Electrically Reconfigurable Phase-Change Transmissive Metasurface.

Programmable and reconfigurable optics hold significant potential for transforming a broad spectrum of applications, spanning space explorations to biomedical imaging, gas sensing, and optical cloaking. The ability to adjust the optical properties of components like filters, lenses, and beam steering devices could result in dramatic reductions in size, weight, and power consumption in future optoelectronic devices. Among the potential candidates for reconfigurable optics, chalcogenide-based phase change materials (PCMs) offer great promise due to their non-volatile and analogue switching characteristics. Although PCM have found widespread use in electronic data storage, these memory devices are deeply sub-micron-sized. To incorporate phase change materials into free-space optical components, it is essential to scale them up to beyond several hundreds of microns while maintaining reliable switching characteristics. This study demonstrated a non-mechanical, non-volatile transmissive filter based on low-loss PCMs with a 200 µm×200 µm switching area. The device/metafilter can be consistently switched between low- and high-transmission states using electrical pulses with a switching contrast ratio of 5.5 dB. The device was reversibly switched for 1250 cycles before accelerated degradation took place. The work represents an important step toward realizing free-space reconfigurable optics based on PCMs. This article is protected by copyright. All rights reserved.

Electrically reconfigurable non-volatile metasurface using low-loss optical phase-change material.

Active metasurfaces promise reconfigurable optics with drastically improved compactness, ruggedness, manufacturability and functionality compared to their traditional bulk counterparts. Optical phase-change materials (PCMs) offer an appealing material solution for active metasurface devices with their large index contrast and non-volatile switching characteristics. Here we report a large-scale, electrically reconfigurable non-volatile metasurface platform based on optical PCMs. The optical PCM alloy used in the devices, Ge2Sb2Se4Te (GSST), uniquely combines giant non-volatile index modulation capability, broadband low optical loss and a large reversible switching volume, enabling notably enhanced light-matter interactions within the active optical PCM medium. Capitalizing on these favourable attributes, we demonstrated quasi-continuously tuneable active metasurfaces with record half-octave spectral tuning range and large optical contrast of over 400%. We further prototyped a polarization-insensitive phase-gradient metasurface to realize dynamic optical beam steering.

Reconfigurable all-dielectric metalens with diffraction-limited performance.

Active metasurfaces, whose optical properties can be modulated post-fabrication, have emerged as an intensively explored field in recent years. The efforts to date, however, still face major performance limitations in tuning range, optical quality, and efficiency, especially for non-mechanical actuation mechanisms. In this paper, we introduce an active metasurface platform combining phase tuning in the full 2π range and diffraction-limited performance using an all-dielectric, low-loss architecture based on optical phase change materials (O-PCMs). We present a generic design principle enabling binary switching of metasurfaces between arbitrary phase profiles and propose a new figure-of-merit (FOM) tailored for reconfigurable meta-optics. We implement the approach to realize a high-performance varifocal metalens operating at 5.2 µm wavelength. The reconfigurable metalens features a record large switching contrast ratio of 29.5 dB. We further validate aberration-free and multi-depth imaging using the metalens, which represents a key experimental demonstration of a non-mechanical tunable metalens with diffraction-limited performance.

Broadband transparent optical phase change materials for high-performance nonvolatile photonics.

Optical phase change materials (O-PCMs), a unique group of materials featuring exceptional optical property contrast upon a solid-state phase transition, have found widespread adoption in photonic applications such as switches, routers and reconfigurable meta-optics. Current O-PCMs, such as Ge-Sb-Te (GST), exhibit large contrast of both refractive index (Δn) and optical loss (Δk), simultaneously. The coupling of both optical properties fundamentally limits the performance of many applications. Here we introduce a new class of O-PCMs based on Ge-Sb-Se-Te (GSST) which breaks this traditional coupling. The optimized alloy, Ge2Sb2Se4Te1, combines broadband transparency (1-18.5 µm), large optical contrast (Δn = 2.0), and significantly improved glass forming ability, enabling an entirely new range of infrared and thermal photonic devices. We further demonstrate nonvolatile integrated optical switches with record low loss and large contrast ratio and an electrically-addressed spatial light modulator pixel, thereby validating its promise as a material for scalable nonvolatile photonics.

Highly efficient all-optical beam modulation utilizing thermo-optic effects.

Suspensions of plasmonic nanoparticles can diffract optical beams due to the combination of thermal lensing and self-phase modulation. Here, we demonstrate extremely efficient optical continuous wave (CW) beam switching across the visible range in optimized suspensions of 5-nm Au and Ag nanoparticles in non-polar solvents, such as hexane and decane. On-axis modulation of greater than 30 dB is achieved at incident beam intensities as low as 100 W/cm2 with response times under 200 µs, at initial solution transparency above 70%. No evidence of laser-induced degradation is observed for the highest intensities used. Numerical modeling of experimental data reveals thermo-optic coefficients of up to -1.3 × 10-3 /K, which, to our knowledge, is the highest observed to date in such nanoparticle suspensions.

Optical nondestructive dynamic measurements of wafer-scale encapsulated nanofluidic channels.

Nanofluidic channels are of great interest for DNA sequencing, chromatography, and drug delivery. However, metrology of embedded or sealed nanochannels and measurement of their fill-state have remained extremely challenging. Existing techniques have been restricted to optical microscopy, which suffers from insufficient resolution, or scanning electron microscopy, which cannot measure sealed or embedded channels without cleaving the sample. Here, we demonstrate a novel method for accurately extracting nanochannel cross-sectional dimensions and monitoring fluid filling, utilizing spectroscopic ellipsometric scatterometry, combined with rigorous electromagnetic simulations. Our technique is capable of measuring channel dimensions with better than 5-nm accuracy and assessing channel filling within seconds. The developed technique is, thus, well suited for both process monitoring of channel fabrication as well as for studying complex phenomena of fluid flow through nanochannel structures.

Long-range wetting transparency on top of layered metal-dielectric substrates.

It has been recently shown that scores of physical and chemical phenomena (including spontaneous emission, scattering and Förster energy transfer) can be controlled by nonlocal dielectric environments provided by metamaterials with hyperbolic dispersion and simpler metal/dielectric structures. At this time, we have researched van der Waals interactions and experimentally studied wetting of several metallic, dielectric and composite multilayered substrates. We have found that the wetting angle of water on top of MgF2 is highly sensitive to the thickness of the MgF2 layer and the nature of the underlying substrate that could be positioned as far as ~100 nm beneath the water/MgF2 interface. We refer to this phenomenon as long range wetting transparency. The latter effect cannot be described in terms of the most basic model of dispersion van der Waals-London forces based on pair-wise summation of dipole-dipole interactions across an interface or a gap separating the two media. We infer that the experimentally observed gradual change of the wetting angle with increase of the thickness of the MgF2 layer can possibly be explained by the distance dependence of the Hamaker function (describing the strength of interaction), which originates from retardation of electromagnetic waves at the distances comparable to a wavelength.

In situ microfluidic SERS assay for monitoring enzymatic breakdown of organophosphates.

In this paper, we report on a method to probe the breakdown of the organophosphate (OP) simulants o,s-diethyl methyl phosphonothioate (OSDMP) and demeton S by the enzyme organophosphorous hydrolase (OPH) in a microfluidic device by surface enhanced Raman spectroscopy (SERS). SERS hotspots were formed on-demand inside the microfluidic device by laser-induced aggregation of injected Ag NPs suspensions. The Ag NP clusters, covering micron-sized areas, were formed within minutes using a conventional confocal Raman laser microscope. These Ag NP clusters were used to enhance the Raman spectra of the thiol products of OP breakdown in the microfluidic device: ethanethiol (EtSH) and (ethylsulfanyl) ethane-1-thiol (2-EET). When the OPH enzyme and its substrates OSDMP and demeton S were introduced, the thiolated breakdown products were generated, resulting in changes in the SERS spectra. With the ability to analyze reaction volumes as low as 20 nL, our approach demonstrates great potential for miniaturization of SERS analytical protocols.

Engineered liquid crystal anchoring energies with nanopatterned surfaces.

The anchoring energy of liquid crystals was shown to be tunable by surface nanopatterning of periodic lines and spaces. Both the pitch and height were varied using hydrogen silsesquioxane negative tone electron beam resist, providing for flexibility in magnitude and spatial distribution of the anchoring energy. Using twisted nematic liquid crystal cells, it was shown that this energy is tunable over an order of magnitude. These results agree with a literature model which predicts the anchoring energy of sinusoidal grooves.

Aluminum plasmonics: optimization of plasmonic properties using liquid-prism-coupled ellipsometry.

We have established a method to quantify and optimize the plasmonic behavior of aluminum thin films by coupling spectroscopic ellipsometry into surface plasmon polaritons using a liquid prism cell in a modified Otto configuration. This procedure was applied to Al thin films deposited by four different methods, as well as to single crystal Al substrates, to determine the broadband optical constants and calculate plasmonic figures of merit. The best performance was achieved with Al films that have been sputter-deposited at high temperatures of 350°C, followed by chemical mechanical polishing. This combination of temperature and post-processing produced aluminum films with both large grain size and low surface roughness. Comparing these figures of merit with literature values of gold, silver, and copper shows that at blue and ultraviolet wavelengths, optimized aluminum has the highest figure of merit of all materials studied. We further employ the Ashcroft and Sturm theory of optical conductivity to extract the electron scattering times for the Drude and effective interband transitions, interband transition energies, and the optical mass of electrons.

Mid-infrared photothermal heterodyne spectroscopy in a liquid crystal using a quantum cascade laser.

We report a technique to measure the mid-infrared photothermal response induced by a tunable quantum cascade laser in the neat liquid crystal 4-octyl-4'-cyanobiphenyl (8CB), without any intercalated dye. Heterodyne detection using a Ti:sapphire laser of the response in the solid, smectic, nematic and isotropic liquid crystal phases allows direct detection of a weak mid-infrared normal mode absorption using an inexpensive photodetector. At high pump power in the nematic phase, we observe an interesting peak splitting in the photothermal response. Tunable lasers that can access still stronger modes will facilitate photothermal heterodyne mid-infrared vibrational spectroscopy.

Rational design and optimization of plasmonic nanoarrays for surface enhanced infrared spectroscopy.

We present an approach for rational design and optimization of plasmonic arrays for ultrasensitive surface enhanced infrared absorption (SEIRA) spectroscopy of specific protein analytes. Motivated by our previous work that demonstrated sub-attomole detection of surface-bound silk fibroin [Proc. Natl. Acad. Sci. U.S.A. 106, 19227 (2009)], we introduce here a general framework that allows for the numerical optimization of metamaterial sensor designs in order to maximize the absorbance signal. A critical feature of our method is the explicit compensation for the perturbative effects of the analyte's refractive index which alters the resonance frequency and line-shape of the metamaterial response, thereby leading to spectral distortion in SEIRA signatures. As an example, we leverage our method to optimize the geometry of periodic arrays of plasmonic nanoparticles on both Si and CaF2 substrates. The optimal geometries result in a three-order of magnitude absorbance enhancement compared to an unstructured Au layer, with the CaF2 substrate offering an additional factor of three enhancement in absorbance over a traditional Si substrate. The latter improvement arises from increase of near-field intensity over the Au nanobar surface for the lower index substrate. Finally, we perform sensitivity analysis for our optimized arrays to predict the effects of fabrication imperfections. We find that <20% deviation from the optimized absorbance response is readily achievable over large areas with modern nanofabrication techniques.

Angle-and polarization-dependent collective excitation of plasmonic nanoarrays for surface enhanced infrared spectroscopy.

Our recent work has showed that diffractively coupled nanoplasmonic arrays for Fourier transform infrared (FTIR) microspectroscopy can enhance the Amide I protein vibrational stretch by up to 10(5) times as compared to plain substrates. In this work we consider computationally the impact of a microscope objective illumination cone on array performance. We derive an approach for computing angular- and spatially-averaged reflectance for various numerical aperture (NA) objectives. We then use this approach to show that arrays that are perfectly optimized for normal incidence undergo significant response degradation even at modest NAs, whereas arrays that are slightly detuned from the perfect grating condition at normal incidence irradiation exhibit only a slight drop in performance when analyzed with a microscope objective. Our simulation results are in good agreement with microscope measurements of experimentally optimized periodic nanoplasmonic arrays.