Mass-correlated rotational Raman spectra with high resolution, broad bandwidth, and absolute frequency accuracy
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- Mass-correlated rotational Raman spectra with high resolution, broad bandwidth, and absolute frequency accuracy
- Schroter, Christian; Lee, Jong Chan; Schultz, Thomas
- multidimensional spectroscopy; correlated measurement; rotational alignment; Raman spectroscopy; high-resolution spectroscopy
- Issue Date
- NATL ACAD SCIENCES
- PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, v.115, no.20, pp.5072 - 5076
- We present mass-correlated rotational alignment spectroscopy, based on the optical excitation of a coherent rotational quantum wave and the observation of temporal wave interferences in a mass spectrometer. Combined electronic and opto-mechanical delays increased the observation time and energy resolution by an order of magnitude compared with preceding time-domain measurements. Rotational transition frequencies were referenced to an external clock for accurate absolute frequency measurements. Rotational Raman spectra for six naturally occurring carbon disulfide isotopologues were resolved with 3 MHz resolution over a spectral range of 500 GHz. Rotational constants were determined with single-kilohertz accuracy, competitive with state-of-the-art frequency domain measurements.
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