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 imaging, which provides detailed information on domain structures but typically lacks spectroscopic detail. In contrast, infrared-visible sum-frequency generation (SFG) spectroscopy reveals details of the atomic structure and bonding via vibrational resonances, but conventionally lacks spatial information. In this work, we combine the benefits of nonlinear optical imaging and SFG spectroscopy by employing SFG spectro-microscopy using an infrared free-electron laser. In particular, we demonstrate the feasibility of SFG spectro-microscopy for spectroscopy using in-plane anisotropic wurtzite-type aluminum nitride as a model system. We find the experimental spectra to agree well with our theoretical calculations, and we show the potential of our microscope to provide spatially resolved spectroscopic information in inhomogeneous systems such as ferroics and their domains in the near future.
Download full-text PDF |
Source |
|---|---|
| http://dx.doi.org/10.1063/5.0220619 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Local field effects of quadrupole contributions on sum frequency generation spectroscopy.
J Chem Phys
December 2024
Department of Chemistry, Graduate School of Science, Tohoku University, Sendai 980-8578, Japan.
In the theory of condensed-phase spectroscopy, local field effect is of general importance to account for intermolecular electrostatic interactions. The present paper extends the microscopic treatment of local field effects on the sum frequency generation (SFG) spectroscopy to incorporate quadrupole interactions, since their roles have been increasingly recognized in the SFG spectroscopy. The extended theory involves some corrections to the conventional formulas of the nonlinear susceptibilities in both the interface and bulk regions, including the χIQB term.
View Article and Find Full Text PDFDissecting the Molecular Structure of the Air/Ice Interface from Quantum Simulations of the Sum-Frequency Generation Spectrum.
J Am Chem Soc
January 2025
Department of Chemistry and Biochemistry, University of California San Diego, La Jolla, California 92093, United States.
Ice interfaces are pivotal in mediating key chemical and physical processes such as heterogeneous chemical reactions in the environment, ice nucleation, and cloud microphysics. At the ice surface, water molecules form a quasi-liquid layer (QLL) with properties distinct from those of the bulk. Despite numerous experimental and theoretical studies, a molecular-level understanding of the QLL has remained elusive.
View Article and Find Full Text PDFMolecular orientation of dielectric layers at indigo/dielectric interfaces impacts the ordering of indigo films in organic field-effect transistors.
J Chem Phys
January 2025
Graduate School of Engineering, Chiba University, 1-33, Yayoi-cho, Inage-ku, Chiba, Chiba 263-8522, Japan.
Organic multilayer systems, which are stacked layers of different organic materials, are used in various organic electronic devices such as organic light-emitting diodes (OLEDs) and organic field-effect transistors (OFETs). In particular, OFETs are promising as key components in flexible electronic devices. In this study, we investigated how the inclusion of an insulating tetratetracontane (TTC) interlayer in ambipolar indigo-based OFETs can be used to alter the crystallinity and electrical properties of the indigo charge transport layer.
View Article and Find Full Text PDFHydrogen bonding blues: Vibrational spectroscopy of the TIP3P water model.
J Chem Phys
January 2025
Department of Chemistry, Boston University, 590 Commonwealth Avenue, Boston, Massachusetts 02215, USA.
The computational spectroscopy of water has proven to be a powerful tool for probing the structure and dynamics of chemical systems and for providing atomistic insight into experimental vibrational spectroscopic results. However, such calculations have been limited for biochemical systems due to the lack of empirical vibrational frequency maps for the TIP3P water model, which is used in many popular biomolecular force fields. Here, we develop an empirical map for the TIP3P model and evaluate its efficacy for reproducing the experimental vibrational spectroscopy of water.
View Article and Find Full Text PDFSurface structure characterization of rubrene(001) single crystal with sum frequency generation spectroscopy and reflection high-energy electron diffraction.
J Chem Phys
January 2025
Department of Chemistry, University of Houston, Houston, Texas 77204, USA.
Rubrene is one of the leading organic semiconductors in scientific and industrial research, showing good conductivities and utilities in devices such as organic field-effect transistors. In these applications, the rubrene crystals often contact ionic liquids and other materials. Consequently, their surface properties and interfacial interactions influence the device's performance.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!