No Arabic abstract
Using a Ramsey-type setup, the lambda-doublet transition in the $J=1,, Omega=1$ level of the $a^3Pi$ state of CO was measured to be 394 064 870(10) Hz. In our molecular beam apparatus, a beam of metastable CO is prepared in a single quantum level by expanding CO into vacuum and exciting the molecules using a narrow-band UV laser system. After passing two microwave zones that are separated by 50 cm, the molecules are state-selectively deflected and detected 1 meter downstream on a position sensitive detector. In order to keep the molecules in a single $m_J^B$ level, a magnetic bias field is applied. We find the field-free transition frequency by taking the average of the $m_J^B = +1 rightarrow m_J^B = +1$ and $m_J^B = -1 rightarrow m_J^B = -1$ transitions, which have an almost equal but opposite Zeeman shift. The accuracy of this proof-of-principle experiment is a factor of 100 more accurate than the previous best value obtained for this transition.
We present a combined experimental and theoretical study on the radiative lifetime of CO in the $a^3Pi_{1,2}, v=0$ state. CO molecules in a beam are prepared in selected rotational levels of this metastable state, Stark-decelerated and electrostatically trapped. From the phosphorescence decay in the trap, the radiative lifetime is measured to be $2.63pm0.03$ ms for the $a^3Pi_1, v=0, J=1$ level. From spin-orbit coupling between the $a^3Pi$ and the $A^1Pi$ state a 20% longer radiative lifetime of 3.16 ms is calculated for this level. It is concluded that coupling to other $^1Pi$ states contributes to the observed phosphorescence rate of metastable CO.
We here report on the experimental realization of a microwave decelerator for neutral polar molecules, suitable for decelerating and focusing molecules in high-field-seeking states. The multi-stage decelerator consists of a cylindrical microwave cavity oscillating on the TE 11n mode, with n=12 electric field maxima along the symmetry axis. By switching the microwave field on and off at the appropriate times, a beam of state-selected ammonia molecules with an incident mean velocity of 25 m/s is guided while being spatially focussed in the transverse direction and bunched in the forward direction. Deceleration from 20.0 m/s to 16.9 m/s and acceleration from 20.0 m/s to 22.7 m/s is demonstrated.
UV frequency metrology has been performed on the a3Pi - X1Sigma+ (0,0) band of various isotopologues of CO using a frequency-quadrupled injection-seeded narrow-band pulsed Titanium:Sapphire laser referenced to a frequency comb laser. The band origin is determined with an accuracy of 5 MHz (delta u / u = 3 * 10^-9), while the energy differences between rotational levels in the a3Pi state are determined with an accuracy of 500 kHz. From these measurements, in combination with previously published radiofrequency and microwave data, a new set of molecular constants is obtained that describes the level structure of the a3Pi state of 12C16O and 13C16O with improved accuracy. Transitions in the different isotopologues are well reproduced by scaling the molecular constants of 12C16O via the common mass-scaling rules. Only the value of the band origin could not be scaled, indicative of a breakdown of the Born-Oppenheimer approximation. Our analysis confirms the extreme sensitivity of two-photon microwave transitions between nearly-degenerate rotational levels of different Omega-manifolds for probing a possible variation of the proton-to-electron mass ratio, mu=m_p/m_e, on a laboratory time scale.
Strong field transient grating spectroscopy has shown to be a very versatile tool in time-resolved molecular spectroscopy. Here we use this technique to investigate the high-order harmonic generation from SF6 molecules vibrationally excited by impulsive stimulated Raman scattering. Transient grating spectroscopy enables us to reveal clear modulations of the harmonic emission. This heterodyne detection shows that the harmonic emission generated between 14 to 26 eV is mainly sensitive to two among the three active Raman modes in SF6, i.e. the strongest and fully symmetric nu 1-A1g mode (774 cm-1, 43 fs) and the slowest mode nu5-T2g (524 cm-1, 63 fs). A time-frequency analysis of the harmonic emission reveals additional dynamics: the strength and central frequency of the nu 1 mode oscillate with a frequency of 52 cm-1 (640 fs). This could be a signature of the vibration of dimers in the generating medium. Harmonic 11 shows a remarkable behavior, oscillating in opposite phase, both on the fast (774 cm-1) and slow (52 cm-1) timescales, which indicates a strong modulation of the recombination matrix element as a function of the nuclear geometry. These results demonstrate that the high sensitivity of high-order harmonic generation to molecularvibrations, associated to the high sensitivity of transient grating spectroscopy, make their combination a unique tool to probe vibrational dynamics.
Ultracold neutrons (UCNs) are formidable probes in precision tests of gravity. With their negligible electric charge, dielectric moment, and polarizability they naturally evade some of the problems plaguing gravity experiments with atomic or macroscopic test bodies. Taking advantage of this fact, the qBounce collaboration has developed a technique - gravity resonance spectroscopy (GRS) - to study bound quantum states of UCN in the gravity field of the Earth. This technique is used as a high-precision tool to search for hypothetical Non-Newtonian gravity on the micrometer scale. In the present article, we describe the recently commissioned Ramsey-type GRS setup, give an unambiguous proof of principle, and discuss possible measurements that will be performed.