相关论文: Anharmonic Coupling between Intermolecular Motions…
Microscopic understanding of low-frequency molecular motions in liquids has been a longstanding goal in soft-matter science. So far, such low-frequency motions have mostly been accessed indirectly by off-resonant optical pulses. A more…
We have observed optical birefringence in liquids induced by single-cycle THz pulses with field strengths exceeding 100 kV/cm. The induced change in polarization is proportional to the square of the THz electric field. The time-dependent…
Water is vital for life, and without it biomolecules and cells cannot maintain their structures and functions. The remarkable properties of water originate from its ability to form hydrogen-bonding networks and dynamics, which the…
Energy dissipation in water is very fast and more efficient than in many other liquids. This behavior is commonly attributed to the intermolecular interactions associated with hydrogen bonding. Here, we investigate the dynamic energy flow…
Terahertz Kerr-effect (TKE) spectroscopy provides a time-domain optical probe of the intermolecular structural dynamics of liquids, but the measured birefringence can only be interpreted microscopically if transient molecular structure,…
The liquid and supercooled states of water show a series of anomalies whose nature is debated. A key role is attributed to the formation of structural aggregates induced by critical phenomena occurring deep in the supercooled region; the…
We report the first coherent excitation of intramolecular vibrational modes via the nonlinear interaction of a TeraHertz (THz) light field with molecular liquids. A terahertz-terahertz-Raman pulse sequence prepares the coherences with a…
Two-dimensional spectroscopic techniques combining terahertz (THz), infrared (IR), and visible pulses offer a wealth of information about coupling among vibrational modes in molecular liquids, thus providing a promising probe of their local…
Because of their central importance in chemistry and biology, water molecules have been the subject of decades of intense spectroscopic investigations. Rotational spectroscopy of water vapor has yielded detailed information about the…
Dynamic structuring of water is a key player in a large class of processes underlying biochemical and technological developments today, the latter often involving electric fields. However, the anisotropic coupling between the water…
The heating effect of terahertz pulse with various frequencies and intensities on the heavy water solution is investigated using the molecular dynamics simulation. Resonant absorptions are found for both heavy water and light water, but at…
Tracking the excitation of water molecules in the homogeneous liquid is challenging due to the ultrafast dissipation of rotational excitation energy through the hydrogen-bonded network. Here we demonstrate strong transient anisotropy of…
Liquid water at ambient temperature displays ultrafast molecular motions and concomitant fluctuations of very strong electric fields originating from the dipolar H2O molecules. We show that such random intermolecular fields induce tunnel…
A computational study of liquid water when the system is coupled with a (model) Fabry-Perot cavity is reported. At this end, the Cavity Born-Oppenheimer Molecular Dynamics approach proposed recently (Li et al., Proc. Nat. Acad. Sci. USA,…
Optically heterodyned detected terahertz Kerr effect of gases of polar molecules is reported. Strikingly, the birefringence signal from fluoroform is found to have opposite polarity compared to water and acetonitrile. This behavior is a…
Molecular dynamics simulations of supercritical water reveal distinctly different distance-dependent modulations of dipolar response and correlations in particle motion compared to ambient conditions. The strongly perturbed H-bond network…
Several years ago, it was shown that strong coupling between an electronic transition in organic molecules and a resonant photonic structure can modify the electronic landscape of the molecules and affect their chemical behavior. Since…
The terahertz (THz) response of solvated electrons in liquid water is studied in nonlinear ultrafast pump-probe experiments. Free electrons with concentrations from c_e = 4 to 140 \times 10-6 moles/liter are generated by high-field THz or…
Liquid water is one of the most studied substances, yet many of its properties are difficult to rationalize. The uniqueness of water is rooted in the dynamic network of hydrogen-bonded molecules with relaxation time constants of about one…
We have employed molecular dynamics simulations based on the TIP4P/2005 water model to investigate the local structural, dynamical, and dielectric properties of the two recently reported body-centered-cubic and face-centered-cubic plastic…