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Physical Review A

Ionization, excitation of high-lying atomic states, and molecular fluorescence in Cs vapor excited at λ =455.7 and 459.4 nm

John Huennekens, Z. Wu, Thad G Walker

Published Jan 1, 1985• 49 citations
Publisher

Abstract

We have studied in detail the ionization and population of high-lying atomic states which occur in cesium vapor excited at the second resonance transition, 6S-7P. We have developed a simple model which qualitatively explains the laser-power dependences of level populations and electron densities which we observed. Measurements of spatial dependences of fluorescence point out the critical role of radiation trapping in these phenomena. Similar observations on rubidium demonstrate the same type of behavior when the first (5S-5P) or second (5S-6P) resonance is excited. At higher densities and temperatures we found that the fluorescence was dominated by diffuse molecular bands. Some of these bands probably consist of transitions to the repulsive $^{3}\mathrm{\ensuremath{\Sigma}}_{\mathrm{u}}^{+}$ state. Additionally four bands observed at 817.5, 826.6, 835.3, and 839.6 nm are tentatively identified as the cesium analog of the $^{3}\mathrm{\ensuremath{\Pi}}_{\mathrm{g}}$${\ensuremath{\rightarrow}}^{3}$${\mathrm{\ensuremath{\Sigma}}}_{\mathrm{u}}^{+}$ satellite bands which have previously been observed in the blue wing of the first resonance doublet of the lighter alkali metals.

DOI
10.1103/physreva.31.196

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Using selective stepwise excitation of the cesium 8S atomic level in Cs vapor, the collisional transfer and the population of the high-lying atomic states were studied in detail. At cesium densities of 10(16)-10(17) cm(-3), the rate coefficient of excitation collision [i. e., 8S+6S --> 6D+6S] was measured. Measurement of fluorescence intensities as a function of Cs density yields k6D = (2.4 +/- 0.5) x 10(-10) cm3 x s(-1). The 5D state was populated by the 8S --> 7P --> 5D transitions. The energy pooling collisions 5D+5D --> nL+6S (nL = 9D, 11S, 7F) were also studied. The rate coefficients were measured relative to the known rate coefficient of the collision [i. e. 6P+5D --> 6S+7D]. The densities of 6P state were combined with measured fluorescence ratios to determine rate coefficients for EP process. The average values (in unites of 10(-10) cm3 x s(-1)) for nL = 9D, 11S and 7F are 6.4 +/- 3.2, 1.0 +/- 0.5 and 8.4 +/- 4.2, respectively.

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Using stepwise excitation of the cesium 8S atoms level in Cs vapor,several collisional and radiative processes have been identified from the intensities and spectra of the Cs fluorescence.The 5D state was populated by 8S→7P→5D transitions.In cesium densities 1016-1017?cm-3,the energy pooling collisions 5D+5D→nL+6S(nL=9D,11S,7F are studied.Since the 5D→6P(3.0-3.6 μm) fluorescence could not be detected with this experiment,the EP rate coefficients have been measured relative to the known rate coefficient of the collision,i.e.,6P+5D→6S+7D.The excited-atom density and spatial distribution were mapped by monitoring the absorption of a counterpropagating single-mode laser beam,tuned to 6P3/2→8S1/2 transition,which could be translated parallel to the pump beam.The excited atom densities are combined with measured fluorescene ratios to determine cross sections for the cesium energy pooling process.The average values(in units of 10-10?cm3s-1) for nL=9D,11S and 7F are 8.4±4.2,7.3±3.6,and 9.7±4.8,respectively.Influence on k11S and k7F of the energy transfer process 11S+6S7F+6S is also dicussed.

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The population and deactivation processes of the first excited 2S and 2D levels of alkali atoms have not been the focus of extensive attention to date, since these levels do not have dipole transitions to the 2S ground state, and the only radiative transitions to the 2p resonance level lie in the IR ( 1-3 fLm). We have demonstrated that in the case of potassium it is possible to populate the 32D and 52S levels in socalled optical collisions by laser excitation of the vapor and also by excitation energy transfer (EET) from the laser-excited Kidimers. 1 The lines of the corresponding 4D--->5P (1.529/1.475 f.lm and 6S ---> 5P (1.367/1.324 f.lm) transitions have also been identified in the laser-induced fluorescence of rubidium vapor,2 although the population mechanism of the levels is not examined in the present study. This st~dy will focus on determining the processes that result in the population of the Rb 42D and 62S levels and to determining the rate constants of these1'rocesses. The spectrum of the LGN-402 argon laser-induced fluorescence of Rb vapors was recorded in the IR by cooled Ge photo diodes selected for IR sensitivity and configured along the outlet slit of an MDR-3 monochromator. The synchronous detection method was employed. A FEU-79 photomultiplier was used in the visible range. Details on the experimental setup can be found in Ref. 3. The Rb vapor was excited by various argon laser lines (514.5-476.5 nm), although the 5l4.5-nm line was of primary interest. The C 1 ITu state of the RB2 dimer is not populated by this laser line; its predissociation efficiently populates the 52P resonance levels4 (see Fig. 1). Moreover the 5l4.5-nm laser line is closer in energy to the Rb 5S--->4D quadrupole transition (M= 75 cm-I). In the experiment at an atomic concentration [Rb] _1016 cm-3 the fluorescence lines from the 62S level (2.5 eV) were weaker by a factor of 50 compared to the lines from the 42D level (2.4 eV). A transition to the shorterwavelength laser excitation lines causes a certain increase in the population efficiency of the 4D level, although it also results in a more rapid growth of the population of the 5P resonance level due to the predissociation of Rb2 (C 1IT u ). I. In pure Rb vapors I) the line intensity of the 4D---> 5P transition has a linear relation to the laser excitation power ,(514.5 nm andp 5X 1016 cm-3 can be attributed to the onset of collisional quenching of the RB 4D state ('Trad =90 nsec). 5 So-called opticaJ.collisions lead to the population of the 4D level in these conditions (Aexc = 514.5 nm and no Na impurities)

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Collision induced fluorescence in Cs vapor excited by a laser diode

M. Allegrini, F. De Tomasi, Slobodan Milošević +1 more

Two experiments on cesium vapor at relative low number densities (≊1010÷1013 cm−3), excited at the first resonance transition 6S1/2→6P3/2 (λ=852 nm) by a cw laser diode are reported. We have measured the rate coefficients at thermal energies for the energy pooling to the 7P levels. In presence of Ne as buffer gas we have observed a striking distortion of the line‐shape.

AIP conference proceedings•Jan 1, 1993•3 citations
We have studied in detail the ionization and population of high-lying atomic states which occur in cesium vapor excited at the second resonance transition, 6S-7P. We have developed a simple model which qualitatively explains the laser-power dependences of level populations and electron densities which we observed. Measurements of spatial dependences of fluorescence point out the critical role of radiation trapping in these phenomena. Similar observations on rubidium demonstrate the same type of behavior when the first (5S-5P) or second (5S-6P) resonance is excited. At higher densities and temperatures we found that the fluorescence was dominated by diffuse molecular bands. Some of these bands probably consist of transitions to the repulsive 3\ensuremathΣu+^{3}\mathrm{\ensuremath{\Sigma}}_{\mathrm{u}}^{+}3\ensuremathΣu+​ state. Additionally four bands observed at 817.5, 826.6, 835.3, and 839.6 nm are tentatively identified as the cesium analog of the ^{3}\mathrm{\ensuremath{\Pi}}_{\mathrm{g}}$${\ensuremath{\rightarrow}}^{3}$${\mathrm{\ensuremath{\Sigma}}}_{\mathrm{u}}^{+} satellite bands which have previously been observed in the blue wing of the first resonance doublet of the lighter alkali metals.
Using selective stepwise excitation of the cesium 8S atomic level in Cs vapor, the collisional transfer and the population of the high-lying atomic states were studied in detail. At cesium densities of 10(16)-10(17) cm(-3), the rate coefficient of excitation collision [i. e., 8S+6S --> 6D+6S] was measured. Measurement of fluorescence intensities as a function of Cs density yields k6D = (2.4 +/- 0.5) x 10(-10) cm3 x s(-1). The 5D state was populated by the 8S --> 7P --> 5D transitions. The energy pooling collisions 5D+5D --> nL+6S (nL = 9D, 11S, 7F) were also studied. The rate coefficients were measured relative to the known rate coefficient of the collision [i. e. 6P+5D --> 6S+7D]. The densities of 6P state were combined with measured fluorescence ratios to determine rate coefficients for EP process. The average values (in unites of 10(-10) cm3 x s(-1)) for nL = 9D, 11S and 7F are 6.4 +/- 3.2, 1.0 +/- 0.5 and 8.4 +/- 4.2, respectively.
Using stepwise excitation of the cesium 8S atoms level in Cs vapor,several collisional and radiative processes have been identified from the intensities and spectra of the Cs fluorescence.The 5D state was populated by 8S→7P→5D transitions.In cesium densities 1016-1017?cm-3,the energy pooling collisions 5D+5D→nL+6S(nL=9D,11S,7F are studied.Since the 5D→6P(3.0-3.6 μm) fluorescence could not be detected with this experiment,the EP rate coefficients have been measured relative to the known rate coefficient of the collision,i.e.,6P+5D→6S+7D.The excited-atom density and spatial distribution were mapped by monitoring the absorption of a counterpropagating single-mode laser beam,tuned to 6P3/2→8S1/2 transition,which could be translated parallel to the pump beam.The excited atom densities are combined with measured fluorescene ratios to determine cross sections for the cesium energy pooling process.The average values(in units of 10-10?cm3s-1) for nL=9D,11S and 7F are 8.4±4.2,7.3±3.6,and 9.7±4.8,respectively.Influence on k11S and k7F of the energy transfer process 11S+6S7F+6S is also dicussed.
The fluorescence spectrum of cesium vapor was studied in a cell irradiated with the light of 852.3 nm resonance line from a single mode laser diode. From the intensities and spectra of the Cs and Cs2 fluorescence we identified several collisional and radiative processes in the excited cesium atom-dimer system. The atomic lines of the highly excited states were the result of collisional energy transfer from Cs(6P 3/2) + Cs(6P 3/2) to Cs(6D, 8S) atoms. The Cs2 (B 1 IIu) band formed in Cs (6P) + Cs2 (X1sigmag+) collisions. The fine-structure mixing in 6 2P atoms was studied through excitation transfer, energy-pooling collision, and collisional excitation transfer between Cs2 and Cs. The authors estimated the value of rate coefficient for the collisional energy transfer from 6P3/2 to 6P1/2 to be (5.2+/-2.1) x 10(-11) cm3 x s(-1). For the excitation transfer process Cs2 (B 1 IIu)+ Cs(6S)--> Cs2 (X 1sigmag+) + Cs(6P1/2 ), a rate coefficient of (1.0+/-0.4) x 10(-9) cm3 x s(-1) was yielded.
Populations of the n 2L(nL=7p,6D)states of Cs atoms by photodissociation of Cs_2 molecules through the use of the fixed frequence line 441.6nm of a He-Cd laser radiation are produced.Combining ratios of atomic to molecular fluorescence at the Cs density range between 1 and 9×10 15 cm -3 ,the ratios of collisional excitation transfer rate coefficients and the predissociation rates are obtained.The cross section for the fine-structure-changing collision [i.e,Cs(7P_ 1/2 )+Cs(6S)Cs(7P_ 3/2 )+Cs(6S)]is 3.5×10 -14 cm 2.
The population and deactivation processes of the first excited 2S and 2D levels of alkali atoms have not been the focus of extensive attention to date, since these levels do not have dipole transitions to the 2S ground state, and the only radiative transitions to the 2p resonance level lie in the IR ( 1-3 fLm). We have demonstrated that in the case of potassium it is possible to populate the 32D and 52S levels in socalled optical collisions by laser excitation of the vapor and also by excitation energy transfer (EET) from the laser-excited Kidimers. 1 The lines of the corresponding 4D--->5P (1.529/1.475 f.lm and 6S ---> 5P (1.367/1.324 f.lm) transitions have also been identified in the laser-induced fluorescence of rubidium vapor,2 although the population mechanism of the levels is not examined in the present study. This st~dy will focus on determining the processes that result in the population of the Rb 42D and 62S levels and to determining the rate constants of these1'rocesses. The spectrum of the LGN-402 argon laser-induced fluorescence of Rb vapors was recorded in the IR by cooled Ge photo diodes selected for IR sensitivity and configured along the outlet slit of an MDR-3 monochromator. The synchronous detection method was employed. A FEU-79 photomultiplier was used in the visible range. Details on the experimental setup can be found in Ref. 3. The Rb vapor was excited by various argon laser lines (514.5-476.5 nm), although the 5l4.5-nm line was of primary interest. The C 1 ITu state of the RB2 dimer is not populated by this laser line; its predissociation efficiently populates the 52P resonance levels4 (see Fig. 1). Moreover the 5l4.5-nm laser line is closer in energy to the Rb 5S--->4D quadrupole transition (M= 75 cm-I). In the experiment at an atomic concentration [Rb] _1016 cm-3 the fluorescence lines from the 62S level (2.5 eV) were weaker by a factor of 50 compared to the lines from the 42D level (2.4 eV). A transition to the shorterwavelength laser excitation lines causes a certain increase in the population efficiency of the 4D level, although it also results in a more rapid growth of the population of the 5P resonance level due to the predissociation of Rb2 (C 1IT u ). I. In pure Rb vapors I) the line intensity of the 4D---> 5P transition has a linear relation to the laser excitation power ,(514.5 nm andp 5X 1016 cm-3 can be attributed to the onset of collisional quenching of the RB 4D state ('Trad =90 nsec). 5 So-called opticaJ.collisions lead to the population of the 4D level in these conditions (Aexc = 514.5 nm and no Na impurities)