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GASDYNAMIC LASERS : SPECTRAL REGION
EXTENDING AND EFFICIENCY INCREASlNG
E. Kudriavtsev
To cite this version:
JOURNAL DE PHYSIQUE CoZZoque C9, suppZdment a u n o l l , Tome 41, novembre 1980, page C9-189
.GASDYNAMIC LASERS : SPECTRAL REGION EXTENDING AND EFFICIENCY INCREASlNG E.M. Kudriavtsev
P.N. Lebedev PhysicaZ I n s t i t u t e o f t h e Academy o f S c i e n c e o f U.S.S.R., Noscow, U.S.S.R.
.
Abstract.- It is reviewed the suggested and realized heat pumped molecular GDL's that are lasing in different spectral regions from visible to submillimeter parts using different active molecules and transitions. These systems differ also by their efficiency that is increased the more the lower laser levels were used.
IN!CRODUCTION
P r e s e n t l y a C02-Gas Dynamic L a s e r
(C02-GDL) w i t h a l a s i n g wavelength of
J b ~
c\,10.6 mkm i s mostly known
/I-3/.
J u s tt h i s GDL was f i r s t r e a l i z e d /4-7/; t h e i n - v e s t i g a t o r s have payed most a t t e n t i o n t o t h i s l a s e r because of i t s very cheap and common a c t i v e mixture components (C02-N2- H20) which a r e a u t o m a t i c a l l y produced (he- a t e d up t o r e q u i r e d t e m p e r a t u r e s ) i n t h e a i r - f lame of u s u a l carbon-hy drogen f ue 1s
/a/.
Another a well-known l a s e r i s CO-GDL w i t h j l l a s ~ 4 . 6+
5.4mkm /9,10,2,3/.From t h e f i r s t works on h e a t pumped GDL ( t h e only type we s h a l l d i s c u s s i n t h i s b r i e f review) t h e p o s s i b i l i t i e s of l a s i n g w i t h t h e h e l p of a n o t h e r molecules were s t u d i e d . The n i t r o g e n m i x t u r e s w i t h B d d i t i o n of C02, R20 and CS2 were suggest-
ed i n t h e t h e o r e t i c a l work /II/. Authors of / I 2 / o b t a i n e d l a s i n g on C02 -N 2- He and
N20-If2-He mixturea. The p o i n t e d tendency
was developed l a t e r , It was t h e g o a l of such a r e s e a r c h t o use t h e main GDL advana , .
%ages: (I) s i g n i f i c a n t power g e n e r a t i o n in
b ~ ;
( 2 ) h e a t pumping: t h a t permit very d i f - r e r e n t methods of p r e h e a t i n g of t h e work-,pg
gas mixture i n c l u d i n g methods whichprovide t h e system's autonomy, independen-
pe
of
power aupply-. However,it
is' advisa;b l e t o hold t h e mentioned advantages a t t h e some time w i t h broad range
3
las Vary- i n g a c c o r d i n g t o t h e problems of s e l e c t i v e l i g h t - m a t t e r i n t e r a c t i o n ( l a s e r i s o t o p e s e p a r a t i o n ; l a s e r chemistry and s o o n ) ; t o t h e problems of t h e atmosphere energy t r a n s m i s s i o n improvements, e t c . A s soon a s we know t h e r e i s no any a p p r o p r i a t e meth-ods of
3
las changing f o r C02-GDL a t t h e r e a l i z e d power of MWf w i t h s u f f i c i e n t e f - f i c i e n c y and i n s p e c t r a l r e g i o n beyond v i b r a t i o n a l - r o t a t i o n a l s t r u c t u r e of C02. CO-GDL h a s r e l a t i v e l y b r o a d e r s p e c t r a i t u n i n g r e g i o n w i t h i n CO-vibrational bands (4.615.4mkm). T h e o r e t i c a l l y i t i s p o s s i b l e t o o b t a i n obertone l a s i n g , a s example f o r CO-GDL/I3/,
i t w i l l s h i f tj\
t o 2 . 3 i 2.7mkm r e g i o n . But t h i s method i s very s p e c i f i c , i t g i v e s only a b l u e , s $ F and h a s very low e f f i c i e n c y .A t p r e s e n t time t h e only method of GDL s i g n i f i c a n t
Alas
v a r i a t i o n i s a>
change of t h e l a s i n g molecule (N20, CS2, SO2 e t c . ) o r l a s i n g t r a n s i t i o n s ( a s f o r I 8 m k m C02-GDL
/I4/).
.
It i s very important t h a t a change :of l a s i n g molecule and working mixture l e - lads to's.ef f i c i e n c y changing of GDL known
!as a low e f f i c i e n c y l a a e r . Having t h e cha-
C9- 190 JOURNAL DE PHYSIQUE
nged l a s i n g molecules w i t h lower l e v e l s one can g e t , g e n e r a l l y s p e a k i n g , GDL e f f i - ciency i n c r e a s i n g , because of h i g h e r l e v e l p o p u l a t i o n s a t t h e same s t a g n a t i o n tempe- r a t u r e s . It i s reasonably t o develop t h i s method of GDL e f f i c i e n c y i n c r e a s i n g / I 5 / t o g e t h e r with a s e l e c t i v e l e v e l pumping method
/I6/
r e a l i z e d i n mixing GDL's sche- me ( s e e / I 2 / , / I 7 / , / I 8 / and review /I9/,).
Thus, t h e GDL s p e c t r a l r e g i o n extend- i n g i s a p p l i e d s o t h a t t h e l a s e r system ef- f i c i e n c y could be i n c r e a s e d .
The problem of t h e e f f i c i e n c y i n c r e a - s i n g by c o r r e c t u s i n g of nonresonance ene- rgy exchange was a l s o ' f o m l a t e d a l o n g w-ith
d i s c u s s i o n of t h e a d v e n t u r e s a p p e a r i n g f o r d i f f e r e n t GDL molecule o p e r a t ion. The p o i n t i s t h a t f o r GDL c o n d i t i o n s t h e smal- l e r quanta o s c i l l a t o r i s e x c i t e d more e f - f e c t i v e l y a t two d i f f e r e n t quanta o s c i l l a - t o r c o l l i s i o n s f o r GDL c o n d i t i o n s because of h i g h e r p r o b a b i l i t y of an e x t r a v i b r a t i - o n a l energy t r a n s f e r t o t r a n s l a t i o n a l deg- r e e of freedom t h a n f o r t h e backward pro- c e s s of t r a n s l a t i o n a 1 energy t r a n s f e r t o v i b r a t i o n s r e q u i r e d f o r t h e e x c i t a t i o n of g r e a t e r quanta o s c i l l a t o r . T h i s e f f e c t i s a main r e a s o n of i n v e r s i o n p o p u l a t i o n s between t h e upper CO-levels w i t h d e c r e a s -
i n g quanta because of unharmonicity /20,
9,
2 , 3/.
The nonresonance exchange affectsn e g a t i v e l y i n t h e c a s e of C02-N2-He(~20)
*
-GDL energy t r a n s f e r from N2 t o C02 be- cause (QO$CO; l e v e l i s h i g h e r t h e n
( V = S " ) N ~ . But t h i s e f f e c t i s p o s i t i v e a s i n t h e c a s e of N20-ITTGDL /22/ a s f o r CS2- CO-GDL ( s e e t h e f o l l o w i n g p a r t ) and t h e a u t h o r s /22/ suggested t o use the same e f f e c t s
f o r P a r t i a l p o p u l a t i o n i n v e r s i o n h e a t - pumped GDL on d i f f e r e n t molecules.
The development of id,ea t o u s e t h e nonresonance e f f e c t i n t h e c a s e of GDL l a -
s i n g GO2 molecule r e s u l t s i n s u g g e s t i o n and r e a l i z a t i o n of I8.4mkm CDL / I 4 / on
V2-V, transition
i n s t e a d of u s u a l C02-GDLv3-
V,,V'
t r a n s i t ions. The mentioned e f f e c t h e l p s i n high speed r e l a x a t i o n t o Boltzmanp o p u l a t i o n d i s t r i b u t i o n with very low n o z z l e t r a n s l a t i o n a l t e m p e r a t u r e on t h e
Fermi-resonating GOg l e v e l s forming a "mu- l t i p l e t w . population i n v e r s i o n a p p e a r s between d i f f e r e n t " m u l t i p l e t f l l e v e l s . T h i s method of population i n v e r s i o n f o r m a t i o n 'was theoretically I n v e s t i g a t e d f o r a num-
b e r of o t h e r t h r e e atomic molecule t r a n s i - t i o n s /23/. For convenience we s h a l l turn i n t h i s r e v i e w t o Fig.1 which p r e s e n t s a l l p u b l i s h e d , suggested ( t o p l i n e s ) and r e a - l i z e d (bottom l i n e s ) h e a t pumped GDL. The
hlas
v a l u e , t r a n s i t i o n , GDL a c t i v e me- d.ia and r e f e r e n c e a r e l i s t e d i n Table I.The
2
las i n c r e a s i n g f o r m o l e c u l a r la- s e r s under c o n s i d e r a t i o n means p h y s i c a l l y a frequency d e c r e a s i n g i n t h e l i n e of l a - s e r t r a n s i t i o n s between e l e c t r o n i c s t a t e s ( s p e c t r a l r e g i o n up t o-
2 mkm, t h e reco- mbination GDL) ; v i b r a t i o n a l l e v e l s of two- a t o m i c s ( s p e c t r a l region*3+7mkm); d i f f e - r e n t mode v i b r a t i o n a l l e v e l s of t h r e e - a t o - mics ( N 7s750mkm); molecular r o t a t i o n a l l e v e l s ( - 2 0 t I 0 0 mkm); dimers and t r i m e r s i n t e r - and i n t r a - m o l e c u l a r mode v i b r a t i o - n a l l e v e l s (h30;IOOmkm)cn"
0,
U ZE9
I' i l l
I
I I I0.6
1.0
Fig. lcussed and e x p e r i m e n t a l l y proved by d i f f e- r e n t i n v e s t i g a t i o n groups ( s e e review i n
/3/)
f o r some two-atomic V I and V I I Mende- l e e v l s P e r i o d i c Table column molecule (02, S2; C 1 2 , Br2 and o t h e r s , s e e Fig.1) and a l s o f o r some three-atomic molecules a s NO2, SO2,Cog.
The advantages of such la- s e r s should be h i g h s p e c i f i c powers (on one o r d e r h i g h e r t h a n f o r I R C02 GDL /24/) mainly because of one o r d e r i n c r e a s i n g of quanta energy, and a l s o of h i g h e f f i c i e n - cy, a s example, about 20% f o r Br2-GDL /24/ Thealas
d e c r e a s i n g l e a d s t o q u i c k e r l a - s e r beam c r o s s - s e c t i o n d e c r e a s i n g having importance f o r energy t r a n s f e r problems. It i s important a l s o t h a t j\ of some recombination l a s e r i s i n v i s i b l e "windowff of t h e atmosphere. The e s s e n t i a l d i s a d v a n t a g e of t h e he- at-pumped recombination GDL i s i t s s m a l l g a i n v a l u e,d<
10'~cm-I /25-29,3/ a t l e a s t f o r t h e f i r s t r e a l i z a t i o n e x p e r i d melits, It could be t h e r e a s o n t h a t s u c h a l a s e r i s n o t r e a l i z e d y e t but one s h o u l d t a k e i n t o account t h a t c a l c u l a t i o n s could n o t be f i n i s h e d without some assumptions because of l a c k of e x p e r i m e n t a l d a t a , Ther e a l i z a t i o n experiments were performed w i t h t h e h e l p of shock t u b e s having o p t i - c a l l e n g t h 9cm /25,26/ and 50cm /3/ - f o r s i n g l e n o z z l e , and I 3 cm
-
f o r n o z z l e g r i d /27,29/. It was d i s c u s s e d / 3 0 / ' t h e p o s s i b i l i - t y t o u s e t h e h i g h p o p u l a t i o n i n v e r s i o n v a l u e s c a l c u l a t e d f o r recombinat i o n l a - s e r s w i t h t h e h e l p of energy t r a n s f e r t o some atomic eystem t h a t p r o v i d e s l a s e r emission.It was suggested t h e o r e t i c a l l y /22/ t o use HF,DF,HCl,HI,DCl,DBr,DI a s l a s i n g molecules of t h e heat-pumped p a r t i a l i n - v e r s i o n GDLts. It i s p o s s i b l e t o g e t l a s - i n g i n seven a r e a s of t h e spectrum between 2.5 and 6.2mkm ( s e e Fig.1) a t t h e approp- r i a t e c h o i c e of t h e e n e r a r e s e r v u a r mo- l e c u l e f o r GDL working mixture ( s e e Table I ) . The comprehensive c a l c u l a t i o n was made i n /22/ ( s e e a l s o /31/) f o r t h e c a s e of HC1-D2-He-GDL. It was shown t h a t t h e e f f i c i e n c y of- s u c h a l a s e r could r e a c h
I-1.5%
st t h e value of s p e d i f i c power ZOO-I 5 0 tut/g/sec, The Alas of HC1-GDL i s abo-
~ 9 - 1 9 2 JOURNAL DE PHYSIQUE
but f o r t h e mixing scheme was made i n /32/ and i t was found t h a t t h e g a i n v a l u e i s not l e s s t h e n 3.10-~cm-I ( s e e a l s o /33, 34/). T h e o r e t i c a l and experimental i n v e s - t i g a t i o n s of HC1-D2-laser were performed i n /35/.
TheAlas of HBr-GDL suggested i n /36/ a l s o g e t s t o t h e same s p e c t r a l region. The c a l c u l a t e d g a i n v a l u e f o r pure H B r is two o r d e r s h i g h e r t h e n CO-N2-GDL g a i n va- l u e . The c a l c u l a t i o n /36/ g i v e s a l s o pure
NO-GDL (
A
Y 5.26mkm) g a i n value com-p a r a b l e w i t h t h a t f o r pure CO-GDL. The 2.352.7mkm p a r t of Pig. I p r e s e n t s t h e obertone CO-GDL s p e c t r a l r e g i o n c a l - c u l a t ed i n /I3/.The g a i n v a l u e &
-
10'~cm" s u f f i c i e n t f o r t h e experimen- t a l a p p r o v a l was c a l c u l a t e d i n / I 3 / f o r s t a g n a t i o n parameters T0=1800K, Po=IOO a t of CO-Ar (I:4)-mixture e s c a p i n g from t h e*
s i n g l e p r o f i l e d n o z z l e w i t h h =0.04cm a t 58cm d i s t a n c e from t h e t h r o a t .
The f i r e t CO-GDL p u b l i c a t i o n s were d i s c u s s e d i n monographs /2,3/. Between new r e p o r t s we should l i k e t o p o i n t o u t two s e r i e s of experiments conducted w i t h a shock t u b e /37-39/ and, a d i a b a t i c t u b e /40, 41/. The 200 W t power and s p e c i f i c energy
5.9Jjg
a t 0.5% e f f i c i e n c y were achievedf o r CO-Ar-mixture i n /37/. It was mention-
B Q
a l s oabaut
l a s i n g r e g i s t r a t i o n f o r t h e c a s e of p u r e CO. The g a l n v a l u e dd
5
3.10'~ctn'~ was measured/38/
by a ca-l i b r a t e d l o s s e s method. T h i s v a l u e
i e
h i g h .e r t h e n t h e p r e v i o u s experimental r e s u l t s s a d i s i n a b e t t e r agreement w i t h t h e t h e - b q e t i c a l c a l c u l a t i o n s . The spectrum
of GO-GDL was i n v e s t i g a t e d and w a s found
kd
be a g r e a b l e w i t h t h e t h e o r y /39/; t h ea u t h o r s a l s o s t u d i e d t h e q u e s t i o n s of r e a l energy output f o r t h i s l a s e r .
The dependences of df2.10-~cm-I on
t h e g a s r e s o n a t o r temperature 7 0 1 T ( 200K f o r t h e c a s e of CO-N2-Ar-GDL were inves- t i g a t e d by t h e probe l a s e r i n /40,4I/ and t h e r e were analyzed time h y s t o r i e s of ma- ny l e v e l p o p u l a t i o n s r e g i s t e r e d f o r d i f f e - r e n t n o z z l e t h r o a t d i s t a n c e s . The new t h e o r e t i c a l CO-GDL p u b l i c a t i o n s a r e /42- 45/. Some q u e s t i o n s of CO-GDL t e c h n i q u e were i n v e s t i g a t e d i n /46/ ( d i f f u s o r prob- lem) and i n /47/ ( p r e l i m i n a r y s t u d y of c l o s e d c i c l e o p e r a t i o n ) .
The C02-GDL with j\ las=9.4; 10.6 mkm
w i l l n o t be discussed h e r e because monog- r a p h s /2,3/ and some reviews /I9,48-52/ a r e devoted mainly t o t h i s l a s e r .
GAS DYNAMIC LASERS WITH
alas
7
I 0 mkm Usual IO.6mkm CO GDL a n & o ~ u ~ 8 _a ) *
-
-
-
---
-2---
( Lra_nsit ~ o n b e J w ~ n - ~ ~ arnddVa,3 m o d e s). From such GDL!~ N20-GDL is t h e c l o s - e s t one by u s u a l 10.6 C02 l a s e r t a k i n g i n - t o account t h e
3
las value ( s e e Fig.1). The experimental a p p r o v a l of N20 a s a l a s - i n g molecule i n GDL w i t h N2 e l e c t r i c a l d i - s c h a r g e e x c i t a t i o n / I 2 / was l i k e l y t o be t h e f i r s t . T h i s molecule was f i r s t u s e f o r t h e heat-pumped GDL i n /53/ where l a s i n g was r e g i s t e r e d and i n /54/ where t h e g a i n ms measured w i t h t h e h e l p of probe l a s e r(see
/55/)
The
fi r e t
t h e o r e t i c a l and comprehensive experimental i n v e s t i g a - t i o n s made i n /21,56-58/ h e l p e d t o o b t a i n some unknown v i b r a t i o n a l r e l a x a t %on cons- t a n t s and t o p r e c i s e a n o t h e r c o n s t a n t s i m ~ p o r t a n t f o r N20-.GDL. There were e s t a b l i s h - r ed t h e t e c h n o l o g i c a l l y important f a c t s :t u r e p o s s i b i l i t y of GDL o p e r a t i o n and ( 2 ) low H20-vapour i n f l u e n c e on t h e g a i n v a l u e ( s e e a l s o /59/). Fig. 2 The g a i n v e r s u s tempereture i n v e s t i g a - t i o n r e s u l t s /21,57/ p r e s e n t e d i n Fig.2 show N20-GDL advantages a t low s t a g n a t i o n t e m p e r a t u r e a s compared t o COiGDL a s a r e s u l t of nonresonance exchange e f f e c t i n - f l u e n c e , The energy exchange N20-N2 measu-
rement B /60/ were important f o r N20-GDL
model r e f inment
.
The e s s e n t i a l advantage of N20-laser i s t h e p o s s i b i l i t y of more e f f e c t i v e ener- gy t r a n s f e r i n t h e atmosphere comparing t o C02-laser /61/. The value s m a l l e r t h a n f o r C02 of N20 d i s s o c i a t i o n energy is t h e i n a d e q u a t e n e s s of N 2 0 - ~ ~ ~ l i m i t i n g t h e s t a g n a t i o n t e m p e r a t u r e by 1800 K. T h i s dis advantage could be avoided i n c a s e of us- i n g of N20-GDL o p e r a t i o n mixing scheme a s i t was s u g g e s t e d i n /61/, The CW heat-pum- ped N20-GDL h a s been j u s t f i r s t r e a l i z e d u s i n g t h i s method of o p e r a t i o n /62/, The N20- and C02-GDL power comparison made on t h e same i n s t a l l a t i o n /I7/ f o r d i f f e r e n t s t a g n a t i o n t e m p e r a t u r e s and o t h e r pakme- t e r s gave t h e r e g i o n where N20-GDL i s t h e c o m p e t i t i v e w i t h C02-GDL; i t was a l s o es- t a b l i s h e d t h e o p e r a t i o n p o s s i b i l i t y f o r
cheap N20-air working mixture /63,64/. The
g a i n
d
G- 11 I. IO-~CIII-' and t h e s a t u r a t i o nparameter Is= 3. 0kwt/cm2 were measured
by t h e method of c a l i b r a t e d l o s s e s and-ap- p e a r s t o be only -10 % l e s s t h e n f o r C02- GDL a t t h e same c o n d i t i o n s /65/. Qualita-
t
i v e l y comparable r e s u l t s were found f o r q u a s i s t a t i o n a l mixing N20- and C02-GDLvs where c o l d l a s i n g g a s e s were provided c l o - s e d t o t h e n o z z l e c r y t i c s e c t i o n /66/.The mixing was produced a t t h e n o z z l e f i n a lp a r t i n /62-65/. Promising N20-GDL was
r e a l i z e d i n /50/ u s i n g C O which was pro- duced by t h e f u e l burning and mixed w i t h c o l d X20 i n t h e ,nozzle. Since ( O O ~ I ) ) N ~ O l e v e l i s lower t h e n ( w = I ) C O l e v e l , t h e n t h e e f f e c t of nonresonance exchange i s
p o s i t i v e f o r N20-CO i n s t e a d of C02-CO mixture f o r which ( O O ~ I ) C O ~ l e v e l i s high- e r t h e n (qJ-=I) C O one. Authors /50/ a r e successed t o o b t a i n CW power 0.8k1#t which i s a r e c o s d now f o r N20-GDL.
CS2-GDL (II,4mkm) i s going t o t h e
next i n Fig.1. T h i s (00'1-10'0) t r a n s i t i a n l a s i n g f o r the heat-pumped CS2-CO-HeiCDL was f i r s t and independently o b t a i n e d by two groups /67,15/ u s i n g a shock tubejI3.7,
45.6 and II7mkm Q3-
an an sit ions
( s e eTable I) were suggested f o r CS2-GDL on t h e
b a s i s of experiment /I5/. CS2 molecule
C9-194 JOURNAL DE PHYSIQUE
II.4mkm CS2 l a s i n g e x p e r i m e n t /15/.CS2- GDL c a l c u l a t i o n and p a r a m e t e r ' s optirnizs- t i o n were made i n /69/ where t h e c o n s t a n t s v a l u e s were t a k e n from /70/.
b ) . I - & ~ t E l t Z p ~ m p ~ d _ ~
ILmk_m
G_DL-(orE2
i n s _ i d e - of-V2- mode t r = n s i t i o n &_ _ _ - -
-
- - - -
Some t h e o r e t i c a l r e p o r t s have been p u b l i s h e d on t h i s problem; we s h a l l n o t d i s c u s s v e r y i n t e r e s t i n g r e s u l t s of an e l e c t r i c d i s c h a r g e e x c i t e d l a s e r (EDGDL) ( s e e / T I / and i t s b i b l i o g r a p h y ) . The m o d i f i c a t i o n of /71/ was c a l c u - l a t e d i n /94/ on t h e b a s i s of u s u a l C02- N2-H2+DL (T0=1200 K , Po=15 a t ) w i t h a d d i - t i o n of s h o r t - p u l s e 9.4mkm pumping. It was s u g g e s t e d i n /72/ t o d e v e l o p /71/ by pro- d u c i n g 9.4mkm c o n t i n u o u s pumping i n u s u a l GDL on t h e C02-N2-H20 ( I : I I : 0 . 5 ) m i x t u r e w i t h t h e h e l p of a d d i t i o n a l s e l e c t i v e r e - s o n a t o r s i t u a t e d c l o s e r t o n o z z l e e n t r a n c e t h e n b a s i c s e l e c t i v e I6mkm r e s o n a t o r . It w a s s u g g e s t e d i n / 7 3 / t o g e t a I6mkm l a s - i n g from u s u a l GDL b u t o p e r a t i n g on t h e m i x t u r e of Co2-Ar(1:g o r I : 4 ) u n d e r con-*
d i t i o n s of T0=2200 K , Po-60 a t , h =0.2mm. An assumed p o s s i b i l i t y of p r o d u c i n g I6mkm l a s i n g w i t h t h e h e l p of u s u a l GDL o p e r a t - i n g on t h e C02-Ar ( 1 : I ) m i x t u r e was a l s o mentioned i n /74/. But c a l c u l a t i o n s / I 4 , 75/ show t h a t s u c h a l a s e r i s u n r e a l beca- u s e of t h e r e q u i r e d e e s e n t i a l f l o w d e n s i t y d e c r e a s i n g (- IO'~), v e r y low s t a g n a t i o n p r e s s u r e Po-- 2q5 a t and C02 c o n t e n t ( ~ 2 % ) i n t h e yiorkirig mixture. These r e s u l t s f o r 16mkm(02~0-01'0) C02 t r a n s i t i o n p o p u l a t i o n i n v e r s i o n a r e more r e a s o n a b l e because ' t h e t h e o r e t i c a l r e l a x a t i o n model / I 4 , 7 5 / is i n good agreement w i t h I 8 m k m C02-Ar-GDL expe- r i m e n t a l r e s u l t s /14,75/, s e e n e x t pa**The I6,7mkm ( 0 3 ' 0 - 0 2 ~ 0 ) and I7,2mkm (04'0-03~0) C o p t r a n s i t i o n s aye a l s o i n s i d e . of -r)2-mode t r a n s i t i o n s , f o r which t h e po- p u l a t :on i n v e r s i o n ( w ~ ~ ' ~ c m - ~ ) and g a i n ( N 0.02 cm") were c a l c u l a t e d / I 4 / i n t h e c a s e of C02-Ar-GDL. But i t was n o t proved i n e x p e r i m e n t s / I 4 , 7 5 / where t h e l a s i n g on t h e s e t r a n s i t i o n s and on I6mkm t r a n s i t i o n was n o t d e t e c t e d . The p o s s i b l e r e a s o n s of
s u c h a d i s a g r e e m e n t a r e d i s c u s s e d i n / I 4 , 75/. The r e a s o n s of .u I6.8mkm SO2-GDL un-
r e a l i t y w i l l be d i s c u s s e d i n n e x t p a r t of t h i s work.
c )
.
sm_kmn
CO,-GDL- - -
and i t s a n a l o g u ~ : bransi-tions-
-
-
between )lzandglmod_ees).- - -
A t p r e s e n t t h e I 8 m h C02-Ar-GDL i s t h e l o n g e s t I R wave-length c o n t i n u o u s g a s dynamic l a s e r /76/. P o p u l a t i o n i n v e r s i o n f o r m a t i o n h a s been i n v e s t i g a t e d i n /7'// t h e o r e t i c a l l y f o r ( 0 3 ' O - I O ~ O ) C O ~ t r a n s i t i- on i n t h e c a s e of a n e l e c t r i c d i s c h a r g e l a s e r ( s e e f i g . 3). C02-Ar m i x t u r e g a s d p a - mic l a s e r w a s s u g g e s t e d i n d e p e n d e n t l y i n / I 4 /
and/74/ a s a development of /77/ and was e x p e r i m e n t a l l y p r o v e d i n / I 4 / w i t h t h e h e l p of shock t u b e . The r e s u l t s of t h e o r e t i c a l and e x p e r i m e n t a l lRmkm C 0 2 G D L i n v e s t i g a t i - ons a r e p r e s e n t e d i n /75/. The l a s i n g was r e c o r d e d /14/ i n a broad r e g i o n o f s t a g n a - t i o n t e m p e r a t u r e 1000-2800 K and measured
Fig. 3 p r i n c i p l e i s r a t h e r u n i v e r s a l and s u i t a b l e f o r d i f f e r e n t molecules.
(ret.1
I":
2 2 2 0
18
16 14
12
10
8
6
Fig. 4and w i t h t h e measured l a s e r power depende* I n t h e c a s e of C02-Ar-mixture it g i - c e s on s t a g n a t i o n parameters, rnixt"* d, e s ves t h e ~ o p u l a t i o n i n v e r s i o n n o t only f o r
and s o on. I t ' s important t o n o t e t h a t 19.4mk m (03'0-10'0) t r a n s i t i o n . There we- h i g h q u a l i t y experimental r e s : ~ l t s /78,.79/ r e c a l c u l a t e d /14/4h/ and d values a l s o
were very h e l p f u l i n t h e model development. f o r I9.7mkm ( 0 4 ~ 0 - 1 1 ' 0 ) : 21.2mkm (04'0-
The s p e c i f i c energy e s t i m a t i o n s 11'0) ; 50.2mkm(04°0-000~) s o f a r without
(
4
6oWt/g/sec) were made f o r t h e new IBmlan q p e r i ~ e n t a l approval.C02 GDL i n /80/, and energy dependence on I n t h e c a s e of Ar-exchanging i n t h e
t h e CO 2- c o n t e n t i n GO2-Ar-mixture a e s e mixture f o r a n o t h e r r a r e g a s e s one can g e t c a l c u l a t e d i n /81/. The nozzle shape, s t a - v a r i a t i o n s i n GDL energy parameters f o r g n a t i o n parameters and H20-impurities e f - d i f f e r e n t t r a n s i t i o n s w i t h t h e g o a l of op- f e c t s were s t u d i e d t h e o r e t ' l c a l l y f o r I8mkm t i m i z a t i o n . 18.4mkm l a s i n g was r e g i s t e r e d C02 GDL parameters i n /82 -34/. It was f o - t o be l e s s i n t e n s i v e f o r GO2-Xe t h e n f o r und t h e r e a l s o t h a t e f f i c i e n c y of t h i s l a - C02-Ar mixture.
s e r c o u l a be a s h i g h as.v2%. T h i s value is I n t h e c a s e of exchange of l a s i n g C02 much higfier t h e n e f f i c i e n c y of u s u a l C02- molecule one can g e t GDL s p e c t r a l r e g i o n GDL (without *'mixingqt). T h i s advantage i s dxtending w i t h t h e h e l p of Ar-mixture w i t h due t o r e l a t i v e l y low l a s e r l e v e l p o s i t i o n , a n o t h e r l i n e a r t h r e e - a t o m i c molecule w i t h d e g e n e r a t i o n of energy s t o r e d v i b r a t i o n a l Fermi-resonance between symmetrical and mode and low b u f f e r r a r e gas h e a t c a p a c i - bending modes. There were c a l c u l a t e d GDL
t y /I5/. parameters /23/ f o r M20-Ar (Jlas=21.5mkm)
C9- 196 JOURNAL DE PHYSIQUE
and 39.3mkm) m i x t u r e s . The method i s d e s c - r i b e d f o r t h e unknown s p o n t a n e o u s p r o b a b i - l i t y c a l c u l a t i o n of a l l mentioned t r a n s i
-
t i o n s and t h e p a p e r p r e s e n t s a l l known r e - l a x a t i o n c o n s t a n t d a t a . A p a r t of t h e r e l a x a t i o n d a t a were measured by u l t r a s o a l c a b s o r p t i o n e s p e c i a l l y f o r B20-Ar-GDL /35/ and CS2-l1r-GDL /86/ i n v e s t i g a t i o n program. The h i g h e s t values of 4 - 7 . T . ~ - ~ c s - ' andAN
,
I G * ~ C P I - ~ were f o&d /23/ f o rCS2-Ar-GDL. The p o p u l a t i o n i n v e r s i o n i s even h i g h e r t h a n i n c a s e of C02-Ar-G3L/75/ a t l o w e r t e m p e r a t u r e T o (800 K i n s t e a d of I200 K ) ,that i s l i k e l y t o s u p p o r t a sugge- s t i o n on h i g h e r e f f i c i e n c y . T h i s r e s u l t i s i n agreement w i t h r e l a t i v e l y l o w e r C S 2 l e - v e l p o s i t i o n /I5/. .
.
d l .
-
GDL on n o n l i n e a r molecule t r a n s i t i o n s .---
---
One of t h e f i r s t a t t e m p t t o s t u d y t h e p o s s i b i l i t y of n o n l i n e a r molecule a p p l i c a - t i o n f o r a h e a t pumped GDL is t h e ' w o r k /87/ where SO2-Ar-GDL p a r a m e t e r s a r e c a l - c u l a t e d f o r2
las=iI. 8 mkm ( s e e Fig.5 ) .
so2
m o l e c u l e i s i n t e r e s t i n g because of two w i d e l y d i f f e r e n t v i b r a t i o n r e l a x a t i o n t i m e s of t h e u p p e r and t h e l o w e r l a s e r l e - v e l s ( a n e x t r a component f o r l o w e r l e v e l r e l a x a t i o n s p e e d i n g l i k e i n t h e c a s e of I 0 mkm C02-GDL i s n o t r e q u i r e d ) . A t t h e same t i m e t h e SO2 y a n d J a r e l a x a t i o n t i m e s a r e long enough f o r n ~ n e ~ u i l i b r i u m v i b r a t i o n a l e n e r g y a c c u m u l a t i o n a t s u p e r - s o n i c e x p a n s i o n c o o l i n g . By t h e a u t h o r s/87/
o p i n i o n from t h e known t h r e e - a t o m i c s SO2 m o l e c u l e i s most p r o m i s i n g one f o r GDL a p p l i c a t i o n . It i s t h e r m a l l y s t a b l e , n o t v e r y t o x i c a l , low p r i c e and h a s r a t h e r good known s p e c t r o s c o p i c a l c o n s t a n t s.
I n /87/ one c a n s e e t h e l i s t of i m p o r t a n t Fig. 5 SO2 r e l a x a t i o n c o n s t a n t 3 and t h e d i s c u s s i - on of p o s s i b i l i t y of O2 a d d i t i o n i n t o wor- k i n g m i x t u r e a s a h e a t - s o u r c e molecule.1t could be p o i n t e d o u t t h a t lower p o s i t i o n of upper l a s e r l e v e l (-1000cm-' l e s s t h a n f o r ( 0 0 ~ 1 ) GO2) w i l l t e n d t o e f f i c i - ency i n c r e a s i n g of t h e proposed SO2-GDL /I5/. The c a l c u l a t e d p o p u l a t i o n i n v e r s i o n i s A N 5. ~ ~ I ~ c r n - ~ f o r t h e t e m p e r a t u r e a s low a s T = 1000 K i n c a s e of SO2-Ar i 2 : 3 ) 0 m i x t u r e . But t h e v a l u e ofa*2.10-~cm-~ is r . e l a t i v e l y s m a l l because of much b i g g e r number of n o n l i n e a r m o l e c u l e r o t a t i o n a l l e v e l s t h a n i n t h e c a s e of C02-molecule. The p r o b a b i l i t y of s p o n t a n e o u s t r a n s i t i o n c a l c u l a t e d i n /87/ i s t e n t i m e s l e s s t h a n f o r 1 h k m COB-GDL. It f o l l o w s from s p e c t - r o s c o p i c d a t a t h a t I6.8mkm (100-OIO)S02 t r a n s i t i o n p r o b a b i l i t y i s 50 t i m e s l e s s t h a n t h e c o r r e s p o n d i n g v a l u e f o r II.8mkm t r a n s i t i o n ( i n s p i t e of comparable popula- t i o n i n v e r s i o n ) ao we c a n c o n c l u d e t h a t 16.8mkm SO2-GDL i s u n r e a l one. A n o t h e r example of n o n l i n e a r l a s i n g m o l e c u l e i s a l s o d i s c u s s e d t h e o r e t i c a l l y .i n /88/ where h e a t pumped H20-GDL- is sug-
i n g t o (001-020) and (100-020) H2C t r a n s i - t i o n s . The d i f f e r e n c e between SO2 /87/and H20 /88/ GDL c a l c u l a t i o n s i s that t h e g a i n
v a l u e s OC =0,9,10'~cm'~ and 0.8.10-~cm-Iare
about 2 o r d e r s h i g h e r f o r 28mkm and 33mkm H20 t r a n s i t i o n s a t t h e t y p i c a l pure water
vapour s t a g n a t i o n c o n d i t i o n s To=2500 K , Po= I a t . I t should be p o s s i b l e v e r y easy t o check such a h i g h g a i n e x p e r i m e n t a l l y . I n accordance w i t h c a l c u l a t i o n s of / 8 8 /
t h e p o p u l a t i o n i n v e r s i o n i s a s h i g h a s 16
I 0 cm'3 and t h e s p e c i f i c energy could r e - a c h t h e value 40Wt/g/sec f o r 28 mkm l a s - ing. The i n v e s t i g a t i o n of t h e p o s s i b l e O2 and H2 i m p u r i t i e s e f f e c t on H20-GDL para- m e t e r s have shown t h a t O2 r o l e i s n e g l i - g a b l e , but H2 changes s u f f i c i e n t l y t h e (001) and (100) l e v e l s p o p u l a t i o n r e s u l t - i n g i n p o p u l a t i o n i n v e r s i o n between them. I n accordance w i t h t h i s conclusion t h e same a u t h o r s c a l c u l a t e d H20-H2-GDL / 8 9 / .
The g a i n v a l u e around N 3.10-~cm-I was
found f o r f i v e d i f f e r e n t s u b m i l l i m e t e r t r a n s i t i o n s -150, 1 6 3 , ~ 1 7 3 , e 2 0 8 , and 733 m k m i n t h e c a s e of To=2500K, PO-0.5at f o r t h e H20-H2(4:I) mixture. e l . GDL on
- - -
- - -
rotational-t~an~i;4.ions_gd, * _ c o ~ d ~ n s l_aserf=
A gasdynamic method of p o p u l a t i o n i n - v e r s i o n p r o d u c t i o n on r o t a t i o n a l s t a t e s of molecules was suggested i n /90/ and a g a i ni n /91/. Authors of /90/ proceed from t h e
assumptions t h a t singlequantum p r o c e s s e s s t a r t t o be moet important c o l l i d i n g . r o t a t i o n a l t r a n s i t i o n s with t h e temperature d e c r e a s i n g , when exchange p r o c e s s e s and t r a n s i t i o n p r o b a b i l i t i e s s t a r t t o ' b e e i g n i f i c a n t l y decreased; t r a n s i t i o n p r o b a b i l i t i e s a r e s t r o n g l y decreased a l s o w i t h i n c r e a s i n g r o t a t i o n a l quantum number. The c a l c u l a t i o n s of HC1-He-GDL /90/ gave p o p u l a t i o n i n v e r s i o n f o r t h e group of ro- t a t i o n a l l e v e l s
(J
=13+20),Alas--
4 0 i 20mkm with ~ - 1 0 - ~ - 1 0 - ~ c m - ' and e f f i c i e n c y-0.1%.
The a u t h o r /91/ who wrote t h e popula- t i o n i n v e r s i o n c o n d i t i o n based on some s i m p l i f i c a t i o n s made n e a r l y t h e same assu- mptions. GDL w i t h c o n v e r s a t i o n of a s o l i d
s t a t e - l i q u i d phase t r a n s i t i o n energy i n t o l a s e r r a d i a t i o n was suggested by a u t h o r s of /92/; they c a l l e d i t a s gasdynamic IVco- ndens l a s e r m . There were d i s c u s s e d two ways of p o p u l a t i o n i n v e r s i o n p r o d u c t i o n s on v i b r a t i o n a l l e v e l s of i n t e r m o l e c u l a r and i n t r a m o l e c u l a r modes a t such condensa- t i o n c o n d i t i o n s when t h e r e e x i s t very ex- c i t e d p r o d u c t s of condensation (dimers and t r i m e r s , i n p a r t i c u l a r ) . The grade of e x c i t a t i o n depends on complex a s s o c i a t i o n energy t h a t is h i g h e s t (5-IOkkal/mol) f o r hydrogen-bond molecules H20, HC1,HF.
It was t h e o r e t i c a l l y shown i n /92/ t h a t t h e g a i n and l a s i n g a r e p o s s i b l e i n ithe r e g i o n of
3
las- 30f I00mkm f o r H20-GD '"condens l a e e r n . S t r o n g l y u n e q u i l i b r i u m i'jspontaneousIR
emission was r e g i s t e r e d ejc-C9-198 JOURNAL DE PHYSIQUE
TABLE : The suggested and realized(*)heat pumped
gas dynamic l a s e r systems
LASING MOLECULE , WORKING REFE- LASIKG MOLECULE WORKING REFE-
TRANSITION MIXTURE RENCE TRAXSITION RENCE
HBr
3.77
H I
4.48
DCl
6.28
CO*)
44.8t.
5.2)
NO
5.26
DBr
5.43
c%*) (081-180)
11.4
so,
(001-010'
11.8
C02 (03'0-02~0)
16.7
C02-fir
I4,75
SO2 (100-010
j
16.8
SO2-Ar
81
CO,
(04'0-63
0 ) 17.2
C02-Br
I 4
,'I5
CO,~$O~'O-1O00) I8,3
8
C02-At
I 4
C02-Xe
C02 (04~0-11'0)
19.7
C02-Ar
I4,75
HCL
(7ohtJ(20t.
HCL-lle
90
40)
co2(oii00-IIIO)
21.2
co2-AT
I4,75
~ 0 ( 0 3 ~ 0 - 1 0 ~ 0 )
21.5
N20-Ar
23
H20(OOI-020
4
28.0
H20
88
COS(IO~O-01 0)
29.5
CGS-AT
23
COS( 11'0-02~0)
29.9
COS-Ar
23
(!20
In
<30*
H20
92
100)
c0S(1I10-02'0)
30.5
COS-AT
23
H~O(IOOO-020)
33.0
H20
88
cq(1o00-01'0)
38.3
C%-AT
I5,23
JOURNAL DE PHYSIQUE
BIBLIOGRAPHY
1.Konyukhov
V.K.,
Prokhorov A.M., Authors certificate No 223954, NovembeP 19,1966. Bullet en izobretenii No 25 (1968) ,Pistmav
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S-Fr.,
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,
Kantrovitz A,R. ,Leonard D., Wilson J. US Patent No 3-543179,1969.Gerry E.T. Laser Focus 6,No I2,27 (1970)
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40,
2575-2577 (19705.9 .McKenzie R,L. App1,phy s
.
Lett.,=,
462 (1970)1O.Watt W.S. Appl,Phys,Lett. ,18,487- (1979 II.Basov N.G.,Oraevsk A.N.,Scheglov V.A. ZHTP 37,339-348 (19675.
12.Bronf in
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