FULL PAPER
DOI: 10.1002/ejoc.201500503
Identifying Solid Luminogens through Gold-Catalysed Intramolecular
Hydroarylation of Alkynes
Aslam C. Shaikh,
[a]
S. Shalini,
[b]
Ramanathan Vaidhyanathan,
[b]
Manoj V. Mane,
[c]
Ayan Kumar Barui,
[d]
Chitta Ranjan Patra,
[d]
Yeduru Venkatesh,
[e]
Prakriti Ranjan Bangal,
[e]
and Nitin T. Patil*
[a]
Keywords: Fluorescence / Luminescence / Solvatochromism / Cell imaging / Dyes/pigments / Gold
The identification of a new class of luminogens based on pyr-
rolo-quinoxaline embedded coumarin (PQC) structures is re-
ported. The reaction relies on the gold-catalyzed hydroaryl-
ation reaction of appropriately substituted aryl alkynoates
Introduction
Luminescent compounds continue to attract intense
interest because of their multifaceted use as probes for bio-
logical applications and molecular sensors and in optoelec-
tronic devices.
[1]
Usually, organic fluorophores are emissive
in solutions but they become nonfluorescent upon aggrega-
tion. Tang and co-workers found that some compounds do
emit light in the solid state
[1d,2]
– the phenomenon was
referred as aggregation-induced emission (AIE) or aggrega-
tion-induced emission enhancement (AIEE).
[3]
However,
the number of materials with AIE/AIEE properties are very
limited to date and such compounds are based on only few
structural frameworks.
[4]
Therefore, the identification of
structurally novel solid emitters with useful photophysical
properties is highly desirable.
Recently, we reported a relay
[5]
catalytic branching
cascade (RCBC), a novel technique for accessing new
scaffolds in diversity oriented synthesis to produce a variety
of polyheterocyclic scaffolds.
[6]
During the study it was ob-
served that many products exhibited weak fluorescence as
[a] Organic Chemistry Division, CSIR – National Chemical
Laboratory,
Dr. Homi Bhabha Road, Pune 411008, India
E-mail: n.patil@ncl.res.in
http:/academic.ncl.res.in/n.patil
[b] Department of Chemistry, Indian Institute of Science
Education and Research,
Pune 411008, India
[c] Physical Chemistry Division, CSIR – National Chemical
Laboratory,
Pune 411008, India
[d] Department of Chemical Biology, CSIR – Indian Institute of
Chemical Technology,
Hyderabad 500607, India
[e] Inorganic and Physical Chemistry Division, CSIR – Indian
Institute of Chemical Technology,
Hyderabad 500607, India
Supporting information for this article is available on the
WWW under http://dx.doi.org/10.1002/ejoc.201500503.
© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim Eur. J. Org. Chem. 2015, 4860–4867 4860
that produces molecules that exhibit solvatochromism and
aggregation-induced emission enhancement (AIEE) phen-
omena. The application of PQCs for live cell imaging has also
been demonstrated.
the structure became planar and rigid. We envisaged that
one of the products obtained from RCBC (cf. P1-OH, Fig-
ure 1) would couple with various aryl propiolic acids A to
give the corresponding alkynoates, which would undergo
metal-catalysed intramolecular hydroarylation reaction to
give luminogens. The following approximations were taken
into consideration for successful design of the strategy:
(1) coumarin-based fluorophores are known in the litera-
ture;
[7]
it is also known that the position of an additional
cycle at the coumarin chromophore increases the quantum
efficiency in solution.
[8]
(2) The presence of flat disk-like
aromatic molecules at the β-position of the -C=O group
will disrupt the planarity, hampering intramolecular rota-
tion (IMR), which is the main requirement for the molecule
to be a solid emitter.
[3]
(3) When structures that are cyclic,
rigid, and electron-donating (e.g., a nitrogen atom) are
attached to the aromatic ring of coumarin the overall push-
pull effect is enhanced. Notably, 7-aminocoumarins are well
known for exhibiting fluorescence in the solution state;
[9]
however, to our knowledge, there is only one report on so-
lid-state emission.
[8a]
Recently, Lavis and co-workers mea-
sured the increase in quantum yield when the N,N-dimethyl
Figure 1. Design of luminescent solid material.