolved resonator parameter readout method which overcomes these limitations and allows measurement of complex material parameters and to enhance $mu$-PCD signals with the ultimate time resolution limit being the resonator time constant. This is achieved by detecting the transient response of microwave resonators on the timescale of a few 100 ns emph{during} the $mu$-PCD decay signal. The method employs a high-stability oscillator working with a fixed frequency which results in a stable and highly accurate measurement.
GaN nanowires grown by molecular beam epitaxy generally suffer from dominant nonradiative recombination, which is believed to originate from point defects. To suppress the formation of these defects, we explore the synthesis of GaN nanowires at temperatures up to 915 ${deg}C$ enabled by the use of thermally stable TiN$_x$/Al$_2$O$_3$ substrates. These samples exhibit indeed bound exciton decay times approaching those measured for state-of-the-art bulk GaN. However, the decay time is not correlated with the growth temperature, but rather with the nanowire diameter. The inverse dependence of the decay time on diameter suggests that the nonradiative process in GaN nanowires is not controlled by the defect density, but by the field ionization of excitons in the radial electric field caused by surface band bending. We propose a unified mechanism accounting for nonradiative recombination in GaN nanowires of arbitrary diameter.
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