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AIAA Plasmadynamics and Lasers Conference

Determining the Two-Photon Absorption Cross-Section for the 52S1/2 --> 52D5/2 Transition in Naturally Occurring Rubidium

Jeffrey Gallagher, Glen P. Perram

Published Jun 1, 2011• 1 citation
Publisher

Abstract

Recently we demonstrated lasing at 420 nm and 455 nm inside of rubidium and cesium vapor cells respectively, by non-resonant, two photon absorption at near infrared pump wavelengths. Two photon absorption from the ground S1/2 state to excited D3/2,5/2 or higher lying S1/2 state via virtual states and subsequent infrared stimulated emission pumps the upper laser levels, the second excited P1/2,3/2 states. To better understand the mechanism and phenomenology of this type of laser, this paper presents a method for determining the two-photon absorption (TPA) cross-section for the 5S1/2 −→ 5D5/2 transition in naturally occurring rubidium. For an incident pump intensity of 392 W cm2 and a rubidium concentration of 3.34 × 10 atoms cm3 , a peak absorbance of 0.10 is observed. The concentration of the Rb in the test cell is determined by one photon absorption spectra of the D2, indicating a vapor curve shifted by 14 C from the exterior wall temperature. The incident laser beam is focused to a waist of 75 μm. The beam quality is consistent with an M = 1.05 − 1.09. A model for the intensity as a function of propagation distance is developed to interpret the observed absorption spectrum and determine a cross-section for the two photon absorption.

DOI
10.2514/6.2011-4005

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arXiv:2007.08452•Physical Review Applied•Oct 23, 2020•9 citations
Recently we demonstrated lasing at 420 nm and 455 nm inside of rubidium and cesium vapor cells respectively, by non-resonant, two photon absorption at near infrared pump wavelengths. Two photon absorption from the ground S1/2 state to excited D3/2,5/2 or higher lying S1/2 state via virtual states and subsequent infrared stimulated emission pumps the upper laser levels, the second excited P1/2,3/2 states. To better understand the mechanism and phenomenology of this type of laser, this paper presents a method for determining the two-photon absorption (TPA) cross-section for the 5S1/2 −→ 5D5/2 transition in naturally occurring rubidium. For an incident pump intensity of 392 W cm2 and a rubidium concentration of 3.34 × 10 atoms cm3 , a peak absorbance of 0.10 is observed. The concentration of the Rb in the test cell is determined by one photon absorption spectra of the D2, indicating a vapor curve shifted by 14 C from the exterior wall temperature. The incident laser beam is focused to a waist of 75 μm. The beam quality is consistent with an M = 1.05 − 1.09. A model for the intensity as a function of propagation distance is developed to interpret the observed absorption spectrum and determine a cross-section for the two photon absorption.
Abstract : The Doppler-broadened two-photon absorption (TPA) cross-section for the 52S1/2- 52D5/2 transition in Rb is measured using direct absorption methods. A detailed model of the intensity profile was developed to account for a focused Gaussian beam propagating through a two-photon absorption medium. A peak absorbance of 24% was observed for an intensity of 6.28 kW/cm2 at the focus, a Rb density of 4.6 x 1015 cm-3 concentrations from 1.61-8.52 x 10(15) cm-3 line. Extracting the hyperfine-broadened TPA cross-section from 87 test configurations, while varying the pump power, alkali concentration and focal length, yielded an error weighted average of 6.75x10-21 cm4/W. This cross-section is sufficient for a pulsed dye laser to bleach the pump transition in the Two-Photon Pumped Alkali Laser (TPAL) that lases at 420 nm and 5.2 mum. Additionally, optically pumped atomic rubidium lasers pumped in the blue satellite of the D2 line from the ground Rb-Ar or Rb-Kr collision pair to the dissociative B2 sum 1/2 produce laser emission at 780.2 nm. Lasing is achieved for the Rb-Ar system and 757.1 - 760.4 nm for the Rb-Kr system. Slope efficiencies exceed 0.25% using a heat pipe configuration. The gain is very high with photon build-up times of 1-3.7 ns.
Cross sections for inelastic transfer between the 82D3/2 and 82D5/2 fine-structure states in rubidium, induced in resonant collisions with ground-state Rb atoms, have been determined using an experimental method involving two-photon excitation of atomic fluorescence. Rubidium vapor in a fluorescence cell was irradiated with pulses of 641 nm radiation from a N2 laser-pumped dye-laser tuned to excite one of the 82D states. The resulting fluorescence included the direct component originating from the optically excited state and a sensitized component arising from the other fine-structure state populated by collisions. Relative intensities of the fluorescent components, determined by photon-counting techniques, yielded the cross sections for excitation transfer: Q(2D3/2 → 2D5/2) = 8.1 × 10−13 cm2; Q(2D3/2 ← 2D5/2) = 5.5 × 1013 cm2; as well as [Formula: see text], the effective quenching cross section. The excitation transfer cross sections which are considered accurate to within ±20% are in the ratio predicted by the principle of detailed balancing.
The goal of this experiment was to measure the hyperfine energy splittings of the ground to first excited state transitions in rubidium using saturated absorption spectroscopy. Using this technique, we measured these transition energy spectra by taking the difference of two photodiode outputs due to multiple beams of a single laser scanned over a range of frequencies and shone through a cell of Rb vapor. When the laser frequency was resonant with an atomic transition, photons of those frequencies were absorbed, leaving a dip in intensity of the beam measured at the photodiode. One of the two laser beams had its excitations saturated by a more intense, counter-propagating pump beam from the same laser. The pump beam saturated the absorption of the velocity equal zero atoms that the counter-propagating probe beam could have also interacted with due to no Doppler shift. At these frequencies the probe beam experienced less absorption that was measured by a photodiode. The photodiode output was calibrated to the change in frequency of the scanned laser using a Fabry-Pérot interferometer. The output of this interferometer served as a reference for how the laser frequency changed. Final results for the 87Rb F=1 spectrum accounted for the largest error with a maximum of 12.2% deviation from accepted energy spacing values due in part to systematic error. Other spectra measurements were in better agreement, possessing error ranging from 2.1% to 10.1% and some agreeing with accepted values to within our uncertainty.
We report the first CW lasing from two-photon pumping via a virtual state. Pulsed and the CW lasing of the 3096 nm 72 P1/2 to 72 S1/2 line are observed from degenerate two-photon pumping of the cesium 72 S1/2 to 62 D3/2 transition. High intensity pulses excite over 17 lasing wavelengths. Under lower intensity CW excitation, 3 μm lasing is still observed with efficiencies of 0.7%. CW experiments utilized a Cs heat pipe at 150 °C to 270 °C, and a highly-focused, single pass, Ti-Sapphire pump with no aid of a cavity. Unlike normal DPALS, this architecture does not require buffer gas, and heat is released optically so a flowing system is not required. Both suggest a very simple device with excellent beam quality is possible. This proof of concept can be greatly enhanced with more optimal conditions such as non-degenerate pumping to further increase the two-photon pump cross section and the addition of a cavity to improve mode volume overlap. These improvements may lead to an increase in efficiencies to a theoretical maximum of 14%. Results suggest two-photon pumping with diodes is feasible.
An ongoing spectroscopic investigation of atomic rubidium utilizes a two-photon, single-laser excitation process. Transitions accessible with our tunable laser include 5P1/2 (F ′ ) ← 5S1/2 (F) and 5P3/2 (F ′ ) ← 5S1/2 (F). The laser is split into a pump and probe beam to allow for Doppler-free measurements of transitions between hyperfine levels. The pump and probe beams are overlapped in a counter-propagating geometry and the laser frequency scans over a transition. Absorption, fluorescence and polarization spectroscopy techniques are applied to this basic experimental setup. The temperature of the vapor cell and the power of the pump and probe beams have been varied to explore line broadening effects and signal-to-noise of each technique. This humble setup will hopefully grow into a more robust experimental arrangement in which double resonance, two-laser excitations are used to explore hyperfine state changing collisions between rubidium atoms and noble gas atoms. Rb-noble gas collisions can transfer population between hyperfine levels, such as 5P3/2 (F ′ = 3) Collision ←− 5P3/2 (F ′ = 2), and the probe beam couples 7S1/2 (F ′′ = 2) ← 5P3/2 (F ′ = 3). Polarization spectroscopy signal depends on the rate of population transfer due to the collision as well as maintaining the orientation created by the pump laser. Fluorescence spectroscopy relies only on transfer of population due to the collision. Comparison of these techniques yields information regarding the change of the magnetic sublevels, mF , during hyperfine state changing collisions.
We propose and demonstrate pump-probe spectroscopy of rubidium absorption that reveals the sub-Doppler hyperfine structure of the ${}^{5}{\mathrm{S}}_{1/2}\ensuremath{\leftrightarrow}{}^{5}{\mathrm{P}}_{3/2}$ (D2{\mathrm{D}}_{2}D2​) transitions. The counterpropagating pump and probe lasers are independently tunable in frequency, with the probe operating at the single-photon level. The two-dimensional spectrum measured as the laser frequencies are scanned shows fluorescence, Doppler-broadened absorption dips, and sub-Doppler features. The detuning between the pump and probe lasers allows compensation of the Doppler shift for all atomic velocities in the room-temperature vapor, meaning we observe sub-Doppler features for all atoms in the beam. We detail a theoretical model of the system that incorporates fluorescence, saturation effects, and optical pumping and compare this with the measured spectrum, finding a mean absolute percentage error of 3.11%. This high level of agreement allows us to extract the number density and temperature of the Rb\mathrm{Rb}Rb vapor from the two-dimensional spectrum. In the future this technique could be used as an atomic frequency standard for calibrating and characterising a single-photon or low-light-level source.