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Vibrational sum frequency generation (SFG) spectroscopy is a powerful technique for investigating molecular structures, orientations, and dynamics at surfaces. However, its spatial resolution is fundamentally restricted to the micrometer…
Our current understanding of the structure and dynamics of aqueous interfaces at the molecular level has grown substantially in the last few decades due to the continuous development of surface-specific spectroscopies, such as vibrational…
Moving the detection wavelength in vibrational sum-frequency generation (VSFG) spectroscopy to the near-infrared (> 700 nm) can potentially enable the study of molecular interfaces absorbing in the visible and give access to buried…
Vibrational sum- and difference-frequency generation (SFG and DFG) spectroscopy probes the nonlinear response of interfaces at mid-infrared (MIR) wavelengths while detecting upconverted signals in the visible. Recent work has moved from…
Experimental insight into the elementary processes underlying charge transfer across interfaces has blossomed with the wide-spread availability of ultra-high vacuum set-ups that allow the preparation and characterization of solid surfaces…
Sum-frequency generation (SFG) is a powerful second-order nonlinear spectroscopic technique that provides detailed insights into molecular structures and absolute orientations at surfaces and interfaces. However, conventional SFG based on…
Understanding the extent of contact between objects is crucial for surface-driven phenomena in the natural world. While interactions are known to occur at subnanometer-length scales, the techniques needed to measure such small-length scales…
Understanding the molecular-level structure and dynamics of ice surfaces is crucial for deciphering several chemical, physical, and atmospheric processes. Vibrational sum-frequency generation (SFG) spectroscopy is the most prominent tool…
Interface-specific hydrogen- (H-)bonding network of water next to a substrate (including air) directly controls the energy transfer and chemical reaction pathway at many charged aqueous interfaces. Yet, experimental characterization of such…
Vibrational sum frequency generation (SFG) is a nonlinear spectroscopic technique widely used to study the molecular structure and dynamics of surface systems. However, the spatial resolution achieved by far-field observations is…
Nonlinear-optical microscopy and spectroscopy provide detailed spatial and spectroscopic contrast, specifically sensitive to structural symmetry and order. Ferroics, in particular, have been widely studied using second harmonic generation…
Sum-frequency generation (SFG) spectroscopy provides a versatile method for the investigation of non-centrosymmetric media and interfaces. Here, using tunable picosecond infrared (IR) pulses from a free-electron laser, the nonlinear optical…
Tailoring spectral properties of photon pairs is of great importance for optical quantum information and measurement applications. High-resolution spectral measurement is a key technique for engineering spectral properties of photons,…
We introduce sum-frequency generation (SFG) as an effective physical two-photon detector for high power two-mode squeezed coherent states with arbitrary frequency separation, as produced by parametric oscillators well above the threshold.…
We present a 100 kHz broadband vibrational sum-frequency generation (VSFG) spectrometer operating in the 5.5-10.5 $\mu$m (950-1750 cm$^{-1}$) wavelength range. The mid-infrared beam of the system is obtained from a collinear, type-I…
This paper proposes a novel feature called spectrum congruency for describing edges in images. The spectrum congruency is a generalization of the phase congruency, which depicts how much each Fourier components of the image are congruent in…
Here we report a detailed study on spectroscopy, structure and dynamics of water molecules at air/water interface, investigated with Sum Frequency Generation Vibrational Spectroscopy (SFG-VS). Quantitative polarization and experimental…
Sum-frequency generation (SFG) allows for coherent upconversion of an electromagnetic signal and has applications in mid-infrared vibrational spectroscopy of molecules. Recent experimental and theoretical studies have shown that plasmonic…
A complete empirical approach from known Raman and IR spectra is used to make corrections to the bond additivity model for quantitative interpretation of Sum Frequency generation Vibrational Spectra (SFG-VS) from molecular interfaces. This…
Second-order nonlinear optical interactions such as sum- and difference-frequency generation are widely used for bioimaging and as selective probes of interfacial environments. However, inefficient nonlinear optical conversion often leads…