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21st Century Nanoscience – A Handbook: Design Strategies for Synthesis and Fabrication (Volume Two)
21st Century Nanoscience – A Handbook: Advanced Analytic Methods and Instrumentation (Volume Three)
21st Century Nanoscience – A Handbook: Low-Dimensional Materials and Morphologies (Volume Four)
21st Century Nanoscience – A Handbook: Exotic Nanostructures and Quantum Systems (Volume Five)
21st Century Nanoscience – A Handbook: Nanophotonics, Nanoelectronics, and Nanoplasmonics (Volume Six)
21st Century Nanoscience – A Handbook: Bioinspired Systems and Methods (Volume Seven)
21st Century Nanoscience – A Handbook: Nanopharmaceuticals, Nanomedicine, and Food Nanoscience (Volume Eight)
21st Century Nanoscience – A Handbook: Public Policy, Education, and Global Trends (Volume Ten)
21st Century Nanoscience – A Handbook
Nanophotonics, Nanoelectronics, and Nanoplasmonics (Volume Six)
Edited by
Klaus D. Sattler
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Editor . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . vii
Contributors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ix
1 Nanophotonic Devices Based on Low-Voltage Emission of 2D Electron Gas
Hong Koo Kim, Myungji Kim, Daud Emon, Siyang Liu, Yu Shi, and Haiming Guo . . . . . . 1-1
2 Polarized Nano-Optics Sophie Brasselet . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2-1
3 Optical Properties of Semiconductor Nanostructures Andres Cantarero . . . . . . . . . . . . . 3-1
4 Hybrid Phase-Change Nanophotonic Circuits Johannes Feldmann and Wolfram Pernice . . 4-1
5 X-Ray Nanophotonics Based on Planar X-Ray Waveguide-Resonator V. K. Egorov
and E. V. Egorov . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5-1
6 Optical Tweezers Jing Liu and Zhi-Yuan Li . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6-1
7 Metal Nanostructures with Plasmonically Enhanced Raman and Photoluminescence
Signals Jeong-Eun Park, Minho Kim, Jiwoong Son, Chungyeon Lee, Sung Min Ko,
and Jwa-Min Nam . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7-1
8 GaN Nanoflowers: Growth to Optoelectronic Device Neha Aggarwal,
Shibin Krishna, and Govind Gupta . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8-1
9 The Future of Nanoelectronics Simon Deleonibus . . . . . . . . . . . . . . . . . . . . . . . . . . . 9-1
10 Semimetal Electronics: Quantum Confinement and Surface Chemistry as Design Tools
Alfonso Sanchez-Soares, Christian König, Conor O’Donnell, Jean-Pierre Colinge, and
James C. Greer . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10-1
11 Neuromorphic Nanoelectronics Jessamyn A. Fairfield . . . . . . . . . . . . . . . . . . . . . . . . . 11-1
12 Single Electronics: Modeling and Simulation Techniques B. S. Pês, E. Oroski,
and J. G. Guimarães . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12-1
13 Single Electron Transport and Possible Quantum Computing in 2D Materials
K. L. Chiu . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13-1
14 Assembly of Plasmonic Nanoparticles Eric H. Hill, Christoph Hanske, Cyrille Hamon,
and Yuebing Zheng . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14-1
15 Coulomb Blockade Plasmonic Switch Ali Khademi, Dao Xiang, and Reuven Gordon . . . . 15-1
16 Amplification of Surface Plasmons Gerard Tatel and M. S. Wartak . . . . . . . . . . . . . . . . 16-1
17 Magneto-plasmonics in Purely Ferromagnetic Subwavelength Arrays S. D. Pappas and
E. Th. Papaioannou . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17-1
18 Cathodoluminescence of Nanoplasmonics Naoki Yamamoto and Takumi Sannomiya . . . . . 18-1
19 Biosensing under Surface Plasmon Resonance Conditions Boris Snopok . . . . . . . . . . . . . 19-1
20 Plasmonic Optical Antenna and Its Enhancement to Infrared Photodetectors
Lin Li, Neda Mojaverian, Guiru Gu, and Xuejun Lu . . . . . . . . . . . . . . . . . . . . . . . . . . 20-1
Index . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . I-1
Editor
Klaus D. Sattler pursued his undergraduate and master’s carbon nanocones. His current work focuses on novel nano-
courses at the University of Karlsruhe in Germany. He materials and solar photocatalysis with nanoparticles for the
earned his PhD under the guidance of Professors G. Busch purification of water. He is the editor of the sister refer-
and H.C. Siegmann at the Swiss Federal Institute of Tech- ences, Carbon Nanomaterials Sourcebook (2016) and Silicon
nology (ETH) in Zurich. For three years he was a Heisenberg Nanomaterials Sourcebook (2017), as well as Fundamen-
fellow at the University of California, Berkeley, where he tals of Picoscience (2014). Among his many other accom-
initiated the first studies with a scanning tunneling micro- plishments, Dr. Sattler was awarded the prestigious Walter
scope of atomic clusters on surfaces. Dr. Sattler accepted a Schottky Prize from the German Physical Society in 1983.
position as professor of physics at the University of Hawaii, At the University of Hawaii, he teaches courses in general
Honolulu, in 1988. In 1994, his group produced the first physics, solid-state physics, and quantum mechanics.
Contributors
1-1
1-2 Nanophotonics, Nanoelectronics, and Nanoplasmonics
FIGURE 1.1 2DEG formed in semiconductor FET devices. (a) MOS. (b) High-electron-mobility transistor (HEMT).
heterostructure had been further developed into HEMTs: low-voltage emission of 2DEG and a subsequent, ultrafast
in this device concept, the 2DEG confined to a poten- energy-efficient transport of electrons in a nanoscale vacuum
tial well exhibits greater mobility than those in MOSFET, (void) channel formed in SiO2 /Si substrate. We recently
since the former device utilizes an undoped channel thereby reported low-voltage (<3 V) operation of a vacuum FET
mitigating the deleterious effect of ionized impurity scat- (Srisonphan 2012): a 2DEG is extracted out at low bias
tering (Sze 1990). The HEMT devices based on III–V (∼1 V) and is injected into a nanovoid channel that is verti-
compound materials (such as GaN or InP) are employed cally etched into a MOS structure. Coulombic repulsion of
for high-speed electronic circuits operating at RF/microwave electrons at channel edge is found to reduce the energy
frequencies. barrier for electron emission, leading to a high-current-
A different class of heterostructures that can host 2DEGs density emission at low bias. In this chapter, we review
are oxides, e.g., ZnO/ZnMgO and LaAlO3 /SrTiO3 (Kozuka two device applications that utilize this low-voltage emission
et al. 2011, Ohtomo & Hwang 2004). The interface between phenomenon of 2DEG for Si-based nanophotonic devices.
LaAlO3 and SrTiO3 exhibits interesting properties that
cannot be found in its constituent materials. Individu-
ally, LaAlO3 and SrTiO3 are nonmagnetic insulators, yet 1.2 Theory: Low-Voltage Emission
their interfaces can exhibit electrical conductivity and large of 2DEG
magnetoresistance (Brinkman et al. 2007). In particular, it
is notable that the LaAlO3 /SrTiO3 interface can accommo- A MOS with 10–20 nm oxide thickness can easily harbor
date a very high level of 2DEG concentration, surpassing high-concentration (1012 –1013 cm−2 ) electron (or hole) gas
1014 cm−2 level. at relatively low bias (<5 V). Consider a MOS structure
Recently, atomically thin solid materials have been devel- with a lateral extent that is finite, for example, terminated
oped, such as graphene and transition metal dichalcogenide by cleaved edges or by vertically etched surface (Figure 1.2).
(TMDC), where electrons are confined to atomic layer thick- The electric field near the edge is determined by an inte-
ness (Novoselov et al. 2005, Zhang et al. 2005, Wang et al. gral of Coulombic interactions with 2DEG. Considering the
2012). The 2DES in graphene can be tuned to either 2DEG small thickness (∼2 nm) of 2DEG, a strong shape-effect is
or 2DHG by applying transverse electric field (i.e., gating) expected in the in-plane direction near the edge: see the
or by performing chemical doping. Aside from being in a field and potential distributions plotted as a function of
variety of practical device applications, 2D systems allow distance from the edge. The horizontal field sharply rises for
many novel physical phenomena such as quantum Hall effect nearer to the edge with surface field exceeding the critical
in 2DEG (von Klitzing 1980) and Hofstadter’s butterfly, a level (∼1 GV/m). From the potential distribution, it is also
fractal structure in the energy versus magnetic field plot evident that the strong surface field near the edge has the
(Dean et al. 2013). effect of reducing energy barrier width. For example, 1013
While the in-plane transport of 2DES along inter- cm−2 2DEG concentration induces ∼1 GV/m surface field,
face is the standard configuration commonly adopted in which results in a narrow potential barrier (2-nm barrier
device applications, we have explored alternative channel width at 2-eV barrier height) enabling 2DEG emission into
media/configurations in a MOS structure by involving air at much reduced bias.
Nanophotonic Devices 1-3
FIGURE 1.2 Low-voltage emission of 2DEG. (a) Schematic of a MOS structure with a cleaved edge. (b) Field distribution near the
edge, plotted as a function of distance from the surface. (c) Potential distribution showing a significant reduction of energy barrier (height
and width).
In graphene-based electronics/photonics research, The space charge density (Q s ) in the semiconductor side
a graphene-oxide-semiconductor (GOS) structure is can be determined by solving the Poisson equation, and is
commonly used in exploring device phenomena (Novoselov expressed as follows (Sze 1981).
et al. 2012, Koppens et al. 2014, Kim & Kim 2015). Similar
to the case of a MOS capacitor, a GOS structure can √
2εs −βϕs
harbor two different types (inversion or accumulation) of Qs = −εs Es = − e + βϕs − 1
βLD
2D electron system at the oxide/Si interface, depending 12
on the polarity of gate bias applied across the oxide layer. np0 βϕs
+ e − βϕs − 1 for p-Si (1.4)
A switching control of this 2DES by oxide field is an ppo
essential function of GOS-based field-effect devices. Below
we calculate the 2DEG density in a GOS structure under where εs is the permittivity of semiconductor and E s is the
inversion bias. electric field at the interface with the oxide layer. ϕs is the
band bending at the semiconductor/oxide interface called
1.2.1 Analysis of a Graphene/SiO2 /Si the surface potential. β = q/kT, and LDqis the extrinsic
εs
(GOS) Capacitor Structure under Debye length for holes, given as LD = qppo β . n po and
Dark, Inversion Bias ppo are the equilibrium densities of electrons and holes,
respectively.
The bias voltage (V ) applied to the graphene/SiO2 /Si struc-
The voltage drop across the oxide layer (V ox ) is related
ture drops across mainly three places: the flat band voltage
to the space charge in Si (Q s ) and oxide capacitance
(V F B ), across the band bending region in semiconductor
(C ox = εox /d) as follows.
(ϕs ), and across the oxide layer (V ox ).
FIGURE 1.3 Analysis of a GOS capacitor structure under reverse bias. (a) Graphene work function (ϕg ). (b) Surface potential (ϕs ).
(c) Depletion width (W ). (d) Space charge density in Si (Q s ). Calculated as a function of reverse bias voltage (V ) applied to a p-Si
GOS in darkness.
1.3.1 Emission of 2DEG in MOS DuBridge 1932). For the thickness of SiO2 layer (23 nm)
employed in this work, the tunneling through the oxide
In extracting photocarriers out of Si, we exploit the
barrier is expected to remain completely negligible. The
phenomenon that a 2DEG induced at SiO2 /Si of a MOS
leakage current through the oxide layer is measured to be
structure can easily emit into air (void channel) at low bias
of ∼10 pA order as tested prior to cleaving (Figure 1.4b,
voltage (<5 V) (Srisonphan et al. 2012, 2014). A MOS
bottom, dashed). This oxide leakage is several orders of
wafer of Al/SiO2 (23 nm)/n-Si structure was cleaved into
magnitude smaller than the channel current observed with a
two pieces: the cleaved facet provides a vertical transport
cleaved MOS (∼100 µA at 1 V), and this confirms negligible
channel on the air side, which connects the 2DEG layer
contribution by tunneling through oxide.
at SiO2 /Si and the Al electrode on top (Figure 1.4a). Note
The situation can be very different for the electrons
that the channel length of the vertical transport in air is
confined in a 2DEG layer. First, let’s imagine an infi-
determined by the oxide layer thickness (23 nm) of MOS
nite extension of 2DEG at SiO2 /Si, that is, the case prior
and is designed to be smaller than the mean-free path of
to cleaving of MOS wafer. The overall charge neutrality
electrons in air (∼60 nm). This is to ensure that emitted
condition is maintained between the 2DEG in Si and the
electrons travel scattering free in the ambient (air) channel,
positive charges induced in the metal side (Ando et al.
as if in a vacuum.
1982, Mead 1961). Along the in-plane direction of 2DEG,
The current-versus-voltage (I –V ) measurement of the
Coulombic repulsion among electrons is canceled out due to
cleaved MOS clearly demonstrates a rectifying character-
the symmetry of electron distribution. Now consider a MOS
istic. Under forward accumulation bias, the MOS current
structure whose lateral extent is finite, i.e., the 2DEG layer
reveals V 3/2 -voltage dependence, indicative of Child–
is terminated by a cleaved edge or a vertically etched trench
Langmuir’s space-charge-limited current in scattering-free
structure. Electrons at the channel edge will then experi-
vacuum environment (Child 1911, Langmuir 1913). The
ence net repulsive force from neighboring electrons inside the
rise of current at relatively low voltage (<∼1 V) indicates
2DEG layer. In the case that the charge neutrality is main-
a significant reduction of energy barrier at the 2DEG/air
tained by relatively remote charges (e.g., opposite polarity
interface. Besides the relatively high electric field (that is,
charges induced across the oxide layer of MOS capacitor),
∼1 V/23 nm = 4 × 105 V/cm) applied to this MOS capac-
strong in-plane Coulombic repulsion is expected to be domi-
itor, the Coulombic repulsion among electrons in 2DEG
nant in the local area around the edge of 2DEG, and
lowers the energy barrier at the cleaved edge as discussed
this can significantly alter the electrostatic potential there
above. Below we demonstrate this barrier lowering effect
as discussed above (Figure 1.2) (Han & Ihm 2000, Zheng
in both MOS and GOS structures and elucidate underlying
et al. 2004, Mayer 2005). For the case of the MOS capac-
mechanisms.
itor structure being discussed here, for example, a 2DEG
Electrons residing inside the bulk Si of a MOS structure
density of ∼1012 cm−2 is obtainable at ∼1 V accumulation
are confined by energy barriers at the surface (with air) and
bias (Srisonphan et al. 2012). The average spacing between
at the interface (with SiO2 ), typically with a vacuum barrier
electrons in the 2DEG is then estimated to be ∼10 nm,
greater than the SiO2 barrier. Electrons, therefore, cannot
smaller than the oxide thickness (23 nm). This will ensure
be easily emitted into air, unless the energy barrier is signifi-
that the in-plane interaction of 2DEG electrons becomes
cantly lowered for thermionic or field emission (Langmuir &
stronger than the dipole charge interaction across the oxide
Kingdon 1923, Fowler & Nordheim 1928, Lau et al. 1994,
layer.
Han et al. 2012) or for photoelectric emission (Fowler 1931,
FIGURE 1.4 Emission and transport of 2DEG at a MOS capacitor with a cleaved facet. (a) A schematic drawing (left) and an optical
micrograph (right: top view of Al electrode; scale bar, 200 µm) of device structure (Al/SiO2 (23 nm)/n-Si). Coulombic repulsion among
electrons in 2DEG at SiO2 /Si reduces the energy barrier at 2DEG/air. (b) Measured I –V characteristic. The cleaved sample clearly
demonstrates a rectifying characteristic (forward slope of 1.5 and reverse slope of 0.5–1.0). The oxide leakage current (measured before
cleaving) remains at 10 pA level (bottom, dashed). (Reprinted from Kim, M. & Kim, H. K., J. Appl. Phys. 118, 104504, 2015.)
1-6 Nanophotonics, Nanoelectronics, and Nanoplasmonics
Similarly the energy barrier in the metal side (metal/air 1.3.2 Photocurrent Response of GOS with
interface) is lowered by the 2D positive charges induced a Void Channel
at metal/SiO2 interface, and the applied capacitor voltage
Now consider a graphene/SiO2 /p-Si (GOS) capacitor struc-
appears mostly across the air gap (i.e., the vertical
ture with a void channel (Figure 1.5). Under illumination
void channel, whose length is defined by the SiO2 layer
at reverse bias, electron–hole pairs are generated in Si and
thickness).
separated by depletion field. The photogenerated minority
The voltage dependence of 2DEG emission is governed
carriers (electrons) drift to the Si/SiO2 interface and become
by the capacitor relationship, Q e ∼ V. Here Q e represents
confined at the potential well there, forming a 2DEG inver-
the 2DEG charge at SiO2 /Si and approximately equals the
sion layer. The photoinduced 2DEG at SiO2 /Si is expected
capacitor charge when accumulation biased. A scattering-
to be emitted into the void channel, similar to the case of
free transport of electrons in a void channel converts the
accumulation 2DEG in a dark, forward-biased MOS capac-
potential energy (eV) to kinetic q energy (m ∗ v 2 /2). The
itor as discussed above.
2eV
terminal velocity is expressed as m∗ , and the average A GOS capacitor structure with a void channel was
transit time across the channel has the following voltage fabricated by employing electron-beam lithography (EBL),
dependence: τ av ∼ V −0.5 . The overall voltage dependence of plasma reactive-ion etching (RIE), and graphene transfer
channel current can then be expressed as I = Q e /τ av ∼ V 1.5 , processes (Figure 1.5a). In brief, a SiO2 layer (23 nm thick-
well matching the measurement result (Figure 1.1e): the ness) was grown by thermal oxidation on p-type Si wafer
slope of Figure 1.5 at forward accumulation bias). Here (B-doped, 10 Ω-cm resistivity; (100)-oriented; 525 µm thick-
it should be mentioned that the Child–Langmuir’s three- ness). A bottom-side electrode was prepared by depositing a
halves-power law assumes space-charge-limited emission at 150-nm-thick Al layer (5N purity) on Si by thermal evapora-
cathode (Child 1911, Langmui 1913, Lau et al. 1994). In tion, followed by Ohmic contact annealing at 350◦ C. Verti-
our case, the electrons injected into air (i.e., a nanovoid cally etched trench or hole structures were then formed by
channel) form a space charge around the anode (Al elec- EBL and RIE: a single or 3 × 3 holes (100–150 nm diam-
trode) edge, and this space charge field limits emission of eter, 100 nm depth, and 500 nm spacing) or a single vertical
2DEG at cathode edge. In reverse bias, part of the bias trench structure (100–440 nm width, 100–200 nm depth,
voltage goes to depletion region formation in Si; therefore and 1-mm trench length). A monolayer graphene (grown
the void-channel section receives less voltage than the accu- by chemical vapor deposition method, 3 mm × 4 mm size)
mulation case. This explains the reduced slope (0.5–1.0) in was then transferred to the hole- or trench-etched SiO2 /Si
reverse bias (Figure 1.4b). substrate (Suk et al. 2011).
FIGURE 1.5 Photocurrent response of a graphene/oxide/Si (GOS) capacitor structure with a void channel. (a) Schematic of GOS
structure (graphene/SiO2 (23 nm)/p-Si) with a hole channel (150 nm diameter, 100 nm depth) covered by a suspended graphene
electrode (3 mm × 4 mm). SEM image of hole channel. Scale bar, 200 nm. (b) Photo I–V characteristic measured at reverse bias under
illumination with a 633 nm laser beam (diameter, 1 mm). (c) Schematic of emission and transport of photogenerated 2DEG. (Reprinted
from Kim, M. & Kim, H. K., J. Appl. Phys. 118, 104504, 2015.)
Nanophotonic Devices 1-7
Figure 1.5b shows the photo I–V characteristic of a near-surface states. Image-potential states are a class of
GOS with a single hole measured under illumination with surface states that are widely observed on metallic surfaces,
a 633-nm laser light (1-mm beam diameter). In reverse bias, but they differ from conventional surface states in that they
the photocurrent saturates at 1.0–3.0 V for 0.1–1.0 mW exist in ambient conditions outside the surface (Cole &
input power. Under 1.0-mW illumination, the saturation Cohen 1969, Silkin et al. 2009, Niesner & Fauster 2014).
photocurrent is read to be 0.35 mA at 3.0 V. This corre- Their origin can be traced back to the attractive poten-
sponds to a responsivity of 0.35 A/W and internal quantum tial acting on an electron at distance in front of a conduc-
efficiency (IQE) of 103%. tive surface. Replacing the metal surface by a conducting
The absorption depth of Si is 3.0 µm at 633 nm wave- graphene sheet, image-potential states are expected to form
length. Since a monolayer graphene absorbs only 2.3% of in air on both sides of suspended graphene.
incident light, most photons are absorbed in/near the deple- Some of the impinging electrons are captured/collected
tion region in Si (910–940 nm width at 2–5 V reverse bias: at the edge of 2D hole system (2DHS) in graphene, while
see Figure 1.3c). Photogenerated carriers are separated by majority initially pass through the suspended graphene
depletion field, and photoelectrons drift to the Si/SiO2 inter- (Figure 1.6b). The transmitted electrons, however, reflect
face forming a 2DEG inversion layer. Similar to the case of back at the image-potential barrier. Greater the kinetic
dark forward-biased MOS discussed above, Coulombic repul- energy of impinging electrons, the farther they will be
sion among electrons around the channel edge is expected transmitted through the graphene. For the bias voltage
to reduce the energy barrier enabling low-voltage emis- (potential energy, eV) given smaller than the work func-
sion of 2DEG into air. Emitted electrons travel ballistically tion barrier, however, the transmitted electrons reflect back
in the nanovoid channel and impinge upon the suspended and are eventually captured/collected by graphene anode
graphene. through back-and-forth reflections at the front and back-
Figure 1.6 depicts a band diagram that schemati- side image potential barriers. Assuming an image-charge
−1
cally illustrates electron emission, transport, and capture potential profile, ϕ = 16πε 0
e2 (ε − 1)/(ε + 1)x (Silkin et al.
processes occurring at 2DEG/air, void channel, and 2009, Stratton 1955), an electron impinging with 3–4 eV
graphene, respectively. Note that the energy band of kinetic energy is expected to travel ∼0.2 nm away from
suspended graphene is drawn flanked by the image- the graphene. Here ε is the dielectric constant of graphene
charge potentials on both sides, implying the presence of and is assumed to be 3 (Santos & Kaxiras 2013). Also the
FIGURE 1.6 Emission and transport of photogenerated 2DEG in GOS. (a) Under reverse bias, photogenerated minority carriers
(electrons) form a 2DEG inversion layer at SiO2 /Si. Electrons are emitted into air and travel toward suspended graphene electrode.
(b) Schematic energy band diagram illustrating the transport of 2DEG: electron emission (along the x -direction), transport (along the
y -direction), and capture/collection by graphene anode. Note that the suspended graphene is flanked by image-charge potentials at both
sides. Impinging electrons can be transmitted through the graphene but are reflected back at the image potential barrier and are collected
by graphene anode. (Reprinted from Kim, M. & Kim, H. K., J. Appl. Phys. 118, 104504, 2015.)
1-8 Nanophotonics, Nanoelectronics, and Nanoplasmonics
suspended graphene anode is assumed to be charged (by (three-terminal) configuration (Spindt 1968, Spindt et al.
holes) for impinging electrons. It is interesting to note that 1991, Brodie 1989). In the latter case, the anode poten-
the potential profile around the graphene resembles that tial is usually set sufficiently high in order to collect
of an ion placed near a cathode surface, which has been incoming electrons transmitted through a graphene grid.
reported to enhance the cathode emission (Tirumala & Go In our case, no external collector is employed other than
2010, Binh et al. 1992). The electrons in transit during the graphene anode. Considering the confining nature of
transmission and reflection form space charge around the graphene’s image-charge potential as discussed above, all
suspended graphene, which will affect cathode emission by the impinging electrons would be captured/collected by the
its space charge field (Srisonphan et al. 2014). positively biased graphene anode, and this will satisfy the
Graphene is known to be transmissive to impinging elec- charge neutrality condition of this two-terminal config-
trons while being impermeable to atoms and molecules uration. The closed-circuit nature (i.e., charge conser-
(Bunch et al. 2008). The electron transparency of graphene vation) of this diode-mode operation was confirmed by
has been the subject of interest and debate in recent liter- performing measurements of anode current with the
ature (Müllerová et al. 2010, Yan et al. 2011, Li et al. system ground connected to the bottom (cathode) or top
2014), and the underlying mechanism is yet to be estab- (anode) electrode, which demonstrate the same amount of
lished especially in terms of understanding the interactions channel current for given bias voltage (Srisonphan et al.
between impinging electrons and in-plane electrons/holes 2014). This configurational difference basically explains
in graphene. Most studies were performed in transmission the apparently contradicting performances (and conflicting
electron microscopes at relatively high energies (100 eV) expectations) reported in the literature of suspended
or in electron holography mode at low energies (∼100 eV) graphene, that is, widely scattered data of graphene’s trans-
demonstrating transparences >70% (Kreuzer et al. 1992, parency or opacity to very-low-energy (<5 eV) impinging
Morin et al. 1996, Mutus et al. 2011). For the case electrons.
of very-low-energy electrons (<5 eV), however, reports
are rare.
1.3.3 Emission and Transport of
In this study, a suspended graphene is utilized as a
Photocarrier 2DEG
collector electrode for photogenerated electrons, and the
electron capture performance is characterized. Note also Figure 1.7 shows the measured photo I–V of GOS with
that, in the present study, a diode (two-terminal) config- a single hole (Figure 1.7b) or a 3 × 3 array of holes
uration is employed, as opposed to a conventional triode (Figure 1.7c) (150 nm diameter, 100 nm depth, and 500 nm
FIGURE 1.7 Photocurrent response of a GOS structure with hole channels. (a) Schematic of device structure and photocurrent
measurement at 633 nm wavelength under reverse bias. SEM images of GOS samples: graphene/SiO2 (23 nm)/p-Si with a single hole
(bottom left) or a 3 × 3 array of holes (bottom right). (b) Measured photo I–V of a single hole sample. (c) Measured photo I–V of
a 3 × 3 array of hole sample. The dashed lines indicate the V 3 dependence of photocurrent. (Reprinted from Kim, M. & Kim, H. K.,
J. Appl. Phys. 118, 104504, 2015.)
Nanophotonic Devices 1-9
FIGURE 1.8 Spectral dependence of photocurrent responsivity and quantum efficiency of a GOS with a trench. (a) Photo I–
V measured at three different wavelengths (325, 780, and 980 nm) with different input power levels. At 325 nm: (top to bottom)
0.50 mW, 0.25 mW, 0.10 mW, and dark. At 780 nm and 980 nm: (top to bottom) 1.00 mW, 0.50 mW, 0.25 mW, 0.10 mW, and dark.
(b) Photo I–V was measured at 325–1,064 nm with input power of ∼0.25 mW. The responsivity (empty circles) and internal quantum
efficiency (filled circles) values were calculated from saturation photocurrents. The internal quantum efficiency calculated without a carrier
multiplication (or photoconductive) effect is shown for comparison (dashed). (Reprinted from Kim, M. & Kim, H. K., J. Appl. Phys. 118,
104504, 2015.)
The enhanced efficiency in UV is ascribed to a carrier and the diffusion current J diff is by
multiplication process involving direct-bandgap transitions
(Γ -point with energy gap of 3.4 eV). αLn qnpo Dn
Jdiff = qφ0 exp (−αWD ) + (1.8)
At steady state, the saturation photocurrent is balanced 1 + αLn Ln
by the photocarrier generation rate in Si. The IQE >100%
indicates involvement of photocarrier multiplication or a Figure 1.9 shows the contributions by drift current and diffu-
photoconductor gain effect. The three-step-cascade profile sion current calculated in the UV-to-NIR range. At ∼530 nm
suggests that different mechanisms are involved depending or shorter wavelength, the drift transport (in the depletion
on spectral range. The NIR regime (>∼800 nm) corresponds region of Si) of photocurrent becomes dominant over the
to near-band-edge absorption. Since the amount of above- diffusion transport (in the quasi-neutral region of Si).
bandgap excess energy is negligible in this regime, the under- The current gain in the photoconductor mode is deter-
lying mechanism is believed to involve a photoconductor mined by the ratio of carrier lifetime to transit time (Sze
gain effect that might be caused by charge trapping at the 1981). Considering the fact that the carrier transit time in
SiO2 /Si interface. It should be mentioned that the Si surface drift transport is much smaller than that of diffusion trans-
passivated by thermally grown oxide is known to contain a port, the second step (rise of IQE) observed at ∼530 nm
residual amount of interface states at ∼1011 cm−2 level (Deal or shorter wavelength is ascribed to a photoconductive
et al. 1967, Miki et al. 1988). effect in conjunction with the change in carrier transit time
In the visible-to-NIR range, photocarriers are gener- (Figure 1.8b). An alternative explanation of the step rise
ated both in the depletion and neutral regions, and at ∼530 nm might be a photoelectric effect on 2DEG at
carrier transport is governed by a drift or diffusion the channel edge (Fowler 1931, DuBridge 1932). This corre-
process, respectively. Under steady-state conditions the total sponds to an apparent threshold energy of ∼2.3 eV for
photocurrent through a reverse-biased depletion layer is photoemission and might have contributed to lowering the
composed of contributions by drift and diffusion transports: energy barrier at the 2DEG/air interface. Most incident
photons, however, are absorbed deep inside the depletion
Jtotal = Jdrift + Jdiff (1.6)
region, and only a small portion falling on the 2DEG edge
where the drift current J drift is given by can contribute to this photoelectric effect. Understanding
the specific contributions by different possible mechanisms
Jdrift = qφ0 [1 − exp(−αWD )] (1.7) requires a further study. The steep rise at <400 nm is mainly
Nanophotonic Devices 1-11
which is prone to environmental degradation when exposed itself. The precise placement and tight confinement of emis-
to moisture or oxidizing ambient. It is desirable to build sive material (QDs) into a nanohole will allow high efficiency
OLED on a platform that is chemically inert and physically of carrier injection, suppressing a leakage current that would
scalable (for smaller pixel/device dimensions) and yet effi- bypass an emissive layer.
cient in carrier injection. As the junction diameter scales down, the perimeter-
As an alternative to conventional transparent conduc- to-area ratio goes higher. This means almost the entire
tive oxide (TCO) substrates, we employed Si substrate for injection will be supplied with 2DEG at the edges. If the
building an OLED structure that can be scaled down to a nanohole diameter is scaled down to 10 nm range, the junc-
deep nanometer range. In this section, we describe a recent tion will contain a single QD (Figure 1.10). This single-QD
progress made in our lab in developing QD-OLED struc- OLED structure can be envisioned as a silicon-based single-
tures on silicon with widely scalable junction dimensions: photon source on demand, which is considered to be an
junction diameter is scaled down from 100 µm to ∼20 nm important optical component in future quantum informa-
range. We observed a phenomenon that injection of accu- tion technology.
mulation 2DEG at junction periphery is the primary mech- Below we describe an experimental work demonstrating
anism of carrier injection into an emissive layer, supplying that the injection of accumulation 2D electron gas (2DEG)
a high current density at relatively low bias voltage. The at junction periphery is the dominant mechanism of carrier
resulting edge emission of light is expected to become even injection into an emissive layer confined in a micrometer-to-
more dominant over area emission when the device dimen- nanometer scale hole-patterned QD-OLED structure.
sion further shrinks to a nanometer scale.
Figure 1.10 shows a schematic of a nanometer-scale
1.4.1 Device Fabrication: QD-OLED with
emitter (LED) array that employs core–shell QDs as an
Edge Injection
emissive material, confined in a nanohole array structure
formed on SiO2 /Si substrate. In this structure, the Si An n-type Si wafer was used as a substrate of QD-OLED
substrate is designed to serve as an electron supplier, while structure (Figure 1.11). Thermally grown SiO2 (23 nm
the upper part of the LED structure is comprised of hole- thick) is utilized to define the OLED device area and
supply/transport layers. Note that electrons are designed to create an isolated OLED array. An array of windows with
get injected primarily from the edges (periphery of nanohole various dimensions (20–500 µm) and geometry (circular,
bottom): under forward bias, a 2DEG accumulates at the ring, and square) were opened in the oxide layer by
SiO2 /Si interface, and owing to the Coulombic repulsion photolithography and etching. A colloidal solution of QDs
among electrons, the 2DEG gets injected into the QD (CdSe/ZnS core–shell QDs, 625 nm emission wavelength,
confined in a nanohole. Note also that the insulating layer core diameter of ∼7.5 nm) was spin coated on the window-
(SiO2 ) is designed to be thick enough to prevent tunneling etched SiO2 /Si substrate as an emissive layer. P-type
of carriers through the oxide layer. The holes injected down organic polymers such as poly(9-vinylcarbazole) (PVK)
from the upper part will get confined/trapped by the hole- and poly(3,4-ethylenedioxythiophene) polystyrene sulfonate
barrier layer introduced on the bottom of nanohole. (PEDOT:PSS) were used as hole-transport and electron-
This 2DEG injection is found to be more efficient than the blocking layers. ITO was sputter deposited on top of the
area injection as demonstrated below. Note that the device polymer layer as a transparent electrode.
structure also allows placing QDs on a predetermined loca- Figure 1.11 shows an energy band diagram of the proposed
tion with nanometer precision. QDs placed outside (i.e., on device. The carriers injected into QD will remain confined
SiO2 layer) will not receive electron injection, and therefore due to the large-bandgap shell layer of ZnS. The 2-nm
the junction area is self-aligned to/defined by a nanohole ZnS shell surrounding the CdSe core also passivates surface
defects. High quantum yield of a core–shell (CdSe/ZnS) QD
facilitates most of the injected electrons and holes to recom-
bine radiatively. PVK is used as a hole-transport layer as well
as an electron-blocking layer due to its low level of highest
occupied molecular orbital (HOMO) and its high level of
lowest unoccupied molecular orbital (LUMO). PEDOT:PSS
is used as a buffer layer to increase anode work function from
4.7 eV (ITO) to 5.2 eV and also to reduce surface damage
by a sputtered ITO film.
FIGURE 1.10 Schematic of nanometer-scale QD-OLED struc- Besides the outstanding potential of nanometer-range
ture that contains core–shell QDs as an emissive material in scalability of junction dimension, the SiO2 /Si substrate
a nanohole formed on SiO2 /Si substrate. By scaling the hole offers an interesting mechanism of carrier injection into junc-
diameter, the number of QDs can be controlled. (a) A nanohole tion area. The OLED structure, when formed on SiO2 /Si
containing a single QD. (b) A nanohole containing multiple QDs. substrate, can be viewed as a MOS structure. The accu-
Note that 2DEG at SiO2 /Si is designed to get injected into QDs mulation 2DEG formed with forward bias can then serve
primarily from the edges (periphery of nanohole bottom). as electron reservoir/supply that is readily available for
Nanophotonic Devices 1-13
FIGURE 1.11 Proposed QD-OLED device structure on Si substrate (a), band diagram in the field oxide area (b), and band diagram
in the active device area (c). (Reprinted from Emon, D. H. et al., J. Vac. Sci. Technol. B 34, 06KJ01, 2016.)
injection into an emissive layer through the junction edges. into an oxide layer (Figure 1.13). This ring trench pattern
Figure 1.11 shows carrier flow in two different areas of OLED provides two edges (inner and outer sides) and was chosen in
device, the insulating oxide area (outside the window) and order to test/avoid any ambiguity that may arise related to
the emissive area on Si (within the window), respectively. an oxide/Si step effect on lateral conduction or spin-coating
process induced nonuniformity. When we start injection, the
device turns on and emits visually detectable luminescence
1.4.2 Edge Emission from QD-OLED
at <5 V. To capture a digital image at relatively short inte-
The SiO2 /Si interface can accumulate a high concentra- gration time (0.5 s), we went up to 12 V bias. At 12 V
tion of 2D electron gas at proper bias, e.g., 1012 cm−2 at pulsed injection, short expose time captures most bright
∼1 V forward bias. At this density level, the average spacing emission region, which appears in this device as the circle
between electrons in the 2DEG is estimated to be ∼10 nm, along the edges (Figure 1.13). But increasing the exposure
smaller than the oxide thickness (23 nm). This close spacing time to 8 s reveals that the other bulk device area also emits
will ensure that the in-plane interaction of 2DEG electrons light, although less bright than the edge lines (Figure 1.4).
becomes stronger than the dipole charge interaction across The bright circles along both the inner and outer edges of
the oxide layer. Due to this Coulombic repulsion at the edge, the ring trench strongly suggest quasi-1D emission induced
the energy barrier for electron emission into the outside is by 2DEG injection.
lowered, enabling electron emission at relatively low bias Regarding the lifetime, this device was tested at elevated
voltage. In the case of a MOS with a void-well channel, it has bias (20 V) for several minutes, and it did not show
been reported that the channel current is proportional to the
perimeter of the well, indicative of edge injection/emission
of 2DEG. A similar behavior is expected with our OLED
structure: the SiO2 /Si interface in the field oxide area under
ITO electrode will accumulate 2DEG at forward bias, which
will be emitted at the edge into the adjacent layer (i.e., the
QD emissive layer) (Figure 1.12).
In order to test/demonstrate this edge-injection mecha-
nism of 2DEG, we also fabricated a ring pattern (50-µm
ring width and 500-µm inner diameter) of windows etched
any degradation or thermal damage. Since the edge was of the hole, not the area of the hole (Figure 1.14b). Here
very brightly emitting, indicative of high density of carrier we note that the diameter (and perimeter) is scaled up
injection, we expected thermal degradation as a form of one order of magnitude, whereas the area is scaled up two
bubble might appear at trench edges. But surprisingly and orders of magnitude. The current at higher voltage follows
interestingly, the edge region remains very stable and degra- perimeter scaling. (The larger current of 20-µm circle at
dation free, even after a long-time operation at large bias lower bias is not clearly understood yet and is ascribed to
voltage (∼20 V). This observation suggests that direct injec- nonideal leakage current.) The measured I–V characteristics
tion of 2DEG into the active layer has greater efficiency also reveal relatively low turn-on voltages (1–2 V) of OLED,
(than bulk area injection of electrons) in generating photons, and this can be attributed to low-voltage injection of 2DEG
possibly by minimizing/avoiding the nonradiative recombi- at the window edges.
nation processes of injected electrons which would otherwise
produce heat causing thermal degradation. Figure 1.13c is
1.4.3 Nanoparticle-Patterned Etch Mask
a measured electroluminescence spectrum showing an emis-
for Nanohole Fabrication
sion peak at 627 nm from CdSe/ZnS QDs.
Since we observed strong and robust emission of light As an alternative to conventional nanolithography tech-
along the edges of trenched OLEDs, as a next step, we niques (such as electron-beam or focused ion beam), we
wanted to determine/compare contributions from area injec- have developed a nonlithographic method that can form
tion and perimeter injection of carriers. We patterned nanoscale hole patterns on SiO2 /Si substrate. In this study,
circular holes of 20-, 200-, and 500-µm diameter on SiO2 /Si we have used colloidal gold nanoparticles to create circular
substrate by photolithography and built the proposed OLED etching windows in a dielectric etch mask film. The etched
structure. The emission photo of the devices shown in holes have a diameter similar to that of the nanoparticle.
Figure 1.14a reveals a strong tendency toward edge emission. The following sections describe the fabrication process of
A comparison of I–V characteristics of the devices shows nanoholes and corresponding nano-OLED samples.
that the injection current is proportional to the perimeter The overall process flow is shown in Figure 1.15. To begin
with, we chose n-Si <100> wafer (phosphorous doped with
a resistivity of 5 Ω cm). After solvent and acid cleaning
(RCA cleaning), a thermal oxide of 25 nm thickness was
grown. An Ohmic contact was prepared on the backside of
bare silicon by depositing 150-nm-thick Al and subsequent
annealing at 350◦ C.
The first step in creating nanoholes is to deposit gold
nanoparticles (Au-NPs) on the substrate (Figure 1.15a).
Three different sizes of citrate-stabilized Au-NPs in colloidal
solution (purchased from Ted Pella) were used: 20, 50, and
200 nm diameter. A valid concern with spin coating of
NPs on SiO2 surface is that the hydroxyl group on the create discontinuities in alumina film through which gold
oxide surface lacks any affinity to citrate-passivated NPs, etchant can diffuse. Due to the conformal coating nature of
and therefore NPs are easily washed away without adhering sputter deposition, the etch window size formed in alumina
to the substrate. To mitigate this surface adhesion issue, is expected to be slightly smaller than the NP diameter.
we modified the oxide substrate with an N-(2-Aminoethyl)- We used aqua regia as the gold etchant since it has a high
3-aminopropyl-trimethoxysilane (AEAPTMS) coating that etch selectivity (over 1,000 for gold over alumina). We found
binds free amine (−NH2 ) group to the surface (Wei & that, at room temperature, aqua regia etches alumina at
Wang 2015). The silane group interacts with the hydroxyl- 0.3 nm/min, while gold is etched at a rate of 10 nm/min.
terminated oxide surface to form siloxane that consists of The sample was then ultrasonicated in aqua regia for 5 min
an amine (−NH2 ) group at the tail. When this sample to break loosely connected alumina film covering the upper
is immersed in the gold colloidal solution, the amine half of the NPs. After rinsing and drying the sample, we get
group becomes protonated forming NH+ 3 which can now nanoporous alumina film where the hole diameter follows
bind the negatively charged citrate ions surrounding the NP size.
gold nanoparticles. Process-wise, the 0.1% AEAPTMS In the fourth step (Figure 1.15d), plasma RIE was
solution in water was spin coated on the SiO2 (25 performed in CHF3 /O2 gas to etch SiO2 through the open-
nm)/n-Si sample at 2,000 rpm followed by a 30-min ings of alumina layer. The CHF3 /O2 gas mixture was found
baking at 120◦ C. The NP colloidal solution was then to have an etch selectivity of ∼10 for Si and SiO2 over
spin coated on this sample. The residual chemicals/ions alumina: the etch rates for Si, SiO2 , and alumina were
on the surface were removed by submerging the sample measured to be 0.9, 1.1, and 0.1 nm/s, respectively. We
in deionized (DI) water for 5 min followed by nitrogen etched the nanoholes for 50 s, rendering a hole depth of
blow dry. 45 nm. In the final step, alumina was removed using 1:1:3
In the next step, we created a complementary hole pattern volumetric ratios of NH4 OH: H2 O2 : H2 O at 80◦ C temper-
from the NP-coated sample by depositing a thin alumina ature. At room temperature, this solution shows a high
film on it and then etching away the NPs (Figure 1.15b,c). (>100) etch selectivity for alumina over Si or SiO2 . It also
Alumina (Al2 O3 ) was chosen as the mask for its high creates a monolayer of SiO2 on bare Si surface, which helps
selectivity of etching against gold and SiO2 etchants. The to passivate the RIE etched hole surface. The SEM image of
alumina film was deposited by radio frequency (RF) sput- the final nanochannel samples processed from 200, 50, and
tering using a 99.9% pure alumina target in Ar ambient with 20 nm nanoparticles are shown in Figure 1.16. As stated
∼0.8 nm/min deposition rate. To prevent complete covering earlier, the resultant hole in the alumina film is always
of NPs, the alumina film thickness needs to be smaller than smaller than the original NP diameter. In our case, the
the NP radius. In our case, the total film thickness was 200-nm NP results in ∼160-nm hole diameter, 50-nm NP
kept at 30, 15, and 7 nm for 200-, 50-, and 20-nm diam- gives 40 nm, and 20-nm NP results in about the same-sized
eter NPs, respectively. Thus, the Au-NPs are expected to holes.
FIGURE 1.16 SEM images of final nanohole-etched samples processed from 200-, 50-, and 20-nm gold NPs: (top row) Au-NPs
embedded in alumina and (bottom row) nanoholes etched into SiO2 /Si substrate. Note that the nanohole diameters are smaller than
corresponding Au-NP diameters.
1-16 Nanophotonics, Nanoelectronics, and Nanoplasmonics
FIGURE 1.17 Optical micrograph of electroluminescence from QD-OLED samples formed on 160- and 40-nm diameter nanoholes.
The bright 200-µm stripe patterns contain nanoholes, while the dark areas are planar oxide without holes.
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