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1.
J Synchrotron Radiat ; 26(Pt 5): 1790-1796, 2019 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-31490171

RESUMO

A multimodal imaging instrument has been developed that integrates scanning near-field optical microscopy with nanofocused synchrotron X-ray diffraction imaging. The instrument allows for the simultaneous nanoscale characterization of electronic/near-field optical properties of materials together with their crystallographic structure, facilitating the investigation of local structure-property relationships. The design, implementation and operating procedures of this instrument are reported. The scientific capabilities are demonstrated in a proof-of-principle study of the insulator-metal phase transition in samarium sulfide (SmS) single crystals induced by applying mechanical pressure via a scanning tip. The multimodal imaging of an in situ tip-written region shows that the near-field optical reflectivity can be correlated with the heterogeneously transformed structure of the near-surface region of the crystal.

2.
Opt Express ; 27(10): 13611-13623, 2019 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-31163822

RESUMO

In this letter, we report optical pump terahertz (THz) near-field probe (n-OPTP) and optical pump THz near-field emission (n-OPTE) experiments of graphene/InAs heterostructures. Near-field imaging contrasts between graphene and InAs using these newly developed techniques as well as spectrally integrated THz nano-imaging (THz s-SNOM) are systematically studied. We demonstrate that in the near-field regime (λ/6000), a single layer of graphene is transparent to near-IR (800 nm) optical excitation and completely "screens" the photo-induced far-infrared (THz) dynamics in its substrate (InAs). Our work reveals unique frequency-selective ultrafast dynamics probed at the near field. It also provides strong evidence that n-OPTE nanoscopy yields contrast that distinguishes single-layer graphene from its substrate.

3.
Adv Mater ; 31(27): e1807788, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31074913

RESUMO

van der Waals (vdW) crystals are promising candidates for integrated phase retardation applications due to their large optical birefringence. Among the two major types of vdW materials, the hyperbolic vdW crystals are inherently inadequate for optical retardation applications since the supported polaritonic modes are exclusively transverse-magnetic (TM) polarized and relatively lossy. Elliptic vdW crystals, on the other hand, represent a superior choice. For example, molybdenum disulfide (MoS2 ) is a natural uniaxial vdW crystal with extreme elliptic anisotropy in the frequency range of optical communication. Both transverse-electric (TE) polarized ordinary and TM polarized extraordinary waveguide modes can be supported in MoS2 microcrystals with suitable thicknesses. In this work, low-loss transmission of these guided modes is demonstrated with nano-optical imaging at the near-infrared (NIR) wavelength (1530 nm). More importantly, by combining theoretical calculations and NIR nanoimaging, the modal birefringence between the orthogonally polarized TE and TM modes is shown to be tunable in both sign and magnitude via varying the thickness of the MoS2 microcrystal. This tunability represents a unique new opportunity to control the polarization behavior of photons with vdW materials.

4.
Adv Mater ; 31(24): e1804774, 2019 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-30932221

RESUMO

Infrared and optical spectroscopy represents one of the most informative methods in advanced materials research. As an important branch of modern optical techniques that has blossomed in the past decade, scattering-type scanning near-field optical microscopy (s-SNOM) promises deterministic characterization of optical properties over a broad spectral range at the nanoscale. It allows ultrabroadband optical (0.5-3000 µm) nanoimaging, and nanospectroscopy with fine spatial (<10 nm), spectral (<1 cm-1 ), and temporal (<10 fs) resolution. The history of s-SNOM is briefly introduced and recent advances which broaden the horizons of this technique in novel material research are summarized. In particular, this includes the pioneering efforts to study the nanoscale electrodynamic properties of plasmonic metamaterials, strongly correlated quantum materials, and polaritonic systems at room or cryogenic temperatures. Technical details, theoretical modeling, and new experimental methods are also discussed extensively, aiming to identify clear technology trends and unsolved challenges in this exciting field of research.

5.
J Phys Condens Matter ; 31(24): 24LT01, 2019 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-30870819

RESUMO

Electromagnetic (EM) waves impinging on finite metallic structures can induce non-uniform electrical currents and create oscillating charge densities. These local charges govern the important physical processes such as plasmonic behavior or enhanced Raman scattering. Yet the quantitative calculation and probing of the spatial distribution of the charge density still remain challenging at the subwavelength scale. This is especially the case if one considers the boundary effect, where the charge density can become divergent and conventional finite element methods fail to obtain accurate information. With an approach we recently developed, we calculate this charge density for subwavelength structures with and without sharp corners: gold disks and equilateral triangles. We also devise an independent way to extract the surface charge density distributions from experiments using scattering-type scanning near-field optical microscope (s-SNOM). We found that the charge density [Formula: see text] is related to the near field signal S n by [Formula: see text] With no adjustable parameters, the extracted surface charge distribution from the experiments matches well with that from the theoretical prediction, both in magnitude and phase. Our work provides a quantitative study of the surface charge distributions and a systematic and rigorous treatment to extract surface charge distributions at the nanoscale, opening opportunities for mining the near-field data from s-SNOM.

6.
Adv Mater ; 31(18): e1900251, 2019 May.
Artigo em Inglês | MEDLINE | ID: mdl-30907483

RESUMO

Unlike conventional plasmonic media, polaritonic van der Waals (vdW) materials hold promise for active control of light-matter interactions. The dispersion relations of elementary excitations such as phonons and plasmons can be tuned in layered vdW systems via stacking using functional substrates. In this work, infrared nanoimaging and nanospectroscopy of hyperbolic phonon polaritons are demonstrated in a novel vdW heterostructure combining hexagonal boron nitride (hBN) and vanadium dioxide (VO2 ). It is observed that the insulator-to-metal transition in VO2 has a profound impact on the polaritons in the proximal hBN layer. In effect, the real-space propagation of hyperbolic polaritons and their spectroscopic resonances can be actively controlled by temperature. This tunability originates from the effective change in local dielectric properties of the VO2 sublayer in the course of the temperature-tuned insulator-to-metal phase transition. The high susceptibility of polaritons to electronic phase transitions opens new possibilities for applications of vdW materials in combination with strongly correlated quantum materials.

7.
Adv Sci (Weinh) ; 5(7): 1700982, 2018 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-30027034

RESUMO

Recent progress in ultrafast spectroscopy and semiconductor technology is enabling unique applications in screening, detection, and diagnostics in the Terahertz (T-ray) regime. The promise of efficaciously operation in this spectral region is tempered by the lack of devices that can spectrally analyze samples at sufficient temporal and spatial resolution. Real-time, multispectral T-ray (Mul-T) imaging is reported by designing and demonstrating hyperspectral metamaterial focal plane array (MM-FPA) interfaces allowing multiband (and individually tunable) responses without compromising on the pixel size. These MM-FPAs are fully compatible with existing microfabrication technologies and have low noise when operating in the ambient environment. When tested with a set of frequency switchable quantum cascade lasers (QCLs) for multicolor illumination, both MM-FPAs and QCLs can be tuned to operate at multiple discrete THz frequencies to match analyte "fingerprints." Versatile imaging capabilities are presented, including unambiguous identification of concealed substances with intrinsic and/or human-engineered THz characteristics as well as effective diagnosis of cancerous tissues without notable spectral signatures in the THz range, underscoring the utility of applying multispectral approaches in this compelling wavelength range for sensing/identification and medical imaging.

8.
J Phys Chem Lett ; 9(10): 2546-2553, 2018 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-29706065

RESUMO

Recent inelastic X-ray scattering (IXS) experiments on mesogens have revealed entirely new capabilities with regards to their nanoscale phonon-assisted heat management. Mesogens such as nematic liquid crystals (LCs) are appealing systems for study because their structure and morphology can easily be tuned. We report on Q-resolved ultra-high-resolution IXS, X-ray diffraction, and THz time-domain spectroscopy experiments combined with large-scale all-atom molecular dynamics simulations on the dynamic properties of 5CB LCs. For the first time, we observe a strong mixing of phonon excitations originating from independent in-phase and out-of-phase van-der-Waals-mediated displacement patterns. The coexistence of transverse acoustic and optical modes of 5CB LCs at near room temperature is revealed through the emergent transverse phonon gap and THz light-phonon coupling taking place within the same energy range. Furthermore, our experimental observations are supported by analysis showing correlations of spontaneous fluctuations of LCs on picosecond time scales. These findings are significant for the design of a new generation of soft molecular vibration-sensitive nanoacoustic and optomechanical applications.

9.
Adv Mater ; 30(20): e1705919, 2018 May.
Artigo em Inglês | MEDLINE | ID: mdl-29582487

RESUMO

Precise patterning of polymer-based biomaterials for functional bio-nanostructures has extensive applications including biosensing, tissue engineering, and regenerative medicine. Remarkable progress is made in both top-down (based on lithographic methods) and bottom-up (via self-assembly) approaches with natural and synthetic biopolymers. However, most methods only yield 2D and pseudo-3D structures with restricted geometries and functionalities. Here, it is reported that precise nanostructuring on genetically engineered spider silk by accurately directing ion and electron beam interactions with the protein's matrix at the nanoscale to create well-defined 2D bionanopatterns and further assemble 3D bionanoarchitectures with shape and function on demand, termed "Protein Bricks." The added control over protein sequence and molecular weight of recombinant spider silk via genetic engineering provides unprecedented lithographic resolution (approaching the molecular limit), sharpness, and biological functions compared to natural proteins. This approach provides a facile method for patterning and immobilizing functional molecules within nanoscopic, hierarchical protein structures, which sheds light on a wide range of biomedical applications such as structure-enhanced fluorescence and biomimetic microenvironments for controlling cell fate.

10.
Nat Commun ; 8(1): 2262, 2017 12 22.
Artigo em Inglês | MEDLINE | ID: mdl-29273808

RESUMO

Broadband tunability is a central theme in contemporary nanophotonics and metamaterials research. Combining metamaterials with phase change media offers a promising approach to achieve such tunability, which requires a comprehensive investigation of the electromagnetic responses of novel materials at subwavelength scales. In this work, we demonstrate an innovative way to tailor band-selective electromagnetic responses at the surface of a heavy fermion compound, samarium sulfide (SmS). By utilizing the intrinsic, pressure sensitive, and multi-band electron responses of SmS, we create a proof-of-principle heavy fermion metamaterial, which is fabricated and characterized using scanning near-field microscopes with <50 nm spatial resolution. The optical responses at the infrared and visible frequency ranges can be selectively and separately tuned via modifying the occupation of the 4f and 5d band electrons. The unique pressure, doping, and temperature tunability demonstrated represents a paradigm shift for nanoscale metamaterial and metasurface design.

11.
Nat Commun ; 8(1): 1471, 2017 11 13.
Artigo em Inglês | MEDLINE | ID: mdl-29133779

RESUMO

Most van der Waals crystals present highly anisotropic optical responses due to their strong in-plane covalent bonding and weak out-of-plane interactions. However, the determination of the polarization-dependent dielectric constants of van der Waals crystals remains a nontrivial task, since the size and dimension of the samples are often below or close to the diffraction limit of the probe light. In this work, we apply an optical nano-imaging technique to determine the anisotropic dielectric constants in representative van der Waals crystals. Through the study of both ordinary and extraordinary waveguide modes in real space, we are able to quantitatively determine the full dielectric tensors of nanometer-thin molybdenum disulfide and hexagonal boron nitride microcrystals, the most-promising van der Waals semiconductor and dielectric. Unlike traditional reflection-based methods, our measurements are reliable below the length scale of the free-space wavelength and reveal a universal route for characterizing low-dimensional crystals with high anisotropies.

12.
Adv Sci (Weinh) ; 4(9): 1700191, 2017 09.
Artigo em Inglês | MEDLINE | ID: mdl-28932678

RESUMO

Precise patterning of biomaterials has widespread applications, including drug release, degradable implants, tissue engineering, and regenerative medicine. Patterning of protein-based microstructures using UV-photolithography has been demonstrated using protein as the resist material. The Achilles heel of existing protein-based biophotoresists is the inevitable wide molecular weight distribution during the protein extraction/regeneration process, hindering their practical uses in the semiconductor industry where reliability and repeatability are paramount. A wafer-scale high resolution patterning of bio-microstructures using well-defined silk fibroin light chain as the resist material is presented showing unprecedent performances. The lithographic and etching performance of silk fibroin light chain resists are evaluated systematically and the underlying mechanisms are thoroughly discussed. The micropatterned silk structures are tested as cellular substrates for the successful spatial guidance of fetal neural stems cells seeded on the patterned substrates. The enhanced patterning resolution, the improved etch resistance, and the inherent biocompatibility of such protein-based photoresist provide new opportunities in fabricating large scale biocompatible functional microstructures.

13.
Nano Lett ; 17(9): 5285-5290, 2017 09 13.
Artigo em Inglês | MEDLINE | ID: mdl-28805397

RESUMO

We investigated phonon-polaritons in hexagonal boron nitride-a naturally hyperbolic van der Waals material-by means of the scattering-type scanning near-field optical microscopy. Real-space nanoimages we have obtained detail how the polaritons are launched when the light incident on a thin hexagonal boron nitride slab is scattered by various intrinsic and extrinsic inhomogeneities, including sample edges, metallic nanodisks deposited on its top surface, random defects, and surface impurities. The scanned tip of the near-field microscope is itself a polariton launcher whose efficiency proves to be superior to all the other types of polariton launchers we studied. Our work may inform future development of polaritonic nanodevices as well as fundamental studies of collective modes in van der Waals materials.

14.
Adv Mater ; 29(15)2017 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-28195379

RESUMO

A set of biocompatible, biodegradable, and biofunctionalizable diffractive optical elements (DOEs) using silk proteins as the building materials is reported. The diffraction pattern of a DOE is highly sensitive to the surrounding environment and the structural integrity, offering numerous opportunities for biosensing applications.


Assuntos
Fibroínas/química , Animais , Materiais Biocompatíveis , Bombyx , Dispositivos Ópticos , Seda
15.
Rep Prog Phys ; 80(1): 014501, 2017 01.
Artigo em Inglês | MEDLINE | ID: mdl-27811387

RESUMO

Electronic, magnetic, and structural phase inhomogeneities are ubiquitous in strongly correlated quantum materials. The characteristic length scales of the phase inhomogeneities can range from atomic to mesoscopic, depending on their microscopic origins as well as various sample dependent factors. Therefore, progress with the understanding of correlated phenomena critically depends on the experimental techniques suitable to provide appropriate spatial resolution. This requirement is difficult to meet for some of the most informative methods in condensed matter physics, including infrared and optical spectroscopy. Yet, recent developments in near-field optics and imaging enabled a detailed characterization of the electromagnetic response with a spatial resolution down to 10 nm. Thus it is now feasible to exploit at the nanoscale well-established capabilities of optical methods for characterization of electronic processes and lattice dynamics in diverse classes of correlated quantum systems. This review offers a concise description of the state-of-the-art near-field techniques applied to prototypical correlated quantum materials. We also discuss complementary microscopic and spectroscopic methods which reveal important mesoscopic dynamics of quantum materials at different energy scales.

16.
Nat Commun ; 7: 13079, 2016 10 07.
Artigo em Inglês | MEDLINE | ID: mdl-27713412

RESUMO

Silk protein fibres produced by silkworms and spiders are renowned for their unparalleled mechanical strength and extensibility arising from their high-ß-sheet crystal contents as natural materials. Investigation of ß-sheet-oriented conformational transitions in silk proteins at the nanoscale remains a challenge using conventional imaging techniques given their limitations in chemical sensitivity or limited spatial resolution. Here, we report on electron-regulated nanoscale polymorphic transitions in silk proteins revealed by near-field infrared imaging and nano-spectroscopy at resolutions approaching the molecular level. The ability to locally probe nanoscale protein structural transitions combined with nanometre-precision electron-beam lithography offers us the capability to finely control the structure of silk proteins in two and three dimensions. Our work paves the way for unlocking essential nanoscopic protein structures and critical conditions for electron-induced conformational transitions, offering new rules to design protein-based nanoarchitectures.


Assuntos
Fibroínas/química , Fibroínas/ultraestrutura , Seda/química , Seda/ultraestrutura , Animais , Bombyx/metabolismo , Imagem Tridimensional/métodos , Conformação Molecular , Espectroscopia de Infravermelho com Transformada de Fourier/métodos , Aranhas/metabolismo
17.
Nat Mater ; 15(9): 956-60, 2016 09.
Artigo em Inglês | MEDLINE | ID: mdl-27400387

RESUMO

A major challenge in condensed-matter physics is active control of quantum phases. Dynamic control with pulsed electromagnetic fields can overcome energetic barriers, enabling access to transient or metastable states that are not thermally accessible. Here we demonstrate strain-engineered tuning of La2/3Ca1/3MnO3 into an emergent charge-ordered insulating phase with extreme photo-susceptibility, where even a single optical pulse can initiate a transition to a long-lived metastable hidden metallic phase. Comprehensive single-shot pulsed excitation measurements demonstrate that the transition is cooperative and ultrafast, requiring a critical absorbed photon density to activate local charge excitations that mediate magnetic-lattice coupling that, in turn, stabilize the metallic phase. These results reveal that strain engineering can tune emergent functionality towards proximal macroscopic states to enable dynamic ultrafast optical phase switching and control.

18.
Nano Lett ; 16(2): 1050-5, 2016 Feb 10.
Artigo em Inglês | MEDLINE | ID: mdl-26690855

RESUMO

Active, widely tunable optical materials have enabled rapid advances in photonics and optoelectronics, especially in the emerging field of meta-devices. Here, we demonstrate that spatially selective defect engineering on the nanometer scale can transform phase-transition materials into optical metasurfaces. Using ion irradiation through nanometer-scale masks, we selectively defect-engineered the insulator-metal transition of vanadium dioxide, a prototypical correlated phase-transition material whose optical properties change dramatically depending on its state. Using this robust technique, we demonstrated several optical metasurfaces, including tunable absorbers with artificially induced phase coexistence and tunable polarizers based on thermally triggered dichroism. Spatially selective nanoscale defect engineering represents a new paradigm for active photonic structures and devices.

19.
Nano Lett ; 14(8): 4529-34, 2014 Aug 13.
Artigo em Inglês | MEDLINE | ID: mdl-25046340

RESUMO

We report on time-resolved mid-infrared (mid-IR) near-field spectroscopy of the narrow bandgap semiconductor InAs. The dominant effect we observed pertains to the dynamics of photoexcited carriers and associated surface plasmons. A novel combination of pump-probe techniques and near-field nanospectroscopy accesses high momentum plasmons and demonstrates efficient, subpicosecond photomodulation of the surface plasmon dispersion with subsequent tens of picoseconds decay under ambient conditions. The photoinduced change of the probe intensity due to plasmons in InAs is found to exceed that of other mid-IR or near-IR media by 1-2 orders of magnitude. Remarkably, the required control pulse fluence is as low as 60 µJ/cm(2), much smaller than fluences of ∼ 1-10 mJ/cm(2) previously utilized in ultrafast control of near-IR plasmonics. These low excitation densities are easily attained with a standard 1.56 µm fiber laser. Thus, InAs--a common semiconductor with favorable plasmonic properties such as a low effective mass--has the potential to become an important building block of optically controlled plasmonic devices operating at infrared frequencies.

20.
Nano Lett ; 14(2): 894-900, 2014 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-24479682

RESUMO

Pump-probe spectroscopy is central for exploring ultrafast dynamics of fundamental excitations, collective modes, and energy transfer processes. Typically carried out using conventional diffraction-limited optics, pump-probe experiments inherently average over local chemical, compositional, and electronic inhomogeneities. Here, we circumvent this deficiency and introduce pump-probe infrared spectroscopy with ∼ 20 nm spatial resolution, far below the diffraction limit, which is accomplished using a scattering scanning near-field optical microscope (s-SNOM). This technique allows us to investigate exfoliated graphene single-layers on SiO2 at technologically significant mid-infrared (MIR) frequencies where the local optical conductivity becomes experimentally accessible through the excitation of surface plasmons via the s-SNOM tip. Optical pumping at near-infrared (NIR) frequencies prompts distinct changes in the plasmonic behavior on 200 fs time scales. The origin of the pump-induced, enhanced plasmonic response is identified as an increase in the effective electron temperature up to several thousand Kelvin, as deduced directly from the Drude weight associated with the plasmonic resonances.

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