Design and evaluation of a pulsed-jet chirped-pulse millimeter-wave spectrometer for the 70-102 GHz region.

Chirped-pulse millimeter-wave (CPmmW) spectroscopy is the first broadband (multi-GHz in each shot) Fourier-transform technique for high-resolution survey spectroscopy in the millimeter-wave region. The design is based on chirped-pulse Fourier-transform microwave (CP-FTMW) spectroscopy [G. G. Brown, B. C. Dian, K. O. Douglass, S. M. Geyer, S. T. Shipman, and B. H. Pate, Rev. Sci. Instrum. 79, 053103 (2008)], which is described for frequencies up to 20 GHz. We have built an instrument that covers the 70-102 GHz frequency region and can acquire up to 12 GHz of spectrum in a single shot. Challenges to using chirped-pulse Fourier-transform spectroscopy in the millimeter-wave region include lower achievable sample polarization, shorter Doppler dephasing times, and problems with signal phase stability. However, these challenges have been partially overcome and preliminary tests indicate a significant advantage over existing millimeter-wave spectrometers in the time required to record survey spectra. Further improvement to the sensitivity is expected as more powerful broadband millimeter-wave amplifiers become affordable. The ability to acquire broadband Fourier-transform millimeter-wave spectra enables rapid measurement of survey spectra at sufficiently high resolution to measure diagnostically important electronic properties such as electric and magnetic dipole moments and hyperfine coupling constants. It should also yield accurate relative line strengths across a broadband region. Several example spectra are presented to demonstrate initial applications of the spectrometer.

Spectrum and infrared intensities of OH-stretching bands of water dimers.

Water dimers have been assembled in He droplets and studied by infrared laser depletion spectroscopy. All four OH stretching bands of the dimer have been identified in the spectral range 3590-3800 cm(-1). Infrared intensities of the bands are also reported. The results are compared with previous measurements and theoretical calculations.

Hydrogen clusters that remain fluid at low temperature.

Superfluidity of hydrogen, predicted three decades ago, continues to elude experimental observation, due to the high freezing temperature of H2 at T=13.8 K. Here, large para-H2 clusters are obtained in a cryogenic pulsed free jet expansion and are studied via nonlinear Raman spectroscopy. Clusters formed from neat pH_{2} are solid as evidenced by the characteristic splitting of the rotational S0(0) line. However, clusters formed of highly diluted pH_{2} (< or = 1%) in He have a single S0(0) line and remain liquid at the estimated superfluid transition temperature of T=1-2 K.