Observation of “Stick” and “Handle” Intermediates along the Fullerene Road

Shvartsburg, Alexandre A.; Hudgins, Robert R.; Dugourd, Philippe; Gutiérrez, Rafael; Frauenheim, Thomas; Jarrold, Martin F.

doi:10.1103/physrevlett.84.2421

Cited by 55 publications

(63 citation statements)

References 36 publications

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“…However, C 61 H + 2 might be more stable. Also note that small carbon chains attached to fullerenes seem to be pretty stable in laboratory conditions of fullerene formation (Pellarin et al 2002;Shvartsburg et al 2000), while C + accretion might efficiently grow such chains in interstellar conditions.…”

Section: Chemistry -Preliminary Remarksmentioning

confidence: 99%

Interstellar fullerene compounds and diffuse interstellar bands

Omont

2016

A&A

100

103

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Recently, the presence of fullerenes in the interstellar medium (ISM) has been confirmed and new findings suggest that these fullerenes may possibly form from polycyclic aromatic hydrocarbons (PAHs) in the ISM. Moreover, the first confirmed identification of two strong diffuse interstellar bands (DIBs) with the fullerene, C + 60 , connects the long standing suggestion that various fullerenes could be DIB carriers. These new discoveries justify reassessing the overall importance of interstellar fullerene compounds, including fullerenes of various sizes with endohedral or exohedral inclusions and heterofullerenes (EEHFs). The phenomenology of fullerene compounds is complex. In addition to fullerene formation in grain shattering, fullerene formation from fully dehydrogenated PAHs in diffuse interstellar clouds could perhaps transform a significant percentage of the tail of low-mass PAH distribution into fullerenes including EEHFs. But many uncertain processes make it extremely difficult to assess their expected abundance, composition and size distribution, except for the substantial abundance measured for C + 60 . EEHFs share many properties with pure fullerenes, such as C 60 , as regards stability, formation/destruction and chemical processes, as well as many basic spectral features. Because DIBs are ubiquitous in all lines of sight in the ISM, we address several questions about the interstellar importance of various EEHFs, especially as possible carriers of diffuse interstellar bands. Specifically, we discuss basic interstellar properties and the likely contributions of fullerenes of various sizes and their charged counterparts such as C + 60 , and then in turn: 1) metallofullerenes; 2) heterofullerenes; 3) fulleranes; 4) fullerene-PAH compounds; 5) H 2 @C 60 . From this reassessment of the literature and from combining it with known DIB line identifications, we conclude that the general landscape of interstellar fullerene compounds is probably much richer than heretofore realized. EEHFs, together with pure fullerenes of various sizes, have many properties necessary to be suitably carriers of DIBs: carbonaceous nature; stability and resilience in the harsh conditions of the ISM; existing with various heteroatoms and ionization states; relatively easy formation; few stable isomers; spectral lines in the right spectral range; various and complex energy internal conversion; rich Jahn-Teller fine structure. This is supported by the first identification of a DIB carrier as C + 60 . Unfortunately, the lack of any precise information about the complex optical spectra of EEHFs and most pure fullerenes other than C 60 and about their interstellar abundances still precludes definitive assessment of the importance of fullerene compounds as DIB carriers. Their compounds could significantly contribute to DIBs, but it still seems difficult that they are the only important DIB carriers. Regardless, DIBs appear as the most promising way of tracing the interstellar abundances of various fullerene compounds if the breakthr...

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Section: Chemistry -Preliminary Remarksmentioning

confidence: 99%

Interstellar fullerene compounds and diffuse interstellar bands

Omont

2016

A&A

100

103

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“…Although a general and comprehensive understanding of the assembling of carbon nanostructures is still lacking, it is generally accepted that linear carbon sp chains are essential ingredients for the formation of carbon fullerenes and nanotubes [6,7]. In particular, while calculations show that carbon chains are stable in high-temperature carbon plasma [8], experiments prove that small sp clusters are found in the mass spectra of laser vaporized graphite [9].…”

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confidence: 99%

“…They are considered as highly reactive, metastable structures, evolving to fullerene cages under annealing [2,3,6,11]. Since they are considered as unstable, non-fullerene clusters have never been considered as building blocks for solid-state carbon structures integrally formed by (or containing) sp species, such as, for example, carbyne or graphine [12]- [14].…”

mentioning

confidence: 99%

“…Gas-phase ion chromatography has shown that clusters up to hundreds of atoms can have, under particular conditions, different isomeric forms consisting of fullerene cages with the short chains attached in stick-and-handle configurations [6]. These are considered as metastable structures and it is generally assumed that large carbon clusters have a fullerene-like structure with sp 2 bonding [2,6]. The presence of very large odd clusters has never been reported in the literature and it suggests that the clusters produced in the PMCS are different from those produced under significant thermal annealing.…”

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confidence: 99%

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Leaving the fullerene road: presence and stability of sp chains in sp²carbon clusters and cluster-assembled solids

et al. 2005

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Abstract. We report an experimental and theoretical investigation of the growth and structure of large carbon clusters produced in a supersonic expansion by a pulsed microplasma source. The absence of a significant thermal annealing during the cluster growth causes the formation of disordered structures, where sp 2 and sp hybridizations coexist for particles larger than ∼90 atoms. Among the various structures, we recognize sp 2 closed networks encaging sp chains. This 'nutshell' configuration can prevent the fragmentation of sp species upon deposition of the clusters, thus allowing the formation of nanostructured films containing carbynoid species, as shown by Raman spectroscopy. Atomistic simulations confirm that the observed Raman spectra are the signature of the sp/sp 2 hybridization typical of isolated clusters and surviving in the film and they provide information about the structure of the sp chains. Endohedral sp chains in sp 2 cages represent a novel way in which carbon nanostructures may be organized with potentially interesting functional properties.

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“…According to both the experimental and theoretical data in the literature, a very small carbon cluster of a few atoms should be linear in structure; if more C atoms are added, it changes to a monocyclic or polycyclic structure at the first critical size, which is in the range of 4 n 1st cri (C) 8 [414]. At the second critical size, which is in the range of 20 < n 2nd cri (C) 30, the C cluster changes to the fullerene form [415][416][417][418][419]. At the critical size of about n 3rd cri (C) ∼ 300 carbon atoms (or a diameter of ∼ 1.3 nm), the carbon cluster becomes an octahedral nanodiamond [420].…”

Section: Critical Size For the Structural Transformation On The Nanosmentioning

confidence: 99%

Self-assembly of InAs quantum dots on GaAs(001) by molecular beam epitaxy

Jin

2015

Front. Phys.

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Currently, the nature of self-assembly of three-dimensional epitaxial islands or quantum dots (QDs) in a lattice-mismatched heteroepitaxial growth system, such as InAs/GaAs(001) and Ge/Si(001) as fabricated by molecular beam epitaxy (MBE), is still puzzling. The purpose of this article is to discuss how the self-assembly of InAs QDs in MBE InAs/GaAs(001) should be properly understood in atomic scale. First, the conventional kinetic theories that have traditionally been used to interpret QD self-assembly in heteroepitaxial growth with a significant lattice mismatch are reviewed briefly by examining the literature of the past two decades. Second, based on their own experimental data, the authors point out that InAs QD self-assembly can proceed in distinctly different kinetic ways depending on the growth conditions and so cannot be framed within a universal kinetic theory, and, furthermore, that the process may be transient, or the time required for a QD to grow to maturity may be significantly short, which is obviously inconsistent with conventional kinetic theories. Third, the authors point out that, in all of these conventional theories, two well-established experimental observations have been overlooked: i) A large number of “floating” indium atoms are present on the growing surface in MBE InAs/GaAs(001); ii) an elastically strained InAs film on the GaAs(001) substrate should be mechanically unstable. These two well-established experimental facts may be highly relevant and should be taken into account in interpreting InAs QD formation. Finally, the authors speculate that the formation of an InAs QD is more likely to be a collective event involving a large number of both indium and arsenic atoms simultaneously or, alternatively, a morphological/structural transformation in which a single atomic InAs sheet is transformed into a three-dimensional InAs island, accompanied by the rehybridization from the sp 2-bonded to sp 3-bonded atomic configuration of both indium and arsenic elements in the heteroepitaxial growth system.

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Observation of “Stick” and “Handle” Intermediates along the Fullerene Road

Cited by 55 publications

References 36 publications

Interstellar fullerene compounds and diffuse interstellar bands

Interstellar fullerene compounds and diffuse interstellar bands

Leaving the fullerene road: presence and stability of sp chains in sp²carbon clusters and cluster-assembled solids

Self-assembly of InAs quantum dots on GaAs(001) by molecular beam epitaxy

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Observation of “Stick” and “Handle” Intermediates along the Fullerene Road

Cited by 55 publications

References 36 publications

Interstellar fullerene compounds and diffuse interstellar bands

Interstellar fullerene compounds and diffuse interstellar bands

Leaving the fullerene road: presence and stability of sp chains in sp2carbon clusters and cluster-assembled solids

Self-assembly of InAs quantum dots on GaAs(001) by molecular beam epitaxy

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Leaving the fullerene road: presence and stability of sp chains in sp²carbon clusters and cluster-assembled solids