Kenneth B. Eisenthal
Summary
In our laboratory we use nonlinear laser spectroscopy to selectively investigate equilibrium and dynamic processes at interfaces, which include the detection and orientation of adsorbed molecules, chemical equilibria, binding of drugs to DNA, and using a method developed in our laboratory we can measure the electrostatic potential of any charged surface that is accessible to light. It is a method that we have used to measure the electrostatic potential of a chemically excited neuron, the pH of an interface, and the binding of the HIV-TAT peptide to membranes without the use of a probe label. We have recently developed a second harmonic interference method that has the potential of detecting changes in DNA structure in response to a molecule binding to it, and antibiotic assisted molecular ion transport across a membrane in real time. With the high time resolution afforded by our use of a femtosecond laser system has enabled us to study ultrafast interfacial phenomena, which include excited state electron transfer at an organic liquid/water interface, intermolecular electronic energy transfer at the air/water interface, excited state solvation, and in plane and out of plane rotational motions of interfacial molecules.
Our challenge is to advance the development and appliction of nonlinear optical methods to probe the physical, chemical, and biological properties of interfaces.
Boamah, M. D., Ohno, P. E., Geiger, F. M., & Eisenthal, K. B. (2018). Relative permittivity in the electrical double layer from nonlinear optics. Journal of Chemical Physics, 148(22) doi:10.1063/1.5011977
Ma, J., Mandal, S., Bronsther, C., Gao, Z., & Eisenthal, K. B. (2017). Second harmonic study of acid-base equilibrium at gold nanoparticle/aqueous interface. Chemical Physics Letters, 683, 166-171. doi:10.1016/j.cplett.2016.12.053
Doughty, B., Rao, Y., Kazer, S. W., Kwok, S. J. J., Turro, N. J., & Eisenthal, K. B. (2013). Probing the relative orientation of molecules bound to DNA through controlled interference using second-harmonic generation. Proceedings of the National Academy of Sciences of the United States of America, 110(15), 5756-5758. doi:10.1073/pnas.1302554110
Doughty, B., Kazer, S. W., & Eisenthal, K. B. (2011). Binding and cleavage of DNA with the restriction enzyme EcoR1 using time-resolved second harmonic generation. Proceedings of the National Academy of Sciences of the United States of America, 108(50), 19979-19984. doi:10.1073/pnas.1115498108
Liu, J., Subir, M., Nguyen, K., & Eisenthal, K. B. (2008). Second harmonie studies of ions crossing liposome membranes in real time. Journal of Physical Chemistry B, 112(48), 15263-15266. doi:10.1021/jp806690z
Jiang, J., Eisenthal, K. B., & Yuste, R. (2007). Second harmonic generation in neurons: Electro-optic mechanism of membrane potential sensitivity. Biophysical Journal, 93(5), L26-L28. doi:10.1529/biophysj.107.111021
McArthur, E. A., & Eisenthal, K. B. (2006). Ultrafast excited-state electron transfer at an organic liquid/aqueous interface. Journal of the American Chemical Society, 128(4), 1068-1069. doi:10.1021/ja056518q
Rao, Y., Comstock, M., & Eisenthal, K. B. (2006). Absolute orientation of molecules at interfaces. Journal of Physical Chemistry B, 110(4), 1727-1732. doi:10.1021/jp055340r
Eisenthal, K. B. (2006). Second harmonic spectroscopy of aqueous nano- and microparticle interfaces. Chemical Reviews, 106(4), 1462-1477. doi:10.1021/cr0403685
Fitts, J. P., MacHesky, M. L., Wesolowski, D. J., Shang, X., Kubicki, J. D., Flynn, G. W., Eisenthal, K. B. (2005). Second-harmonic generation and theoretical studies of protonation at the water/α-TiO2(1 1 0) interface. Chemical Physics Letters, 411(4-6), 399-403. doi:10.1016/j.cplett.2005.03.152
Fitts, J. P., Shang, X., Flynn, G. W., Heinz, T. F., & Eisenthal, K. B. (2005). Electrostatic surface charge at aqueous/α-al 2O 3 single-crystal interfaces as probed by optical second-harmonic generation. Journal of Physical Chemistry B, 109(16), 7981-7986. doi:10.1021/jp040297d
Liu, J., Shang, X., Pompano, R., & Eisenthal, K. B. (2005). Antibiotic assisted molecular ion transport across a membrane in real time. Faraday Discussions, 129, 291-299. doi:10.1039/b405410e
Benderskii, A. V., & Eisenthal, K. B. (2002). Dynamical time scales of aqueous solvation at negatively charged lipid/water interfaces. Journal of Physical Chemistry A, 106(33), 7482-7490. doi:10.1021/jp0120155
Liu, Y., Yan, E. C. Y., Zhao, X., & Eisenthal, K. B. (2001). Surface potential of charged liposomes determined by second harmonic generation. Langmuir, 17(7), 2063-2066. doi:10.1021/la0011634
Shang, X., Liu, Y., Yan, E., & Eisenthal, K. B. (2001). Effects of counterions on molecular transport across liposome bilayer: Probed by second harmonic generation. Journal of Physical Chemistry B, 105(51), 12816-12822. doi:10.1021/jp0120918
Benderskii, A. V., & Eisenthal, K. B. (2000). Effect of organic surfactant on femtosecond solvation dynamics at the air-water interface. Journal of Physical Chemistry B, 104(49), 11723-11728.
Yan, E. C. Y., & Eisenthal, K. B. (2000). Effect of cholesterol on molecular transport of organic cations across liposome bilayers probed by second harmonic generation. Biophysical Journal, 79(2), 898-903. doi:10.1016/S0006-3495(00)76345-4
Wang, H., Borguet, E., & Eisenthal, K. B. (1998). Generalized interface polarity scale based on second harmonic spectroscopy. Journal of Physical Chemistry B, 102(25), 4927-4932.
Yan, E. C. Y., Liu, Y., & Eisenthal, K. B. (1998). New method for determination of surface potential of microscopic particles by second harmonic generation. Journal of Physical Chemistry B, 102(33), 6331-6336.
Zhang, D., Gutow, J., & Eisenthal, K. B. (1994). Vibrational spectra, orientations, and phase transitions in long-chain amphiphiles at the air/water interface: Probing the head and tail groups by sum frequency generation. Journal of Physical Chemistry, 98(51), 13729-13734. doi:10.1021/j100102a045