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C Japanese Society of Electron Microscopy Journal of Electron Microscopy 47(4): 335-343 (1998)

Full-length paper

EDS elemental mapping of a DRAM with an


FE-TEM
Masahiro Kawasaki 1 , Tetsuo Oikawa1, Katsuhiko Ibe 1 , Kyung-ho Park2, and
Makoto Shiojiri3
'JEOL Ltd, Akishima, Tokyo 196-8558, Japan, 2Texas Instruments Inc., 13570 North Central Expressway, MS3740,
Dallas, TX 75243, USA, and 3Kyoto Institute of Technology, Matsugasaki, Sakyo, Kyoto 606-8585, Japan

Abstract The elemental distribution in an O-N-0 dielectric multi-layer within a


dynamic random access memory (DRAM) device was investigated by X-ray
elemental mapping using a field-emission (scanning) transmission electron
microscope (FE-(S)TEM). The O-N-0 layer is designed to be an insulator
between a single-crystal silicon substrate and a poly-crystalline silicon in a
capacitor region. The nominal structure of the layer is SiO2-Si3N4-SiO2. A
small amount of phosphorus is doped in the poly-crystalline silicon to make
the poly-crystalline silicon conductive. Transmission electron microscopy
(TEM) was first used to view the microstructure in the layer. A bright field
image gave dear contrast in the O-N-0 layer, however, TEM images do not
provide direct information about the elemental distribution. X-ray mapping
was thus used to show this distribution. Initial observation of the oxygen
map and the nitrogen map confirmed that the layer composition was not
constructed as fabricated but oxygen and nitrogen migrated into each other
layer. The phosphorus map showed phosphorus segregation along the
interface between the poly-crystalline silicon and the neighbouring oxygen
layer, which is of importance to understand the device electrical property.
This phosphorus layer was not visible in the TEM image. Since the elemental
distributions across the structure were presumed to be uniform, X-ray
intensity profiles of Si, O, N and P could be obtained by compressing the
original X-ray images. The X-ray intensity of each column pixel was sufficient
to compute the concentration and thus elemental concentration line profiles
were obtained to characterize the structure quantitatively from the previously
obtained elemental maps.
Keywords EDS, elemental mapping, DRAM, FE-(S)TEM, quantitative analysis
Received 26 November 1997, accepted 21 April 1998

Introduction characterization of semiconductor devices [3], especi-


ally for investigating the dopant segregation phenomenon
A field-emission transmission electron microscope
(FE-TEM) significantly improves the material analytical in poly-crystalline silicon [4] and for other general
resolution in terms of both analysis time and space due dopant segregation in ultra-large-scale integration (ULSI)
to the significantly smaller and brighter source available devices [5]. However, very few studies have been reported
from the FE emitter. It is thus a unique nanometer scale on measuring and characterizing elemental distribution
analytical tool for materials science [1]. Elemental analysis in these devices using the X-ray elemental mapping
through energy dispersive X-ray spectroscopy (EDS) and technique. This technique, the most improved through
electron energy loss spectroscopy (EELS) has been success- the use of an FE gun, provides a reliable method to inspect
fully applied to materials research especially in conjunc- the chemical composition of a device on a nanoscale. In
tion with a focused probe for point analysis [2]. This this study, a dielectric O-N-0 layer at a capacitor region
point analysis method has been used extensively in the in a DRAM was carefully analysed, and especially the
336 JOURNAL OF ELECTRON M I C R O S C OP Y, Vol. 47, No. 4, 1998

analysis of the dopant migration behaviour was of impor- lent to a commercial 16-mega bit DRAM. In order to
tance as it directly influences the electrical property of make it suitable for TEM analysis, the specimen was
the device. Thus the elemental distribution on the O-N- thinned using the cross-section ion milling method. The
O layer in the DRAM device was successfully visualized O-N-O layer located at a capacitor portion of trench-type
qualitatively and also analysed quantitatively using X-ray cell in the device was examined using a JEM-2010F
mapping. FE-(S)TEM with an objective lens spherical aberration
coefficient of 1.0 mm and a consequent probe size/
probe current of 0.5 nm and 100 pA, respectively. The
Experimental microscope was further equipped with a JEOL ultra-thin-
The specimen selected for this experiment was cut from window (UTW) type-EDS detector capable of detecting
a fully processed test-elements group (TEG) device equiva- boron and a NORAN EDS system for signal processing.
The solid angle for the X-ray detection is 0.13 sr. This
combination of the FE gun and the objective lens system
has enabled EDS analysis perform with high detection
sensitivity [6]. The microscope was operated at 200 kV
during the entire experiment. High resolution TEM was
first employed to observe the O-N-0 layer, and the layered
structure observed in the O-N-0 layer by TEM was then
probed with a focused beam of 0.5 nm for EDS analysis.
Subsequently, X-ray elemental mapping was performed
for the specific elements previously detected by point
analysis.
An elemental map is obtained by scanning the focused
probe in a raster fashion across the specimen. Preset
characteristic X-ray energy windows from previously iden-

Table 2. The applied energy windows for Si, P, O and N to acquire


elemental maps of the O-N-O layer.

Low limit High limit Width


Elements (keV) (keV) (keV)
Si 1.69 1.8.0 0.11
2.07
P 1.96 0.11
O 0.48 0.57 0.09
N 0.34 0.43 0.09

Table 3. The measured layer widths of P, O and N with the STEM BF


contrast width of the O-N-0 layer.
Measured layer widths
Elements or item (pixel number)
STEM BF contrast of O-N-O layer 5.7-8.0
Fig. 1 A schematic diagram of digital EDS elemental mapping. After the
76-83
energy windows of desired elements are set, the EDS computer controls P
the probe scan digitally. Meanwhile, a STEM image signal from a PMT O 57-68, 69-80
and X-ray intensities of the desired elements from an X-ray analyser are
N 57-80
monitored in accordance with the scan position.

Table 1. Examples of various image acquisition parameter settings when 1 nm spatial resolution is required. The applied probe size should be
optimized because the spatial resoluuon in practice is limited by the beam broadening rather than the applied probe size.

Scan area Pixels Magnification Pixel size Dwell time Total time
(nm) (nm 2 ) (msec) (min)
31 X 31 64X64 2000 000 0.482 50 3 41
62.5 X 62.5 128 X 128 1000 00O 0.482 25 6.83
150 X 150 256X256 500 000 0.48 2 15 16.38
M. Kawasaki et al. EDS elemental mapping of a DRAM 337

Single-crystal silicon O O Poly-crystalline silicon


2.2nm 2.6nm

Fig. 2 A high resolution TEM image of the O-N-0 layer. The TEM image contrast across the insulator indicates that there are three layers. Circles
A, B and C indicate the positions where EDS point analysis was accomplished.

tified elements are set and intensity maps are generated further quantitative processing. FE-TEMs generally pro-
using these window intensities, each point in the X-ray vide sufficient probe current in 1-nm and smaller probes
map corresponding to an image point in the scanned for elemental mapping and can thus give a reasonable
image. Either digital or analog scans can be used to signal-to-noise ratio with a spatial resolution of ~1 nm
generate the maps. The former can only map one element [8]. The spatial resolution is a function of the applied
at a time and can only display the presence or absence of probe size and the image pixel size (actual distance
an element. No relative intensity information can be between pixel points on the image), and the signal-to-
generated. In the latter case, probe scan is controlled noise ratio is related to the probe current and the dwell
digitally by the EDS computer and all necessary X-ray time. Table 1 shows examples of various image acquisition
maps are produced simultaneously. In addition, a relative parameter settings. The consuming time for a total acquisi-
X-ray intensity is represented at each scanned point. A tion shown in Table 1 is based on without dead-rime
STEM image can also be obtained corresponding to the correction and the processing time on each pixel so
maps by collecting the transmitted electrons with a photo- that the aaual total acquisition time will become longer
multiplier (PMT). Figure 1 shows the schematic for digital accordingly. In order to obtain the best signal-to-noise
X-ray elemental mapping [7]. ratio at the highest spatial resolution, it is necessary to
In this study digital mapping was utilized to allow set the longest acquisition time per point consistent with
338 JOURNAL OF ELECTRON MI C R 0 S C OP Y, Vol. 47, No. 4, 1998

200 acquisition times per pixel volume are typically very much
less than average pixel to pixel drift rates, and the distorted
X-ray map/STEM image are thus accurate representations
of the spatially resolved chemical distribution. Today there
is software that will compensate for specimen drift, thus
allowing cumulative acquisitions with high spatial reso-
lution. In this experiment, the image drift was confirmed
negligible by comparing two images taken before and
after the acquisition so that any drift compensation was
not accomplished.
In this manner the O-N-0 layer was chemically visual-
ized by elemental maps showing Si, O, N, and P. Quantitat-
ive line profiles were then derived from the obtained
elemental maps.

Results and discussion


High resolution TEM observation
Figure 2 shows a high resolution TEM image of the O-N-0
layer. There are three clearly different contrast variations
between the crystal silicon substrate and the poly-crystal-
line silicon. The interfaces of these contrast layers are
not dearly defined. The layers appear to be -2.2 nm,
-5.7 nm, and -2.6 nm in width. Based on known fabrica-
tion parameters, the layers are likely to be SiO2, Si3N4
and SiO2 amorphous phases. This is to be subsequently
determined by EDS analysis.

200- EDS analysis


c Figure 3 shows EDS speara obtained from the three
SI layers. These point-analysed spectra were collected in a
30 s live time using a 0.5 nm probe with -100 pA. These
J spectra represent the chemical composition of these layers
as they were fabricated though two of the layers repres-

><
1 00- - ented by position A and C contain some nitrogen and the
a layer represented by position B contains some oxygen. O
layers should contain only Si and O, and N layer should
contain only Si and N. Though this result appears to

0-
0
A JL.1 2
X-ray
3
energy (keV)
4 5
contradict the presumed fabrication parameters, its valid-
ity can be ascertained by considering the actual spatial
resolution of the measurement. The spatial resolution is
determined by both the initial probe size and the magni-
tude of beam broadening as the beam traverses the
specimen. To calculate the beam broadening, it is neces-
Fig. 3 EDS speara from positions A, B and C obtained at the effective sary to know the thickness of the specimen. The thickness
probe size 0.7 nm and acquisition time of 30 s. Oxygen and nitrogen
exist in both layers. This suggests that some oxygen and nitrogen diffused of the analysed area was roughly estimated to be 60 nm
into neighbouring layers. by comparing the analysis position with the first Si(lll)
equal thickness fringe from the thin edge of the specimen.
Then, by assuming the thickness uniformity across the
a resolution-limiting probe and a specimen drift rate. If O-N-0 layer, the beam broadening inside the specimen
one is dissatisfied with the image distortion caused by was calculated basically with the single scattering model
image drift (on STEM, image drift is associated with [9,10] but the constant part of the original beam
specimen drift and probe drift), the map is still very broadening expression was modified from the experi-
useful for analysis since the X-ray intensity of each mental result. The sample used for this experiment was
pixel corresponds to a commensurate image pixel. Pixel an MgO cubic crystal sample. The probe size was measured
M. Kawasaki et al. EDS elemental mapping of a DRAM 339

14

12--

r 10

s
sen
JB
8
"S
1 6
Probe

2--

100 200 300 400 500 600 700 800


Thickness(nm)
Fig. 4 The beam broadening as a function of the specimen thickness. The solid line is experimental result and the dashed line is derived from
calculation. The probe size recorded on an IP was measured containing 90% of the scattered elearons. Then the experimental beam broadening b
was obtained using b2 = bm2 - b02, where bm and b0 are the beam sizes at the exit surface and at the entrance surface of the specimen, respectively.

by an imaging plate (IP) which has a linear sensitivity Both oxygen and nitrogen X-rays are absorbed by the
property to the electron intensity with wide dynamic specimen. Fluorescence of these elements by Si is not a
range [11]. The measured beam broadening was compared factor in the quantification of oxygen and nitrogen since
with the calculated value by the single scattering model. the sample is too thin for fluorescence to be a factor.
Figure 4 shows the beam broadening as a function of the Therefore, since the effective probe size is smaller than
specimen thickness obtained by the above experiment the layer to be analysed, it does not excite X-rays from
and the calculation. The solid line shows the experimental adjacent layers. Thus, the chemical composition of the
result and the dashed line is derived from calculation. layers is confirmed as being specific to each layer and
From this experimental result, the constant part in the that further, the composition does not conform to that
original expression was modified to fit the calculated predicted by the fabrication compositions, indicating that
beam broadening values to the experimentally measured both oxygen and nitrogen have migrated into regions that
ones and thus the beam broadening b that was used in were thought to be bereft of both.
this study is obtained as Also not predicted but of importance is the existence
of phosphorus in position C. This shows that phosphorus
b = 0.63 X 105 X X X migrates from the poly-crystalline silicon to the neigh-
bouring oxygen layer. Phosphorus is doped in the poly-
where Z is atomic number, A is atomic weight, Eo is crystalline silicon area to make a poly-crystalline silicon
accelerating voltage (eV), p is density (g/cm3), and t is as a conductor. It is also necessary to make this phosphorus
specimen thickness (cm). doping as uniform as possible in the area. Otherwise if
The effective probe size, which is the combination of phosphorus segregates in a certain area, it would become
the beam size at the entrance surface of the specimen (in a path of electrons and then it could cause current leakage
this case 0.5 nm) and the beam broadening inside the to damage the device. The existence of phosphorus may
specimen obtained from the above expression (in this be thought to contribute to the TEM contrast and explain
case 0.2 run) was now estimated to be 0.7 nm. the contrast variation between two layers of oxygen.
340 JOURNAL OF ELECTRON M I C R O S C O P Y, Vol. 47, No. 4, 1998

STEM image 0N0 poly Si

lOnm

EDS maps Si

Fig. 5 EDS digital maps of Si, O, N and P. The elemental distribution on the insulation layer is visualized chemically. Oxygen is distributed on the
outside of the insulator and the nitrogen in its middle. P map shows phosphorus segregation along the interface with poly-crystalline silicon.
M. Kawasaki et al. EDS elemental mapping of a DRAM 341

128

128
Fig. 6 The concentration profiles of Si, O, N and P across the layer overlaid on the corresponding elemental maps. P is segregated over a width
-3 nm across the interface of the oxide layer and the poly-crystalline silicon. P concentration is -2.2 at%.

However, the amount of doped phosphorus in the device ally for oxygen and nitrogen so that each individual
is extremely small and thus does not likely give rise to energy intensity was well resolved and collected. The
TEM image contrast. The phosphorous is thus detected condition for the elemental mapping was such that each
exclusively by EDS analysis [5]. digital image size was 128X128 pixels corresponding to a
scanned area of 62.5X62.5 nm, the electron probe size
EDS elemental mapping was 0.7 nm with 230 pA and the dwell time per pixel
EDS digital elemental mapping was used to visualize was 25 ms. A complete map including the STEM image
elemental distribution; particularly phosphorus distribu- thus took ~7 min to complete. The maps clearly show the
tion was of more interest because of above mentioned distribution of N and O in the three layers and more
reason. Figure 5 shows EDS maps of Si, O, N and P with importantly P segregation along the interface between the
a STEM image. Table 2 shows the energy window widths poly-crystalline silicon and the neighbouring O layer.
for the applied elements. These windows were set especi- In order to understand the elemental distribution in a
342 JOURNAL OF ELECTRON M I C R 0 S C O P Y, Vol. 47, No. 4, 1998

(a) Incident probe Phosphorus segregation


0.7nm<!> O-N-0 -4 Poly-Si

Pixel
(0.48x0.48nm2) / / / / / / / / / / / / /

(b)

Pixel

Fig. 7 A schematic diagram of a digitally scanned probe across the phosphorus segregation (a) and the corresponding X-ray intensity distribution
(b). The incident probe size of 0.7 nm onto a pixel size of 0.48 nm 2 is broadened by specimen thickness to 0.9 nm. Two pixels before and after the
probe scans the elemental distribution contribute to the X-ray generation of the element.

quantitative manner, the axis parallel to the layer was Thus the highest X-ray intensity positions of N and O
compressed and accordingly adequate statistical signific- were presumed to be Si3N4 and SiO2 respectively and
ance could be obtained to attempt to quantify the intensity used as standard to calculate the k-factors. On the other
and consequently the composition across each layer. hand, the k-factor of P for Si was determined through
Fortunately, the specimen thickness changes parallel to potassium by using two standard samples of known
the layer direction insignificantly so that the absorption stoichiometry KT1OPO4 and KAlSi3O8 Consequent k-
of oxygen and nitrogen X-rays across the layer is assumed factors of N, O and P for Si were obtained as 6.3, 6.9 and
to be constant. By integrating column pixels, each column 1.0 respectively. Figure 6 shows calculated concentration
pixel dwell time became equivalent to a 3.2 s acquisition profiles of Si, P, O and N across the layer overlaid onto
time and thus gave reasonable signal intensity from which the corresponding elemental map. The statistical errors
to convert to a concentration. The background intensity defined by three times of standard deviation for Si, O,
of each elemental energy window was subtracted before N and P concentration profiles are 5.48%, 5.49%,
quantification. The background intensity was estimated 2.65% and 0.21% respectively [12]. When the edge
in such a way that N and P do not exist on the single to edge pixel width of a peak is considered for measuring
crystal silicon, therefore the averaged intensities of N and the layer width, the two layers of oxygen are thus both
P on the single crystal silicon could be regarded as 12 pixels, and the nitrogen layer is 24 pixels corresponding
background intensities for N and P. And also these energy to 5 nm, 11 nm in real space. Table 3 shows the measured
windows were of the same width as those of O and Si, layer widths in pixel of P, O and N with the simultaneously
and the energies of N and O, and P and Si are close each obtained STEM bright field (BF) contrast width. This
other. Hence these background intensities of N and P result shows that oxygen and nitrogen diffuse into the
could be substituted to the ones of O and Si, respectively. neighbouring layer but still preserve the layer structure.
The k-factors of N and O for Si were determined by such The full peak width of phosphorus is 8 pixels across the
a way that while oxygen and nitrogen migrated into each boundary of the oxide layer and poly-crystalline silicon.
other, the centre regions of oxygen and nitrogen layers The effective probe size 0.9 nm, which is the combination
could be considered to still preserve the composition. of the probe size 0.7 nm and the beam broadening 0.2
M. Kawasaki et al. EDS elemental mapping of a DRAM 343

run, was larger than t h e pixel size on t h e image. Therefore J o v D c - R o m i 8 A D and


' Go ld * tein J l PP- 191-204, (Plenum.
N e w
, . i i_ i J * i_ i- . York)-
each o n e pixel before a n d after t h e probe scans t h e ;"" ;-, : ", '. "V ;-
10 Reed S J B (1982) The single-scattering model and spatial resolution
distribution of P contributes to t h e P X-ray generation as j n x . r a y analysis of thin foils, uitramicwscopy T. 495-410.
illustrated in Fig. 7. The p h o s p h o r o u s Segregation is thus u M o r i N_ oikawa T. Harada Y, and Miyahara J (1990) Development
estimated as 6 pixels width, which is 3 n m in real space of the imaging plate for the transmission electron microscope and Its
and the concentration of P corresponds to 2.2 at% from
Fig. 6. The scale and concentration of phosphorus migra-
tion obtained by elemental maps agree with those in other microscopy, ed. Joy D c, Romig A D, and Goldstein j i, pp. 188-189,
reports [5]. Therefore these maps with concentration are (Plenum. New York).
clearly showing the elemental distribution of the O-N-O
layer quantitatively. The mechanism of the contrast differ-
ence of these two oxide layers is still unknown. However,
it would be most likely related to migration of oxygen
and nitrogen with silicon. A further experiment should
be carried out to measure the concentration with higher
spatial resolution to investigate the mechanism of the
contrast difference.

Conclusion
The nitrogen and oxygen distribution was visualized by
EDS elemental mapping. This technique provides informa-
tion on spatially distributed elements and is a more reliable
method to inspect the device fabrication parameters than
conventional bright field TEM imaging. The elemental
concentration was also obtained by quantitative X-ray
intensity calculation using the elemental maps. X-ray
elemental mapping is a very powerful tool for failure
analysis and also determining the fabrication parameters
and compositions.

References
1 Honda T, Tomita T, Kaneyama T, and Ishida Y (1994) Field emission
ultrahigh-resolution analytical electron microscope. Ultramicroscopy
54: 132-144.
2 Bando Y (1994) Microstructure analysis of advanced ceramics by
high-resolution analytical transmission electron microscopy.
J Electron Microsc- 44: 115-123.
3 Mullan C A, Weatherly G C, and Thompson D A (1996) STEM
analysis of compositional modulations in InGaAsP films grown on
patterned substrates. JEOL News 32E-1: 12-15.
4 Grevenor C R M, Batson P E, Smith D A, and Wong C (1984) As
segregation to grain boundaries in Si. Philosophical Magazine A 50:
409-423.
5 Park K H. Hashimoto S, Kawasaki M, and Ibe K (1995) Sub-
nanometric elemental analysis on ULSI devices with FEG-TEM. In:
Institute of Physics Conference Series No. 146, ed. Cullis A G and Staton-
Bevan A E, jpjp. 575-578, (The institute of Physics, London).
6 Cook J, Sloan J, Chu A, Heesom R, Green M L H , Hutchison J L,
and Kawasaki M (1996) Identifying materials incorporated into
carbon nanotubes by HREM and microanalysis. JEOL News 32E-1:
2-5.
7 Newbury D E (1997) Chemical compositional mapping by mlcrobeam
analysis at the micrometer scale and finer. Microelectronics J. 28:
489-508.
8 Murakoshi H, Kakibayashi H, and Tsuchiya T (1996) High resolution
X-ray elemental mapping using 300-kV field emission TEM. J. Electron
Microsc. 45: 236-238.
9 Goldstein J I, Williams D B, and Cliff G (1986) Beam broadening and
X-ray spatial resolution. In: Principles of analytical electron microscopy.

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