A phase-resolved heterodyne shearing interferometer concept is under development for high-rate, whole field observations of transient surface motion. The sensor utilizes frequency and polarization multiplexing with two temporal carrier frequencies to separate each segment of a shearing Mach-Zehnder interferometer. Post-processing routines have been developed to recombine the segments by extracting the scattered object phase from Doppler shifted intermediate carrier frequencies. The processing routines provide quantitative relative phase changes and information required to generate phase resolved shearographic fringe patterns without temporal or spatial phase shifting. Separation of each segment allows for adjustment of shearing distance and direction as well as simultaneous whole field Doppler velocity (LDV) measurements. This paper presents background theory and numerical model results leading to a sensor concept.
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http://dx.doi.org/10.1364/OE.25.006169 | DOI Listing |
J Chem Phys
February 2024
Department of Chemistry, Yale University, New Haven, Connecticut 06520, USA.
Chirality-selective vibrational sum frequency generation (chiral SFG) spectroscopy has emerged as a powerful technique for the study of biomolecular hydration water due to its sensitivity to the induced chirality of the first hydration shell. Thus far, water O-H vibrational bands in phase-resolved heterodyne chiral SFG spectra have been fit using one Lorentzian function per vibrational band, and the resulting fit has been used to infer the underlying frequency distribution. Here, we show that this approach may not correctly reveal the structure and dynamics of hydration water.
View Article and Find Full Text PDFJ Phys Chem A
October 2023
Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States.
We have employed amplitude- and phase-resolved second-harmonic generation spectroscopy to investigate ion-specific effects of monovalent cations at the fused silica:water interface maintained under acidic, neutral, and alkaline conditions. We find a negligible dependence of the total potential (as negative as -400 mV at pH 14), the second-order nonlinear susceptibility (as large as 1.5 × 10 m V at pH 14), the number of Stern layer water molecules (1 × 10 cm at pH 5.
View Article and Find Full Text PDFJ Chem Phys
March 2022
Molecular Spectroscopy Department, Max Planck Institute for Polymer Research, Ackermannweg 10, Mainz 55128, Germany.
Many essential processes occur at soft interfaces, from chemical reactions on aqueous aerosols in the atmosphere to biochemical recognition and binding at the surface of cell membranes. The spatial arrangement of molecules specifically at these interfaces is crucial for many of such processes. The accurate determination of the interfacial molecular orientation has been challenging due to the low number of molecules at interfaces and the ambiguity of their orientational distribution.
View Article and Find Full Text PDFNat Commun
February 2022
Department of Physics and JILA, University of Colorado, Boulder, CO, 80309, USA.
Ultrafast infrared nano-imaging has demonstrated access to ultrafast carrier dynamics on the nanoscale in semiconductor, correlated-electron, or polaritonic materials. However, mostly limited to short-lived transient states, the contrast obtained has remained insufficient to probe important long-lived excitations, which arise from many-body interactions induced by strong perturbation among carriers, lattice phonons, or molecular vibrations. Here, we demonstrate ultrafast infrared nano-imaging based on excitation modulation and sideband detection to characterize electron and vibration dynamics with nano- to micro-second lifetimes.
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