Chirped-pulse millimeter-wave spectroscopy: Spectrum, dynamics, and manipulation of Rydberg-Rydberg transitions
- Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139 (United States)
We apply the chirped-pulse millimeter-wave (CPmmW) technique to transitions between Rydberg states in calcium atoms. The unique feature of Rydberg-Rydberg transitions is that they have enormous electric dipole transition moments ({approx}5 kiloDebye at n*{approx} 40, where n* is the effective principal quantum number), so they interact strongly with the mm-wave radiation. After polarization by a mm-wave pulse in the 70-84 GHz frequency region, the excited transitions re-radiate free induction decay (FID) at their resonant frequencies, and the FID is heterodyne-detected by the CPmmW spectrometer. Data collection and averaging are performed in the time domain. The spectral resolution is {approx}100 kHz. Because of the large transition dipole moments, the available mm-wave power is sufficient to polarize the entire bandwidth of the spectrometer (12 GHz) in each pulse, and high-resolution survey spectra may be collected. Both absorptive and emissive transitions are observed, and they are distinguished by the phase of their FID relative to that of the excitation pulse. With the combination of the large transition dipole moments and direct monitoring of transitions, we observe dynamics, such as transient nutations from the interference of the excitation pulse with the polarization that it induces in the sample. Since the waveform produced by the mm-wave source may be precisely controlled, we can populate states with high angular momentum by a sequence of pulses while recording the results of these manipulations in the time domain. We also probe the superradiant decay of the Rydberg sample using photon echoes. The application of the CPmmW technique to transitions between Rydberg states of molecules is discussed.
- OSTI ID:
- 22099159
- Journal Information:
- Journal of Chemical Physics, Vol. 138, Issue 1; Other Information: (c) 2013 American Institute of Physics; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
ANGULAR MOMENTUM
CALCIUM
DECAY
DIPOLE MOMENTS
E1-TRANSITIONS
EXCITATION
GHZ RANGE 01-100
KHZ RANGE 01-100
PHOTONS
POLARIZATION
PULSES
RESOLUTION
RYDBERG STATES
SPECTRA
SPECTROMETERS
SPECTROSCOPY
WAVE FORMS
WAVE POWER