J Forensic Sci, May 2016, Vol. 61, No.

3
doi: 10.1111/1556-4029.13076
TECHNICAL NOTE Available online at: onlinelibrary.wiley.com

QUESTIONED DOCUMENTS

Jiye Kim,1,2 M.Sc.; MinJung Kim,3 M.Sc.; JinWook An,4 Ph.D.; and Yunje Kim,1 Ph.D.

Determination of the sequence of intersecting

lines using Focused Ion Beam/Scanning
Electron Microscope*

ABSTRACT: The aim of this study was to verify that the combination of focused ion beam (FIB) and scanning electron microscope/energy-
dispersive X-ray (SEM/EDX) could be applied to determine the sequence of line crossings. The samples were transferred into FIB/SEM for
FIB milling and an imaging operation. EDX was able to explore the chemical components and the corresponding elemental distribution in the
intersection. The technique was successful in determining the sequence of heterogeneous line intersections produced using gel pens and red
sealing ink with highest success rate (100% correctness). These observations show that the FIB/SEM was the appropriate instrument for an
overall examination of document.

KEYWORDS: forensic science, document examination, scanning electron microscope, sequence discrimination, intersections, line sequence

Seals are often used to form an impression in ink on personal
documents, office paperwork, contracts, art, and other docu-
ments, as an alternative of in addition to a handwritten signature
in Far East Asia (1). The determination of the order of crossing
lines is appropriate in cases of suspicions that the content of a
document has been altered at a later date by adding a part to it,
for instance, in a will or signed legal agreement (blank signature)
(2). Therefore, the determination of the sequence of crossing
stroke (3–5) can provide important information when investigat-
ing a fraud (6).
This technique has already proven its applicability in the char-
acterization of biological samples (7–9). A combination of
focused ion beam (FIB) milling and scanning electron micro-
scope (SEM) observation in a dual-beam apparatus makes imag-
ing of sample cross sections possible in well-defined areas (10).
An energy-dispersive X-ray spectroscopy (EDX) system for
chemical composition analysis is added to our dual-beam sys-
tem. In situ EDX is used to select among particles of diverse
compositions a specific particle to be milled. Thus, this combina-
tion of an ion beam with an electron beam allows extensive
analysis of the surfaces or the interiors of questioned documents
(11).
1
Environmental Technology Research Center, Korea Institute of Science
and Technology, 131, Cheongryang, Seoul, Korea.
2 Sign of approximately equal width and thickness was drawn
Department of Chemistry, Korea University, 145, Anam-ro, Seongbuk-gu,
Seoul, Korea.
3
Forensic Science Division in Supreme Prosecution Service, Document
Examination Section of National Digital Forensic Center, 157 Banpo-daero,
Seocho-gu, Seoul, Korea.
4
Kyunghee Univirsity, Hoegi-dong, Dongdaemun-gu, Seoul, Korea.
*Financial support provided by the research project of Forensic Science
Division in Supreme Prosecution Service.
Received 11 Feb. 2015; and in revised form 1 June 2015; accepted 13
June 2015.
However, to our knowledge, the combination of FIB and
SEM techniques has not been applied to the study of forensic
document examination. When applied to intersecting lines on
paper, the combined FIB/SEM technique provides high-resolu-
tion imaging of the paper surface, gel pen ink, and red sealing
ink particle, while, at the same time, it makes cross-sectioned
samples available for postmodification analysis by other tech-
niques, such as traditional SEM or atomic force microscopy
(AFM).
Here, we present examples of the efficient incorporation of
FIB/SEM into morphological and compositional research dealing
with forensic document samples.
Experimental
The samples were prepared in the following manner to ana-
lyze the sequence of intersecting lines. The substrate used was
uncoated paper supplied by Double A Public Co., Ltd. Five
black gel ink pens and three red sealing inks (the most com-
monly used product in Korea) were collected from various com-
panies and coded with their data as shown in table 1.
Three types of specimens were prepared: Specimen A con-
sisted of red sealing ink layered over gel pen ink, and specimen
B consisted of gel pen ink layered over red sealing ink. Speci-
men C consisted of red sealing ink layered over red sealing ink.
using the tested pens on paper sample. The first ink was allowed
to dry for 1 h before the application of second ink when making
the intersections. All of specimens were left at room temperature
for 3 days before analysis.
Focused ion beam/scanning electron microscope (FIB/SEM)
experiments were performed using an Helios 600 Nanolab (FEI,
Einthoven, Netherland) with a liquid gallium and field emission
electron sources. The sample was then sputter-coated with a

© 2016 American Academy of Forensic Sciences 803

804 JOURNAL OF FORENSIC SCIENCES

TABLE 1––List of writing instruments (red sealing inks and pen) of different morphological analysis alone of intersections involving red
brands used in the study. sealing ink is problematic due to its high penetrability (12).
Focused ion beam/scanning electron microscope offers the
Type of
No. Instrument Company Model
ability to perform accurate, homogeneous slicing and to select a
specific site of interest. Figure 2 shows a FIB-milled cross sec-
1 Gel pen MITSUBISHI PENCIL CO., Uni-ball Signo DX tion through questioned document. A platinum layer has been
LTD. 0.28
2 Gel pen PILOT BPS-GP-XB-B
vapor-deposited in situ, to protect the top surface of the red seal-
3 Gel pen Delistar No.6600 GEL PEN ing ink particles and gel pen ink particles from the ion beam
0.5 and ensure that surface topography is preserved during milling.
4 Gel pen Dong-A U-KNOCK Gel 0.5 As this example shows, the FIB/SEM approach allows us to
5 Gel pen ZEBRA BR-6A-SK-BK 60 visualize the interior of the specimen in a very precise manner.
6 Red sealing ink Hwashin Ink pad (threaded)
7 Red sealing ink Gail Quick set ink The application of FIB/SEM technique is a very powerful for
8 Red sealing ink KOREA STAMP Quick set Super Red such line crossing investigations. This method based on the sur-
Sun face examination of the ink deposits in the intersection area.

Gel Pens Layered over Red Sealing Inks and Reversed

palladium alloy (a thickness of 50~100 nm) to eliminate the
electrostatic effects (E-1030 ion sputter; Hitachi, Tokyo, Japan).
The FIB provided a 30 kV Ga+ ion beam with a current of
approximately 93 pA. The simultaneous imaging was performed
via the SEM. To ensure the EDX analysis results are reliable
and consistent, EDX spectrums were taken at different locations
of the individual defect for all samples.
Results and Discussion
One of the popular methods is that an examiner magnified the
intersecting area of red seal impression and signature in the doc-
ument with an aid of an optical microscope to visually discrimi-
nate whether the red seal is impressed over or under the
signature (12,13). This method states that the strokes’ sequence
resulted in the examination depends on optical effects, such as
color. However, when all strokes are the same color, the classi-
cal method based on color characteristics cannot solve problem
successfully.
The SEM images were objective evidence, but some of them
were relatively unclear. Other authors already argued that
(Specimen A, B)
We tested in the case of the gel pen layered over the red seal-
ing ink (Specimen A). As depicted on scanning electron micro-
graphs of regions (Fig. 1), a certain amount of red sealing ink
particles appear flattened and damaged, possibly caused by the
mechanical force of the gel pen-tip. This observation indicates
that the red sealing ink particles are overwritten by gel pen ink.
Figure 2(a,b) shows detailed pictures of the cross-sectional
views of the interface between gel pen inks and red sealing ink
particles. There is a clear boundary between the ink deposits and
the red sealing ink deposits. The feature indicated by an arrow is
part of the ink deposit region located at the base of the red seal-
ing ink deposits (seen in the centre of Fig. 2b).
Energy-dispersive X-ray analysis was used to check the chem-
ical composition of the exposed surface of specimen A (Fig. 2c,
d). When the two spectra are compared, the difference in metal
composition can be seen clearly. As expected in the spectrum,
major amounts of carbon and oxygen were detected.
We checked the opposite case of the red sealing ink over the
gel pen layered (specimen B). Figure 3 presents the SEM images

FIG. 1––Scanning Electron Microscope image of specimen A (gel pen layered over red sealing ink). (a) Magnification: 80x, Tilt: 25° (b) Magnification: 80x,
Tilt: 45°.
 KIM ET AL. . DETERMINATION OF INTERSECTING LINES 805

(a) (b)

HV mode WD HFW mag tilt 4 µm HV mode WD HFW mag tilt 1 µm

2.00 kV SE 4.0 mm 12.8 µm 10 000 x 52 ° KIST 2.00 kV SE 4.0 mm 3.66 µm 35 000 x 52 ° KIST

(c) Spectrum 4 Spectrum 1

(d)

C
Ca
C
Ca
Cl

O Ca O Ca
Ca Cl Cl Ca
0 1 2 3 4 5 6 0.5 1 1.5 2 2.5 3 3.5 4 4.5
Full Scale 9577 cts Cursor: 1.340 (126 cts) keV Full Scale 5976 cts Cursor: 1.340 (83 cts) keV

FIG. 2––(a, b) Scanning Electron Microscope image showing the region where the FIB milling is taking place. (c, d) The FIB-exposed region was EDX
analyzed.

FIG. 3––Scanning Electron Microscope image of specimen B (red sealing ink layered over gel pen). (a) Magnification: 80x, Tilt: 25° (b) Magnification:
500x, Tilt: 45°.
806 JOURNAL OF FORENSIC SCIENCES

of crossing areas and shows the granular pigment particles lie on
top of the ink paste (gel pen). It clearly shows that red sealing
line was made after gel pen line, because its shape is continuous,
whereas line is interrupted. As can be noted, a characteristic of
the second line is that it “overlaps” the first one.
The same sample crossings as shown above have been
checked by FIB/SEM examination which confirmed the SEM
results. One of these regions is clearly visible in Fig. 4a,b as a
result of the weak contrast of the dislocations.
The FIB-exposed region was EDX analyzed. The EDX spots
spectra at two different locations on the FIB-exposed surface of
specimen B. When the two spectra are compared, the difference
in metal composition can be seen clearly.
We tried five kinds of gel pen inks and three kinds of red
sealing inks individually and showed same results.
Red Sealing Inks Layered over the Red Sealing Inks (specimen
C)
The crossing zones of the prepared samples were examined
by SEM. Figure 5 shows the case of crossing between two types
of red sealing ink. Both lines could be distinguished by their sur-
face appearance. As depicted on Fig. 5(a,b), one granular pig-
ment particles lie on the top of the other ink paste, and
therefore, the sequence is clearly recognizable.
The samples were further investigated using FIB/SEM for a
better characterization of the interface. The feature indicated by
an arrow is part of the ink deposit region (B) located at the base
of the red sealing ink deposits (A) (seen in the centre of
Fig. 6b).
The same sample crossings as shown above have been
checked by EDX. When the two spectra are compared, the dif-
ference in metal composition can be seen clearly. As expected in
the spectrum, major amounts of carbon and oxygen were
detected. We tried three kinds of red sealing inks individually
and showed same results.
Blind Testing
A blind sample was prepared with the same red sealing ink
and gel pen. The FIB/SEM photograph and EDX mapping were
collected by same method as aforementioned. Twelve volunteers
were chosen to test the effectiveness of this method. After being
given the basic knowledge of this method, the volunteers were
demanded the analysis of the FIB/SEM photograph and EDX
mapping of the blind sample (Figs 1 and 2). One-hundred per-
centage of them think blind sample is consisted of gel pen lay-
ered over red sealing ink, which correct answer. Therefore, these
data show the apparent usefulness of FIB/SEM in field of foren-
sic science.
Conclusions
The combination of FIB lithography and high-resolution SEM
in a double-beam instrument has proven to be a useful tool for
the study forensic document examination. This technique allows

(a) (b)

HV mode WD HFW mag tilt 5 µm HV mode WD HFW mag tilt 4 µm

2.00 kV SE 4.0 mm 19.7 µm 6 500 x 52 ° KIST 15.00 kV SE 4.0 mm 10.7 µm 12 000 x 52 ° KIST

Spectrum 1 Spectrum 2
(c) (d)

C
Ca C
Ca
Cl
Ca
O Cl Cl Ca Ca O Ca

0.5 1 1.5 2 2.5 3 3.5 4 4. 0.5 1 1.5 2 2.5 3 3.5 4 4.

Full Scale 6973 act Cursor: 2.576 (66 cts) keV Full Scale 6973 act Cursor: 2.576 (66 cts) keV

FIG. 4––(a, b) Scanning Electron Microscope image showing the region where the FIB milling is taking place. (c, d) The FIB-exposed region was EDX ana-
lyzed.
 KIM ET AL. . DETERMINATION OF INTERSECTING LINES 807

(a) (b)

FIG. 5––Scanning Electron Microscope image of specimen B (red sealing ink layered over the other red sealing ink). (a) Magnification: 350x, Tilt: 25° (b)
Magnification: 1500x, Tilt: 45°.

(a) (b)

HV mode WD HFW mag tilt 4 µm HV mode WD HFW mag tilt 1 µm

2.00 kV SE 4.0 mm 12.8 µm 10 000 x 52 ° KIST 2.00 kV SE 4.0 mm 5.12 µm 25 000 x 52 ° KIST

(c) Spectrum 5 Cl (d) Spectrum 8

C
Ca

C
Ca

Cl O
O S Cl Ca Cl Ca
S Cl Ca Cl Ca

0 0.5 1 1.5 2 2.5 3 3.5 4 4.5 5 0.5 1 1.5 2 2.5 3 3.5 4 4.5 5
Full Scale 6312 cts Cursor: 0.000 keV Full Scale 1578 cts Cursor: 2.489 (45) cts keV

FIG. 6––(a, b) Scanning Electron Microscope image showing the region where the FIB milling is taking place. (c, d) The FIB-exposed region was EDX ana-
lyzed.
808 JOURNAL OF FORENSIC SCIENCES
us to achieve high-resolution imaging of localized cross sections
of the questioned documents. When using the FIB/SEM tech-
nique with samples that have been properly prepared, it is possi-
ble to image the sequence of intersecting lines.
Experiment results show that the proposed method can be
applied to forensic investigation for falsely signed documents by
discriminating the sequence of seal impression and signature in
the documents.
Also, we plan to extend the scope of this research by conduct-
ing a detailed investigation through which we will be able to
distinguish between nonpigmented stamp inks and fluid-based
inks with respect to technique and expression, thereby improving
the content.
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Additional Information and reprint requests:
Yunje Kim, Ph.D.
Center for Clean Energy
Korea Institute of Science and Technology
P.O.Box 131
Cheongryang
Seoul
Korea
E-mail: yjkim@kist.re.kr