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Bulk photovoltaic effect (BPVE), featuring polarization-dependent uniform photoresponse at zero external bias, holds potential for exceeding the Shockley-Queisser limit in the efficiency of existing opto-electronic devices. However, the implementation of BPVE has been limited to the naturally existing materials with broken inversion symmetry, such as ferroelectrics, which suffer low efficiencies. Here, we propose metasurface-mediated graphene photodetectors with cascaded polarization-sensitive photoresponse under uniform illumination, mimicking an artificial BPVE. With the assistance of non-centrosymmetric metallic nanoantennas, the hot photocarriers in graphene gain a momentum upon their excitation and form a shift current which is nonlocal and directional. Thereafter, we demonstrate zero-bias uncooled mid-infrared photodetectors with three orders higher responsivity than conventional BPVE and a noise equivalent power of 0.12 nW Hz−1/2. Besides, we observe a vectorial photoresponse which allows us to detect the polarization angle of incident light with a single device. Our strategy opens up alternative possibilities for scalable, low-cost, multifunctional infrared photodetectors., Here, graphene-based plasmonic metamaterials are used to generate an artificial bulk photovoltaic effect, enabling the realization of mid-infrared photodetectors with enhanced responsivity and calibration-free polarization detection at room temperature.

This research developed an effective and efficient approach for improving the slow convergence in the scattering analysis of a one-dimensional graphene grating, made of a periodic array of parallel graphene strips, illuminated by a TM-polarized plane wave. Specifically, the electric fields over the graphene strips and slit regions in a unit cell are individually expressed as an expansion of local basis functions inherently satisfying edge conditions. Interestingly, convergence rate is highly improved compared to the customary and modified Fourier modal method. Additionally, with the aid of local basis functions, the Gibbs phenomenon occurring at both edges of graphene strip can be removed.

Molecular and atomic imaging required the development of electron and scanning probe microscopies to surpass the physical limits dictated by diffraction. Nano-infrared experiments and pico-cavity tip-enhanced Raman spectroscopy imaging later demonstrated that radiation in the visible range can surpass this limit by using scanning probe tips to access the near-field regime. Here we show that ultimate resolution can be obtained by using scanning microwave imaging microscopy to reveal structures with feature sizes down to 1~nm using a radiation of 0.1~m in wavelength. As a test material we use twisted bilayer graphene, which is not only a very important recent topic due to the discovery of correlated electron effects such as superconductivity, but also because it provides a sample where we can systematically tune a superstructure Moir\'e patterns modulation from below one up to tens of nanometers. By analyzing the tip-sample distance dynamics, we demonstrate that this ultimate 10$^8$ probe-to-pattern resolution can be achieved by using liquid immersion microscopy concepts and exquisite force control exerted on nanoscale water menisci., Comment: suppl. mat included, movies not included and available upon request by email to gilberto@dcc.ufmg.br

Plasma waves play an important role in many solid-state phenomena and devices. They also become significant in electronic device structures as the operation frequencies of these devices increase. A prominent example is field-effect transistors (FETs), that witness increased attention for application as rectifying detectors and mixers of electromagnetic waves at gigahertz and terahertz frequencies, where they exhibit very good sensitivity even high above the cut-off frequency defined by the carrier transit time. Transport theory predicts that the coupling of radiation at THz frequencies into the channel of an antenna-coupled FET leads to the development of a gated plasma wave, collectively involving the charge carriers of both the two-dimensional electron gas and the gate electrode. In this paper, we present the first direct visualization of these waves. Employing graphene FETs containing a buried gate electrode, we utilize near-field THz nanoscopy at room temperature to directly probe the envelope function of the electric field amplitude on the exposed graphene sheet and the neighboring antenna regions. Mapping of the field distribution documents that wave injection is unidirectional from the source side since the oscillating electrical potentials on the gate and drain are equalized by capacitive shunting. The plasma waves, excited at 2 THz, are overdamped, and their decay time lies in the range of 25–70 fs. Despite this short decay time, the decay length is rather long, i.e., 0.3-0.5 μm, because of the rather large propagation speed of the plasma waves, which is found to lie in the range of 3.5–7 × 106 m/s, in good agreement with theory. The propagation speed depends only weakly on the gate voltage swing and is consistent with the theoretically predicted $$\frac{1}{4}$$ 1 4 power law.

The intriguing carrier dynamics in graphene heterojunctions have stimulated great interest in modulating the optoelectronic features to realize high-performance photodetectors. However, for most phototransistors, the photoresponse characteristics are modulated with an electrical gate or a static field. In this paper, we demonstrate a graphene/C60/pentacene vertical phototransistor to tune both the photoresponse time and photocurrent based on light modulation. By exploiting the power-dependent multiple states of the photocurrent, remarkable logical photocurrent switching under infrared light modulation occurs in a thick C60 layer (11 nm) device, which implies competition of the photogenerated carriers between graphene/C60 and C60/pentacene. Meanwhile, we observe a complete positive-negative alternating process under continuous 405 nm irradiation. Furthermore, infrared light modulation of a thin C60 (5 nm) device results in a photoresponsivity improvement from 3425 A/W up to 7673 A/W, and we clearly probe the primary reason for the distinct modulation results between the 5 and 11 nm C60 devices. In addition, the tuneable bandwidth of the infrared response from 10 to 3 × 103 Hz under visible light modulation is explored. Such distinct types of optical modulation phenomena and logical photocurrent inversion characteristics pave the way for future tuneable logical photocurrent switching devices and high-performance phototransistors with vertical graphene heterojunction structures., Phototransistors: a carbon sandwich for logic with light Two forms of carbon and a hydrocarbon are combined in a phototransistor, which creates changes in optical and electronic behavior in response to different wavelengths of light, with properties that will be useful for both research and commercial applications. The innovative phototransistor has been developed by Jiayue Han and colleagues at the University of Electronic Science and Technology of China, in Chengdu, with co-workers at other Chinese research centers. It has a layer composed of spherical C60 molecules, sandwiched between the form of carbon known as graphene and the hydrocarbon pentacene. Gold and silicon-based electrodes complete the structure. The optoelectronic properties created at the junctions between the different layers overcome limitations of simpler graphene based devices. The modulation of optical and electronic behavior achieved by the system could be used in new logical switching devices.

Nanoscale photothermal effects enable important applications in cancer therapy, imaging and catalysis. These effects also induce substantial changes in the optical response experienced by the probing light, thus suggesting their application in all-optical modulation. Here, we demonstrate the ability of graphene, thin metal films, and graphene/metal hybrid systems to undergo photothermal optical modulation with depths as large as >70% over a wide spectral range extending from the visible to the terahertz frequency domains. We envision the use of ultrafast pump laser pulses to raise the electron temperature of graphene during a picosecond timescale in which its mid-infrared plasmon resonances undergo dramatic shifts and broadenings, while visible and near-infrared plasmons in the neighboring metal films are severely attenuated by the presence of hot graphene electrons. Our study opens a promising avenue toward the active photothermal manipulation of the optical response in atomically thin materials with potential applications in ultrafast light modulation., Plasmonics: photothermal modulation A new breed of ultrafast light modulators that operate across the visible to terahertz regions may be possible by harnessing photothermal control of plasmons in graphene and thin-metal films. Theoretical analysis performed by Eduardo Dias and coworkers from the ICFO research institute in Barcelona, Spain suggests that ultrafast optical excitation of thin gold/silver-graphene structures can significantly raise the electron temperature in the carbon layer and as a result dramatically modify the plasmonic response. Calculations indicate that strong changes (>70%) in the optical reflection of such structures are possible, with a strength that increases with the fluence of the excitation pulses. Importantly, the fluence is below the damage threshold of the materials. The photothermal modulation approach could have useful applications ranging from all-optical light modulation to optical sensing.

The graphene quantum dot (GQD) is a carbon allotrope with a planar surface amenable for functionalization and nanoscale dimensions that confer photoluminescent properties. Collectively, these properties render GQDs an advantageous platform for nanobiotechnology applications, including as optical biosensors and delivery platforms. In particular, noncovalent functionalization offers a route to reversible modification and preservation of the pristine GQD substrate. However, a clear paradigm for GQD noncovalent functionalization has yet to be realized. Herein, we demonstrate the feasibility of noncovalent polymer adsorption to the GQD surface, with a specific focus on single-stranded DNA (ssDNA). We study how GQD oxidation level affects the propensity for polymer adsorption by synthesizing and characterizing four types of GQD substrates and investigating noncovalent polymer association to these substrates. Distinct adsorption methods are developed for successful ssDNA attachment based upon the GQD’s initial level of oxidation. ssDNA adsorption to the GQD is confirmed by atomic force microscopy, by inducing ssDNA desorption, and with molecular dynamics simulations. ssDNA is determined to adsorb strongly to no-oxidation GQDs, weakly to low-oxidation GQDs, and not at all for heavily oxidized GQDs. We hypothesize that high GQD oxygen content disrupts the graphitic carbon domains responsible for stacking with the aromatic ssDNA bases, thus preventing the formation of stable polymer-GQD complexes. Finally, we develop a more generic adsorption platform and assess how the GQD system is tunable by modifying both the polymer sequence and type.

In recent years there has been much interest concerning the development of modulators in the mid- to long-wave infrared, based on emerging materials such as graphene. These have been frequently pursued for optical communications, though also for other specialized applications such as infrared scene projectors. Here we investigate a new application for graphene modulators in the mid- to long-wave infrared. We demonstrate, for the first time, computational spectroscopy in the mid- to long-wave infrared using a graphene-based metasurface modulator. Furthermore, our metasurface device operates at low gate voltage. To demonstrate computational spectroscopy, we provide our algorithm with the measured reflection spectra of the modulator at different gate voltages. We also provide it with the measured reflected light power as a function of the gate voltage. The algorithm then estimates the input spectrum. We show that the reconstructed spectrum is in good agreement with that measured directly by a Fourier transform infrared spectrometer, with a normalized mean-absolute-error (NMAE) of 0.021.

Two-dimensional (2D) transition metal dichalcogenides (TMDCs) and graphene compose a new family of crystalline materials with atomic thicknesses and exotic mechanical, electronic, and optical properties. Due to their inherent exceptional mechanical flexibility and strength, these 2D materials provide an ideal platform for strain engineering, enabling versatile modulation and significant enhancement of their optical properties. For instance, recent theoretical and experimental investigations have demonstrated flexible control over their electronic states via application of external strains, such as uniaxial strain and biaxial strain. Meanwhile, many nondestructive optical measurement methods, typically including absorption, reflectance, photoluminescence, and Raman spectroscopies, can be readily exploited to quantitatively determine strain-engineered optical properties. This review begins with an introduction to the macroscopic theory of crystal elasticity and microscopic effective low-energy Hamiltonians coupled with strain fields, and then summarizes recent advances in strain-induced optical responses of 2D TMDCs and graphene, followed by the strain engineering techniques. It concludes with exciting applications associated with strained 2D materials, discussions on existing open questions, and an outlook on this intriguing emerging field., Optics: 2D materials feel the strain A review of recent advances in strain-induced new optical responses of two-dimensional (2D) materials concludes with various applications associated with strain-engineered 2D materials. The review, conducted by Dangyuan Lei and colleagues at The City University of Hong Kong, in collaboration with a researcher from The Hong Kong Polytechnic University, first provides a brief introduction to the macroscopic theory of crystal elasticity and how external strain affects the physical and optical properties of 2D materials. It then summarizes how recent advances in the application of external strains in 2D materials, including TMDCs and graphene, can be used to modify their unique physical and optical properties, followed by a summary of strain engineering techniques. The review concludes by highlighting some of the peculiar applications associated with strained 2D materials, such as high-sensitivity optical resonators and flexible electronic devices.

Plasmonic biosensing has emerged as the most sensitive label-free technique to detect various molecular species in solutions and has already proved crucial in drug discovery, food safety and studies of bio-reactions. This technique relies on surface plasmon resonances in ~50 nm metallic films and the possibility to functionalize the surface of the metal in order to achieve selectivity. At the same time, most metals corrode in bio-solutions, which reduces the quality factor and darkness of plasmonic resonances and thus the sensitivity. Furthermore, functionalization itself might have a detrimental effect on the quality of the surface, also reducing sensitivity. Here we demonstrate that the use of graphene and other layered materials for passivation and functionalization broadens the range of metals which can be used for plasmonic biosensing and increases the sensitivity by 3-4 orders of magnitude, as it guarantees stability of a metal in liquid and preserves the plasmonic resonances under biofunctionalization. We use this approach to detect low molecular weight HT-2 toxins (crucial for food safety), achieving phase sensitivity~0.5 fg/mL, three orders of magnitude higher than previously reported. This proves that layered materials provide a new platform for surface plasmon resonance biosensing, paving the way for compact biosensors for point of care testing.

Mid-infrared (MIR) light-emitting devices play a key role in optical communications, thermal imaging, and material analysis applications. Two-dimensional (2D) materials offer a promising direction for next-generation MIR devices owing to their exotic optical properties, as well as the ultimate thickness limit. More importantly, van der Waals heterostructures—combining the best of various 2D materials at an artificial atomic level—provide many new possibilities for constructing MIR light-emitting devices of large tuneability and high integration. Here, we introduce a simple but novel van der Waals heterostructure for MIR light-emission applications built from thin-film BP and transition metal dichalcogenides (TMDCs), in which BP acts as an MIR light-emission layer. For BP–WSe2 heterostructures, an enhancement of ~200% in the photoluminescence intensities in the MIR region is observed, demonstrating highly efficient energy transfer in this heterostructure with type-I band alignment. For BP–MoS2 heterostructures, a room temperature MIR light-emitting diode (LED) is enabled through the formation of a vertical PN heterojunction at the interface. Our work reveals that the BP–TMDC heterostructure with efficient light emission in the MIR range, either optically or electrically activated, provides a promising platform for infrared light property studies and applications., Thin-film semiconductors enhance black phosphorus mid-infrared light emission Layering thin films of semiconducting transition metal dichalcogenides with thin-film black phosphorus enhances its ability to emit mid-infrared (MIR) light, which could facilitate MIR light emission investigations and applications. Xiaolong Chen of China’s Southern University of Science and Technology and colleagues layered thin flakes of black phosphorus (BP) with one or the other of a monolayer of tungsten diselenide (WSe2) or a thin film of molybdenum disulfide (MoS2). Thin-film BP is considered a promising MIR material, with potential applications in MIR photodetection and optical modulation. WSe2 efficiently transferred light energy to the BP, enhancing its MIR photoluminescence by up to 192%. On the other hand, the interface created by layering BP with MoS2 enabled the formation of a MIR light-emitting diode at room temperature.

In this paper, we present a tight-binding model based on DFT calculations for investigation the electronic and optical properties of monolayer Germanene. The thermal properties are investigated using Green function method. The required tight binding parameters including the onsite energies and third nearest neighbors hopping and overlap integrals are obtained based on our DFT calculations. Germanene is a semiconductor with zero band gap and linear band dispersion around the K point. The band gap opening occurs in the presence of bias voltage. The band gap is increased linearly with increase of the bias voltage strength. The tight binding results for position of the two first peaks in the optical Infrared region is same with the DFT results. By applying and increasing bias voltage, the dielectric function shows the blue shift by reduction the peak intensity in the energy range E

The composition of Van-der-Waals heterostructures is conclusively determined using a hybrid evaluation scheme of data acquired by optical microspectroscopy. This scheme deploys a parameter set comprising both change in reflectance and wavelength shift of distinct extreme values in reflectance spectra. Furthermore, the method is supported by an accurate analytical model describing reflectance of multilayer systems acquired by optical microspectroscopy. This approach allows uniquely for discrimination of 2D materials like graphene and hBN and, thus, quantitative analysis of Van-der-Waals heterostructures containing structurally very similar materials. The physical model features a transfer matrix method which allows for flexible, modular description of complex optical systems and may easily be extended to individual setups. It accounts for numerical apertures of applied objective lenses and a glass fiber which guides the light into the spectrometer by two individual weighting functions. The scheme is proven by highly accurate quantification of the number of layers of graphene and hBN in Van-der-Waals heterostructures. In this exemplary case, the fingerprint of graphene involves distinct deviations of reflectance accompanied by additional wavelength shifts of extreme values. In contrast to graphene the fingerprint of hBN reveals a negligible deviation in absolute reflectance causing this material being only detectable by spectral shifts of extreme values., Comment: 12 pages, 4 figures

Controlling extra charge carriers is pivotal in manipulating electronic, optical, and magnetic properties of various two-dimensional materials. Nonetheless, the ubiquitous hole doping of two-dimensional materials in the air and acids has been controversial in its mechanistic details. Here we show their common origin is an electrochemical reaction driven by redox couples of oxygen and water molecules. Using real-time photoluminescence imaging of WS2 and Raman spectroscopy of graphene, we capture molecular diffusion through the two-dimensional nanoscopic space between two-dimensional materials and hydrophilic substrates, and show that the latter accommodate water molecules also serving as a hydrating solvent. We also demonstrate that HCl-induced doping is governed by dissolved O2 and pH in accordance with the Nernst equation. The nanoscopic electrochemistry anatomized in this work sets an ambient limit to material properties, which is universal to not only 2D but also other forms of materials., Manipulation of charge carriers is promising for tuning electronic, optical and magnetic properties in two-dimensional materials, but mechanistic details are not fully understood. Here, the authors report that ambient redox reactions govern charge transfer doping in graphene and tungsten disulfide.

Metamaterials have recently established a new paradigm for enhanced light absorption in state-of-the-art photodetectors. Here, we demonstrate broadband, highly efficient, polarization-insensitive, and gate-tunable photodetection at room temperature in a novel metadevice based on gold/graphene Sierpinski carpet plasmonic fractals. We observed an unprecedented internal quantum efficiency up to 100% from the near-infrared to the visible range with an upper bound of optical detectivity of $10^{11}$ Jones and a gain up to $10^{6}$, which is a fingerprint of multiple hot carriers photogenerated in graphene. Also, we show a 100-fold enhanced photodetection due to highly focused (up to a record factor of $|E/E_{0}|\approx20$ for graphene) electromagnetic fields induced by electrically tunable multimodal plasmons, spatially localized in self-similar fashion on the metasurface. Our findings give direct insight into the physical processes governing graphene plasmonic fractal metamaterials. The proposed structure represents a promising route for the realization of a broadband, compact, and active platform for future optoelectronic devices including multiband bio/chemical and light sensors., Comment: 10 pages, 6 figures

Sensitive photodetection is crucial for modern optoelectronic technology. Two-dimensional molybdenum disulfide (MoS2) with unique crystal structure, and extraordinary electrical and optical properties is a promising candidate for ultrasensitive photodetection. Previously reported methods to improve the performance of MoS2 photodetectors have focused on complex hybrid systems in which leakage paths and dark currents inevitably increase, thereby reducing the photodetectivity. Here, we report an ultrasensitive negative capacitance (NC) MoS2 phototransistor with a layer of ferroelectric hafnium zirconium oxide film in the gate dielectric stack. The prototype photodetectors demonstrate a hysteresis-free ultra-steep subthreshold slope of 17.64 mV/dec and ultrahigh photodetectivity of 4.75 × 1014 cm Hz1/2 W−1 at room temperature. The enhanced performance benefits from the combined action of the strong photogating effect induced by ferroelectric local electrostatic field and the voltage amplification based on ferroelectric NC effect. These results address the key challenges for MoS2 photodetectors and offer inspiration for the development of other optoelectronic devices., Here, the authors report ultrasensitive negative capacitance phototransistors based on MoS2 regulated by a layer of ferroelectric hafnium zirconium oxide film to demonstrate a hysteresis-free ultra-steep subthreshold slope of 17.64 mV/dec and specific detectivity of 4.75 × 1014 cm Hz1/2 W−1 at room temperature.

Electromagnetically induced transparency (EIT) arises from the coherent coupling and interference between a superradiant (bright) mode in one resonator and a subradiant (dark) mode in an adjacent resonator. Generally, the two adjacent resonators are structurally or spatially asymmetric. Here, by numerical simulation, we demonstrate that tunable EIT can be induced by graphene ribbon pairs without structurally or spatially asymmetry. The mechanism originates from the fact that the resonate frequencies of the bright mode and the dark mode supported by the symmetrical graphene ribbon pairs can be respectively tuned by electrical doping levels, and when they are tuned to be equal the graphene plasmon coupling and interference occurs. The EIT in symmetrical nanostructure which avoids deliberately breaking the element symmetry in shape as well as in size facilitates the design and fabrication of the structure. In addition, the work regarding to EIT in the structurally symmetric could provide a fresh contribution to a more comprehensive physical understanding of Fano resonance.

Photonic sensors that are able to detect and track biochemical molecules offer powerful tools for information acquisition in applications ranging from environmental analysis to medical diagnosis. The ultimate aim of biochemical sensing is to achieve both quantitative sensitivity and selectivity. As atomically thick films with remarkable optoelectronic tunability, graphene and its derived materials have shown unique potential as a chemically tunable platform for sensing, thus enabling significant performance enhancement, versatile functionalization and flexible device integration. Here, we demonstrate a partially reduced graphene oxide (prGO) inner-coated and fiber-calibrated Fabry-Perot dye resonator for biochemical detection. Versatile functionalization in the prGO film enables the intracavity fluorescent resonance energy transfer (FRET) to be chemically selective in the visible band. Moreover, by measuring the intermode interference via noise canceled beat notes and locked-in heterodyne detection with Hz-level precision, we achieved individual molecule sensitivity for dopamine, nicotine and single-strand DNA detection. This work combines atomic-layer nanoscience and high-resolution optoelectronics, providing a way toward high-performance biochemical sensors and systems.

Photonic crystals are commonly implemented in media with periodically varying optical properties. Photonic crystals enable exquisite control of light propagation in integrated optical circuits, and also emulate advanced physical concepts. However, common photonic crystals are unfit for in-operando on/off controls. We overcome this limitation and demonstrate a broadly tunable two-dimensional photonic crystal for surface plasmon polaritons. Our platform consists of a continuous graphene monolayer integrated in a back-gated platform with nano-structured gate insulators. Infrared nano-imaging reveals the formation of a photonic bandgap and strong modulation of the local plasmonic density of states that can be turned on/off or gradually tuned by the applied gate voltage. We also implement an artificial domain wall which supports highly confined one-dimensional plasmonic modes. Our electrostatically-tunable photonic crystals are derived from standard metal oxide semiconductor field effect transistor technology and pave a way for practical on-chip light manipulation., Traditional photonic crystals consist of periodic media with a pre-defined optical response. Here, the authors combine nanostructured back-gate insulators with a continuous layer of graphene to demonstrate an electrically tunable two-dimensional photonic crystal suitable for controlling the propagation of surface plasmon polaritons.

Near Infra-Red Surface Enhanced Raman Spectroscopy (NIR SERS) has gained huge attention in recent years as the conventional visible SERS suffers from overwhelming fluorescence background from the fluorophore resulting in the masking of Raman signals. In this paper, we propose a novel multi-layered SERS substrate- (Cu2O - Au) - Graphene – Au - for efficient NIR SERS applications. The proposed structure has a monolayer of Cu2O - Au core-shell particles on a Au substrate with 1 nm thick graphene spacer layer. Mie simulations are used to optimize the aspect ratios of core-shell particles to shift their plasmon resonances to NIR region using MieLab software. Further, Finite Difference Time Domain (FDTD) simulations using Lumerical software are used for the design of the multiparticle layered SERS substrate as MieLab software works only for single particle systems. Designed structure is shown to provide high field enhancement factor of the order of 108 at an excitation of 1064 nm thus ensuring the possibility of using the proposed structure as efficient NIR SERS substrate which could probably be used for various NIR sensing applications.

We proposed perfect absorbers of ultra-wide bandwidths based on prism coupling with wavelength-insensitive phase matching, which consists of three dielectric layers (Prism-Cavity-Air) with monolayer graphene embedded in the cavity layer. Due to inherent material dispersion of the dielectric layers, with the proper choice of the incidence angle and the cavity thickness, the proposed perfect absorbers can satisfy the phase matching condition over a wide wavelength range, inducing enormous enhancement of the absorption bandwidth. The requirement on the material dispersions of the prism and the cavity layer for the wavelength-insensitive phase matching over a wavelength range of the interest has been derived, and it has been demonstrated that the various kinds of materials can meet the requirement. Our theoretical investigation with the transfer matrix method (TMM) has revealed that a 99% absorption bandwidth of ~300 nm with perfect absorption at λ = 1.51 μm can be achieved when BK7 and PDMS are used as the prism and the cavity layer, respectively, which is ~7 times wider than the conceptual design based on the non-dispersive materials. The full width at half maximum of our designed perfect absorber is larger than 1.5 μm.

Graphene’s giant nonlinear optical response along with its integrability has made it a vaunted material for on-chip photonics. Despite a multitude of studies confirming its strong nonlinearity, there is a lack of reports examining the fundamental processes that govern the response. Addressing this gap in knowledge we analyse the role of experimental parameters by systematically measuring the near-infrared spectral dependence, the sub-picosecond temporal evolution and pulse-width dependence of the effective Kerr coefficient (n2,eff) of graphene in hundreds of femtosecond regime. The spectral dependence measured using the Z-scan technique is corroborated by a density matrix quantum theory formulation to extract a n2,eff ∝ λ2 dependence. The temporal evolution obtained using the time-resolved Z-scan measurement shows the nonlinearity peaking at zero delay time and relaxing on a time-scale of carrier relaxation. The dependence of the n2,eff on pulse duration is obtained by expanding the input pulse using a prism-pair set-up. Our results provide an avenue for controllable tunability of the nonlinear response in graphene, which is limited in silicon photonics.

Detection of visible blind UV radiation is not only interesting but also of technologically important. Herein, we demonstrate the efficient detection of UV radiation by using cluster like ZnS quantum dot solid nanostructures prepared by simple reflux condensation technique. The short-chain ligand 3-mercaptopropionic acid (MPA) involved in the synthesis lead to the cluster like formation of ZnS quantum dots into solids upon prolonged synthesis conditions. The ZnS QD solid formation resulted in the strong delocalization of electronic wave function between the neighboring quantum dots. It increases the photocurrent value, which can be further confirmed by the decrease in the average lifetime values from 64 to 4.6 ns upon ZnS cluster like QD solid formation from ZnS QDs. The ZnS quantum dot solid based UV sensor shows good photocurrent response and a maximum responsivity of 0.31 (A/W) at a wavelength of 390 nm, is not only competitive when compared with previous reports but also better than ZnS and metal oxide-based photodetectors. The device exhibits a high current value under low-intensity UV light source and an on/off ratio of IUV/Idark = 413 at zero biasing voltage with a fast response. Further, photocurrent device has been constructed using ZnS quantum dot solid nanostructures with graphene hybrids as an active layer to improve the enhancement of photoresponsivity.

We report on improvement of sensitivity for molecular detection utilizing terahertz time domain spectroscopy. Based on confining and enhancing electromagnetic field with metallic nanoslot antennas, we additionally employ monolayer graphene sheet whose edge and hydrophobic surface nature lead to increase detecting performance. Terahertz transmittance in monolayer graphene/metallic nanoslot structure exhibits more unambiguous change after lactose molecules are attached, compared to that in metallic nanoslot structure without monolayer graphene. We attribute the prominent change to that more lactose molecules are guided inside/near the metal gap region due to edge and hydrophobic surface nature of monolayer graphene. This monolayer graphene/metallic nanoslot structure can be expanded in other organic or bio-molecular detection.

Topographic corrugations, such as wrinkles, are known to introduce diverse physical phenomena that can significantly modify the electrical, optical and chemical properties of two-dimensional materials. This range of assets can be expanded even further when the crystal lattices of the walls of the wrinkle are aligned and form a superlattice, thereby creating a high aspect ratio analogue of a twisted bilayer or multilayer – the so-called twisted wrinkle. Here we present an experimental proof that such twisted wrinkles exist in graphene monolayers on the scale of several micrometres. Combining atomic force microscopy and Raman spectral mapping using a wide range of visible excitation energies, we show that the wrinkles are extremely narrow and their Raman spectra exhibit all the characteristic features of twisted bilayer or multilayer graphene. In light of a recent breakthrough – the superconductivity of a magic-angle graphene bilayer, the collapsed wrinkles represent naturally occurring systems with tuneable collective regimes. Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material.

By coupling dye molecules with a graphene layer and localizing the molecules through quantification of fluorescence lifetime quenching, a novel imaging system offers unprecedented 1-nm resolution with angstrom precision in the axial dimension.

We report a combined theoretical/experimental study of dynamic screening of excitons in media with frequency-dependent dielectric functions. We develop an analytical model showing that interparticle interactions in an exciton are screened in the range of frequencies from zero to the characteristic binding energy depending on the symmetries and transition energies of that exciton. The problem of the dynamic screening is then reduced to simply solving the Schrodinger equation with an effectively frequency-independent potential. Quantitative predictions of the model are experimentally verified using a test system: neutral, charged and defect-bound excitons in two-dimensional monolayer WS2, screened by metallic, liquid, and semiconducting environments. The screening-induced shifts of the excitonic peaks in photoluminescence spectra are in good agreement with our model.

The pursuit of optoelectronic devices operating in the mid-infrared regime is driven by both fundamental interests and envisioned applications ranging from imaging, sensing to communications. Despite continued achievements in traditional semiconductors, notorious obstacles such as the complicated growth processes and cryogenic operation preclude the usage of infrared detectors. As an alternative path towards high-performance photodetectors, hybrid semiconductor/graphene structures have been intensively explored. However, the operation bandwidth of such photodetectors has been limited to visible and near-infrared regimes. Here we demonstrate a mid-infrared hybrid photodetector enabled by coupling graphene with a narrow bandgap semiconductor, Ti2O3 (Eg = 0.09 eV), which achieves a high responsivity of 300 A W−1 in a broadband wavelength range up to 10 µm. The obtained responsivity is about two orders of magnitude higher than that of the commercial mid-infrared photodetectors. Our work opens a route towards achieving high-performance optoelectronics operating in the mid-infrared regime., Coupling graphene with narrow band-gap Ti2O3 nanoparticles can enable efficient mid-infrared photodetection. Here, the authors report a graphene-Ti2O3 based hybrid photodetector with high responsivity of ~300 A W-1 up to 10 μm by varying the number of graphene layers and size of Ti2O3 nanoparticles.

We investigate, both theoretically and numerically, a graphene-coated nano-cylinder illuminated by a plane electromagnetic wave in the far-infrared range of frequencies. We have derived an analytical formula that enables fast evaluation of the spectral window with a substantial reduction in scattering efficiency for a sufficiently thin cylinder. This polarization-dependent effect leads to tunable resonant invisibility that can be achieved via modification of graphene chemical potential monitored by the gate voltage. A multi-frequency cloaking mechanism based on dimer coated nanowires is also discussed in detail.

We report a combined theoretical/experimental study of dynamic screening of excitons in media with frequency-dependent dielectric functions. We develop an analytical model showing that interparticle interactions in an exciton are screened in the range of frequencies from zero to the characteristic binding energy depending on the symmetries and transition energies of that exciton. The problem of the dynamic screening is then reduced to simply solving the Schrodinger equation with an effectively frequency-independent potential. Quantitative predictions of the model are experimentally verified using a test system: neutral, charged and defect-bound excitons in two-dimensional monolayer WS2, screened by metallic, liquid, and semiconducting environments. The screening-induced shifts of the excitonic peaks in photoluminescence spectra are in good agreement with our model.

The marriage of photochromic molecules with the rapidly expanding portfolio of nanocarbons is providing new multifunctional and responsive nanomaterials. Here, the authors review recent progress in such materials' fabrication and their possible implementations, and suggest future directions of study., Multifunctional carbon-based nanomaterials offer routes towards the realization of smart and high-performing (opto)electronic (nano)devices, sensors and logic gates. Meanwhile photochromic molecules exhibit reversible transformation between two forms, induced by the absorption of electromagnetic radiation. By combining carbon-based nanomaterials with photochromic molecules, one can achieve reversible changes in geometrical structure, electronic properties and nanoscale mechanics triggering by light. This thus enables a reversible modulation of numerous physical and chemical properties of the carbon-based nanomaterials towards the fabrication of cognitive devices. This review examines the state of the art with respect to these responsive materials, and seeks to identify future directions for investigation.

Nonlinear optical processes, such as harmonic generation, are of great interest for various applications, e.g., microscopy, therapy, and frequency conversion. However, high-order harmonic conversion is typically much less efficient than low-order, due to the weak intrinsic response of the higher-order nonlinear processes. Here we report ultra-strong optical nonlinearities in monolayer MoS2 (1L-MoS2): the third harmonic is 30 times stronger than the second, and the fourth is comparable to the second. The third harmonic generation efficiency for 1L-MoS2 is approximately three times higher than that for graphene, which was reported to have a large χ(3). We explain this by calculating the nonlinear response functions of 1L-MoS2 with a continuum-model Hamiltonian and quantum mechanical diagrammatic perturbation theory, highlighting the role of trigonal warping. A similar effect is expected in all other transition-metal dichalcogenides. Our results pave the way for efficient harmonic generation based on layered materials for applications such as microscopy and imaging., published version, peerReviewed

The optical properties of carbon nanowall (CNW) films in the visible range have been studied and reported for the first time. Depending on the film structure, ultra-low total reflectance up to 0.13% can be reached, which makes the CNW films a promising candidate for the black body-like coating, and thus for a wide range of applications as a light absorber. We have estimated important trends in the optical property variation from sample to sample, and identified the presence of edge states and domain boundaries in carbon nanowalls as well as the film mass density variation as the key factors. Also we demonstrated that at much lower film thickness and density than for a carbon nanotube forest the CNWs yield one order higher specific light absorption.

An efficient route to synthesize macroscopic amounts of graphene is highly desired and bulk characterization of such samples, in terms of the number of layers, is equally important. We present a Raman spectroscopy-based method to determine the typical upper limit of the number of graphene layers in chemically exfoliated graphene. We utilize a controlled vapour-phase potassium intercalation technique and identify a lightly doped stage, where the Raman modes of undoped and doped few-layer graphene flakes coexist. The spectra can be unambiguously distinguished from alkali doped graphite, and modeling with the typical upper limit of the layers yields an upper limit of flake thickness of five layers with a significant single-layer graphene content. Complementary statistical AFM measurements on individual few-layer graphene flakes find a consistent distribution of the layer numbers.

The ability to generate, amplify, mix, and modulate sound with no harmonic distortion in a passive opto-acoustic device would revolutionize the field of acoustics. The photo-thermo-acoustic (PTA) effect allows to transduce light into sound without any bulk electro-mechanically moving parts and electrical connections, as for conventional loudspeakers. Also, PTA devices can be integrated with standard silicon complementary metal-oxide semiconductor (CMOS) fabrication techniques. Here, we demonstrate that the ultimate PTA efficiency of graphene aerogels, depending on their particular thermal and optical properties, can be experimentally achieved by reducing their mass density. Furthermore, we illustrate that the aerogels behave as an omnidirectional point-source throughout the audible range with no harmonic distortion. This research represents a breakthrough for audio-visual consumer technologies and it could pave the way to novel opto-acoustic sensing devices., 6 pages, 4 figures