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Quantum theoretical approach to a near-®eld optical system

Quantum theoretical approach to a near-®eld optical system

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Quantum theoretical approach to a near-®eld optical system

K. KOBAYASHI* & M. OHTSU*²
*ERATO Ohtsu Localized Photon Project, Japan Science and Technology Corporation, 687-1
Tsuruma, Machida, Tokyo 194-0004, Japan
²Interdisciplinary Graduate School of Science and Engineering, Tokyo Institute of Technology,
4259 Nagatsuta-cho, Midori, Yokohama, Kanagawa 226-8502, Japan
Key words. Probe tip±sample interaction, projection operators, quantum theory,
virtual photon model, Yukawa-type interaction.
Summary
The paper proposes a quantum theoretical formulation of
an optical near-®eld system based on the projection-
operator method. Special attention is paid to a nanometric
probe tip±quantum mechanical sample system, whose
interactions are essential for describing such phenomena
as atom guidance and manipulation, or local excitation of a
single quantum dot. The relationship to the virtual photon
model ± an intuitive model ± is discussed, and the latter's
empirical assumption of the Yukawa-type interaction
between probe and sample is justi®ed theoretically. Several
applications of the theory are brie¯y outlined.
1. Introduction
Recent experimental study has revealed the possibility of
local excitation of a sample by means of an optical near ®eld
beyond the diffraction limit, as well as high-resolution imaging.
The ¯uorescence lifetime of a single molecule, for example, has
been measured and its quenching behaviour has been discussed
in terms of the sample±probe distance and the aperture size
of the probe (Trautmann & Ambrose, 1997).
Photoluminescence spectroscopy of a single quantum dot
at low temperature has been also investigated to obtain
information about electronic-level structures, the spin±
relaxation mechanism, and the switching effect (Flack et al.,
1996; Matsumoto et al., 1998; Saiki & Ohtsu, 1998; Saiki
et al., 1998; Toda et al., 1998). Such experimental results
exemplify the need for quantum theoretical treatment of
optical near-®eld problems. Several authors, in fact, have
semi-classically analysed near-®eld spectroscopic problems
(Girard et al., 1995; Cho et al., 1996; Kobayashi, 1998),
formulating electronic structures in terms of quantum
mechanics and optical near ®elds in terms of classical
electromagnetics.
An atom, as a small sample, may be considered as an
ultimate candidate for nano/atom photonics. To this end,
atom re¯ection by a near ®eld induced over a prism surface
has been experimentally veri®ed (Balykin et al., 1988;
Aminoff et al., 1993; Landragin et al., 1996), and atoms
have been guided through a micrometre-sized hollow ®bre by
means of blue-detuned optical near ®eld (Ito et al., 1996).
Atomic deposition with nanometric precision using very-
low-energy atom de¯ection or manipulation has also
been proposed (Ito et al., 1997; Ito et al., 1998), and
experimental veri®cation is expected after technical chal-
lenges such as ®bre probe improvement (Mononobe et al.,
1998; Yatsui et al., 1998) and manipulation and detection
schemes (Hori, 1993; Ohtsu et al., 1993; Klimov & Letokov,
1995; Ito & Ohtsu, 1998).
Atom±substrate interactions via a propagating light ®eld,
being a more basic physics issue, have been investigated
both theoretically and experimentally. Classical antenna
theory can predict some kinds of atomic behaviour, but the
existence of pure cavity quantum electrodynamic (QED)
effects is well known (Hinds, 1994). The energy shift in the
ground state of an atom is one example in which quantum
theory is essential for explaining the phenomenon.
From the above observation it is natural to quantum-
theoretically formulate a near-®eld optical system consist-
ing of an atom or molecule and an optical near-®eld probe.
Such a formulation would be preferable if it could be related
to an intuitive model giving clear insights into the near-®eld
optical system as well as scanning image characteristics. It
may be possible to use a semi-classical approach in order to
predict the quantum-mechanical states of matter, but we
will employ a full quantum-mechanical approach, for the
following reasons. Experimental progress shows that an
optical near-®eld probe tip reaches 1±50nm in diameter
(Ohtsu, 1995), and it is not clear to deal with such a
microscopic tip and an atom or a molecule as two isolated
systems when they are coupled via a macroscopic bath
system (incident light, substrate, and/or ®bre probe). Under
Journal of Microscopy, Vol. 194, Pt 2/3, May/June 1999, pp. 249±254.
Received 6 December 1998; accepted 9 February 1999
q 1999 The Royal Microscopical Society 249
Correspondence to: K. Kobayashi. Tel: ÷ 81 42 788 6036; fax: ÷ 81 42 788
6031; e-mail: kkoba@ohtsu.jst.go.jp
this condition, the states of the total system should be
different from those of the two isolated systems, and it is
very important to consistently handle the interaction
between the two from the quantum-mechanical viewpoint,
although the existing theoretical approaches have neglected
to do so from the outset. Moreover there have been no attempts
to give any intuitive model from microscopic approaches.
We pay special attention to a nanometric probe tip±
quantum mechanical sample system whose interactions are
essential for describing such phenomena as those in atom
de¯ection or manipulation experiments using optical near
®elds. The purpose of this paper is to propose a uni®ed and
systematic formulation of optical near-®eld problems in order
to discuss the quantum-mechanical observables of such a
system. We will then discuss the relationship to the virtual
photon model (Hori, 1993; Kobayashi & Ohtsu, 1998; Ohtsu
& Hori, 1998) ± an intuitive model based on experimental
results ± which assumes the Yukawa-type interaction between
a probe tip and sample as an elementary process. Taking
advantage of the characteristics of the virtual photon model,
we will then describe a potential application of the theory.
The paper is organized as follows. The next section
outlines the method on which our approach is based. In
Section 3, Yukawa-type interaction between sample and
probe tip, which was empirically assumed in the virtual
photon model, is derived as an effective sample±probe
interaction. One example of a case in which the virtual
photon model can offer physical insight is discussed in
Section 4, and we also give an example of the application of
our formulation on the basis of the virtual photon model.
Finally, Section 5 offers some concluding remarks.
2. Method of projection operators
We will employ the method of projection operators and
discuss the near-®eld optical system, since we have to
describe the difference between coupled and isolated
quantum-mechanical states in a uni®ed and systematic
way. It is very appropriate to extract an arbitrary number of
degrees of freedom from the many degrees of freedom of the
system, and to renormalize the effects of the other degrees of
freedom. Even if we are, for example, not able to obtain all of
the exact states for the total system, we can derive the exact
effective interaction in terms of a few states for the isolated
system, as will be shown below (see Eqs.(10±11)).
First, let us brie¯y outline the method of static projection
operators (Hyuga & Ohtsubo, 1978; Kobayashi & Kohmura,
1984; Fulde, 1995). Let the total Hamiltonian H
Ã
for a near-
®eld optical system such as a near-®eld optical microscope
and spectroscope be
Ã
H =
Ã
H
0
÷
Ã
V; (1)
Ã
H
0
=
Ã
H
A
÷
Ã
H
B
÷
Ã
H
bath
; (2)
where the Hamiltonians H
Ã
A
and H
Ã
B
describe the states of the
probe tip and sample, respectively, as isolated quantum-
mechanical systems. The Hamiltonian H
Ã
bath
represents the
states of light and in®nite matter (substrate or ®bre probe),
while V
Ã
denotes the interaction between the system A (or B)
and the bath system (Fig. 1). Steady states of H
Ã
and H
Ã
0
are
assumed in the following discussion, and the eigenvalues
and eigenstates of H
Ã
are written as E
l
and [W
l
), respectively,
i.e.
Ã
H[W
l
) = (
Ã
H
0
÷
Ã
V)[W
l
) = E
l
[W
l
): (3)
De®ning the static projection operators P and Q=1÷P in
the usual manner as
[W
(1)
l
) = P[W
l
); [W
(2)
l
) = Q[W
l
); (4)
P
2
= P; PQ = QP = 0; (5)
we divide the eigenstates [W
l
) into two groups, [W
( 1)
l
) in P-
space and [W
( 2)
l
) in Q-space. It is possible to formally express
Q[W
( 2)
l
) by P[W
( 1)
l
) as
Q[W
(2)
l
) = J(E
l
÷
Ã
H
0
)
÷1
Q
Ã
VP[W
(1)
l
); (6)
J =
_
1 ÷ (E
l
÷
Ã
H
0
)
÷1
Q
Ã
V
¸
÷1
; (7)
and the eigenstates [W
l
) for the total Hamiltonian can then
be expressed in terms of the eigenstates in P-space as
[W
l
) = (P ÷ Q)[W
l
) = JP[W
(1)
l
): (8)
Since both of the states satisfy the normalization condition,
we can rewrite this as
[W
l
) = JP(PJ
²
JP)
÷1=2
[W
(1)
l
): (9)
We thus obtain an effective operator O
Ã
eff
in the P-space,
which is equivalent to an arbitrary operator O
Ã
in the full
space, corresponding to physical observables (Kobayashi &
Kohmura, 1984):
¸W
m
[
Ã
O[W
l
) = ¸W
(1)
m
[
Ã
O
eff
[W
(1)
l
); (10)
Ã
O
eff
= (PJ
²
JP)
÷1=2
(PJ
²
Ã
OJP) (PJ
²
JP)
÷1=2
: (11)
From the above Eqs (10±11), it follows that relevant
quantities such as the probe tip±sample interaction and
transition dipole moments can be exactly expressed by using
a small number of bases in P-space after renormalizing the
effects from Q-space. This is one of the advantages of the
method, and is desirable from the computational viewpoint.
3. Effective sample±probe interaction and virtual photon
model
On the basis of the above formalism, we now discuss the
virtual photon model (Hori, 1993; Kobayashi & Ohtsu,
1998; Ohtsu & Hori, 1998) ± a unique and intuitive
model ± in particular, its empirical assumption regarding
250 K. KOBAYASHI AND M. OHTSU
q 1999 The Royal Microscopical Society, Journal of Microscopy, 194, 249±254
the probe±sample interaction in a fundamental process. The
model assumes virtual photons with nonzero mass (m
eff
)
tunnelling between nanometric objects, similar to electron
tunnelling in scanning tunnelling microscopy (STM). This
means that the Yukawa-type interaction is responsible for
the interaction between a nanometric probe tip and sample.
In other words, the Yukawa potential (e
÷m
eff
t
/t) is assumed
to be generated near the nanometric object (source) as a
result of the interaction between incident light and the
object, for both of the illumination and collection modes in
near-®eld optical microscopy and spectroscopy. Owing to the
assumption, it can describe optical near ®elds localized on
the material surface without solving the Maxwell equation,
and a novel scheme for manipulating atoms by using the
optical near ®eld was successfully proposed and analysed
(Hori, 1993; Ohtsu et al., 1993).
Let us now adopt more speci®c Hamiltonians as
components of H
Ã
0
in order to derive an explicit form of
the effective sample±probe interaction. First we choose a
Hamiltonian for H
Ã
a
(a=A, B),
Ã
H
a
=

n
E
n
(a)Ã e
²
na
à c
na;
(12)
E
n
(a) =
"
2
k
2
a
2m
c
=
"
2
2m
e
np
a
_ _
2
or
"
2
2m
e
np
b
_ _
2
; (13)
where the creation and annihilation operators are denoted
as c
Ã
²
na
and c
Ã
na
, and the relevant energy levels are designated
as E
n
(a), and electric dipole transitions between those levels
are allowed. Note that this Hamiltonian corresponds to one
in which electrons with effective mass m
e
and wave number
k
a
are con®ned in an in®nite well potential of size a(b). The
ground and excited states will be designated as [A), [A*),
[B), [B*), for later use.
Next, let us describe H
Ã
bath
in terms of excitons (B
Ã
²
, B
Ã
),
photons (a
Ã
²
, a
Ã
), and their interactions. Excitons with
energy "Q represent an in®nite crystal lattice with
site number j. Photons with a wave vector k~÷G~and energy
"q interact with the excitons as ÷m
Ã
~
j
´D
Ã
~ (r ~
j
) in a multipolar
QED Hamiltonian (Craig & Thirunamachandran, 1984),
where m
Ã
~and D
Ã
~(r ~
j
) are the dipole operator of matter and the
displacement ®eld operator at site j, respectively. As is well
known (Hop®eld, 1958; Knoester & Mukamel, 1989;
Juzeliunas & Andrews, 1994), this Hamiltonian can be
diagonalized in terms of exciton-polariton modes (energy
"q
k~n
, creation/annihilation operator y
²
k~v
, y
Ã
k~n
as
Ã
H
bath
=

j

3
i=1
"Q
Ã
B
²
ji
Ã
B
ji
÷

~
k;
~
G

2
l=1
"q
~

~
C
à a
²
~

~
G;l
à a
~

~
G;l
÷

i
Ã
~ m
j
´
Ã
~
D(~r
j
) (14)
=

~
k;n
"q
~
kn
Ã
y
²
~
kn
Ã
y
~
kn
: (15)
Here the indices i and l label the three Cartesian
axes and the transverse polarization of light, respectively.
The k~ summation extends over the ®rst Brillouin zone,
and G~ runs over the reciprocal lattice. The summation of u
runs over all branches of exciton-polaritons. We will use the
ground state of H
Ã
bath
, [0) as one component of the P-space.
It follows from Eq. (15) that photons and in®nite matter
may be a collection of harmonic oscillators. In this
representation, a near-®eld optical probe tip interacts with
a nanometric sample via exciton-polariton mediation as
q 1999 The Royal Microscopical Society, Journal of Microscopy, 194, 249±254
Fig. 1. Schematic illustration of how to compose a total Hamiltonian
H
Ã
for a near-®eld optical system from three components, H
Ã
A
, H
Ã
B
,
and H
Ã
bath
. (a) The states of the probe tip, the sample, and the
bath system, as each isolated system, are described by the Hamilto-
nian H
Ã
A
, H
Ã
B
, and H
Ã
bath
, respectively. Depending on the sample, H
Ã
B
may contain the centre of mass motion as well as internal degrees
of freedom. Atom de¯ection system by the optical near ®eld
described by the total Hamiltonian H
Ã
as an example. Incident
and de¯ected atoms have the momenta "k~and "k~
/
, respectively.
QUANTUM THEORETI CAL APPROACH TO NEAR- FI ELD OPTI CAL SYSTEM 251
follows:
Ã
V = ÷

B
a=A
Ã
~ m
a
´
Ã
~
D(~r
a
)
= ÷

B
a=A

~
kn
i"

V
0
_

2p
"
_
(K
/
~
kn
(a)
Ã
y
~
kn
÷ K
/+
~
kn
(a)
Ã
y
²
~
kn
)(
Ã
b
²
a
÷
Ã
b
a
);
(16)
where K
/
k~n
(a) and K
/
*
k~n
(a) are the coupling coef®cients
between the probe (sample) and exciton-polaritons, and b
Ã
²
a
and b
Ã
a
are the creation and annihilation operators leading
to electric dipole transitions of the sample±probe system,
relating to Eq. (12). It is worth reminding ourselves that
there is no direct interaction between sample and probe tip
in this Hamiltonian.
As explained in the previous section, one can exactly
express the relevant interaction by using a small number of
bases in the P-space, after renormalizing the effects from the
Q-space. We then choose a combination of the ®ve states,
[A), [A*), [B), [B*) and [0), as the P-space bases illustrated in
Fig. 2, and set [W~
(1)
l
) = [A) [B*) [0), [W
(1)
m
) = [A*) [B) [0), in
order to evaluate the effective sample±probe interaction V
eff
(AB) from Eqs (10) and (11):
V
eff
(AB) = W
(1)
m
[
Ã
V
eff
[W
(1)
l
¸ _
= W
(1)
m
[(PJ
²
JP)
÷1=2
(PJ
²
Ã
VJP) (PJ
²
JP)
÷1=2
[W
(1)
l
_ _
(17)
Noting that the operator J satis®es the equation
[ J;
Ã
H
0
]P = (E ÷
Ã
H
0
)JP ÷ J(E ÷
Ã
H
0
)P
=
Ã
VJP ÷ JP
Ã
VJP; (18)
let us expand J as J =P÷S
¥
n=1
g
(n)
J
(n)
, and obtain pertur-
bative solutions of J. We can then determine V
eff
(AB)
perturbatively in the order of V
Ã
. Since there are no
contributions in the lowest order of V
Ã
because PV
Ã
P=0,
the nonzero contributions to V
eff
(AB) come from the second
order of V
Ã
as
V
eff
(AB) = ¸A
+
[¸B[¸0[
_
P
Ã
VQ(E
0
p
÷ E
0
Q
)
÷1
Ã
VP
÷ P
Ã
V(E
0
p
÷ E
0
Q
)
÷1
Q
Ã
VP
¸
[A)[B
+
)[0) (19)
=
4p
(2p)
3

n
_
d
3
k
K
/
~
kn
(A)K
/+
~
kn
(B)
q
~
kn
÷ Q
0
(B)
÷
K
/
~
kn
(B)K
/+
~
kn
(A)
q
~
kn
÷Q
0
(A)
_ _
:
(20)
Here the summation of k~ is replaced by integrating k~, and
H
Ã
0
in the denominators with respect to the corresponding
eigenvalues. The excitation energies, "Q
0
(A) and "Q
0
(B),
are
"Q
0
(A) =
3"
2
2m
e
p
a
_ _
2
; "Q
0
(B) =
3"
2
2m
e
p
b
_ _
2
; (21)
from Eq. (13). We can similarly show how ¸W
( 1)
l
[V
Ã
eff
[W
(1)
m
)
contribute to the effective sample±probe interaction
V
eff
(BA).
On the basis of the dispersion relation of an exciton-
polariton (effective mass: m
p
, one of the solutions of the
dispersion relation: q
k
) obtained from Eq. (15), we make the
following assumptions, which would be appropriate for
actual near-®eld experiments:
(i) q
~
kn
= q
k
÷
"
2m
p
k
2
,
"
2m
p
k
2
; (q
k
< Q
0
);
(ii) K
/
~
kn
,const ´ exp (i
~
k´~r):
De®ning the ratio g =(3m
p
/m
e
)
1/2
for exciton-polaritons
and electrons in the probe tip (sample), we apply these
assumptions to Eq. (20), and obtain the explicit function
form of
V
eff
(AB) ÷ V
eff
(BA) ~
exp[(igpt)=b]
t
÷
exp[÷(gpt)=a]
t
÷
exp[(igpt)=a]
t
÷
exp[÷(gpt)=b]
t
;
t = [~t
A
÷ ~t
B
[: (22)
This gives the effective sample±probe interaction derived
from microscopic consideration, and the second and fourth
terms are the Yukawa function, which was empirically
assumed in the virtual photon model. The formula also
shows that optical near ®eld is effectively localized near the
sample±probe system, and that the decay length is
proportional to the inverse of the probe (sample) size and
consistent with the experimental results (Saiki et al., 1996).
In addition, we can infer the so-called resonance condition
that a similar size gives maximum coupling between sample
and probe tip, as can be determined by a simple estimation
based on the static dipole model.
Fig. 2. P- and Q-space spanned by bases each of which corresponds
to an eigenstate of H
Ã
A
, H
Ã
B
, and H
Ã
bath
. The P-space is depicted by
hatching.
252 K. KOBAYASHI AND M. OHTSU
q 1999 The Royal Microscopical Society, Journal of Microscopy, 194, 249±254
4. Practical implications of the virtual photon model and
application of our formulation
Since the empirical assumption of the virtual photon model
was justi®ed on the basis of microscopic theory in the
previous section, we can take advantage of the character-
istics of the model to develop an application of our
formulation. We have, so far, emphasized the quantum-
mechanical aspects of the optical near-®eld systems. The
model also predicts the fundamental performance of near-
®eld optical microscopy much faster than the conventional
approach in computation time, that is, the intensity
distribution in the near-®eld region of a subwavelength
metallic circular aperture irradiated by the propagating
light. The resolution of the microscope was also clearly
explained by the model. In addition, we can easily handle
more realistic probe±sample systems, and discuss the
dependence of detected signals on the probe shape, or on
the taper angle v (see Fig. 3). Let the probe be a set of
dielectric spheres of different diameters that approximates a
conical shape. From Eq. (22), the Yukawa potential is
generated between two arbitrary points on the surfaces of
the probe sphere p
i
and sample sphere s
j
. Thus pickup signal
I can be written as
I ~

probe
i

sample
j
_
dj
dr
1
_
pi
dt
2
V
eff
(t
12
)
¸
¸
¸
¸
¸
¸
¸
¸
2
; t
12
= [~t
1
÷ ~t
2
[:
(23)
If the so-called resonance condition is satis®ed, the pickup
signal becomes proportional to exp[±const/sin(v/2)].
Turning to the quantum-mechanical system again, we
discuss the possibility of applying the formulation to atom
de¯ection and manipulation with a sharpened ®bre probe.
These techniques are unique and will be essential for
carrying an atom to a desired point on a substrate with high
spatial accuracy far beyond the diffraction limit. As shown
in Fig. 1, suppose that an incident atom with momentum
"k
~
is de¯ected into momentum "k
~
/
by an optical near ®eld
V
eff
. Then the differential cross-section or angular distribu-
tion of the de¯ected atom is given by
dj
dQ
~
M
2p"
2
~
k
/
_ ¸
¸
¸V
eff
~
k
¸
¸
¸
_
¸
¸
¸
¸
¸
¸
¸
¸
2
(24)
where M is the mass of the atom. This kind of evaluation
will be required in the design of atom guidance and
manipulation systems using the optical near ®eld, as well as
in the discussion of basic experimental results.
One implication related to cavity QED problems is that the
transition dipole moment of an atom or a molecule m~
0
is
changed by the in¯uence of the probe tip and optical near
®eld, that is, the difference between the isolated and coupled
states. Perturbative evaluation of Eqs (10) and (11) with
O
Ã
=m
Ã
~ shows that the renormalized transition dipole
moment m~
eff
can be categorized into two classes: one directly
renormalized into m~
0
, and the other not renormalized into m~
0
,
owing to transitions between higher energy levels. It is
interesting to estimate these effects numerically.
5. Conclusion
We have developed a microscopic theory for an optical near-
®eld system, using a quantum-mechanical technique
known as the projection-operator method. It was shown
that the Yukawa-type interaction is involved in effective
probe tip±sample interaction, indicating that the empirical
assumption of the virtual photon model is justi®ed. The key
points are that a probe tip exists near the sample, and that
the electron energies in the probe tip or sample are inversely
proportional to the square of its size, owing to the
q 1999 The Royal Microscopical Society, Journal of Microscopy, 194, 249±254
Fig. 3. Fibre probe tip with taper angle v as a collection of dielectric
spheres with different radii. The i-th and j-th spheres of the probe
and sample are denoted as p
i
and s
j
, respectively. The probe±sample
separation is shown as d.
QUANTUM THEORETI CAL APPROACH TO NEAR- FI ELD OPTI CAL SYSTEM 253
con®nement effect. We discussed a few applications of the
theory, taking advantage of the characteristics of the virtual
photon model. In future, we need to examine in detail the
assumptions and approximations used, as well as what kind
of normal modes should be included for optical near-®eld
problems, in order to make the formulation more rigid.
Acknowledgements
The authors gratefully acknowledge fruitful conversations
with H. Hori of Yamanashi University and H. Ito of Tokyo
Institute of Technology. K.K. also appreciates valuable
suggestions from T. Kohmura of University of Tsukuba.
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254 K. KOBAYASHI AND M. OHTSU
q 1999 The Royal Microscopical Society, Journal of Microscopy, 194, 249±254

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