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Journal of the Optical Society of America B

Efficient 5D excitation of trapped Rb atoms using pulses of diode-laser light in the counterintuitive order

Wenko Süptitz, B. C. Duncan, P. L. Gould

Published May 1, 1997• 37 citations
Publisher

Abstract

We demonstrate that appropriately time-ordered pulses of diode-laser light can provide efficient population transfer in a three-level cascade system. Laser-trapped Rb atoms are excited from the 5S ground state to the highly-excited 5D level (through the 5P intermediate level) with a transfer efficiency approaching 100%. Diode-laser light at 780 nm (5S→5P) and 776 nm (5P→5D) is switched with acousto-optic modulators to provide the excitation. The measured variation of transfer efficiency with relative delay between the two pulses is in reasonable agreement with theoretical predictions. However, the intensities needed for efficient transfer are significantly higher than expected. In general, optimum excitation occurs for the counterintuitive pulse ordering, i.e., when the upper transition is driven first.

DOI
10.1364/josab.14.001001

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arXiv:1106.0959•Journal of Physics B Atomic Molecular and Optical Physics•Oct 18, 2011•24 citations
We demonstrate that appropriately time-ordered pulses of diode-laser light can provide efficient population transfer in a three-level cascade system. Laser-trapped Rb atoms are excited from the 5S ground state to the highly-excited 5D level (through the 5P intermediate level) with a transfer efficiency approaching 100%. Diode-laser light at 780 nm (5S→5P) and 776 nm (5P→5D) is switched with acousto-optic modulators to provide the excitation. The measured variation of transfer efficiency with relative delay between the two pulses is in reasonable agreement with theoretical predictions. However, the intensities needed for efficient transfer are significantly higher than expected. In general, optimum excitation occurs for the counterintuitive pulse ordering, i.e., when the upper transition is driven first.
The authors have demonstrated that appropriately time-ordered pulses of diode-laser light can provide efficient population transfer in a three-level cascade system. Laser-trapped Rb atoms are excited from the 5S ground state to the highly-excited 5D level (via the 5P intermediate level) with nearly 100% efficiency. Diode-lasers at 780 nm (5S{yields}5P) and 776 nm (5P{yields}5D) are pulsed with acousto-optic modulators to provide the excitation. The variation of transfer efficiency with relative delay between the two pulses is in good agreement with theoretical expectations. Optimum excitation occurs for the counterintuitive pulse ordering, i.e., when the upper transition is driven first.
A series of experiments is performed on cold 85Rb atoms confined in a magneto-optical trap. A variation of Stimulated Raman adiabatic passage (STIRAP) is used to transfer population from the 5S 1/2 ground state to the 5D5/2 state with an efficiency exceeding 80%. This process relies on moderately intense pulses arriving in the counterintuitive order, i.e., the upper transition (5P → 5D) driven before the lower transition (5S → 5P ). There is reasonable agreement with computer simulations, excepting a marked discrepancy between measured intensities and those used in the simulations. With a large ensemble of 5D atoms available, the 5D photoionization cross section at four different laser wavelengths (1064, 788, 647 and 532 nm) is determined via trap loss measurements. The theoretical calculations agree well with the experimental results (17.7, 10.9, 7.6 and 5.2 Mb, respectively). An experiment to measure the 5S-5D collisional rate constant sets an order-of-magnitude upper bound of 10−10 cm3/s, assuming all atoms are 5S-5D pairs. ^
Enhanced population transfer from the lowest to the highest level in the three-state ladder 5s->5p->5d of the rubidium atom by frequency swept ultra short laser pulses is observed if the frequency sweep first makes the pulse resonant with the 5s->5p transition, and later with the 5p->5d transition. With this intuitive scheme it is possible to achieve complete population inversion via the intermediate level by two successive adiabatic passages. Complete inversion is also obtained by a {open_quote}counterintuitive{close_quote} direction of the frequency-sweep, in which case population of the intermediate level during the pulse is strongly reduced. The atomic system can be seen as a model system for multistep vibrational excitation in an anharmonic molecular potential.
Enhancement and reduction of the fluorescence intensity in Rb atomic vapor are observed. The reduction is due to a depopulation of the 5P - {3/2 } state upon illumination of a Rb vapor cell with light corresponding to the 5P - {3/2 }→5D - {5/2 } transition. Collisional transfer of the 5D - {5/2 } atoms to the 5D - {3/2 } state, followed by radiative decay to the 5P - {1/2 } state, creates an increase in the population of the 5P - {1/2 } state. The increase in the excited state population results in an increase in the fluorescence intensity of the 5P - {1/2 }→5S - {1/2 } transition. The laser-induced population changes are monitored by the decrease or increase of the corresponding fluorescence signals. Using the steady-state rate equations, the rate constants for the stimulated emission(i.e., 5D - {5/2 }→5P - {3/2 }) is 2.0×10 +8s + {-1 }. The cross section for the fine-structure changing collision(i.e., 5D - {5/2 }→5D - {3/2 }) is 6.4×10 + {-14 }cm +2.
Excitation of a quantum ladder system by frequency-swept (-chirped) laser pulses has been investigated by studying an atomic model system, the 5s-5p-5d ladder of rubidium. The population transfer is significantly enhanced when the frequency is swept such that it follows the spacing of the ladder. At intermediate intensities we observe oscillations in the population transfer to the upper level (5d), which can be attributed to interference between two routes of excitation: sequential transfer and direct two-photon excitation via a virtual intermediate state. We determine simultaneously the population transfer to the upper level (5d) and the direct three-photon ionization, the latter corresponding to a three-step ladder with the final state being in the continuum: 5s-5p-5d-\ensuremath{\varepsilon}p/\ensuremath{\varepsilon}f. Experiments were performed, using 100 fs pulses at \ensuremath{\sim}780 nm from a self-mode-locked Ti:Al2{\mathrm{Al}}_{2}Al2​O3{\mathrm{O}}_{3}O3​ oscillator amplified at 10 Hz.
We investigate the excitation of the 5D_{5/2} level in Rb atoms using counter-propagating laser beams, which are nearly resonant to the one-photon 5S_{1/2} - 5P_{3/2} and 5P_{3/2} - 5D_{5/2} transitions, ensuring that a sum of the optical frequencies corresponds to the 5S_{1/2} - 5D_{5/2} transition. The excitation produced by two-photon and step-wise processes is detected via spontaneously emitted fluorescence at 420 nm arising from the 6P_{3/2} - 5S_{1/2} transition. The dependences of blue fluorescence intensity on atomic density and laser detuning from the intermediate 5P_{3/2} level have been investigated. The sensitivity of the frequency detuned bi-chromatic scheme for atom detection has been estimated. A novel method for sum frequency stabilization of two free-running lasers has been suggested and implemented using two-photon Doppler-free fluorescence and polarization resonances.