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Applied Physics Letters

Four level, atomic Cs laser at 852.1 nm with a quantum efficiency above 98%: Observation of three body photoassociation

Jason D. Readle, James Gary Eden, J. T. Verdeyen, David L. Carroll

Published Jul 12, 2010• 33 citations
Publisher

Abstract

Lasing on the D2 (6p P23/2→6s S21/2) transition of atomic Cs at 852.1 nm has been observed with a four level system in which the Cs 6p P23/2 state is pumped by the photoassociation and subsequent dissociation of Cs-rare gas collision pairs. Characterized by a quantum efficiency >98%, this laser requires no atomic precursor to the upper laser level and provides oscillation on an alkali transition inaccessible to three level, photopumped alkali laser systems. Measurements of photoabsorption and pump energy threshold in Cs–Ar–Kr mixtures reveal the influence of three body photoassociation.

DOI
10.1063/1.3452338

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Lasing on the D2 (6p P23/2→6s S21/2) transition of atomic Cs at 852.1 nm has been observed with a four level system in which the Cs 6p P23/2 state is pumped by the photoassociation and subsequent dissociation of Cs-rare gas collision pairs. Characterized by a quantum efficiency >98%, this laser requires no atomic precursor to the upper laser level and provides oscillation on an alkali transition inaccessible to three level, photopumped alkali laser systems. Measurements of photoabsorption and pump energy threshold in Cs–Ar–Kr mixtures reveal the influence of three body photoassociation.
Photoassociation of alkali-rare gas atomic collision pairs provides an alternative approach to optically pumping atomic alkali lasers. Lasing on the 6 P21/2→6 S21/2 (D1) transition of Cs has been observed when the blue satellite of the 6 P23/2←6 S21/2 (D2) transition, peaking at ∼837 nm for mixtures of Cs vapor, Ar, and ethane, is pumped by a pulsed dye laser. For 50% output coupling, laser threshold with respect to absorbed pump energy is ∼40 μJ at T=435 K and the slope efficiency approaches 10%. The measured spectral breadth for the blue satellite (≳5 nm at 410 K) will accommodate cw pumping of the Cs laser with conventional semiconductor lasers.
Lasing on the D(1) transition (6P1/22-->6S1/22) of Cs has been observed by photoassociating Cs-Kr atomic pairs with a tunable, pulsed dye laser. Pumping of the blue or red satellites of the Cs D(2) line (62P3/2<==>62S1/2), peaking at approximately 841.1 nm and approximately 853 nm (respectively) in Cs/Kr/C(2)H(6) gas mixtures, provides a photodissociation laser in which the CsKr excimer parent molecule is not, at any point in the pumping process, in a bound electronic state. Relative to the absorbed pump pulse energy, laser slope efficiencies greater than or approximately 5% have been measured when the Cs number density is in the range of 5x10(14)-1.5x10(15) cm(-3) and the pump wavelength is 841.1 nm. Direct photoexcitation of the Cs 6P3/22 state at 852.1 nm under these conditions is a less efficient pathway for pumping the 894.3 nm laser, presumably as a result of competing nonlinear optical processes such as 1+2 resonantly enhanced multiphoton ionization of the alkali atom.
Lasing on the 62P1/2→62S1/2(D1) resonance transition of atomic Cs at 894.3 nm has been demonstrated in mixtures of Ar, ethane, and Cs vapor by the photoexcitation of ground state Cs-Ar collision pairs and subsequent dissociation of diatomic, electronically-excited CsAr molecules (exciplexes or excimers). The blue satellites of the alkali D2 lines provide a pathway for optically pumping atomic alkali lasers on the principal series (resonance) transitions with broad linewidth (>2 nm) semiconductor diode lasers. In this paper we discuss different variations of this new laser system and the experiments of the initial demonstration.
Optical amplification by the stimulated emission of Cs(6p 2P3/2)-Ar atomic pairs, observed in pump-probe experiments over a ∼290 GHz-wide spectral region lying to the red of the Cs D2 line (852.1 nm), has been realized by photoexciting thermalized, ground state Cs-Ar atoms in the 834-849 nm wavelength interval. When the gain medium is pumped at the peak of the CsAr B2Σ1/2+←X2Σ1/2+ transition at 836.7 nm, maximum gain occurs between 852.2 nm and 852.3 nm and >28% of the energy stored in the upper laser level is extracted with 8 ns (FWHM) probe pulses in a single pass. From the measured rate of saturation of the extracted pulse energy with increasing probe intensity, the product of γ0L and Esat, the saturation pulse energy, is measured directly to be 400 ± 20 µJ and the lower limit for the saturation intensity (Isat) of this amplifier is estimated to be 10 kW-cm−2 at 852.2 nm. Circularly polarizing the optical pump beam increases the optical-to-optical conversion efficiency by 20%, and the storage lifetime of the upper laser level is observed from temporally-resolved gain spectra to be 5 ± 1 ns. Pump excitation spectra also reveal a significant contribution from Ar-Cs-Ar (3-body) photoassociation and suprathermal Ar atoms generated by the dissociation of the CsAr B2Σ1/2+ complex. Multipass-amplifier geometries with broad-bandwidth probe signals are expected to yield upper state energy extraction efficiencies above 50%. This alkali-rare gas amplifier demonstrates the efficiencies available with the storage of energy in, and optical extraction from, excited atomic collision pairs.