Luminescence and formation of alkalihalide ionic excimers in solid Ne and Ar
Transitions from ionic states A²⁺X– of alkalihalides CsF, CsCl and RbF isolated in solid Ne and Ar films recorded under pulsed e-beam excitation are studied. The B(²∑₁/₂)-X(²∑₁/₂) and C(²П₃/₂)-A(²П₃/₂) luminescence bands of Cs2+F– (196.5 nm, 227 nm), Cs²⁺Cl– (220.1 nm, 249.2 nm) and Rb²⁺F– (136 nm)...
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nasplib_isofts_kiev_ua-123456789-1289382025-02-09T22:44:44Z Luminescence and formation of alkalihalide ionic excimers in solid Ne and Ar Śliwiński, G. Frankowski, M. Schwentner, N. Spectroscopy in Cryocrystals and Matrices Transitions from ionic states A²⁺X– of alkalihalides CsF, CsCl and RbF isolated in solid Ne and Ar films recorded under pulsed e-beam excitation are studied. The B(²∑₁/₂)-X(²∑₁/₂) and C(²П₃/₂)-A(²П₃/₂) luminescence bands of Cs2+F– (196.5 nm, 227 nm), Cs²⁺Cl– (220.1 nm, 249.2 nm) and Rb²⁺F– (136 nm) in Ne, and a weakerB–X emission of Cs²⁺F– (211.2 nm) in Ar are identified. For CsF the depopulation of the A²⁺X– state is dominated by the radiative decay. A ratio of the recorded exciplex emission intensities of I(CsF)/I(CsCl)/I(RbF) = 20/5/1 reflects the luminescence efficiency and for RbF and CsCl a competitive emission channel due to predissociation in the A²⁺X⁻(B²∑₁/₂) state is observed. For these molecules an efficient formation of the state X*₂ is confirmed through recording the molecular D`(³П₂g)-A`(³П₂u) transition. A strong dependence of the luminescence intensities on the alkalihalide content reveals quenching at concentrations higher than 0.7%. 2003 Article Luminescence and formation of alkalihalide ionic excimers in solid Ne and Ar / G. Śliwiński, M. Frankowski, N. Schwentner // Физика низких температур. — 2003. — Т. 29, № 9-10. — С. 1113-1117. — Бібліогр.: 18 назв. — англ. 0132-6414 PACS: 78.45.+h, 78.55.Fv https://nasplib.isofts.kiev.ua/handle/123456789/128938 en Физика низких температур application/pdf Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України |
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Spectroscopy in Cryocrystals and Matrices Spectroscopy in Cryocrystals and Matrices |
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Spectroscopy in Cryocrystals and Matrices Spectroscopy in Cryocrystals and Matrices Śliwiński, G. Frankowski, M. Schwentner, N. Luminescence and formation of alkalihalide ionic excimers in solid Ne and Ar Физика низких температур |
| description |
Transitions from ionic states A²⁺X– of alkalihalides CsF, CsCl and RbF isolated in solid Ne and Ar films recorded under pulsed e-beam excitation are studied. The B(²∑₁/₂)-X(²∑₁/₂) and C(²П₃/₂)-A(²П₃/₂) luminescence bands of Cs2+F– (196.5 nm, 227 nm), Cs²⁺Cl– (220.1 nm, 249.2 nm) and Rb²⁺F– (136 nm) in Ne, and a weakerB–X emission of Cs²⁺F– (211.2 nm) in Ar are identified. For CsF the depopulation of the A²⁺X– state is dominated by the radiative decay. A ratio of the recorded exciplex emission intensities of I(CsF)/I(CsCl)/I(RbF) = 20/5/1 reflects the luminescence efficiency and for RbF and CsCl a competitive emission channel due to predissociation in the A²⁺X⁻(B²∑₁/₂) state is observed. For these molecules an efficient formation of the state X*₂ is confirmed through recording the molecular D`(³П₂g)-A`(³П₂u) transition. A strong dependence of the luminescence intensities on the alkalihalide content reveals quenching at concentrations higher than 0.7%. |
| format |
Article |
| author |
Śliwiński, G. Frankowski, M. Schwentner, N. |
| author_facet |
Śliwiński, G. Frankowski, M. Schwentner, N. |
| author_sort |
Śliwiński, G. |
| title |
Luminescence and formation of alkalihalide ionic excimers in solid Ne and Ar |
| title_short |
Luminescence and formation of alkalihalide ionic excimers in solid Ne and Ar |
| title_full |
Luminescence and formation of alkalihalide ionic excimers in solid Ne and Ar |
| title_fullStr |
Luminescence and formation of alkalihalide ionic excimers in solid Ne and Ar |
| title_full_unstemmed |
Luminescence and formation of alkalihalide ionic excimers in solid Ne and Ar |
| title_sort |
luminescence and formation of alkalihalide ionic excimers in solid ne and ar |
| publisher |
Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України |
| publishDate |
2003 |
| topic_facet |
Spectroscopy in Cryocrystals and Matrices |
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| citation_txt |
Luminescence and formation of alkalihalide ionic excimers in solid Ne and Ar / G. Śliwiński, M. Frankowski, N. Schwentner // Физика низких температур. — 2003. — Т. 29, № 9-10. — С. 1113-1117. — Бібліогр.: 18 назв. — англ. |
| series |
Физика низких температур |
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AT sliwinskig luminescenceandformationofalkalihalideionicexcimersinsolidneandar AT frankowskim luminescenceandformationofalkalihalideionicexcimersinsolidneandar AT schwentnern luminescenceandformationofalkalihalideionicexcimersinsolidneandar |
| first_indexed |
2025-12-01T11:59:27Z |
| last_indexed |
2025-12-01T11:59:27Z |
| _version_ |
1850307110845284352 |
| fulltext |
Fizika Nizkikh Temperatur, 2003, v. 29, Nos. 9/10, p. 1113–1117
Luminescence and formation of alkalihalide ionic
excimers in solid Ne and Ar
G. Œliwiñski and M. Frankowski
Polish Academy of Sciences, IF-FM, Fiszera 14, PL 80-952 Gdansk, Poland
E-mail: gerards@imp.gda.pl
N. Schwentner
Institute of Experimental Physics, Free University, Arnimallee 14, Berlin D-14195, Germany
Transitions from ionic states A2+X– of alkalihalides CsF, CsCl and RbF isolated in solid Ne and
Ar films recorded under pulsed e-beam excitation are studied. The B /( )2
1 2� –X /( )2
1 2� and
C /( )2
3 2� –A /( )2
3 2� luminescence bands of Cs2+F– (196.5 nm, 227 nm), Cs2+Cl– (220.1 nm, 249.2
nm) and Rb2+F– (136 nm) in Ne, and a weaker B–X emission of Cs2+F– (211.2 nm) in Ar are iden-
tified. For CsF the depopulation of the A2+X– state is dominated by the radiative decay. A ratio of
the recorded exciplex emission intensities of I(CsF)/I(CsCl)/I(RbF) = 20/5/1 reflects the lu-
minescence efficiency and for RbF and CsCl a competitive emission channel due to predissociation
in the A X2 2
1 2
� �( )B /� state is observed. For these molecules an efficient formation of the state X2
� is
confirmed through recording the molecular � � �D Ag u( ) ( )3
2
3
2� � transition. A strong dependence of
the luminescence intensities on the alkalihalide content reveals quenching at concentrations higher
than 0.7%.
PACS: 78.45.+h, 78.55.Fv
1. Introduction
Luminescence of ionic excimers covers the VUV
and deep UV wavelength region and represents an in-
teresting perspective for an extension of the gas phase
excimer media towards shorter wavelengths. Since the
first considerations around 1985 [1,2] the ionic sys-
tems are extensively investigated. Spectroscopic stud-
ies in the gas phase provided emission from ionic states
A2+X– of alkalihalides (AX), and from diatomic
(RgA)+ and triatomic (Rg2A)+ rare gas alkali ions
[3–8]. Optical gain has been achieved [9], however,
the recent kinetic studies indicate quenching processes
which can seriously limit amplification [10].
The electronic configurations for the family of
alkalihalide ions (AX)+ correspond to those of rare
gas halides RgX in the ground state and correlate to
the atomic states A+(1S) and X(2P). Also the
ionically bound upper states (A2+X–) due to transfer
of an alkali 5p-core electron to the halogen are
isoelectronic to Rg+X– exciplex states with similar po-
tential surfaces and correlate to A2+(2P) and X–(1S)
atomic states. Since the potential of the lower (AX)+
state has a dissociative character it is anticipated, that
population inversion can be obtained in these systems.
The upper bound state can be directly populated by
photoionization of AX. Radiative transitions with
large cross-section for stimulated emission and short
radiative lifetimes of the order of 1 ns can be expected
for A2+X–. These ions considered in the condensed
phase combine the favorable properties of the short
wavelength, strong excimer emissions known from the
gas phase with the high number densities of excited
states attainable in the solid.
Recently deep UV fluorescence bands of A2+X–
ions were observed for CsF, CsCl and RbF isolated in
Ne and Ar matrices under e-beam excitation [11,12].
It was shown, that the exciplex states B /
2
1 2� and
X /
2
3 2� are effectively populated via host excitons
resulting mainly in the B X/ /
2
1 2
2
1 2� �� emission.
Also a much weaker C A/ /
2
3 2
2
3 2� �� transition
for the ionic states of CsF and CsCl was observed. The
observed transitions were red shifted compared to the
gas phase due to interaction with the dielectric host.
The first indication for the homonuclear � � �D A transi-
tion of Cl2
� and F2
� was reported and ascribed to
predissociation via the A+X� state [13].
© G. Œliwiñski, M. Frankowski, and N. Schwentner, 2003
1114 Fizika Nizkikh Temperatur, 2003, v. 29, Nos. 9/10
In this work the spectroscopic data and formation
of the ionic states A2+X– of alkalihalides: CsF, CsCl
and RbF isolated in thin Ne and Ar films, are studied.
Conclusions on the formation efficiency of X2
� mole-
cules due to predissociation in the A2+X–(B /
2
1 2� )
state of RbF and CsCl following from the concentra-
tion dependent measurements are discussed.
2. Transitions from alkalihalide ionic states
For understanding of the excitation and decay pro-
cesses it is instructive to consider the energy level
scheme of the alkalihalide states involved in the ob-
served radiative transitions. Since the problem was dis-
cussed for the CsCl elsewhere [12] here just features
will be recalled which are valid for the general case of
the A+X– ionic states. For this purpose it is convenient
to consider the energy of states in units equal to the
binding potential of the AX ground state and the
internuclear separation in units of equilibrium distance
re – see Fig. 1. The states relevant for discussion are de-
scribed by potential curves and for the other ones only
positions of the dissociation limits are given. The rare
gas excitons formed in the host by the pulsed electron
beam are responsible for the A+(1S) core ionization of
the 1� ground state of AX molecules (an upward arrow
in Fig. 1). Due to the equilibrium distance re in this
state the higher vibrational levels ��� of the
A2+(2P)X–(1S) state are populated, and a fast radia-
tionless relaxation to the ��� = 0 level occurs because of
the low temperature around 5 K. It is followed by the
bound-free radiative transition
A X AX2� � � �( ) h� (1)
to the repulsive part of the lower X /
2
1 2� potential
and characterized by the emission of UV photons on a
time scale close to one nanosecond (a downward ar-
row, Fig. 1). Energy wise population of the closely
spaced B and C states of A2+X– is equally likely and
emissions from these states are observed in contrary
to the D state which lies higher in energy by the
2
3 2
2
1 2P P/ /� spin-orbit splitting of the A2+ ion.
The bound states, i.e. the ground state 1�, the
A+X*, and the ionic B /
2
1 2� , potential curves in Fig. 1
are based on the truncated Rittner potential (at 1/r4)
with the effect of the dielectric host taken into ac-
count by introducing the1/
factor into the coulombic
and 1/r4 terms. Bond lengths and polarizabilities are
taken from literature [4,14]. For the lower A+X state
the Born–Mayer potential
V r r re( ) exp[ ( )]� � �
�0 0 (2)
is used with the assumption that the consideration re-
fers to the vicinity of the equilibrium distance re,
with
0 being the energy of the lower state at r = re.
The shape of V(r) and also the
0 and �0 values are
derived from experimental data for the gas phase
B–X transitions of A2+X– ions. The potential minima
of the X /
2
1 2� states are taken equal to their gas
phase counterparts [4].
The transition energies observed in experiment are
red shifted by
E relative to the gas phase. This can be
explained by means of the cavity shell model for a
transition dipole moment
� given by the relation
( ) ( )
�
2 3� C Ed (3)
with C /( ) . ( ) ( )
� � �0125 2 1 1 , d corresponding to
the cavity diameter, and
being the dielectric constant
of the surrounding. The measured
E values yield the
estimates for
� and the measured transition energies
result in potential minima of the upper A2+X–(B /
2
1 2� )
states with the red shifts reflecting the solvation energy
of the ionic states of AX molecules.
For CsCl and RbF it can be deduced from Fig. 1,
that the Frank—Condon region corresponding to the
G. Šliwiòski and M. Frankowski, N. Schwentner
1
0
1
2
3
4
5
0.7 1.0 1.3 1.7 2.0 �
E
n
e
rg
y,
a
rb
.u
n
its
( P)2
A++ X ( S)1+
A+ + +X
+XA +
A+*+ X
A+( S)1
+X ( P)2*
A+( S)1
+
+
X
( S)1
A+( S)1
X
( P)2
VUV/UV Iuminescence
B2
�1/2
�1/2X2
�0
1
excitation
Internuclear distance, re
Fig. 1. The potential energy diagram of the alkalihalides;
energy and internuclear separation are in units of the
ground state binding potential, and re, respectively; the
relevant states are described by the shell configurations
and for the other ones only the energetic positions at
r � � are given; states C2� and A2� resulting from the
spin-orbit splitting of the upper and lower excimer state,
respectively, are not shown for simplicity. Selective exci-
tation of the ground state A+X– molecule is provided by
the e-beam via rare gas excitons — dashed arrow. The ra-
diative decay follows a fast radiationless relaxation to the
� �� 0 level of the A2+X– ionic bound state.
excitation of the 1� state falls close to the crossing
point of the A2+X– and A+X� potential surfaces. This
indicates predissociation of the A2+X– state as the
probable depopulation channel due to the reaction
A2+X–
A+ + X�
(4)
which is accompanied by a partial, nonradiative en-
ergy loss. Similar to the gas phase results [5] the com-
peting predissociation effect is only observed for CsCl
and RbF doped samples and in both cases the X2
� mo-
lecular emission
X X2 2
� � �h h h� � �1 1, (5)
occurs. However, in the host a strong cage effect traps
the excited X* atoms in the lattice. This leads to a de-
crease of the population of X2 molecules finally formed
in the ground state. For CsF doped samples the X2
�
emission was not observed so in the matrix as well as
in the gas phase. The difference in separations of the
crossing point of A2+X– and A+X* potentials from the
bottom of the 1� potential (re = 1) in Fig. 1, and also
the longer radiative lifetime of the C state explain the
low intensity of the C–A band for CsF and CsCl in Ne
obtained from experiment. The spectroscopic data of
the observed ionic transitions for RbF, CsCl, and CsF
are calculated following the procedure described previ-
ously [15], and are given in Table.
Table
Spectroscopic properties of matrix isolated, core excited
RbF, CsF and CsCl alkalihalides in the VUV and deep UV
spectral range: �em — peak position, fwhm — halfwidth,
� s — cross section for stimulated emission, and �f —
radiative lifetime
Molecule,
transition
Matrix
�em,
nm
fwhm,
nm
� s,
10–16 cm2
�r,
ns
Rb++F–
B X� Ne 136 4.5 1.5 0.9
Cs++F–
B X� Ne 196.5 9.5 2.5 1.2
C A� Ne 227.1 15 0.22 11.3
B X� Ar 211.2 11.3 2.74 0.8
Cs++Cl–
B X� Ne 220.1 10.4 2.22 1.4
C A� Ne 249.2 14.8 0.29 12.6
As the most of data obtained refer to the Ne host a
comment should be added for the transition energies
observed in the solid. These are shown as the ma-
trix-dependent (Ne, Ar, or Kr) peak positions of the
emission bands together with respective data from gas
phase measurements and those of the solid state XeF
excimer for reference – Fig. 2. The peak positions are
given for optimal contents of the alkalihalides CsF
(0.45% in Ar, and 0.7% in Ne), CsCl (0.37%), and
RbF (0.6%) in solid Ar and Ne films. The variable
( ) ( )
� �1 2 1/ describes the host interaction and
slanted lines connect data of the same dopant. In com-
parison to the gas phase results [5] the matrix shift of
the B X� luminescence from the ionic states of RbF,
CsF and CsCl has a value of 0.43, 0.39 and 0.33 eV,
respectively. This is in a good agreement with values
of 0.3–0.4 eV predicted from relation (3) and coin-
cides with the results obtained for the XeF excimer in
solid Ne and Ar [15,16]. Moreover, the values ob-
tained so far from experiment (solid data points) al-
low to deduce the estimates of transition energies for
Luminescence and formation of alkalihalide ionic excimers in solid Ne and Ar
Fizika Nizkikh Temperatur, 2003, v. 29, Nos. 9/10 1115
Ne
Matrix
Ar
Kr
0
4
5
6
7
8
9
10
Rb F (B X)++
Cs F (B X)++
Cs Cl (B X)++
Cs F (C A)++
Cs Cl (C A)++
+Xe F (D X)
0.1 0.2
( 1)/(2 + 1)
Fig. 2. The matrix-dependent transition energies of the
e-beam excited CsF, CsCl, and RbF in Ar and Ne solid
films for the optimal alkalihalide concentrations, and XeF
data for reference; values for ( ) ( )
� � �1 2 1 0/ correspond
to the gas phase data already measured (solid data points)
and postulated (hollow points).
1116 Fizika Nizkikh Temperatur, 2003, v. 29, Nos. 9/10
emission bands not observed yet in the solid and in the
gas phase as well (hollow data points).
3. The concentration effect
The measured intensities of the B–X band are highly
sensitive to changes in the original sample composition.
Dependences of the peak intensity values versus the dop-
ant concentrations in Ne films presented in the form of
experimental data sets for CsF, RbF (up and down tri-
angles), and CsCl (squares) are summarized in Fig. 3.
The dependence observed for CsCl is more pronounced
than for CsF and for RbF only two data points are avail-
able due to the relatively low signal. In all cases the op-
timal alkalihalide content corresponding to the maxi-
mum band intensity lies around 0.6–0.8% and is in
accordance with the data obtained for the gas phase [4]
and also coincides with those from our previous results
reported for XeF [15,16]. A comparison of the band in-
tensities for the optimal concentrations related to the
highest one (CsF) lead to the ratio of
I(CsF)/I(CsCl)/I(RbF) = 20/5/1 and reflects the
energy transfer efficiency for the investigated species. In
the case of CsF a change of the concentration dependent
intensity of almost two orders of magnitude is observed.
The data for CsCl indicate on weaker concentration de-
pendence for samples doped below optimum than for the
higher doped ones. In the low doping range exclusively
an occurrence of the predissociation of molecules in the
ionic state can be observed. This is confirmed by the de-
tailed analysis of the CsF and CsCl spectra reported
elsewhere [11,12]. The relevant decay channels of the
Cs2+Cl–( )B /
2
1 2� state become more evident when the
� � �D Ag u( ) ( )3
2
3
2� � transition of the Cl2
� molecule
is taken into account. An appearance of the molecular
emission can only be observed for CsCl content not ex-
ceeding values of about 0.6–0.7%. The intensity of this
transition is even much larger from that of B–X for
lower concentrations, around 0.1–0.2 %. This together
with a decrease of the Cl2
� band intensity for CsCl con-
tent increasing in that range reflects a strong competi-
tion between the deep UV emission and the concentration
quenching process which is due to short-range energy mi-
gration, aggregation and also self-absorption by the ground
state CsCl( )1� molecules. For a concentration increase in
the range from about 0.4 up to 0.9% the optimal values
of the dopant content correspond to the highest band in-
tensities. The AX content larger than 0.9% results in a
decrease of the B–X band intensities. Moreover, in that
doping region a rapid growth of the intrinsic fluores-
cence bands originating from aggregates occurs. In the
case of CsF the concentration quenching seems to repre-
sent the main negative contribution to the emission effi-
ciency of the excimer band. In general, the effect ob-
served most clearly for CsCl is representative for the
decay of (AX)+ states of alkalihalides in general. This is
supported by the similar concentration dependences of
the band intensities observed for CsF and in part for
RbF, too [17,18].
4. Conclusion
The favorable population of the A2+X– state of
alkalihalides by ionization of the trapped AX mole-
cules via host excitons of solid Ne and Ar can be de-
duced from the energy level scheme and is confirmed
experimentally. The B X/ /( ) ( )2
1 2
2
1 2� �� radiative
transition from ionic states represents the most effi-
cient depopulation channel for e-beam excited, rare
gas matrix-isolated CsF, CsCl and RbF. Also the
much weaker emission bands C A( ) ( )2 2� �� of
Cs2+F– and Cs2+Cl– occur besides the intrinsic lumi-
nescence bands of aggregates. For RbF and CsCl the
concentration dependent formation of X2
� molecules
due to predissociation in the A2+X–( )B /
2
1 2� state is
observed in experiment. The resulting molecular tran-
sition �D g( )3
2� – �A u( )3
2� competes efficiently with
the exciplex emissions at low doping concentrations
around 0.1%. A strong dependence of the emission in-
tensities on the alkalihalide content leads to aggrega-
G. Šliwiòski and M. Frankowski, N. Schwentner
a
b
CsF
CsCl
RbF
CsCl solid
Cl 2*
10
10
4
3
0
0.1
0.1 1
1
Concentration, %
In
te
n
si
ty
(c
o
u
n
ts
)
1
2
Fig. 3. Emission intensities of the B X� transition of the
A2+X– exciplexes vs. the AX concentration in Ne solid
films for CsF (�), CsCl (�) and for RbF (�) (a), and
the case of CsCl doped Ne sample; luminescence intensi-
ties of the Cl2
� molecular transition � � �D Ag u( ) ( )3
2
3
2� �
and of the intrinsic band of CsCl aggregates (245 nm), re-
lated to the B X/ /
2
1 2
2
1 2� �� band intensity vs. concen-
tration (b); concentrations are percentages and intensities
are the peak values measured.
tion and quenching at doping concentrations higher
than the optimal range of about 0.7 %. Marked differ-
ence in the B–X emissions intensities observed for
alkalihalides CsF, CsCl and RbF is explained by the
position of the crossing point of the A2+X– and A+X*
potential surfaces relative to the equilibrium
internuclear separation of the A+X- ground state. The
condensed phase ionic excimer Cs2+F– represents the
best emission properties compared to Cs2+Cl– and
Rb2+F–. This is demonstrated by the B–X fluorescent
transition dominating the excited state decay and also
the fluorescence intensity exceeding those of Cs2+Cl–
and Rb2+F– by a factor of about 6 and 20, respectively.
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