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Plasmon Enhanced Terahertz Electron Paramagnetic Resonance
- Božena Čechalová
- Jan Čechal
- Tomáš Šikola
Chalcogenide phase-change materials (PCMs) exhibit optical phonons at terahertz (THz) frequencies, which can be used for studying basic properties of the phase transition and which lead to a strong dielectric contrast that could be exploited for THz photonics applications. Here, we demonstrate that the phonons of PCMs can be studied by frequency-tunable THz scattering-type scanning near-field optical microscopy (s-SNOM). Specifically, we perform spectroscopic THz nanoimaging of a PCM sample comprising amorphous and crystalline phases. We observe phonon signatures, yielding strong s-SNOM signals and, most important, clear spectral differences between the amorphous and crystalline PCM, which allows for distinguishing the PCM phases with high confidence on the nanoscale. We also found that the spectral signature can be enhanced, regarding both signal strength and spectral contrast, by increasing the radius of the probing tip. From a general perspective, our results establish THz s-SNOM for nanoscale structural and chemical mapping based on local phonon spectroscopy.
Hybrid materials consisting of organic semiconductors and molecular quantum bits promise to provide a novel platform for quantum spintronic applications. However, investigations of such materials, elucidating both the electrical and quantum dynamical properties of the same material have never been reported. Here the preparation of hybrid materials consisting of con-ducting polymers and molecular quantum bits is reported. Organic ﬁeld-effect transistor measurements demonstrate that the favorable electrical proper-ties are preserved in the presence of the qubits. Chemical doping introduces charge carriers into the material, and variable-temperature charge transport measurements reveal the existence of mobile charge carriers at temperatures as low as 15 K. Importantly, quantum coherence of the qubit is shown to be preserved up to temperatures of at least 30 K, that is, in the presence of mobile charge carriers. These results pave the way for employing such hybrid materials in novel molecular quantum spintronic architectures.
We theoretically study plasmonic antennas featuring areas of extremely concentrated electric or magnetic field, known as hot spots. We combine two types of electric-magnetic complementarity to increase the degree of freedom for the design of the antennas: bowtie and diabolo duality and Babinet’s principle. We evaluate the figures of merit for different plasmon-enhanced optical spectroscopy methods and optical trapping: field enhancement, decay rate enhancement, quality factor of the plasmon resonances, and trapping potential depth. The role of Babinet’s principle in interchanging electric and magnetic field hot spots and its consequences for practical antenna design are discussed. In particular, diabolo antennas exhibit slightly better performance than bowties in terms of larger field enhancement and larger Q factor. For specific resonance frequency, diabolo antennas are considerably smaller than bowties, which makes them favorable for the integration into more complex devices but also makes their fabrication more demanding in terms of spatial resolution. Finally, we propose a Babinet-type dimer antenna featuring electromagnetic hot spot with both the electric and magnetic field components treated on an equal footing.
Scattering-type scanning near-field microscopy (s-SNOM) at terahertz (THz) frequencies could become a highly valuable tool for studying a variety of phenomena of both fundamental and applied interest, including mobile carrier excitations or phase transitions in 2D materials or exotic conductors. Applications, however, are strongly challenged by the limited signal-to-noise ratio. One major reason is that standard atomic force microscope (AFM) tips, which have made s-SNOM a highly practical and rapidly emerging tool, provide weak scattering efficiencies at THz frequencies. Here, we report a combined experimental and theoretical study of commercial and custom-made AFM tips of different apex diameter and length, in order to understand signal formation in THz s-SNOM and to provide insights for tip optimization. Contrary to common beliefs, we find that AFM tips with large (micrometer-scale) apex diameter can enhance s-SNOM signals by more than 1 order of magnitude, while still offering a spatial resolution in the 100 nm range at a wavelength of λ = 119 μm. On the other hand, exploiting the increase of s-SNOM signals with tip length, we succeeded in sub-15 nm (<λ/8000) resolved THz imaging employing a tungsten tip with 6 nm apex radius. We explain our findings and provide novel insights into s-SNOM via rigorous numerical modeling of the near-field scattering process. Our findings will be of critical importance for pushing THz nanoscopy to its ultimate limits regarding sensitivity and spatial resolution.
Scattering-type scanning near-field optical microscopy (s-SNOM) allows for nanoscale-resolved Infrared (IR) and Terahertz (THz) imaging, and thus has manifold applications ranging from materials to biosciences. However, a quantitatively accurate understanding of image contrast formation at materials boundaries, and thus spatial resolution is a surprisingly unexplored terrain. Here we introduce the read/write head of a commercial hard disk drive (HDD) as a most suitable test sample for fundamental studies, given its well-defined sharp material boundaries perpendicular to its ultrasmooth surface. We obtain unprecedented and unexpected insights into the s-SNOM image formation process, free of topography-induced contrasts that often mask and artificially modify the pure near-field optical contrast. Across metal-dielectric boundaries, we observe non-point-symmetric line profiles for both IR and THz illumination, which are fully corroborated by numerical simulations. We explain our findings by a sample-dependent confinement and screening of the near fields at the tip apex, which will be of crucial importance for an accurate understanding and proper interpretation of high-resolution s-SNOM images of nanocomposite materials. We also demonstrate that with ultrasharp tungsten tips the apparent width (resolution) of sharp material boundaries can be reduced to about 5 nm.