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HAL Id: jpa-00224491

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Submitted on 1 Jan 1985

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COLLISIONAL IONISATION OF EXCITED RUBIDIUM ATOMS

M. Chéret, L. Barbier

To cite this version:

M. Chéret, L. Barbier. COLLISIONAL IONISATION OF EXCITED RUBIDIUM ATOMS. Journal

de Physique Colloques, 1985, 46 (C1), pp.C1-193-C1-197. �10.1051/jphyscol:1985119�. �jpa-00224491�

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JOURNAL DE PHYSIQUE

Colloque C l , suppl6ment au nO1, Tome 46, janvier 1985 page Cl-193

COLLISIONAL IONISATION OF EXCITED RUBIDIUM ATOMS

M.

Ch&ret and

L .

Barbier

Centre drEtudes Nucl6aires de Saclay, Service de Physique des Atomes e t des Surfaces, 91 191 Gif-sur-Yvette Cedex, France

R6sun6 - -Dans une vapeur de rubidium,la n e s u r e des c o u r a n t s d ' i o n s Rb+, Rb+ e t Rb a ~ e r m i s de c a r a c t z r i s e r l e s processus c o l l i s i o n n e l s de forma- t i o n d ' i o n s 2 b p a r t i r d'atomes e x c i t e s e t de determiner l e s c o e f f i c i e n t s de t a u x d ' i o n i s a t i o n a s s o c i 6 s b c e s r e a c t i o n s .

+ +

A b s t r a c t - Ion c u r r e n t measurements f o r Rb , Rb and Rb- i o n s allowed t o c h a r a c t e r i z e i o n i z i n g c o l l i s i o n a l p r o c e s s e s i n v o l v i n g e x c i t e d atoms i n a 2 Rb vapour. Rate c o e f f i c i e n t s f o r t h e s e r e a c t i o n s a r e d e t e r n i n e d .

When an a l k a l i vapor i s i r r a d i a t e d with high power l a s e r beams a complex medium i s c r e a t e d and it i s not very e a s y t o s e p a r a t e l a s e r f i e l d s e f f e c t s from p u r e l y c o l l i - s i o n a l mechanisms. It i s t h u s important t o understand f i r s t t h e involved c o l l i s i o n a l r e a c t ions.

Low power l a s e r s allow t o s t u d y t h i s p r o c e s s e s i n a s i n p l e medium.

Two C.W. multimode dye l a s e r s c r o s s i n g a t t h e c e n t r e of a c y l i n d r i c a l c e l l a r e used t o pump , i n a f i r s t s t e p rubidium atoms i n a r e s o n a n t l e v e l Rb(5p) and i n a second s t e p i n a h i g h l y e x c i t e d l e v e l ~ b ( n ' L ) ( I = s o r d ) . The experimental s e t up has been d e s c r i b e d p r e v i o u s l y / l 1. Typical experimental c o n d i t i o n s correspond t o :p=l 0-4 T o r r ,

Rb(5s)=lO l 2 cm-3, Rb(5d)

=

10 cm-3, Rb ( n l ) = 10' c n 3 . The main p r o c e s s e s a r e :

liornbeclc-blolnar a s s o c i a t i v e i o n i z a t i o n

Rb(nZ)+ Rb(5s)-Rb; + e-

Penning atomic i o n i z a t i o n

:

Beside t h e s e r e a c t i o n s t h e follorving p r o c e s s e s have a l s o been observe0 : Energy p o o l i n g r e a c t i o n :

Peqning a s s o c i a t i v e i o n i z a t i o n :

Ion p a i r formation

R e s u l t s concerning energy pooling r e a c t i o n have been published f o r t h e Rb case / 2 / and M. A l l e g r i n i p r e s e n t s a review on t h i s s u b j e c t a t t h e p r e s e n t conference.

The o t h e r r e a c t i o n s correspond t o i o n i z i n g mechanisms i n v o l v i n g h i g h l y e x c i t e d Rb atoms. Ions a r e analyzed w i t h a mass spectrometer wired t o a l t e r n a t e l y d e t e c t e d po- s i t i v e - o r n e g a t i v e i o n s . A t y p i c a l r e s u l t of mass scanping i s p r e s e n t e d i n f i g . 1 . The Rb c u r r e n t i s 5000 t i n e s lower t h a n t h e Rb+ o r Rb 2 c u r r e n t and consequently ion p a i r formation does n o t c o n t r i b u t e s i g n i f i c a n t l y t o t h e Rb+ c u r r e n t . Photoionisa- t i o n by t h e l a s e r beams : Rb(n1) + h*--+RbC + e- i s an important mechanism c o n t r i - b u t i n g t o t h e Rb+ c u r r e n t . The c r o s s s e c t i o n s f o r t h i s p r o c e s s a r e w e l l known /3/

and t h e p h o t o i o n i s a t i o n c o n t r i b u t i o n i s used t o d e t e r n i n e d t h e e x c i t e d s t a t e densi- t i e s / l / .

Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphyscol:1985119

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c l - 1 9 4 JOURNAL DE PHYSIQUE

I

R E L . U N I T

t

The p r e s e n t paper only r e p o r t s on Penning a t o n i c i o n i s a t i o n and i o n p a i r format i o n .

The Penning i o n i z a t i o n occurs v i a c o l l i s i o n between a h i g h l y e x c i t e d atom and a r e s o n a n t s t a t e atom.

I n f a c t when a h i g h l y e x c i t e d s t a t e i s pumped t h e r a d i a t i v e cascading d e e x c i t a t i o n p o p u l a t e s t h e neigh- bouring l e v e l s . s and d l e v e l s es-

s e n t i a l l y decay t o p l e v e l s and consequently t h e s t u d i e d medium i s composed of che e x c i t e d s o r d le-.

v e l and of t h e v a r i o u s lower p l e v e l s . The t o t a l d e n s i t y of t h e s e p l e v e l s r e p r e s e n t s 80% of t h e den- s i t y of t h e pumped s l e v e l and 2CX of t h e pumped d l e v e l . The mea- sured q u a n t i t i e s correspond t o t h e c o n t r i b u t i o n of t h e pumped s t a t e and of t h e r a d i a t i v e l y populated p l e v e l s . t h e n a s s t a t e i s populated t h e p l e v e l d e n s i t i e s a l o n e can e x p l a i n t h e e x p e r i n e n t a l observa- t i o n s / l / - I dependency of t h e r a t e c o e f f i c i e n t s w i l l be known only i f t h e p c o n t r i b u t i o n i s c o r r e c t l y deduced.

Measured r a t e c o e f f i c i e n t s l i e i n t h e range 10-8 cm3 s - l . T h e o r e t i c a l - l y two mechanisms a r e u s u a l l y consi- Fig. l - Mass scanning of p o s i t i v e ( a ) and dered. The f i r s t one i s t h e d i p o l e - n e g a t i v e ions f o r t h e e x c i t a t i o n of t h e d i p o l e i n t e r a c t i o n which g i v e r a t e 6d 2 ~ l e v e l . ~ / ~ c o e f f i c i e n t s i n t h e range 10-9 a d s - l

f o r d o r p l e v e l s and i n t h e range 10-1

0

cm3 s-l f o r s l e v e l . The second one i s t h e exchange t h e o r y ; Kimura f o r Rb atoms found r a t e c o e f f i c i e n t s 1 i n - dependent lying i n t h e range 10-8 cm3 s-l 141. It i s t h e n important t o determine t h e

1

dependency of t h e Penning r a t e c o e f f i c i e n t .

T h i s h a s been done by p o p u l a t i n g t h e e x c i t e d s t a t e s w i t h p u l s e d l a s e r s . As an exam- p l e i f t h e 7 s l e v e l i s e x c i t e d i t s c o n c e n t r a t i o n decays e x p o n e n t i a l l y and p o p u l a t e s t h e 6p l e v e l . 200 n s a f t e r t h e l a s e r s h o t t h e 6p d e n s i t y becomes h i g h e r t h a n t h e 7 s d e n s i t y ( f i g . 2 ) . I f oile of t h e Penning r a t e c o e f f i c i e n t f o r 7 s o r 6d l e v e l i s s t r o n g l y predominant t h e ~ b + c u r r e n t w i l l vary a s t h e 7s o r a s t h e 6p d e n s i t y . I f t h e two l e v e l s have e q u a l r a t e c o e f f i c i e n t s t h e Rb+ c u r r e n t w i l l t h e n decay a s t h e sum of t h e 7 s and 6d d e n s i t i e s . Experimental v a r i a t i o n ( p o i n t s f i g . 2 ) accounts f o r t h i s l a s t hypothesis. The same r e s u l t s have been obtained when t h e 5d, 6d o r 8 s

l e v e l i s e x c i t e d : e x p e r i m e n t a l r e s u l t s c l e a r l y show t h a t t h e Penning r a t e c o e f f i - c i e n t i s l i n d e p e n d e n t . The r a t e c o e f f i c i e n t s o b t a i n e d with t h e C.N. system t h e n can be c o r r e c t e d from cascading r a d i a t i v e mechanisms. The r e s u l t s a r e p r e s e n t e d i n f i g . 3 t o g e t h e r with t h e d i p o l e - d i p o l e c a l c u l a t i o n s f o r s ( x ) , p ( o ) , d ( + ) l e v e l s and Kimura's c a l c u l a t i o n s

( 0 )

f o r l e v e l s 6d, 8 s and 7d.

A s p r e s e n t e d i n f i g . 1 mass scanning of n e g a t i v e i o n s i n d i c a t e s t h e presence of a low Rb- c u r r e n t . Molecules a r e commonly considered a s r e s p o n s i b l e f o r n e g a t i v e i o n formation 151, t h e main r e a c t i o n s being :

Rb, + e -Rb(5s) + ~ b -

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l d e n s i t i e s

( R . L . U ~ T )

F i g . 2 - E x c i t a t i o n of t h e 7 s l e v e l . Tine v a r i a t i o n of t h e 7s and 6p d e n s i t i e s calcu-

l a t e d with measured l i f e t i m e , Experimental p o i n t s deduced from t h e ~ b + c u r r e n t .

Fig.3 - Rate c o e f f i c i e n t f o r Penning i o n i z a t i o n k a g a i n s t t h e e f f e c t i v e quantum number n* of

p i

t h e e x c i t e d s t a t e .

Under our experimental c o n d i t i o n s ( c e l l temperature 4 5 0 ' ~ ) t h e r a t i o between t h e dimer d e n s i t y and t h e atom d e n s i t y i s e q u a l t o 4 x 1 0 - ~ Experimental checks show t h a t : - n e g a t i v e i o n f o r n a t i o n r e q u i r e s both l a s e r s t o be r e s o n a n t . - n e g a t i v e i o n c u r r e n t does n o t vary when t h e Rb2 c o n c e n t r a t i o n i s i n c r e a s e d by a f a c t o r of 10 (by v a r y i n g t h e c e l l temperature a t

c o n s t a n t Rb p r e s s u r e ) .

- n e g a t i v e i o n c u r r e n t v a r i e s l i n e a r l y w i t h b o t h l a s e r powers.

These o b s e r v a t i o n s r u l e o u t r e a c - t i o n s i n v o l v i n g any of t h e f o l l o - wing p a r t i c l e s

:

molecules, mole- c u l a r i o n s , photons, e l e c t r o n s . Ion p a i r formation by a c o l l i s i o n between a h i g h l y e x c i t e d atom and a ground s t a t e atom, namely Rb(n1) + Rb(5s) Rb'

+

~ b -

i s a r e a c t i o n t h a t f u l l f i l l s a l l our experimental checks. T h i s r e a c t i o n i n v o l v e s t h e same p a r t n e r s Rb(n1) and Rb(5s) than t h e Hornbeck- Molnar a s s o c i a t i v e i o n i z a t i o n . The r a t e c o e f f i c i e n t f o r i o n p a i r f o r - n a t i o n , nk-(nl) , can be deduced from t h e r a t e c o e f f i c i e n t f o r as- s o c i a t i v e i o n i z a t i o n kAI(nl) by comparing t h e n e g a t i v e Ion c u r r e n t I(Rb-) t o t h e molecular i o n c u r r e n t I(Rb3) :

When t h e 6d D ' l e v e l i s e x c i t e d ,

0

b e t - t h e c e l l terape?&ure varyin, ween 383°K and 4 5 3 O ~ a t c o n s t a n t Rb p r e s s u r e , t h e k-(6d) v a l u e s , r e p o r t e d on f i g . 4 a r e measured. As t h e e l e c t r o n a f f i n i t y of t h e Rb atom is e q u a l t o 3919.2

t h e r e a c t i o n i s e x o e r g i c by 1082.4 cm-l f o r t h e 6d 2 ~ l e v e l . The ~ , ~ experimental v a l u e s of t h e r a t e c o e f f i c i e n t can be f i t t e d with a c r o s s s e c t i o n Q - e q u a l t o 1.3

X

10-1 6 m 2 above t h e t h r e s h o l d and e q u a l t o z e r o below t h i s l i m i t and w i t h a maxwellian v e l o c i t y d i s t r i - b u t i o n f ( v ) being assumed, leading

t o

W

k-

=

v ~ ( v ) dv.

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JOURNAL DE PHYSIQUE

Fig.4 - k-(6d 2 D5,2) a g a i n s t c e l l temperature - .

experimental p o i n t s

-16 2 f i t t e d curve w i t h - = I .3x10 cm .

{E

cm"

-f

- - - - --- -

I Sd

2s

ooa . . - -

100 ZOO 300

R a . ~

+ -

Fig.5 - Rb , Rb coulonbic curve c a l c u l a t e d - 1 w i t h an e l e c t r o n a f f i n i t y e q u a l t o 391 9 . 2 cm .

T h i s c r o s s s e c t i o n v a l u e i s not theore- t i c a l l y e x p l a i n e d . A Landau-Zener c a l c u l a - t i o n /5/ a t t h e cros- s i n g p o i n t between t h e unperturbed ato- mic curve and t h e coulombic Rb+, Rb- i o n p a i r curve ( f i g . 5) g i v e a n e g l i g i b l e con- t r i b u t i o n : i t i s n o t s u r p r i s i n g a s t h e c r o s s i n g p o i n t (203 a.u) i s passed diaba- t i c a l l y .

Negative i o n c u r r e n t neasurements have been performed on l e - v e l s l y i n g e n e r g e t i c a l

l y under (.5d, 7 s , 6d, 8 s ) o r above (7d, 9s) t h e ~ b + , Rb- l i m i t . I n f i g . 6 a r e p l o t t e d t h e k-(n\) v a l u e s a g a i n s t t h e energy d e f e c t of t h e r a c t i o n . The corresponding

c r o s s s e c t i o n a r e r e p o r t e d i n f i g . 7 . As f o r t h e 6d l e v e l t h e Landau- Zener c a l c u l a t i o n a t t h e c r o s s i n g p o i n t between t h e atomic curve and t h e i o n i c curve does n o t e x p l a i n t h e s e r e s u l t s f o r l e v e l s under t h e Rb", Rb- l i m i t . For l e v e l s above such a c a l c u l a t i o n i s n o t p o s s i b l e . More s o p h i s t i c a t e d theo- r e c t i c a l approaches a r e t h e n nee- ded. One may c o n s i d e r c r o s s i n g p o i n t s a t s h o r t e r d i s t a n c e s o b t a i - ned by s p l i t t i n g t h e e x c i t e d l e v e l

/6/ o r by manifold c r o s s i n g s i n t h e molecular system ( f i g . 8 ) . Another p o s s i b i l i t y i s a d e l o c a l i - sed c a l c u l a t i o n a s a p p l i e d by S i d i s /7/ t o t h e H+, H- system. ( f i g . 9 ) These v a r i o u s methods r e q u i r e f i r s t t h e knowledge of t h e molecular p o t e n t i a l curves.

For t h e f i r s t time i o n p a i r f o r n a t i o n have been observed i n an e x c i t e d vapor. As

t h e e x i t . channel f o r t h e r e a c t i o n ( i . e . t h e Coulombic ~ b + , Rb- curve) is w e l l

known t h i s process appears a p p e a l i n g t o check t h e o t h e r involved molecular poten-

t i a l curves.

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Fig. 6 F i g . 7

r a t e c o e f f i c i e n t ( f i g . 6 ) and c r o s s s e c t i o n ( f i g . 7 ) f o r i o n p a i r f o r n a t i o n v e r s u s t h e energy d e f e c t of t h e r e a c t i o n .

Fig.8 - (a) s p l i t t i n g of t h e a t o n i c curve F i g . 3 - D e l o c a l i s e d schene i n (b) c r o s s i n g i n t h e n o l e c u l a r system. t h e n o l e c u l a r s y s t e n .

R e f e r e n c e s

/ l / CHERET M . , BARBIER L . , LINDINGER W. and DELOCHE R., J. Phys. B . E ( l 9 8 2 ) 3463 / 2 / BARBIER L., CHERET M . , J . Phys. B16 (1 983) 3213.

1 3 1 AYMAR M., ROBAUX and WANE S., J. P h y s . B E (1984) 993.

I 4 1 KIMURA M. and OLSON R.E., 1 3 t h I. C. P. E.A. C. B e r l i n (1 983) 662.

/ 5 1 SMIRNOV B.M., Negative i o n s

MC

Graw H i l l ed. (1 982).

I 6 1 FREY P . , BREYER F. and HmOP H., J. P h y s . B E (1978) L589.

171 OLSON R.E., SMITH F.T. and BAUER E., Appl. Opt. 10 (1971) 1848.

/ 8 / KOWALCZYZ P . , J. Phys.B E (1 984) 817.

/ g / SIDIS V . , KUBACH C. and FUSSEAU D . , Phys. Rev. A ( 1 983) 2431.

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