Probing liquid/liquid interfaces at and away from equilibrium using vibrational sum frequency generation

Benjamin Doughty; Uvinduni I. Premadasa; Lu Lin; Ying Zhong Ma; Robert L. Sacci; Vera Bocharova; Nikki A. Thiele

doi:10.1117/12.2677555

Probing liquid/liquid interfaces at and away from equilibrium using vibrational sum frequency generation

Benjamin Doughty, Uvinduni I. Premadasa, Lu Lin, Ying Zhong Ma, Robert L. Sacci, Vera Bocharova, Nikki A. Thiele

Oak Ridge National Laboratory

Research output: Chapter in Book/Report/Conference proceeding › Conference contribution › peer-review

Abstract

The self-assembly and transport of species at oil/aqueous interfaces represent key mechanistic steps in processes spanning from liquid extraction to soft-matter neuromorphic electrical devices. While technologically and fundamentally important, there is a notable lack of chemical understanding regarding these buried interfaces due to challenges in differentiating species located at the surface from the nearby bulk phases. In this work, we will describe some of the challenges in probing chemistry at these liquid/liquid interfaces and detail the approaches we have developed using vibrational sum frequency generation to enable studies of these complex interfaces at and away from equilibrium. From these spectroscopic developments, new insight into solvation, ion pairing, aggregation, complexation, and transport will be discussed in the context of solvent extraction chemistry. Notably, we show how the presence of both oil and aqueous phases provides an environment to drive fundamentally different phenomena from what is observed at model air/aqueous interfaces. This difference arises from key differences in solvation and bulk populations that feedback onto the surface to drive emergent and often functional molecular assemblies.

Original language	English
Title of host publication	Ultrafast Nonlinear Imaging and Spectroscopy XI
Editors	Zhiwen Liu, Demetri Psaltis, Kebin Shi
Publisher	SPIE
ISBN (Electronic)	9781510665767
DOIs	https://doi.org/10.1117/12.2677555
State	Published - 2023
Event	Ultrafast Nonlinear Imaging and Spectroscopy XI 2023 - San Diego, United States Duration: Aug 21 2023 → Aug 22 2023

Publication series

Name	Proceedings of SPIE - The International Society for Optical Engineering
Volume	12681
ISSN (Print)	0277-786X
ISSN (Electronic)	1996-756X

Conference

Conference	Ultrafast Nonlinear Imaging and Spectroscopy XI 2023
Country/Territory	United States
City	San Diego
Period	08/21/23 → 08/22/23

Bibliographical note

Publisher Copyright:
© 2023 SPIE. All rights reserved.

Funding

U.I.P., L.L., Y.-Z.M., N.A.T., and B.D. were supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. V.B. and R.L.S. thank the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science & Engineering Division for partial financial support.

Funders	Funder number
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Division of Materials Sciences and Engineering
Chemical Sciences, Geosciences, and Biosciences Division

Keywords

chemical separations
nonequilibrium
nonlinear optics
surface dynamics
surface specific

Access to Document

10.1117/12.2677555

Cite this

Doughty, B., Premadasa, U. I., Lin, L., Ma, Y. Z., Sacci, R. L., Bocharova, V., & Thiele, N. A. (2023). Probing liquid/liquid interfaces at and away from equilibrium using vibrational sum frequency generation. In Z. Liu, D. Psaltis, & K. Shi (Eds.), Ultrafast Nonlinear Imaging and Spectroscopy XI Article 126810D (Proceedings of SPIE - The International Society for Optical Engineering; Vol. 12681). SPIE. https://doi.org/10.1117/12.2677555

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abstract = "The self-assembly and transport of species at oil/aqueous interfaces represent key mechanistic steps in processes spanning from liquid extraction to soft-matter neuromorphic electrical devices. While technologically and fundamentally important, there is a notable lack of chemical understanding regarding these buried interfaces due to challenges in differentiating species located at the surface from the nearby bulk phases. In this work, we will describe some of the challenges in probing chemistry at these liquid/liquid interfaces and detail the approaches we have developed using vibrational sum frequency generation to enable studies of these complex interfaces at and away from equilibrium. From these spectroscopic developments, new insight into solvation, ion pairing, aggregation, complexation, and transport will be discussed in the context of solvent extraction chemistry. Notably, we show how the presence of both oil and aqueous phases provides an environment to drive fundamentally different phenomena from what is observed at model air/aqueous interfaces. This difference arises from key differences in solvation and bulk populations that feedback onto the surface to drive emergent and often functional molecular assemblies.",

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Doughty, B , Premadasa, UI, Lin, L, Ma, YZ , Sacci, RL , Bocharova, V & Thiele, NA 2023, Probing liquid/liquid interfaces at and away from equilibrium using vibrational sum frequency generation. in Z Liu, D Psaltis & K Shi (eds), Ultrafast Nonlinear Imaging and Spectroscopy XI., 126810D, Proceedings of SPIE - The International Society for Optical Engineering, vol. 12681, SPIE, Ultrafast Nonlinear Imaging and Spectroscopy XI 2023, San Diego, United States, 08/21/23. https://doi.org/10.1117/12.2677555

Probing liquid/liquid interfaces at and away from equilibrium using vibrational sum frequency generation. / Doughty, Benjamin ; Premadasa, Uvinduni I.; Lin, Lu et al.
Ultrafast Nonlinear Imaging and Spectroscopy XI. ed. / Zhiwen Liu; Demetri Psaltis; Kebin Shi. SPIE, 2023. 126810D (Proceedings of SPIE - The International Society for Optical Engineering; Vol. 12681).

Research output: Chapter in Book/Report/Conference proceeding › Conference contribution › peer-review

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AU - Bocharova, Vera

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N2 - The self-assembly and transport of species at oil/aqueous interfaces represent key mechanistic steps in processes spanning from liquid extraction to soft-matter neuromorphic electrical devices. While technologically and fundamentally important, there is a notable lack of chemical understanding regarding these buried interfaces due to challenges in differentiating species located at the surface from the nearby bulk phases. In this work, we will describe some of the challenges in probing chemistry at these liquid/liquid interfaces and detail the approaches we have developed using vibrational sum frequency generation to enable studies of these complex interfaces at and away from equilibrium. From these spectroscopic developments, new insight into solvation, ion pairing, aggregation, complexation, and transport will be discussed in the context of solvent extraction chemistry. Notably, we show how the presence of both oil and aqueous phases provides an environment to drive fundamentally different phenomena from what is observed at model air/aqueous interfaces. This difference arises from key differences in solvation and bulk populations that feedback onto the surface to drive emergent and often functional molecular assemblies.

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Doughty B , Premadasa UI, Lin L, Ma YZ , Sacci RL , Bocharova V et al. Probing liquid/liquid interfaces at and away from equilibrium using vibrational sum frequency generation. In Liu Z, Psaltis D, Shi K, editors, Ultrafast Nonlinear Imaging and Spectroscopy XI. SPIE. 2023. 126810D. (Proceedings of SPIE - The International Society for Optical Engineering). doi: 10.1117/12.2677555

Probing liquid/liquid interfaces at and away from equilibrium using vibrational sum frequency generation

Abstract

Publication series

Conference

Bibliographical note

Funding

Keywords

Access to Document

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