SearcharxivSearch

arXiv subjects

Finn L. Sebastian

Publications and source records attributed to Finn L. Sebastian.

8 recordsLinked to original sources

Resolving Scale-Dependent Diffusivity in the Brain Extracellular Space

Transport through the brain extracellular space has traditionally been summarized by effective diffusion coefficients measured over specific observation ranges. Whether local mobility remains predictive as the same molecule explores larger distances remains unresolved. Here, we track individual ultrashort carbon nanotubes in three dimensions within living hippocampal tissue, following their motion from nanometre to micrometre scales. Using freely diffusing nanotubes in water as an experimental reference, we resolve trajectory-specific crossover lengths beyond which instantaneous diffusivity decreases, with slice-level medians of 0.67 $\mu$m in the pyramidal layer and 0.52 $\mu$m in the radiatum. The pyramidal layer combines higher short-time diffusivity with an approximately twofold larger post-crossover restriction exponent than the radiatum ($\vartheta$ = 0.77 versus 0.38). This decoupling of local mobility from larger-scale exploration is incompatible with a scale-independent rescaling of transport, showing that effective extracellular diffusivity must be interpreted relative to the scale of exploration.

physics.bio-ph

Photonic Waveguide Circuit Integrated with Carbon Nanotube Single-Photon Source Operating at Room Temperature

Photonic integrated circuits require robust room-temperature single-photon sources to enable scalable quantum technologies. Single-walled carbon nanotubes (CNTs), with their unique excitonic properties and chemical tunability, are attractive candidates, but their integration into photonic circuits remains challenging. In this work, we demonstrate the integration of functionalized CNTs as room-temperature single-photon emitters into photonic cavities and waveguide circuits. (6,5) CNTs with aryl sp$^3$ defects are either stochastically deposited via drop-casting or deterministically positioned on photonic cavities using an anthracene-assisted transfer method guided by real-time photoluminescence monitoring. Photoluminescence spectra reveal cavity-enhanced emission, while second-order autocorrelation measurements confirm single-photon propagation through the photonic integrated circuit, highlighting the potential of CNTs for scalable, room-temperature quantum photonic applications.

physics.optics

Ultrashort Carbon Nanotubes with Luminescent Color Centers are Bright NIR-II Nano-Emitters

In the fields of bioimaging, photonics, and quantum science, it is equally crucial to combine high brightness with nanoscale size in short-wave infrared (SWIR) emitters. However, such nano-emitters are currently lacking. Here, we report that when functionalized with luminescent color centers, ultrashort carbon nanotubes with length much shorter than 100 nm, are surprisingly bright in the near-infrared second-biological window (NIR-II) of the SWIR domain. We discuss the origin of this exceptional brightness based on the uncontrollable presence of quenching defects in dispersed carbon nanotubes. We further investigate the nonlinear photoluminescence behavior of color centers functionalized carbon nanotubes in response to varying excitation conditions, spanning from ensemble measurements to single-nanotube experiments. We discuss how this behavior influences the determination of their photoluminescence quantum yields, which can reach values as high as 20% for ultrashort ones detected at the single nanotube level. Notably, the corresponding NIR-II brightness exceeds that of well-known visible emitters, including quantum dots. After rendering them biocompatible, we demonstrate point-spread function engineering and high-resolution, 3-dimensional single-particle tracking using these bright ultrashort carbon nanotubes allowing nanoscale imaging in the NIR-II window within thick brain tissue.

cond-mat.mtrl-sci

How to Recognize Clustering of Luminescent Defects in Single-Wall Carbon Nanotubes

Semiconducting single-wall carbon nanotubes (SWCNTs) are a promising material platform for near-infrared in-vivo imaging, optical sensing, and single-photon emission at telecommunication wavelengths. The functionalization of SWCNTs with luminescent defects can lead to significantly enhanced photoluminescence (PL) properties due to efficient trapping of highly mobile excitons and red-shifted emission from these trap states. Among the most studied luminescent defect types are oxygen and aryl defects that have largely similar optical properties. So far, no direct comparison between SWCNTs functionalized with oxygen and aryl defects under identical conditions has been performed. Here, we employ a combination of spectroscopic techniques to quantify the number of defects, their distribution along the nanotubes and thus their exciton trapping efficiencies. The different slopes of Raman D/G+ ratios versus calculated defect densities from PL quantum yield measurements indicate substantial dissimilarities between oxygen and aryl defects. Supported by statistical analysis of single-nanotube PL spectra at cryogenic temperatures it reveals clustering of oxygen defects. The clustering of 2-3 oxygen defects, which act as a single exciton trap, occurs irrespective of the functionalization method and thus enables the use of simple equations to determine the density of oxygen defects and oxygen defect clusters in SWCNTs based on standard Raman spectroscopy. The presented analytical approach is a versatile and sensitive tool to study defect distribution and clustering in SWCNTs and can be applied to any new functionalization method.

cond-mat.mtrl-sci

Easy Access to Bright Oxygen Defects in Biocompatible Single-Walled Carbon Nanotubes via a Fenton-Like Reaction

The covalent functionalization of single-walled carbon nanotubes (SWNTs) with luminescent oxygen defects increases their brightness and enables their application as optical biosensors or fluorescent probes for in-vivo imaging in the second-biological window (NIR-II). However, obtaining luminescent defects with high brightness is challenging with the current functionalization methods due to a restricted window of reaction conditions or the necessity for controlled irradiation with ultraviolet light. Here we report a method for introducing luminescent oxygen defects via a Fenton-like reaction that uses benign and inexpensive chemicals without light irradiation. (6,5) SWNTs in aqueous dispersion functionalized with this method show bright $E_{11}$* emission (1105 nm) with 3.2-times higher peak intensities than the pristine $E_{11}$ emission and a reproducible photoluminescence quantum yield of 3%. The functionalization can be performed within a wide range of reaction parameters and even with unsorted nanotube raw material at high concentrations (100 mg/L), giving access to large amounts of brightly luminescent SWNTs. We further find that the introduced oxygen defects rearrange under light irradiation, which gives additional insights into the structure and dynamics of oxygen defects. Finally, the functionalization of ultra-short SWNTs with oxygen defects also enables high photoluminescence quantum yields and their excellent emission properties are retained after surfactant exchange with biocompatible pegylated phospholipids or single-stranded DNA to make them suitable for in-vivo NIR-II imaging and dopamine sensing.

cond-mat.mtrl-sci

Unified Quantification of Quantum Defects in Small-Diameter Single-Walled Carbon Nanotubes by Raman Spectroscopy

The covalent functionalization of single-walled carbon nanotubes (SWCNTs) with luminescent quantum defects enables their application as near-infrared single-photon sources, as optical sensors, and for in-vivo tissue imaging. Tuning the emission wavelength and defect density are crucial for these applications. While the former can be controlled by different synthetic protocols and is easily measured, defect densities are still determined as relative rather than absolute values, limiting the comparability between different nanotube batches and chiralities. Here, we present an absolute and unified quantification metric for the defect density in SWCNT samples based on Raman spectroscopy. It is applicable to a range of small-diameter nanotubes and for arbitrary laser wavelengths. We observe a clear inverse correlation of the D/G$^{+}$ ratio increase with nanotube diameter, indicating that curvature effects contribute significantly to the defect-activation of Raman modes. Correlation of intermediate frequency modes with defect densities further corroborates their activation by defects and provides additional quantitative metrics for the characterization of functionalized SWCNTs.

cond-mat.mtrl-sci

Tuning Electroluminescence from Functionalized SWCNT Networks further into the Near-Infrared

Near-infrared electroluminescence from carbon-based emitters, especially in the second biological window (NIR-II) or at telecommunication wavelengths, is difficult to achieve. Single-walled carbon nanotubes (SWCNTs) have been proposed as a possible solution due to their tunable and narrowband emission in the near-infrared and high charge carrier mobilities. Furthermore, the covalent functionalization of SWCNTs with a controlled number of luminescent sp$^{3}$ defects leads to even more red-shifted photoluminescence with enhanced quantum yields. Here, we demonstrate that by tailoring the binding configuration of the introduced sp$^{3}$ defects and hence tuning their optical trap depth we can generate emission from polymer-sorted (6,5) and (7,5) nanotubes that is mainly occurring in the telecommunication O-band (1260-1360 nm). Networks of these functionalized nanotubes are integrated in ambipolar, light-emitting field-effect transistors to yield the corresponding narrowband near-infrared electroluminescence. Further investigation of the current and carrier density-dependent electro- and photoluminescence spectra enable insights into the impact of different sp$^{3}$ defects on charge transport in networks of functionalized SWCNTs.

physics.app-ph

Absolute Quantification of sp$^{3}$ Defects in Semiconducting Single-Wall Carbon Nanotubes by Raman Spectroscopy

The functionalization of semiconducting single-wall carbon nanotubes (SWCNTs) with luminescent sp$^{3}$ defects creates red-shifted emission features in the near-infrared and boosts their photoluminescence quantum yields (PLQYs). While multiple synthetic routes for the selective introduction of sp$^{3}$ defects have been developed, a convenient metric to precisely quantify the number of defects on a SWCNT lattice is not available. Here, we present a direct and simple quantification protocol based on a linear correlation of the integrated Raman D/G$^{+}$ signal ratios and defect densities as extracted from PLQY measurements. Corroborated by a statistical analysis of single-nanotube emission spectra at cryogenic temperature, this method enables the quantitative evaluation of sp$^{3}$ defect densities in (6,5) SWCNTs with an error of $\pm$ 3 defects per micrometer and the determination of oscillator strengths for different defect types. The developed protocol requires only standard Raman spectroscopy and is independent of the defect configuration, dispersion solvent and nanotube length.

cond-mat.mtrl-sci