Study of Elastic and Structural Properties of BaFe2As2 Ultrathin Film Using Picosecond Ultrasonics.

We obtain the through-thickness elastic stiffness coefficient (C33) in nominal 9 nm and 60 nm BaFe2As2 (Ba-122) thin films by using picosecond ultrasonics. Particularly, we reveal the increase in elastic stiffness as film thickness decreases from bulk value down to 9 nm, which we attribute to the increase in intrinsic strain near the film-substrate interface. Our density functional theory (DFT) calculations reproduce the observed acoustic oscillation frequencies well. In addition, temperature dependence of longitudinal acoustic (LA) phonon mode frequency for 9 nm Ba-122 thin film is reported. The frequency change is attributed to the change in Ba-122 orthorhombicity (a-b)/(a+b). This conclusion can be corroborated by our previous ultrafast ellipticity measurements in 9 nm Ba-122 thin film, which exhibit strong temperature dependence and indicate the structural phase transition temperature Ts.

Wavelength conversion through plasmon-coupled surface states.

Surface states generally degrade semiconductor device performance by raising the charge injection barrier height, introducing localized trap states, inducing surface leakage current, and altering the electric potential. We show that the giant built-in electric field created by the surface states can be harnessed to enable passive wavelength conversion without utilizing any nonlinear optical phenomena. Photo-excited surface plasmons are coupled to the surface states to generate an electron gas, which is routed to a nanoantenna array through the giant electric field created by the surface states. The induced current on the nanoantennas, which contains mixing product of different optical frequency components, generates radiation at the beat frequencies of the incident photons. We utilize the functionalities of plasmon-coupled surface states to demonstrate passive wavelength conversion of nanojoule optical pulses at a 1550 nm center wavelength to terahertz regime with efficiencies that exceed nonlinear optical methods by 4-orders of magnitude.

A light-induced phononic symmetry switch and giant dissipationless topological photocurrent in ZrTe5.

Dissipationless currents from topologically protected states are promising for disorder-tolerant electronics and quantum computation. Here, we photogenerate giant anisotropic terahertz nonlinear currents with vanishing scattering, driven by laser-induced coherent phonons of broken inversion symmetry in a centrosymmetric Dirac material ZrTe5. Our work suggests that this phononic terahertz symmetry switching leads to formation of Weyl points, whose chirality manifests in a transverse, helicity-dependent current, orthogonal to the dynamical inversion symmetry breaking axis, via circular photogalvanic effect. The temperature-dependent topological photocurrent exhibits several distinct features: Berry curvature dominance, particle-hole reversal near conical points and chirality protection that is responsible for an exceptional ballistic transport length of ~10 µm. These results, together with first-principles modelling, indicate two pairs of Weyl points dynamically created by B1u phonons of broken inversion symmetry. Such phononic terahertz control breaks ground for coherent manipulation of Weyl nodes and robust quantum transport without application of static electric or magnetic fields.

Light management in perovskite solar cells and organic LEDs with microlens arrays.

We demonstrate enhanced absorption in solar cells and enhanced light emission in OLEDs by light interaction with a periodically structured microlens array. We simulate n-i-p perovskite solar cells with a microlens at the air-glass interface, with rigorous scattering matrix simulations. The microlens focuses light in nanoscale regions within the absorber layer enhancing the solar cell. Optimal period of ~700 nm and microlens height of ~800-1000 nm, provides absorption (photocurrent) enhancement of 6% (6.3%). An external polymer microlens array on the air-glass side of the OLED generates experimental and theoretical enhancements >100%, by outcoupling trapped modes in the glass substrate.

Reducing optical losses in organic solar cells using microlens arrays: theoretical and experimental investigation of microlens dimensions.

The performance of organic photovoltaic devices is improving steadily and efficiencies have now exceeded 10%. However, the incident solar spectrum still largely remains poorly absorbed. To reduce optical losses, we employed a microlens array (MLA) layer on the side of the glass substrate facing the incident light; this approach does not interfere with the processing of the active-layer. We observed up to 10% enhancement in the short circuit current of poly({4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl}{3-fluoro-2-[(2-ethylhexyl)carbonyl] thieno[3,4-b]thiophenediyl}):(6,6)-phenyl C71-butyric acid methyl ester (PTB7:PC71BM) OPV cells. Theoretically and experimentally investigating several MLA dimensions, we found that photocurrent increases with the ratio of the height to the pitch size of MLA. Simulations reveal the enhancement mechanisms: MLA focuses light, and also increases the light path within the active-layer by diffraction. Photocurrent enhancements increase for a polymer system with thinner active-layers, as demonstrated in poly[N-9'-heptadecanyl-2,7-carbazole-alt-5,5-(4',7'-di-2-thienyl-2',1',3'-benzothiadiazole)] (PCDTBT):PC71BM OPVs with 17% improvement in short circuit current.

Oxygen and relative humidity monitoring with films tailored for enhanced photoluminescence.

Approaches to generate porous or doped sensing films, which significantly enhance the photoluminescence (PL) of oxygen optical sensors, and thus improve the signal-to-noise (S/N) ratio, are presented. Tailored films, which enable monitoring the relative humidity (RH) as well, are also presented. Effective porous structures, in which the O2-sensitive dye Pt octaethylporphyrin (PtOEP) or the Pd analog PdOEP was embedded, were realized by first generating blend films of polyethylene glycol (PEG) with polystyrene (PS) or with ethyl cellulose (EC), and then immersing the dried films in water to remove the water-soluble PEG. This approach creates pores (voids) in the sensing films. The dielectric contrast between the films' constituents and the voids increases photon scattering, which in turn increases the optical path of the excitation light within the film, and hence light absorption by the dye, and its PL. Optimized sensing films with a PEG:PS ratio of 1:4 (PEG's molecular weight Mw ∼8000) led to ∼4.4× enhancement in the PL (in comparison to PS films). Lower Mw ∼200 PEG with a PEG:EC ratio of 1:1 led to a PL enhancement of ∼4.7×. Film-dependent PL enhancements were observed at all oxygen concentrations. The strong PL enhancement enables (i) using lower dye (luminophore) concentrations, (ii) reducing power consumption and enhancing the sensor's operational lifetime when using organic light emitting diodes (OLEDs) as excitation sources, (iii) improving performance when using compact photodetectors with no internal gain, and (iv) reliably extending the dynamic range. The effect of RH on O2 sensing is also presented. Dye:EC films are sensitive to the RH, as shown by the change of the dye's PL decay time with RH at a given O2 concentration. Surprisingly, this RH sensitivity vanishes by adding PEG to EC, including by washing PEG off. In contrast, doping EC with TiO2 nanoparticles maintains the RH effect with the advantage of significant PL enhancement. This enhancement enables differentiation of <10% changes in the RH, which is unattained with the dye:EC sensing films. The results are discussed in terms of the composition, thickness, and microstructure, whether porous or nanoparticle doped, of the composite films.

Metal-nanowall grating transparent electrodes: achieving high optical transmittance at high incident angles with minimal diffraction.

A novel architecture has been employed to fabricate transparent electrodes with high conductivity and high optical transmittance at high incident angles. Soft lithography is used to fabricate polymer grating patterns onto which thin metallic films are deposited. Etching removes excess metal leaving tall walls of metal. Polymer encapsulation of the structure both protects the metal and minimizes diffraction. Transmission is dependent upon the height of the walls and encapsulation and varies from 60% to 80% for structures with heights of 1400 nm to 300 nm. In encapsulated structures, very little distortion is visible (either parallel to or perpendicular to standing walls) even at viewing angles 60° from the normal. Diffraction is at characterized through measurement of intensity for zeroth through third order diffraction spots. Encapsulation is shown to significantly reduce diffraction. Measurements are supported by optical simulations.

Microlens array induced light absorption enhancement in polymer solar cells.

Over the last decade, polymer solar cells (PSCs) have attracted a lot of attention and highest power conversion efficiencies (PCE) are now close to 10%. Here we employ an optical structure - the microlens array (MLA) - to increase light absorption inside the active layer, and PCE of PSCs increased even for optimized devices. Normal incident light rays are refracted at the MLA and travel longer optical paths inside the active layers. Two PSC systems - poly(3-hexylthiophene-2,5-diyl):(6,6)-phenyl C61 butyric acid methyl ester (P3HT:PCBM) and poly[[9-(1-octylnonyl)-9H-carbazole-2,7-diyl]-2,5-thiophenediyl-2,1,3-benzothiadiazole-4,7-diyl-2,5-thiophenediyl]:(6,6)-phenyl C71 butyric acid methyl ester (PCDTBT:PC70BM) - were investigated. In the P3HT:PCBM system, MLA increased the absorption, absolute external quantum efficiency, and the PCE of an optimized device by ∼4.3%. In the PCDTBT:PC70BM system, MLA increased the absorption, absolute external quantum efficiency, and PCE by more than 10%. In addition, simulations incorporating optical parameters of all structural layers were performed and they support the enhancement of absorption in the active layer with the assistance of MLA. Our results show that utilizing MLA is an effective strategy to further increase light absorption in PSCs, in which optical losses account for ∼40% of total losses. MLA also does not pose materials processing challenges to the active layers since it is on the other side of the transparent substrate.

Microporous phase-separated films of polymer blends for enhanced outcoupling of light from OLEDs.

Thin microporous films were formed by dropcasting a toluene solution containing various ratios of polystyrene:polyethylene glycol blends on a glass substrate, with OLEDs on the ITO that coated the opposite side of that substrate. We demonstrate for the first time that such easily-fabricated films with surface and bulk micropores in the index-matching polystyrene can serve as random microlens-like arrays to improve forward OLED light extraction by up to ~60%. A theoretical interpretation of the angular emission profile of the device, considering the geometrical change at the substrate/air interface and the scattering by the pores within the films, was established in excellent agreement with the experiments. The use of such blended thin films provides an economical method, independent of the OLED fabrication technique, for improving the outcoupling efficiency.

Soft holographic interference lithography microlens for enhanced organic light emitting diode light extraction.

Very uniform 2 µm-pitch square microlens arrays (µLAs), embossed on the blank glass side of an indium-tin-oxide (ITO)-coated 1.1 mm-thick glass, are used to enhance light extraction from organic light-emitting diodes (OLEDs) by ~100%, significantly higher than enhancements reported previously. The array design and size relative to the OLED pixel size appear to be responsible for this enhancement. The arrays are fabricated by very economical soft lithography imprinting of a polydimethylsiloxane (PDMS) mold (itself obtained from a Ni master stamp that is generated from holographic interference lithography of a photoresist) on a UV-curable polyurethane drop placed on the glass. Green and blue OLEDs are then fabricated on the ITO to complete the device. When the µLA is ~15 × 15 mm(2), i.e., much larger than the ~3 × 3 mm(2) OLED pixel, the electroluminescence (EL) in the forward direction is enhanced by ~100%. Similarly, a 19 × 25 mm(2) µLA enhances the EL extracted from a 3 × 3 array of 2 × 2 mm(2) OLED pixels by 96%. Simulations that include the effects of absorption in the organic and ITO layers are in accordance with the experimental results and indicate that a thinner 0.7 mm thick glass would yield a ~140% enhancement.

Fabrication of metallic nanowires and nanoribbons using laser interference lithography and shadow lithography.

Ordered and free-standing metallic nanowires were fabricated by e-beam deposition on patterned polymer templates made by interference lithography. The dimensions of the nanowires can be controlled through adjustment of deposition conditions and polymer templates. Grain size, polarized optical transmission and electrical resistivity were measured with ordered and free-standing nanowires.