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Surface-enhanced Raman spectroscopy (SERS) demands reliable, high enhancement substrates in order to be used in different fields of application. Here, we introduce freestanding porous gold membranes (PAuM) as easy to produce, scalable, mechanically stable, and effective SERS substrates. We fabricate large-scale sub-30 thick PAuM, that form freestanding membranes with varying morphologies depending on the nominal gold thickness. These PAuM are mechanically stable for pressures up to $>3$ bar, and exhibit surface-enhanced Raman scattering with local enhancement factors of $10^4$ to $10^5$, which we demonstrate by wavelength-dependent and spatially resolved Raman measurements using graphene as a local Raman probe. Numerical simulations reveal that the enhancement arises from individual, nanoscale pores in the membrane acting as optical slot antennas. Our PAuM are mechanically stable, provide robust SERS enhancement for excitation power densities up to $10^6$W$\,$cm$^{-2}$, and may find use as a building block in flow-through sensor applications based on SERS., Roman M. Wyss and Markus Parzefal contributed equally. Supporting Information included

Ultramicroelectrodes (UMEs) are electrochemical working electrodes with at least one dimension less than 25 μm. Here, we demonstrate a method to fabricate pristine (contamination and doping-free) monolayer graphene UMEs and characterise its electrochemical properties. Graphene is particularly sensitive to both contamination from device fabrication and doping from the substrate, and these effects are detrimental to accurate measurements of fundamental electrochemical properties as well as electrochemical electrode applications. We demonstrate a UME design and fabrication steps which ensure that the electro-active surface of the graphene never comes into contact with contaminants such as process polymers and solvents, has a well-defined area due to self-aligned fabrication, and we shield the converse side of the graphene monolayer with the highly inert dielectric hexagonal boron nitride (h-BN). Cyclic voltammetry demonstrates the expected steady-state behaviour for a UME in the hemispherical diffusion regime. The reduction of IrCl62− in weak KCl electrolytes was employed to investigate the electron transfer characteristics of the pristine graphene UMEs and the reproducibility of the measurements. Values of the standard rate constant, k0 and the transfer coefficient, α were measured to be 3.04 ± 0.78 × 10−3 cm s−1 and 0.272 ± 0.024 respectively. These values are consistent for monolayer graphene with reduced charge doping from contaminants and the substrate. This is further confirmed by Raman spectroscopy measurements of the graphene UME before and after the electrochemical measurements.

The electromagnetic enhancement theory describes surface-enhanced Raman scattering (SERS) as a Raman effect that takes place in the near-field of a plasmonic nanostructure. The theory has been very successful in explaining the fundamental properties of SERS, modelling the performance of different metals as enhancing materials and optimizing SERS hotspots for strongest possible enhancement. Over the last decade, a number of carefully designed experimental studies have examined predictions of the electromagnetic theory like the size and shape of SERS hotspots, the absolute magnitude of the enhancement and the width of the SERS resonance. Although the overall picture was quite satisfactory, the theory failed to predict key aspects of SERS, for example, the absolute magnitude of the plasmonic enhancement. We scrutinize these experiments and review them focusing on the results that require going beyond the electromagnetic enhancement theory. We argue that the results of these experiments create the need to develop the theory of SERS further, especially the exact role of plasmonic enhancement in inelastic light scattering.

We experimentally quantify the Raman scattering from individual carbyne chains confined in double-walled carbon nanotubes. We find that the resonant differential Raman cross section of confined carbyne is on the order of 10−22 cm2 sr−1 per atom, making it the strongest Raman scatterer ever reported., Nano Letters, 20 (9), ISSN:1530-6984, ISSN:1530-6992

Carbyne is an infinitely long linear chain of carbon atoms with sp1 hybridization and the truly one-dimensional allotrope of carbon. While obtaining freestanding carbyne is still an open challenge, the study of confined carbyne, linear chains of carbon encapsulated in carbon nanotubes, provides a pathway to explore carbyne and its remarkable properties in a well-defined environment. In this review, we discuss the basics and recent advances in studying single confined carbyne chains by Raman spectroscopy, which is their primary spectroscopic characterization method. We highlight where single carbyne chain studies are needed to advance our understanding of confined carbyne as a material system and provide an overview of the open questions that need to be addressed and of those aspects currently under debate.

We investigate the anti-Stokes Raman scattering of single carbyne chains confined inside double-walled carbon nanotubes. Individual chains are identified using tip-enhanced Raman scattering (TERS) and heated by resonant excitation with varying laser powers. We study the temperature dependence of carbyne's Raman spectrum and quantify the laser-induced heating based on the anti-Stokes/Stokes ratio. Due to its molecular size and its large Raman cross section, carbyne holds great promise for local temperature monitoring, with potential applications ranging from nanoelectronics to biology.

While the basal plane of graphene is inert, defects in it are centers of chemical activity. An attractive application of such defects is towards controlled functionalization of graphene with foreign molecules. However, the interaction of the defects with reactive environment, such as ambient, decreases the efficiency of functionalization and makes it poorly controlled. Here, we report a novel approach to generate, monitor with time resolution, and functionalize the defects $\textit{in situ}$ without ever exposing them to the ambient. The defects are generated by an energetic Argon plasma and their properties are monitored using $\textit{in situ}$ Raman spectroscopy. We find that these defects are functional, very reactive, and strongly change their density from $\approx 1\cdot10^{13} cm^{-2}$ to $\approx 5\cdot10^{11} cm^{-2}$ upon exposure to air. We perform the proof of principle $\textit{in situ}$ functionalization by generating defects using the Argon plasma and functionalizing them $\textit{in situ}$ using Ammonia functional. The functionalization induces the n-doping with a carrier density up to $5\cdot10^{12} cm^{-2}$ in graphene and remains stable in ambient conditions., Comment: 12 pages, 4 figures, including Supplementary Information with 6 pages, 6 figures and 1 table

Carbon, 139, ISSN:0008-6223

In the field of phononics, periodic patterning controls vibrations and thereby the flow of heat and sound in matter. Bandgaps arising in such phononic crystals realize low-dissipation vibrational modes and enable applications towards mechanical qubits, efficient waveguides, and state-of-the-art sensing. Here, we combine phononics and two-dimensional materials and explore the possibility of manipulating phononic crystals via applied mechanical pressure. To this end, we fabricate the thinnest possible phononic crystal from monolayer graphene and simulate its vibrational properties. We find a bandgap in the MHz regime, within which we localize a defect mode with a small effective mass of 0.72 ag = 0.002 $m_{physical}$. Finally, we take advantage of graphene's flexibility and mechanically tune a finite size phononic crystal. Under electrostatic pressure up to 30 kPa, we observe an upshift in frequency of the entire phononic system by more than 350%. At the same time, the defect mode stays within the bandgap and remains localized, suggesting a high-quality, dynamically tunable mechanical system., Comment: 19 pages, 4 figures; Supplementary Information of additional 19 pages and 9 figures

Nano Letters, 19 (9), ISSN:1530-6984, ISSN:1530-6992

Surface-enhanced Raman scattering (SERS) and resonant Raman scattering are widely used techniques to enhance the Raman intensity of molecules and nanomaterials by several orders of magnitude. In SERS, typically, molecules are investigated and their intrinsic resonance is often ignored while discussing the plasmonic enhancement. Here, we study α-sexithiophenes encapsulated in carbon nanotubes placed in the center of a nanodimer. By dielectrophoretic deposition, we place the nanotubes precisely in the center of a plasmonic gold nanodimer and observe SERS enhancement from individual tube bundles. The encapsulated molecules are not subjected to chemical enhancement because of the protective character of the nanotube. Polarization-dependent Raman measurements confirm the alignment of the molecules within the carbon nanotubes (CNTs) and reveal the influence of the plasmonic near field on the molecule’s Raman intensity. We investigate the encapsulated molecules in small CNT bundles with and without plasmonic enhancement and determine the molecular and plasmonic resonance by tuning the excitation wavelength. We observe a strong red shift of the maximum Raman intensity under plasmonic enhancement toward the plasmon resonance., The Journal of Physical Chemistry C, 123 (16), ISSN:1932-7455, ISSN:1932-7447

We present a two-step procedure to probe hotspots of plasmon-enhanced Raman scattering with carbon nanotubes (CNTs). Dielectrophoretic deposition places a small CNT bundle on top of a plasmonic Au nanodimer. After 'pre-characterizing' both the nanotubes and dimer structure, we subsequently use the tip of an atomic force microscope to push the bundle into the plasmonic hotspot located in the 25 nm wide dimer gap, characterize its location inside the gap, and observe the onset of plasmon-enhanced Raman scattering. Evidence for the activation of the CNT's double-resonant D-mode by the near-field of the plasmonic hotspot is discussed.

Long linear carbon chains encapsulated inside carbon nanotubes are a very close realization of carbyne, the truly one-dimensional allotrope of carbon. Here we study individual pairs of double-walled carbon nanotubes and encapsulated linear carbon chains by tip-enhanced Raman scattering. We observe that the radial breathing mode of the inner nanotube correlates with the frequency of the carbon chain's Raman mode, revealing that the nanotube chirality determines the vibronic and electronic properties of the encapsulated carbon chain. We provide the missing link that connects the properties of the encapsulated long linear carbon chain with the structure of the host nanotube., Comment: keywords: linear carbon chains; carbyne; carbon nanotubes; tip-enhanced Raman scattering; TERS; Significant changes compared to first version of the manuscript. Current version includes Supporting Information

Light interacting with metallic nanoparticles creates a strongly localized near-field around the particle that enhances inelastic light scattering by several orders of magnitude. Surface-enhanced Raman scattering describes the enhancement of the Raman intensity by plasmonic nanoparticles. We present an extensive Raman characterization of a plasmonic gold nanodimer covered with graphene. Its two-dimensional nature and energy-independent optical properties make graphene an excellent material for investigating local electromagnetic near-fields. We show the localization of the near-field of the plasmonic dimer by spatial Raman measurements. Energy- and polarization-dependent measurements reveal the local near-field resonance of the plasmonic system. To investigate the far-field resonance we perform dark-field spectroscopy and find that near-field and far-field resonance energies differ by 170 meV, much more than expected from the model of a damped oscillator (40 meV).

Bottom-up assembly by dielectrophoresis (DEP) has emerged in recent years as a viable alternative to conventional top–down fabrication of electronic devices from nanomaterials, particularly carbon nanotubes and graphene. Here, we demonstrate how this technique can be extended to fabricate devices containing carbon nanotubes and graphene suspended between two electrodes over a back-gate electrode. The suspended device geometry is critical for the development of nano-electromechanical devices and to extract maximum performance out of electronic and optoelectronic devices. This technique allows for parallel assembly of devices over large scale. (© 2015 WILEY-VCH Verlag GmbH &Co. KGaA, Weinheim)

Integrating layered two-dimensional (2D) materials into 3D heterostructures offers opportunities for novel material functionalities and applications in electronics and photonics. In order to build the highest quality heterostructures, it is crucial to preserve the cleanliness and morphology of 2D material surfaces that come in contact with polymers such as PDMS during transfer. Here we report that substantial residues and up to ~0.22% compressive strain can be present in monolayer MoS$_{2}$ flakes transferred using PDMS. We show that a UV-ozone pre-cleaning of the PDMS surface before exfoliation significantly reduces organic residues on transferred MoS$_{2}$ flakes. An additional 200$^{\circ}$C vacuum anneal after transfer efficiently removes interfacial bubbles and wrinkles as well as accumulated strain, thereby restoring the surface morphology of transferred flakes to their native state. Our recipe is important for building clean heterostructures of 2D materials and increasing the reproducibility and reliability of devices based on them., Comment: To appear in Nanotechnology (2018)

Discussions.

The properties of graphene depend sensitively on strain and doping affecting its behavior in devices and allowing an advanced tailoring of this material. A knowledge of the strain configuration, i.e. the relative magnitude of the components of the strain tensor, is particularly crucial, because it governs effects like band-gap opening, pseudo-magnetic fields, and induced superconductivity. It also enters critically in the analysis of the doping level. We propose a method for evaluating unknown strain configurations and simultaneous doping in graphene using Raman spectroscopy. In our analysis we first extract the bare peak shift of the G and 2D modes by eliminating their splitting due to shear strain. The shifts from hydrostatic strain and doping are separated by a correlation analysis of the 2D and G frequencies, where we find ∆ω2D/∆ωG = 2.21 ± 0.05 for pure hydrostatic strain. We obtain the local hydrostatic strain, shear strain and doping without any assumption on the strain configuration prior to the analysis, as we demonstrate for two model cases: Graphene under uniaxial stress and graphene suspended on nanostructures that induce strain. Raman scattering with circular corotating polarization is ideal for analyzing frequency shifts, especially for weak strain when the peak splitting by shear strain cannot be resolved., 2D Materials, 5 (1), ISSN:2053-1583

We report plasmon-enhanced Raman scattering of the order of 103 by a metallic carbon nanotube partially suspended inside a near-field cavity. The tube is part of a small bundle, and is interfaced with an Au nanodisc dimer using a recently developed assembly scheme based on dielectrophoretic deposition. Spatially resolved Raman measurements with two excitation wavelengths and two orthogonal polarizations confirm that the enhancement arises from a 65 nm long suspended tube segment. We show that the orientation of the tube inside the cavity can be as effective for generating enhancement as placing the nanotube precisely in a plasmonic hotspot. Position and shape of the G-peak show that the suspended part of the tube is free of strain and doped with a Fermi energy shift ≤40 meV. (© 2014 WILEY-VCH Verlag GmbH &Co. KGaA, Weinheim)

We present the Raman spectra of metallic carbon nanotubes in solution and deposited onto a Si/SiO2 substrate. In the different nanotube samples, we observe qualitatively similar behavior: an upshifted and narrowed metallic LO peak in solution compared to the spectrum on the substrate. This behavior is due to the Fermi energy shifting away from the intrinsic value in the solutions, which we confirm by in situ electrochemical Raman measurements. Our results have implications for all spectroscopic methods that probe nanotubes in aqueous solutions. Raman spectra of metallic nanotubes in solution (orange) and on a Si/SiO2 substrate (black). The inset depicts the position of the Fermi energy in both situations.

We recently reported a significant deviation in the photoluminescence intensities of HiPco nanotubes solubilized with a perylene-based surfactant, C16, compared to bile salt surfactants. For C16, the photoluminescence emission of chiralities (9,5), (10,3), and (11,1) is enhanced by up to 430%. Resonant Raman spectroscopy is less sensitive to bundling state and also yields disparate chirality intensity ratios: The (11,0) zigzag tube signal increases by 100% compared to (8,6), (9,4), and (10,2) after suspension with C16. We also report the change in photoluminescence intensity distribution after the swelling of bile salt suspended nanotubes with a series of small organic chromophores in DCM. These changes are attributed to chromophore-induced surfactant reorganization, resulting in better nanotube individualization. The chirality for which the PL intensity is most enhanced is (11,1) for all chromophores, a chirality also increased by 300% in the C16-solubilized sample. Conjointly, these measurements indicate that both preferential solubilization and enhanced debundling contribute to the PL intensity distribution in the C16-solubilized nanotube sample. This has wide ranging implications for the design of chirally selective surfactants and the demonstration of their selectivity, which is typically only shown through luminescence measurements. (© 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

We isolated the plasmonic contribution to surface-enhanced Raman scattering (SERS) and found it to be much stronger than expected. Organic dyes encapsulated in single-walled carbon nanotubes are ideal probes for quantifying plasmonic enhancement in a Raman experiment. The molecules are chemically protected through the nanotube wall and spatially isolated from the metal, which prevents enhancement by chemical means and through surface roughness. The tubes carry molecules into SERS hotspots, thereby defining molecular position and making it accessible for structural characterization with atomic-force and electron microscopy. We measured a SERS enhancement factor of 106 on α-sexithiophene (6T) molecules in the gap of a plasmonic nanodimer. This is two orders of magnitude stronger than predicted by the electromagnetic enhancement theory (104). We discuss various phenomena that may explain the discrepancy (including hybridization, static and dynamic charge transfer, surface roughness, uncertainties in molecular position and orientation), but found all of them lacking in enhancement for our probe system. We suggest that plasmonic enhancement in SERS is, in fact, much stronger than currently anticipated. We discuss novel approaches for treating SERS quantum mechanically that appear promising for predicting correct enhancement factors. Our findings have important consequences on the understanding of SERS as well as for designing and optimizing plasmonic substrates.

Pluripotent stem cells represent a promising source of differentiated tissue-specific stem and multipotent progenitor cells for regenerative medicine and drug testing. The realisation of this potential relies on the establishment of robust and reproducible protocols of differentiation. Several reports have highlighted the importance of biomaterials in assisting directed differentiation. Graphene oxide (GO) is a novel material that has attracted increasing interest in the field of biomedicine. In this study, we demonstrate that GO coated substrates significantly enhance the differentiation of mouse embryonic stem (ES) cells to both primitive and definitive haematopoietic cells. GO does not affect cell proliferation or survival of differentiated cells but rather enhances the transition of haemangioblasts to haemogenic endothelial cells, a key step during haematopoietic specification. Importantly, GO also improves, in addition to murine, human ES cell differentiation to blood cells. Taken together, our study reveals a positive role for GO in haematopoietic differentiation and suggests that further functionalization of GO could represent a valid strategy for the generation of large numbers of functional blood cells. Producing these cells would accelerate haematopoietic drug toxicity testing and treatment of patients with blood disorders or malignancies.

Scientific Reports 6: Article number: 2591710.1038/srep25917; published online: May202016; updated: July042016 The original version of this Article contained a typographical error in the spelling of the author Maria Iliut which was incorrectly given as Maria Iluit. This has now been corrected in the PDF and HTML versions of the Article.

We study the photoluminescence and photoluminescence excitation intensities of single-walled carbon nanotubes. To derive the chirality fractions of semiconducting tubes from these optical methods requires a thorough analysis of the experimental parameters and the lifetimes of the excitonic states. We obtain the intensity distribution from the product of the widths of the first and second excitonic transition and the intensity of the absorption of the second excited state. Compared with previous analysis protocols our intensity distribution points towards a chirality abundance which is (i) narrower in diameter, (ii) centred at smaller diameters and (iii) more strongly dominated by armchair-like tubes. We present a recipe for the fit of luminescence data.

A simple, high throughput fractionation procedure for aqueous/SDS (sodium dodecyl sulfate) suspensions of single-walled carbon nanotubes (SWNTs) is presented, which yields thin bundles of semiconducting-SWNTs with small chiral angles. To demonstrate this we show the photoluminescence signatures of nanotube suspensions that contain almost exclusively zigzag and near-zigzag tubes. Starting suspensions and resulting fractions were characterized using optical absorption, resonance Raman and photoluminescence spectroscopies as well as scanning force microscopy. Taken together with literature observations, our findings suggest that near zigzag edge tubes of similar diameters in a bundle are harder to separate from each other than for other chiral index combinations. We discuss the implications of these observations for SWNT growth and dispersion.

In this paper, we investigate how photoluminescence excitation spectra of single-walled carbon nanotubes are influenced by experimental conditions. The use of incoherent light sources leads to a broadening of the second excitonic transition. We describe the broadening by a straight forward simulation and deliver the width of the second excitonic transition free of experimental influences. A set of simulated data allows for the correction of experimental influences for arbitrary nanotubes chiralities and excitation bandpasses.

We investigated the spectral data of three carbon nanotube (CNT) species obtained by Raman spectroscopy and photoluminescence (PL) measurements. The corresponding relative signal intensities without further corrections yielded significantly different relative distributions of the CNT species. Theoretical calculations of optical transition probabilities and electron-phonon coupling were included, providing simple models in order to estimate the relative distribution of the three species within the sample. We proposed the product of PL and PL excitation intensities to be a candidate for quantitative analysis of CNT species. Applying the models, we confirmed that both spectroscopic methods agree on one nanotube species dominating the distribution.

We propose to understand surface-enhanced Raman scattering (SERS) as a higher- order Raman process that contains the plasmonic excitation. The SERS amplitudes are calculated with third- and fourth-order perturbation theory. Treating the plasmonic excitation as a quasiparticle, we derive analytic expressions for all coupling matrix elements. This leads to a general theory of plasmonic enhancement in SERS that can be applied to arbitrary plasmonic nanostructures. We obtain the plasmon eigenvectors of a gold nanosphere and a nanosphere dimer. They are used to calculate the enhancement of the Raman cross section of a molecule coupled to the dipole plasmon mode. The enhancement of the cross section is up to three orders of magnitude stronger than predicted by the theory of electromagnetic enhancement. The difference is most pronounced in vacuum and decreases with increasing dielectric constant of the embedding medium. The predictions from understanding SERS as a higher- order Raman process agree well with recent experiments; they highlight the dominance of plasmonic enhancement in SERS.

We report plasmon-enhanced Raman scattering in graphene coupled to a single plasmonic hotspot measured as a function of laser energy. The enhancement profiles of the G peak show strong enhancement (up to $10^5$) and narrow resonances (30 meV) that are induced by the localized surface plasmon of a gold nanodimer. We observe the evolution of defect-mode scattering in a defect-free graphene lattice in resonance with the plasmon. We propose a quantum theory of plasmon-enhanced Raman scattering, where the plasmon forms an integral part of the excitation process. Quantum interferences between scattering channels explain the experimentally observed resonance profiles, in particular, the marked difference in enhancement factors for incoming and outgoing resonance and the appearance of the defect-type modes., Keywords: plasmon-enhanced Raman scattering, SERS, graphene, quantum interferences, microscopic theory of Raman scattering. Content: 22 pages including 5 figures + 11 pages supporting information

We recently reported a significant deviation in the photoluminescence intensities of HiPco nanotubes solubilized with a perylene-based surfactant, C16, compared to bile salt surfactants. For C16, the photoluminescence emission of chiralities (9,5), (10,3), and (11,1) is enhanced by up to 430%. Resonant Raman spectroscopy is less sensitive to bundling state and also yields disparate chirality intensity ratios: The (11,0) zigzag tube signal increases by 100% compared to (8,6), (9,4), and (10,2) after suspension with C16. We also report the change in photoluminescence intensity distribution after the swelling of bile salt suspended nanotubes with a series of small organic chromophores in DCM. These changes are attributed to chromophore-induced surfactant reorganization, resulting in better nanotube individualization. The chirality for which the PL intensity is most enhanced is (11,1) for all chromophores, a chirality also increased by 300% in the C16-solubilized sample. Conjointly, these measurements indicate that both preferential solubilization and enhanced debundling contribute to the PL intensity distribution in the C16-solubilized nanotube sample. This has wide ranging implications for the design of chirally selective surfactants and the demonstration of their selectivity, which is typically only shown through luminescence measurements.

We realize the coupling of carbon nanotubes as a one-dimensional model system to near-field cavities for plasmon-enhanced Raman scattering. Directed dielectrophoretic assembly places single-walled carbon nanotubes precisely into the gap of gold nanodimers. The plasmonic cavities enhance the Raman signal of a small nanotube bundle by a factor of 103. The enhanced signal arises exclusively from tube segments within the cavity as we confirm by spatially resolved Raman measurements. Through the energy and polarization of the excitation we address the extrinsic plasmonic and the intrinsic nanotube optical response independently. For all incident light polarizations, the nanotube Raman features arise from fully symmetric vibrations only. We find strong evidence that the signal enhancement depends on the orientation of the carbon nanotube relative to the cavity axis. © 2014 American Chemical Society.

The longitudinal optical phonon of metallic nanotubes shifts by 23 cm${}^{\ensuremath{-}1}$ to lower energies when the nanotubes are deposited from a solution onto a substrate. The linewidth increases by 13 cm${}^{\ensuremath{-}1}$. The changes are explained in terms of shifts in the Fermi energy that influence the Kohn anomaly in the longitudinal optical phonon branch in metallic nanotubes. Using in situ electrochemical Raman measurements we show that the Fermi energy is 0.16 eV below its intrinsic value in metallic nanotubes in solution. Our results impact the application of Raman spectroscopy to distinguish between metallic and semiconducting tubes by examining the high-energy mode line shape.

We characterize plasmonic enhancement in a hotspot between two Au nanodisks using Raman scattering of graphene. Single layer graphene is suspended across the dimer cavity and provides an ideal two-dimensional test material for the local near-field distribution. We detect a Raman enhancement of the order of 10(3) originating from the cavity. Spatially resolved Raman measurements reveal a near-field localization one order of magnitude smaller than the wavelength of the excitation, which can be turned off by rotating the polarization of the excitation. The suspended graphene is under tensile strain. The resulting phonon mode softening allows for a clear identification of the enhanced signal compared to unperturbed graphene.

Dieser Beitrag ist mit Zustimmung des Rechteinhabers aufgrund einer (DFG geförderten) Allianz- bzw. Nationallizenz frei zugänglich. This publication is with permission of the rights owner freely accessible due to an Alliance licence and a national licence (funded by the DFG, German Research Foundation) respectively. Taking advantage of the non-covalent interaction between alkyl chains and the sidewalls of a single-walled carbon nanotube (SWCNT), a nanocarbon hybrid of SWCNT and a fullerene (C60) derivative with long alkyl chains was constructed as a donor–acceptor pair for photovoltaics and nanodevice investigations. It was found that SWCNT could be mostly unbundled by the alkylated C60 (1) and was well-dispersed in organic solvents. As a photoactive material, the resultant nanocarbon hybrid, 1-SWCNT, performed well in light-energy harvesting applications in photoelectrochemical cells and nanoscale field-effect transistors (FET). Moreover, the 1-SWCNT assembly exhibited superhydrophobicity, providing an interesting opportunity to fabricate nanocarbon-based waterproof optoelectronic devices. In order to understand the photoexcitation process, the 1-SWCNT assembly was electrochemically and spectroscopically characterized. The electrochemical results showed that the SWCNT facilitated electronic communication between 1 and the electrode. The steady-state and time-resolved fluorescence and the photoluminescence excitation studies suggested efficient quenching of the singlet excited state of C60. Nanosecond transient absorption data revealed the one-electron reduction of fullerene, C60˙−, thereby demonstrating the photoinduced electron transfer from SWCNT to the C60 unit in the 1-SWCNT assembly.