Characterization of just one atom using synchrotron X-rays.

Since the discovery of X-rays by Roentgen in 1895, its use has been ubiquitous, from medical and environmental applications to materials sciences1-5. X-ray characterization requires a large number of atoms and reducing the material quantity is a long-standing goal. Here we show that X-rays can be used to characterize the elemental and chemical state of just one atom. Using a specialized tip as a detector, X-ray-excited currents generated from an iron and a terbium atom coordinated to organic ligands are detected. The fingerprints of a single atom, the L2,3 and M4,5 absorption edge signals for iron and terbium, respectively, are clearly observed in the X-ray absorption spectra. The chemical states of these atoms are characterized by means of near-edge X-ray absorption signals, in which X-ray-excited resonance tunnelling (X-ERT) is dominant for the iron atom. The X-ray signal can be sensed only when the tip is located directly above the atom in extreme proximity, which confirms atomically localized detection in the tunnelling regime. Our work connects synchrotron X-rays with a quantum tunnelling process and opens future X-rays experiments for simultaneous characterizations of elemental and chemical properties of materials at the ultimate single-atom limit.

Dual-band selective circular dichroism in mid-infrared chiral metasurfaces.

Most chiral metamaterials and metasurfaces are designed to operate in a single wavelength band and with a certain circular dichroism (CD) value. Here, mid-infrared chiral metasurface absorbers with selective CD in dual-wavelength bands are designed and demonstrated. The dual-band CD selectivity and tunability in the chiral metasurface absorbers are enabled by the unique design of a unit cell with two coupled rectangular bars. It is shown that the sign of CD in each wavelength band can be independently controlled and flipped by simply adjusting the geometric parameters, the width and the length, of the vertical rectangular bars. The mechanism of the dual-band CD selection in the chiral metasurface absorber is further revealed by studying the electric field and magnetic field distributions of the antibonding and bonding modes supported in the coupled bars under circularly polarized incident light. Furthermore, the chiral resonance wavelength can be continuously increased by scaling up the geometric parameters of the metasurface unit cell. The demonstrated results will contribute to the advance of future mid-infrared applications such as chiral molecular sensing, thermophotovoltaics, and optical communication.

A variable X-ray chopper system for phase-sensitive detection in synchrotron X-ray scanning tunneling microscopy.

An ultra-high-vacuum compatible X-ray chopper system has been designed, constructed and integrated into the XTIP beamline at the Advanced Photon Source at Argonne National Laboratory. The XTIP beamline can operate at soft X-ray energies from 400 eV to 1900 eV while providing a focused beam down to about 10 µm × 10 µm into the synchrotron X-ray scanning tunneling microscopy (SX-STM) endstation instrument. The X-ray chopper is a critical component for separating topographic information from chemical information in SX-STM through phase-sensitive current detection. Depending on the experimental needs, the modulation frequency can be controlled from 100 Hz to 10 kHz. In addition, the chopper system is fully bakeable and can achieve a base pressure of 10-10 mbar. Facilities for active water cooling have been designed, but passive cooling through copper braids has been shown to be sufficient at standard chopping frequencies. Using an Fe/Al2O3/CoAl(111) sample, the separation of the SX-STM current into a chemical component and a stable feedback signal is demonstrated.

XTIP - the world's first beamline dedicated to the synchrotron X-ray scanning tunneling microscopy technique.

In recent years, there have been numerous efforts worldwide to develop the synchrotron X-ray scanning tunneling microscopy (SX-STM) technique. Here, the inauguration of XTIP, the world's first beamline fully dedicated to SX-STM, is reported. The XTIP beamline is located at Sector 4 of the Advanced Photon Source at Argonne National Laboratory. It features an insertion device that can provide left- or right-circular as well as horizontal- and vertical-linear polarization. XTIP delivers monochromatic soft X-rays of between 400 and 1900 eV focused into an environmental enclosure that houses the endstation instrument. This article discusses the beamline system design and its performance.

Plasmon-phonon coupling between mid-infrared chiral metasurfaces and molecular vibrations.

Plasmon-phonon coupling between metamaterials and molecular vibrations provides a new path for studying mid-infrared light-matter interactions and molecular detection. So far, the coupling between the plasmonic resonances of metamaterials and the phonon vibrational modes of molecules has been realized under linearly polarized light. Here, mid-infrared chiral plasmonic metasurfaces with high circular dichroism (CD) in absorption over 0.65 in the frequency range of 50 to 60 THz are demonstrated to strongly interact with the phonon vibrational resonance of polymethyl methacrylate (PMMA) molecules at 52 THz, under both left-handed and right-handed circularly polarized (LCP and RCP) light. The mode splitting features in the absorption spectra of the coupled metasurface-PMMA systems under both circular polarizations are studied in PMMA layers with different thicknesses. The relation between the mode splitting gap and the PMMA thickness is also revealed. The demonstrated results can be applied in areas of chiral molecular sensing, thermal emission, and thermal energy harvesting.

Chiral plasmonic metasurface absorbers in the mid-infrared wavelength range.

Chiral metamaterials in the mid-infrared wavelength range have tremendous potential for studying thermal emission manipulation and molecular vibration sensing. Here, we present one type of chiral plasmonic metasurface absorber with high circular dichroism (CD) in absorption of more than 0.56 across the mid-infrared wavelength range of 5-5.5 µm. The demonstrated chiral metasurface absorbers exhibit a maximum chiral absorption of 0.87 and a maximum CD in absorption of around 0.60. By adjusting the geometric parameters of the unit cell structure of the metasurface, the chiral absorption peak can be shifted to different wavelengths. Due to the strong chiroptical response, the thermal analysis of the designed chiral metasurface absorber further shows the large temperature difference between the left-handed and right-handed circularly polarized light. The demonstrated results can be utilized in various applications such as molecular detection, mid-infrared filter, thermal emission, and chiral imaging.

Broadband infrared circular dichroism in chiral metasurface absorbers.

Chirality is ubiquitous in nature and it is essential in many fields, but natural materials possess weak and narrow-band chiroptical effects. Here, chiral plasmonic metasurface absorbers are designed and demonstrated to achieve large broadband infrared circular dichroism (CD). The broadband chiral absorber is made of multiple double-rectangle resonators with different sizes, showing strong absorption of left-handed or right-handed circularly polarized (LCP or RCP) light above 0.7 and large CD in absorption more than 0.5 covering the wavelength range from 1.35 µm to 1.85 µm. High broadband polarization-dependent local temperature increase is also obtained. The switchable infrared reflective chiral images are further presented by changing the wavelength and polarization of incident light. The broadband chiral metasurface absorbers promise future applications in many areas such as polarization detection, thermophotovoltaics, and chiral imaging.

Nonlinear Mode Coupling and One-to-One Internal Resonances in a Monolayer WS2 Nanoresonator.

Nanomechanical resonators make exquisite force sensors due to their small footprint, low dissipation, and high frequencies. Because the lowest resolvable force is limited by ambient thermal noise, resonators are either operated at cryogenic temperatures or coupled to a high-finesse optical or microwave cavity to reach sub aN Hz-1/2 sensitivity. Here, we show that operating a monolayer WS2 nanoresonator in the strongly nonlinear regime can lead to comparable force sensitivities at room temperature. Cavity interferometry was used to transduce the nonlinear response of the nanoresonator, which was characterized by multiple pairs of 1:1 internal resonance. Some of the modes exhibited exotic line shapes due to the appearance of Hopf bifurcations, where the bifurcation frequency varied linearly with the driving force and forms the basis of the advanced sensing modality. The modality is less sensitive to the measurement bandwidth, limited only by the intrinsic frequency fluctuations, and therefore, advantageous in the detection of weak incoherent forces.

Strong circular dichroism in chiral plasmonic metasurfaces optimized by micro-genetic algorithm.

Strong circular dichroism in absorption in the near-infrared wavelength range is realized by designing binary-pattern chiral plasmonic metasurfaces via the micro-genetic algorithm optimization method. The influence of geometric parameter modifications in the binary-pattern nanostructures on the circular dichroism performance is studied. The strong circular dichroism in absorption is attributed to the simultaneous excitation and field interference of the resonant modes with relative phase delay under linearly polarized incident light. This work provides a universal design method toward the on-demand properties of chiral metasurfaces, which paves the way for future applications in chemical and biological sensing, chiral imaging and spectroscopy.

Near-infrared chiral plasmonic metasurface absorbers.

Chirality plays an essential role in the fields of biology, medicine and physics. However, natural materials exhibit very weak chiroptical response. In this paper, near-infrared chiral plasmonic metasurface absorbers are demonstrated to selectively absorb either the left-handed or right-handed circularly polarized light for achieving large circular dichroism (CD) across the wavelength range from 1.3 µm to 1.8 µm. It is shown that the maximum chiral absorption can reach to 0.87 and that the maximum CD in absorption is around 0.70. The current chiral metasurface design is able to achieve strong chiroptical response, which also leads to high thermal CD for the local temperature increase. The high-contrast reflective chiral images are also realized with the designed metasurface absorbers. The demonstrated chiral metasurface absorbers can be applied in many areas, such as optical filters, thermal energy harvesting, optical communication, and chiral imaging.

Realizing structural color generation with aluminum plasmonic V-groove metasurfaces.

Structural color printing based on all-aluminum plasmonic V-groove metasurfaces is demonstrated under both bright field and dark field illumination conditions. A broad visible color range is realized with the plasmonic V-groove arrays etched on an aluminum surface by simply varying the groove depth while keeping the groove period as a constant. Polarization dependent structural color printing is further achieved with interlaced V-groove arrays along both the horizontal and vertical directions. These results pave the way towards the use of an all-aluminum structural color printing platform for many practical applications such as security marking and information storage.

Local X-ray magnetic circular dichroism study of Fe/Cu(111) using a tunneling smart tip.

Localized spectroscopy with simultaneous topographic, elemental and magnetic information is presented. A synchrotron X-ray scanning tunneling microscope has been employed for the local study of the X-ray magnetic circular dichroism at the Fe L2,3-edges of a thin iron film grown on Cu(111). Polarization-dependent X-ray absorption spectra have been obtained through a tunneling smart tip that serves as a photoelectron detector. In contrast to conventional spin-polarized scanning tunneling microscopy, X-ray excitations provide magnetic contrast even with a non-magnetic tip. Intensity variations in the photoexcited tip current point to chemical variations within a single magnetic Fe domain.

All-metal structural color printing based on aluminum plasmonic metasurfaces.

An all-metal structural color printing platform based on aluminum plasmonic metasurfaces is proposed and demonstrated with high color performance using only a one-step etching process on aluminum surface. A wide visible color range is realized with the designed metallic square-shaped disk arrays by simply adjusting the geometrical parameters of the disk etching depth, disk width and unit cell period. The demonstrated all-metal microscale structural color printing on aluminum surface offers great potential for many practical color related applications.

Analyzing Single Giant Unilamellar Vesicles With a Slotline-Based RF Nanometer Sensor.

Novel techniques that enable reagent free detection and analysis of single cells are of great interest for the development of biological and medical sciences as well as point-of-care health service technologies. Highly sensitive and broadband radio-frequency (RF) sensors are promising candidates for such a technique. In this work, we present a highly sensitive and tunable RF sensor, which is based on interference processes and built with a 100 nm slotline structure. The highly concentrated RF fields, up to ~1.76×107 V/m, enable strong interactions between Giant unilamellar vesicles (GUVs) and fields for high sensitivity operations. We also provide two modeling approaches to extract cell dielectric properties from measured scattering parameters. GUVs of different molecular compositions are synthesized and analyzed with the RF sensor at ~2 GHz, ~2.5 GHz, and ~2.8 GHz with an initial |S21 | min of ~-100 dB. Corresponding GUV dielectric properties are obtained. A one-dimensional scanning of single GUV is also demonstrated.

Enhanced structural color generation in aluminum metamaterials coated with a thin polymer layer.

A high-resolution and angle-insensitive structural color generation platform is demonstrated based on triple-layer aluminum-silica-aluminum metamaterials supporting surface plasmon resonances tunable across the entire visible spectrum. The color performances of the fabricated aluminum metamaterials can be strongly enhanced by coating a thin transparent polymer layer on top. The results show that the presence of the polymer layer induces a better impedance matching for the plasmonic resonances to the free space so that strong light absorption can be obtained, leading to the generation of pure colors in cyan, magenta, yellow and black (CMYK) with high color saturation.

Aluminum plasmonic metamaterials for structural color printing.

We report a structural color printing platform based on aluminum plasmonic metamaterials supporting near perfect light absorption and narrow-band spectral response tunable across the visible spectrum to realize high-resolution, angle-insensitive color printing with high color purity and saturation. Additionally, the fabricated metamaterials can be protected by a transparent polymer thin layer for ambient use with further improved color performance. The demonstrated structural color printing with aluminum plasmonic metamaterials offers great potential for relevant applications such as security marking and information storage.

Broadband perfect absorber based on one ultrathin layer of refractory metal.

Broadband perfect absorber based on one ultrathin layer of the refractory metal chromium without structure patterning is proposed and demonstrated. The ideal permittivity of the metal layer for achieving broadband perfect absorption is derived based on the impedance transformation method. Since the permittivity of the refractory metal chromium matches this ideal permittivity well in the visible and near-infrared range, a silica-chromium-silica three-layer absorber is fabricated to demonstrate the broadband perfect absorption. The experimental results under normal incidence show that the absorption is above 90% over the wavelength range of 0.4-1.4 µm, and the measurements under angled incidence within 400-800 nm prove that the absorber is angle-insensitive and polarization-independent.

Elemental fingerprinting of materials with sensitivity at the atomic limit.

By using synchrotron X-rays as a probe and a nanofabricated smart tip of a tunneling microscope as a detector, we have achieved chemical fingerprinting of individual nickel clusters on a Cu(111) surface at 2 nm lateral resolution, and at the ultimate single-atomic height sensitivity. Moreover, by varying the photon energy, we have succeeded to locally measure photoionization cross sections of just a single Ni nanocluster, which opens new exciting opportunities for chemical imaging of nanoscale materials.

Experimental demonstration of near-infrared epsilon-near-zero multilayer metamaterial slabs.

Near-infrared epsilon-near-zero (ENZ) metamaterial slabs based on silver-germanium (Ag-Ge) multilayers are experimentally demonstrated. Transmission, reflection and absorption spectra are characterized and used to determine the complex refractive indices and the effective permittivities of the ENZ metamaterial slabs, which match the results obtained from both the numerical simulations and the optical nonlocalities analysis. A rapid post-annealing process is used to reduce the collision frequency of silver and therefore decrease the optical absorption loss of multilayer metamaterial slabs. Furthermore, multilayer grating structures are studied to enhance the optical transmission and also tune the location of ENZ wavelength. The demonstrated near-infrared ENZ multilayer metamaterial slabs are important for realizing many exotic applications, such as phase front shaping and engineering of photonic density of states.

A universal metasurface transfer technique for heterogeneous integration.

Metasurfaces offer a versatile platform for engineering the wavefront of light using nanostructures with subwavelength dimensions and hold great promise for dramatically miniaturizing conventional optical elements due to their small footprint and broad functionality. However, metasurfaces so far have been mainly demonstrated on bulky and planar substrates that are often orders of magnitude thicker than the metasurface itself. Conventional substrates not only nullify the reduced footprint advantage of metasurfaces, but also limit their application scenarios. The bulk substrate also determines the metasurface dielectric environment, with potentially undesired optical effects that undermine the optical performance. Here we develop a universal polymer-assisted transfer technique to tackle this challenge by decoupling the substrate employed on the fabrication of metasurfaces from that used for the target application. As an example, Huygens' metasurfaces with 120 nm thickness in the visible range (532 nm) are demonstrated to be transferred onto a 100 nm thick freestanding SiNx membrane while maintaining excellent structural integrity and optical performance of diffraction-limited focusing. This transfer method not only enables the thinnest dielectric metalens to the best of our knowledge, but also opens up new opportunities in integrating cascaded and multilayer metasurfaces, as well as the heterogeneous integration with nonconventional substrates and various electronic/photonic devices.