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Register a new userOptical-microwave pump-probe studies of electronic properties in novel materials
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Added by
S\\'andor Kollarics
Publication date
2020
fields
Physics
and research's language is
English
Authors
S. Kollarics
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Combined microwave-optical pump-probe methods are emerging to study the quantum state of spin qubit centers and the charge dynamics in semiconductors. A major hindrance is the limited bandwidth of microwave irradiation/detection circuitry which could be overcome with the use of broadband coplanar waveguides (CPW). We present the development and performance characterization of two spectrometers: an optically detected magnetic resonance spectrometer (ODMR) and a microwave detected photoconductivity measurement. In the first method light serves as detection and microwaves excite the investigated medium, while in the second the roles are interchanged. The performance is demonstrated by measuring ODMR maps on the nitrogen-vacancy center in diamond and time resolved photoconductivity in p-doped silicon. The results demonstrate both an efficient coupling of the microwave irradiation to the samples as well as an excellent sensitivity for minute changes in sample conductivity.
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Optical pump-probe spectroscopy is a powerful tool for the study of non-equilibrium electronic dynamics and finds wide applications across a range of fields, from physics and chemistry to material science and biology. However, a shortcoming of conventional pump-probe spectroscopy is that photoinduced changes in transmission, reflection and scattering can simultaneously contribute to the measured differential spectra, leading to ambiguities in assigning the origin of spectral signatures and ruling out quantitative interpretation of the spectra. Ideally, these methods would measure the underlying dielectric function (or the complex refractive index) which would then directly provide quantitative information on the transient excited state dynamics free of these ambiguities. Here we present and test a model independent route to transform differential transmission or reflection spectra, measured via conventional optical pump-probe spectroscopy, to changes in the quantitative transient dielectric function. We benchmark this method against changes in the real refractive index measured using time-resolved Frequency Domain Interferometry in prototypical inorganic and organic semiconductor films. Our methodology can be applied to existing and future pump-probe data sets, allowing for an unambiguous and quantitative characterisation of the transient photoexcited spectra of materials. This in turn will accelerate the adoption of pump-probe spectroscopy as a facile and robust materials characterisation and screening tool.
Antiferromagnetism in stacked nanographite is investigated with using the Hubbard-type model. We find that the open shell electronic structure can be an origin of the decreasing magnetic moment with the decrease of the inter-graphene distance, as experiments on adsorption of molecules suggest. Next, possible charge-separated states are considered using the extended Hubbard model with nearest-neighbor interactions. The charge-polarized state could appear, when a static electric field is present in the graphene plane for example. Finally, superperiodic patterns with a long distance in a nanographene sheet observed by STM are discussed in terms of the interference of electronic wave functions with a static linear potential theoretically. In the analysis by the k-p model, the oscillation period decreases spatially in agreement with experiments.
Characterization of electronic properties of novel materials is of great importance for exploratory materials development and also for the discovery of new correlated phases. As several novel compounds are available in powder form only, contactless methods, which also work on air sensitive samples, are higly desired. We present that the microwave cavity perturbation technique is a versatile tool to study conductivity in such systems. The examples include studies on semiconducting-metallic crossover in carbon nanotubes upon alkali doping, study of vortex motion in the K$_3$C$_{60}$ superconductor, and the characterization of various alkali atom doped phases of black phosphorus.
Luminescent colloidal CdSe nanorings are a new type of semiconductor structure that have attracted interest due to the potential for unique physics arising from their non-trivial toroidal shape. However, the exciton properties and dynamics of these materials with complex topology are not yet well understood. Here, we use a combination of femtosecond vibrational spectroscopy, temperature-resolved photoluminescence (PL), and single particle measurements to study these materials. We find that on transformation of CdSe nanoplatelets to nanorings, by perforating the center of platelets, the emission lifetime decreases and the emission spectrum broadens due to ensemble variations in the ring size and thickness. The reduced PL quantum yield of nanorings (~10%) compared to platelets (~30%) is attributed to an enhanced coupling between: (i) excitons and CdSe LO-phonons at 200 cm-1 and (ii) negatively charged selenium-rich traps which give nanorings a high surface charge (~-50 mV). Population of these weakly emissive trap sites dominates the emission properties with an increased trap emission at low temperatures relative to excitonic emission. Our results provide a detailed picture of the nature of excitons in nanorings and the influence of phonons and surface charge in explaining the broad shape of the PL spectrum and the origin of PL quantum yield losses. Furthermore, they suggest that the excitonic properties of nanorings are not solely a consequence of the toroidal shape but are also a result of traps introduced by puncturing the platelet center.
X-ray absorption spectroscopy (XAS) is one of the most widely used experimental techniques to study the electronic and spatial structure of materials. Fluorescence yield mode is bulk-sensitive, but has several serious problems coming from saturation effects. In this study, we show the usefulness of partial fluorescence yields in addressing these problems. We discuss the different behaviors of La2NiMnO6 and LiMnO2 at the Mn 2p absorption edges. The total fluorescence yield produces misleading spectra for LiMnO2 due to the absence of high-Z (Z: atomic number) elements. We conclude that the measurement of the inverse partial fluorescence yield is essential in studies of LiMnO2, which is a hotly debated Li-ion battery material.
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