Applied Surface Science 604 (2022) 154524

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Applied Surface Science

journal homepage: www.elsevier.com/locate/apsusc

Full Length Article

A robust and scalable electron transparent multi-stacked graphene gate for

effective electron-beam convergence in field emission digital X-ray sources
Yujung Ahn a, b, Seong Jun Kim b, Eunsol Go a, b, Jeong-Woong Lee a, b, Sora Park b,
Jin-Woo Jeong b, Jae-Woo Kim b, Jun-Tae Kang b, Ki Nam Yun b, Sunghoon Choi b,
Sunghee Kim b, Ji-Hwan Yeon b, Yoon-Ho Song a, b, *
a
ETRI ICT School (Advanced Devices Engineering), University of Science and Technology, 217 Gajeong-ro, Yuseong-gu, Daejeon 34113, South Korea
b
Nano-Electron Source Research Section., Electronics and Telecommunications Research Institute (ETRI), 218 Gajeong-ro, Yuseong-gu, Daejeon 34129, South Korea

A R T I C L E I N F O A B S T R A C T

Keywords: Recently, carbon nanotube (CNT)-based field emission digital X-ray sources have received enormous attention in
Field emissions medical and industrial imaging systems. For high-resolution X-ray images, the field-emitted electron-beam (e-
CNT emitter beam) must create a small focal spot size onto an anode by properly converging and focusing of e-beam. Here,
E-beam convergence
multi-stacked graphene by using a layer-by-layer (LBL) stacking method was fabricated as an electron trans­
Triode structure
parent graphene gate (ETGG) for effective e-beam convergence. The ETGG that was completely made on mo­
Graphene
Micro-lens lybdenum (Mo) apertures with scalable diameters of 300 µm extracted and then effectively converged e-beams
onto the anode in a triode structure. From the current–voltage measurements, the ETGG reduced turn-on voltage
of CNT paste emitters by approximately 24%, as compared with an aperture-gate. The e-beam area originating
from the CNT paste emitters with the ETGG was largely converged (almost 77%) compared to the aperture-gate,
and scattering of the primary e-beams was eliminated with an optimized collimation module. Long-term dura­
bility of the ETGG was confirmed, as the graphene on the apertures robustly remained without any deterioration
even upon the 140,000 shots of several-keV-electron bombardment in pulse operation mode. These results
demonstrate the potential and suitability of the ETGG for application in field emission digital X-ray sources.

1. Introduction
Since the discovery of field emission via quantum mechanical
tunneling, the field emission electron sources have received a lot of
attention, particularly as an advanced technology to replace conven­
tional filament-based thermionic electron sources. They offer the ad­
vantages of miniaturization, lowered operating temperature, and an
electron beam (e-beam) with narrow energy distribution [1–4]. These
field-emitted e-beams have been widely investigated for digital X-ray
sources, including industrial inspection equipment, biopsies of various
organs, and real-time medical diagnosis/therapy [5–10]. Carbon nano­
tubes (CNTs) as cold-cathode emitters are a promising material for field
emission device applications, given their high aspect ratios (>103) and
the molecular geometry of the sp2 hybrid orbitals, thereby result in
enhanced local electric field, and chemical/thermal stability [11–14].
Most of field emission digital X-ray sources using CNT emitters have
adopted a triode structure with a gate electrode in order to indepen­
dently control the e-beam current and acceleration voltage [15,16].
Even though the aperture-gate, normally used in field emission devices,
has a higher electron transmission efficiency, it has a critical flaw in that
the e-beam divergence is inevitably occurred due to the distorted po­
tential distribution between the cathode and gate electrodes, resulting in
low-resolution X-ray images.
To circumvent the e-beam divergence in the vicinity of the aperture,
some researchers have suggested a hybrid structure which incorporates
an electron-transparent graphene layer onto the conventional aperture-

Abbreviations: carbon nanotube, CNT; e-beam, electron-beam; layer-by-layer, LBL; electron transparent graphene gate, ETGG; molybdenum, Mo; multi-layer
graphene, MLG; multi-stacked graphene, MSG; 3-dimensional finite element method, 3D-FEM; single-layer graphene, SLG; Poly(methyl methacrylate), PMMA;
ammonium persulfate, APS; atomic force microscopy, AFM; active-current control, ACC; scanning electron microscopy, SEM; Fowler-Nordheim, F-N; FWHM, Full
Width at Half Maximum.
* Corresponding author at: ETRI ICT School (Advanced Devices Engineering), University of Science and Technology, 217 Gajeong-ro, Yuseong-gu, Daejeon 34113,
South Korea.
E-mail address: yhsong@etri.re.kr (Y.-H. Song).

https://doi.org/10.1016/j.apsusc.2022.154524
Received 25 May 2022; Received in revised form 9 August 2022; Accepted 9 August 2022
Available online 11 August 2022
0169-4332/© 2022 Elsevier B.V. All rights reserved.
Y. Ahn et al.
gate, to perform the function of a focusing lens [17,18]. In previous
reports, Li et al. fabricated a hybrid structure with graphene transferred
onto a molybdenum (Mo) grid with 100 µm aperture [17]. This graphene
hybrid gate showed a reduced gate turn-on voltage and improved
transmission efficiency. Nevertheless, a large leakage current was
generated at the gate electrode because the diameter of the suspended
graphene gate aperture was considerably smaller than that of the
emitter. Jeon et al. also demonstrated a multi-layer graphene (MLG)-
gated triode structure to decrease the e-beam divergence [18]. The MLG
had almost 12-layers, and was tightly suspended on the aperture-gate
with a diameter of 350 μm, thereby reducing the gate leakage current.
However, a non-uniform thickness distribution and the presence of
micro-pores on the MLG surface significantly reduced the durability of
the suspended MLG-gate when it is driven for a long time, leading to
deterioration of the field emission property.
In this study, we have demonstrated a robust and scalable electron
transparent graphene gate (ETGG) by a layer-by-layer (LBL) stacking
method. Herein, the robustness and the scalability stand for intrinsic
durability of ETGG upon energetic electron bombardment of several-keV
and large enough so as to afford e-beams for field emission X-ray sour­
ces, respectively. The robust and scalable ETGG applicable to the actual
devices has not been reported yet.
Unlike other previous studies, we investigated an approach to
improve durability of the ETGGs by controlling the number of graphene
layers. By using the LBL stacking method, ultra-thin and scalable multi-
stacked graphene (MSG) with uniform thickness over all area was ob­
tained. The thickness of the MSG was precisely controlled in proportion
to the number of LBL stacking with a single graphene, and the yield of
the ETGGs was explored by the number of free-standing MSGs existing
on the gate consisting of seven apertures with a diameter of 300 μm. The
field electron emission properties of the CNT-based emitters gated with
the ETGGs consisting of tri- (3L), penta- (5L) and septi-layered (7L)
MSGs, were evaluated in a vacuum chamber, and they were compared
with the conventional aperture-gate. After that, the degree of each e-
beam convergence including scattering of the primary e-beams by gra­
phene while passing through the MSG was confirmed by comparing the
e-beam spot sizes projected onto a fluorescent anode. We also identified
the e-beam convergence and the electric field distribution between the
cathode and gate with and without the ETGGs through the computa­
tional simulation using 3-dimensional finite element method (3D-FEM)
with a commercial OPERA-3D simulator. In addition, a beam-halo
Fig. 1. Schematic of the fabrication procedures of multi-stacked graphene (MSG) by the layer-by-layer (LBL) method.
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Applied Surface Science 604 (2022) 154524
originated from the scattered e-beam, which would deteriorate spatial
resolution of an X-ray source, was estimated and eliminated with an
optimized collimation module. A long-term durability test was con­
ducted to examine the degree of deterioration of the MSG used in the
ETGG through a prolonged electron bombardment of about 3 keV, which
secured the requirement for field emission digital X-ray sources. This
work could pave the way for advanced applications as a high-resolution
X-ray source for medical and industrial imaging devices.
2. Results and discussion
Fig. 1 shows the facile LBL-graphene stacking method. Purchased
single-layer graphene (SLG) synthesized on a Cu foil by thermal chem­
ical vapor deposition process was used in the experiments. Poly(methyl
methacrylate) (PMMA) was spin-coated on the SLG/Cu substrate. The
PMMA/SLG layer was achieved by etching the Cu foil in a 3 M ammo­
nium persulfate (APS) solution. The PMMA/SLG layer was transferred
onto the newly prepared SLG/Cu foil. Eventually, the LBL-stacked bi-
layered graphene was obtained on the Cu foil after PMMA was removed
by acetone. We can easily create the MSG layers on the Cu foil by cycling
the above process.
Fig. 2(a)-(d) shows the optical images of the transferred SLG and
MSGs on a SiO2/Si substrate with different colors depending on the
number of layers. It was confirmed that they uniformly covered the
entire SiO2 surface without any damage. The surface morphology and
thickness profiles of the SLG and MSGs_3L, _5L, and _7L were identified
by atomic force microscopy (AFM), as shown in Fig. 2(e)-(h). The
thickness of the stacked graphene was obtained by measuring the height
differences of the graphene edge and the SiO2/Si substrate. Based on the
two height profiles (red and green lines), the thicknesses of the 1-, 3-, 5-,
and 7- layered graphene are about 0.73, 1.43, 2.15, and 2.95 nm,
respectively. Although the theoretical thickness of the SLG is 0.35 nm,
the AFM measurement slightly increased due to the variation in the
attractive force between the AFM-tip and graphene, depending on the
substrate type [19,20].
tmeasured − t0
NGL = (1)
t*
where, NGL is the number of stacked graphene layers, tmeasured is the
measured thickness of the graphene via AFM, t0 is an instrumental offset,
and t* is the theoretical thickness of the single layer graphene.
Y. Ahn et al. Applied Surface Science 604 (2022) 154524

Fig. 2. (a)-(d) Optical microscope images and (e)-(h) AFM images with layer thickness profiles for (a), (e) single-layer graphene (SLG) and (b), (f) tri- (3L), (c), (g)
penta- (5L) and (d), (h) septi-layered (7L) MSGs transferred onto the SiO2/Si substrates, respectively. (i)-(j) UV–Visible and Raman spectra for SLG and MSGs with 2-,
3-, 4-, 5- and 7 layers on the glass substrates and the SiO2/Si substrates, respectively. The inset in (i) shows the optical microscope images of SLG and MSGs with 3-, 5-
, and 7 layers on glass substrates in a macro-scale.

Consequently, the number of graphene stacks calculated in the above
equation was estimated to be approximately 1-, 3-, 5-, and 7-layers,
which corresponds to the stacked graphene layers in our experiment.
In addition, stacked graphene layers fabricated by the LBL stacking
method has uniform thickness over all area.
The optical transmittance of the MSG layers transferred onto the
glass substrate was measured by UV–Vis spectroscopy (Fig. 2(i)). Ac­
cording to Nair et al., the transmittance theoretically decreases by 2.3%
as the number of graphene layers increases in the visible region [21].
Therefore, the transmittance (T) as a function of the number of the
stacked graphene layers can be expressed as follows [22,23].
T (%) = (1 − πα)N × 100
where, πα is the absorption (~2.3% for the SLG) and N is the number of
stacked graphene layers. The optical transmittance of our graphene
stacks from 1 to 7 layers, measured at λ = 550 nm, were 97.5, 95.1, 92.8,
90.1, 87.5 and 83.5%, respectively. Raman spectroscopy is a non-
destructive analysis method which can provide the chemical structure
and thickness information of graphene. Fig. 2(j) shows the Raman
spectra of graphene transferred onto the SiO2/Si substrates with
different numbers of the stacked layers. Two predominant peaks, a G-
band peak related to the in-plane phonon mode and a 2D-band peak
related to the two phonon double resonance Raman processes, were
observed at around 1580 and 2680 cm− 1, respectively, in the SLG [24].
As the number of stacked graphene layers increases, the peak position of
the 2D-band gradually shifts toward a higher frequency [25]. In addi­
tion, the intensity ratios of the 2D-band over G-band (I2D/IG) of the
stacked graphene layers decreased from 2 to 0.37 as the number of
(2) stacked graphene layers increased, which corresponds to the AFM and
optical transmittance results [26].
Fig. 3(a) shows the fabrication process of the ETGG. Firstly, the
PMMA-coated MSG was transferred to a Mo gate sheet with seven

3
Y. Ahn et al.
Fig. 3. (a) Schematic of transferring the MSG onto Mo apertures with a vacuum annealing process for removing the PMMA. (b) Optical images (top and bottom) of
the PMMA-coated MSG on the aperture sheet. (c) Optical images of the bare aperture-gate and apertures with MSGs_3L, _5L, _7L, respectively. (d) Fabrication yield of
ETGG evaluated from ten Mo gate sheets that have seven apertures for each as a function of the number of the stacked layers.
apertures. Next, PMMA is removed by a vacuum annealing process at
400 ◦ C after drying. Eventually, we can obtain an MSG that is stably
placed onto the aperture-gate with a diameter of 300 µm. Fig. 3(b)
displays the optical images of the ETGG and the PMMA-coated MSG.
Fig. 3(c) shows the aperture-gate and the ETGGs. Compared to the
aperture-gate, the ETGG can be distinguished by the difference of the
light transmittance of microscope. The graph in Fig. 3(d) shows the yield
(%) of the MSG perfectly suspended on the gate sheet as a function of the
stacked layers. The error bars denoted in this graph were evaluated from
ten Mo gate sheets that have seven apertures for each. This result indi­
cated that the MSG with 5 layers or more could be perfectly suspended
on all apertures of the gate even with a large diameter of 300 µm. This
high fabrication yield of ETGG presumably comes from the relieved
stress–strain of the uniform and very thin MSG fabricated by the LBL
transfer method.
The field emission characteristics of a single-dot CNT paste emitter
with and without the ETGG were investigated using an active-current
control (ACC) unit in a pulse operation mode [27] with the LabVIEW
in-house program, as shown in the circuit diagram of the triode structure
of Fig. 4(a). The single-dot CNT paste emitter was subjected to an aging
process [28] prior to investigation of the field emission characteristics
for the aperture-gate and the ETGG with the number of stacked gra­
phene. As shown in the left scanning electron microscopy (SEM) image
of Fig. 4(a), CNTs are still densely arranged in the vertical direction even
after the prolonged field emission. Fig. 4(b) shows the optical image of a
cathode-gate module where each part is electrically insulated by
ceramic plates, and the gap distance between the gate and cathode is
300 µm. By adjusting the four screws attached to the gate jig, it is
possible to accurately and easily align the 200-µm-diameter-CNT paste
emitter to the center of the aperture-gate of 300 µm in diameter, as
illustrated in the inset in Fig. 4(b). Fig. 4(c) shows the cathode current-
gate voltage (Ic-Vg) characteristics of a single-dot CNT paste emitter in
the triode structures with the aperture-gate and the MSG_3L-, _5L-, and
_7L-ETGGs along with the diode structure where the anode was placed at
the gate position (Vg means the anode voltage in the diode). For the
triode structure, the Ic-Vg was achieved under a constant anode voltage
of 5 kV. From the Ic-Vg curves, the turn-on voltage of the CNT paste
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Applied Surface Science 604 (2022) 154524
emitter in the aperture-gate triode structure increased by 380 V
compared to that in the diode structure, due to diverted and weaken
electric field strength around the aperture of the gate. Interestingly,
when the aperture-gate was covered with an electron-transparent gra­
phene, the planar electric field expanded near the aperture like in the
diode structure, and as a result, the turn-on gate voltage was signifi­
cantly reduced from 1,440 to 1,100 V compared to the conventional
aperture-gate. Furthermore, the reduction in the turn-on gate voltage in
the ETGG was almost constant regardless of the number of stacked
graphene layers.
The Fowler-Nordheim (F-N) plots of Ic-Vg, as shown in the inset in
Fig. 4(c), provided crucial parameters associated with the field emission
characteristics of the CNT paste emitters. The F-N equation can be
described as follows [29]:
( )
− BΦ3/2
E
J = AΦ− 1 E2 PF e (3)
where J is the emission current density, E is the applied electric field, A
and B are the constant values corresponding to 1.54 × 10− 6 (AV− 2eV)
and 6.83 × 109 (eV− 3/2Vm− 1) respectively, PF is 1, which is used as the
tunneling prefactor [30], and Ф is a work-function of CNT (5.0 eV). In
V
equation (3), E and J can be generally substituted by β dg and Iαc ,
respectively, where β is a field enhancement factor, d is a distance be­
tween the gate (or anode) and cathode in a triode (or diode) structure,
and α denotes an effective emission area coming from the number of
emission sites. Here, β can be expressed as follows:
(4)
3
β = BΦ2 d/S
where S is the slope of the F-N plot. Based on the equation, β of the
single-dot CNT paste emitter was 2,104 for the diode configuration and
were 2,016, 2,018, and 2,076 for the triode structures with 3L-, 5L-, and
7L-ETGGs, respectively. Meanwhile, β was 1,386 for the conventional
aperture-gate triode. The fact that the ETGG triode has nearly the same β
with the diode structure, much higher value than the conventional
aperture-gate triode, is attributed to planar electric fields in the vicinity
Y. Ahn et al.
Fig. 4. (a) Schematic of the field emission measurement setup with an active-current control (ACC) unit used previously [27], together with a SEM image of the CNT
paste emitter after the electron emission measurement. (b) Optical image of the cathode-gate module with a single-dot CNT paste emitter aligned to the center of the
ETGG. (c) Cathode current-gate voltage (Ic-Vg) characteristics for the aperture-gate and MSG_3L-, _5L-, and _7L-ETGGs along with the diode structure where the anode
was placed at the gate position (Vg means the anode voltage in the diode). The inset graph exhibits the F-N plot of each Ic-Vg. (d) Gate leakage currents as a function of
Ic for the aperture-gate and 3L-, 5L-, and 7L-ETGGs.
of the aperture covered by graphene. The computational simulation
confirmed that the ETGG forms the planar electric fields near the
aperture and increases the local electric fields at the tips of the CNT
emitters, and so emits more electrons, like the diode structure (Fig. S1)
[31,32]. It is noted that α for the all samples was calculated to be around
5 × 10− 12 cm2. Fig. 4(d) shows the gate leakage currents (Ig) as a func­
tion of Ic for the CNT paste emitters with the aperture-gate, and 3L-, 5L-,
and 7L-ETGGs, respectively, in the triode structures. Ig of all the samples
increased with an increase in Ic. Notably, among these samples, the
highest Ig appeared in the 7L-ETGG. These results are clearly consistent
with the fluorescent brightness of the anode bombarded with the e-
beams from the CNT paste emitters. Here, the electron transmission
efficiency (ηt) can be calculated using the following equation:
Ia Ia
ηt = = (5)
Ia + Ig Ic
where Ia is the anode current. ηt of the CNT paste emitter with the
aperture-gate, and 3L-, 5L-, and 7L-ETGGs were 97.2, 95.5, 94.1, and
92.0%, respectively, at an Ic of 100μA. The increase in Ig, in other words,
the decrease in ηt with the number of graphene layers would be caused
by scattering of the e-beam at the MSG of ETGG. Thicker MSGs resulted
in larger Ig and smaller ηt. Nevertheless, it should be noted that ηt of our
ETGG-CNT paste emitters was over 90%, remarkably larger than the
previously reported values [17].
The electric fields and e-beam trajectories were calculated using the
commercial OPERA-3D simulator based on 3D-FEM, as shown in Fig. 5
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Applied Surface Science 604 (2022) 154524
(a). In the conventional aperture-gate triode, the e-beam divergence
inevitably occurs due to the convex potential distribution around the
aperture. Meanwhile, the MSG of ETGGs flattens the potential contours
even near the aperture, like the diode structure, resulting in the strongly
converged e-beam trajectory of 89◦ of the e-beam angle measured from
the gate in-plane, compared with 82◦ for the aperture-gate triode. To
verify the e-beam convergence effect of the ETGGs together with the
influence of the number of the stacked graphene layers in the ETGGs,
field electron emission of the single-dot CNT paste emitter of 200 µm in
diameter was measured using the fluorescent anode. Fig. 5(b) shows the
fluorescent images of the e-beams projected onto the anode for the
triode structures with the aperture-gate, and 3L-, 5L-, and 7L-ETGGs.
The projected images of the e-beam spots were obtained at an Ic of 10
µA while applying a constant anode voltage of 5 kV. It was observed that
the primary e-beams from the single-dot CNT paste emitter are pre­
dominantly converged or focused by the ETGGs, by 77%, compared with
the aperture-gate if neglecting the halo region appeared around the
primary e-beam spots. The beam-halo region became wider and brighter
as the number of the stacked graphene layers in the ETGGs, probably
resulting from scattering of the primary e-beams by graphene while
passing through the MSG. Secondary electrons could be hardly gener­
ated during the passing of the primary e-beam through graphene [33].
Since the scattered electrons in the beam-halo region deteriorate
spatial resolution (called focal spot size, determined by the landed area
of the e-beam onto the anode target) of an X-ray source when they are
accelerated and impinged onto the anode target, we quantitatively
Y. Ahn et al. Applied Surface Science 604 (2022) 154524

Fig. 5. (a) Computational simulations of the e-beam trajectories for a diode structure and triode structures with an aperture-gate and an ETGG. (b) Fluorescent
images of the e-beams projected onto the anode in the triode structures with the aperture-gate and 3L-, 5L-, and 7L-ETGGs at an Ic of 10 μA. (c) Simulated mapping
images of the e-beams projected onto the anode in the triode structures with the aperture-gate and 3L-, 5L-, and 7L-ETGGs in sequence. (d) Schematic of the
(enlarged) ETGG triode structure with a collimator module that would block the scattered electrons. (e) Fluorescent images of the e-beams projected onto the anode
in the 7L-ETGG triode structure with and without the collimator at an Ic of 30 μA. The collimator has a single aperture of 550 μm in diameter and 4 mm in height.

analyzed and then removed them using an optimized collimator. As
shown in Fig. 5(c), the relative e-beam concentration on the fluorescent
anode could be quantified through the pixel intensity in the contour
mapping images, indicating that a broad, irregular intensity distribution
of the e-beam spot in the aperture-gate changes into narrow, uniform
distributions in the ETGGs while the area of the beam-halo is slightly
broadened as the number of stacked graphene increases. The dark points
in the images are patterns on the fluorescent anode for indicating the
scales of the e-beam spots. For the more quantitative calculation of the
beam-halo around the primary e-beam, the horizontal pixel intensity
profiles of each e-beam spot were obtained, as shown in Fig. S2. The raw
pixel intensity profile was deconvoluted into the primary and scattered
e-beam sub-profiles of Gaussian distributions [34]. The relative intensity
proportions occupied by the beam-halo around the primary e-beam, the
yellow-shaded regions under the profiles in Fig. S2, were approximately
calculated to be 9.6 %, 11.7 %, and 17.4 % in the total e-beam intensities
for the 3L-, 5L-, and 7L-ETGGs, respectively. The degree of the beam-
halo was increased as the number of the stacked graphene layers,
showing the broader and higher scattering of the primary e-beam at the
thicker graphene layers. It is, however, noted that the same FWHM (Full
Width at Half Maximum) of 90 of the primary sub-profiles for the 3L-,
5L-, and 7L-ETGGs means effective converging of the primary e-beams
regardless of the number of graphene layers. Here, the scattered e-beam
may vary depending on the atomistic parameters, like twisted angle, of
graphene layers in the LBL stacking procedure, but its impact would be
minimal because the energy of the transmitted electron is as high as
several-keV.
In order to eliminate the beam-halo region of the scattered electrons

6
Y. Ahn et al. Applied Surface Science 604 (2022) 154524

in the ETGGs, a collimator functioning as a field stop would be used, as

shown in Fig. 5(d). The collimator was designed by considering the e-
beam divergence from the CNT paste emitter to the anode by the e-beam
trajectory simulation. In this study, we take account into only the
divergence of the primary e-beam from the CNT paste emitter because
the MSG of ETGGs keeps the potential contours flatten in the vicinity of
the aperture. When the height of the cylindrical collimator, Hcoll, is fixed
to 4 mm, the diameter of the collimator can be calculated by the
following equation.
Hcoll + Tg + Gc−
(6)
g
Dcoll = Demit + 2
tanα

where Demit is the diameter of the CNT paste emitter, Tg is the gate
thickness, Gc-g is the cathode-gate distance, and tan α is the divergence
angle of the primary e-beam, as shown in Fig. S3. Here, tan α can be
expressed as follows.
Gc− a
tanα = (7)
(Dbeam 2− Demit )

where Gc-a is the cathode–anode distance, Dbeam is the diameter of the

primary e-beam at the anode. From the simulated Dbeam under the given
geometric parameters of Demit, Gc-a, etc., Dcoll of the collimator was
predicted to be 550 µm for the Hcoll of 4 mm, based on the equations (6)
and (7). Fig. 5(e) shows the e-beam spots projected onto the fluorescent
anode in the 7L-ETGG triode with and without the optimized collimator.
Both e-beam spots were observed at an Ic of 30 µA, and Ig of 5 µA and 2
µA with and without the collimator, respectively. By implementing the
collimator onto the gate electrode, we could acquire the distinct primary
e-beam with little beam-halo region, successfully eliminating the scat­
tered electrons. As a result, the ETGGs with the optimized collimator can
provide strongly converged or focused e-beams even from the dispersed
CNT paste emitters.
Durability of MSG in ETGGs is very crucial for their application to
field emission digital X-ray sources. A prolonged electron emission and
then bombardment onto the MSG of ETGGs would damage the graphene
layers, probably resulting in instability or unreliability in field emission
and finally fatal electrical arcs on the MSG and/or CNT emitters. We
verified the durability of MSG in ETGGs by measuring prolonged field
emission from the CNT paste emitters in a high vacuum. Fig. 6(a) shows
the cathode current and its density as the number of operation shots for Fig. 6. (a) Cathode current (with its density) versus number of pulse shots for
the single-dot CNT paste emitter gated with the 7L-ETGG in a vacuum the 7L-ETGG triode structure with a single-dot CNT paste emitter of 200 μm in
chamber under about 10− 8 torr. The measurement was carried out by diameter. (b) SEM and optical images, (c) Raman spectra of the 7L-ETGG before
using the ACC unit in the pulse mode of a 100 µs pulse-width and a 1 s and after the long-term electron emission measurement, respectively.
period under a constant anode voltage of 5 kV [27]. The diameter of the
single-dot CNT paste emitter was 200 µm, the distance between the defects was almost the same. As a result, the chemical bonding state and
cathode and gate electrodes was 300 µm, and a tungsten anode with a composition of the MSG_7L-ETGG were not changed, ensuring that the
thickness of 5 mm was used. As shown in Fig. 6(a), the field emission 7L-ETGG has an atomistic durability upon the prolonged electron
cathode current was very stable over 140,000 operation shots with a bombardment of about 3 keV at a transmission current density of 1.4
standard deviation of 0.7 at a current of around 100 µA. Moreover, the mA/mm2, which secured the requirement for field emission digital X-ray
cathode current was consistently maintained without any arcing until sources.
the long-term stability measurement was completed. The MSG in 7L-
ETGG was checked through the SEM and optical images before and
3. Conclusion
after the long-term stability measurement, as shown in Fig. 6(b). Even
after continuously driving 140,000 pulses of electron collision under a
In summary, we demonstrated an optimized ETGG for field emission
high energy of 2.7 keV, the MSG layer was observed to still remain on
electron sources. A robust and scalable MSG with uniform thickness was
the aperture-gate without any tears or micro-pores. While the 7L-ETGG
attained by accurately controlling the thickness using a facile LBL-
exhibited the stable field emission, the 5L-ETGG showed unexpected
stacking process. The MSGs with 5 layers or more were perfectly sus­
large fluctuations in the cathode current with couples of small electrical
pended on Mo apertures with scalable diameters of 300 μm. The field
arcs. We observed several micro-pores near the edge of the MSG_5L-
electron emission properties of CNT paste emitter gated with the ETGGs
ETGG after the long-term durability test by the SEM image shown in
and the conventional aperture-gate were evaluated in a vacuum cham­
Fig. S4.
ber at a pressure below 10− 6 torr. Since the ETGG flattens the potential
Fig. 6(c) shows the Raman spectra of the MSG_7L-ETGG before and
contours near the aperture and enhances the local electric fields at the
after the long-term stability test. The peak positions of both G- and 2D-
tips of the CNT emitters, the turn-on gate voltage of CNT paste emitter
bands, related to graphene components, had not changed even upon the
gated with ETGGs is significantly reduced by approximately 24%
long-term stability test. Also, the peak intensity of the D-band related to
compared to the conventional aperture-gate. Thereafter, the e-beam

7
Y. Ahn et al.
spot size projected onto a fluorescent anode was measured to verify the
e-beam convergence effect of the ETGGs. As a result, the ETGG exhibited
an improved convergence of 77% compared to the conventional
aperture-gate. In addition, the beam-halo around the primary e-beam
occurred by the scattered electrons while passing through the ETGG was
qualitatively estimated and perfectly eliminated by using the optimized
collimation module. Lastly, the 7L-ETGG showed good durability upon
the prolonged high-energy electron collision over 140,000 times
without any deterioration of the MSG. The single aperture 7L- ETGG of a
current level of 100 μA has potential to be directly applied to the bi­
opsies of various organs, and a current level of over several-mA can be
easily attained with multiple ETGGs in the form of an array for emitters/
gates and then be applied to a high-performance X-ray source for med­
ical and industrial imaging devices.
4. Experimental section
A CNT paste emitter was configured as a triode structure using the
ETGG with MSG and conventional aperture-gate. The CNT paste
composed of multi-walled CNTs with an average length of 10 μm (Xin­
Nano Materials, Inc), nano-sized silicon carbide (SiC), nickel (Ni) as
inorganic fillers, ethyl cellulose as organic binders, and terpineol as
solvents was formulated by using a ball-milling process. The formulated
CNT paste was screen-printed on a Kovar cathode substrate. To remove
the solvents and organic binders, the screen-printed CNT paste emitter
was dried at 90 ◦ C for 10 min and sintered in air at 300 ◦ C for 3 h. And
then, a vacuum annealing process at a higher temperature of about
800 ◦ C under a pressure of ~ 10− 7 torr was conducted to promote
chemical reactions between the inorganic fillers and the cathode sub­
strate, and so to enhance adhesion of the CNT paste emitter. Lastly, the
CNT paste emitter was completed by arranging CNTs in a vertical di­
rection by performing the surface treatment process using an adhesive
roller after the sintering and vacuum annealing processes, respectively
[35,36].
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgments
Yujung Ahn and Seong Jun Kim contributed equally to this work.
This work was partly supported by Institute of Information & Commu­
nications Technology Planning & Evaluation (IITP) grant funded by the
Korea government (MSIT) (No.2020-0-00009, Development of digital
microfocus X-ray tubes and their high-productivity in-line inspection
equipment for ultra-integrated ICT products), Industry & Energy
(MOTIE, Korea) under Industrial Technology Innovation Program
(No.20000935).
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.apsusc.2022.154524.
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