Triplet excited states in organic molecules are generally optically inactive due to spin-forbidden transitions to the singlet ground state. Recent studies have extensively investigated triplet states to circumvent limitations imposed by spin statistics in organic light-emitting diodes. Room-temperature electrophosphorescence and electrofluorescence have previously been observed in thienyl-substituted phenazines without heavy metals; however, phosphorescence was absent when spin density was localized on the thiophene units, despite the expected heavy-atom effect from the sulfur atom. In this study, we investigate the spin dynamics of thiophene-fused π-systems lacking phenazine units to enable the effective utilization of triplet states in thiophene-containing π-systems. This investigation reveals delayed emission in the excited dimers of fused thiophenes, likely associated with triplet-triplet annihilation. Optical and EPR measurements, together with quantum chemical calculations, indicate that the fused thiophenes form head-to-tail dimers in both the ground and excited states.
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http://dx.doi.org/10.1063/5.0246271 | DOI Listing |
Proc Natl Acad Sci U S A
March 2025
Institute of Physics, École Polytechnique Fédérale de Lausanne, Lausanne CH-1015, Switzerland.
Low-energy excitations play a key role in all condensed-matter systems, yet there is limited understanding of their nature in glasses, where they correspond to local rearrangements of groups of particles. Here, we introduce an algorithm to systematically uncover these excitations up to the activation energy scale relevant to structural relaxation. We use it in a model system to measure the density of states on a scale never achieved before, confirming that this quantity shifts to higher energy under cooling, precisely as the activation energy does.
View Article and Find Full Text PDFJpn J Radiol
March 2025
Department of Radiology, Kyorin University Faculty of Medicine, 6-20-2 Shinkawa, Mitaka, Tokyo, 181-8611, Japan.
Digital subtraction angiography (DSA) is the gold standard for assessing cerebrovascular hemodynamics. DSA is predominantly utilized to evaluate the hemodynamic information of various cerebral diseases. However, DSA is relatively invasive and involves radiation exposure and risks of allergic reactions or renal dysfunction related to iodine-based contrast agents.
View Article and Find Full Text PDFScience
March 2025
D-Wave Quantum Inc., Burnaby, British Columbia, Canada.
Quantum computers hold the promise of solving certain problems that lie beyond the reach of conventional computers. Establishing this capability, especially for impactful and meaningful problems, remains a central challenge. Here we show that superconducting quantum annealing processors can rapidly generate samples in close agreement with solutions of the Schrödinger equation.
View Article and Find Full Text PDFNat Commun
March 2025
Department of Physics, The Ohio State University, Columbus, OH, USA.
We propose a mechanism to explain the emergence of an intermediate gapless spin liquid phase in the antiferromagnetic Kitaev model in an externally applied magnetic field, sandwiched between the well-known gapped chiral spin liquid and the gapped partially polarized phase. We propose that, in moderate fields, π-fluxes nucleate in the ground state and trap Majorana zero modes. As these fluxes proliferate with increasing field, the Majorana zero modes overlap creating an emergent quantum Majorana metallic state with a "Fermi surface" at zero energy.
View Article and Find Full Text PDFJ Comput Chem
March 2025
J. Heyrovský Institute of Physical Chemistry of the Czech Academy of Sciences, Prague 8, Czech Republic.
A computational study of I-BODIPY (2-ethyl-4,4-difluoro-6,7-diiodo-1,3-dimethyl-4-bora-3a,4a-diaza-s-indacene) has been carried out to investigate its key photophysical properties as a potential triplet photosensitizer capable of generating singlet oxygen. Multireference CASPT2 and CASSCF methods have been used to calculate vertical excitation energies and spin-orbit couplings (SOCs), respectively, in a model (mono-iodinated BODIPY) molecule to assess the applicability of the single-reference second-order algebraic diagrammatic construction, ADC(2), method to this and similar molecules. Subsequently, time-dependent density functional theory (TD-DFT), possibly within the Tamm-Dancoff approximation (TDA), using several exchange-correlation functionals has been tested on I-BODIPY against ADC(2), both employing a basis set with a two-component pseudopotential on the iodine atoms.
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