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Acta Phys. -Chim. Sin. 2013, 29 (7), 1370-1384

1370

July

doi: 10.3866/PKU.WHXB201304191

[Review]

www.whxb.pku.edu.cn

1,2

(1 , 100190;

1,*

1,*

, 100871)

(NC-AFM). NC-AFM

. NC-AFM
. NC-AFM qPlus ,
, NC-AFM
, (KPFM)(LCPD)
. NC-AFM .
:

; ;

qPlus ; ; ; ;

O647

Research Progress in Atomic Resolution Microscopy


YUAN Bing-Kai1,2

CHEN Peng-Cheng1
ZHANG Jun1
QIU Xiao-Hui1,*
WANG Chen1,*

CHENG Zhi-Hai1

(1National Center for Nanoscience and Technology, Beijing 100190, P. R. China; 2Academy for Advanced Interdisciplinary Studies,
Peking University, Beijing 100871, P. R. China)
Abstract: Tremendous progress has been made in non-contact atomic force microscopy (NC-AFM)
recently. The spatial resolution of NC-AFM imaging and spectroscopy of individual molecules on surfaces
has reached true atomic resolution and bond differentiation level. Combination of NC-AFM with other
scanning probe techniques can open a new way for materials, physics, chemistry, and biochemistry
studies. In this review, we first introduce the basic principle of NC-AFM and qPlus sensor. The interaction
force at atomic scale and precise measurement of short-range force are discussed. We summarize the
recent advances in structural determination of organic molecules, chemical identification, electronic
structure, and atomic manipulation at the atomic scale. In addition, we also discuss the application of
Kelvin probe force microscopy (KPFM) in measurement of local contact potential difference (LCPD).
Finally, perspectives and challenges in NC-AFM techniques are presented.
Key Words:

Scanning probe microscopy; Non-contact atomic force microscopy; qPlus sensor;


Chemical identification; Atomic manipulation; Electronic structure; Kelvin probe force
microscopy

Received: January 14, 2013; Revised: April 17, 2013; Published on Web: April 19, 2013.

Corresponding authors. WANG Chen, Email: wangch@nanoctr.cn; Tel: +86-10-82545609. QIU Xiao-Hui, Email: xhqiu@nanoctr.cn;
Tel: +86-10-82545583.
The project was supported by the National Key Basic Research Program of China (2012CB933001) and National Natural Science Foundation of
China (21173058).
(2012CB933001)(21173058)

Editorial office of Acta Physico-Chimica Sinica

No.7

(SPM)
, 20 80
/. 1981 IBM (international
business machines corporation)
Binnig 1 (STM).
,

. STM (STS)

. , STM /

. STM
. STM
, ,
.
STM ,
,
.2,3 1986 , BinnigQuate Gerber4

,
(AFM). AFM
, ,
. ,
AFM
.
AFM : (contact
mode)(amplitude-modulation mode)
(frequency-modulation mode).5
AFM, AFM,
, .
, -,
. AFM,6,7 AFM,
.
,
, . , -
,
, ,
,
.
, , AFM
, .
, -

1371

,
. , AFM
105, AFM ,
, . 1991 , Albrecht
8 . AFM,
(NC-AFM), -
(f).
NC-AFM AFM .
, NC-AFM
, .
NC-AFM AFM
,
. , qPlus ,
NC-AFM ,
.9,10 NCAFM

.11 ,
,
. , NC-AFM
(KPFM)
,
.12,13 NC-AFM
.14
NC-AFM ;
-
-;
NC-AFM ,
qPlus ;
;
NC-AFM

KPFM ,
.

2
2.1

AFM -
.
. (k)
(f0)(Q). ,
f0 , (A)
. , -

1372

Acta Phys. -Chim. Sin. 2013

,
. f

.
NC-AFM 15( 1)
.
,
. .
/2,
. .
,
, .
,
--(PID )
, .
.
, . , AFM
,

f ,
. ,
,
,
.
2.2
, AFM -

Vol.29

.
, Pauli
. ,
. , ,
, ,
.
( 100 nm).
(0.1 nm ). AFM
-
. AFM
, ,
, .
,
.16 ,
.
,
.17

Pauli .18,19
, -,
, ,
. ,
-.
2.3
f NC-AFM ,
-
(Fts), Fts
. , f Fts :20
-u
f0 1

du (1)
F
[z
+
A
(1
+
u)]
ts
0
0

2
kA0 -1
1
u

z0 -, k
f = -

, A0 . (kernel
function)

K(u) = -u
u {-1, 1}
(2)
2
1-u
, , f

1 NC-AFM (
)15
Fig.1 Block diagram of the non-contact AFM feedback
loop for constant amplitude control and frequency-shift
measurement15

(u=-1);
u=1 , -
( 2).20 f
. (
0.1 nm), f -
:

No.7

f=ktsf0/2k
(3)
kts -, -
(-dFts/dz). ,
, kts .
, f .
Nm-1
Nm-1, . 0.1 nm
,
, (jump to contact).21
0.1 nm ,
Nm-1.
,
NC-AFM ,
(quartz LER)22,23,
qPlus 24 .25
LER
.26 LER
f,
. k Nm-1,
0.5 MHz MHz. 2008 , Hasegawa 23

1373

LER AFM pm Si(111)-(7


7). qPlus
Giessibl ,
. qPlus
f,
. ,
k Nm-1, 32-200 kHz. 3
qPlus .
, .
LER ,
. Si , qPlus
LER :15,27
Nm-1 Nm-1,
, Pauli
, ; ,
;
Si ; ,
,
, , . ,
qPlus LER AFM STM .
STM/AFM -
.
,
.
2.4
NC-AFM
. -

K(u) 20
Fig.2 Total interaction force between tip apex and
surface and the behavior of the kernel function K(u)20

K (u) = -u
2

u { - 1, 1}
1-u
ks: spring constant of the cantilever; A0: the amplitude of the
cantilever; R: the nominal radius of the tip apex; d: the closest
tip-surface distance; Fint: the interaction force

3 qPlus
Fig.3 Micrograph of a qPlus sensor
The qPlus sensor consists of three parts: a tuning fork, a ceramic
substrate, and a tip. The tip is connected with a squeezed gold wire
(diameter 12.7 m) in order to measure tunneling current.

1374

Acta Phys. -Chim. Sin. 2013

, /
. -
(f)-
(z), f(z). f(z),

. f(z),

, XY
, .

.
(1). (1)
-, Fts(z) Ets(z). Sader
Jarvis28 , .
-
. /
,
.
, ,
. ,
, .
()f(z),

. Hamaker 29
, R
1/z2,30,31
FvdW(z).
-
Fshort-range(z). -
,
,

.
f(x, y, z)
.11
,
.
, .

,
.32-36 Albers
37,38 .
f ,

Vol.29

, f (image-by-image)
,
, -,
, f(z). f(z)
Fts(z) Ets(z).
Fts(x, y, z) Ets(x, y, z).
,
.
,
.

3
3.1

. STM
. STM
, STM
, .
Temirov 39-42
(scanning tunneling hydrogen microscopy)
. 1995 , Giessibl43
NC-AFM Si . ,
(Si(100)-(21)GaAs(110)InP(110)
InAs(110))(HOPG)
; (NaClMgO )
(Cu(100)Ag(100))
; C60
.44,45
, qPlus , NC-AFM
STM ,
, .
Giessibl 46,47 Si(111)
W . 2009 ,
IBM Gross 48
,
AFM . 4(a)
Cu(111) STM
, 4(b-f) AFM .
, STM
. AFM
,
CH . CO
,

No.7

,18 Pauli
,
.
Pauli ,
. ,
,
(Pauli ), 100 pm
. ,
qPlus 30-100 pm . ,

, /
. CO . CO

.
, Pawlak 49,50
C60
, C60 .
Boneschanscher 51 CO
, ,

.
NC-AFM ,

,
,

1375

. , Gross 10
CO
CC ,
CC ( 4(i, j)). CC
: (1) CC
, ; (2) CO
35 CC .

.52 , Gross 53
qPlus ,
,
(cephalandole A)( 4(g,
h)), .
,
. , Welker
Giessibl54 qPlus
CO
, Cu(111)
CO . ,
,

.
STM NC-AFM , qPlus
SPM ,
. Mohn 55

4 NC-AFM 10,48,53
Fig.4 NC-AFM images of molecules with atomic resolution 10,48,53
(a) STM image of pentacene on Cu(111). (b) constant-height AFM image of pentacene on Cu(111) with CO tip. (c-f) constant-height AFM images
of pentacene on NaCl(2 ML)/Cu(111) with different tip terminations, (c) Ag tip, (d) CO tip, (e) Cl tip, (f) pentacene tip. (g, h) constant-height AFM
image of cephalandole A and the same image with superimposed molecular model, respectively. (i, j) molecular model and the constant-height AFM
image of C60, the inset in (i) is the STM image of C60.

1376

Acta Phys. -Chim. Sin. 2013

STM NC-AFM NaCl(2ML)/Cu(111)


(PTCDA) Au
. STM
, NC-AFM Au
/. Pavliek 56
STM (dibenzo[1,8]
thianthrene, DBTH) NaCl(2ML)/Cu(111)
. NC-AFM
DBTH ,
. , STM NC-AFM
STM .
, NC-AFM

, .
,
. , NC-AFM
, CO , NC-AFM
. ,
, NC-AFM
,

,
.
,

.
3.2
/
. STM
. Ho 57
Cu(100)
CH CD .
NC-AFM
. NC-AFM 58,59
60-63 10,48,53,55 .
,
-.

.60,61,63
. 2001
Lantz 64
Si(111)-(77) Si

Vol.29

. 2007 , Sugimoto 59
-, SiSn Pb
( 5).
,
,
-.
(
5(a, c)), ,

( 5(b, d)), Pb Si
0.59, Sn Si
0.77.
, Si, Pb Sn ,
( 5(e, f)).
Setvn 58 III-IV

5
59
Fig.5 Chemical identification of individual surface atoms
by probing short-range chemical interaction forces59
(a) sets of short range force curves obtained over structurally
equivalent Sn and Si atoms. The tips differ from set to set. (b) the
same force curves as in (a) with the curves in each set normalized to
the absolute value of the minimum short range force of the Si curve.
(c, d) sets of short-range force curves for Pb and Si, before (c) and
after (d) normalization. (e) NC-AFM image showing the local
chemical composition of a surface alloy composed of Si, Sn and Pb
atoms blended in equal proportions on a Si(111) substrate. Green,
blue, and red atoms correspond to Pb, Sn and Si, respectively.
(f) atom counts as a function of the maximum attractive total force
measured over the Pb, Sn and Si atoms.

No.7

, Si(100)-(21) In Sn
, .
, :9
CC ;
;
;
, ,
, . ,
CC
.
,

,65 . STM
NC-AFM .
3.3

, /. /
1990 IBM Eigler 66
. STM Ni(110) Xe
. (push, pull or
slide),67 ;
,68,69
.
, ,
70 71 ;
,
, . ,
AFM ,

Fig.6

1377

.72,73 STM , AFM


,
.

Morita . /
, STM
,
AFM . 2003 ,
Morita 74 NC-AFM Si(111)(77). Morita
75 Si(111)-(77)
. 76,77
NC-AFM Ge(111)-c(28)
, AFM
Ge(111)-c(28) Sn Ge
( 6(d)).
-
. 6(a)
. ( 6
(b)), Sn Ge . 6(b)
,
Sn Ge .
( 6(b)),
. ,
-,
. , Sn Ge
, .
-
.

6 72
Lateral interchange manipulation on semiconductor surfaces72

(a) schematic illustration of lateral interchange manipulation. (b, c) AFM images before and after the lateral manipulation of Sn atoms (higher
protrusions) on the Ge(111)-c(28)surface, and the scan direction is highlighted in (b) by the arrow in the blue square. (d) final atomic design after
lateral interchange manipulation. Identical method has been successfully applied in other surfaces of different structure and composition.
(e) Sn/Si(111)-( 3 3)R30, (f) In/Si(111)-( 3 3)R30, (g) Sb/Si(111)-(77)

1378

Acta Phys. -Chim. Sin. 2013

, 6(d).
,
,72,78 Sn/Si(111)-( 3 3)
R30, In/Si(111)-( 3 3)R30 Sb/Si(111)-(77) (
6(e-g)). , Morita 79 Sn/Si(111)-( 3
3)R30 Si Sn
, Si
,
.
, /
, ,
.80
,
, . NC-AFM
/ . 2006 ,
Hirth 81 CaF2(111)
. , Morita 82
KCl(100)
. 83
.
/
,
.
/
, qPlus
/.
- ,
NC-AFM /,
,
, -
. STM
,
,
,
. 2008 , Ternes 84

. Pt(111) Co
210 pN, Cu(111) Co
17 pN, Co
. Cu(111) Co CO
, CO
160 pN. , Co
, CO

Vol.29

. Co CO
,
.
,
. ,
85 Pb(111)
(H2Pc) H2Pc
. ,
25 pN,
.

, ,
.
,
.
. STM AFM, Temirov 86,87
Ag(111) Au(111) PTCDA
.
Ag(111) PTCDA
, Au(111)
. Ag(111),
; Au(111)
. Pawlak 88 NC-AFM
.
, (100 100
pm2).
, ,
.
.
3.4

.89,90 /
91-94 95,96
. STM .
. STM AFM,
. 2000
, Schirmeisen 92
.
.97-100 Sawada 97
Si(111)-(77)
101 Si

No.7

. 2011 , Ternes 98 qPlus


AFM (DFT)

-
.
, .
,
.

NC-AFM ,
. Hauptmann 100
Cu-C60 C60-C60 ,
C60-C60 Cu-C60
. Schull 102,103 STM
Cu-C60 C60-C60 .
/

. Sweetman 104
NC-AFM
.
. Si(100)

, buckled dimers . Buckled dimers


,
,
.
3.5
KPFM
(CPD), Nonnenmacher 105 1991
. , CPD
:
sample - tip
VCPD =
(4)
|e|
, tip sample , e
. ,
, VCPD,

. KPFM :13
KPFM f(V). KPFM ,
( 0)-
, f 0 .
f
CPD. , f (Vbias)

1379

. f(V)
CPD, f
-.
- z f(V), f Vbias
z .106,107
CPD
, .
KPFM CPD
(LCPD). LCPD Wandelt108,109
.

. LCPD .
LCPD
.
,
.
, AFM
, LCPD .
, KPFM
. KPFM LCPD
,110 Si(111)-(77)Si(111)-( 5 3 5 3 )
TiO2(110)NaCl KBr . KPFM
meV LCPD
. KPFM ,
.
KPFM
/.
KPFM
. 2009 , Gross 111
qPlus KPFM,
, ,
.
, NaCl(2 ML)/Cu(111)
( Au Ag )
, Au- Au0 Ag+ Ag0.
f(V),
LCPD, ,
LCPD ,
. 2012 12 LCPD
(naphthalocyanine)
112 . 7(a)
LCPD . 7(b, c)
LCPD ,

1380

Acta Phys. -Chim. Sin. 2013

Vol.29

insula

ting fi
lm

condu

cing s

ubstra
te

7 LCPD 12
Fig.7 LCPD images of the tautomerization switching of naphthalocyanine12
(a) schematic illustration of the LCPD imaging and measurement principle. The frequency shift as a function of the sample bias voltage is recorded at
each grid position (inset, red circles). The maximum of the fitted parabola (inset, solid black line) yields CPD for that position. (b, c) LCPD images of
naphthalocyanine on NaCl(2 ML)/Cu(111) before and after switching the tautomerization state of the molecule, respectively. (d) LCPD images of a
naphthalocyanine molecule recorded with a CO-terminated tip. (e) DFT-calculated z-component of the electric field above a free naphthalocyanine
molecule at a distance d=0.3 nm from the molecular plane. The DFT-calculated atomic positions are overlaid in the upper halves of (b)-(e).
Carbon, hydrogen, and nitrogen atoms are in grey, white, and blue, respectively.

LCPD
LCPD. CO LCPD
( 7(d)). , LCPD
( 7(d, e)).
,
,
, ,

.
Leoni 113 STM KPFM
. STM
NaCl(2 ML)/Cu(111) bis-dibenzoylmethanato-copper (Cu(dbm)2)
, KPFM
,
. 114
.
Heyde 115 STM/AFM
SPM
. 116 STS Ag(100)
MgO ,
KPFM LCPD.
LCPD , KPFM

. STM AFM
KPFM LCPD
, 117 Ni/Al(110)
F2+.
STM , KPFM (
),
, ,
KPFM .
/
.
,
/. Nikiforov 118
KPFM
. HOPG
.
HOPG , HOPG
, HOPG ,
HOPG CPD -50 mV, ,
, /
. Ichii 119
Au(111) CuPc LCPD
. LCPD /
. Glatzel110 (truxene) KBr

No.7

. truxene
LCPD . Truxene LCPD 200
mV, .
LCPD ,
. LCPD
,
.

.
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