The vibration-rotation of H₂O and its complexation with CO₂ in solid argon revisited
Fourier-transform infrared spectroscopy in the frequency range 400–4000 cm–¹ has been used to investigate the absorption of H₂O and H₂O:CO₂ complex isolated in solid argon. Thanks to the lowest temperature reached in our experiment, temperature effects and nuclear spin conversion studies allow us to...
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Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України
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| Цитувати: | The vibration-rotation of H₂O and its complexation with CO₂ in solid argon revisited / Xavier Michaut, Anne-Marie Vasserot, Luce Abouaf-Marguin // Физика низких температур. — 2003. — Т. 29, № 9-10. — С. 1118-1124. — Бібліогр.: 27 назв. — англ. |
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| author | Michaut, Xavier Vasserot, Anne-Marie Abouaf-Marguin, Luce |
| author_facet | Michaut, Xavier Vasserot, Anne-Marie Abouaf-Marguin, Luce |
| citation_txt | The vibration-rotation of H₂O and its complexation with CO₂ in solid argon revisited / Xavier Michaut, Anne-Marie Vasserot, Luce Abouaf-Marguin // Физика низких температур. — 2003. — Т. 29, № 9-10. — С. 1118-1124. — Бібліогр.: 27 назв. — англ. |
| collection | DSpace DC |
| container_title | Физика низких температур |
| description | Fourier-transform infrared spectroscopy in the frequency range 400–4000 cm–¹ has been used to investigate the absorption of H₂O and H₂O:CO₂ complex isolated in solid argon. Thanks to the lowest temperature reached in our experiment, temperature effects and nuclear spin conversion studies allow us to propose a new assignment of the rovibrational lines in the bending band n₂ for the quasi-freely rotating H₂O. An additional wide structure observed in this band shows two maxima around 1657.4 and 1661.3 cm–¹, with nuclear spin conversion of the high frequency part into the low frequency one. This structure is tentatively attributed to a rotation-ranslation coupling of the molecule in the cage. However, the equivalent effect is not observed in the vibrational stretching bands n₁ and n₃. Finally, by double doping experiments with CO₂, important new structures appear, leading us to unambiguously extract the frequencies of the lines of the H₂O:CO₂ complex.
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Fizika Nizkikh Temperatur, 2003, v. 29, Nos. 9/10, p. 1118–1124
The vibration-rotation of H2O and its complexation
with CO2 in solid argon revisited
Xavier Michaut, Anne-Marie Vasserot, and Luce Abouaf-Marguin
Laboratoire de Physique Moléculaire et Applications, UMR CNRS 7092
Université Pierre et Marie Curie, boîte 76, 4 place Jussieu
75252 Paris, Cedex 05, France
E-mail: xmichaut@ccr.jussieu.fr
Fourier-transform infrared spectroscopy in the frequency range 400–4000 cm–1 has been used to
investigate the absorption of H2O and H2O:CO2 complex isolated in solid argon. Thanks to the
lowest temperature reached in our experiment, temperature effects and nuclear spin conversion
studies allow us to propose a new assignment of the rovibrational lines in the bending band �2 for
the quasi-freely rotating H2O. An additional wide structure observed in this band shows two max-
ima around 1657.4 and 1661.3 cm–1, with nuclear spin conversion of the high frequency part into
the low frequency one. This structure is tentatively attributed to a rotation-translation coupling of
the molecule in the cage. However, the equivalent effect is not observed in the vibrational stretch-
ing bands �1 and �3. Finally, by double doping experiments with CO2, important new structures
appear, leading us to unambiguously extract the frequencies of the lines of the H2O:CO2 complex.
PACS: 33.15.Mt, 33.20.Ea, 33.20.Vq
1. Introduction
The water molecule is of C2v symmetry. In the gas
phase, its rovibrational spectrum is well known up to
26000 cm–1 [1–3] and in the solid state, the structures
of the different forms of ice have been extensively
studied [4–6]. Ice grains play an important role in the
chemistry of the interstellar medium and of planetary
atmospheres [7,8]. D’Hendecourt et al. [9] have
shown from IRAS-LRS observations of protostars,
that CO2 is a wide-spread and very common compo-
nent of the interstellar medium. The complexes be-
tween H2O and CO2 have been also the subject of se-
veral previous studies [10,11].
It is well known that the matrix isolation tech-
nique, combined with IR absorption spectroscopy, re-
mains a powerful tool to study the formation and the
geometry of weakly bonded complexes. Before looking
at the H2O:CO2 complex, pure H2O in matrices had
to be studied under our experimental conditions. Since
the work of Glasel [12], all evidence indicates that
H2O trapped in inert matrices, is almost freely rotat-
ing [13–17]. After some initial controversies, there is
now general agreement on the assignment of the
rovibrational absorptions in the �2 and �1/�3 regions
in solid argon [16]. This assignment is also very im-
portant for all matrix isolation studies because water
is a common impurity. In the same way, as CO2 is also
always present as an impurity in matrix experiments,
the identification of complexes of water with CO2 is
essential.
In the present paper, we will focus attention on the
hindered rotational motion of water molecules in solid
argon. After a brief description of the experimental
conditions, we will present the calculation of the cold
gas transitions. Then, experimental results will be
presented including temperature and time effects. An
assignment of the lines will be proposed. The last sec-
tion is devoted to identification of absorption lines of
CO2:H2O weakly bonded complexes through double
doping experiments with CO2. The results will be dis-
cussed in the light of recent data.
2. Experimental
The experimental setup has already been described
[18]. We only review here the main and specific fea-
tures. Ar and CO2 (L’Air Liquide – 99.995 % and
99.99 % respective purity) are used without purifica-
tion. Water is deionized, doubly distilled and care-
fully degassed. The gaseous mixture is obtained by
standard manometric procedures. As water is adsorbed
© Xavier Michaut, Anne-Marie Vasserot, and Luce Abouaf-Marguin, 2003
on the walls of the stainless steel part of the sample
system, we carefully passivated the system with a
pressure of water equal to its partial pressure in the
gas mixture. During deposition, we checked that wa-
ter absorptions were proportional to the amount of de-
posited gas mixture.
To study weakly bonded complexes, the relative
concentrations have to be carefully chosen [19]. For
molecules which do not react with each other, as is the
present case [10], more than the statistical number of
mixed pairs can be obtained by premixing the two
molecules with argon in the gas sample [20].
The samples were obtained by the slow spray-on
technique (10 mmol/h) of the gaseous mixture onto a
gold plated mirror held at 20 K. The solid sample is
then cooled to 6 K and annealed at least up to 30 K to
allow a reorganization of the polycristalline film (nar-
rowing of the lines) and a migration of molecular spe-
cies.
Absorption spectroscopy is performed using a
Bruker IFS 113V FTIR spectrometer, with a maxi-
mum resolution of 0.03 cm–1 and, for this resolution,
an accuracy better than 0.02 cm–1. Broad lines fre-
quencies are estimated within a 0.1 cm–1 precision.
3. Calculation of the «cold» gas transitions
As the rotation is almost free, a comparison with
the expected spectrum of the gas at 6 and 20 K is help-
ful for the transition assignments. The water mole-
cule, C2v symmetry type, is an asymmetric rotor, with
two magnetic species, ortho (spin degeneracy 3) and
para (spin degeneracy 1). In Fig. 1, the rovibrational
transitions are indicated for the three fundamental
bands of H2O, numbered in increasing frequencies of
the gas phase. At 20 K, the J = 0 and 1 energy levels are
the only ones sufficiently populated to give rise to de-
tectable absorptions. If the nuclear spin conversion were
fast, for the �2 mode, only the para line 4 should appear
at 6 K. But, as well known, the conversion is very slow
in low temperature matrices [21]. Then 2 other lines, the
ortho 3 and 5 ones, remain detectable, as long as
Boltzmann population of 20 K is trapped for some time
on the 101 ortho level. Using the intensities reported in
HITRAN96 data base [1], bar spectra can be calculated
at 20 and 6 K (graphs labeled G on Figs. 2).
4. Experimental results in the �2 region of H2O
We will now discuss in detail the �2 range and
then, give the results obtained with similar arguments
for the �1 and �3 bands. The observed frequencies,
measured with 0.03 cm–1 maximum resolution are in
Table 1, and compared to the most recent literature
data [16].
A typical spectrum of a sample H2O/Ar = 1/500
is presented in Fig. 2 at 20 and 6 K.
Temperature effect
The two lines at 1556.6 and 1573.2 cm–1 and the
broad structure around 1690 cm–1 which appear at
20 K, disappear totally at 6 K. The effect is reversible.
By comparison with the gas spectrum, it seems obvi-
ous that those structures correspond, respectively, to
lines 1, 2 and 6/7. Intensity comparisons with the gas
are also in favor of this interpretation, as it is known
that the matrix does not change dramatically the rela-
tive intensities of the transitions.
The vibration-rotation of H2O and its complexation with CO2 in solid argon revisited
Fizika Nizkikh Temperatur, 2003, v. 29, Nos. 9/10 1119
Fig. 1. Rovibrational transitions of the three modes of gas-
eous H2O at 20 K: �1 band (a); �2 band (b); �3 band (c);
J, Ka, Kc are the rotational quantum numbers of the asym-
metric rotator; S is the nuclear spin quantum number.
Table 1
Frequencies (cm–1) and assignments of absorption lines of
monomeric H2O in the �2 region in solid argon
Line Transition Magnetic
species
Gas [1] This work Perchard
[16]
1 1
11
�0
00
para 1557.611 1556.6a 1556.7
2 1
10
�0
01
ortho 1576.188 1573.2a 1573.1
1589.2c
(NRM)
3 1
01
�1
10
ortho 1616.714 1607.82b 1607.9
4 0
00
�1
11
para 1634.970 1623.72b 1623.8
5 1
01
�2
12
ortho 1653.268 1636.3b 1636.5
RTC
Rotation
translation
coupling
para
ortho
�
�
�
1657.4
1661.3
b
b
�
�
�
��
6 1
10
�2
21
ortho 1699.935 1697.8a 1661.4
7 1
11
�2
20
para 1706.355 1689.7a 1657.2
1687.6
1699.9
(Phonon
activation)
aMeasured at 20 K. bMeasured at 6 K. cNonrotating
molecule.
At this point, we would disagree with the conclu-
sions of previous work in solid argon [13–16] which
assign lines 6 and 7 to the double structure observed at
1660 cm–1. This does not seem possible since these
lines do not start from the lowest energy level. They
should disappear at 6 K, as lines 1, 2 and 6/7,
whereas this 1660 cm–1 double structure remains. On
the other hand, the 1690 cm–1 structure appears only
when the temperature is raised. Our very recent expe-
riments, at 20 K, with high optical density samples
[22], show that in this broad structure at 1690 cm–1,
which exhibits clearly two maxima (1689.7 and 1697.8
cm–1), the low frequency maximum decreases much
faster than the high frequency one as the temperature is
lowered. This low frequency shoulder corresponds then
to a transition from a level with a higher energy gap to
the fundamental than the high frequency one and should
be assigned to line 7. So the line at 1697.8 cm–1 corre-
sponds to transition 6. Those lines are broad, as the
1636.3 one, compared to lines 2, 4 and 5, because they
involve a J = 2 level which is more affected than levels
J = 0 or 1 by the coupling to the matrix.
1120 Fizika Nizkikh Temperatur, 2003, v. 29, Nos. 9/10
Xavier Michaut, Anne-Marie Vasserot, and Luce Abouaf-Marguin
Fig. 2. Spectra at 20 and 6 K of the �1, �2, �3 regions of H2O. G is the simulated bar spectrum of the gas, the numbers
refer to the transitions of Fig. 1; E is the experimental spectrum (H2O/Ar = 1/500) recorded with 0.15 cm–1 resolution,
just after deposition at 20 K (thickness � 250 �m), the arrows indicate the present assignments, RTC is the rotation-transla-
tion coupling structure and AS corresponds to the H2O dimmer; o and p are orthomagnetic and paramagnetic species.
At 6 K, the 1607.82, 1623.72 and 1636.3 cm–1 lines
correspond respectively to transitions 3, 4 and 5 in
agreement with previous assignments. Transition 5,
which involves a J = 2 level, is also broad.
So far, there is no obvious assignment for the dou-
ble structure at 1660 cm–1, which remains at 6 K, does
not vanish at 20 K, showing only a weak broadening.
By changing the concentrations, and upon annealing,
we have checked that its intensity is related to the
concentration of the monomer absorbers.
In Fig. 2, one additional line appears at 1592.94
cm–1, which corresponds to the dimer of H2O, in
agreement with previous work as we notice later on
Table 3 (see Sec. 6).
Furthermore, the line measured at 1589.2 cm–1
[16] may be assigned to nonrotating molecules
[13–16]. Whatever our experimental conditions, with
samples of pure H2O, this line was always very weak.
In section 6 of this paper, we will show that it is due
to the H2O:CO2 complex, since CO2 is generally pres-
ent as an impurity in the samples.
Time effect
As already mentioned, the nuclear spin conversion
from the ortho to the para form is slow in low tempe-
rature matrices [21]. The time evolution of the spectra
can confirm the assignments, since ortho lines should
decrease to the benefit of para lines, when starting
from nonequilibrated Boltzmann populations at 6 K.
Figure 3 exhibits these intensity changes after two
hours. The first spectrum is taken just after a fast
cooling from 30 K. Lines 3 and 5 decrease when 4 in-
creases, which is consistent with the assignments. In
the double structure near 1660 cm–1, the high fre-
quency part (1661.3 cm–1) decreases and the low fre-
quency one (1657.4 cm–1) increases correlatively.
This structure presents an ortho and a para compo-
nents, is situated between 50 and 100 cm–1 far from
the pure vibrational frequency and remains at 6 K. It
does not belong to the rovibrational structure, but is
related to the number of rotating molecules. It may
then be a manifestation of the rotation-translation
coupling (RTC) involved in the movement of the mo-
lecule in its cage [23].
The weak lines at 1592.94 and 1610.12 cm–1 are due
to dimers (Table 3). The line 1610.12 cm–1 is hidden
in the high frequency wing of line 3 in Fig. 2 but
appears after annealing to 30 K (Fig. 3).
5. Experimental results in the �1 and �3 regions
of H2O
The 3600–3800 cm–1 region is represented in Fig. 2
at 20 and 6 K (H2O/Ar = 1/500), together with the
calculated gaseous bar spectra. With the same argu-
ments as for �2, we present the assignments in Table 2,
which agree with the most recent work [16].
Table 2
Frequencies (cm–1) and assignments of absorption lines of
monomeric H2O in the �1 and �3 region in solid argon
Line Transition Magnetic
species
Gas [1] This work Perchard
[16]
�
1
band
1 1
10
�1
01
ortho 3638.082 3622.4a 3622.7
3638.3c
(NRM)
2 1
01
�1
10
ortho 3674.697 3653.38b 3653.5
3 0
00
�1
11
para 3693.294 3669.85b 3669.7
�
3
band
1 1
01
�0
00
ortho 3732.135 3711.2a 3711.3
2 1
10
�1
11
ortho 3749.331 3724.7a 3724.9
3736.0c
(NRM)
3 1
11
�1
10
para 3759.845 3739.4a 3739.0
4 0
00
�1
01
para 3779.493 3756.49b 3756.6
6 1
01
�2
02
ortho 3801.420 3776.30b 3776.4
7 1
10
�2
11
ortho 3807.014 3784.5a
aMeasured at 20 K. bMeasured at 6 K. cNonrotating
molecule.
The vibration-rotation of H2O and its complexation with CO2 in solid argon revisited
Fizika Nizkikh Temperatur, 2003, v. 29, Nos. 9/10 1121
Fig. 3. Time effect in the �2 region of H2O, due to nuclear
spin conversion at 6 K. The spectra (H2O/Ar = 1/1000)
are recorded with 0.15 cm–1 resolution, after annealing at
30 K (thickness � 220 �m) after a time t = 0 (a) and 2
(b) hours; the numbers refer to the transitions of Fig. 1;
(c) presents the difference of spectra (a) and (b), o and p
are orthomagnetic and paramagnetic species.
However, two points should be noted: i) the lines
involving a J = 2 level are not as broad as in the �2
case, ii) there is no evidence of a RTC structure as ob-
served for �2.
This could be explained by a coupling of the
rotation-vibration to the translation in the cage
weaker for the stretching modes �1, �
than for the
bending mode �2.
Some dimeric species are also observed in this fre-
quency range. The measured frequencies (see Table 3)
are in good agreement with the literature [16].
6. Double doping experiments with CO2: the
complex
H2O frequency ranges
To look at the H2O:CO2 complex near H2O absorp-
tions, the sample should be concentrated in CO2 [19].
However, as CO2 has a great tendency to form poly-
mers, its concentration should be kept low enough to
avoid aggregates of H2O with more than one CO2 mo-
lecule. In Fig. 4, we can compare typical spectra ob-
tained with a sample of pure H2O (spectrum P —
H2O/A = 1/500) to spectra of CO2 double doped
samples (spectra D1 — H2O/CO2/Ar = 10/5/5000
and D2 — H2O/CO2/Ar = 10/2/5000), recorded
with 0.03 cm–1 resolution. The spectra were recorded at
6 K, after an annealing at 30 K, which enhances the
complex absorptions. Some new lines appear in the
double doped experiment due to the simultaneous pres-
ence of H2O and CO2. As the dilutions remain high
enough, there is a weak probability of trimolecular
species. With the H2O dimer absorptions, for the
H2O:CO2 complex, the most intense narrow structures
which can be measured are indicated in Table 3. By
varying the relative concentration of CO2, we have
checked that the behavior of these lines is consistent
with a 1:1 pair, as they grow proportionally with the
concentration of CO2 for a given concentration of
H2O. Our results are compared in Table 3 with the
recent ones of Svensson et al. [24].
Table 3
Most intense observed lines (cm–1) of H2O dimer and
H2O:CO2 complex isolated in solid argon
Line
H
2
O:H
2
O H
2
O:CO
2
This work Perchard [16] This work Svensson
et al. [24]
H
2
O (v1) 3574.77
3633.22
3574.0 (PD)
3633.1 (PA)
3638.0
3632.7
H
2
O (v2)
1592.94
1610.12
1593.1 (PA)
1610.6 (PD)
1589.48
1589.86
1590.54
1593.1
H
2
O (v3) 3708.5
3738.1
3708.0 (PD)
3715.7 (PA)
3737.8 (PA)
3732.46 3732.9
CO
2
(v2)
656.03
667.95
668.05
656.0
668.0
CO
2
(v3) 2340.20 2340.5
PA: proton acceptor; PD: proton donor.
In the H2O �1 range, beside the combination bands
(2����
) of CO2 reported by Schriver et al. [25]
around 3596.9 and 3602.98 cm–1, only a weak line due
to the double presence of H2O and CO2 can be de-
1122 Fizika Nizkikh Temperatur, 2003, v. 29, Nos. 9/10
Xavier Michaut, Anne-Marie Vasserot, and Luce Abouaf-Marguin
Fig. 4. Double doping with CO2: water regions at 6 K. The
spectra are recorded with 0.03 cm–1 resolution, after anneal-
ing at 30 K; P is a pure H2O sample (H2O/Ar = 10/5000,
thickness � 60 �m); D1 and D2 are the double doped sam-
ples (D1: H2O/CO2/Ar = 10/5/5000, thickness � 80 �m;
D2: H2O/CO2/Ar = 10/2/5000, thickness � 60 �m).
tected at 3638 cm–1. Near �2, two clear structures ap-
pear at 1589.48 cm–1, with shoulders at 1589.04 and
1589.81 cm–1 and a narrower line at 1589.86 cm–1.
The broad and weak absorptions around 1591.5 and
1591.8 cm–1 are also due to the presence of CO2. The
spectra, for the �3 mode, exhibit clearly a broader ab-
sorption at 3732.46 cm–1 close to the combination
bands (�
��
) of CO2 [25].
The number of these absorptions, especially for the
�2 mode of H2O, is probably due to multiple trapping
sites for the complex and different geometries, as the
vibrational modes of H2O are not degenerate. The
broad structures could be due to very perturbed crys-
talline double cages.
CO2 frequency ranges
In typical experiment presented in Fig. 5, the sam-
ples are more dilute in CO2 (spectra P: CO2/Ar =
= 1/5000 and D: CO2/H2O/Ar = 1/10/5000). The
striking new features are: one narrow structure at
668.05 cm–1 (with a shoulder at 667.95 cm–1), a much
weaker broad one at 656.03 cm–1 in the �2 range, and
one narrow line at 2340.20 cm–1 in the �3 range. These
results are consistent with those reported in the litera-
ture [24]. We should mention that the line at
2340.2 cm–1 had already been assigned to this complex
by Guasti et al. [26] in 1978, in experiment on CO2 in
solid argon, for which an amount of water was present
due to a leak in the system.
7. Conclusion
Our new experimental data has led to some new as-
signments of the rovibrational frequencies of H2O on
the �2 mode, and the absorptions of the H2O:CO2
complex in the H2O regions in argon matrix. From our
refined measurements of rovibrational frequencies, the
«effective» rotational constants of water trapped in
solid argon may be determined. Furthermore, our ex-
perimental results will support calculations able to ex-
plain the RTC structure. For the complex with CO2,
some more experimental work is needed to understand
the different trapping sites and structures. A modeling
similar to that developed for the CO:CO2 complex
[27] will be attempted.
Acknowledgments
The authors acknowledge Louise Schriver-Mazzuoli
for helpful discussions.
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1124 Fizika Nizkikh Temperatur, 2003, v. 29, Nos. 9/10
Xavier Michaut, Anne-Marie Vasserot, and Luce Abouaf-Marguin
|
| id | nasplib_isofts_kiev_ua-123456789-128939 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 0132-6414 |
| language | English |
| last_indexed | 2025-11-27T14:18:26Z |
| publishDate | 2003 |
| publisher | Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України |
| record_format | dspace |
| spelling | Michaut, Xavier Vasserot, Anne-Marie Abouaf-Marguin, Luce 2018-01-14T13:18:29Z 2018-01-14T13:18:29Z 2003 The vibration-rotation of H₂O and its complexation with CO₂ in solid argon revisited / Xavier Michaut, Anne-Marie Vasserot, Luce Abouaf-Marguin // Физика низких температур. — 2003. — Т. 29, № 9-10. — С. 1118-1124. — Бібліогр.: 27 назв. — англ. 0132-6414 PACS: 33.15.Mt, 33.20.Ea, 33.20.Vq https://nasplib.isofts.kiev.ua/handle/123456789/128939 Fourier-transform infrared spectroscopy in the frequency range 400–4000 cm–¹ has been used to investigate the absorption of H₂O and H₂O:CO₂ complex isolated in solid argon. Thanks to the lowest temperature reached in our experiment, temperature effects and nuclear spin conversion studies allow us to propose a new assignment of the rovibrational lines in the bending band n₂ for the quasi-freely rotating H₂O. An additional wide structure observed in this band shows two maxima around 1657.4 and 1661.3 cm–¹, with nuclear spin conversion of the high frequency part into the low frequency one. This structure is tentatively attributed to a rotation-ranslation coupling of the molecule in the cage. However, the equivalent effect is not observed in the vibrational stretching bands n₁ and n₃. Finally, by double doping experiments with CO₂, important new structures appear, leading us to unambiguously extract the frequencies of the lines of the H₂O:CO₂ complex. The authors acknowledge Louise Schriver-Mazzuoli for helpful discussions. en Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України Физика низких температур Spectroscopy in Cryocrystals and Matrices The vibration-rotation of H₂O and its complexation with CO₂ in solid argon revisited Article published earlier |
| spellingShingle | The vibration-rotation of H₂O and its complexation with CO₂ in solid argon revisited Michaut, Xavier Vasserot, Anne-Marie Abouaf-Marguin, Luce Spectroscopy in Cryocrystals and Matrices |
| title | The vibration-rotation of H₂O and its complexation with CO₂ in solid argon revisited |
| title_full | The vibration-rotation of H₂O and its complexation with CO₂ in solid argon revisited |
| title_fullStr | The vibration-rotation of H₂O and its complexation with CO₂ in solid argon revisited |
| title_full_unstemmed | The vibration-rotation of H₂O and its complexation with CO₂ in solid argon revisited |
| title_short | The vibration-rotation of H₂O and its complexation with CO₂ in solid argon revisited |
| title_sort | vibration-rotation of h₂o and its complexation with co₂ in solid argon revisited |
| topic | Spectroscopy in Cryocrystals and Matrices |
| topic_facet | Spectroscopy in Cryocrystals and Matrices |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/128939 |
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