散射式太赫兹扫描近场光学显微技术研究

基于散射式近场探测原理,设计并搭建了散射式太赫兹扫描近场光学显微系统(THz s-SNOM),实现了纳米量级空间分辨率的太赫兹近场显微成像测量。该系统以输出频率范围为0.1~0.3THz的太赫兹倍频模块为发射源,通过纳米探针的针尖产生纳米光源与样品相互作用,并将样品表面的倏逝波转化为可在远场测量的辐射波。通过探针逐点扫描样品表面,同时获得了样品表面的形貌图和太赫兹近场显微图。该系统的显微分辨率取决于探针针尖的曲率半径,而与太赫兹波的波长无关。使用该系统测量了金薄膜/硅衬底样品和石墨烯样品的近场显微图,结果表明,近场显微的空间分辨率优于60nm,波长与空间分辨率之比高达λ/26000。     

Nano-slit probes for near-field optical microscopy fabricated by focused ion beams

The near-field probes described in this paper are based on metallized non-contact atomic force microscope cantilevers made of silicon. For application in high-resolution near-field optical/infrared microscopy, we use aperture probes with the aperture being fabricated by focused ion beams. This technique allows us to create apertures of sub-wavelength dimensions with different geometries. In this paper we present the use of slit-shaped apertures which show a polarization-dependent transmission efficiency and a lateral resolution of < 100 nm at a wavelength of 1064 nm. As a test sample to characterize the near-field probes we investigated gold/palladium structures, deposited on an ultrathin chromium sublayer on a silicon wafer, in constant-height mode.     

太赫兹近场光学亚表面检测技术研究

研究了太赫兹散射式扫描近场光学显微镜（Terahertz scattering-type scanning near-field optical microscopy,THz s-SNOM）对亚表面金属微纳结构的显微成像检测。首次采用自主搭建的THz s-SNOM系统对表面覆盖了六方氮化硼薄膜的金微米线进行太赫兹近场显微测量,获得了具有纳米量级空间分辨率和较高对比度的近场显微图。结合全波数值模拟,分析了THz s-SNOM探测亚表面金属微纳结构的空间分辨率、近场散射信号强度和成像对比度。研究表明,THz s-SNOM具有优良的亚表面显微成像检测能力,可应用于微纳电子器件的亚表面结构表征和缺陷检测。     

Mid-infrared scanning near-field optical microscope resolves 30 nm

We explore the performance of a scanning near-field infrared microscope, which works by scattering tightly focused CO₂ laser radiation (λ = 10  μ m) from the apex of a metallized atomic force microscope tip. The infrared images of test samples prove a spatial resolution of 30 nm and are free of topographical and inertial artefacts, thus they should be of great interest for practical applications. We also observe that the infrared contrast vanishes when the input beam polarization is orthogonal to the tip axis, in accordance with theoretical expectations for a mechanism of longitudinal field interaction.     

Polarization contrast in reflection near-field optical microscopy with uncoated fibre tips

Using cross-hatched, patterned semiconductor surfaces and round 20-nm-thick gold pads on semiconductor wafers, we investigate the imaging characteristics of a reflection near-field optical microscope with an uncoated fibre tip for different polarization configurations and light wavelengths. It is shown that cross-polarized detection allows one to effectively suppress far-field components in the detected signal and to realize imaging of optical contrast on the sub-wavelength scale. The sensitivity window of our microscope, i.e. the scale on which near-field optical images represent mainly optical contrast, is found to be ≈100 nm for light wavelengths in the visible region. We demonstrate imaging of near-field components of a dipole field and purely dielectric contrast (related to well-width fluctuations in a semiconductor quantum well) with a spatial resolution of ≈100 nm. The results obtained show that such a near-field technique can be used for polarization-sensitive imaging with reasonably high spatial resolution and suggest a number of applications for this technique.     

Fluorescence anisotropy near-field scanning optical microscopy (FANSOM): a new technique for nanoscale microviscometry

A near-field scanning optical microscope system was implemented and adapted for nanoscale steady-state fluorescence anisotropy measurement. The system as implemented can resolve 0.1 cP microviscosity variations with a resolution of 250 nm laterally in the near field, or 10 μm when employed in a vertical scanning mode. The system was initially used to investigate the extent of microviscous vicinal water over surfaces of varying hydrophilicity. Water above a cleaved mica surface was found to have a decreased microviscosity, while water above a hydrophobic surface showed no change (detection limit 0.1 cP at 30+ nm from the surface).     

Single molecule mapping of the optical field distribution of probes for near-field microscopy

The most difficult task in near-field scanning optical microscopy (NSOM) is to make a high quality subwavelength aperture probe. Recently, we have developed high definition NSOM probes by focused ion beam (FIB) milling. These probes have a higher brightness, better polarization characteristics, better aperture definition and a flatter end face than conventional NSOM probes. We have determined the quality of these probes in four independent ways: by FIB imaging and by shear-force microscopy (both providing geometrical information), by far-field optical measurements (yielding throughput and polarization characteristics), and ultimately by single molecule imaging in the near-field. In this paper, we report on a new method using shear-force microscopy to study the size of the aperture and the end face of the probe (with a roughness smaller than 1.5 nm). More importantly, we demonstrate the use of single molecules to measure the full three-dimensional optical near-field distribution of the probe with molecular spatial resolution. The single molecule images exhibit various intensity patterns, varying from circular and elliptical to double arc and ring structures, which depend on the orientation of the molecules with respect to the probe. The optical resolution in the measurements is not determined by the size of the aperture, but by the high optical field gradients at the rims of the aperture. With a 70 nm aperture probe, we obtain fluorescence field patterns with 45 nm FWHM. Clearly, this unprecedented near-field optical resolution constitutes an order of magnitude improvement over far-field methods like confocal microscopy.     

Nano-slit probes for near-field optical microscopy fabricated by focused ion beams

The near-field probes described in this paper are based on metallized non-contact atomic force microscope cantilevers made of silicon. For application in high-resolution near-field optical/infrared microscopy, we use aperture probes with the aperture being fabricated by focused ion beams. This technique allows us to create apertures of sub-wavelength dimensions with different geometries. In this paper we present the use of slit-shaped apertures which show a polarization-dependent transmission efficiency and a lateral resolution of < 100 nm at a wavelength of 1064 nm. As a test sample to characterize the near-field probes we investigated gold/palladium structures, deposited on an ultrathin chromium sublayer on a silicon wafer, in constant-height mode.     

Magneto-optical near-field microscopy of ultrathin films in ultrahigh vacuum

In this study, guiding of surface plasmon polaritons excited at a gold film surface along corrugation‐free channels in regions that are covered with randomly located surface scatterers, is considered using near‐field microscopy for imaging of surface plasmon polariton intensity distributions at the surface. In the wavelength range 713–815 nm, we observed complete inhibition of the surface plasmon polariton propagation inside the random structures composed of individual (≈ 70 nm high) gold bumps (and their clusters) placed on a 55 nm thick gold film with a bump density of 75 µm^?2. We demonstrate well‐defined surface plasmon polariton guiding along corrugation‐free 2 µm wide channels in random structures and, in the wavelength range 738–774 nm, low‐loss guiding around 20° bends having a bend radius of ≈ 15 µm.     

Optical microcantilever consisting of channel waveguide for scanning near-field optical microscopy controlled by atomic force

We develop a novel optical microcantilever for scanning near-field optical microscopy controlled by atomic force mode (SNOM/AFM). The optical microcantilever has the bent channel waveguide, the corner of which acts as aperture with a large tip angle. The resonance frequency of the optical microcantilever is 9 kHz, and the spring constant is estimated to be 0.59 N/m. The optical microcantilever can be operated in contact mode of SNOM/AFM and we obtain the optical resolution of about 200 nm, which is as same size as the diameter of aperture. We confirm that the throughput of optical microcantilever with an aperture of 170 nm diameter would be improved to be more than 10⁻⁵.     

Fluorescence imaging with a laser trapping scanning near-field optical microscope

We investigated fluorescence imaging using a near-field scanning optical microscope which uses a laser-stabilized gold nanoparticle as a near-field probe. This microscope is suitable for observations of biological specimens in aqueous solutions because the probe particle is held by a noncontact force exerted by a laser beam. Theoretical calculations based on Mie scattering theory are presented to evaluate the near-field enhancement by a gold particle of 40 nm diameter. We also present fluorescence images of a single fluorescent bead and discuss the near-field contribution to the fluorescence image in this type of microscope.     

Femtosecond near-field spectroscopy: carrier relaxation and transport in single quantum wires

Quasi-two-colour femtosecond pump and probe spectroscopy and near-field scanning optical microscopy are combined to study the carrier dynamics in single semiconductor nanostructures. In temporally, spectrally and spatially resolved measurements with a time resolution of 200 fs and a spatial resolution of 200 nm, the non-linear change in reflectivity of a single quantum wire is mapped in real space and time. The experiments show that carrier relaxation into a single quantum wire occurs on a 100 fs time scale at room temperature. Evidence is given for a transient unipolar electron transport along the wire axis on a picosecond time and 100 nm length scale.     

Evaluation of nano-optical probe from scanning near-field optical microscope images

We studied a nanometre-sized optical probe in a scanning near-field optical microscope. The probe profile is determined by using a knife-edge method and a modulated transfer function evaluation method which uses nanometre-sized line-and-space tungsten patterns (with spaces 1 μm to 50 nm apart) on SiO₂ substrates. The aluminium-covered, pipette-pulled fibre probe used here has two optical probes: one with a large diameter (350 nm) and the other with a small diameter (10 nm). The small-diameter probe has an optical intensity ≈63 times larger than that of the large-diameter probe, but the power is about 1/25 of that of the large probe.     

Near-field second harmonic imaging of the c/a/c/a polydomain structure of epitaxial PbZrxTi1–xO3 thin films

Near-field optical second harmonic microscopy has been applied to imaging of the c/a/c/a polydomain structure of epitaxial PbZr _x Ti_{1– x} O₃ thin films in the 0 <  x  < 0.4 range. Comparison of the near-field optical images and the results of atomic force microscopy and X-ray diffraction studies show that an optical resolution of the order of 100 nm is achieved. Symmetry properties of the near-field second harmonic signal allow us to obtain good optical contrast between the local second harmonic generation in c- and a-domains. Experimentally measured near-field second harmonic images have been compared with the results of theoretical calculations. Good agreement between theory and experiment is demonstrated.     

Imaging 'intact' myofibrils with a near-field scanning optical microscope

Fluorescently labelled myofibrils were imaged in physiological salt solution by near-field scanning optical microscopy and shear-force microscopy. These myofibrils were imaged in vitro , naturally adhering to glass while retaining their ability to contract. The Z-line protein structure of the myofibrils was antibody labelled and easily identified in the near-field fluorescence images. The distinctive protein banding structure of the myofibril was also seen clearly in the shear-force images without any labelling requirement. With the microscope in the transmission mode, resolution of the fluorescence images was degraded significantly by excessive specimen thickness (>1 μm), whereas the shear-force images were less affected by specimen thickness and more affected by poor adherence to the substrate. Although the exact mechanism generating contrast in the shear-force images is still unknown, shear-force imaging appears to be a promising new imaging modality.     

Inducing superconductivity at a nanoscale: photodoping with a near-field scanning optical microscope

The local modification of an insulating GdBa₂Cu₃O_6.5 thin film, made superconducting by illumination with a near-field scanning optical microscope (NSOM), is reported. A 100-nm aperture NSOM probe acts as a sub-wavelength light source of wavelength λ_exc = 480–650 nm, locally generating photocarriers in an otherwise insulating GdBa₂–Cu₃O_6.5 thin film. Of the photogenerated electron–hole pairs, electrons are trapped in the crystallographic lattice, defining an electrostatic confining potential to enable the holes to move. Reflectance measurements at λ = 1.55 μm at room temperature show that photocarriers can be induced and constrained to move on a ≈200 nm scale for all investigated λ_exc. Photogenerated wires present a superconducting critical temperature T _c = 12 K with a critical current density J _c = 10⁴ A cm⁻². Exploiting the flexibility provided by photodoping through a NSOM probe, a junction was written by photodoping a wire with a narrow (≈ 50 nm) under-illuminated gap. The strong magnetic field modulation of the critical current provides a clear signature of the existence of a Josephson effect in the junction.     

Writing subwavelength-sized structures into aluminium films by thermo-chemical aperture-less near-field optical microscopy

An optical near-field at the tip of an atomic force microscope probe is utilised to pattern aluminium thin films on glass substrates by photo-thermally induced corrosion in water. Aluminium forms a thin passivating oxide layer when immersed into neutral water at room temperature. Owing to the high energy density of the near-field, the metal below the probe tip can be heated to 100°C due to absorption of the light, which then provokes breakdown of the passivation and metal corrosion. The localised near-field is generated by tip-induced enhancement of an evanescent field originating from a laser beam, that is totally internally reflected at the glass–aluminium–water interface. The process is governed by surface plasmons excited in the aluminium film by the evanescent waves and the field enhancement of the probe tip. Holes of 40 nm diameter and lines below 100 nm width have been written into a 20-nm-thick aluminium film. Applications of the scanning probe lithography process may include the one-step fabrication of point contacts or contact masks for near-field optical lithography and reactive ion etching.     

Nanometric patterning of zinc by optical near-field photochemical vapour deposition

A new technique, optical near-field photochemical vapour deposition (NFO-PCVD) enables maskless production of nanometric structures with controllable size, chemical composition and morphology. By placing a near-field optical microscope inside the reaction chamber for photochemical vapour deposition we have deposited nanoscale metal patterns. We demonstrate for the first time, successfully deposited in the near-field region, lines of metallic zinc with the observed stripe width of 20 nm.     

Spectroscopic scanning near-field optical microscopy with a free electron laser: CH2 bond imaging in diamond films

Hydrogen chemistry in thin films and biological systems is one of the most difficult experimental problems in today's science and technology. We successfully tested a novel solution, based on the spectroscopic version of scanning near-field optical microscopy (SNOM). The tunable infrared radiation of the Vanderbilt free electron laser enabled us to reveal clearly hydrogen-decorated grain boundaries on nominally hydrogen-free diamond films. The images were obtained by SNOM detection of reflected 3.5 µm photons, corresponding to the C–H stretch absorption, and reached a lateral resolution of 0.2 µm, well below the λ/2 (λ= wavelength) limit of classical microscopy.     

单层MoS2和WS2的太赫兹近场显微成像研究

采用太赫兹散射式扫描近场光学显微镜(THz s-SNOM)研究了化学气相沉积法制备的单层MoS₂和WS₂晶粒的太赫兹近场响应。在没有可见光激发时,未探测到可分辨的太赫兹近场响应,说明晶粒具有较低的掺杂载流子浓度。有可见光激发时,由于光生载流子的太赫兹近场响应,能够测得与晶粒轮廓完全吻合的太赫兹近场显微图。在相同的光激发条件下,MoS₂的太赫兹近场响应强于WS₂,反映了两者之间载流子浓度或迁移率的差异。研究结果表明,THz s-SNOM兼具超高的空间分辨率和对光生载流子的灵敏探测能力,对二维半导体材料和器件光电特性的微观机理研究具有独特的优势。