2011/07/05 by David S. Wilcox, Kelly M. Hotopp, Brian C. Dian · 1 citation
Chemistry · Mathematics · Physics and Astronomy · #Autocorrelation #Bandwidth (computing) #Broadband #Coherence (philosophical gambling strategy) #Computer science #Fourier transform #Fourier transform infrared spectroscopy #Fourier transform spectroscopy #Materials science #Mathematics #Microwave #Molecular spectroscopy and chirality #Nuclear magnetic resonance #Optics #Physics #Pulse sequence #Spectrometer #Spectroscopy #Spectroscopy and Laser Applications #Spectroscopy and Quantum Chemical Studies #Telecommunications
paper · doi:10.1021/jp2043202
openalex publication_date 2011/07/05 · openalex created_date 2025/10/10 · openalex updated_date 2026/06/15
Two-dimensional (2D) correlation techniques are developed for chirped-pulse Fourier transform microwave (CP-FTMW) spectroscopy. The broadband nature of the spectrometer coupled with fast digital electronics permits the generation of arbitrary pulse sequences and simultaneous detection of the 8-18 GHz region of the microwave spectrum. This significantly increases the number of rotation transitions that can be simultaneously probed, as well as the bandwidth in both frequency dimensions. We theoretically and experimentally evaluate coherence transfer of three- and four-level systems to relate the method with previous studies. We then extend the principles of single-quantum and autocorrelation to incorporate broadband excitation and detection. Global connectivity of the rotational energy level structure is demonstrated through the transfer of multiple coherences in a single 2D experiment. Additionally, open-system effects are observed from irradiating many-level systems. Quadrature detection in the indirectly measured frequency dimension and phase cycling are also adapted for 2D CP-FTMW spectroscopy.