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Physical interpretation of measured rises and decays of fluorescence waveforms involving coupled energy levels

Bogdanov, V. K., D.J. Booth, W. Wayt Gibbs, Douglas Robert MacFarlane, Newman, P. J.

Published Jan 1, 2000• 0 citations
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Physical interpretation of fluorescence waveforms from coupled energy levels

Bogdanov, V. K., D.J. Booth, W. Wayt Gibbs

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The fluorescence intensities and lifetimes of various no-phonon lines in ruby samples with 2.1 and 0.94% ${\mathrm{Cr}}^{3+}$ were studied from 13 to 700\ifmmode^\circ\else\textdegree\fi{}K. The temperature dependences of the intensities of numerous lines were used to determine the energy levels of two pair systems. The relative intensities of the single-ion ($R$) lines and the pair ($N$) lines are proportional to Boltzmann factors ${e}^{\frac{\ensuremath{-}\ensuremath{\Delta}E}{\mathrm{kT}}}$, where $\ensuremath{\Delta}E$ is the difference in energy of the metastable states, at high temperatures but not at low temperatures. The deviation from this law is greater and occurs at higher temperatures in the less concentrated sample. The fluorescence decays of the $R$ and $N$ lines are pure exponentials in the temperature region where the $N$ lines follow a Boltzmann law; at low temperatures the $N$ lines have an initial rise in fluorescence and then a decay. These results are interpreted in terms of coupled fluorescence systems consisting of single ions and pairs. A phonon-assisted cross-relaxation coupling process is suggested which allows for thermalization of the systems at high temperatures and direct pumping of the pair systems by the single-ion system at low temperatures. Energy transfer from single-ion to multi-ion systems was also observed.

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Narrow spectral feature in resonance fluorescence with a single monochromatic laser field

Jörg Evers, Christoph H. Keitel

We describe the resonance fluorescence spectrum of an atomic three-level system where two of the states are coupled by a single monochromatic laser field. The influence of the third energy level, which interacts with the two laser-coupled states only via radiative decays, is studied in detail. For a suitable choice of parameters, this system gives rise to a very narrow structure at the laser frequency in the fluorescence spectrum which is not present in the spectrum of a two-level atom. We find those parameter ranges by a numerical analysis and use the results to derive analytical expressions for the additional narrow peak. We also derive an exact expression for the peak intensity under the assumption that a random telegraph model is applicable to the system. This model and a simple spring model are then used to describe the physical origins of the additional peak. Using these results, we explain the connection between our system, a three-level system in the V configuration where both transitions are laser driven, and a related experiment that was recently reported.

arXiv:quant-ph/0109117•Physical Review A•Feb 13, 2002•13 citations

Experiments on Er3+ in SrF2. III. Coupled-Ion Effects

M. R. Brown, H. Thomas, James M. Williams +2 more

The pumping intensity and concentration dependences of the fluorescence output from three infrared quantum-counter schemes that involve coupled ions in Er3+-doped SrF2 have been measured at 300 and 77°K. The pumping intensity depended linearly on the numbers of photons absorbed in the schemes. The power of the concentration dependence was found to be noninteger in the range 1%–10%. This has been interpreted as indicating the importance of energy migration between the Er3+ ions as mechanism for populating the energy levels of the coupled ions.

The Journal of Chemical Physics•Oct 15, 1969•28 citations
The fluorescence intensities and lifetimes of various no-phonon lines in ruby samples with 2.1 and 0.94% Cr3+{\mathrm{Cr}}^{3+}Cr3+ were studied from 13 to 700\ifmmode^\circ\else\textdegree\fi{}K. The temperature dependences of the intensities of numerous lines were used to determine the energy levels of two pair systems. The relative intensities of the single-ion (RRR) lines and the pair (NNN) lines are proportional to Boltzmann factors ${e}^{\frac{\ensuremath{-}\ensuremath{\Delta}E}{\mathrm{kT}}}$, where $\ensuremath{\Delta}E$ is the difference in energy of the metastable states, at high temperatures but not at low temperatures. The deviation from this law is greater and occurs at higher temperatures in the less concentrated sample. The fluorescence decays of the RRR and NNN lines are pure exponentials in the temperature region where the NNN lines follow a Boltzmann law; at low temperatures the NNN lines have an initial rise in fluorescence and then a decay. These results are interpreted in terms of coupled fluorescence systems consisting of single ions and pairs. A phonon-assisted cross-relaxation coupling process is suggested which allows for thermalization of the systems at high temperatures and direct pumping of the pair systems by the single-ion system at low temperatures. Energy transfer from single-ion to multi-ion systems was also observed.
We describe the resonance fluorescence spectrum of an atomic three-level system where two of the states are coupled by a single monochromatic laser field. The influence of the third energy level, which interacts with the two laser-coupled states only via radiative decays, is studied in detail. For a suitable choice of parameters, this system gives rise to a very narrow structure at the laser frequency in the fluorescence spectrum which is not present in the spectrum of a two-level atom. We find those parameter ranges by a numerical analysis and use the results to derive analytical expressions for the additional narrow peak. We also derive an exact expression for the peak intensity under the assumption that a random telegraph model is applicable to the system. This model and a simple spring model are then used to describe the physical origins of the additional peak. Using these results, we explain the connection between our system, a three-level system in the V configuration where both transitions are laser driven, and a related experiment that was recently reported.
The pumping intensity and concentration dependences of the fluorescence output from three infrared quantum-counter schemes that involve coupled ions in Er3+-doped SrF2 have been measured at 300 and 77°K. The pumping intensity depended linearly on the numbers of photons absorbed in the schemes. The power of the concentration dependence was found to be noninteger in the range 1%–10%. This has been interpreted as indicating the importance of energy migration between the Er3+ ions as mechanism for populating the energy levels of the coupled ions.