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Surface Science Letters
Light emission from a single atom
M. Sakurai a,*, C. Thirstrup b, M. Aono a,c
a National Institute for Materials Science (NIMS), 1-2-1, Sengen, Tsukuba, Ibaraki 305-0047, Japanb Vir A/S, Kuldyssen 10, 2630 Taastrup, Denmark
c Department of Precision Science and Technology, Osaka University, Suita, Osaka 565-0871, Japan
Received 18 October 2002; accepted for publication 14 November 2002
Abstract
Scanning tunneling microscope (STM)-induced light emission from a single Si dangling bond on a Si(0 0 1)-(2� 1)–
D surface was studied at room temperature. Switching events of a single Si dangling bond were observed in the light
intensity map and in the topographic image recorded at a bias voltage of )3 V. High spatial resolution of a light in-
tensity map supports that the light emission is due to radiative transition of electrons between the localized surface state
of Si dangling bond and the surface state of the STM tip.
� 2002 Elsevier Science B.V. All rights reserved.
Keywords: Scanning tunneling microscopy; Luminescence; Surface electronic phenomena (work function, surface potential, surface
states, etc.); Silicon; Deuterium
Manipulation of light using nanoscale struc-
tures has been studied actively [1], and the studies
are related to applications such as photonic or
optoelectronic devices. Scanning tunneling mi-
croscope (STM)-induced light detection is one
method employed to study optical properties of
nanoscale structures [2]. Utilizing the fact that theSTM tip is an atomic scale injection source enables
us to measure the optical response of a single atom
and helps understanding the mechanisms of STM-
induced light emission [3]. In a present paper, the
studies have been focused on precise spatial dis-
tribution of the light emission from a single Si
dangling bond at room temperature. Although
light emission from a single molecule has been
studied using near-field optics [4], the present
sample made of Si and deuterium (D) atoms has
the unique character that the area of light emission
is localized to a single Si atom site and that the
position of a single Si dangling bond can be con-
trolled by the bias voltage applied to the STMtunneling gap [5]. Based on experimental results,
we propose a single atom light switch.
All experiments were performed in an ultra-
high vacuum (UHV) chamber with a base pressure
of 1� 10�8 Pa using an STM and electrolytically
sharpened tungsten (W) tips. Exposure of a clean
Si(0 0 1)-(2� 1) surface (antimony-doped, n ¼ 1�1018 cm�3) to atomic D gas at a sample tempera-ture of 600 K produced a Si(0 0 1)-(2� 1)–D surface
structure, similar to the hydrogen (H)-termination
technique [6]. In the present experiment, D atoms
*Corresponding author.
E-mail address: [email protected] (M. Sakurai).
0039-6028/02/$ - see front matter � 2002 Elsevier Science B.V. All rights reserved.
doi:10.1016/S0039-6028(02)02654-7
Surface Science 526 (2003) L123–L126
www.elsevier.com/locate/susc
were used rather than H atoms for the surface
termination, because the STM-induced desorption
yield of D is much lower than the corresponding
desorption yield of H [7]. After creating a few Si
single dangling bonds by the extraction of D atoms
using the STM tip [8], the light demitted from thetunneling gap was collected by an optical fiber
bunch, and it was guided to a detecting plane of a
water-cooled photon multiplier tube [9]. The de-
tectable range of light in the present system is 350–
850 nm.
Fig. 1(a) and (b) show occupied-state and un-
occupied-state STM images of a Si(0 0 1)-(2� 1)–
D surface, respectively. Bright spots on the terracein Fig. 1(a) correspond to single Si dangling bonds.
In Fig. 1(b), the dark ring surrounding the bright
spot of a single dangling bond is formed by the
change of potential. The electric charge occupied
on a surface state of a single dangling bond [10] is
screened by the holes induced by the positive
sample bias voltage. Then the decrease of electric
charge density around a single dangling bond leads
to the dark ring in the unoccupied-state image.
The ring pattern in the unoccupied-state image can
be used as judgment on a single or double dangling
bond. The bright spots marked A, B, C, and D in
Fig. 1(a) correspond to single dangling bonds. Fig.
1(c) and (d) are a light intensity map and a topo-graphic STM image of the same area, respectively.
The images were recorded simultaneously at a
sample bias voltage (Vs) of )3 V, a tunneling cur-
rent (It) of 3 nA, and a scanning velocity (vt) of 9nm/s. In the light intensity map, light is emitted
when the tip is located above Si dangling bond
sites. The light intensity on dangling bond sites is
100–150 counts per second (cps), which corre-sponds to the quantum efficiency of the order of
10�6 photons/electron. The average light intensity
on D-terminated areas is 3–5 cps, which is com-
parable to the dark count level of the system.
The contrast formation in the light intensity
map is caused by the difference of the surface states
below the tip apex from following reasons. Bulk Si
materials emit few photons due to its indirect bandgap. Tip-induced surface plasmon gives small
contribution to the light emission, because plasma
resonance energies of Si and tungsten materials
formed the tunneling junction are not in the visible
spectral range. On Si dangling bond sites, surface
states of the Si dangling bond are positioned near
the Fermi level. On D-terminated areas, the sur-
face states are lost by the bond formation. Theninelastic tunneling of electrons from the occupied
surface state of Si dangling bond near the Fermi
level to an unoccupied surface state of the tip leads
to the visible light emission.
Fig. 2(a) shows the magnified topographic im-
age of the single Si dangling bond marked as C in
Fig. 1(d), suggesting that the Si dangling bond
switches sites during the tip scanning. On the lineas marked by the white arrows, the Si dangling
bond is located on the right hand side of the Si
dimer. On the line as marked by the gray arrows,
the dangling bond is on the left hand side of the Si
dimer. The scanning condition of Vs ¼ �3 V is in
the range that an STM-induced switch of a single
Si dangling bond occurs frequently (�3:2 <Vs < �2:2 V) [5].
Fig. 2(b) shows the corresponding light inten-
sity map of a single Si dangling bond. The light
A
B
CD
(a) (b)
(c) (d)
6 nm
A
B
C
D
A
B
C
D
A
B
CD
Fig. 1. Topographic (a) occupied-state and (b) unoccupied-
state STM images of a Si(0 0 1)-(2� 1)–D surface with a few
single Si dangling bonds. (c) Light intensity map and (d) to-
pographic image of the same area recorded simultaneously at
Vs ¼ �3 V, It ¼ 3 nA, and vt ¼ 9 nm/s.
L124 M. Sakurai et al. / Surface Science 526 (2003) L123–L126SU
RFACE
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LETTERS
intensity map exhibits switching of the light in-tensity as similar to the switching of a single Si
dangling bond in the topographic image. Fig. 2(c)
depicts cross-sectional line profiles of the light in-
tensity map. In the second, third and seventh line
profiles, the protrusion of light intensity is posi-
tioned on the right hand side, whilst in the fifth
and sixth profiles the protrusion is positioned onthe left hand side. The region of the light emission
changes similarly to the motion of the Si dangling
bond. In the fourth profile, light is not emitted,
because the switching event occurred when the tip
was located near the right hand side of the dimer
where the Si dangling bond occupies. The rela-
tionship among the tip, the single Si dangling
bond, and the light emission is schematically il-lustrated in Fig. 2(d). The lateral extension of the
light emitting area is the same as that of the wave
function of the single Si dangling bond [11], sug-
gesting that the event of the light emission oc-
curred by the transition from the localized surface
state of the single Si dangling bond. It should be
noticed that the switching event is caused by the
STM tip, whose electric field reduces the energybarrier between the two sites of a dimer [5]. Then
the light emission including the switching can be
controlled by the precise position of the Si dan-
gling bond to the tip apex under suitable bias
voltage condition.
Fig. 3(a) and (b) are occupied-state and unoc-
cupied-state STM images of a Si(0 0 1)-(2� 1)–D
surface with a few Si dangling bonds, respectively.The Si dangling bonds marked as A and B in the
figures are double Si dangling bonds, whose pH
state in the unoccupied-state image exhibits a node
plane between the dimer atoms [12]. Fig. 3(c) and
(d) shows topographic STM image and light
1 nm
(a) (c)
(b)
(d)
ON OFF
0.8 nm
Si dangling bond D atom
STM tip
Si dimer
Light
Ligh
tin
tens
ity[a
rb. u
nits
]
Fig. 2. (a) Focused topographic image around the single Si
dangling bond marked as C in Fig. 1(d). The Si dangling bond
switches sites during the line scan. (b) Corresponding focused
light intensity map. (c) Cross-section line profile of light in-
tensity along each horizontal line in (b). (d) Schematic illus-
tration of a single atom light switch using the STM tip apex and
one Si dimer with one Si dangling bond.
(a) (b) (c) (d)
A
B
A
B
A
B
A
B
3 nm
Fig. 3. Topographic (a) occupied-state and (b) unoccupied-state images of double Si dangling bonds as marked A, B. (c) Topographic
STM image and (d) light intensity map of the same area recorded at Vs ¼ �3 V, It ¼ 3 nA, and vt ¼ 9 nm/s.
M. Sakurai et al. / Surface Science 526 (2003) L123–L126 L125
SURFA
CESCIEN
CE
LETTERS
intensity map of the same area recorded at Vs ¼ �3
V, It ¼ 3 nA, and vt ¼ 9 nm/s. The cross-sectional
line profile of the double Si dangling bonds in the
light intensity map has the similar protrusion tothat of the p state of the Si dimer in the topo-
graphic image, supporting that the light is created
by radiative transition of electrons from the oc-
cupied p state of double Si dangling.
Fig. 4(a) and (b) are occupied-state and unoc-
cupied-state STM images of Si(0 0 1)-(2� 1)–D
surface with a few Si dangling bonds. Fig. 4(c) is
the light intensity map of the same area recordedat Vs ¼ þ3 V, It ¼ 0:4 nA, and vt ¼ 9 nm/s. In the
case of the positive Vs, the switching event of a
single Si dangling bond was rarely observed. The
lateral extension of the light emission is localized
to the Si dangling bond sites, indicating that the
light is created by the radiative transition of elec-
trons to the localized surface state of the Si dan-
gling bond.Since the light is emitted from a single Si atom
below the tip apex and since the switching of a
single Si dangling bond can be controlled by the
applied bias voltage, a simple system made of the
STM tip and one Si dangling bond can be used as
a single atom light switch. The idea is schemati-
cally illustrated in Fig. 2(d). When the tip is lo-
cated above a single Si dangling bond, light is �ON�(left panel in Fig. 2(d)). If we apply suitable neg-
ative Vs between the tip and the single Si dangling
bond, the Si dangling bond switches to the other
site of the dimer and switches off the light (right
panel in Fig. 2(d)).
In summary, intensity maps of light emission
from a single or double dangling bond on D-ter-
minated Si surface have the high spatial resolution.
The spatial localization of the light emission on the
dangling bond sites at both polarities of Vs sup-
ports the mechanism of the light emission by theradiative transition between the surface states
across the tunneling gap. Present results based on
a single atom light emission suggest one possibility
of forthcoming single atom devices.
Acknowledgements
This research was supported by Atomic-Scale
Sciengineering Research in RIKEN (The Institute
of Physical and Chemical Research).
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(a) (c)(b)
A
B
C
D
A
B
C
D
A
B
C
D
3 nm
Fig. 4. Topographic (a) occupied-state and (b) unoccupied-
state STM images of a Si(0 0 1)-(2� 1)–D surface. (c) Light
intensity map at Vs ¼ þ3 V, It ¼ 0:4 nA, and vt ¼ 9 nm/s on the
area as shown in (a).
L126 M. Sakurai et al. / Surface Science 526 (2003) L123–L126SU
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SCIENCE
LETTERS