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Papers by Anuja Singh
Physical Chemistry Chemical Physics, 2018
Photophysical understanding of organic fluorophores with π-conjugated scaffolds is crucial as suc... more Photophysical understanding of organic fluorophores with π-conjugated scaffolds is crucial as such dyes are central to optoelectronic applications.
The Journal of Physical Chemistry A, 2019
Organic fluorophores with extended π-conjugation are important for their widespread applications.... more Organic fluorophores with extended π-conjugation are important for their widespread applications. The present work provides photophysical insights of a diacetylene bridged classical donor-acceptor electronic energy pair, naphthalene-pyrene, in comparison with its part molecular structures, naphthyl and pyrenyl acetylenes as well as parent naphthalene and pyrene chromophores. The diacetylenic dye loses individual spectral identities of the donor and acceptor fluorophores exhibiting a locally excited (LE) emission (~411 nm) from the overall molecular entity with high fluorescence quantum yields (0.55-0.84) in non-aqueous media. In contrast to parent pyrene, the hybrid derivative shows strongly allowed S0→S1 transition. In mixed-aqueous media, the dye forms J-aggregates displaying a new red-shifted absorption (~425 nm) as well as emission (~510 nm) band. Unlike the hybrid dye, the naphthyl and pyrenyl acetylenes do not form aggregates. In the aggregate state of the hybrid fluorophore, electronic energy transfer takes place from the naphthyl moiety to pyrenyl ring. The excited state photophysical properties of the dye is exploited to vapor sensing in solid state.
Chemical Physics, 2019
Fluorescent aggregates find widespread applications in modern optoelectronics. Here, we study the... more Fluorescent aggregates find widespread applications in modern optoelectronics. Here, we study the photophysics of organic fluorophores composed of benzene, pyrene, naphthalene, and anthracene moieties connected via a Y-shaped enediyne π-spacer in water-acetonitrile solvent mixtures and solid forms. The fluorophores show a predominant aggregate emission band, which is ca. 4000 cm −1 red-shifted compared to their locally excited (LE) emission energies in water-acetonitrile. The aggregate emission is however blue-shifted compared to an intramolecular charge transfer (ICT) emission band. The interplay of the LE, ICT, and aggregate emissive states depends on peripheral aromatic units, electronic substituents and microenvironments. The LE to aggregate emission spectral shift is exploited to sensitively probe micro-heterogeneity in bile salts, which are complemented by fluorescence intensity and fluorescence anisotropy changes. The solution phase aggregate emissions closely resemble the solid state aggregate emission bands, which are attributed to excimer states. The aggregate fluorescence states in the solids are altered by external stimuli and reversibly switched multiple of cycles. The aggregates undergo photoreactions in mixed-aqueous solvents, but they remain unreactive in solid powder forms.
Resolving fluorescence signatures of a photoconvertible fluorophore by fluorescence spectroscopy and MCR-ALS-based combinatorial approach
Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, 2021
Photoconvertible fluorophores are important for a myriad of applications in chemistry and biology... more Photoconvertible fluorophores are important for a myriad of applications in chemistry and biology. Here, we spectrally resolve and quantify individual photophysical information of a dual-emitting photoconvertible fluorophore by fluorescence spectroscopy and multivariate curve resolution-alternate least square techniques. We found that the reactant fluorophore, which shows a weak locally excited (LE) emission and a dominant intramolecular charge transfer (ICT) emission, also exhibits an intermolecular charge transfer emission. The ICT emission bands of both the reactant and product fluorophores are originated from their respective LE states. The reactant fluorophore is a mixture of its different ground state conformers. Higher yields of photoconversion of the yellow-emitting reactant fluorophore are achieved via a visible light photoreaction, leading to formation of pure white light at an intermediate photoreaction time. These findings together help us to glean new photophysical and photochemical insights into the photoreaction of a dual-emitting photoconvertible fluorophore.
Physical Chemistry Chemical Physics, 2018
Photophysical understanding of organic fluorophores with π-conjugated scaffolds is crucial as suc... more Photophysical understanding of organic fluorophores with π-conjugated scaffolds is crucial as such dyes are central to optoelectronic applications.
The Journal of Physical Chemistry A, 2019
Organic fluorophores with extended π-conjugation are important for their widespread applications.... more Organic fluorophores with extended π-conjugation are important for their widespread applications. The present work provides photophysical insights of a diacetylene bridged classical donor-acceptor electronic energy pair, naphthalene-pyrene, in comparison with its part molecular structures, naphthyl and pyrenyl acetylenes as well as parent naphthalene and pyrene chromophores. The diacetylenic dye loses individual spectral identities of the donor and acceptor fluorophores exhibiting a locally excited (LE) emission (~411 nm) from the overall molecular entity with high fluorescence quantum yields (0.55-0.84) in non-aqueous media. In contrast to parent pyrene, the hybrid derivative shows strongly allowed S0→S1 transition. In mixed-aqueous media, the dye forms J-aggregates displaying a new red-shifted absorption (~425 nm) as well as emission (~510 nm) band. Unlike the hybrid dye, the naphthyl and pyrenyl acetylenes do not form aggregates. In the aggregate state of the hybrid fluorophore, electronic energy transfer takes place from the naphthyl moiety to pyrenyl ring. The excited state photophysical properties of the dye is exploited to vapor sensing in solid state.
Chemical Physics, 2019
Fluorescent aggregates find widespread applications in modern optoelectronics. Here, we study the... more Fluorescent aggregates find widespread applications in modern optoelectronics. Here, we study the photophysics of organic fluorophores composed of benzene, pyrene, naphthalene, and anthracene moieties connected via a Y-shaped enediyne π-spacer in water-acetonitrile solvent mixtures and solid forms. The fluorophores show a predominant aggregate emission band, which is ca. 4000 cm −1 red-shifted compared to their locally excited (LE) emission energies in water-acetonitrile. The aggregate emission is however blue-shifted compared to an intramolecular charge transfer (ICT) emission band. The interplay of the LE, ICT, and aggregate emissive states depends on peripheral aromatic units, electronic substituents and microenvironments. The LE to aggregate emission spectral shift is exploited to sensitively probe micro-heterogeneity in bile salts, which are complemented by fluorescence intensity and fluorescence anisotropy changes. The solution phase aggregate emissions closely resemble the solid state aggregate emission bands, which are attributed to excimer states. The aggregate fluorescence states in the solids are altered by external stimuli and reversibly switched multiple of cycles. The aggregates undergo photoreactions in mixed-aqueous solvents, but they remain unreactive in solid powder forms.
Resolving fluorescence signatures of a photoconvertible fluorophore by fluorescence spectroscopy and MCR-ALS-based combinatorial approach
Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, 2021
Photoconvertible fluorophores are important for a myriad of applications in chemistry and biology... more Photoconvertible fluorophores are important for a myriad of applications in chemistry and biology. Here, we spectrally resolve and quantify individual photophysical information of a dual-emitting photoconvertible fluorophore by fluorescence spectroscopy and multivariate curve resolution-alternate least square techniques. We found that the reactant fluorophore, which shows a weak locally excited (LE) emission and a dominant intramolecular charge transfer (ICT) emission, also exhibits an intermolecular charge transfer emission. The ICT emission bands of both the reactant and product fluorophores are originated from their respective LE states. The reactant fluorophore is a mixture of its different ground state conformers. Higher yields of photoconversion of the yellow-emitting reactant fluorophore are achieved via a visible light photoreaction, leading to formation of pure white light at an intermediate photoreaction time. These findings together help us to glean new photophysical and photochemical insights into the photoreaction of a dual-emitting photoconvertible fluorophore.