Embedding and self-organization of

nanoparticles in phospholipid multilayers

Cite as: J. Chem. Phys. 121, 510 (2004); https://doi.org/10.1063/1.1760077
Submitted: 14 January 2004 • Accepted: 07 April 2004 • Published Online: 18 June 2004

Annegret Terheiden, Bernd Rellinghaus, Sonja Stappert, et al.

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J. Chem. Phys. 121, 510 (2004); https://doi.org/10.1063/1.1760077 121, 510

© 2004 American Institute of Physics.

JOURNAL OF CHEMICAL PHYSICS VOLUME 121, NUMBER 1 1 JULY 2004

Embedding and self-organization of nanoparticles

in phospholipid multilayers
Annegret Terheiden
Institut für Chemie, Universität Duisburg-Essen, 47048 Duisburg, Germany
Bernd Rellinghaus
IFW Dresden, Helmholtzstr. 20, 01069, Dresden, Germany
Sonja Stappert and Mehmet Acet
Institut für Physik, Universität Duisburg-Essen, 47048 Duisburg, Germany
Christian Mayera)
Institut für Chemie, Universität Duisburg-Essen, 47048 Duisburg, Germany
共Received 14 January 2004; accepted 7 April 2004兲
Multilayers of various phospholipids on silicon substrates are used to induce spontaneous
embedding of nanoparticles deposited from the gas phase. The resulting nanoparticle arrangement
on the substrate surface is characterized using atomic force and scanning electron microscopy. In the
intermediate phase and the liquid crystalline phase of the lipid, a monolayer is formed around
individual nanoparticles which leads to an increase in interparticle distances. At the same time, the
molecular mobility of the multilayers allows for self-assembly of the particles in regular
two-dimensional arrangements. © 2004 American Institute of Physics.
关DOI: 10.1063/1.1760077兴

I. INTRODUCTION aries. In the vicinity of planar surfaces, they spontaneously

Phospholipid–water systems play a major role in mul-
tiple intracellular structures, mainly by forming the major
constituent of biological membranes. Within the large diver-
sity of living organisms, they have undergone a long natural
evolution for ideal properties of their lamellar arrangements.
This is reflected by the wide variety of phospholipids and
their specific occurrence pattern in different species. With
their amphiphilicity and their capability to form lamellar liq-
uid crystalline phases, they appear perfectly suited for the
spontaneous formation of stable molecular layers on polar
surfaces, while at the same time they preserve a great deal of
molecular mobility.
Phospholipids are known to form a large variety of ther-
modynamically stable structures in the presence of water or
other solvents.1–3 Depending on the solvent content and the
physical conditions, they may aggregate in bilayers, multi-
layers, hexagonal phases, cubic phases, micelles and
vesicles. The main driving force for these phenomena is the
strong amphiphilicity of the phospholipid molecules which is
based on an extremely polar 共often zwitterionic兲 head group
combined with two unpolar hydrocarbon chains 共Fig. 1兲. At
elevated temperatures, multilayers show typical features of
thermotropic, or, in presence of excess water, lyotropic liquid
crystals: local anisotropy together with a considerable
amount of molecular mobility.1–5
Due to their distinct amphiphilic properties, phospho-
lipid molecules tend to arrange along given phase bound-
a兲
Author to whom correspondence should be addressed. Electronic mail:
hi408ma@uni-duisburg.de; Tel: 0049 203 379 3317; Fax: 0049 203 379
3522.
form oriented single, double, or multilayers.1–3,6 On the other
hand, their ability to adopt curved structures is similarly well
known; vesicles, micelles, and inverted micelles are promi-
nent examples. These structures should be facilitated by the
presence of spherical phase boundaries such as the surface of
a small nanoparticle. Consequently, small spherical particles
coming in contact with a liquid crystalline phospholipid
multilayer could possibly induce the formation of an inter-
esting two-phase system: nanoparticles encapsulated by
single spherical layers of phospholipid molecules in close
lateral arrangement 共Fig. 2兲. With the polar head groups
pointing towards the particle surface, this structure would
show some analogy to inverted micelles with the polar sides
of the amphiphilic molecules forming the hydrophilic center.
The structure is also similar to surfactant layers which have
been used to stabilize magnetic nanoparticles in liquid
dispersions.7,8
Ferromagnetic metallic nanoparticles with high coerciv-
ity evenly spread on a planar surface may have very inter-
esting applications especially for magnetic storage devices
such as hard disks. Suitable nanoparticles e.g. of an iron–
platinum 共FePt兲 alloy can be synthesized either in a liquid or
in a gas phase.9,10 The preparation in a gas phase offers two
significant advantages: excellent material purity and the op-
tion to sinter the particles at high temperatures prior to the
embedding in an organic layer. The possibility to assemble
particles from the gas phase in an organic layer could have a
future potential for the preparation of surfaces with a high
magnetic storage capacity.
Multilayers of various phospholipids have been prepared
on 共110兲 silicon wafers in order to study their suitability to
induce the formation of planar particle arrangements. Three

0021-9606/2004/121(1)/510/7/$22.00 510 © 2004 American Institute of Physics

J. Chem. Phys., Vol. 121, No. 1, 1 July 2004
FIG. 1. Schematic sketch of a typical representative of a phospholipid mol-
ecule 共1,2-dipalmitoyl-sn-glycero-3-phosphatidylcholine, DPPC兲 showing
the most important structural elements: a zwitterionic head group 共top兲 con-
nected to two hydrocarbon chains 共bottom兲 via a glycerol backbone.
lipid types have been chosen to obtain multilayers in three
different phase states under given temperature and moisture
conditions. In a second step, metallic nanoparticles 共FePt, d
⫽6 nm, ␴ ⫽1.15) were generated in the gas phase and de-
posited onto the multilayer surfaces at ambient temperature.
Finally, after deposition, the layers were treated with mois-
ture at elevated temperature to allow for thermodynamically
driven particle rearrangement. The phospholipid multilayers
and the resulting particle patterns were studied using scan-
ning electron and atomic force microscopy.
II. MATERIALS AND METHODS
A. Materials
For preparation of lipid multilayers, the following mate-
rials have been used:
共a兲 1,2-dipalmitoyl-sn-glycero-3-phosphatidylcholine
共DPPC兲, main transition from the intermediate phase
P ␤ ⬘ to the liquid crystalline phase L ␣ at 41 °C 共above
50% water content兲.2
共b兲 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphatidylcholine
共POPC兲, main transition from the intermediate phase
P ␤ ⬘ to the liquid crystalline phase L ␣ at ⫺2 °C 共above
50% water content兲.11
共c兲 1,2-dioleoyl-sn-glycero-3-phosphatidylcholine
Nanoparticles in phospholipid multilayers 511
FIG. 2. Cross section through a postulated arrangement formed by the in-
teraction of polar nanoparticles 共circles兲 with amphiphilic phospholipid mol-
ecules from a phospholipid multilayer: 共a兲 initial interaction after particle
deposition, 共b兲 full particle embedding.
共DOPC兲, main transition from the intermediate phase
P ␤ ⬘ to the liquid crystalline phase L ␣ at ⫺20 °C 共above
50% water content兲.12
Phospholipids were purchased from Sigma-Aldrich Fine
Chemicals 共DPPC, DOPC兲 and Avanti Polar Lipids Inc.
共POPC兲 and used without further purification.
B. Preparation of phospholipid multilayers
All phospholipid multilayers are prepared by spin coat-
ing following the method developed by Mennicke and
Salditt.13 Generally, 4⫻4 mm silicon substrates are used as
carriers for the lipid multilayers. Prior to deposition, each
wafer fragment is subjected to four successive ultrasonic
cleaning steps in presence of chloroform, acetone, isopro-
panol, and methanol followed by extensive rinsing in ultra-
pure water. The surface is then dried under a nitrogen atmo-
sphere to avoid further contamination. For spin coating, a
total of 5 ␮l of a solution of the lipid in chloroform 共10
mg/ml兲 is pipetted centrally onto the static substrate. After
the initial spreading of the solution, the sample is spun at
5000 revolutions per minute for 30 s. Solvent evaporation
under atmospheric pressure in presence of ambient moisture
leads to the formation of a well defined multilayer.13 The
512 J. Chem. Phys., Vol. 121, No. 1, 1 July 2004
residual organic solvent is removed by evaporation in high
vacuum over 20 h, while a water content of approximately
3% 共about one molecule of water per lipid molecule兲 is pre-
served. The readily prepared multilayer samples are stored in
a dark and cool environment prior to further handling. Par-
allel to the multilayer samples, an uncoated silicon substrate
is used as a reference sample for further experiments.
C. Particle generation, deposition,
and postdeposition treatment
The procedure for the generation and deposition of FePt-
nanoparticles has been described in detail elsewhere.14 –17
FePt-particles are prepared by dc sputtering in an Ar/He at-
mosphere at 0.5 mbar pressure and sintered in the gas phase
at 600 °C. Under these conditions, the obtained particles are
nearly spherical and show a high degree of mono-
dispersity.14 –16 Particles are collected by thermal deposition
on the carrier surfaces 共multilayers and reference兲 under con-
trolled temperature conditions 共20 °C兲. After deposition, the
carriers are exposed to an atmosphere of a relative humidity
of approximately 100% at 35 °C for 90 min to induce reor-
ganization of the multilayers. Samples were handled under
minimal light exposure throughout the whole preparation
process to avoid possible polymerization reactions of unsat-
urated lipids.
D. Atomic force and scanning electron microscopy
„AFM and SEM…
Atomic force microscopy 共AFM兲 measurements are per-
formed in air at room temperature using a Nanoscope IIIa
MultiMode atomic force microscope 共Digital Instruments兲
equipped with a J-scanner operating in the tapping mode.
Etched silicon probes 共RTESP, Veeco Instruments兲 with a
spring constant of 20– 80 N/m and a nominal tip radius of
curvature of less than 10 nm are applied at a resonance fre-
quency of 200– 400 kHz. All images are recorded at a scan
rate of 0.5 Hz. The surface roughness is determined over an
area of approximately 250⫻500 nm by use of the instrument
software.
Scanning electron microscopy 共SEM兲 is performed with-
out further sample treatment using a LEO 1530 共LEO Elec-
tron Microscopy兲 scanning electron microscope with a stan-
dard SE-detector at an acceleration voltage of 10 kV.
E. Differential scanning calorimetry
All DSC experiments are run on a Perkin Elmer DSC 7
instrument. The phospholipid multilayers 共4 –9 mg兲 are pre-
pared in reusable steel crucibles 共50 ␮l兲 that can be tightly
sealed to avoid any exchange of moisture with the atmo-
sphere. The preparation procedure is generally as described
in Sec. II B except for the spinning step which is omitted.
Generally, only thermograms of the second or third heating
step are analyzed for phase transitions. For all measurements,
the heating rate is set to 10 °C/min, the upper and lower
limits of the temperature program are adjusted according to
the expected phase transition temperatures.
Terheiden et al.
FIG. 3. DSC thermograms of phospholipid multilayers obtained by the pro-
cedure outlined in Sec. II B. All plots are normalized to specific heat flows
共in mW per mg sample兲 and randomly shifted on the vertical scale to en-
hance readability.
III. RESULTS
A. Multilayer characterization
Thermograms resulting from DSC measurements on
multilayers of the three different phospholipids are plotted in
Fig. 3. The samples are prepared in tightly sealed 50 ␮l
sample crucibles using the procedure described in Sec. II B
共except for spinning兲 which leads to partially ordered phos-
pholipid multilayers with a minimal water content, similar to
the conditions during particle deposition. While layers of
DPPC and POPC show large transition enthalpies, the phase
transition endotherms of DOPC are barely detectable. At the
given water content, the phospholipids are expected to un-
dergo a pretransition from the L ␤ ⬘ 共gel-兲 phase to an inter-
mediate phase ( P ␤ ⬘ ) and a main transition from the interme-
diate phase to the L ␣ 共liquid crystalline兲 phase.2 For DPPC
and POPC, the main transitions could be located near 90 °C
and 40 °C, while the pretransitions occur near 50 °C and
15 °C, respectively. In case of DOPC, only the main transi-
tion near ⫺5 °C could be detected.
Optical microscopy of the multilayers reveals the forma-
tion of defects in the spin coated lipid structure, as has been
observed previously.13 However, large areas of the sample
surface appear to be homogeneously covered. These sections
are further studied by atomic force microscopy 共AFM兲 in
order to determine the surface roughness and other structural
details. A graphic representation of an AFM result 关Fig. 4共a兲兴
clearly shows that, at sufficient distance from the outer
edges, the multilayer appears smooth and homogeneous. The
cross section scan 关Fig. 4共b兲兴 reveals an overall thickness of
106 nm, corresponding to 21 double layers of phospholipid
molecules. Within a sample section of 250⫻500 nm, a re-
sidual roughness of 0.12 nm is detected. At some locations
near the outer edges of the multilayer, it is possible to iden-
tify height steps corresponding to individual bilayers which
amount to approximately 5 nm 关Fig. 4共c兲兴.
B. Particle deposition and embedding
After particle deposition and sample annealing, the AFM
images of the multilayer surfaces show significant differ-
ences depending on the type of lipid which is being used
共Fig. 5兲. The appearance of the particles in the postdeposition
DPPC multilayer 关Fig. 5共b兲兴 strongly resembles that in the
J. Chem. Phys., Vol. 121, No. 1, 1 July 2004
FIG. 4. AFM images of a typical lipid multilayer prepared by spin coating.
The outer edges reveal the multilayer structure with step heights correspond-
ing to individual double layers: 共a兲 top view; 共b兲 and 共c兲 cross section scans
at different locations.
untreated reference sample 关Fig. 5共a兲兴. Particle clusters 共and,
in case of the reference sample, even individual particles兲 are
clearly observable. The height difference between the top
level and the underlying surface reflects the particle size, an
overall roughness of 2.35 nm for the DPPC multilayer and
3.39 nm for the reference sample is detected 共Table I兲. In
case of POPC multilayers, the AFM images look completely
different: the particles and particle clusters are hardly visible,
the overall roughness 共0.79 nm兲 is much smaller than the
particle radius 关Fig. 5共c兲兴. Finally, the appearance of DOPC
multilayers is completely unaffected by the particle deposi-
tion process. The surface seems to remain absolutely smooth,
with a roughness of 0.18 nm which is almost as small as for
the original multilayer with 0.12 nm 关Fig. 5共d兲兴.
Scanning electron microscopy reveals further details on
the particle distribution after the deposition/annealing pro-
cess. A SEM micrograph of the reference sample is shown in
Fig. 6共a兲. With the given deposition density, the particles
Nanoparticles in phospholipid multilayers 513
form a submonolayer on the wafer surface. The particle dis-
tribution shows a random pattern with accidental particle
clusters. The minimal distance between adjacent particle cen-
ters 共such as observed in particle clusters兲 is determined as
7⫾1 nm by image analysis 共Table I兲.
Particle assemblies generated on different phospholipid
multilayers in different phase states are represented by cor-
responding micrographs shown in Figs. 6共b兲– 6共c兲. In com-
parison with the result observed for the reference sample
关Fig. 6共a兲兴, the presence of lipid multilayers obviously in-
duces a significant rearrangement of the metallic nanopar-
ticles leading to a strong deviation from the statistical pat-
tern. All types of lipids allow for a similar degree of lateral
particle mobility. While the particles assemble in condensed
two-dimensional arrangements, empty regions on the
multilayer surface are formed.
Interestingly, significant variations of the interparticle
distances are observed depending on the type of surface
共Table I兲. While no obvious difference of the distance is
found for the reference sample and DPPC multilayers (7
⫾1 nm in both cases兲, the result looks somewhat different
for POPC multilayers 关Fig. 6共c兲兴. In this case, the presence of
the lipid multilayers leads to a significant expansion of the
particle pattern, with typical distances increasing from 7
⫾1 nm to 10.5⫾1 nm 共Table I兲. This effect reaches its maxi-
mum for DOPC, where finally an average distance of 11.5
⫾1 nm is accomplished 关Fig. 6共d兲兴. In all cases where lipid
multilayers are present, the particles tend to self-organize in
hexagonal patterns 关Figs. 6共b兲– 6共d兲兴.
IV. DISCUSSION
Morphological studies on the initial multilayers using
optical as well as atomic force microscopy reveal a smooth
outer surface over areas of at least several tens of microme-
ters in size. According to the coating thickness of approxi-
mately 100 nm, the multilayer is composed of about 20 well
organized double layers, a finding which is further supported
by the observed structure near the outer edges 共Fig. 4兲. The
method described by Mennicke and Salditt13 clearly en-
hances the suitability of spin coating for the preparation of
well defined multilayers.
The capability of a multilayer system for the spontane-
ous encapsulation of nanoparticles largely depends on its
phase state during the deposition. At a given temperature, the
latter is determined by the type of lipid and the solvent con-
tent. At low water content and 20 °C, a multilayer of DPPC is
at a temperature well below its pretransition and adopts the
L ␤ ⬘ 共gel兲 state 共Fig. 3兲. Under this condition, the intermo-
lecular mobility is distinctly limited and the ability of indi-
vidual molecules to undergo lateral motion within a layer is
extremely reduced.4,5 At the same temperature and water
content, a multilayer of POPC is found just above the pre-
transition and below the main transition, a condition which is
known as the intermediate ( P ␤ ⬘ ) phase. This state is charac-
terized by an inhomogeneous mobility, with one component
resembling the liquid crystalline state.4,5 Finally, again at
20 °C, the DOPC multilayer is in the liquid crystalline (L ␣ )
state, a condition that exhibits rapid molecular exchange
within each layer and a wide variety of other types of
514 J. Chem. Phys., Vol. 121, No. 1, 1 July 2004 Terheiden et al.

FIG. 5. AFM images of the original

silicon surface and of different lipid
multilayers after particle deposition at
20 °C. While particle clusters are ob-
servable for the reference 共a兲 and for
DPPC 共b兲, the particles become par-
tially and fully embedded in multilay-
ers of POPC 共c兲 and DOPC 共d兲, re-
spectively.

mobility.4,5 Particle depositions have been performed on multilayer region which is directly affected by the impact. In
multilayers in all three different phase states: this case, the multilayer remains a passive surface. However,
during the subsequent annealing step 共90 min at 35 °C at
A. Multilayers in the gel phase
excess moisture兲, it allows the particles to develop a consid-
In the essentially rigid gel phase 共DPPC at 20 °C兲, the erable amount of lateral mobility and to assemble in con-
phospholipids do not observably interact with the nanopar- densed two-dimensional arrangements forming a nearly
ticles. The AFM images indicate the presence of particles regular hexagonal lattice 关Fig. 6共b兲兴. As no encapsulation
residing on a smooth underlying surface with little or no occurs, the average distance between adjacent particle cen-
tendency to penetrate into the multilayer. With an approxi- ters comes close to the one observed in the absence of phos-
mated velocity of 1 m s⫺1, the kinetic energy of a single FePt pholipids. Similar results are found after particle deposition
particle does not suffice to change the structure of the on multilayers of POPC at ⫺20 °C which are in the gel state
as well 共data not shown兲.
TABLE I. Interparticle distance and surface roughness detected on different
surfaces after particle deposition at 20 °C.
B. Multilayers in the intermediate phase
Typical
If the phospholipid multilayer is in a more mobile phase
Carrier surface Main phase transition distance Surface
preparation between roughnesses state such as the intermediate phase 共POPC at 20 °C兲, the
temperature
共average thickness adjacent as lateral mobility of phospholipid molecules allows for the for-
and phase condition Fully Partially particle determined mation of single lipid layers on the particle surface during
hydrated hydrated
during particle centers by AFM particle deposition 共Fig. 2兲. The assumption that the metallic
deposition兲 共nm兲 共nm兲
particles are completely coated is clearly supported by the
Reference sample ⬃7⫾1 a 3.39 AFM images which indicate almost complete particle em-
共no lipid multilayer兲 bedding in the multilayer surface 关Fig. 5共c兲兴. Moreover, it is
DPPC ⫹41 °C ⬃90 °C 7⫾1 2.35 in accordance with the increase of the observed interparticle
共101 nm, gel phase兲
POPC ⫺2 °C ⬃40 °C 10.5⫾1 0.79
distance from 7⫾1 nm to 10.5⫾1 nm which means that par-
共119 nm, ticle surfaces are separated by approximately 3.5 nm 共Table
intermediate phase兲 I兲. The phenomenon of a two-dimensional expansion is
DOPC ⫺20 °C ⬃⫺5 °C 11.5⫾1 0.18 clearly visible in a comparison between Figs. 6共b兲 and 6共c兲.
共106 nm, The surface to surface distance of 3.5 nm corresponds to a
liquid crystalline phase兲
separating molecular structure formed by two phospholipid
a
Minimal distance between adjacent particles in clusters. monolayers with their head groups pointing toward the nano-
J. Chem. Phys., Vol. 121, No. 1, 1 July 2004 Nanoparticles in phospholipid multilayers 515

FIG. 6. Scanning electron micrographs showing the particle arrangement on a neat wafer surface 共a兲 compared to structures obtained on lipid multilayers from
phospholipids in different phase states at 20 °C: 共b兲 DPPC 共gel phase兲, 共c兲 POPC 共intermediate phase兲, 共d兲 DOPC 共liquid crystalline phase兲. The inserts
represent the assumed configuration of the particles on each sample surface which is compatible with the corresponding AFM result.

particles while the aliphatic chains are interdigitated as de-
picted in Fig. 2. No overlap between adjacent particles is
observed, so all particles seem to arrange in a single plane.
Similar results are found after particle deposition on multi-
layers of DOPC at ⫺20 °C 共data not shown兲.
C. Multilayers in the liquid crystalline phase
The result observed after particle deposition on a liquid
crystalline multilayer 共DOPC at 20 °C兲 resembles the one
obtained for the intermediate state 关Fig. 6共d兲兴. Compared to
the particle rearrangement of POPC multilayers at 20 °C, the
interparticle distances have increased by 1 nm 共Table I兲,
which may indicate an improved coating of individual par-
ticles. The typical spacing between the particle surfaces now
amounts to 4.5 nm and comes close to the overall bilayer
thickness 共5 nm兲. The AFM result 关Fig. 5共d兲兴 reveals an even
smoother sample surface after deposition, indicating that the
particles are fully embedded in the multilayer. Even then,
they remain in a planar arrangement, as no traces of a second
layer or a significant reduction of the overall number of vis-
ible particles was found.
On a local scale, the structures formed in the intermedi-
ate as well as in the liquid crystalline phase represent the
desired conditions for possible high density storage applica-
tions: variable spatial separation together with the tendency
to form a two-dimensional array. With the particle deposition
density approaching 100%, the observed structure could be
obtained over an extended area. Based on the observed lat-
eral mobility, one can expect a similar degree of rotational
mobility of individual nanoparticles. Therefore, orientation
in a magnetic field should be possible as well. An interesting
technical option is offered if the multilayers are formed by
phospholipids with unsaturated hydrocarbon chains such as
POPC or DOPC. In this case, the liquid crystalline matrix is
easily turned into a solid polymer: UV- or ␥-irradiation of the
finished layer induces polymerization of the unsaturated hy-
drocarbon chains in a radical chain reaction.18 Hereby, the
516 J. Chem. Phys., Vol. 121, No. 1, 1 July 2004 Terheiden et al.

final structure gains mechanical stability and blocks any kind for the assistance in preparing the REM micrographs. This
of undesired particle rearrangement. work was supported by the Deutsche Forschungsgemein-
The potential of this particle embedding procedure is schaft in connection with the research Project No. SFB 445.
manifold. In connection with particle deposition from the gas
1
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to a large variety of particles collected by gas phase deposi- Soc. Symp. Proc. 705, 315 共2002兲.
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ACKNOWLEDGMENTS Growth 252, 440 共2003兲.
17
A. Terheiden, C. Mayer, K. Moh, B. Stahlmecke, S. Stappert, M. Acet, and
The authors acknowledge the support of A. Lorke, espe-
B. Rellinghaus, Appl. Phys. Lett. 共to be published兲.
cially for kindly allowing us to use spin coating facilities and 18
L. Shen, A. Stachowiak, T. A. Hatton, and P. E. Laibinis, Langmuir 16,
an AFM instrument. We further want to thank B. Stahlmecke 9907 共2000兲.