JOSA L E T T E R S

Induced dichroism in molecular gases

A. Marcano O. and F. García-Golding

Instituto Venezolano de Investigaciones Científicas, Centro de Física, Apdo. 1827, C a r a c a s 1010A, Venezuela

Received December 7,1981

Induced dichroism i n molecular gases was studied using a three-level scheme. A density-matrix calculation i n a l l
orders of the pump field that are linear i n the probé field may lead to a coherent dip i n the absorption-line shape
of the probé field, depending on the polarization arrangement. S u c h a coherent dip is a manifestation of the polar-
i z a r o n pulsation induced by the fields.

I t is well known that a beam of intense (pump) polarized W / . 1

light induces dichroism and birefringence i n a n originally
isotropic médium. T h e change in the polarization of a weak
1,2

(probé) field passing through the excited médium can be used 1 i v V" tQml-lm' nml(2lm'\
(1)
for measuring these effects. Different aspects of the theory fl k=a,b,c l = -~jk

of induced dichroism and birefringence in atomic gases have

dpi PaO Pa
been treated in the l i t e r a t u r e . 3-5

dt Ti
Analogous effects were observed i n molecular g a s e s . 6-8

Because of the complexity of molecular gases compared w i t h i jk

/Qm¡_¡ „,mlc*lm\
+ - z t \&ahPk (2)
atomic ones, it is desirable to search for the best conditions fl k=a,b,c l = —}¡
under which the induced dichroism is enhanced or does not
appear at all. Furthermore, it is well known that the resonant where a, ¡3 = a, b; c, S¡5Í = {k, l\(E + E i ) | a , m); d is the 0

interaction between a strong field and matter splits the system molecule dipole moment; T is the polarization relaxation 2

levéis, creating a coherent dip in the absorption line of the time; Ti is the rotation-relaxation time that includes the
médium. T h i s complicates the process of induced dichroism
9
reorientational relaxation; is the resonant frequeney that
is independent of m a n d m'; p b = pf = 0; p™ = l/(2j + 1);
and birefringence. I t is the purpose of this Letter to study the 0 0 0 a

influence of degeneracy, polarization arrangement, and i n - and j , it,, and j are the rotational quantum numbers of the
a c

tensity dependence of this effect in a homogeneously broad- states | a ) , | b), and | c ) , respectively.
ened molecular system, such as CO2 or N2O. I n E q s . (1) and (2) the lower indexes refer to the v i b r a -
tional-rotational quantum numbers and the upper ones to the
I n the analysis we consider a three-level scheme-of v i b r a -
magnetic quantum number.
tional-rotational states as shown in Fig. 1. T h e strong field
interacts with the states \) and | b >. T h e weak field is ab- We solve these equations in all orders in the pump field and
sorbed, sharing a common state with the pump field, e.g., the first order in the probé field. We first calcúlate the m a -
between | a > and | c ) . Also we assume that the line shapes for trix-density elements i n the absence of the probé field; then
the transitions |a) -* |b) and |a) ~*\c) do not overlap. we use this result to get from E q s . (1) and (2) the first-order
approximation i n the probé field.
T h e remaining states particípate in the interaction through
the process of rotational relaxation. A s usual, the vibrational I f E i = 0, the exact stationary solutions of E q s . (1) and (2)
relaxation is neglected. 10
for a single field (pump) are similar to the solutions for a
two-level system.
E a c h of the states with rotational quantum number j is (2j
9

+ 1) times degenerate, according to the orientation of the I n the rotating-wave approximation, we find that
angular momentum.
„mm(0) .mm'fO) _ (2jg + I)" 1

T h e pump and probé fields are of the form P aa P bb (3)

E 0 = Eoeo exp[í(a> f — k • r)] + c e ,

0

E i = i ? i e i exp[t(ci)i£ — k • r)] + c e , nmm'(0) ^ -ÍT2do hoEm 0 ( 0 ) _ m 'm'(0)]

" ab y Yr'aa Pbb
where a>> <^i, e , and e i are the frequencies and polarizations
u 0

of the pump and probé fields, respectively.

X exp[—¿(o) í — k r ) ] , . 0 (4)
I n order to simplify the analysis, we suppose that the pump
and probé fields are circularly polarized. mm(0) _
Pee
m'm(0)
n

yac
— mm'(0) _ A
Hbc > u
(5)
T h e density-matrix equations describing our system are as
follows: where the superscript (0) refers to the zero approximation in

Reprinted from Journal of the Optical Society of America, V o l . 72, page 957, J u l y 1982
Copyright © 1982 by the Optical Society of America and reprinted by permission of the copyright owner
958 J . Opt. Soc. A m . / V o l . 72, No. 7 / J u l y 1982 J O S A Letters

where P = -ih\(T Nd \( E\lh)

0 2 2 ) is the polarization in the
absence of the pump field,
1/2
E d 2 l m /(2; a + l)
m=-j a

T h e matrix elements d and c¡om can be determined, for

lm

example, from the equations given in paragraph 29 of Ref.

11.

NONDEGENERATE CASE
For understanding the influence of degeneracy we first con-
sider that d\ and d in E q . (8) do not depend on the number
0m

m. I n this case, the absorption line for the probé field versus
F i g . 1. E n e r g y - l e v e l scheme. T h e rotational relaxation is repre- detuning Ao) = 0)1 — u parametrized by ü is shown in F i g 2.
sented by the wavy arrows. We observe the typical saturation effect for small valúes of ü.
For valúes of 0 greater than 0.5, we see a splitting of the line
the probé field, similar to that which appears i n the ac Stark effect for a two-
h =[i(u -w )T +l]-\
0 0 ba 2 level system. However, in this case it is a polarization p u l -
sation. I n other words, using a hand-waving argument, the
y = T /T ,d = (b, m'|(de )|a,m>,m' = m ± l d e p e n d i n g
weak field makes transitions between the level |c) and the ac
1 2 0m 0

on whether the pump field is left or right circularly polarized,

Stark-split levéis | a) and | b ) .
respectively,
i/2
D E G E N E R A T E C A S E (y = 20) a
\m=j a 2] a + 1
The absorption-line shape for the right-hand circularly ( R H C )
and 12 = doEr¡T /h is the R a b i frequency i n units of I / T 2 .
2

polarized probé field and R H C polarized pump versus de-

Because we are interested in the absorption of the weak field
tuning is plotted in Fig. 3. T h e pump field is absorbed in the
that interacts with the states | a) and | c >, we calcúlate the
P branch, whereas the probé field is absorbed in the R branch.
nondiagonal element p™ at the frequency u>\, where m "
cm

We see that for the same range used in the nondegenerate case
= m ± 1, depending on the circular polarization of the probé
there is an absence of line-splitting effects; in other words, the
field.
degeneracy washes out the polarization-pulsation phenome-
I n the first order i n the probé field, taking into account
non. However, when the probé field is left-hand circularly
conditions (5), we obtain from E q s . (1) and (2)
and the pump field is R H C polarized, we again get the co-
íU T Qmm' m'm(0)
herent dip ( F i g . 4).
r t

mm(0) 1 in l ¿> p
. h\T 2S ac
P aa ' 2 2 ab ba

_mm"(l)
Comparing Figs. 3 and 4, we note that, for example, for Í2
(6) ~ 0.8, the ratio of the absorption coefficients at the center of
h [1 + h^üHdoJdc) ] 2

where the line is about 3. T h i s large ratio motivates the use of po-
larization spectroscopy to test the line-shape behavior.
fei = [¿(a>i - o ) ) T + l ] " , c a 2 1
I t should be noted that this analysis is based on the strong
h2 = [ i ( w i - o) - o ) ) T 0 c b 2 + colusión m o d e l for the rotational and reorientational re-
10

laxation, which basically states that the relaxation time T i in

The matrix element p ^ in E q . (6) may be calculated fromm ( 0 )
E q . (2) does not depend on the quantum numbers ; and
E q . (3), and the normalized condition p í T ' + pií ' = l/(2j 10 m w a

+ 1) and the element p & = ( p ^ ' ' ) * from E q . (4). m ( 0 ) 1 0

T h e polarization at the probé frequency 0)1 is given by

Ja
mm"(l)
P = N T. dp lm (7)
08-

I n E q . (7), d\ = ( c , m"|(dei)|o, m), and N is the relative

population of the state | a >.
o
Using E q s . (3), (4), and (6), we get from E q . (7) I-
Q-

9¡ 0.4

Po 1 Ja
P =
2; + 1
a m i '10
l + h-Ji ü 2 2

1 - 2í2%* /i2(dom /do ) 0 2 2

1 + (8)
1 + 4fiW7(do m 2 /do ) 2
Fig. 2. Absorption line versus detuning Aw = coi — o) ca parametrized
by fi for the nondegenerated case.
J O S A Letters V o l . 72, No. 7 / J u l y 1 9 8 2 / J . Opt. Soc. A m . 959

for temperatures up to 400 K both models are i n agreement

a • o 2A T, • 2 T
to w i t h i n 20%.
2

08h / \ <"tn Because the phenomenon described here is predominantly

05

//O.BU
a coherent effect, we t h i n k t h a t a polarization-spectroscopy
O 0.6
///A\ experiment is a better ground for testing the scope of the
1.5WÍ
strong collision model.

0.4 -
if/ vi2

ACKNOWLEDGMENTS

0 2 -- T h e authors would like to t h a n k R . M e d i n a for many i l l u m i -

nating discussions.

0.0 i i 1

-2 o 2
REFERENCES
(ui,

Fig. 3. Absorption line versus detuning Acó = coi — io parametrized ca

1. C. W i e m a n and T . W . Hánsch, "Doppler-free láser polarization
by íl for the degenerated case (j = 20). R H C pump and probé fields
a
spectroscopy," P h y s . R e v . L e t t . 36, 1170-1173 (1976).
are absorbed i n the P and the R branches, respectively. 2. D . F . L i a o and G . C . B j o r k l u n d , " P o l a r i z a t i o n rotation effects i n
atomic sodium vapor," P h y s . R e v . A 15, 2009-2018 (1977).
3. V . M . A r u t y u n y a n a n d G . C . Adonts, " I n d u c e d dichroism a n d
gyrotropy i n a resonance médium," Opt. Spectrosc. ( U S S R ) 46,
451-453 (1979).
4. N . K . Rumyantseeva, V . S. Smirnov, and A . M . T u m a i k i n , " A n -
T, = 2 T 2
isotropy of gaseous media in a strong electromagnetic field," Opt.
08 - C0 = «Jbo
0
Spectrosc. ( U S S R ) 46, 76-79 (1979).
XI - 0 . 2
5. G . G . Adonts and L . M . K o c h a r y a n , "Rotation of the polarization
ellipse i n cases of one- and two-photon resonances," Opt. Spec-
O 0.6 trosc. ( U S S R ) 40, 410-412 (1976).
6. V . Stert and R . Fischer, "Doppler-free polarization spectroscopy
using linear polarized light," A p p l . P h y s . 17,151-154 (1978).
04- / 0 5 \ 7. W . Detroder, Láser Spectroscopy, Springer Series i n Chemical
P h y s i c s (Springer-Verlag, Berlín, 1981), V o l . 5, pp. 504-520.
A \ ° V A 8. R . E . Teets, F . V . K o w a l s k i , W . T . H U I , N . W . Carlson, and T . W .
0.2- Hánsch, "Láser polarization spectroscopy," Proc. Soc. Photo-Opt.
I n s t r u m . E n g . 113, 80 (1977).
9. M . Sargent I I I , "Spectroscopic techniques based on L a m b ' s láser
0 0'
-6 -2 0 2
theory," P h y s . R e p . 43, 223-265 (1978).
10. F . A . Hopf and C . K . Rhodes, "Influence of vibrational rotational
AlD = ( o j , -Cü )
relaxation on pulse amplification i n molecular amplifiers," P h y s .
C Q

Fig. 4. Absorption line versus detuning Acó = coi — w parametrized ca R e v . A 8, 912-929 (1973).
by Í2 for the degradation case (j = 20). R H C pump field is absorbed
a 11. L . D . L a n d a u a n d E . M . L i f s h i t z , Quantum Mechantes: Non-
in the P branch, whereas L H C probé field is absorbed i n the R Relatiuistic Theory (Pergamon, Oxford, 1965).
branch. 12. J . K . Figueira, W. H . Reichelt, G . T . Shappert, T . K . Stratton, and
C. A . Fenstechmacher, "Nanosecond pulse amplification i n
electrón beam pumped CO2 amplifiers," A p p l . P h y s . L e t t . 22,
216-218 (1973).
13. E . E . S t a r k , J r . , W . H . Reichelt, G . T . Schappert, and T . F .
Comparisons of theory and short-pulse energy-extraction S t r a t t i b , "Comparison of theory and experiment for nanosec-
experiments - 12 13 i n CO2 show t h a t the strong collision model ond-pulse amplification i n high-gain CO2 amplifier systems,"
is a reasonable assumption, at least i n situations t h a t are not A p p l . P h y s . L e t t . 23, 322-324 (1973).
14. A . Marcano O. and V . T . Platonenko, " C a l c u l a t i o n of the s a t u -
sensitive to coherent effects. F u r t h e r m o r e , a recent calcu-
ration kinetics of vibrational-rotational transitions i n the diffu-
lation 14 based on the rate equations, comparing the strong and sion approximation," Moscow U n i v . P h y s . B u l l . 35, 53-59
weak collision (diffusion) models, leads to the conclusión that (1980).