The University of Osaka · Materials Science
Professor Hikaru Sotome's research lab specializes in ultrafast photochemistry and photophysics of functional organic molecules, with a focus on understanding the dynamics of excited-state processes in photochromic systems and stable open-shell organic semiconductors. The lab employs advanced ultrafast laser spectroscopy techniques—such as femtosecond transient absorption and fluorescence spectroscopy—to investigate reaction mechanisms, conical intersections, and non-radiative decay pathways in diarylethenes and triangulene derivatives. A key research direction involves manipulating electronic structures through molecular design, including nitrogen doping and symmetry breaking, to achieve stable triplet states and near-infrared emission. The lab also explores supramolecular self-assembly of π-conjugated molecules, where aggregation-induced emission is achieved through controlled stacking and steric engineering.
Figures are computed from collected data and may differ slightly.
Two-color, two-pulse femtosecond pulsed excitation was applied to the elucidation of the dynamics and mechanism of cycloreversion reaction of a diarylethene derivative in the higher excited states. Transient absorption spectroscopy under one-photon visible excitation revealed that the 1B state produced by the excitation undergoes the internal conversion into the 2A state with a time constant of 200 fs. Geometrical rearrangement of the 2A state takes place concomitantly with the vibrational cooli
A kinetically-stabilized nitrogen-doped triangulene cation derivative has been synthesized and isolated as the stable diradical with a triplet ground state that exhibits near-infrared emission. As was the case for a triangulene derivative we previously synthesized, the triplet ground state with a large singlet-triplet energy gap was experimentally confirmed by magnetic measurements. In contrast to the triangulene derivative, the nitrogen-doped triangulene cation derivative is highly stable even
Off-resonant excitation of the closed-ring isomer of a photochromic diarylethene derivative at 730 nm induced the efficient cycloreversion reaction with a yield of ∼20%, while the reaction yield was only 2% under one-photon excitation at 365 nm. Excitation wavelength dependence of the one-photon cycloreversion reaction yield under steady-state irradiation in a wide wavelength range showed that the specific electronic state leading to the large cycloreversion reaction yield, which is originally f
Because supramolecular polymerization of emissive π-conjugated molecules depends strongly on π-π stacking interaction, the formation of well-defined one-dimensional nanostructures often results in a decrease or only a small increase of emission efficiency. This is also true for our barbiturate-based supramolecular polymers wherein hydrogen-bonded rosettes of barbiturates stack quasi-one-dimensionally through π-π stacking interaction. Herein we report supramolecular polymerization-induced emissio
Dynamics of the cycloreversion reaction of a photochromic diarylethene derivative with a small ring-opening reaction yield (∼1%) was investigated by using femtosecond transient absorption spectroscopy. The reaction rate constant and activation barrier on the reaction coordinate were quantitatively analyzed on the basis of the temperature and excitation wavelength dependencies of the reaction yield and excited state dynamics. From the comparison of the present results with those in a more reactiv
Photocyclization reaction dynamics of an inverse type diarylethene derivative was investigated in alkane solutions by means of ultrafast laser spectroscopies. Femtosecond transient absorption spectroscopy showed that the Franck-Condon state formed by photoexcitation is geometrically relaxed to a transient species within 100 fs and subsequently the cyclization process takes place with a time constant of 36 ps. This time constant is much longer than those in normal type derivatives. Steady-state a
The self-assembled state of molecules plays a pivotal role in determining how inherent molecular properties transform and give rise to supramolecular functionalities and has long attracted attention. However, understanding the influence of morphologies spanning the nano- to mesoscopic scales of supramolecular assemblies derived from identical intermolecular interactions has been notoriously challenging due to dynamic structural change and monomer exchange of assemblies in solution. In this study
The geometrical evolution of the reactant and formation of the photoproduct in the cycloreversion reaction of a diarylethene derivative were probed using time-resolved absorption spectroscopies in the visible to near-infrared and mid-infrared regions. The time-domain vibrational data in the visible region show that the initially formed Franck-Condon state is geometrically relaxed into the minimum in the excited state potential energy surface, concomitantly with the low-frequency coherent vibrati
Near-infrared two-photon absorption and excited state dynamics of a fluorescent diarylethene (fDAE) derivative were investigated by time-resolved absorption and fluorescence spectroscopies. Prescreening with quantum chemical calculation predicted that a derivative with methylthienyl groups (mt-fDAE) in the closed-ring isomer has a two-photon absorption cross-section larger than 1000 GM, which was experimentally verified by Z-scan measurements and excitation power dependence in transient absorpti
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