Wang, Jizhou and Wang, Kai and Shen, Yujie and Han, Zehua and Li, Fu and He, Zhe and Wang, Da-wei and Sokolov, Alexei V. and Scully, Marlan O. (2021) Femtosecond Time-Resolved Infrared-Resonant Third-Order Sum-Frequency Spectroscopy. ACS Photonics, 8 (4). pp. 1137-1142. ISSN 2330-4022. doi:10.1021/acsphotonics.0c01940. https://resolver.caltech.edu/CaltechAUTHORS:20210217-103651180
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Abstract
We demonstrate a coherent vibrational spectroscopy based on molecular infrared (IR)-active resonance. We apply two femtosecond pulses (one in near-IR and the other in mid-IR) to generate the femtosecond time-resolved IR-resonant third-order sum-frequency signal. The mid-IR pulse is tuned to be resonant with molecular vibrations. This experimental configuration converts the IR light into a visible signal and exhibits high sensitivity to the vibrational mode of the molecule. The technique can be applied to acquire chemical information on various biological samples, including living tissues in their natural water-rich state. This approach can also be used to study the dynamics of IR-active vibrational modes, that is, measure the decoherence time.
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| Additional Information: | © 2021 The Authors. Published by American Chemical Society. Made available through a Creative Commons CC-BY-NC-ND License. Received: December 22, 2020; Published: February 12, 2021. We thank Prof. Volker Deckert for the useful discussion. We gratefully acknowledge the support from the Office of Naval Research (Award Nos. N00014-16-1-2578 and N00014-20-1-2184), the Robert A. Welch Foundation (Grant Nos. A-1261 and A-1547), National Science Foundation (Grant No. PHY-2013771), the Air Force Office of Scientific Research (Award No. FA9550-20-1-0366 DEF), the National Natural Science Foundation of China (Grant No. 11934011), the Major Scientific Research Project of Zhejiang Lab (Nos. 2019MB0AD01 and 20190057), and Fundamental Research Funds for the Central Universities of China. Z.H., F.L., and Z.H. were supported by the Herman F. Heep and Minnie Belle Heep Texas A&M University Endowed Fund held/administered by the Texas A&M Foundation. | ||||||||||||||||||||||||
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| Subject Keywords: | midinfrared spectroscopy, third-order nonlinearity, sum-frequency generation, molecular dynamics, decoherence time | ||||||||||||||||||||||||
| Issue or Number: | 4 | ||||||||||||||||||||||||
| DOI: | 10.1021/acsphotonics.0c01940 | ||||||||||||||||||||||||
| Record Number: | CaltechAUTHORS:20210217-103651180 | ||||||||||||||||||||||||
| Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20210217-103651180 | ||||||||||||||||||||||||
| Official Citation: | Femtosecond Time-Resolved Infrared-Resonant Third-Order Sum-Frequency Spectroscopy. Jizhou Wang, Kai Wang, Yujie Shen, Zehua Han, Fu Li, Zhe He, Da-wei Wang, Alexei V. Sokolov, and Marlan O. Scully. ACS Photonics 2021 8 (4), 1137-1142; DOI: 10.1021/acsphotonics.0c01940 | ||||||||||||||||||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||||||||||||
| ID Code: | 108088 | ||||||||||||||||||||||||
| Collection: | CaltechAUTHORS | ||||||||||||||||||||||||
| Deposited By: | Tony Diaz | ||||||||||||||||||||||||
| Deposited On: | 18 Feb 2021 19:16 | ||||||||||||||||||||||||
| Last Modified: | 23 Apr 2021 17:56 |
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