Vibrational excitations of low frequency collective modes are essential for functionally important conformational transitions in proteins. Here we report the first direct measurement on the lifetime of vibrational excitations of the collective modes at 87 microm (115 cm(-1)) in bacteriorhodopsin, a transmembrane protein. The data show that these modes have extremely long lifetime of vibrational excitations, over 500 ps, accommodating 1500 vibrations. We suggest that there is a connection between this relatively slow anharmonic relaxation rate of approximately 10(9) sec(-1) and the similar observed rate of conformational transitions in proteins, which require multilevel vibrational excitations.
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http://dx.doi.org/10.1103/PhysRevLett.88.018102 | DOI Listing |
Nanophotonics
January 2025
Institute of Physics, Swiss Federal Institute of Technology Lausanne (EPFL), CH-1015 Lausanne, Switzerland.
Sum-frequency generation (SFG) enables the coherent upconversion of electromagnetic signals and plays a significant role in mid-infrared vibrational spectroscopy for molecular analysis. Recent research indicates that plasmonic nanocavities, which confine light to extremely small volumes, can facilitate the detection of vibrational SFG signals from individual molecules by leveraging surface-enhanced Raman scattering combined with mid-infrared laser excitation. In this article, we compute the degree of second order coherence ( (0)) of the upconverted mid-infrared field under realistic parameters and accounting for the anharmonic potential that characterizes vibrational modes of individual molecules.
View Article and Find Full Text PDFFront Neurosci
January 2025
School of Electronic Information and Communications, Huazhong University of Science and Technology, Wuhan City, China.
Introduction: Transcranial magnetic stimulation (TMS) is widely used for the noninvasive activation of neurons in the human brain. It utilizes a pulsed magnetic field to induce electric pulses that act on the central nervous system, altering the membrane potential of nerve cells in the cerebral cortex to treat certain mental diseases. However, the effectiveness of TMS can be compromised by significant heat generation and the clicking noise produced by the pulse in the TMS coil.
View Article and Find Full Text PDFJ Phys Chem C Nanomater Interfaces
January 2025
Center for Quantum Nanoscience, Institute for Basic Science, Seoul 03760, South Korea.
Precise description of the interaction between molecular oxygen and metal surfaces is one of the most challenging topics in quantum chemistry. In this work, we use low-temperature scanning tunneling microscopy (STM) to identify and characterize an adsorption state of molecular oxygen that coordinates to three Ag atoms (μ) on Ag(100). Surprisingly, μ-O cannot be identified as a stable configuration with generalized gradient approximation (GGA)-level density functional theory (DFT) calculations.
View Article and Find Full Text PDFJ Phys Chem C Nanomater Interfaces
January 2025
School of Chemistry, University of East Anglia, Norwich NR4 7TJ, U.K.
Understanding the role of structural and environmental dynamics in the excited state properties of strongly coupled chromophores is of paramount importance in molecular photonics. Ultrafast, coherent, and multidimensional spectroscopies have been utilized to investigate such dynamics in the simplest model system, the molecular dimer. Here, we present a half-broadband two-dimensional electronic spectroscopy (HB2DES) study of the previously reported ultrafast symmetry-breaking charge separation (SB-CS) in the subphthalocyanine oxo-bridged homodimer μ-OSubPc.
View Article and Find Full Text PDFSoft Matter
January 2025
Physics Department, Wesleyan University, Middletown, CT 06459, USA.
We examine the collective motion in computational models of a two-dimensional dusty plasma crystal and a charged colloidal suspension as they approach their respective melting transitions. To unambiguously identify rearrangement events in the crystal, we map the trajectory of configurations from an equilibrium molecular dynamics simulation to the corresponding sequence of configurations of local potential energy minima ("inherent structures"). This inherent structure (IS) trajectory eliminates the ambiguity that arises from localized vibrational motion.
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