Femtosecond spectral interferometry of optical activity: Theory

Hanju Rhee, Jeong Hyon Ha, Seung Joon Jeon, Minhaeng Cho

Research output: Contribution to journalArticle

27 Citations (Scopus)

Abstract

Optical activities such as circular dichroism (CD) and optical rotatory dispersion (ORD) are manifested by almost all natural products. However, the CD is an extremely weak effect so that time-resolved CD spectroscopy has been found to be experimentally difficult and even impossible for vibrational CD with current technology. Here, we show that the weak-signal and nonzero background problems can be overcome by heterodyned spectral interferometric detection of the phase and amplitude of optical activity free-induction-decay (OA FID) field. A detailed theoretical description and a cross-polarization scheme for selectively measuring the OA FID are presented and discussed. It is shown that the parallel and perpendicular electric fields when the solution sample contains chiral molecules are coupled to each other. Therefore, simultaneous spectral interferometric measurements of the parallel and perpendicular FID fields can provide the complex susceptibility, which is associated with the circular dichroism and optical rotatory dispersion as its imaginary and real parts, respectively. On the basis of the theoretical results, to examine its experimental possibility, we present numerical simulations for a model system. We anticipate the method discussed here to be a valuable tool for detecting electronic or vibrational optical activity in femtosecond time scale.

Original languageEnglish
Article number094507
JournalJournal of Chemical Physics
Volume129
Issue number9
DOIs
Publication statusPublished - 2008

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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