Scanning Near-field Optical Microscopy Images Research Articles

Accelerated Nano-Optical Imaging through Sparse Sampling.

The integration time and signal-to-noise ratio are inextricably linked when performing scanning probe microscopy based on raster scanning. This often yields a large lower bound on the measurement time, for example, in nano-optical imaging experiments performed using a scanning near-field optical microscope (SNOM). Here, we utilize sparse scanning augmented with Gaussian process regression to bypass the time constraint. We apply this approach to image charge-transfer polaritons in graphene residing on ruthenium trichloride (α-RuCl3) and obtain key features such as polariton damping and dispersion. Critically, nano-optical SNOM imaging data obtained via sparse sampling are in good agreement with those extracted from traditional raster scans but require 11 times fewer sampled points. As a result, Gaussian process-aided sparse spiral scans offer a major decrease in scanning time.

(Invited) Near-Field Optics and Its Applications in Nanophotonic Devices: A Review

In our presentation, we will offer an overview of aperture-type scanning near field optical microscopy (SNOM) – a family of nano-optical imaging techniques derived from scanning probe microscopy which are capable of subwavelength resolution, and the development of three dimensional (3D) SNOM methods undertaken by our group to locally image the distribution of the electromagnetic radiation in the proximity of nanoparticles and nano-objects.[1] We will discuss a few applications in which we took advantage of 3D-SNOM to design specific optical nanosystems for light harvesting device applications. Specific case studies that will be presented include the design of plasmonic thin-film solar cells enhanced by random arrays of copper nanoparticles,[2] and the use of 3D-SNOM for characterizing evanescent waveguides self-assembled from of copper nanoparticles assembled on thin films of graphene.[3] In the final part of our talk, we will we present near-field scanning thermoreflectance imaging (NeSTRI), a new pump-probe technique invented in our group (see Figure 1) in which an aperture-type SNOM is used to contactlessly determine the thermal conductivity of inhomogeneous thin films and low-dimensional systems at the nanoscale for heat-spreading and thermoelectric applications.[4,5] These examples well represent the versatility of SNOM imaging and its potential for designing an even wider family of nano-optical devices.[1] P Bazylewski, S Ezugwu, G Fanchini, Applied Sciences 7 (2017) 973[2] S Ezugwu, H Ye, G Fanchini, Nanoscale 7 (2016) 252-260[3] T Ouyang, A Akbari-Sharbaf, J Park, R Bauld, MG Cottam, G Fanchini, RSC Advances 5 (2015) 98814-98821[4] S Ezugwu, S Kazemian, DYW Choi, G Fanchini, Nanoscale 9 (2017) 4097-4106[5] S Kazemian, S Ezugwu, G Fanchini, Proc. SPIE 10926, Quantum Sensing and Nano Electronics and Photonics XVI, 109260L (1 February 2019); doi: 10.1117/12.2509828 Figure 1

Dark-probe scanning near-field microscopy

Scanning near-field optical microscopy (SNOM) is a well-known powerful optical technique for visualization of surface nanostructures and fields far beyond the diffraction limit and thus indispensable in material- and nanoscience. While the SNOM resolution is theoretically unlimited, the SNOM performance is in practice constrained by the signal-to-background ratio, simply because of light scattering scaling down as the sixth power of a nanoparticle size and useful signals rapidly drowning in the background for very small objects. In modern instruments, this problem is usually ameliorated through advanced post-processing techniques. Here, we suggest using, instead or in parallel, a ‘dark’ SNOM probe designed to suppress the background light scattering, so that the scattering occurs only when the probe is very close to a nanoscopic object. We argue and demonstrate with simulations that the dark-probe SNOM imaging is much more sensitive to the presence of tiny nanoparticles or any other nanoscale features, allowing thereby for superior resolution and sensing capabilities that are invaluable for nano-optical characterization.

Substrate-enhanced photothermal nano-imaging of surface polaritons in monolayer graphene

Surface polaritons comprise a wealth of light–matter interactions with deep sub-wavelength scale confinement of electromagnetic modes. However, their nanoscale localized dissipation and thermalization processes are not readily accessible experimentally. Here, we introduce photothermal force microscopy to image surface plasmon polaritons (SPPs) in monolayer graphene through their non-radiative SiO2 substrate dissipation. We demonstrate the real-space SPP imaging via photo-induced atomic force detection, and from comparison with scattering-type scanning near-field optical microscopy imaging attribute the force response to substrate dissipation-enhanced thermal expansion. This work illustrates that nano-optical tip–sample induced dissipative forces facilitate a direct mechanical detection of surface polariton interactions with monolayer sensitivity.

Effect of sample anisotropy on scanning near-field optical microscope images

Scattering-type scanning near-field optical microscopy (s-SNOM) has been widely used to characterize strongly correlated electronic, two dimensional, and plasmonic materials, and it has enormous potential for biological applications. Many of these materials exhibit anisotropic responses that complicate the extraction of dielectric constants from s-SNOM measurements. Here, we generalize our recently developed approach for retrieving the near-field scattering signal from isotropic systems and apply it to anisotropic dielectrics. Specifically, we compare our theoretical results with experimental measurements on modestly anisotropic sapphire that exhibit strong resonances at the infrared frequency range. Good agreement with the experimental result is found. Our result is important for understanding the near-field response of low damping, anisotropic polaritonic states in dielectric media.

Visibility of subsurface nanostructures in scattering-type scanning near-field optical microscopy imaging.

Detecting structures below a cover film at the nanoscale resolution is of essential importance. In this work, we explored factors affecting subsurface material contrast and structural visibility in scattering-type scanning near-field optical microscopy (s-SNOM). A kind of multilayered reference samples containing different buried structures was fabricated and applied for s-SNOM imaging. The dependence of near-field optical contrast on structure geometry, dimension and cover thickness was investigated. Results demonstrate that distinguishing the buried slit pattern is easier than the circular hole with the same critical dimension. The s-SNOM can sense material difference under a more than 100 nm thick polymethyl methacrylate layer and it has a subsurface spatial resolution better than 100 nm.

Ultra-structural analysis of human spermatozoa by aperture scanning near-field optical microscopy.

Scanning near-field optical microscopy (SNOM) represents a potential candidate for investigation of ultrastructure in human spermatozoa. It is a noninvasive optical technique that offers two main advantages: minimal sample preparation and simultaneous topographical and optical images acquisition with a spatial resolution beyond the diffraction limit. This enables the combination of surface characterization and information from the inner cellular organization in a single acquisition providing an immediate and comprehensive analysis of the cellular portions. In this work spermatozoa are immobilized on poly-L-lysine coated coverslips, fixed according to a standard protocol and imaged by aperture-SNOM in air. In the SNOM images, all peculiar sperm portions show well-resolved optical features, which exhibit good similarities with the structures revealed in transmission electron microscopy images, as compared with literature data. The optical features of anomalous spermatozoa are clearly different as respect with those observed for healthy ones. This analysis reveals the potentialities of SNOM and opens to its application to high-resolution analysis of sperm morphological alterations, which might be relevant in reproductive medicine.

Ultrabroadband 3D invisibility with fast-light cloaks

An invisibility cloak should completely hide an object from an observer, ideally across the visible spectrum and for all angles of incidence and polarizations of light, in three dimensions. However, until now, all such devices have been limited to either small bandwidths or have disregarded the phase of the impinging wave or worked only along specific directions. Here, we show that these seemingly fundamental restrictions can be lifted by using cloaks made of fast-light media, termed tachyonic cloaks, where the wave group velocity is larger than the speed of light in vacuum. On the basis of exact analytic calculations and full-wave causal simulations, we demonstrate three-dimensional cloaking that cannot be detected even interferometrically across the entire visible regime. Our results open the road for ultrabroadband invisibility of large objects, with direct implications for stealth and information technology, non-disturbing sensors, near-field scanning optical microscopy imaging, and superluminal propagation.

Control of Wigner localization and electron cavity effects in near-field emission spectra of In(Ga)P/GaInP quantum-dot structures

Structural and emission properties of few-electron In(Ga)P/GaInP quantum dots (QDs) representing natural Wigner molecules (WM) and whispering gallery mode (WGM) electron ($e$) cavities have been investigated. QD structures were grown using self-organized metal-organic vapor phase epitaxy and deposition from $\ensuremath{\sim}3$ to 7 monolayers of InP at $700{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\mathrm{C}$. Using atomic force microscopy, transmission electron microscopy, near-field scanning optical microscopy (NSOM), and $\ensuremath{\mu}$-photoluminescence ($\ensuremath{\mu}$-PL) spectra we obtained In(Ga)P/GaInP QDs having lateral size 80--180 nm, height 5--30 nm, Ga content 0.0--0.4, density $2\ensuremath{-}10\phantom{\rule{0.16em}{0ex}}\ensuremath{\mu}{\mathrm{m}}^{\ensuremath{-}2}$, and electron population up to 20 and demonstrated control of their density and size distribution. Using high-spatial-resolution low-temperature PL spectra, NSOM imaging, and calculations of charge density distributions we observed Wigner localization and $e$-cavity effects for a series of dots having quantum confinement $\ensuremath{\hbar}{\ensuremath{\omega}}_{0}=0.5\ensuremath{-}6\phantom{\rule{0.16em}{0ex}}\mathrm{meV}$. We used these data together with time-resolved PL measurements to clarify the effect of Coulomb interaction and WM formation on emission spectra of few-electron QDs. We present direct observation of $2e$, $6e$, and $9e$ WMs; $2e$ and $4e$ WGMs; and Fabry-Perot $e$ modes and establish conditions of $e$-WGM-cavity formation in these QDs.

Wigner Localization and Whispering Gallery Modes of Electrons in Quantum Dots

We used a low temperature near-field scanning optical microscopy (NSOM) to study a formation of Wigner molecules (WMs) in the emission spectra of self-organized InP/GaInP QDs having up to seven electrons. We used a Schottky diode structure for the electrostatic control of the number of the electrons (N) in QD, and we observed the emission of the charged excitons (for N 2) in the regime of weak Wigner localization. We show, that a contribution of whispering gallery modes (WGMs) of the electrons and rearrangement of the electrons between the WM and WGM states in the QDs, can explain the anomalous dependence of NSOM image size on the quantum confinement observed for some dots.

Wigner localization and whispering gallery modes of electrons in quantum dots

AbstractWe used a low temperature near-field scanning optical microscopy (NSOM) to study a formation of Wigner molecules (WMs) in the emission spectra of self-organized InP/GaInP QDs having up to seven electrons. We used a Schottky diode structure for the electrostatic control of the number of the electrons ( N ) in QD, and we observed the emission of the charged excitons (for N < 3) and of the WMs (for N > 2) in the regime of weak Wigner localization. We show, that a contribution of whispering gallery modes (WGMs) of the electrons and rearrangement of the electrons between the WM and WGM states in the QDs, can explain the anomalous dependence of NSOM image size on the quantum confinement observed for some dots.

Nanospectroscopy Imaging Techniques: Using NSOM and TERS for Semiconductor Materials Imaging

In this article, we introduce the theory and instrumentation that is relevant to nanospectroscopy imaging techniques, including near-field scanning optical microscope (NSOM) and tip-enhanced Raman scattering (TERS) imaging. We also demonstrate the NSOM and TERS imaging functions in emiconductor samples. Our findings support the view that NSOM and TERS imaging techniques can increase the space resolution and emphasize the surface information for the target surface layer. Thus, these techniques are applicable to the studies of materials with nanoscale patterns in the future.

Investigation of photoconductivity of individual InAs/GaAs(001) quantum dots by Scanning Near-field Optical Microscopy

The spatial distribution of the photocurrent in the input window plane of a GaAs-based p–i–n photodiode with embedded self-assembled InAs quantum dots (QDs) has been studied with the photoexcitation through a Scanning Near-field Optical Microscope (SNOM) probe at the emission wavelength greater than the intrinsic absorption edge of the host material (GaAs). The inhomogeneities related to the interband absorption in the individual InAs/GaAs(001) QDs have been observed in the photocurrent SNOM images. Thus, the possibility of imaging the individual InAs/GaAs(001) QDs in the photocurrent SNOM images with the lateral spatial resolution ∼ 100 nm (of the same order of magnitude as the SNOM probe aperture size) has been demonstrated.

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.

Wigner molecules and charged excitons in near-field magnetophotoluminescence spectra of self-organized InP/GaInP quantum dots

We used high-spatial-resolution, low-temperature near-field scanning optical microscopy (NSOM) operating at magnetic fields $B=0--10\phantom{\rule{0.16em}{0ex}}\mathrm{T}$ to study the effects of Wigner localization (WL) on emission spectra of single self-organized InP/GaInP quantum dots (QDs) and investigate the stability of singly (trion) and doubly (tetron) charged exciton complexes in the weak quantum confinement regime. Using NSOM measurements together with configuration interaction calculations, we identify the dots having different electron population $\mathrm{N}(\mathrm{N}=1--12)$, quantum confinement $(\ensuremath{\hbar}{\ensuremath{\omega}}_{0}=0.6--8\phantom{\rule{0.16em}{0ex}}\mathrm{meV})$ and size $D(D=70--170\phantom{\rule{0.16em}{0ex}}\mathrm{nm})$. For $\mathrm{N}=2$, we observed a magnetic-field-induced molecular-droplet transition, accompanied by the decomposition of the tetron into a Wigner molecule complex (WMC), and the activation of rotovibronic structure. For $\mathrm{N}=1$, unusually strong vibronic structure resulting from a trion-type WMC was observed. We have shown that magnetic-field-induced shifts of this structure allow measurement of single particle Fock-Darwin levels and angular momentum transitions of the WMC. In addition, we demonstrated the use of NSOM imaging to probe the charge density distribution and observed anomalous dependence of the image size on the quantum confinement, implying a pairing of electrons or formation of whispering gallery modes in the QD. We demonstrated that InP/GaInP QDs, provide a Wigner-Seitz radius $({r}_{s})$ up to 13, and that the measurements of NSOM magneto-optical spectroscopy using these dots makes it possible to study effects arising from strong Coulomb interaction of a few confined electrons (holes).

Use of scanning near-field optical microscope with an aperture probe for detection of luminescent nanodiamonds

The suitability of scanning near-field optical microscopy (SNOM) to image photoluminescent diamond nanoparticles with nanoscale resolution is demonstrated. Isolated diamond nanocrystals with an average size of 100 nm, containing negatively charged nitrogen-vacancy (NV−) centers, were chosen as tested material. The NV− luminescence was stimulated by continuous 532 nm laser light. Sizes of analyzed crystallites were monitored by an atomic force microscope. The lateral resolution of the order of 100 nm was reached in SNOM imaging of diamond nanoparticles using 150 nm square aperture of the probe.

Enhanced Emission from Single Isolated Gold Quantum Dots Investigated Using Two-Photon-Excited Fluorescence Near-Field Scanning Optical Microscopy.

New approaches in molecular nanoscopy are greatly desired for interrogation of biological, organic, and inorganic objects with sizes below the diffraction limit. Our current work investigates emergent monolayer-protected gold quantum dots (nanoclusters, NCs) composed of 25 Au atoms by utilizing two-photon-excited fluorescence (TPEF) near-field scanning optical microscopy (NSOM) at single NC concentrations. Here, we demonstrate an approach to synthesize and isolate single NCs on solid glass substrates. Subsequent investigation of the NCs using TPEF NSOM reveals that, even when they are separated by distances of several tens of nanometers, we can excite and interrogate single NCs individually. Interestingly, we observe an enhanced two-photon absorption (TPA) cross section for single Au25 NCs that can be attributed to few-atom local field effects and to local field-induced microscopic cascading, indicating their potential for use in ultrasensitive sensing, disease diagnostics, cancer cell therapy, and molecular computers. Finally, we report room-temperature aperture-based TPEF NSOM imaging of these NCs for the first time at 30 nm point resolution, which is a ∼5-fold improvement compared to the previous best result for the same technique. This report unveils the unique combination of an unusually large TPA cross section and the high photostability of Au NCs to (non-destructively) investigate stable isolated single NCs using TPEF NSOM. This is the first reported optical study of monolayer-protected single quantum clusters, opening some very promising opportunities in spectroscopy of nanosized objects, bioimaging, ultrasensitive sensing, molecular computers, and high-density data storage.

Magnetic domain structure investigation of Bi: YIG-thin films by combination of AFM and cantilever-based aperture SNOM

We present the results of magnetic domain structure investigation by combination of atomic force microscopy (AFM) and scanning near-field optical microscopy (SNOM). Special hollow-pyramid AFM cantilevers with aperture was used. This combination allows us use same probe for both topography and domain structure visualization of Bi -substituted ferrite garnet films of micro- and nano-meter thickness. Samples were excited through aperture by tightly focused linearly polarized laser beam. Magneto-optical effect rotates polarization of transmitted light depend on domain orientation. Visualization of magnetic domains was performed by detecting cross polarized component of transmitted light. SNOM allows to obtain high resolution magnetic domain image and prevent sample from any disturbance by magnetic probe. Same area SNOM and MFM images are presented.

Optical and mechanical detection of near-field light by atomic force microscopy using a piezoelectric cantilever

In this study, we developed an atomic force microscopy (AFM) system with scanning near-field optical microscopy (SNOM) using a microfabricated force-sensing cantilever with a lead zirconate titanate (PZT) thin film. Both optical and mechanical detection techniques were adopted in SNOM to detect scattered light induced by the interaction of the PZT cantilever tip apex and evanescent light, and SNOM images were obtained for each detection scheme. The mechanical detection technique did allow for a clear observation of the light scattered from the PZT cantilever without the interference observed by the optical detection technique, which used an objective lens, a pinhole, and a photomultiplier tube.

The light-matter interaction of a single semiconducting AlGaN nanowire and noble metal Au nanoparticles in the sub-diffraction limit.

Near field scanning optical microscopy (NSOM) is not only a tool for imaging of sub-diffraction limited objects but also a prominent characteristic tool for understanding the intrinsic properties of nanostructures. In order to understand light-matter interactions in the near field regime using a NSOM technique with an excitation of 532 nm (2.33 eV), we selected an isolated single semiconducting AlGaN nanowire (NW) of diameter ∼120 nm grown via a vapor liquid solid (VLS) mechanism along with a metallic Au nanoparticle (NP) catalyst. The role of electronic transitions from different native defect related energy states of AlGaN is discussed in understanding the NSOM images for the semiconducting NW. The effect of strong surface plasmon resonance absorption of an excitation laser on the NSOM images for Au NPs, involved in the VLS growth mechanism of NWs, is also observed.