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Nucleation and growth of thin (Ba,Sr)TiO3 films in a MOCVD reactor

Nucleation and growth of thin (Ba,Sr)TiO3 films in a MOCVD reactor

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Published by Fotis Fitsilis
S. Regnery, Y. Ding, P. Ehrhart, F. Fitsilis, et. al. „Nucleation and growth of thin (Ba,Sr)TiO3 films in a MOCVD reactor”, MRS Proc. Vol. 748, p. U15.6.1 - U15.6.6 (2003)
S. Regnery, Y. Ding, P. Ehrhart, F. Fitsilis, et. al. „Nucleation and growth of thin (Ba,Sr)TiO3 films in a MOCVD reactor”, MRS Proc. Vol. 748, p. U15.6.1 - U15.6.6 (2003)

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Nucleation and growth of thin (Ba,Sr)TiO
3
films in a MOCVD reactor
S. Regnery
1,2
, Y. Ding
1
, P. Ehrhart
1
, F. Fitsilis
1
, C.L. Jia
1
, K. Szot
1
, R. Waser
1
,F. Schienle
2
, M. Schumacher
2
, T.McEntee
21)
IFF Forschungszentrum Jülich, D-52425 Jülich, Germany
2)
Aixtron AG Aachen, Kackertstr. 15-17, D-52072 Aachen, Germany
ABSTRACT
(Ba
x
Sr
1-x
)TiO
3
thin films were deposited on Pt electrodes in a planetary multi-wafer MOCVDreactor combined with a liquid delivery system. The nucleation behavior and the size of thestable nuclei were investigated by different SPM techniques and by XPS. Characteristicdifferences were observed between deposition temperatures of 565°C and 655°C, i.e. ahomogeneous nucleation of small BST grains on the larger Pt grains (100 – 200 nm in-planesize) at low temperatures and a dominating nucleation at the grain boundaries at hightemperatures. Further film growth was investigated for nominal film thickness between 5 and100 nm and details of the grain structure are revealed by HRTEM, e.g., randomly oriented grains(typical in-plane size 10-20nm) with a high density of twins at 565°C and (100)-oriented defectfree grains of slightly increased size at 655°C. As the electrical properties like permittivity andalso leakage current depend on film thickness the final discussions of the electrical properties arebased on thickness series and evaluated within the phenomenological dead layer model.
INTRODUCTION
High-K perovskite thin films, such as (Ba
x
Sr
1-x
)TiO
3
, (BST), have been proposed for a verybroad application area, including capacitor dielectrics for future dynamic random accessmemories (DRAMs), embedded capacitors, tunable devices, as well as gate oxides for fieldeffect transistors [1]. For capacitor applications of BST films, i.e., metal-insulator-metal (MIM)structures, Pt is considered as a standard metal electrode [2] and with MOCVD (metal organicchemical vapor deposition) different textures of the films have been observed for differentdeposition temperatures, e.g. typically BST-(100) on Pt-(111) for temperatures above 600°C andmore randomly orientated grains at lower temperatures [3]. However, details of the nucleationand growth behavior are still unknown. In this study a broad spectrum of analytic methodsincluding different types of scanning probe microscopy (SPM), high resolution transmissionelectron microscopy (HRTEM), and x-ray photoelectron spectroscopy (XPS) were used to get amore quantitative understanding. As electrical properties such as permittivity and also leakagecurrent depend on film thickness [4] the final discussions of the electrical properties are based onthickness series and evaluated within the phenomenological dead layer model.
EXPERIMENTAL DETAILS
(Ba
0.7
Sr
0.3
)TiO
3
films were deposited in an AIXTRON 2600G3 Planetary Reactor
 
, which canhandle five 6-inch wafers simultaneously. This reactor is characterized by a central gas inletwhich provides a pure horizontal gas flow and makes this reactor a radial flow system asdescribed previously [3]. The main process conditions are summarized in Table 1. The
U15.6.1Mat. Res. Soc. Symp. Proc. Vol. 748 © 2003 Materials Research Society
 
temperature of the wafer surface can be assumed to be 20° - 50°C lower than the directlymeasured susceptor temperature. The liquid precursors, 0.35molar solutions of Sr(thd)
2
andBa(thd)
2
and a 0.4molar solution of Ti(O-iPr)
2
(thd)
2
were supplied by an ATMI-300B liquiddelivery system.
Table I.
MOCVD process parametersSusceptor temperature 565°C, 655°CProcess Pressure 2.0 mbarGrowth rate 2 - 3 nm/minNominal film thickness 0.3 90 nmNominal stoichiometryBa
0.7
Sr
0.3
; Gr-II/Ti
0.96Generally, we used Pt/TiO
2
 /SiO
x
 /Si substrates, pre-annealed at 600°C, with a platinumthickness of 100nm. Additionally, substrates with ZrO
2
instead of TiO
2
adhesion layers wereused for XRF analysis. Because precise measurements are limited to about 5nm, the nominalthickness of thin film samples (0.3nm, 0.5nm, 1.5nm) was calculated from the deposition time;due to an uncertainty of about 3s in the switching time of the run–vent valve we have to consideran error of 30% in thickness specification for the thinnest films.SPM measurements were performed with a JEOL 4210 system in contact mode for themapping the electrical conductivity and in an AC SFM mode for the surface morphology. For theconductivity scans 0.1V was applied between the cantilever and the platinum bottom electrode.Similarly, conductivity scans of thin films (0.3nm and 0.5nm) were recorded. Assuming that thehigh resistivity areas can be related to the deposited BST, this mapping gives a good location of initial nuclei in relation to the bigger platinum grains.TEM and HRTEM investigations were carried out using a JEOL 4000EX electron microscopewith a Scherzer resolution of 0.17 nm at 400 kV. Cross-sectional as well as backside-polishedplan-view samples were prepared from the original wafers. After mechanical grinding anddimpling, these specimens were ion-milled to perforation on a stage cooled by liquid nitrogen.
NUCLEATION OF BST ON PT(111)
We start with the discussion of the conductivity mapping images. Fig.1a shows the platinumsubstrate. The image is dominated by the homogeneous distribution of the maximumconductivity, i.e. a current of almost 10nA, which is limited by the actual mating surfacebetween tip and bottom electrode. Randomly orientated darker spots indicate grain boundaries orsimply disruption during mapping. Fig.1b show a very thin film, nominally 0.3nm, grown at655°C, where we do not expect a complete coverage. Indeed, the deposited material firstaccumulates in the region of the platinum grain boundaries. Hence the platinum grain structure isnow clearly visible. This is an indication that the diffusion length of the precursor gases at thistemperature (655°C) is larger than the grain size of the platinum of 50nm to 200nm. For anincreased thickness of 0.5nm, Fig.1c, the insulating area has increased and most of the surface iscovered as additionally documented by a line scan which displays the values for theconductivity. The difference between maximum and minimum conductivity in the line scan isthree orders of magnitude.At a deposition temperature of 565°C there are significant differences in the deposition of thevery first nuclei. The brightest parts in Fig.2 have about the same conductivity as at 655°C. But
U15.6.2
 
the main area of the platinum grains is covered with insulating BST and there is no indication forpreferred nucleation at the Pt grain boundaries. In addition, a super-structure occurs with typicallength scales of about 30nm to 50nm. A sample with 0.5nm thickness shows no significantdifference in structure.
 Fig.1:
AFM conductivity mapping with images sizes of 500nm*500nm: a) platinum substrate. b)0.3nm BST layer, grown at 65C. Low conductivity is observed at the platinum grainboundaries. c) 0.5nm BST layer. The position of a line scan is indicated in the image; onlysmall regions with maximum conductivity are left.
Although topographic images can be obtained along with the conductivity mapping theresolution is not sufficient to deduce the critical features and additional scans were performed inan AC AFM mode. Fig. 3a shows the example of a 0.5nm thick film grown at 565°C. Weobserve round nuclei with a size between 10nm 20nm and there is an indication for anagglomeration without coalescence and structural rearrangement. For a further growth stage,3.0nm thickness, we can assume that the layer is now complete and the dominant structures mustbe considered as replicas of the platinum structure. Nevertheless, we additionally observe someline structure on the platinum grains, which are in good correlation with the structures on Fig.2;however, the resolution is not sufficient for further atomic details.
a bc
0.1nA2.0nA8.0nA1.0nA0.1nA2.0nA8.0nA1.0nA
 Fig.2:
Conductivity map of a 0.3nm BST/Pt filmdeposited at 565 °C. Image size: 500*500nm
2
. A line scan shows the modulation of depositionon a platinum grain.
U15.6.3

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