We examine electron-electron mediated relaxation following ultrafast electric field pump excitation of the fermionic degrees of freedom in the Falicov-Kimball model for correlated electrons. The results reveal a dichotomy in the temporal evolution of the system as one tunes through the Mott metal-to-insulator transition: in the metallic regime relaxation can be characterized by evolution toward a steady state well described by Fermi-Dirac statistics with an increased effective temperature; however, in the insulating regime this quasithermal paradigm breaks down with relaxation toward a nonthermal state with a complicated electronic distribution as a function of momentum. We characterize the behavior by studying changes in the energy, photoemission response, and electronic distribution as functions of time. This relaxation may be observable qualitatively on short enough time scales that the electrons behave like an isolated system not in contact with additional degrees of freedom which would act as a thermal bath, especially when using strong driving fields and studying materials whose physics may manifest the effects of correlations.
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http://dx.doi.org/10.1103/PhysRevLett.111.077401 | DOI Listing |
J Phys Chem B
January 2025
Institute of Physics, Lodz University of Technology, ul. Wólczańska 217/221, 93-590 Łódź, Poland.
Photocycloreversion reactions of three diarylethene derivatives whose structures differ only in the placement of two sulfur atoms in the cyclopentene rings are investigated. Despite the minuscule differences between the molecules, both the yields and times of the photoreactions vary considerably. Using UV-vis and infrared femtosecond spectroscopy and quantum chemical dynamics simulations, we elucidate the relationships among the quantum yield, electronic and vibrational relaxation time, and structural properties of the dithienylethene photoswitches.
View Article and Find Full Text PDFBioengineering (Basel)
December 2024
Center of Biomedical Imaging, Department of Radiology, New York University Grossman School of Medicine, New York, NY 10016, USA.
Non-linear least squares (NLS) methods are commonly used for quantitative magnetic resonance imaging (MRI), especially for multi-exponential T1ρ mapping, which provides precise parameter estimation for different relaxation models in tissues, such as mono-exponential (ME), bi-exponential (BE), and stretched-exponential (SE) models. However, NLS may suffer from problems like sensitivity to initial guesses, slow convergence speed, and high computational cost. While deep learning (DL)-based T1ρ fitting methods offer faster alternatives, they often face challenges such as noise sensitivity and reliance on NLS-generated reference data for training.
View Article and Find Full Text PDFJ Phys Chem Lett
January 2025
State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai 200241, China.
Flavonoids, a group of natural pigments, have attracted notable attention for their intrinsic fluorescent bioactive properties and potential therapeutic implications. Recent studies have suggested that the photoexcitation of specific flavonoids can also lead to the formation of triplet states, thereby potentially enhancing their applications in photoactivated antioxidant mechanisms. However, the crucial mechanism details about triplet state formation are still poorly understood.
View Article and Find Full Text PDFJ Phys Chem Lett
January 2025
Molecular Spectroscopy Laboratory, RIKEN, 2-1 Hirosawa, Wako 351-0198, Japan.
Elucidation of the vibrational relaxation process of interfacial water is indispensable for understanding energy dissipation at the aqueous interface. In this study, the vibrational relaxation dynamics of the hydrogen-bonded OH (HB OH) stretch vibration was investigated at the air/isotopically diluted water (HOD-DO) interface by time-resolved heterodyne-detected vibrational sum frequency generation (TR-HD-VSFG) spectroscopy. We observed the temporal change of the excited-state band ( = 1 → 2 transition), which enables a reliable determination of the time of interfacial water.
View Article and Find Full Text PDFJ Phys Chem B
January 2025
School of Physics and Optoelectronic Engineering, Yangtze University, Jingzhou 434023, China.
Chromophores incorporated into rigid polymer matrices may exhibit novel photophysical properties distinct from those in liquid solutions. In this work, we explored the decay path of the second ππ* state (2ππ*) of riboflavin in poly(vinyl alcohol) (PVA) solutions and films with various acidities. Highly efficient internal conversion from 2ππ* to the lowest ππ* state (1ππ*) induced by slight in-plane motion is demonstrated in all PVA solutions and films, irrespective of environmental acidity and rigidification.
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