Journal Name
COMMUNICATION
This journal is © The Royal Society of Chemistry 20xx J. Name ., 2013, 00 , 1-3 | 1
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Received 00th January 20xx,
Accepted 00th January 20xx
DOI: 10.1039/x0xx00000x
www.rsc.org/
Aggregation-induced emission of [3]cumulenes functionalized
with heptagon-containing polyphenylenes
Vicente G. Jiménez,
a
Rubén Tapia,
a
Miguel A. Medel,
a
Inês F. A. Mariz,
b
Tânia Ribeiro,
b
Victor
Blanco,
a
Juan M. Cuerva,
a
Ermelinda Maçôas
b
and Araceli G. Campaña*
a
Lighting on the fluorescence of [3]cumulenes: we report the
luminiscence at room temperature by aggregate formation of
[3]cumulenes functionalized with propeller-like heptagon-
containing polyphenylenes. These endgroups turn on the emission
of a [3]cumulene by steric protection and restriction of their
intramolecular rotations in the aggregates.
[n]Cumulenes, organic molecules with n double bonds in a
contiguous sequence, have attracted increasing interest in
recent years as promising model compounds for the
understanding of carbyne.
1
In comparison to other related
conjugated molecules as polyenes or polyynes, [n]cumulenes
are more reactive and therefore less stable. Nevertheless,
extraordinary synthetic efforts have been made and thus the
structural and electronic properties of [3] to [9]cumulenes have
been studied by X-ray crystallography and UV-Vis absorption
spectroscopy.
2
However, photoluminescence properties of
[n]cumulenes remain almost unexplored.
3
As planar conjugated
systems, [n]cumulenes tend to easily aggregate leading to the
quenching of their emission. Aggregation-caused quenching
(ACQ) is a general effect of conventional π-conjugated
chromophores which limits their applications in biological
aqueous media or as solids or films. In contrast to ACQ, the
alternative phenomenon of aggregation-induced emission (AIE)
has received major attention since B. Z. Tang et. al. described it
in 2001
4
and extensive progress and many applications have
been reported.
5
Typical examples of structural motifs present in
AIE-active molecules are hexaphenylsilole (HPS) or
tetraphenylethene (TPE, Chart 1).
6
As AIE-luminogens, both
compounds are non-emissive in solution, as solvation allows the
rotation of their phenyl rings which dissipates their excited-
state energy by a non-radiative deactivation. In contrast, their
emission is activated upon aggregation due to the restriction of
the intramolecular motion (RIM) of the phenyl rings resulting in
slower non-radiative decay rates and higher fluorescence
emission yields.
We envisioned that the introduction of adequate endgroups
could turn on the emission of [3]cumulenes at room
temperature in polar media as a result of an AIE phenomenon.
Hence, herein we report that the steric protection of the
[3]cumulene fluorophore by propeller-like heptagon-containing
polyphenylenes as endgroups turns on its emission upon
aggregation (Chart 1, compound 1). In addition, we show the
two-photon based upconversion of the [3]cumulene 1-
aggregates. This strategy opens up the possibility of using
[n]cumulenes as active luminogens upon aggregation.
Chart 1 Compounds studied as AIE-emitters: [3]cumulene derivatives 1-4 and
tetraphenylbutatriene (TPBT). Related previously reported AIE-luminogens
tetraphenylethene (TPE)
6b
and 5,5’-dibenzo[a,d][7]annulenylidene (BDBA)
10
.
a.
Departamento de Química Orgánica. Facultad de Ciencias, Universidad de
Granada, E-18071 Granada, Spain.
b.
Centro de Química Estructural and Institute of Nanoscience and Nanotechnology
(IN), Instituto Superior Técnico, University of Lisbon, Av. Rovisco Pais, 1, 1049-001
Lisboa, Portugal.
Electronic Supplementary Information (ESI) available: General details, synthesis and
spectroscopy data. Experimental details on optical measurements. Crystal data and
structure refinement of compounds 1, 3, 8 and TPBT. CCDC 1817320-1817323.
Further details on theoretical calculations and Cartesian coordinates of computed
structures. See DOI: 10.1039/x0xx00000x