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Singlet fission can generate an exchange-coupled quintet triplet pair state TT, which could lead to the realization of quantum computing and quantum sensing using entangled multiple qubits even at room temperature. However, the observation of the quantum coherence of TT has been limited to cryogenic temperatures, and the fundamental question is what kind of material design will enable its room-temperature quantum coherence. Here, we show that the quantum coherence of singlet fission-derived TT in a chromophore-integrated metal-organic framework can be over hundred nanoseconds at room temperature. The suppressed motion of the chromophores in ordered domains within the metal-organic framework leads to the enough fluctuation of the exchange interaction necessary for TT generation but, at the same time, does not cause severe TT decoherence. Furthermore, the phase and amplitude of quantum beating depend on the molecular motion, opening the way to room-temperature molecular quantum computing based on multiple quantum gate control.
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http://dx.doi.org/10.1126/sciadv.adi3147 | DOI Listing |
J Phys Chem A
September 2025
Department of Chemistry, Virginia Commonwealth University, Richmond, Virginia 23284, United States.
Ionization of alkanes to form radical cations activates their otherwise unreactive C-H bonds, facilitating important chemical processes such as hydrocarbon cracking. This work investigates the radical cation dissociation dynamics of hexane (CH) structural isomers by using femtosecond time-resolved mass spectrometry and quantum chemical calculations. All five isomers exhibit competition between the yields of fragment ions arising from direct C-C bond cleavage or dissociative rearrangement with hydrogen migration on dynamical time scales of ∼50-300 fs, suggesting that hydrogen migration in the metastable cations operates on such short time scales.
View Article and Find Full Text PDFAdv Mater
September 2025
School of Chemistry and Biochemistry, School of Materials Science and Engineering, Center for Organic Photonics and Electronics, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
Molecular spin systems that can be chemically tuned, coherently controlled, and readily integrated within devices remain central to the realization of emerging quantum technologies. Organic high-spin materials are prime candidates owing to their similarity in electronic structure to leading solid-state defect-based systems, light element composition, and the potential for entanglement and qubit operations mediated through spin-spin exchange. However, the inherent instability of these species precludes their rational design, development, and application.
View Article and Find Full Text PDFNat Commun
September 2025
Institute of Physics, University of Rostock, Albert-Einstein-Str. 23, 18059, Rostock, Germany.
The concept of parity-time symmetry has firmly established non-Hermiticity as a versatile degree of freedom on a variety of physical platforms. In general, the non-Hermitian dynamics of open systems are perceived to be inextricably linked to complex-valued potentials facilitating the local attenuation and coherent amplification in wave mechanics. Along these lines, time reversal symmetry is associated with a complex conjugation of the potential landscape, in essence swapping gain and loss.
View Article and Find Full Text PDFSci Adv
September 2025
Laboratory of Ultrafast Spectroscopy, SB-ISIC, and Lausanne Centre for Ultrafast Science (LACUS), Ecole Polytechnique Fédérale de Lausanne, Station 6, CH-1015 Lausanne, Switzerland.
The electronic properties of correlated insulators are governed by the strength of Coulomb interactions, enabling the control of electronic conductivity with external stimuli. This work highlights that the strength of electronic correlations in nickel oxide (NiO), a prototypical charge-transfer insulator, can be coherently reduced by tuning the intensity of an optical pulse excitation. This weakening of correlations persists for hundreds of picoseconds and exhibits a recovery time independent of photodoping density across two orders of magnitude.
View Article and Find Full Text PDFACS Nano
September 2025
School of Physics and Astronomy, Monash University, Clayton, VIC 3800, Australia.
Strong electron-hole interactions in a semimetal or narrow-gap semiconductor may drive a ground state of condensed excitons. Monolayer WTe has been proposed as a host material for such an exciton condensate, but the order parameter─the key signature of a macroscopic quantum-coherent condensate─has not been observed. Here, we use Fourier-transform scanning tunneling spectroscopy (FT-STS) to study quasiparticle interference (QPI) and periodic modulations of the local density of states (LDOS) in monolayer WTe.
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