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Multimodal Nonlinear Hyperspectral Chemical Imaging Using Line-Scanning Vibrational Sum-Frequency Generation Microscopy

Vibrational sum-frequency generation (VSFG), a second-order nonlinear optical signal, has traditionally been used to study molecules at interfaces as a ...

UC San Diego

Physical properties are commonly represented by tensors, such as optical susceptibilities. The conventional approach of deriving non-vanishing tensor elements of symmetric systems relies on the intuitive consideration of positive/negative sign flipping after symmetry operations, which could be tedious and prone to miscalculation. Here, we present a matrix-based approach that gives a physical picture centered on Neumann's principle. The principle states that symmetries in geometric systems are adopted by their physical properties. We mathematically apply the principle to the tensor expressions and show a procedure with clear physical intuition to derive non-vanishing tensor elements based on eigensystems. The validity of the approach is demonstrated by examples of commonly known second and third-order nonlinear susceptibilities of chiral/achiral surfaces, together with complicated scenarios involving symmetries such as D and O symmetries. We then further applied this method to higher-rank tensors that are useful for 2D and high-order spectroscopy. We also extended our approach to derive nonlinear tensor elements with magnetization, which is critical for measuring spin polarization on surfaces for quantum information technologies. A Mathematica code based on this generalized approach is included that can be applied to any symmetry and higher order nonlinear processes.

Zishan Wu

Department of Chemistry and Biochemistry

UC San Diego

Multimodal Nonlinear Hyperspectral Chemical Imaging Using Line-Scanning Vibrational Sum-Frequency Generation Microscopy

Zishan Wu

.css-o250i3{font-size:18px;font-family:Open Sans,sans-serif;line-height:21.6px;}Department of Chemistry and Biochemistry

UC San Diego

Multimodal Nonlinear Hyperspectral Chemical Imaging Using Line-Scanning Vibrational Sum-Frequency Generation Microscopy

Department of Chemistry and Biochemistry