Near-field Optical Microscopy Research Articles

13C- and 15N-labeling of amyloid-β and inhibitory peptides to study their interaction via nanoscale infrared spectroscopy

Interactions between molecules are fundamental in biology. They occur also between amyloidogenic peptides or proteins that are associated with different amyloid diseases, which makes it important to study the mutual influence of two polypeptides on each other’s properties in mixed samples. However, addressing this research question with imaging techniques faces the challenge to distinguish different polypeptides without adding artificial probes for detection. Here, we show that nanoscale infrared spectroscopy in combination with 13C, 15N-labeling solves this problem. We studied aggregated amyloid-β peptide (Aβ) and its interaction with an inhibitory peptide (NCAM1-PrP) using scattering-type scanning near-field optical microscopy. Although having similar secondary structure, labeled and unlabeled peptides could be distinguished by comparing optical phase images taken at wavenumbers characteristic for either the labeled or the unlabeled peptide. NCAM1-PrP seems to be able to associate with or to dissolve existing Aβ fibrils because pure Aβ fibrils were not detected after mixing.

Advanced active polymer probe for near-field optics.

We report on a novel, to the best of our knowledge, active probe for scanning near-field optical microscopy (SNOM). A fluorescent nanosphere, acting as the secondary source, is grafted in an electrostatic manner at the apex of a polymer tip integrated into the extremity of an optical fiber. Thanks to the high photostability and sensitivity of the secondary source, the near-field interaction with a gold nanocube is investigated. It is shown that the spatial resolution is well defined by the size of the fluorescent nanosphere. The polarization-dependent near-field images, which are consistent with the simulation, are ascribed to the local excitation rate enhancement. Meanwhile, measurement of the distance-dependent fluorescence lifetime of the nanosphere provides strong evidence that the local density of states is modified so that extra information on nano-emitters can be extracted during near-field scanning. This advanced active probe can thus potentially broaden the range of applications to include nanoscale thermal imaging, biochemical sensors, and the manipulation of nanoparticles.

Polaritonic Probe of an Emergent 2D Dipole Interface.

The use of work-function-mediated charge transfer has recently emerged as a reliable route toward nanoscale electrostatic control of individual atomic layers. Using α-RuCl3 as a 2D electron acceptor, we are able to induce emergent nano-optical behavior in hexagonal boron nitride (hBN) that arises due to interlayer charge polarization. Using scattering-type scanning near-field optical microscopy (s-SNOM), we find that a thin layer of α-RuCl3 adjacent to an hBN slab reduces the propagation length of hBN phonon polaritons (PhPs) in significant excess of what can be attributed to intrinsic optical losses. Concomitant nano-optical spectroscopy experiments reveal a novel resonance that aligns energetically with the region of excess PhP losses. These experimental observations are elucidated by first-principles density-functional theory and near-field model calculations, which show that the formation of a large interfacial dipole suppresses out-of-plane PhP propagation. Our results demonstrate the potential utility of charge-transfer heterostructures for tailoring optoelectronic properties of 2D insulators.

Analyzing Three-dimensional Tip Near-field Scattering of Infrared Polaritons through Peak Force Scattering-type Near-field Optical Microscopy.

Analyzing Three-dimensional Tip Near-field Scattering of Infrared Polaritons through Peak Force Scattering-type Near-field Optical Microscopy.

Pseudoheterodyne interferometry for multicolor near-field imaging.

We report the development and characterization of a detection technique for scattering-type scanning near-field optical microscopy (s-SNOM) that enables near-field amplitude and phase imaging at two or more wavelengths simultaneously. To this end, we introduce multispectral pseudoheterodyne (PSH) interferometry, where infrared lasers are combined to form a beam with a discrete spectrum of laser lines and a time-multiplexing scheme is employed to allow for the use of a single infrared detector. We first describe and validate the implementation of multispectral PSH into a commercial s-SNOM instrument. We then demonstrate its application for the real-time correction of the negative phase contrast (NPC), which provides reliable imaging of weak IR absorption at the nanoscale. We anticipate that multispectral PSH could improve data throughput, reduce effects of sample and interferometer drift, and help to establish multicolor s-SNOM imaging as a regular imaging modality, which could be particularly interesting as new infrared light sources become available.

High spatial resolution imaging of light localization in hyperuniform disordered patterns of circular air pores in a dielectric slab

Hyperuniform disordered photonic structures are a peculiar category of disordered photonic heterostructures located between random structures and ordered photonic crystals. These materials, thanks to the presence of a photonic bandgap, exhibit the advantages of random and ordered structures since they have been shown to support in a small spatial footprint a high density of Anderson-localized modes, which naturally occur at the bandgap edges with peculiar features like relatively high Q/V ratios. Different localization behaviors have been recently reported in hyperuniform disordered luminescent materials, with a well-established and widely studied design, based on disordered networks. Here, we explore an alternative design, based on circular holes of different sizes hyperuniformely distributed, that we investigate theoretically and experimentally by means of scanning near-field optical microscopy. We report that the spectral features of hyperuniform disordered networks can also be extended to a different design, which, in turn, displays pseudo-photonic bandgaps and light localization. The ability of generating different kinds of hyperuniform disordered photonic systems that share the same theoretical and experimental optical features can largely extend practical potentialities and integration in many optoelectronic applications.

Reference-free self-calibrating tip-based scattering-type THz near-field microscopy

In this work, we present a quantitative analysis model based on reference-free self-calibration to analyze scattered fields and approach curves on a dielectric substrate for terahertz scattering-type scanning near-field optical microscopy. The results of our model are compared with experimentally measured data and a fully numerical analysis based on a line dipole image method and a quasi-electrostatic approximation. The model is used to extract the effective radius of the tip and the relative permittivity of the silicon substrate to the near-field scattering signal. The measured approach curves on Au and silicon substrates show good agreement with the calculated approach curves, and the refractive index for silicon is precisely determined to be 3.42. For a tip-based THz scattering-type scanning near-field optical microscope, the proposed analysis model allows for the extraction of the effective probe radius and dielectric functions, thereby enabling conclusive measurements of geometric parameters and optical constants.

Terahertz near-field imaging of graphene disks

Due to the weak power of Terahertz sources, metal tips are often used to enhance the signal intensity of the Terahertz scattering scanning near-field optical microscope (THz s-SNOM). However, while enhancing the near-field, metal tips also affect the field distribution on the sample surface. In this paper, a home-built 97.8GHz sub-Terahertz near-field imaging system was used to image graphene disks with dozens of microns in diameter. It was found that the field distribution was significantly different from that without the tip, and was related to the incident direction of the terahertz wave.

Integrating collapsible plasmonic gaps on near-field probes for polarization-resolved mapping of plasmon-enhanced emission in 2D material.

Scanning near-field optical microscopy (SNOM) is an important technique used to study the optical properties of material systems at the nanoscale. In previous work, we reported on the use of nanoimprinting to improve the reproducibility and throughput of near-field probes including complicated optical antenna structures such as the 'campanile' probe. However, precise control over the plasmonic gap size, which determines the near-field enhancement and spatial resolution, remains a challenge. Here, we present a novel approach to fabricating a sub-20 nm plasmonic gap in a near-field plasmonic probe through the controlled collapse of imprinted nanostructures using atomic layer deposition (ALD) coatings to define the gap width. The resulting ultranarrow gap at the apex of the probe provides a strong polarization-sensitive near-field optical response, which results in an enhancement of the optical transmission in a broad wavelength range from 620 to 820 nm, enabling tip-enhanced photoluminescence (TEPL) mapping of 2-dimensional (2D) materials. We demonstrate the potential of this near-field probe by mapping a 2D exciton coupled to a linearly polarized plasmonic resonance with below 30 nm spatial resolution. This work proposes a novel approach for integrating a plasmonic antenna at the apex of the near-field probe, paving the way for the fundamental study of light-matter interactions at the nanoscale.

Sub-terahertz scanning near-field optical microscope using a quartz tuning fork based probe.

We report a sub-terahertz scattering-type scanning near-field microscope (sub-THz s-SNOM) which uses a 6 mm long metallic tip driven by a quartz tuning fork as the near-field probe. Under continuous-wave illumination by a 94 GHz Gunn diode oscillator, terahertz near-field images are obtained by demodulating the scattered wave at both the fundamental and the second harmonic of the tuning fork oscillation frequency together with the atomic-force-microscope (AFM) image. The terahertz near-field image of a gold grating with a period of 2.3 µm obtained at the fundamental modulation frequency agrees well with the AFM image. The experimental relationship between the signal demodulated at the fundamental frequency and the tip-sample distance is well fitted with the coupled dipole model indicating that the scattered signal from the long probe is mainly contributed by the near-field interaction between the tip and the sample. This near-filed probe scheme using quartz tuning fork can adjust the tip length flexibly to match the wavelength over the entire terahertz frequency range and allows for operation in cryogenic environment.

Near-Field Localization of the Boson Peak on Tantalum Films for Superconducting Quantum Devices.

Superconducting circuits are among the most advanced quantum computing technologies; however, their performance is limited by losses found in surface oxides and disordered materials. In this work, we demonstrate the identification and spatial localization of a near-field signature of loss centers on tantalum films using terahertz scattering-type scanning near-field optical microscopy. By utilizing terahertz nanospectroscopy, we observe a localized excess vibrational mode around 0.5 THz and identify this resonance as the boson peak, a signature of amorphous materials. Grazing-incidence wide-angle X-ray scattering reveals that oxides on freshly solvent-cleaned samples are amorphous, whereas crystalline phases emerge after aging in air. Through nanoscale localization of defect centers, our findings provide valuable insights for the optimization of fabrication procedures for new low-loss superconducting circuits.

Deep learning Hamiltonians from disordered image data in quantum materials

The capabilities of image probe experiments are rapidly expanding, providing new information about quantum materials on unprecedented length and time scales. Many such materials feature inhomogeneous electronic properties with intricate pattern formation on the observable surface. This rich spatial structure contains information about interactions, dimensionality, and disorder -- a spatial encoding of the Hamiltonian driving the pattern formation. Image recognition techniques from machine learning are an excellent tool for interpreting information encoded in the spatial relationships in such images. Here, we develop a deep learning framework for using the rich information available in these spatial correlations in order to discover the underlying Hamiltonian driving the patterns. We first vet the method on a known case, scanning near-field optical microscopy on a thin film of VO2. We then apply our trained convolutional neural network architecture to new optical microscope images of a different VO2 film as it goes through the metal-insulator transition. We find that a two-dimensional Hamiltonian with both interactions and random field disorder is required to explain the intricate, fractal intertwining of metal and insulator domains during the transition. This detailed knowledge about the underlying Hamiltonian paves the way to using the model to control the pattern formation via, e.g., tailored hysteresis protocols. We also introduce a distribution-based confidence measure on the results of a multi-label classifier, which does not rely on adversarial training. In addition, we propose a new machine learning based criterion for diagnosing a physical system's proximity to criticality.

Mechanism of near-field optical nanopatterning on noble metal nano-films by a nanosecond laser irradiating a cantilevered scanning near-field optical microscopy probe.

To overcome the diffraction limit, a laser irradiating cantilevered scanning near-field optical microscopy (SNOM) probe has been used in near-field optical nanopatterning. In this paper, the mechanism of nanopatterning on noble metal nano-films by this technique is investigated by the finite element method. It is proposed that the main mechanism of this phenomenon is the melt and reshaping of the nano-film under the SNOM tip. The melt is caused by the surface plasmon polariton-assisted enhancement and restriction within the SNOM tip aperture. The impacts of the gap g between the tip and substrate and the polarization of the laser are further analyzed.

Nanoscale Enhancement of the Local Optical Conductivity near Cracks in Metallic SrRuO3 Film.

Cracking has been recognized as a major obstacle degrading material properties, including structural stability, electrical conductivity, and thermal conductivity. Recently, there have been several reports on the nanosized cracks (nanocracks), particularly in the insulating oxides. In this work, we comprehensively investigate how nanocracks affect the physical properties of metallic SrRuO3 (SRO) thin films. We grow SRO/SrTiO3 (STO) bilayers on KTaO3 (KTO) (001) substrates, which provide +1.7% tensile strain if the SRO layer is grown epitaxially. However, the SRO/STO bilayers suffer from the generation and propagation of nanocracks, and then, the strain becomes inhomogeneously relaxed. As the thickness increases, the nanocracks in the SRO layer become percolated, and its dc conductivity approaches zero. Notably, we observe an enhancement of the local optical conductivity near the nanocrack region using scanning-type near-field optical microscopy. This enhancement is attributed to the strain relaxation near the nanocracks. Our work indicates that nanocracks can be utilized as promising platforms for investigating local emergent phenomena related to strain effects.

Scanning Near-Field Optical Microscopy of Ultrathin Gold Films.

Ultrathin metal films are an essential platform for two-dimensional (2D) material compatible and flexible optoelectronics. Characterization of thin and ultrathin film-based devices requires a thorough consideration of the crystalline structure and local optical and electrical properties of the metal-2D material interface since they could be dramatically different from the bulk material. Recently, it was demonstrated that the growth of gold on the chemical vapor deposited monolayer MoS2 leads to a continuous metal film that preserves plasmonic optical response and conductivity even at thicknesses below 10 nm. Here, we examined the optical response and morphology of ultrathin gold films deposited on exfoliated MoS2 crystal flakes on the SiO2/Si substrate via scattering-type scanning near-field optical microscopy (s-SNOM). We demonstrate a direct relationship between the ability of thin film to support guided surface plasmon polaritons (SPP) and the s-SNOM signal intensity with a very high spatial resolution. Using this relationship, we observed the evolution of the structure of gold films grown on SiO2 and MoS2 with an increase in thickness. The continuous morphology and superior ability with respect to supporting SPPs of the ultrathin (≤10 nm) gold on MoS2 is further confirmed with scanning electron microscopy and direct observation of SPP fringes via s-SNOM. Our results establish s-SNOM as a tool for testing plasmonic films and motivate further theoretical research on the impact of the interplay between the guided modes and the local optical properties on the s-SNOM signal.

Domain-Dependent Surface Adhesion in Twisted Few-Layer Graphene: Platform for Moiré-Assisted Chemistry.

Twisted van der Waals multilayers are widely regarded as a rich platform to access novel electronic phases thanks to the multiple degrees of freedom available for controlling their electronic and chemical properties. Here, we propose that the stacking domains that form naturally due to the relative twist between successive layers act as an additional "knob" for controlling the behavior of these systems and report the emergence and engineering of stacking domain-dependent surface chemistry in twisted few-layer graphene. Using mid-infrared near-field optical microscopy and atomic force microscopy, we observe a selective adhesion of metallic nanoparticles and liquid water at the domains with rhombohedral stacking configurations of minimally twisted double bi- and trilayer graphene. Furthermore, we demonstrate that the manipulation of nanoparticles located at certain stacking domains can locally reconfigure the moiré superlattice in their vicinity at the micrometer scale. Our findings establish a new approach to controlling moiré-assisted chemistry and nanoengineering.

Deep-learning-aided extraction of optical constants in scanning near-field optical microscopy

Scanning near-field optical microscopy is one of the most effective techniques for spectroscopy of nanoscale systems. However, inferring optical constants from the measured near-field signal can be challenging because of a complicated and highly nonlinear interaction between the scanned probe and the sample. Conventional fitting methods applied to this problem often suffer from the lack of convergence or require human intervention. Here, we develop an alternative approach where the optical parameter extraction is automated by a deep learning network. The network provides an initial estimate that is subsequently refined by a traditional fitting algorithm. We show that this method demonstrates superior accuracy, stability against noise, and computational speed when applied to simulated near-field spectra.

Terahertz nanospectroscopy of plasmon polaritons for the evaluation of doping in quantum devices

Abstract Terahertz (THz) waves are a highly sensitive probe of free carrier concentrations in semiconducting materials. However, most experiments operate in the far-field, which precludes the observation of nanoscale features that affect the material response. Here, we demonstrate the use of nanoscale THz plasmon polaritons as an indicator of surface quality in prototypical quantum devices properties. Using THz near-field hyperspectral measurements, we observe polaritonic features in doped silicon near a metal-semiconductor interface. The presence of the THz surface plasmon polariton indicates the existence of a thin film doped layer on the device. Using a multilayer extraction procedure utilising vector calibration, we quantitatively probe the doped surface layer and determine its thickness and complex permittivity. The recovered multilayer characteristics match the dielectric conditions necessary to support the THz surface plasmon polariton. Applying these findings to superconducting resonators, we show that etching of this doped layer leads to an increase of the quality factor as determined by cryogenic measurements. This study demonstrates that THz scattering-type scanning near-field optical microscopy (s-SNOM) is a promising diagnostic tool for characterization of surface dielectric properties of quantum devices.

Localized surface plasmon controlled chemistry at and beyond the nanoscale

Gaining valuable insight into chemistry-related fields, such as molecular and catalytic systems, surface science, and biochemistry, requires probing physical and chemical processes at the sub-nanoscale level. Recent progress and advancements in nano-optics and nano-photonics, particularly in scanning near-field optical microscopy, have enabled the coupling of light with nano-objects using surface plasmons with sub-nanoscale precision, providing access to photophysical and photochemical processes. Herein, this review highlights the basic concepts of surface plasmons and recent experimental findings of tip-assisted plasmon-induced research works and offers a glimpse into future perspectives.

A sub-2 Kelvin cryogenic magneto-terahertz scattering-type scanning near-field optical microscope (cm-THz-sSNOM)

We have developed a versatile near-field microscopy platform that can operate at high magnetic fields and below liquid-helium temperatures. We use this platform to demonstrate an extreme terahertz (THz) nanoscope operation and to obtain the first cryogenic magneto-THz time-domain nano-spectroscopy/imaging at temperatures as low as 1.8 K, magnetic fields of up to 5 T, and with operation of 0–2 THz. Our Cryogenic Magneto-Terahertz Scattering-type Scanning Near-field Optical Microscope (or cm-THz-sSNOM) instrument is comprised of three main equipment: (i) a 5 T split pair magnetic cryostat with a custom made insert, (ii) a custom sSNOM instrument capable of accepting ultrafast THz excitation, and (iii) a MHz repetition rate, femtosecond laser amplifier for broadband THz pulse generation and sensitive detection. We apply the cm-THz-sSNOM to obtain proof of principle measurements of superconductors and topological semimetals. The new capabilities demonstrated break grounds for studying quantum materials that require an extreme environment of cryogenic operation and/or applied magnetic fields in nanometer space, femtosecond time, and THz energy scales.