A theoretical description of the vibrational sum frequency generation spectroscopy of interfaces [electronic resource] / Perry, Angela S. [Tampa, Fla.] : University of South Florida, 2005. eng ABSTRACT: Our work investigates theoretical approximations to the interface specific sum frequency generation (SFG) spectra at aqueous interfaces constructed using time correlation function (TCF) and instantaneous normal mode (INM) methods. Both approaches lead to signals in excellent agreement with experimental measurements. This work demonstrates how TCF and INM methods can be used in a complementary fashion to describe interfacial vibrational spectroscopy. Our approach is to compare TCF spectra with experiment to establish that our molecular dynamics (MD) methods can reliably describe the system of interest. We then employ INM methods to analyze the molecular and dynamical basis for the observed spectroscopy. We have been able to elucidate, on a molecularly detailed basis, a number of interfacial line shapes, most notably the origin of the complex O-H stretching SFG signal, and the identity of several intermolecular modes in the SFG spectra for the water/vapor interface. Thesis (Ph.D.)--University of South Florida, 2005. Includes bibliographical references. Text (Electronic thesis) in PDF format. System requirements: World Wide Web browser and PDF reader. Mode of access: World Wide Web. ABSTRACT: Our work investigates theoretical approximations to the interface specific sum frequency generation (SFG) spectra at aqueous interfaces constructed using time correlation function (TCF) and instantaneous normal mode (INM) methods. Both approaches lead to signals in excellent agreement with experimental measurements. This work demonstrates how TCF and INM methods can be used in a complementary fashion to describe interfacial vibrational spectroscopy. Our approach is to compare TCF spectra with experiment to establish that our molecular dynamics (MD) methods can reliably describe the system of interest. We then employ INM methods to analyze the molecular and dynamical basis for the observed spectroscopy. We have been able to elucidate, on a molecularly detailed basis, a number of interfacial line shapes, most notably the origin of the complex O-H stretching SFG signal, and the identity of several intermolecular modes in the SFG spectra for the water/vapor interface. Adviser: Brian Space. Water. Molecular dynamics. Liquid/vapor interface. Nonlinear spectroscopy. SFG.
A theoretical description of the vibrational sum frequency generation spectroscopy of interfaces [electronic resource] /
Perry, Angela S.
[Tampa, Fla.] : University of South Florida,
2005.
eng
ABSTRACT: Our work investigates theoretical approximations to the interface specific sum frequency generation (SFG) spectra at aqueous interfaces constructed using time correlation function (TCF) and instantaneous normal mode (INM) methods. Both approaches lead to signals in excellent agreement with experimental measurements. This work demonstrates how TCF and INM methods can be used in a complementary fashion to describe interfacial vibrational spectroscopy. Our approach is to compare TCF spectra with experiment to establish that our molecular dynamics (MD) methods can reliably describe the system of interest. We then employ INM methods to analyze the molecular and dynamical basis for the observed spectroscopy. We have been able to elucidate, on a molecularly detailed basis, a number of interfacial line shapes, most notably the origin of the complex O-H stretching SFG signal, and the identity of several intermolecular modes in the SFG spectra for the water/vapor interface.
Thesis (Ph.D.)--University of South Florida, 2005.
Includes bibliographical references.
Text (Electronic thesis) in PDF format.
System requirements: World Wide Web browser and PDF reader.
Mode of access: World Wide Web.
ABSTRACT: Our work investigates theoretical approximations to the interface specific sum frequency generation (SFG) spectra at aqueous interfaces constructed using time correlation function (TCF) and instantaneous normal mode (INM) methods. Both approaches lead to signals in excellent agreement with experimental measurements. This work demonstrates how TCF and INM methods can be used in a complementary fashion to describe interfacial vibrational spectroscopy. Our approach is to compare TCF spectra with experiment to establish that our molecular dynamics (MD) methods can reliably describe the system of interest. We then employ INM methods to analyze the molecular and dynamical basis for the observed spectroscopy. We have been able to elucidate, on a molecularly detailed basis, a number of interfacial line shapes, most notably the origin of the complex O-H stretching SFG signal, and the identity of several intermolecular modes in the SFG spectra for the water/vapor interface.
Adviser: Brian Space.
Water.
Molecular dynamics.
Liquid/vapor interface.
Nonlinear spectroscopy.
SFG.