Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 40, Pages 22004-22009Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202109345
Keywords
chiral Raman spectroscopy; circularly polarized Raman; electronic circular dichroism; finite-lifetime approach; resonance Raman optical activity
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Funding
- Natural Sciences and Engineering Research Council of Canada
- Canada Foundation for Innovation
- Alberta Enterprise, Advanced Education
- Ministry of Education of the Czech Republic [CZ.02.1.01/0.0/0.0/16_019/0000729]
- Alberta Excellence Graduate Scholarship
- Gunning Physical Chemistry Fellowship
- University of Alberta
- Compute Canada [20-10144S]
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A new form of chiral Raman spectroscopy, eCP-Raman, combining electronic circular dichroism and circularly polarized Raman, has been developed to capture experimental patterns of chiral molecules under resonance. This innovation opens up opportunities for applications of eCP-Raman spectroscopy and for extracting true RROA experimentally.
Resonance Raman optical activity (RROA) is commonly measured as the difference in intensity of Raman scattered right and left circularly polarized light, I-R-I-L, when a randomly polarized light is in resonance with a chiral molecule. Strong and sometimes mono-signate experimental RROA spectra of several chiral solutes were reported previously, although their signs and relative intensities could not be reproduced theoretically. By examining multiple light-matter interaction events which can occur simultaneously under resonance, we show that a new form of chiral Raman spectroscopy, eCP-Raman, a combination of electronic circular dichroism and circularly polarized Raman, prevails. By incorporating the finite-lifetime approach for resonance, the experimental patterns of the model chiral solutes are captured theoretically by eCP-Raman, without any RROA contribution. The results open opportunity for applications of eCP-Raman spectroscopy and for extracting true RROA experimentally.
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