Structural and optical properties of monocrystalline and polycrystalline gold plasmonic nanorods.

The quality of lithographically prepared structures is intimately related to the properties of the metal film from which they are fabricated. Here we compare two kinds of thin gold films on a silicon nitride membrane: a conventional polycrystalline thin film deposited by magnetron sputtering and monocrystalline gold microplates that were chemically synthesised directly on the membrane's surface for the first time. Both pristine metals were used to fabricate plasmonic nanorods using focused ion beam lithography. The structural and optical properties of the nanorods were characterized by analytical transmission electron microscopy including electron energy loss spectroscopy. The dimensions of the nanorods in both substrates reproduced well the designed size of 240×80 nm2 with the deviations up to 20 nm in both length and width. The shape reproducibility was considerably improved among monocrystalline nanorods fabricated from the same microplate. Interestingly, monocrystalline nanorods featured inclined boundaries while the boundaries of the polycrystalline nanorods were upright. Q factors and peak loss probabilities of the modes in both structures are within the experimental uncertainty identical. We demonstrate that the optical response of the plasmonic nanorods is not deteriorated when the polycrystalline metal is used instead of the monocrystalline metal.

High-Resolution Quantitative Phase Imaging of Plasmonic Metasurfaces with Sensitivity down to a Single Nanoantenna.

Optical metasurfaces have emerged as a new generation of building blocks for multifunctional optics. Design and realization of metasurface elements place ever-increasing demands on accurate assessment of phase alterations introduced by complex nanoantenna arrays, a process referred to as quantitative phase imaging. Despite considerable effort, the widefield (nonscanning) phase imaging that would approach resolution limits of optical microscopy and indicate the response of a single nanoantenna still remains a challenge. Here, we report on a new strategy in incoherent holographic imaging of metasurfaces, in which unprecedented spatial resolution and light sensitivity are achieved by taking full advantage of the polarization selective control of light through the geometric (Pancharatnam-Berry) phase. The measurement is carried out in an inherently stable common-path setup composed of a standard optical microscope and an add-on imaging module. Phase information is acquired from the mutual coherence function attainable in records created in broadband spatially incoherent light by the self-interference of scattered and leakage light coming from the metasurface. In calibration measurements, the phase was mapped with the precision and spatial background noise better than 0.01 and 0.05 rad, respectively. The imaging excels at the high spatial resolution that was demonstrated experimentally by the precise amplitude and phase restoration of vortex metalenses and a metasurface grating with 833 lines/mm. Thanks to superior light sensitivity of the method, we demonstrated for the first time to our knowledge the widefield measurement of the phase altered by a single nanoantenna while maintaining the precision well below 0.15 rad.

Imaging of near-field interference patterns by aperture-type SNOM - influence of illumination wavelength and polarization state.

Scanning near-field optical microscopy (SNOM) in combination with interference structures is a powerful tool for imaging and analysis of surface plasmon polaritons (SPPs). However, the correct interpretation of SNOM images requires profound understanding of principles behind their formation. To study fundamental principles of SNOM imaging in detail, we performed spectroscopic measurements by an aperture-type SNOM setup equipped with a supercontinuum laser and a polarizer, which gave us all the degrees of freedom necessary for our investigation. The series of wavelength- and polarization-resolved measurements, together with results of numerical simulations, then allowed us to identify the role of individual near-field components in formation of SNOM images, and to show that the out-of-plane component generally dominates within a broad range of parameters explored in our study. Our results challenge the widespread notion that this component does not couple to the aperture-type SNOM probe and indicate that the issue of SNOM probe sensitivity towards the in-plane and out-of-plane near-field components - one of the most challenging tasks of near field interference SNOM measurements - is not yet fully resolved.

Analytical electron microscopy analysis of insulating and metallic phases in nanostructured vanadium dioxide.

Vanadium dioxide (VO2) is a strongly correlated material that exhibits the insulator-to-metal transition (IMT) near room temperature, which makes it a promising candidate for applications in nanophotonics or optoelectronics. However, creating VO2 nanostructures with the desired functionality can be challenging due to microscopic inhomogeneities that can significantly impact the local optical and electronic properties. Thin lamellas, produced by focused ion beam milling from a homogeneous layer, provide a useful prototype for studying VO2 at the truly microscopic level using a scanning transmission electron microscope (STEM). High-resolution imaging is used to identify structural inhomogeneities while electron energy-loss spectroscopy (EELS) supported by statistical analysis helps to detect V x O y stoichiometries with a reduced oxidation number of vanadium at the areas of thickness below 70 nm. On the other hand, the thicker areas are dominated by vanadium dioxide, where the signatures of the IMT are detected in both core-loss and low-loss EELS experiments with in situ heating. The experimental results are interpreted with ab initio and semi-classical calculations. This work shows that structural inhomogeneities such as pores and cracks present no harm to the desired optical properties of VO2 samples.

Plasmonic Properties of Individual Gallium Nanoparticles.

Gallium is a plasmonic material offering ultraviolet to near-infrared tunability, facile and scalable preparation, and good stability of nanoparticles. In this work, we experimentally demonstrate the link between the shape and size of individual gallium nanoparticles and their optical properties. To this end, we utilize scanning transmission electron microscopy combined with electron energy loss spectroscopy. Lens-shaped gallium nanoparticles with a diameter between 10 and 200 nm were grown directly on a silicon nitride membrane using an effusion cell developed in house that was operated under ultra-high-vacuum conditions. We have experimentally proven that they support localized surface plasmon resonances and their dipole mode can be tuned through their size from the ultraviolet to near-infrared spectral region. The measurements are supported by numerical simulations using realistic particle shapes and sizes. Our results pave the way for future applications of gallium nanoparticles such as hyperspectral absorption of sunlight in energy harvesting or plasmon-enhanced luminescence of ultraviolet emitters.

Correlative Imaging of Individual CsPbBr3 Nanocrystals: Role of Isolated Grains in Photoluminescence of Perovskite Polycrystalline Thin Films.

We report on the optical properties of a CsPbBr3 polycrystalline thin film on a single grain level. A sample composed of isolated nanocrystals (NCs) mimicking the properties of the polycrystalline thin film grains that can be individually probed by photoluminescence spectroscopy was prepared. These NCs were analyzed using correlative microscopy allowing the examination of structural, chemical, and optical properties from identical sites. Our results show that the stoichiometry of the CsPbBr3 NCs is uniform and independent of the NCs' morphology. The photoluminescence (PL) peak emission wavelength is slightly dependent on the dimensions of NCs, with a blue shift up to 9 nm for the smallest analyzed NCs. The magnitude of the blueshift is smaller than the emission line width, thus detectable only by high-resolution PL mapping. By comparing the emission energies obtained from the experiment and a rigorous effective mass model, we can fully attribute the observed variations to the size-dependent quantum confinement effect.

Disproportionation and metallization at low-spin to high-spin transition in multiorbital Mott systems.

We study the thermally driven spin state transition in a two-orbital Hubbard model with crystal-field splitting, which provides a minimal description of the physics of LaCoO(3). We employ the dynamical mean-field theory with a quantum Monte Carlo impurity solver. At intermediate temperatures we find a spin disproportionated phase characterized by a checkerboard order of sites with small and large spin moments. The high temperature transition from the disproportionated to a homogeneous phase is accompanied by a vanishing of the charge gap. With the increasing crystal-field splitting the temperature range of the disproportionated phase shrinks and eventually disappears completely.

Plasmonic Metasurface Resonators to Enhance Terahertz Magnetic Fields for High-Frequency Electron Paramagnetic Resonance.

Nanoscale magnetic systems play a decisive role in areas ranging from biology to spintronics. Although, in principle, THz electron paramagnetic resonance (EPR) provides high-resolution access to their properties, lack of sensitivity has precluded realizing this potential. To resolve this issue, the principle of plasmonic enhancement of electromagnetic fields that is used in electric dipole spectroscopies with great success is exploited, and a new type of resonators for the enhancement of THz magnetic fields in a microscopic volume is proposed. A resonator composed of an array of diabolo antennas with a back-reflecting mirror is designed and fabricated. Simulations and THz EPR measurements demonstrate a 30-fold signal increase for thin film samples. This enhancement factor increases to a theoretical value of 7500 for samples confined to the active region of the antennas. These findings open the door to the elucidation of fundamental processes in nanoscale samples, including junctions in spintronic devices or biological membranes.

Vacuum Rabi splitting of a dark plasmonic cavity mode revealed by fast electrons.

Recent years have seen a growing interest in strong coupling between plasmons and excitons, as a way to generate new quantum optical testbeds and influence chemical dynamics and reactivity. Strong coupling to bright plasmonic modes has been achieved even with single quantum emitters. Dark plasmonic modes fare better in some applications due to longer lifetimes, but are difficult to probe as they are subradiant. Here, we apply electron energy loss (EEL) spectroscopy to demonstrate that a dark mode of an individual plasmonic bowtie can interact with a small number of quantum emitters, as evidenced by Rabi-split spectra. Coupling strengths of up to 85 meV place the bowtie-emitter devices at the onset of the strong coupling regime. Remarkably, the coupling occurs at the periphery of the bowtie gaps, even while the electron beam probes their center. Our findings pave the way for using EEL spectroscopy to study exciton-plasmon interactions involving non-emissive photonic modes.

Comparative study of plasmonic antennas fabricated by electron beam and focused ion beam lithography.

We present a comparative study of plasmonic antennas fabricated by electron beam lithography and direct focused ion beam milling. We have investigated optical and structural properties and chemical composition of gold disc-shaped plasmonic antennas on a silicon nitride membrane fabricated by both methods to identify their advantages and disadvantages. Plasmonic antennas were characterized using transmission electron microscopy including electron energy loss spectroscopy and energy dispersive X-ray spectroscopy, and atomic force microscopy. We have found stronger plasmonic response with better field confinement in the antennas fabricated by electron beam lithography, which is attributed to their better structural quality, homogeneous thickness, and only moderate contamination mostly of organic nature. Plasmonic antennas fabricated by focused ion beam lithography feature weaker plasmonic response, lower structural quality with pronounced thickness fluctuations, and strong contamination, both organic and inorganic, including implanted ions from the focused beam. While both techniques are suitable for the fabrication of plasmonic antennas, electron beam lithography shall be prioritized over focused ion beam lithography due to better quality and performance of its products.

Near-field digital holography: a tool for plasmon phase imaging.

The knowledge of the phase distribution of the near electromagnetic field has become very important for many applications. However, its experimental observation is still technologically a very demanding task. In this work, we propose a novel method for the measurement of the phase distribution of the near electric field based on the principles of phase-shifting digital holography. In contrast to previous methods the holographic interference occurs already in the near field and the phase distribution can be determined purely from the scanning near-field optical microscopy measurements without the need for additional far-field interferometric methods. This opens a way towards on-chip phase imaging. We demonstrate the capabilities of the proposed method by reconstruction of the phase difference between interfering surface plasmon waves and by imaging the phase of a single surface plasmon wave. We also demonstrate a selectivity of the method towards individual components of the field.

Uniaxial stress flips the natural quantization axis of a quantum dot for integrated quantum photonics.

The optical selection rules in epitaxial quantum dots are strongly influenced by the orientation of their natural quantization axis, which is usually parallel to the growth direction. This configuration is well suited for vertically emitting devices, but not for planar photonic circuits because of the poorly controlled orientation of the transition dipoles in the growth plane. Here we show that the quantization axis of gallium arsenide dots can be flipped into the growth plane via moderate in-plane uniaxial stress. By using piezoelectric strain-actuators featuring strain amplification, we study the evolution of the selection rules and excitonic fine structure in a regime, in which quantum confinement can be regarded as a perturbation compared to strain in determining the symmetry-properties of the system. The experimental and computational results suggest that uniaxial stress may be the right tool to obtain quantum-light sources with ideally oriented transition dipoles and enhanced oscillator strengths for integrated quantum photonics.