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Title: Hierarchical Self-Assembly of Carbon Dots into High-Aspect-Ratio Nanowires

Journal Article · · Nano Letters

Here, we report a spontaneous and hierarchical self-assembly mechanism of carbon dots prepared from citric acid and urea into nanowire structures with large aspect ratios (>50). Scattering-type scanning near-field optical microscopy (s-SNOM) with broadly tunable mid-IR excitation was used to interrogate details of the self-assembly process by generating nanoscopic chemical maps of local wire morphology and composition. s-SNOM images capture the evolution of wire formation and the complex interplay between different chemical constituents directing assembly over the nano- to microscopic length scales. We propose that residual citrate promotes tautomerization of melamine surface functionalities to produce supramolecular shape synthons comprised of melamine-cyanurate adducts capable of forming long-range and highly directional hydrogen-bonding networks. This intrinsic, heterogeneity-driven self-assembly mechanism reflects synergistic combinations of high chemical specificity and long-range cooperativity that may be harnessed to reproducibly fabricate functional structures on arbitrary surfaces.

Research Organization:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)
Grant/Contract Number:
NA0003525; 2154617
OSTI ID:
2311341
Report Number(s):
SAND-2023-13189J
Journal Information:
Nano Letters, Vol. 23, Issue 20; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (39)

Photoinduced Self‐Assembly of Carbon Nitride Quantum Dots journal July 2021
Synthesis of Carbon Dots with Multiple Color Emission by Controlled Graphitization and Surface Functionalization journal November 2017
Graphitic carbon nitride nanotubes: a new material for emerging applications journal January 2020
Infrared Spectroscopic Mapping of Single Nanoparticles and Viruses at Nanoscale Resolution journal July 2006
Discrete boronate ester ladders from the dynamic covalent self-assembly of oligo(phenylene ethynylene) derivatives and phenylenebis(boronic acid) journal January 2020
Specificity in Two-Component Signal Transduction Pathways journal December 2007
Carbon dots with hydrogen bond-controlled aggregation behavior journal January 2023
Citric Acid Derived Carbon Dots, the Challenge of Understanding the Synthesis-Structure Relationship journal December 2020
Luminescence phenomena of carbon dots derived from citric acid and urea – a molecular insight journal January 2018
Molecular Origin and Self-Assembly of Fluorescent Carbon Nanodots in Polar Solvents journal February 2017
Complex shapes self-assembled from single-stranded DNA tiles journal May 2012
Self-assembling fluorescent hydrogel for highly efficient water purification and photothermal conversion journal March 2022
Self-assembly of surface functionalized amphiphilic carbon dots: tuning in morphological manifestations journal January 2019
Citric acid as complexing agent in synthesis of mesoporous strontium titanate via neutral-templated self-assembly sol–gel combustion method journal May 2016
The Role of Surface Groups in Dictating the Chiral‐Solvent‐Induced Assembly of Carbon Dots into Structures Exhibiting Circularly Polarized Luminescence journal December 2022
Induced Supramolecular Chirality in Nanostructured Materials:  Ionic Self-Assembly of Perylene-Chiral Surfactant Complexes journal March 2006
Large and Emissive Crystals from Carbon Quantum Dots onto Interfacial Organized Templates journal August 2020
Absorption Spectra and Tautomerism of Cyanuric Acid, Melamine and Some Related Compounds journal April 1947
The Spectral Signatures of Frenkel Polarons in H- and J-Aggregates journal March 2010
In Situ Visualization of Self-Assembly of Charged Gold Nanoparticles journal February 2013
Poly(ionic liquid)-Assisted Synthesis of Open-Ended Carbon Nitride Tube for Efficient Photocatalytic Hydrogen Evolution under Visible-Light Irradiation journal May 2019
A new approach to measure melamine, cyanuric acid, and melamine cyanurate using surface enhanced Raman spectroscopy coupled with gold nanosubstrates journal March 2008
Multiple mode exciton-vibrational coupling in H-aggregates: Synergistic enhancement of the quantum yield journal March 2010
Insights into photoluminescence mechanisms of carbon dots: advances and perspectives journal April 2021
Tracking the Source of Carbon Dot Photoluminescence: Aromatic Domains versus Molecular Fluorophores journal November 2017
Synthesis and Photoluminescence Mechanism of Multicolored Nitrogen-Doped Carbon Nanodots and Their Application in Polymer Self-Assemblies journal June 2022
Molecular Fluorophores Self-Organize into C-Dot Seeds and Incorporate into C-Dot Structures journal August 2020
Citric Acid-Based Carbon Dots and Their Application in Energy Conversion journal September 2022
The Effect of Hydrogen Bonding on Self‐Assembled Polyaniline Nanostructures journal July 2004
Large-Area Carbon Nanosheets Doped with Phosphorus: A High-Performance Anode Material for Sodium-Ion Batteries journal September 2016
Constraints imposed by non‐functional protein–protein interactions on gene expression and proteome size journal January 2008
Supra-(carbon dots) with versatile morphologies and promising optical properties journal February 2023
Undesired usage and the robust self-assembly of heterogeneous structures journal February 2015
Theoretical Understanding of Structure–Property Relationships in Luminescence of Carbon Dots journal August 2021
Shedding light on the effective fluorophore structure of high fluorescence quantum yield carbon nanodots journal January 2017
FT-Raman Determination of Melamine and Melamine Cyanurate in Nylon journal April 1994
Molecular Sensitivity of Near-Field Vibrational Infrared Imaging journal September 2020
Three-Dimensional Structures Self-Assembled from DNA Bricks journal November 2012
Nanoscale Infrared Absorption Spectroscopy of Individual Nanoparticles Enabled by Scattering-Type Near-Field Microscopy journal July 2011