Ligand-Shell-Directed Assembly and Depolymerization of Patchy Nanoparticles

Offer Zeiri; Yifeng Wang; Alevtina Neyman; Francesco Stellacci; Ira A. Weinstock

doi:10.1002/ange.201207177

Ligand-Shell-Directed Assembly and Depolymerization of Patchy Nanoparticles

Angewandte Chemie International Edition ◽

10.1002/anie.201207177 ◽

2012 ◽

Vol 52 (3) ◽

pp. 968-972 ◽

Cited By ~ 11

Author(s):

Offer Zeiri ◽

Yifeng Wang ◽

Alevtina Neyman ◽

Francesco Stellacci ◽

Ira A. Weinstock

Keyword(s):

Directed Assembly ◽

Ligand Shell ◽

Patchy Nanoparticles

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Self-limiting directional nanoparticle bonding governed by reaction stoichiometry

Science ◽

10.1126/science.aba8653 ◽

2020 ◽

Vol 369 (6509) ◽

pp. 1369-1374 ◽

Cited By ~ 3

Author(s):

Chenglin Yi ◽

Hong Liu ◽

Shaoyi Zhang ◽

Yiqun Yang ◽

Yan Zhang ◽

...

Keyword(s):

Covalent Bonding ◽

High Yield ◽

Hierarchical Nanostructures ◽

Surface Patches ◽

Reactive Polymers ◽

Ligand Shell ◽

Nanoparticle Clusters ◽

Stoichiometric Reaction ◽

Reaction Stoichiometry ◽

Patchy Nanoparticles

Nanoparticle clusters with molecular-like configurations are an emerging class of colloidal materials. Particles decorated with attractive surface patches acting as analogs of functional groups are used to assemble colloidal molecules (CMs); however, high-yield generation of patchy nanoparticles remains a challenge. We show that for nanoparticles capped with complementary reactive polymers, a stoichiometric reaction leads to reorganization of the uniform ligand shell and self-limiting nanoparticle bonding, whereas electrostatic repulsion between colloidal bonds governs CM symmetry. This mechanism enables high-yield CM generation and their programmable organization in hierarchical nanostructures. Our work bridges the gap between covalent bonding taking place at an atomic level and colloidal bonding occurring at the length scale two orders of magnitude larger and broadens the methods for nanomaterial fabrication.

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Directed Assembly of Nanowires using Silicon Grooves and Localized Surface Treatments

10.1557/proc-1144-ll20-11 ◽

2008 ◽

Author(s):

Sabrina Habtoun ◽

Christian Bergaud ◽

Monique Dilhan ◽

David Bourrier

Keyword(s):

Directed Assembly ◽

Surface Treatments

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Engineering Electronic Structure to Protect Phase Memory in Molecular Qubits by Minimising Orbital Angular Momentum

10.26434/chemrxiv.7067645.v1 ◽

2018 ◽

Cited By ~ 1

Author(s):

Ana Maria Ariciu ◽

David H. Woen ◽

Daniel N. Huh ◽

Lydia Nodaraki ◽

Andreas Kostopoulos ◽

...

Keyword(s):

Electron Spin ◽

Quantum Coherence ◽

Quantum Information Processing ◽

Pulse Sequences ◽

Grover Algorithm ◽

Ligand Shell ◽

Information Strategies ◽

Spin Qubit ◽

Molecular Spin ◽

The Impact

Using electron spins within molecules for quantum information processing (QIP) was first proposed by Leuenberger and Loss (1), who showed how the Grover algorithm could be mapped onto a Mn12 cage (2). Since then several groups have examined two-level (S = ½) molecular spin systems as possible qubits (3-12). There has also been a report of the implementation of the Grover algorithm in a four-level molecular qudit (13). A major challenge is to protect the spin qubit from noise that causes loss of phase information; strategies to minimize the impact of noise on qubits can be categorized as corrective, reductive, or protective. Corrective approaches allow noise and correct for its impact on the qubit using advanced microwave pulse sequences (3). Reductive approaches reduce the noise by minimising the number of nearby nuclear spins (7-11), and increasing the rigidity of molecules to minimise the effect of vibrations (which can cause a fluctuating magnetic field via spin-orbit coupling) (9,11); this is essentially engineering the ligand shell surrounding the electron spin. A protective approach would seek to make the qubit less sensitive to noise: an example of the protective approach is the use of clock transitions to render spin states immune to magnetic fields at first order (12). Here we present a further protective method that would complement reductive and corrective approaches to enhancing quantum coherence in molecular qubits. The target is a molecular spin qubit with an effective 2S ground state: we achieve this with a family of divalent rare-earth molecules that have negligible magnetic anisotropy such that the isotropic nature of the electron spin renders the qubit markedly less sensitive to magnetic noise, allowing coherent spin manipulations even at room temperature. If combined with the other strategies, we believe this could lead to molecular qubits with substantial advantages over competing qubit proposals.<br>

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Enhanced-Fluorescence of a Dye on DNA- assembled Gold Nano-Dimers Discriminated by Lifetime Correlation Spectroscopy

10.26434/chemrxiv.5728446.v1 ◽

2017 ◽

Author(s):

Pedro M. R. Paulo ◽

David Botequim ◽

Agnieszka Jóskowiak ◽

Sofia Martins ◽

Duarte M. F. Prazeres ◽

...

Keyword(s):

Single Molecule ◽

Fluorescence Emission ◽

Directed Assembly ◽

Plasmon Mode ◽

Correlation Spectroscopy ◽

Enhanced Fluorescence ◽

Detection Volume ◽

Relaxation Component ◽

Good Agreement ◽

Confocal Detection

<div> <div> <div> <p>We have employed DNA-directed assembly to prepare dimers of gold nanoparticles and used their longitudinally coupled plasmon mode to enhance the fluorescence emission of an organic red-emitting dye, Atto-655. The plasmon- enhanced fluorescence of this dye using dimers of 80 nm particles was measured at single molecule detection level. The top enhancement factors were above 1000-fold in 71% of the dimers within a total of 32 dimers measured, and, in some cases, they reached almost 4000-fold, in good agreement with model simulations. Additionally, fluorescence lifetime correlation analysis enabled the separation of enhanced from non-enhanced emission simultaneously collected in our confocal detection volume. This approach allowed us to recover a short relaxation component exclusive to enhanced emission that is attributed to the interaction of the dye with DNA in the interparticle gaps. </p> </div> </div> </div>

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