Elimination of unwanted echoes and reduction of dead time in three-pulse electron spin-echo spectroscopy

Coherent Transient and Holeburning Spectroscopy of Rare Earth Ions in Solids

Coherent multidimensional vibrational spectroscopy (CMDVS) is an emerging field that offers new oportunities to probe specifically intramolecular and intermolecular interactions in complex samples with the improved resolution and selectivity expected of a multidimensional method. In particular, it provides structural and dynamical information about correlations between modes. It provides this information on the picosecond time scales characteristic of vibrational dephasing. CMDVS is based on the perturbations that are induced in a mode when other coupled modes are excited. It is the vibrational analogue to multidimensional nucler magnetic resonance (NMR). In this review, we present the background that led to the development of CMDVS, a brief summary of the different methods of non-linear laser spectroscopy and how they can achieve CMDVS, the relationships between CMDVS and multidimensional NMR, and the theory necessary to understand the experimental results. The experimental approaches reviewed fall into ...

Coherent multidimensional vibrational spectroscopy

Electronic Energy Level Structure

Optical read-out and manipulation of the nuclear spin state of single rare-earth ions doped in a crystal enable the large-scale storage and the transport of quantum information. Here, we report the photo-luminescence excitation spectroscopy results of single Pr3+ ions in a bulk crystal of LaF3 at 1.5 K. In a bulk sample, the signal from a single ion at the focus is often hidden under the background signal originating from numerous out-of-focus ions in the entire sample. To combine with a homemade cryogenic confocal microscope, we developed a reflecting objective that works in superfluid helium with a numerical aperture of 0.99, which increases the signal by increasing the solid angle of collection to 1.16π and reduces the background by decreasing the focal volume. The photo-luminescence excitation spectrum of single Pr3+ was measured at a wing of the spectral line of the 3H4 → 3P0 transition at 627.33 THz (477.89 nm). The spectrum of individual Pr3+ ions appears on top of the background of 60 cps as isolated peaks with intensities of 20–30 cps and full-width at half-maximum widths of approximately 3 MHz at an excitation intensity of 80 W cm−2.

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K. Chiang

Papers

Spectroscopic and relaxation character of the P 0 3 − H 4 3 transition in La F 3 : Pr 3 + measured by photon echoes