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High-Resolution Sum-Frequency Generation Vibrational Spectroscopy
Capability Development Project WBS

EMSL Project ID


The objective of this WBS element is to further develop experimental and user service capability to perform surface nonlinear spectroscopy and dynamics measurements with both high spectral resolution (~ 0.6cm-1) and ultrafast time resolution (~35 fs). The first high-resolution broadband sum-frequency generation vibrational spectroscopy/dynamics (HR-BB-SFG-VS) system has been built with the support of EMSL capital project, and the unique spectral resolving power of HR-BB-SFG-VS has been initially demonstrated. In order to further demonstrate its application to experiments of interest, two systematic studies need to be carried out: a). explore the conditions and sample preparation to make HR-BB-SFG-VS measurement on specific surfaces and interfaces; b). based on these data explore procedures and processes to analyze and interpret the high-resolution SFG data. This data analysis is extremely important, since such high-resolution and high signal-to noise SFG vibrational spectra have ever been obtained. A systematic procedure to process and analyze such data needs to be developed in establishing new model systems for the future studies on this new ground. Moreover, in order to understand these high resolution SFG spectra, comparison to the infrared (IR) and Raman spectra with similar spectral resolution of the same molecule or material in solution or solid phase is also needed for these model systems. However, such IR and Raman spectra are either scarce in the literature or database, or their quality and resolution is insufficient. This situation can be solved since we have discovered that using the same laser system that enables HR-BB-SFG-VS measurements can be used for high-resolution broadband stimulated Raman and IR absorption measurement for the same molecules or materials in solution or solid phase. These require additional effort in the capability development in order to make the unique HR-BB-SFG-VS capability useful for users.

Project Details

Start Date
End Date


Principal Investigator

Hongfei Wang
Fudan University

Team Members

Yu Gong
College of Charleston

Hui Shi
Pacific Northwest National Laboratory

Li Fu
Environmental Molecular Sciences Laboratory

Patrick El-Khoury
Pacific Northwest National Laboratory

Libing Zhang
Washington State University Tri-Cities

Zhehao Wei
Pacific Northwest National Laboratory

Bin Yang
Washington State University Tri-Cities

Related Publications

Feng RR, Y Guo, and H Wang. 2014. "Reorientation of the ‘free OH’ group In the top-most layer of air/water interface of sodium fluoride aqueous solution probed with sum-frequency generation vibrational spectroscopy." Journal of Chemical Physics 141(18):18C507-1 to 18C507-10. doi:10.1063/1.4895561
Fu L, Y Zhang, Z Wei, and H Wang. 2014. "Intrinsic Chirality and Prochirality at Air/R-(+)- and S-(-)-Limonene Interfaces: Spectral Signatures with Interference Chiral Sum-Frequency Generation Vibrational Spectroscopy." Chirality 26:149-160. doi:10.1002/chir.22337
Mark R Watry, Teresa L Tarbuck, Stephen Wilson, Randi Yeager, and Joseph Radzialowski. 2014. "VSFG spectra of surfactants with amino acid head groups and lipids at aqueous interfaces." 246th National American Chemical Society Meeting, Indianapolis, IN, September 2013.
Velarde Ruiz Esparza LA, and H Wang. 2013. "Capturing inhomogeneous broadening of the -CN stretch vibration in a Langmuir monolayer with high-resolution spectra and ultrafast vibrational dynamics in sum-frequecy generation vibrational spectroscopy (SFG-VS)." Journal of Chemical Physics 139(8):084204-1 to 084204-14.
Velarde Ruiz Esparza LA, and H Wang. 2013. "Unified treatment and measurement of the spectral resolution and temporal effects in frequency-resolved sum-frequency generation vibrational spectroscopy (SFG-VS)." Physical Chemistry Chemical Physics. PCCP 15(46):19970-19984. doi:10.1039/C3CP52577E
Velarde Ruiz Esparza LA, and H Wang. 2013. "Unique determination of the -CN group tilt angle in Langmuir monolayers using sum-frequency polarization null angle and phase." Chemical Physics Letters 585:42-48.
Zhang L, Y Pu, JR Cort, AJ Ragauskas, and B Yang. 2016. "Revealing the Molecular Structural Transformation of Hardwood and Softwood in Dilute Acid Flowthrough Pretreatment." ACS Sustainable Chemistry & Engineering 4(2):6618-6628. doi:10.1021/acssuschemeng.6b01491
Zhang L, Z Lu, LA Velarde Ruiz Esparza, L Fu, Y Pu, SY Ding, AJ Ragauskas, H Wang, and B Yang. 2015. "Vibrational Spectral Signatures of Crystalline Cellulose Using High Resolution Broadband Sum Frequency Generation Vibrational Spectroscopy (HR-BB-SFG-VS)." Cellulose. doi:10.1007/s10570-015-0588-0