Physics at Virginia

Until about 2005, molecular rotational spectroscopy was performed using narrowband (~1 MHz) excitation of a low-pressure gas in a resonant cavity.  This method offers high sensitivity for each data acquisition, but the time required to perform a spectrum scan over about 10 GHz, needed to capture the rotational spectrum, was a major limitation to applications of the technique.  Advances in high-speed digital electronics have made it possible to design spectrometers that offer instantaneous, broadband (> 10 GHz) performance.  During our initial work with high-speed arbitrary waveform generators and digitizers (with Tom Gallagher) we developed the method of chirped pulse Fourier transform rotational spectroscopy that uses a pulse with linear chirp to phase-reproducibly excite the gas sample.  The subsequent coherent emission (free induction decay) is detected with the high-speed digitizer and the frequency domain spectrum is obtained using FFT analysis.  Since the introduction of the technique in 2008 [1], the method has been applied to unimolecular reaction dynamics [2], the structures of molecular clusters [3], and the laboratory identification of molecules in the interstellar medium [4].  The technique has been extended to mm-wave spectroscopy with applications to Rydberg spectroscopy [5], chemical reaction dynamics, and analytical chemistry.  The broadband technique has also enabled a new generation of molecular structure studies in the field of chirality [6] with the potential for solving significant challenges for real-time pharmaceutical manufacturing.



[1] G.G. Brown, B.C. Dian, K.O. Douglass, S.M. Geyer, and B.H. Pate, “A Broadband Fourier Transform Microwave Spectrometer Based on Chirped Pulse Excitation” Rev. Sci. Instrum. 79, 053103 (2008).

[2] B.C. Dian, G.G. Brown, K.O. Douglass, and B.H. Pate, “Measuring Picosecond Isomerization Dynamics via Ultra-broadband Fourier Transform Microwave Spectroscopy”, Science 320, 924-928 (2008).

[3] C. Pérez, M.T. Muckle, D.P. Zaleski, N.A. Seifert, B. Temelso, G.C. Shields, Z. Kisiel, and B.H. Pate, “Structures of Cage, Prism, and Book Isomers of Water Hexamer from Broadband Rotational Spectroscopy”, Science 336, 897-901 (2012).

[4] D.P. Zaleski, N.A. Seifert, A.L. Steber, M.T. Muckle, R.A. Loomis, J.F. Corby, O. Martinez, Jr., K.N. Crabtree, P.R. Jewell, J.M. Hollis, F.J. Lovas, D. Vasquez, J. Nyiramahirwe, N.  Sciortino, K. Johnson, M.C. McCarthy, A.J. Remijan, and B.H. Pate, “Detection of E-cyanomethanimine towards Sagittarius B2(N) in the Green Bank Telescope PRIMOS Survey”, Ap. J. Letters, 765, L10 (2013).

[5] K. Prozument, A.P. Colombo, Y. Zhou, G.B. Park, V.S. Petrovic, S.L. Coy, and R.W. Field, “Chirped-pulse Millimeter-wave Spectroscopy of Rydberg-Rydberg Transitions”, Phys. Rev. Lett. 107, 143001 (2011).

[6] D. Patterson, M. Schnell, and J.M. Doyle, “Enantiomer-specific detection of chiral molecules via microwave spectroscopy”, Nature 497, 475 (2013).

Friday, October 23, 2015
3:30 PM
Physics Building, Room 204
Note special room.

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