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Phys. Status Solidi B 247, No. 6, 1424–1447 (2010) / DOI 10.1002/pssb.200983195 b
www.pss-b.com
basic solid state physics
Institut für Angewandte Physik, Karlsruher Institut für Technologie (KIT), Wolfgang Gaede Str. 1, 76131 Karlsruhe, Germany
* Corresponding author: e-mail claus.klingshirn@kit.edu, Phone: þ49 (0)721 608 3417, Fax: þ49(0)721 608 8480
The research on ZnO has a long history but experiences an properties identical to bulk samples and end in several cases
extremely vivid revival during the last 10 years. We critically with data on quantum wells or nano crystallites. Since it is a
discuss in this didactical review old and new results concen- didactical review, we present explicitly misconceptions found
trating on optical properties but presenting shortly also a few frequently in submitted or published papers, with the aim to
aspects of other fields like transport or magnetic properties. We help young scientists entering this field to improve the quality of
start generally with the properties of bulk samples, proceed then their submitted manuscripts. We finish with an appendix on
to epitaxial layers and nanorods, which have in many respects quasi two- and one-dimensional exciton cavity polaritons.
1 Introduction Zinc oxide (ZnO) is a wide gap This huge number of publications makes it completely
semiconductor [Eg(0 K) ¼ (3.441 0.003) eV; Eg(300 K) impossible to cite or even to read all relevant ones for this
¼ (3.365 0.005) eV]. It belongs to the group of IIb-VI contribution. We restrict ourselves therefore to a small,
compound semiconductors. It crystallizes almost exclu- partly arbitrary selection of references, refer the reader for
sively in the hexagonal wurtzite type structure (point group more e.g. to the databases mentioned above or the more recent
C6v or 6 mm, space group C46v or P63mc). Compared to ones of the reviews and apologize for this shortcoming.
similar IIb–VI (e.g. ZnS) or III–V (e.g. GaN) semiconductors After this introduction, we shortly review some aspects
it has a relatively strong polar binding and a relatively large of present and future applications, growth, doping, electronic
exciton binding energy of (59.5 0.5) meV. Due to the light transport, band structure and deep centre luminescence.
mass of oxygen, the up most LO phonon has a relatively high Then we present in more detail linear and nonlinear optical
energy of 72 meV. The density of ZnO is 5.6 gcm3 properties close to the fundamental absorption edge,
corresponding to 4.2 1022 ZnO molecules per cm3. including lasing and stimulated emission as well as
These data can be found e.g. in a recent data collection dynamics. The contribution closes with a short outlook,
[1] and references therein. followed by an appendix in which we comment recent work
ZnO is a long known semiconductor, with research going on quasi one- and two-dimensional cavities.
back to the first quarter of the last century. The time
mentioned in the title of this paper is simply based on the fact 2 Applications The present world wide research
that the oldest references which are cited here are from the activities on ZnO, its alloys Zn1xAxO (with A ¼ Cd, Mg
year 1944. or Be) and on nano- or quantum structures based on them, are
The research history, with peaks occurring from time to driven by various hopes. The predominant one is possibly
time, is documented apart from many scientific papers by a the hope to obtain a material for optoelectronics covering the
large number of review articles and books, from which we give spectral range from the green (A ¼ Cd) over the blue to the
here a selection [2–10, 12–16]. During the last 5 to 10 years, the near UV (A ¼ Mg or Be), especially to obtain light emitting
research on ZnO experiences a very vivid renaissance (or (LED) or laser diodes (LD) in these spectral ranges. ZnO
hype) with more than 2 000 ZnO relevant papers per year. could in case of success supplement or replace the GaN-
The total number of these papers exceeds 26 000 as indicated based devices. The main problem here is still a high, stable,
e.g. by the databases INSPEC or web of science. reproducible p-type doping.
There are many reports on LED involving both temperature (RT) are due to the doped or alloyed ZnO itself
homojunctions based on ZnO and its alloys and heterojunc- or to precipitates and clusters of other phases or even of the
tions in which generally electrons from n-type ZnO are substrate alone [14, 22, 25]. For a short list of pro and contra
injected into a p-type material like GaN, SiC etc. including papers see e.g. Ref. [24] and references therein. Note that the
even organic semiconductors. For a few examples see absence of diffraction orders other than ZnO related ones in
Refs. [8–17] and references therein. There are up to now only XRD is a necessary but by no means sufficient criterion to
very few claims of electrically pumped LDs [18, 19]. exclude other phases. Raman scattering revealed e.g. other
A common feature is the fact that the luminescence yield phases, which have not been seen in XRD [26].
is in all cases in these L(E)D very low and the emission The observation of ferromagnetism immediately trig-
spectrum has frequently large contributions from deep centre gered heavy speculations to use ZnO:X in spintronics or even
emission. For a LD a light output of 0.5 mW has been in quantum computing. The facts that the para- or
reported for a forward current of 60 mA at Ub 20 V [19]. If ferromagnetic magnetization is tiny (apart from the sign
we calculate the efficiency h in the favourable way as frequently of the same order of magnitude as diamagnetism
[27] and that the resulting magnetic flux densities B can only
h ¼ photon flux out=electronhole flux in (1) be measured with high sensitive SQUID arrangements and
are orders of magnitude smaller than the magnetic field of the
we find h 105 even neglecting in this definition the fact earth, shed serious doubt on this field of applications [28].
that the forward bias voltage Ub is considerably higher than Other future hopes of application which are partly
the emitted photon energy. The present situation is (possibly already in use or close to it are:
unintentionally) very well characterized by the cover photo
of [15] which shows presumably the optically pumped blue/ – transparent electronics, based on the large band gap of ZnO,
UV emission from a ZnO sample in the upper half and a e.g. in the form of field effect transistors (FET) or
LED in the lower which is still dark. Hopefully, it will emit (transparent) thin film transitions (TFT or TTFT, respec-
bright blue/UV light in the future. tively), which do not necessarily require a p–n junction
Another aspect driving the present research is the strong [29, 30],
tendency of ZnO to self-organized growth in the form of – the use of ZnO:Y (with Y ¼ Al but also In or Ga) as a highly
nano rods [10–13] and references therein. For an example of conductive transparent oxide (TCO), in addition to the
regular growth on a prepatterned surface see Fig. 1. Such more expensive and poisonous ITO [30, 31],
nanostructures could help to develop nano lasers etc. – the use of ZnO as a gas sensor, due to the strong sensitivity
Apart from more or less well aligned ensembles of of its (surface-) conductivity on the surrounding gas
nanorods, there are other self organized nanostructures, like atmosphere [32],
nano cabbages, corals etc. which are frequently nothing but – the use of pointed nanorods as field emitters [33],
unsuccessful attempts to grow a good epitaxial layer or nano – the use as material for random lasers as discussed in Section
rods. 10 below with Refs. [109–111],
Still another driving force for the ZnO revival is the fact – the application in solar cells. [11]
that diluted magnetic or even ferromagnetic samples can be
grown by doping ZnO:X with ‘magnetic’ ions like Mn, Fe,
Co, Ni, V or even with nonmagnetic ones like Ag, Cu, N or Actually ZnO is used already by 100 000 tons per year as
with intrinsic defects [22, 23]. It is still an open question if the additive to concrete or to the rubber of tires and in smaller
resulting hysteresis loops observed partly up to room quantities as additive to human and animal food, as UV
blocker in sun crèmes, as anti-inflammatory component in
crèmes and ointments, as white pigment in paints and glazes,
as catalyst etc. [14–16].
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temperature through a maximum of a few 1 000 cm2/Vs ordering has been (quietly) accepted by many authors since
around 100 K and decays at lower temperature due to then [49]. The idea of the normal VB ordering has been
scattering with (ionized) impurities. revived with the renaissance of ZnO research, partly by the
In quasi two-dimensional QWs and heterojunctions, this same authors [50]. It has been shown that both the old and the
latter process can be reduced and values between 3 000 and new arguments in favour of the normal VB ordering in ZnO
10 000 cm2/Vs have been obtained in the 1 K region [46]. lack stringency [51]. These arguments against the normal
These values are sufficient to observe the integer quantum- ordering have been written up several times [9, 14, 16].
Hall effect (IQHE) in ZnO [46]. Therefore it is not necessary to repeat them here. In
If scattering at grain boundaries comes additionally agreement with [15] we state that the inverted VB-ordering
into play, e.g. in pressed and sintered samples or in has been adopted in the meantime by the majority of
(epi-)layers consisting of small grains, the mobility may be scientists and use it throughout in the following.
significantly reduced, at RT to values as low as a few ten
cm2/Vs [43, 44] or even below. 7 Deep centre luminescence Similarly to other
The hole mobility is generally considerably lower than wide gap semiconductors, ZnO has a lot of defect levels in
the electron mobility. Typical values reported at RT range the forbidden gap. Many of them can give rise to
from a few to some ten cm2/Vs [45]. luminescence and absorption bands covering the spectral
range from the violet over the whole visible to the IR [52]. A
6 Band structure and band alignments The band colour photograph published in Refs. [11, 14] illustrates
structure is shown schematically in Fig. 3. As stated already, some of these emission bands. In the past many of these
ZnO is a wide, direct gap semiconductor. The conduction emission bands have been attributed to extrinsic defects like
band (CB) with symmetry G7 including spin originates from substitutional Cuzn (giving a green emission band with a well
the empty 4s levels of Znþþ or the antibonding sp3 hybrid pronounced phonon structure) [52, 53] which has also been
states, adapting the views of ionic or covalent binding, partly attributed to Vanadium [54]. In the red to yellow
respectively. The valence band (VB) results in this sense spectral range recombination via deep Li and Na acceptors
from the occupied 2p levels of O– or the bonding sp3 states. It has been identified. This identification was very thoroughly
is split by the hexagonal crystal field and by spin orbit made based on optical spectroscopy, doping experiments,
coupling into three, two fold degenerate sub-VBs, which are EPR and thermo luminescence studies. See the work of D.Z.
called from top to bottom A, B and C VB in all wurtzite type in Ref. [39] or Refs. [52, 55].
semiconductors. The usual ordering is AG9, BG7 and CG7. In In recent years intrinsic defects have been stressed more,
ZnO the inverted VB ordering has been introduced in Ref. with the exception of an unstructured green emission band,
[47] and since then there is a discussion about ‘normal’ or which has been attributed since decades to an oxygen
‘inverted’ VB ordering in ZnO [48]. The inverted VB vacancy V0 [56]. Now many of these emission bands
including one in the violet are attributed to all types of
intrinsic defects like vacancies or interstitials or anti-site
defects. However, these interpretations are still strongly
controversial [57] and the arguments for the identification
are often less stringent, so that more detailed results are
required, to come to clear assignments.
The external luminescence yield of deep centres (and of
the near edge luminescence) is typically around or below
10% at low temperatures and decreases with increasing
temperature [58]. Very weak deep centre luminescence can
be a sign of good sample quality or of the presence of fast non
radiative recombination centres like Co, Fe or Ni [59] but
also Cu at higher concentrations.
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stimulated emission in the range between a few times are presented and discussed in Refs. [110, 111] and in an
1017 cm3 to a few times 1018 cm3. Surprisingly most of the invited contribution [113] to this conference [112]. For hints
recent authors claim the gain mechanism for RT stimulated towards random lasing in disordered ensembles of nano rods
emission to be inelastic X–X scattering. The energetic see Ref. [114].
scattering of the data at RT in Fig. 15 immediately makes To conclude this section we give a few words on claims
clear that different processes are involved. of stimulated emission under optical pumping with power
The inspection of Fig. 17 shows that excitons do no densities as low as 10 Wcm2 [116, 117].
longer exist at these densities at RT as individual quasi- An excitation power of 10 Wcm2 results with reason-
particles since the remaining (or renormalized) binding able values for lifetime (1 ns, see below) and excitation
energy is smaller than the homogeneous width. Therefore the depth (1 mm) determined essentially by diffusion in a density
assignment of gain at RT to excitonic processes will be in np ¼ 5 1014 cm3. This value is too low to produce an EHP
most cases a misconception. The data given by open full stars [116] or significant X–X scattering [117]. The appearance of
are assigned in Ref. [95] to recombination in an inverted modes observed in Ref. [116] may also occur for spon-
EHP. This interpretation is most probably a wrong one. At taneous emission [118] and slopes above one [117] can be
450 K the BGR had to be at least 300 meV resulting in np explained without stimulated emission by simple (e.g.
values well beyond 1020 cm3. These values are neither quadratic) recombination kinetics [28] as well.
compatible with the experimental excitation conditions nor
with the damage threshold of the sample. 11 Dynamics The luminescence decay time of ZnO
On the other hand it is an experimental fact that bulk samples and nano structures has been measured by
stimulated emission is observed at RT in the density regime many research groups. See e.g. Refs. [9, 119] and [120] and
mentioned above though neither excitons exist as good quasi references therein for some examples for bulk, epilayers,
particles nor is an EHP inverted. Therefore we proposed in rods, QWs and nano crystallites. There are also data given on
Refs. [14, 66] and [107] two other recombination processes, dephasing and intra- or inter (sub-) band relaxation. We
which can occur already in a non-degenerate EHP, which has concentrate here mainly on the lifetime. The decay dynamics
some residual Coulomb correlation between the carriers. We is frequently not exponential, so that one cannot speak about
note first that in this density regime the position of the a luminescence decay constant, but only about an effective
renormalized gap E0 g(np) coincides approximately with the decay time tl valid for the given density interval. Frequently
exciton energy at low densities. One of the two processes is the decaying intensity is followed in the experiments only
the recombination of an electron–hole pair in the EHP under over one order of magnitude or even less. This interval is by
emission of a photon and of one or two LO phonons (or more far not sufficient to claim a single or even multi-exponential
accurately plasmon–phonon mixed state quanta). This decay. Fitting with a power law or a stretched exponential is
suggestion is supported by the fact that the data given by usually also possible and partly physically even more
the open stars in Fig. 15 extrapolate the X-2LO process reasonable. To claim a single exponential decay, the signal
observed at lower temperatures and densities. The full stars should be followed at least over three orders of magnitude
in contrast extrapolate beautifully the X-e line and could [121]. The value of tl varies from sample to sample, with
therefore be explained by a process in which again an temperature and with the excitation conditions. Both for free
electron–hole pair recombines in the EHP under emission of and bound excitons and their LO-phonon replica tl is found
a photon and simultaneously transfers part of its energy and generally in the interval
its momentum to a third carrier, most probably another
electron. A detailed many-particle calculation is necessary to 0:1 ns tl 3 ns: (13)
verify or to falsify these concepts.
The explanation developed above may be valid for bulk Differences in tl may already occur between the upper
samples, platelets, epilayers, micro- and nano-rods, for nano and LPBs [122]. Since the (external) luminescence yield h of
crystals and even in QWs. the near edge emission is typically around 0.1 in high quality
Nano rods have a pronounced wave guide property and samples at low temperatures and tends to decrease towards
mode structure. We show in Fig. 19 the stimulated emission higher T [58] this luminescence decay time is significantly
from a single rod at 11 K under band-to-band excitation with different from the radiative lifetime tr. To identify tl with tr is
5 ns pulses from the 3rd harmonic of a Nd-YAG laser. The only correct if h is close to one. However, this precondition is
laser modes are clearly visible. They show mode competition generally not verified.
with increasing excitation (see inset and Fig. 20c) and a Under conditions of stimulated emission the decay time
small blue shift. We will come back to these aspects later. may become much shorter than the range indicated by Eq.
If there is no mode available for a certain emission process (13) reaching down to 10 ps.
(e.g. the X–X process at low temperatures) this process may We show in Fig. 20 a rather illustrative example. A single
be suppressed [108]. nano rod has been excited in the band-to-band transition
Random lasing has been observed in ZnO powders [109]. region with 150 fs pulses. The luminescence was spectrally
Recent results of this topic including the observation of the and temporally resolved by the combination of a spec-
coexistence of spatially extended and more confined modes trometer with a streak camera. At low cw-excitation the
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unfortunate consequence that the luminescence originates while only kz can be varied (quasi-) continuously in the limit
not from the ZnO, but either from a spatially indirect of a very long rod [129–131].
transition across the interface or from the other material of We start with a relatively trivial point. It has been
the hetero-junction. These materials have partly an intrinsi- claimed that the dispersion of the empty cavity modes (i.e. of
cally low luminescence yield if they have an indirect gap the cavity containing no QW) and being described by the
(like SiC) or they can also be doped n-type themselves (like constant refractive index of air or better of the barrier
GaN), thus casting some doubt on the technical relevance of material of the well nb is parabolic [28, 129]. This statement
the heterostructures. is wrong. The intersection of a light cone defined over the
To conclude we may state that beautiful old and new kk k? plane by
physics can be investigated in ZnO, its alloys and nano
structures and that many applications for ZnO exist or are E2 ðkk ; k? Þ ¼ ðhvÞ2 ¼ ðk2k þ k2? Þc2 h2 =n2b ; (14a)
emerging. The question if ZnO will see a major breakthrough
with the plane given by
in (opto-) electronics depends strongly on the availability of
high, efficient, stable and reproducible p-type doping and of k? ¼ mp=d; (14b)
efficient LEDs and LDs based on it in the next (very few!!)
years to come. results in a hyperbola and not a parabola. See e.g. Fig. 17.1d
in Ref. [28]. The curvature of this hyperbola is in its
minimum given by
Acknowledgements The authors want to thank the
Deutsche Forschungsgemeinschaft for financial support in an @ðhvÞ=@kk2 ¼ ch k? =nb ; (15)
individual grant (Kl 354/23) and through the CFN and the Landes-
stiftung Baden-Württemberg through the Kompetenznetz
If one translates this curvature into an effective mass meff
‘Funktionelle Nanostukturen’ Project A1.
one obtains
Appendix The fact that the deadline for the paper meff ¼ hv=c2 nb : (16)
submission to the proceedings of the 14th International
Conference on II-VI Compounds was about 3 weeks after the This means that the effective mass in the minimum is just
end of the conference has an advantage. Some thoughts about given by a modified Einstein relation
contributions to the conference can be included in this
review. It is clear to the main author of this appendix (CK) E ¼ hv ¼ meff c2 : (17)
that not all of the ideas presented below are yet mature. Partly
This corresponds indeed to the very low effective mass
they even contradict present state theoretical modelling.
quoted usually in connection with claims of Bose Einstein
They are therefore meant as a stimulus for discussion in the
condensation (BEC) of cavity polaritons. However, it must
scientific community.
be kept in mind that for a hyperbolic dispersion meff is not
We consider here some aspects of exciton cavity
constant, but increases rapidly for finite kjj and asymptoti-
polaritons in quasi two-dimensional and quasi one-dimen-
cally reaches the value infinity in the linear part of the
sional systems, which are both relevant for ZnO [125–131]
hyperbola. Possibly one could think to introduce a concept of
and compare them to bulk material. Quasi two-dimensional
meff based on the first derivative as used e.g. in metal physics
systems are in the present context Fabry–Perot resonators
around the Fermi energy [28]
with plane, highly reflecting mirrors on both sides (generally
Bragg reflectors) containing in this cavity one or a few QW, meff ¼ h2 k=ð@E=@kÞ: (18)
with the exciton resonance of these QW overlapping
energetically with the two-dimensional dispersion E(kjj,k? ) The next aspect is excitonic or polaritonic Bose-Einstein
of the cavity modes without these QW, the so-called empty condensation (BEC). At least one of the authors of this
cavity. The value of k? is quantized by the cavity modes to review (CK) is notoriously sceptic about excitonic BEC [28],
mp/d where d is the geometrical thickness of the cavity and because he has seen in the 35 or more years of his scientific
m ¼ 1, 2, 3. . .. The in-plane wave vector is given by career too many claims of excitonic BEC appearing and
kjj ¼ kxex þ kyey where ex and ey are the unit vectors in the disappearing again. See for some recent examples e.g. Refs.
plane of the cavity. Without loss of generality we can choose [133, 134] and the references therein. However, the results
ky ¼ 0 for a system isotropic in the x–y plane. Examples are presented at this conference [126–128] start to be convinc-
e.g. GaAs, ZnO or CdTe based cavities [28, 126–128] and ing, especially since both thermal quasi-equilibrium con-
[132]. A good overview of this field is found in Ref. [138] and ditions in the BEC ground state have been reached and the
the references therein. differences to polariton lasing have been worked out and also
The quasi one-dimensional situation has been realized in to a process analogous to two-photon or hyper-Raman
ZnO micro rods of some micrometers in diameter and some scattering in bulk samples [93] under a so-called magic
10 mm in length by whispering gallery modes (WGM), in angle. The first difference i.e. polariton lasing is a very
which the k vector is quantized in the two-dimensional plane common phenomenon in semiconductors [14, 93] and
perpendicular to the growth-, z- or c-axis of the micro rod, includes among other processes the inelastic polariton–
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polariton (or exciton–exciton) scattering which results in the lz is much smaller than the width of the cavity d
Pi-bands (i ¼ 2,3. . .1). See above or Ref. [28]. This positive
statement about BEC of cavity polaritons is made being 10 nm lz d 500 nm: (19)
aware of the implications (or difficulties) of BEC in a quasi
two-dimensional system, which has in meff–approximation This means that only a small fraction of the cavity
ideally a Heavyside function for the density of states instead volume contains the exciton resonance. The Q-value or
of the square root one and in reality tail states resulting from finesse of the cavity and the dephasing time T2 of the exciton
inhomogeneous and homogeneous broadening induced e.g. can be varied independently. The strong coupling regime
by width fluctuations of both the QW and of the cavity and with the pronounced non-crossing behaviour between the
from scattering processes e.g. with phonons. dispersion curves of the empty cavity mode and of the
A third point addresses the concepts of strong and exciton is reached if T2 is several times the round trip time tr
weak coupling between cavity modes and exciton resonance, of the light in the cavity, typically requiring T2 1 ps.
since we think that there are significant differences in the Furthermore, the small volume fraction occupied by the QW
three- and quasi two- and one-dimensional systems dis- has the advantage that the absorption of the QW hardly
cussed here. affects the finesse of the cavity. Even with a ¼ 105 cm1 and
In a bulk sample, the coupling between light and exciton lz ¼ 10 nm one obtains an optical density of only a lz ¼ 0.1.
resonances is an intrinsic feature and so is the resulting The Rabi splitting is then given in the case of strong coupling
exciton polariton dispersion curve. Consequently, one is for by the minimal energetic distance between the lower and
excitons in direct gap semiconductors generally in the strong upper polariton branches of the cavity exciton polariton
coupling limit. Even for damping zero one has a significant resulting from the (quantum-mechanical) non-crossing rule.
imaginary part of k or k [28] between the transverse and It can be much higher than in bulk samples.
longitudinal exciton eigen-energies, which makes the In the case of weak coupling, the exciton resonance is so
direct observation of the dispersion in this spectral range a strongly (in-) homogeneously broadened (and so is the
non-trivial problem. Frequently processes of nonlinear contribution of this resonance to the whole system consisting
optics are used for its experimental verification like two- of cavity mode and exciton) that it hardly influences the
photon absorption or hyper-Raman scattering [28]. In linear hyperbolic empty cavity dispersion. Also this behaviour is
optics the polariton dispersion can be deduced by the favoured by the small volume fraction occupied by the QW.
refraction at a thin prism, from resonant Brillouin scattering The situation is now significantly different for the quasi
or from the Fabry–Perot modes of thin platelets. See for one-dimensional longitudinal cavity formed by the micro rod
some references [28]. Care has to be taken for the or for the transverse WGM and starts to resemble again the
observability of the dispersion between the transverse and situation of bulk material, since in this case the whole cavity
longitudinal eigen energies of the bulk exciton polariton is formed by and filled with the medium containing the
resonances that the optical density of the platelet type exciton resonance and is described by its complex index of
samples a(£v)d remains below or around 1, despite the fact refraction
that the reflectivity for the intensity under normal incidence n~ðvÞ ¼ nðvÞ þ ikðvÞ: (20)
reaches values around 0.8 for a single surface on the LPB.
This value is almost comparable to the one of real Bragg
mirrors and results from the fact that the real part n(£v)of the This means that these cavity modes are determined
complex index of refraction reaches values beyond 10 in the completely by this ñ(v). The absorption coefficient a( hv)
above mentioned range. See e.g. Figs 13.17 and 20 in Ref. reaches in ZnO throughout the whole cavity values
[28]. If a(£v)d grows considerably beyond unity, the a(hv) 2 105/cm in the spectral range between the
observability of the Fabry–Perot modes becomes quenched transverse and longitudinal eigen energies of the bulk
simply by absorption, though one is still in the strong exciton. See Fig. 5. Consequently, alz ¼ ad ¼ 20 already
coupling limit. for d ¼ 1 mm. This fact has the consequence that the visibility
For Fabry–Perot (i.e. micro-cavity) modes on one side of the micro rod cavity modes is completely quenched when
and WGM on the other, the situations are different, too, since approaching this spectral range. Actually, to the memory of
several round trips of the light are necessary to form the one of the authors (CK), no cavity modes where visible in
polariton. Strong losses in the cavity caused e.g. by a large Refs. [129–131] around 3.31 eV, the position of the A and B
optical density necessarily destroy the modes [28]. See G5 nB ¼ 1 exciton resonances at RT, but only a broad
above. luminescence band from the free exciton and its LO-phonon
For the quasi two-dimensional case, the cavity is replica. See Fig. 7.
essentially filled with the barrier material of the QW, which Towards lower photon energies where ZnO becomes
has in the spectral region of interest – the exciton resonances transparent, the one-dimensional exciton cavity polariton
of the QW – an almost constant refractive index nb and dispersion became visible in the beautiful experiments
negligible absorption. The exciton of the QW has a mentioned above, with an energetic distance and curvature
dispersion with much higher effective mass mex ¼ me þ mh increasing with decreasing energy of the branch due to the
than the empty cavity. The thickness of the QW in the cavity decrease of n(v) below the exciton resonance towards lower
photon energies. The increasing curvature leads for finite kjj surfaces but should become transparent and show well-
to a crossing between the dispersion curves of adjacent resolved WGM if the light circulates in these modes.
branches and in case of coupling between them to an avoided As mentioned already, in the ZnO rods it is not possible
crossing. Since photons in vacuum do not interact, this to vary the finesse of the resonator and the damping of the
coupling is based on the excitonic part of the polariton wave exciton resonance within wide limits independently as in the
function (more generally the electronic parts, which include case of a QW exciton in a micro cavity formed by two Bragg
also the band-to-band transitions or the presence of an EHP, mirrors, but the whole system remains determined by ñ(v).
see below). The wave function of an exciton polariton has This remains true if the exciton resonance is broadened by
substantial exciton-like character about more than ten times increasing temperature T or if an increasing density np of
the longitudinal-transverse DLT splitting below and above electron–hole pairs lead to increasing screening of the
the exciton energy [135]. Since the sum of DLT is for the exciton up to the limit of an EHP where excitons do no longer
(A þ B)G5 excitons more than 10 meV, the exciton like exist as individual quasi particles. Also in this situation the
character of the polariton wave function extends quite a bit system is described by ñ(v,T, np). The influence of the
below the resonance. This fact is confirmed by the density dependent changes of the refractive index on the
observation of luminescence from the cavity polariton longitudinal modes in a nano rod has been presented already
modes, since an empty cavity does not show luminescence. above with Fig. 20, including the onset of recovery with time
The fact that the dispersion and visibility of the WGM is after pulsed excitation. The same phenomenon was obvi-
completely determined by the complex index of refraction ously observed in Ref. [129] when the spectral position of the
ñ(v) ¼ n(v) þ ik(v) remains true, if the (in-) homogeneous WGM shifted in the case of stimulated emission. Their
broadening G(T) increases from about 1 meV at 2 K to values properties are then simply determined by ñ(v, T, np) and the
of above 20 meV HWHM at RT. This effect influences the geometry of the micro rod.
dispersion of the exciton cavity polariton only close to In bulk, the dispersion of light in ZnO in the presence of
resonance in the strongly absorbing regime but not below, an EHP would be simply given by a modified polariton
where cavity polaritons remain clearly visible. The width of equation
the cavity modes in the transparent regime is determined by
the finesse or Q-factor of the cavity (or by the photonic decay c2 k2 =v2 ¼ n~2 ðv; T; np Þ ¼ eðv; k; T; np Þ: (21)
time) and the residual absorption, both being directly
determined by ñ(v). In the context of micro or nano rods we consider the
If a phenomenological damping constant is introduced in WGM in micro rods and the longitudinal modes in nano rods
the Lorentz oscillator model, the damping of the polariton as two limiting cases with a continuous transition between
i.e. the absorption coefficient or the imaginary part of ñ(v) them in the following sense: For the fundamental longi-
decreases strongly with increasing energetic distance below tudinal modes in a nano rod the wave vector is almost
the resonance as is also obvious for bulk exciton polaritons. completely determined by the quantized kjj, while k? is
See Fig. 5 above or Figs 4.5 and 13.9 in Ref. [28]. Therefore marginal. This situation changes if one goes to higher
the spectral width of the cavity polaritons decreases, too. For transversal modes [108]. Then k? increases at the expense of
more detailed considerations of the damping of cavity kjj for constant energy of the light quanta or the modes shift to
polaritons see e.g. Ref. [139]. In a microscopic model one the blue for fixed kjj. For WGM one has the opposite
may consider scattering processes e.g. with phonons or with situation. In a mode, which circulates completely in the
other polaritons to describe damping. The steep decrease of hexagonal cross section of the rod, k? is quantized and makes
the damping especially below the bulk exciton resonance up the whole wave vector. For observation under an oblique
may then be attributed to the small DOS of both bulk and angle to the rod- or c-axis kjj increasingly comes into play
cavity polaritons. It should be noted that at RT the damping now at the expense of k? . In principle it should be possible to
of the exciton resonances is in ZnO mainly determined by give a general description of modes in a hexagonal rod for all
scattering with LO phonons. See the experimental data in (k? ,kjj) which includes the above limiting cases.
Fig. 8 or Ref. [66]. To conclude this appendix, one may ask if it makes sense
A huge Rabi splitting of more than 300 meV (i.e. more to separate the strong and weak coupling limits in ZnO rods?
than five times the exciton binding energy) has been claimed A situation where one sits spectrally on the bulk exciton
in Ref. [129] from a fitting procedure. It is not clear to the resonance and still has a high finesse cavity is not possible for
author to which extend this value corresponds to a real the rods as mentioned above. At this resonance, where the
splitting between the lower and upper polariton branches at coupling between electromagnetic field and the exciton is
the WGM exciton polariton resonance in the sense strongest, one has necessarily strong damping and low
introduced above, because the WG is opaque in the range finesse and in the transparent region below the exciton the
of A and BG5 excitons and of their higher states including the finesse and the width of the modes get better, but the coupling
ionization continuum, or if it is simply a fitting parameter between excitons and electromagnetic field decreases.
deduced from the low energy data in the transparent region of A more detailed theoretical treatment of this problem
the sample. It is difficult to imagine that a micro rod is opaque [136, 137] came to a Rabi splitting for WGM of the order of
in a simple transmission measurement through two opposite 200 meV in agreement with the value cited above as a new
solidi
physica
status
1442 C. Klingshirn et al.: 65 years of ZnO research – old and very recent results
energy scale, which is larger than the exciton binding energy, T. Minami et al., SPIE Proc. 5274, 399 (2003). P. Chen,
but claims that possibly only the LPB may be visible but not X. Ma, and D. Yang, Appl. Phys. Lett. 89, 111112
the UPB, which should actually be situated already in the (2006). J. Kennedy, J. Pithie, and A. Markwitz, SPIE
excitonic ionization continuum. Since already bulk ZnO is Proc. 6800, 1P-1 (2007). K. Wang, Y. Vygranenko, and
transparent only on the LPB up to the bottleneck, these A. Nathan, Thin Solid Films 515, 6981 (2007). S. Karan
and B. Mallik, Nanotechnology 19, 495202 (2008). L. Ae,
results may even give some support to the tentative and
Chen Jie, and M. C. Lux-Steiner, Nanotechnology 47,
qualitative considerations above. 475201 (2008). P. Klason et al., Microel. J. 40, 706 (2009).
Yu. Quing-Xuan et al., Appl. Phys. Lett. 83, 4713 (2003).
Ya. I. Avilov et al., Appl. Phys. Lett. 83, 2942 and 4719
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