Related papers: Second-Harmonic Scattering as a Probe of Structura…
Imaging through dynamic scattering media, such as biological tissue, presents a fundamental challenge due to light scattering and the formation of speckle patterns. These patterns not only degrade image quality but also decorrelate rapidly,…
We introduce and demonstrate a new approach to measuring coherent electron wave packets using high-harmonic spectroscopy. By preparing a molecule in a coherent superposition of electronic states, we show that electronic coherence opens…
The nanoscale structure of molecular assemblies plays a major role in many ($\mu$)-biological mechanisms. Molecular crystals are one of the most simple of these assemblies and are widely used in a variety of applications from…
Simulating liquid water to an accuracy that matches its wealth of available experimental data requires both precise electronic structure methods and reliable sampling of nuclear (quantum) motion. This is challenging because applying the…
We model, simulate, and analyze the intramolecular modes of liquid H2O and D2O to elucidate how energy excitation, relaxation, and vibrational dephasing interplay through anharmonic mode-mode coupling. Our analysis employs two-dimensional…
We show that the momentum flexibility of inelastic x-ray scattering may be exploited to invert its loss function, alowing real time imaging of density disturbances in a medium. We show the disturbance arising from a point source in liquid…
To investigate the possibility of measuring the intermolecular and intramolecular anharmonic coupling of balk water, we calculate third-order two-dimensional (2D) infrared (IR) spectra and fifth-order 2D IR-IR-Raman-Raman spectra expressed…
Spontaneous vibrational Raman scattering is a ubiquitous form of light-matter interaction whose description necessitates quantization of the electromagnetic field. It is usually considered as an incoherent process because the scattered…
Electron scattering on liquid samples has been enabled recently by the development of ultrathin liquid sheet technologies. The data treatment of liquid-phase electron scattering has been mostly reliant on methodologies developed for gas…
Liquid water is reluctant to lose hydrogen-bond coordination. Here we reveal that it also demands contraction and reorientation of the second molecular shell to compensate for coordination defects. Such molecular principle will be shown to…
Ionic liquids are widely used as electrolytes in electrochemical devices. In this context, many experimental and theoretical approaches have been recently developed for characterizing their interface with electrodes. In this perspective…
Over times shorter than that required for relaxation of enthalpy, a liquid can exhibit striking heterogeneities. The picture of these heterogeneities is complex with transient patches of rigidity, irregular yet persistent, intersected by…
Second-order nonlinear optical processes do not manifest in the bulk of centrosymmetric materials, but may occur in the angstroms-thick layer at surfaces. At such length-scales, quantum mechanical effects come into play which could be…
The theory of light scattering for a system of linear molecules with anisotropic polarizabilities is considered. As a starting point for our theory, we express the result of a scattering experiment in VV and VH symmetry as dynamic…
Neutrons and x-rays are coherent probes, and their coherent properties are used in scattering experiments. Only coherent scattering probes can elucidate collective molecular motions. While phonons in crystals were studied for half a century…
We have experimentally measured the distribution of the second-harmonic intensity that is generated inside a highly-scattering slab of porous gallium phosphide. Two complementary techniques for determining the distribution are used. First,…
Second harmonic generation (SHG) is forbidden in centrosymmetric molecular materials. However, a signal is frequently observed from interfaces where the symmetry is broken. Whereas the effect can be phenomenologically accommodated, an ab…
An open question is whether the liquid and glassy phases of water are thermodynamically distinct or continuous. Here we address this question using molecular dynamics simulations in comparison with neutron scattering experiments to study…
Metal coordination is ubiquitous in Nature and central in many applications ranging from nanotechnology to catalysis and environmental chemistry. Complex formation results from the subtle interplay between different thermodynamic, kinetic,…
We develop and verify a phase-sensitive second harmonic generation spectroscopic scheme that allows for direct determination of the absolute surface charge density and surface potential of a water interface without need of prior interfacial…