Publications

2018
Yi, J. ; Li, B. ; Jiang, N. ; Yetisen, A. K. ; Yan, Q. ; Qiu, T. ; Iyer, K. S. ; Dai, H. ; Li, S. Painful Terminal Neuroma Prevention by Capping PRGD/PDLLA Conduit in Rat Sciatic Nerves. Advanced Science. DOI: 10.1002/advs.201700876 2018. Publisher's Version
Khalid, M. W. ; Ahmed, R. ; Yetisen, A. K. ; Butt, H. Flexible Polymeric Dynamic Corner Cube Retroreflector Array for Temperature and Strain Sensing. RSC Advances 2018, 8 7588-7598. Publisher's VersionAbstract
Optical sensors for detecting temperature and strain play a crucial role in the analysis of environmental conditions and real-time remote sensing. However, the development of a single optical device that can sense temperature and strain simultaneously remains a challenge. Here, a flexible corner cube retroreflector (CCR) array based on passive dual optical sensing (temperature and strain) is demonstrated. A mechanical embossing process was utilised to replicate a three-dimensional (3D) CCR array in a soft flexible polymer film. The fabricated flexible CCR array samples were experimentally characterised through reflection measurements followed by computational modelling. As fabricated samples were illuminated with a monochromatic laser beam (635, 532, and 450 nm), a triangular shape reflection was obtained at the far-field. The fabricated flexible CCR array samples tuned retroreflected light based on external stimuli (temperature and strain as an applied force). For strain and temperature sensing, an applied force and temperature, in the form of weight suspension, and heat flow was applied to alter the replicated CCR surface structure, which in turn changed its optical response. Directional reflection from the heated flexible CCR array surface was also measured with tilt angle variation (max. up to 10°). Soft polymer CCRs may have potential in remote sensing applications, including measuring the temperature in space and in nuclear power stations.
Jiang, N. ; Yin, Y. X. ; Y. Wang, ; Li, B. B. ; Qiu, T. ; van Rijn, P. ; Yetisen, A. K. ; Tian, G. ; Yan, Q. J. ; Yi, J. L. ; et al. bFGF and Poly-RGD Cooperatively Establish Biointerface for Stem Cell Adhesion, Proliferation and Differentiation. Advanced Materials Interfaces. DOI: 10.1002/admi.201700702 2018. Publisher's VersionAbstract
Biointerface design is widely used to functionalize biomaterials with controllable physicochemical properties. Functionalized biointerface provides a versatile platform to connect biological entities and nonbiogenic materials. Existing nanofabrication approaches to create such a nanostructured biointerface involve in low stability of the functionalized nanolayer and simple functionalities that limit its applicability. Here, a stable nanolayered synthetic polypeptide (poly[LA-co-(Glc-alt-Lys)] and modified with arginine-glycine-aspartic acid, PRGD)/basic fibroblast growth factor (bFGF) biointerface is created via structural matching, charge interaction, and hydrogen bonding. The cooperative effect of the PRGD/bFGF biointerface shows multiple functionalities in promoting stem cell adhesion by 33% increase in cell adhesion to poly(d,l-lactic acid) substrate as compared to experiments on bare substrate as a control. Moreover, the biointerface enhances proliferation by 40% in cell density, potential differentiation by 62%, and gene expression by 40 and 80% respectively as compared to the control samples. The fabricated biointerface may have applications in nerve regeneration, tissue repair, and stem cell-based therapy.
Hassaan, M. U. ; Liu, Y. C. ; Yetisen, A. K. ; Butt, H. ; Friend, R. H. Energy Landscape of Vertically Anisotropic Polymer Blend Films toward Highly Efficient Polymer Light-Emitting Diodes (PLEDs). Advanced Functional Materials, DOI: 10.1002/adfm.201705903 (2018) 2018. Publisher's VersionAbstract
A blend of two hole-dominant polymers is created and used as the light emissive layer in light-emitting diodes to achieve high luminous efficiency up to 22 cd A−1. The polymer blend F81−xSYxis based on poly(9,9-dioctylfluorene) (F8) and poly(para-phenylene vinylene) derivative superyellow (SY). The blend system exhibits a preferential vertical concentration distribution. The resulting energy landscape modifies the overall charge transport behavior of the blend emissive layer. The large difference between the highest unoccupied molecular orbital levels of F8 (5.8 eV) and SY (5.3 eV) introduces hole traps at SY sites within the F8 polymer matrix. This slows down the hole mobility and facilitates a balance between the transport behavior of both the charge carriers. The balance due to such energy landscape facilitates efficient formation of excitons within the emission zone well away from the cathode and minimizes the surface quenching effects. By bringing the light-emission zone in the middle of the F81−xSYx film, the bulk of the film is exploited for the light emission. Due to the charge trapping nature of SY molecules in F8 matrix and pushing the emission zone in the center, the radiative recombination rate also increases, resulting in excellent device performance.
Jiang, N. ; Ahmed, R. ; Rifat, A. A. ; Guo, J. ; Yin, Y. X. ; Butt, H., Y. A. K. Functionalized Flexible Soft Polymer Optical Fibers for Laser Photomedicine. Advanced Optical Materials 2018, 6. Publisher's VersionAbstract
Optical waveguides allow propagating light through biological tissue in optogenetics and photomedicine applications. However, achieving efficient light delivery to deep tissues for long-term implantation has been limited with solid-state optical fibers. Here, a method is created to rapidly fabricate flexible, functionalized soft polymer optical fibers (SPOFs) coupled with silica fibers. A step-index core/cladded poly(acrylamide-co-poly(ethylene glycol) diacrylate)/Ca alginate SPOF is fabricated through free-radical polymerization in a mold. The SPOF is integrated with a solid-state silica fiber coupler for efficient light delivery. The cladded SPOF shows ≈1.5-fold increase in light propagation compared to the noncladded fiber. The optical loss of the SPOF is measured as 0.6 dB cm−1 at the bending angle of 70° and 0.28 dB cm−1 through a phantom tissue. The SPOF (inner Ø = 200 µm) integrated with a 21 gauge needle (inner Ø = 514 µm) is inserted within a porcine tissue. The intensity of light decreases ≈60%, as the SPOF is implanted as deep as 2 cm. Doped with fluorescent dye and gold nanoparticles, the SPOF fiber exhibits yellow-red and red illumination. Living cells can also be incorporated within the SPOF with viability. The flexible SPOFs may have applications in photodynamic light therapy, optical biosensors, and photomedicine.
Jiang, N. ; Montelongo, Y. ; Butt, H. ; Yetisen, A. K. Microfluidic Contact Lenses. Small. DOI: 10.1002/smll.201704363 2018. Publisher's Version
Zhang, Z. ; Dou, Q. ; Gao, H. ; Bai, B. ; Zhang, Y. ; Hu, D. ; A.K., Y. ; Butt, H. ; Yang, X. ; Li, C. ; et al. 30 s Response Time of K+ Ion-Selective Hydrogels Functionalized with 18-Crown-6 Ether Based on QCM Sensor. Advanced Healthcare Materials. DOI: 10.1002/adhm.201700873 2018. Publisher's VersionAbstract
Potassium detection is critical in monitoring imbalances in electrolytes and physiological status. The development of rapid and robust potassium sensors is desirable in clinical chemistry and point-of-care applications. In this study, composite supramolecular hydrogels are investigated: polyethylene glycol methacrylate and acrylamide copolymer (P(PEGMA-co-AM)) are functionalized with 18-crown-6 ether by employing surface initiated polymerization. Real-time potassium ion monitoring is realized by combining these compounds with quartz crystal microbalance. The device demonstrates a rapid response time of ≈30 s and a concentration detection range from 0.5 to 7.0 × 10−3 m. These hydrogels also exhibit high reusability and K+ ion selectivity relative to other cations in biofluids such as Na+, NH4+, Mg2+, and Ca2+. These results provide a new approach for sensing alkali metal ions using P(PEGMA-co-AM) hydrogels.
Kim, H. ; Beack, S. ; Han, S. ; Shin, M. ; Lee, T. ; Park, Y. ; Kim, K. S. ; Yetisen, A. K. ; Yun, S. H. ; Kwon, W. ; et al. Photonic Nanomaterials for Diagnostic, Therapeutic, and Theranostic Applications. Advanced Materials. DOI: 10.1002/adma.201701460 2018. Publisher's VersionAbstract
The last decade has seen dramatic progress in the principle, design, and fabrication of photonic nanomaterials with various optical properties and functionalities. Light-emitting and light-responsive nanomaterials, such as semiconductor quantum dots, plasmonic metal nanoparticles, organic carbon, and polymeric nanomaterials, offer promising approaches to low-cost and effective diagnostic, therapeutic, and theranostic applications. Reasonable endeavors have begun to translate some of the promising photonic nanomaterials to the clinic. Here, current research on the state-of-the-art and emerging photonic nanomaterials for diverse biomedical applications is reviewed, and the remaining challenges and future perspectives are discussed.
2017
Deng, S. ; Jwad, T. ; Li, C. ; Benton, D. ; Yetisen, A. K. ; Jiang, K. ; Dai, Q. ; Butt, H. Carbon Nanotube Array Based Binary Gabor Zone Plate Lenses. Scientific Reports 2017, 7 15256. Publisher's VersionAbstract
Diffractive zone plates have a wide range of applications from focusing x-ray to extreme UV radiation. The Gabor zone plate, which suppresses the higher-order foci to a pair of conjugate foci, is an attractive alternative to the conventional Fresnel zone plate. In this work, we developed a novel type of Beynon Gabor zone plate based on perfectly absorbing carbon nanotube forest. Lensing performances of 0, 8 and 20 sector Gabor zone plates were experimentally analyzed. Numerical investigations of Beynon Gabor zone plate configurations were in agreement with the experimental results. A high-contrast focal spot having 487 times higher intensity than the average background was obtained.
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AlQattan, B. ; Benton, D. ; Yetisen, A. K. ; Butt, H. Laser Nanopatterning of Colored Ink Thin Films for Photonic Devices. ACS Applied Materials & Interfaces 2017, 9 39641-39649. Publisher's VersionAbstract
Nanofabrication through conventional methods such as electron beam writing and photolithography is time-consuming, high cost, complex, and limited in terms of the materials which can be processed. Here, we present the development of a nanosecond Nd:YAG laser (532 nm, 220 mJ) in holographic Denisyuk reflection mode method for creating ablative nanopatterns from thin films of four ink colors (black, red, blue, and brown). We establish the use of ink as a recording medium in different colors and absorption ranges to rapidly produce optical nanostructures in 1D geometries. The gratings produced with four different types of ink had the same periodicity (840 nm); however, they produce distant wavelength dependent diffraction responses to monochromatic and broadband light. The nanostructures of gratings consisting of blue and red inks displayed high diffraction efficiency of certain wavelengths while the black and brown ink based gratings diffracted broadband light. These gratings have high potential to be used as low-cost photonic structures in wavelength-dependent optical filters. We anticipate that the rapid production of gratings based on different ink formulations can enable optics applications such as holographic displays in data storage, light trapping, security systems, and sensors.
Jiang, N. ; Butt, H. ; Montelongo, Y. ; Liu, F. ; Afewerki, S. ; Ying, G. L. ; Dai, Q. ; Montelongo, Y. ; Yun, S. H. ; Yetisen, A. K. Laser Interference Lithography for the Nanofabrication of Stimuli-Responsive Bragg Stacks. Advanced Functional Materials. DOI: 10.1002/adfm.201702715 2017. Publisher's VersionAbstract
Dynamic structural coloration in Tmesisternus isabellae beetle elytra is a unique example of Bragg stack-based wavelength tuning in response to external stimuli. The underlying principles could guide the design of quantitative optical stimuli-responsive polymers. Existing nanofabrication techniques to create such materials are costly, time-consuming, and require high expertise. This study reports a nanofabrication method to produce slanted Bragg stack structures in poly(acrylamide-co-poly(ethylene glycol) diacrylate) hydrogel films by combining laser interference lithography and silver halide chemistry in a cost-effective and rapid process (≈10 min). The Bragg stacks consist of silver bromide nanocrystal multilayers having a lattice spacing of ≈200 nm. Upon broadband light illumination, the Bragg stacks diffract a narrow-band peak at 520 nm at ≈10° with respect to the normal incidence. The lattice spacing of the hydrogel films can be modulated by external stimuli to shift the Bragg peak for dynamic quantitative measurements. To demonstrate the utility of this method, the Bragg stacks are functionalized with phenylboronic acid molecules. Bragg peak shift analysis allows reversible glucose sensing within a physiological dynamic range (0.0–20.0 mmol L−1) having a sensitivity of 0.2 mmol L−1. The developed Bragg stacks may have application in portable, wearable, and implantable real-time medical diagnostics at point-of-care settings.
Wavelength-Selective Diffraction from Silica Thin-Film Gratings. ACS Photonics. DOI: 10.1021/acsphotonics.7b00419 2017. Publisher's VersionAbstract
A reflective diffraction grating with a periodic square-wave profile will combine the effects of thin-film interference with conventional grating behavior when composed of features having a different refractive index than that of the substrate. A grating period of 700–1300 nm was modeled and compared for both silicon (Si) and silicon dioxide (SiO2) to determine the behavior of light interaction with the structures. Finite element analysis was used to study nanostructures having a multirefractive index grating and a conventional single material grating. A multimaterial grating has the same diffraction efficiency as that of a grating formed in a single material, but had the advantage of having an ordered relationship between the grating dimensions (thickness and period) and the intensity of reflected and diffracted optical wavelengths. We demonstrate a color-selective feature of the modeled SiO2 grating by fabricating samples with grating periods of 800 and 1000 nm, respectively. A high diffraction efficiency was measured for the green wavelength region as compared to other colors in the spectrum for 800 nm grating periodicity; whereas wavelengths within the red region of spectrum interfered constructively for the grating with 1000 nm periodicity resulting a higher efficiency for red color bandwidth. The results show that diffraction effects can be enhanced by the thin-film interference phenomenon to produce color selective optical devices.
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Alqurashi, T. ; Montelongo, Y. ; Penchev, P. ; Yetisen, A. K. ; Dimov, S. ; Butt, H. Femtosecond laser ablation of transparent microphotonic devices and computer-generated holograms. Nanoscale 2017, 9 13808-13819. Publisher's VersionAbstract
Femtosecond laser ablation allows direct patterning of engineering materials in industrial settings without requiring multistage processes such as photolithography or electron beam lithography. However, femtosecond lasers have not been widely used to construct volumetric microphotonic devices and holograms with high reliability and cost efficiency. Here, a direct femtosecond laser writing process is developed to rapidly produce transmission 1D/2D gratings, Fresnel Zone Plate lenses, and computer-generated holograms. The optical properties including light transmission, angle-dependent resolution, and light polarization effects for the microphotonic devices have been characterized. Varying the depth of the microgratings from 400 nm to 1.5 μm allowed the control over their transmission intensity profile. The optical properties of the 1D/2D gratings were validated through a geometrical theory of diffraction model involving 2D phase modulation. The produced Fresnel lenses had transmission efficiency of ∼60% at normal incidence and they preserved the polarization of incident light. The computer-generated holograms had an average transmission efficiency of 35% over the visible spectrum. These microphotonic devices had wettability resistance of contact angle ranging from 44° to 125°. These devices can be used in a variety of applications including wavelength-selective filters, dynamic displays, fiber optics, and biomedical devices.
Dou, Q. ; Hu, D. ; Gao, H. ; Zhang, Y. ; Yetisen, A. K. ; Butt, H. ; Wang, J. ; Nie, G. ; Dai, Q. High performance boronic acid-containing hydrogel for biocompatible continuous glucose monitoring. RSC Advances 2017, 7 41384-41390. Publisher's VersionAbstract
Rapid and robust hydrogels are essential in realizing continuous glucose monitoring in diabetes monitoring. However, existing hydrogels are limited in satisfying all of the sensory requirements such as detection range, response time, recoverability and biocompatibility. Here, we have developed a surface-initiated polymerization method to chemically immobilize a nano-boronic acid-hydrogel membrane onto a quartz crystal, then used a quartz crystal microbalance (QCM) to achieve real-time monitoring of glucose. The experimental results show that this hydrogel possesses enhanced binding properties to glucose under physiological conditions (pH 7.0–7.5) and blood glucose concentration (BGC) (1.1–33.3 mM). Moreover, our hydrogel displayed a rapid response time (∼100 s) to glucose, high biocompatibility in vivo through an animal model. The hydrogel has a great potential as a sensitive glucose probe for implantable continuous glucose sensors.
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Bentaleb, E. M. ; Messaoudi, M. D. E. ; Abid, M. ; Messaoudi, M. ; Yetisen, A. K. ; Sefrioui, H. ; Amzazi, S. ; Benhassou, H. A. Plasmid-based High-Resolution Melting Analysis for Rapid Detection of rpoB Mutations in Mycobacterium tuberculosis Isolates from Moroccan Patients. BMC Infectious Diseases 2017, 17, 548.Abstract

Background

Rapid diagnosis of drug resistance in tuberculosis (TB) is pivotal for the timely initiation of effective antibiotic treatment to prevent the spread of drug-resistant strains. The development of low-cost, rapid and robust methods for drug-resistant TB detection is highly desirable for resource-limited settings.

Methods

We report the use of an in house plasmid-based quantitative polymerase chain reaction-high-resolution melting (qPCR-HRM) analysis for the detection of mutations related to rifampicin-resistant Mycobacterium tuberculosis (MTB) in clinical isolates from Moroccan patients. Five recombinant plasmids containing predominant mutations (S531L, S531W, H526Y and D516V) and the wild-type sequence of the Rifampicin Resistance-Determining Region (RRDR) have been used as controls to screen 45 rifampicin-resistant and 22 rifampicin-susceptible MTB isolates.

Results

The sensitivity and the specificity of the qPCR-HRM analysis were 88.8% and 100% respectively as compared to rifampicin Drug Susceptibility Testing (DST). The results of qPCR-HRM and DNA sequencing had a concordance of 100%.

Conclusion

Our qPCR-HRM assay is a sensitive, accurate and cost-effective assay for the high-throughput screening of mutation-based drug resistance in TB reference laboratories.

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Vega, K. ; Jiang, N. ; Kan, V. ; Liu, X. ; Barry, N. ; Maes, P. ; Yetisen, A. K. ; Paradiso, J. The Dermal Abyss: Interfacing with the Skin by Tattooing Biosensors. ISWC2017 2017, 138-145. Publisher's VersionAbstract
The Dermal Abyss (d-abyss) presents an approach to biointerfaces in which the body surface is rendered as an interactive display by patterning biosensors into the skin to produce color changes in response to biomarker variations in the interstitial fluid. It combines advances in biotechnology with traditional methods in tattoo artistry. d-abyss is designed to use the aesthetics, permanence, and visible nature of tattoos to encode information. In the present work, we replace traditional inks with colorimetric and fluorescent biosensors that can report on the concentration of sodium, glucose, and pH in the interstitial fluid of the skin. We report the preliminary evaluation of these biosensors in an ex vivo skin model, assessing their visibility from the dermis. We describe different applications of d-abyss in the medical, lifestyle, and security domains. This work is a proof of concept of a platform in which the skin reveals information inside the body, tattoos form wearable displays within the skin, and the body’s metabolism works as an input for the d-abyss biosensors.
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Tamayol, A. ; Najafabadi, A. H. ; Mostafalu, P. ; Memic, A. ; Yetisen, A. K. ; Commotto, M. ; Aldhaheri, M. ; Shaban, M. ; Annabi, N. ; Yun, S. H. ; et al. Biodegradable elastic nanofibrous platforms with integrated flexible heaters for on-demand drug delivery. Scientific Reports 2017, 7 9220.Abstract
Delivery of drugs with controlled temporal profiles is essential for wound treatment and regenerative medicine applications. For example, bacterial infection is a key challenge in the treatment of chronic and deep wounds. Current treatment strategies are based on systemic administration of high doses of antibiotics, which result in side effects and drug resistance. On-demand delivery of drugs with controlled temporal profile is highly desirable. Here, we have developed thermally controllable, antibiotic-releasing nanofibrous sheets. Poly(glycerol sebacate)- poly(caprolactone) (PGS-PCL) blends were electrospun to form elastic polymeric sheets with fiber diameters ranging from 350 to 1100 nm and substrates with a tensile modulus of approximately 4-8 MPa. A bioresorbable metallic heater was patterned directly on the nanofibrous substrate for applying thermal stimulation to release antibiotics on-demand. In vitro studies confirmed the platform’s biocompatibility and biodegradability. The released antibiotics were potent against tested bacterial strains. These results may pave the path toward developing electronically controllable wound dressings that can deliver drugs with desired temporal patterns.
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Ahmed, R. ; Rifat, A. A. ; Hassan, M. U. ; Yetisen, A. K. ; Butt, H. Phase-conjugated directional diffraction from a retroreflector array hologram. RSC Advances 2017, 7 25657-25664. Publisher's VersionAbstract

A corner cube retroreflector (CCR) consists of three perpendicular flat surfaces and reflects the incident light back to its source. Optical properties of CCR arrays have applications in free space optical communication, low power wireless networks and sensing applications. Conventional top-down CCR array fabrication is complex and requires expensive equipment and limited to broadband reflection only. Here, we utilize laser assisted copying of a CCR array to a light sensitive holography polymer film (∼10 μm) which was placed parallel to the object plane (CCR array) during the recording. Optical characterization of the recorded CCR array hologram was carried out using reflection and color-selective diffraction measurements. Angle dependent optical properties were also simulated computationally followed by their experimental realization, which confirm our experimental findings. In a broadband illumination setting, a broadband white light reflection and a narrowband color diffraction were observed. A linear relationship between the incidence angle of the broadband light and the diffraction angle of the diffracted color light was observed. Bright and well-defined 2nd order far-field diffraction patterns were observed using an image-screen experiment. Maximum diffraction efficiency (DE) of ∼50% was observed for the monochromatic green light at normal illumination setting. The far-field diffraction interspacing/intensity exhibits increasing/decreasing trend with illumination tilt angles, measured between 10 to 50 degrees. The recorded CCR array holograms offer potential applications in color selective diffraction optics and customized optical devices.

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Alqurashi, T. ; Sabouri, A. ; Penchev, P. ; Yetisen, A. K. ; Dimov, S. ; Butt, H. Femtosecond Laser Directed Fabrication of Optical Diffusers. RSC Advances 2017, 7 18019-18023. Publisher's VersionAbstract

Optical diffusers are widely used in filament lamps, imaging systems, display technologies, lasers, and Light Emitting Diodes (LEDs). Here, a method for the fabrication of optical diffusers through femtosecond laser machining is demonstrated. Float glass surfaces were ablated with femtosecond laser light to form nanoscale ripples with dimensions comparable to the wavelength of visible light. These structures produce highly efficient and wide field of view diffusers. The machined patterns altered the average surface roughness, with the majority of particles in the range of a few hundred nanometers. The optical diffusion characteristic and a maximum diffusion angle of near 172° was achieved with optimum machining parameters. The transmission performance of the diffusers was measured to be ∼30% across the visible spectrum. The demonstrated technique has potential for producing low-cost large area optical devices. The process benefits from the flexibility of the laser writing method and enables the production of custom optical diffusers.

Deng, S. ; Butt, H. ; Jiang, K. ; Dlubak, B. ; Kidambi, P. R. ; Seneor, P. ; Xavier, S. ; Yetisen, A. K. Graphene Nanoribbons Based Plasmonic Fresnel Zone Plate Lenses. RSC Advances 2017, 7 16594-16601. Publisher's VersionAbstract

A graphene-based metamaterial lens is theoretically proposed by combining plasmonic nanoribbons with Fresnel Zone Plate (FZP) architecture to realize wavelength-selective and tunable lensing. The plasmonic FZP lens shows higher focal intensity and efficiency compared to conventional FZP. As compared with normal graphene FZP, the lensing effect of the plasmonic FZP can be enhanced by 83 times. When compared with Au thin film based FZP lenses, the graphene plasmonic lenses can achieve comparable lensing effects, but with a thinner geometry and with an additional advantage of being wavelength selective and tuneable. The analyses of selectivity and tunability of the plasmonic lens show that the plasmonic lens functions as a filter with broadband incident light or as a switch which can be turned on and off via changing the Fermi levels. The diffraction between neighboring graphene nanoribbons and the effect of the substrate on the lensing effect is also discussed. The plasmonic effect of the nanoribbons only contributes to the focal intensity without affecting the diffraction properties of Fresnel zone plate lenses such as focal lengths. This plasmonic FZP lens is an ideal combination of near and far field optics. However, the complex interaction of diffractions within and between the FZP rings could lead to a significant change of the lensing effect, which opens the possibility of creating innovative graphene metamaterial devices. The findings in this work can be used for developing wavelength-selective electro-optical applications operating in the infrared and terahertz ranges.

 

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