Ion and electron beam nanofabrication of the which-way double-slit

experiment in a transmission electron microscope

Stefano Frabboni, Gian Carlo Gazzadi, and Giulio Pozzi

Citation: Appl. Phys. Lett. 97, 263101 (2010); doi: 10.1063/1.3529947

View online: http://dx.doi.org/10.1063/1.3529947
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Published by the American Institute of Physics.

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 APPLIED PHYSICS LETTERS 97, 263101 共2010兲

Ion and electron beam nanofabrication of the which-way double-slit

experiment in a transmission electron microscope
Stefano Frabboni,1,a兲 Gian Carlo Gazzadi,2 and Giulio Pozzi3
1
Department of Physics, University of Modena and Reggio Emilia and CNR-Institute of Nanoscience-S3, via
G. Campi 213/a, 41100 Modena, Italy
2
CNR-Institute of Nanoscience-S3, via G. Campi 213/a, 41100 Modena, Italy
3
Department of Physics, University of Bologna, viale B. Pichat 6/2, 40127 Bologna, Italy
共Received 11 November 2010; accepted 2 December 2010; published online 28 December 2010兲
We have realized a which-way experiment closely resembling the original Feynman’s proposal
exploiting focused ion beam milling to prepare two nanoslits and electron beam induced deposition
to grow, selectively over one of them, electron transparent layers of low atomic number amorphous
material to realize a which-way detector for high energy electrons. By carrying out the experiment
in an electron microscope equipped with an energy filter, we show that the inelastic scattering of
electron transmitted through amorphous layers of different thicknesses provides the control of the
dissipative interaction process responsible for the localization phenomena which cancels out the
interference effects. © 2010 American Institute of Physics. 关doi:10.1063/1.3529947兴

Probably the most famous thought or “gedanken” ex-
periment is the one proposed by Feynman concerning the
double-slit experiment with single electrons “which contain
all the mysteries of quantum mechanics.”1 In its original for-
mulation the experiment consists of three parts. The first con-
cerns the observation of interference fringes in a double-slit
setup,2,3 highlighting the particle versus wave behavior when
it is carried out at low intensity, i.e., with single electrons in
the apparatus. This part was carried out not with slits, but
using an electron biprism4 as wave-front division interferom-
eter and detectors able to register the arrival of single
electrons.5,6 The second part discusses the comparison of the
electron distributions when one of the slits is closed,7 and its
analysis leads to the idea of probability amplitude. The third
part of this experiment, subsequently renamed which-way
共or which-path兲, aims at demonstrating that, when the setup
is modified so as to obtain the information through which slit
the electron passes, then the interference phenomena disap-
pear 共complementarity principle兲. Experiments of this kind
were realized in neutron8 atomic or molecular9 interference
setups, as well as with electrons in semiconductor
systems.10,11 With free electrons, some biprism based experi-
ments in inelastic electron holography12 and electron
interferometry13 can be considered a variant.
In this letter we show how this experiment can be carried
out, by using a conventional transmission electron micro-
scope 共TEM兲, in a form which is directly inspired to the
original Feynman proposal, by exploiting focused ion beam
共FIB兲 milling to prepare two nanoslits and electron beam
induced deposition to grow, selectively over one of them,
layers of low atomic number amorphous material to realize a
which-way detector for high energy electrons. The inelastic
scattering events within the amorphous layer, monitored by
electron energy loss spectroscopy 共EELS兲,14 provide the con-
trol of the dissipative interaction process responsible for the
localization mechanism of the electron path.12
In Fig. 1 the proposed which-way experiment is de-
scribed in detail. The incident electron wave function is as-
a兲
Electronic mail: stefano.frabboni@unimore.it.
sumed to be a plane wave, which after the interaction with
the open slits propagates as two interfering cylindrical waves
关Fig. 1共a兲兴. The experimental EELS spectrum of the electrons
transmitted by a single open slit is reported in Fig. 1共b兲. It
shows the intrinsic energy spread of the thermoionic electron
beam which is about 1.5 eV.
When one of the slits is covered by a relatively thick
amorphous layer of low atomic number material 关Fig. 1共c兲兴,
the probability of inelastic scattering becomes much greater
than the probability of elastic scattering, as shown by EELS
spectrum of the electrons transmitted by the covered slit re-
ported in Fig. 1共d兲.
The electron suffering an inelastic scattering event is
therefore necessarily localized at the covered slit, and can be
thought as a spherical wave propagating after the slit, having
no longer any phase correlation with the cylindrical wave of
elastically scattered electron.
Filtering-out those incoherent inelastically scattered
electrons by inserting a slit at the energy dispersion plane
around the zero loss peak, marked by the black frame in
Figs. 1共d兲 and 1共f兲, will produce an imbalance between the
elastic probability amplitudes transmitted by the two slits.
The consequent reduction of interference fringes contrast,
FIG. 1. 共Color online兲 Schematic setup and EELS spectra in our double-slit
which-way experiment. The black rectangular frame around the zero loss
peaks shows the energy window adopted to filter-out inelastic electrons, so
producing which-way localization.

0003-6951/2010/97共26兲/263101/3/$30.00 97, 263101-1 © 2010 American Institute of Physics

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263101-2 Frabboni, Gazzadi, and Pozzi
expected in the Fraunhofer diffraction pattern recorded on
the final detector 共not reported in Fig. 1兲, gives the which-
way localization with a probability related to the thickness of
the amorphous layer deposited over the slit.
When, as in the case of Fig. 1共c兲, the thickness of the
layer is greater than four inelastic mean free paths, an almost
negligible fraction of the transmitted electrons is observed
inside the zero loss peak of the EELS spectrum of Fig. 1共d兲,
thus interference effects are expected to be canceled out al-
most completely.
When the thickness of the amorphous layer is decreased
as in Fig. 1共e兲, the EELS spectrum of the electrons transmit-
ted by the covered slit 关Fig. 1共f兲兴 shows an increase of elastic
scattering probability at expense of the inelastic one; the
elastically scattered electrons can be described again by two
cylindrical waves with different amplitude and intrinsic
phase difference both dependent on the thickness of the
amorphous layer. Interference effects, measured by the con-
trast of interference fringes, are expected to be recovered
although at reduced strength.
We point out that in the present experiment a low atomic
number amorphous material has been chosen for the EBID
nanofabrication step of the which-way detector, in order to
maximize the total intensity transmitted by the covered slit,
since our goal is to control the ratio between coherent and
incoherent fraction of the transmitted electrons by energy
filtering. This is an opposite requirement with respect to our
previous work,7 where, in order to compare single and
double-slit diffraction intensity profiles, the aim of the nano-
fabrication process, achieved by Pt-based EBID deposition,
was to minimize the total intensity transmitted from the cov-
ered slit.
The slits were fabricated by FIB milling a commercial
carbon copper grid coated by flash evaporation with a gold
layer about 250 nm thick. FIB milling was performed with a
dual beam apparatus 共FEI Strata DB235M兲.7 To open the
slits, a 10 pA beam, corresponding to a nominal spot size of
10 nm, was scanned over 100⫻ 1500 nm rectangular pat-
terns, 450 nm spaced, for 5 s each pattern, which results in
slits about 90 nm wide, spaced by 450 and 1540 nm long.
The amorphous layer covering the slits was deposited by
EBID of a tetraethylorthosilicate 共C8H20O4Si兲 gas
precursor15 共chamber pressure P = 5 ⫻ 10−5 mbar兲, using a 15
keV electron beam scanned over rectangular patterns of
200⫻ 1800 nm. Beam dwell time over the pattern was var-
ied between 60 and 720 s to obtain increasing layer thick-
ness. To cover the slits shown in Figs. 2共d兲 and 2共g兲, beam
dwell time was set to 300 and 60 s, respectively. Separation
共450 nm兲 and width 共90 nm兲 have been kept similar to those
adopted in our previous experiment,7 as this geometry allows
us to overlook possible “delocalization” effects of inelasti-
cally scattered electrons, known to be in the 10 nm range.14
The observations were carried out with a TEM JEM 2010,
equipped with a LaB6 source, operating at 200 keV 共de Bro-
glie wavelength 2.51 pm兲 and a Gatan imaging filter
共GIF®200兲. This electro-optical device allows the recording
of EELS spectra and, by means of the energy selecting slit,
typically ⫾5 eV wide, it enables the separation in the image
and in the Fraunhofer diffraction pattern of elastically scat-
tered electrons from inelastically scattered ones.14 It is thus
possible to assess their relative contribution to both images.
Owing to the small deflections associated with the separation
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Appl. Phys. Lett. 97, 263101 共2010兲
FIG. 2. 共Color online兲 SEM images, TEM elastic images, and their intensity
line scans of two open slits 共a, b, c兲, with one slit completely covered 共d, e,
f兲, and partly covered 共g, h, i兲.
of the slits, of the order of 5 ⫻ 10−6 rad, the Fraunhofer dif-
fraction patterns were observed in the so called low-angle
diffraction mode such as in our previous work.7 Diffraction
patterns, images, and EELS spectra were recorded on the
same Gatan 794, 1024⫻ 1024 pixels, Peltier-cooled charge-
coupled device camera located beyond the energy dispersive
plane.
Figure 2 shows the scanning electron microscope 共SEM兲
images 共left column兲, the TEM images 共central column兲
formed with elastic electrons 共hereafter elastic image兲, and
the corresponding intensity line scans across the two slits
共right column兲, without 共a, b, c兲, and with 共d, e, f兲 共g, h, i兲 a
deposited layer of decreasing thickness covering one of
them. The ratio between the elastic transmitted intensities of
the slits, which are related to the mean thickness of the amor-
phous layer deposited over the covered slit by the exponen-
tial factor exp共−t / ␭i兲, where ␭i is the inelastic mean free path
and t is the thickness,14 is 1 for 共c兲, no layer, 0.013 for the
thicker 共t ⬃ 550 nm兲 layer 共f兲, and 0.09 for the thinner 共t
⬃ 390 nm兲 one 共i兲, respectively. The corresponding ratios
measured from images recorded without the insertion of the
energy selecting aperture, not reported here, are 1, ⬃0.77,
and ⬃0.85, respectively, thus confirming that the electron is
transmitted through and not absorbed by the covered slit.
Figure 3 reports the results obtained by the TEM Fraun-
hofer observations with elastic electrons by switching the
microscope in low angle diffraction mode: the upper parts
show the Fraunhofer images, and the lower their intensity
line scans. The images have been taken with acquisition
times ranging between 120 and 300 s due to low intensity of
the partially coherent electron beam produced by the ther-
moionic LaB6 electron source of our TEM. The low intensity
of the electron beam yields a negligible probability of simul-
taneous presence of more than one electron along the path
from the source to the detector,5,6 a fundamental requirement
or the realization of the Feynman ideal experiment with
single electrons.1,5,6
Figure 3共a兲 shows, as reference, the results obtained with
the open slits. It can be seen that interference fringes are
present in the Fraunhofer image, whose intensity is modu-
lated by the single slit diffraction and by the partial coher-
263101-3 Frabboni, Gazzadi, and Pozzi
FIG. 3. 共Color online兲 Fraunhofer low angle diffraction images 共a, c, e兲 and
corresponding intensity line scans, averaged over five pixels, 共b, d, f兲 of the
open slits 共a, b兲, with one slit completely covered 共c, d兲 and partly covered
共e, f兲 of Fig. 2.
ence of the beam, Fig. 3共b兲. In the case of one slit covered
with the thicker layer, Fig. 3共c兲, the interference phenomena
cancel out almost completely and only the diffraction enve-
lope of the uncovered slit remains, Fig. 3共d兲. The intensity
line scan of the elastic electrons, reported in Fig. 2共f兲, shows
that the total elastic intensity through the covered slits drops
to 0.013 times the value of the uncovered slit, indicating that
only a negligible fraction of incident electrons is transmitted
after elastic scattering with the atoms of the amorphous ma-
terials of the covered slit and participate to the formation of
elastic Fraunhofer image. On the other hand the EELS spec-
trum of the total electron transmittance of the covered slit,
reported in Fig. 1共d兲, shows that inelastically scattered elec-
trons are transmitted through the amorphous layer, thus con-
firming that they are localized by inelastic interaction in the
covered slits and therefore not able to contribute to the inter-
ference pattern. When the thickness of the amorphous layer
covering the slit is reduced, to determine an increase of elas-
tic scattering probability at expense of the inelastic one, 关see
Fig. 2共i兲 and EELS spectrum of Fig. 1共f兲兴, the elastic Fraun-
hofer image shows again a faint system of interference
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Appl. Phys. Lett. 97, 263101 共2010兲
fringes, Fig. 3共e兲, clearly visible in the intensity line scan
reported in Fig. 3共f兲. Another interesting feature of Fig. 3共f兲
is the slight asymmetry of the fringe system, which is the
signature of the fact that not only the intensity, but also the
phase of the transmitted electron wave, is affected by the
layer through the mean inner potential.16
Finally it must be noticed that Fraunhofer images very
similar to those reported in Fig. 3 have been obtained with-
out the insertion of the energy filtering aperture along the
electron paths, thus allowing both elastic and inelastic elec-
trons transmitted by the sample to reach the diffraction de-
tector with a total angular acceptance of about 10−4 rad. The
close similarity between those images clearly support the
conclusion that only elastically scattered electrons participate
to the interference phenomena, whereas the inelastic elec-
trons, although transmitted, result localized by scattering and
do not participate to the interference process. According to
Heisenberg’s uncertainty principle, localization of 200 keV
electrons by means of inelastic scattering with most probable
energy loss of about 20 eV is associated to an angular delo-
calization greater than 5 ⫻ 10−5 rad, one order of magnitude
greater than the angular spacing of the interference maxima.
This means that inelastically scattered electrons, instead to
be focused into diffraction spots are widespread all over the
observation plane.
In conclusion, an experimental setup which closely re-
sembles the ideal Feynman which-way experiment has been
realized and the results discussed. Inelastic scattering of high
energy electron through amorphous layers of different thick-
nesses, deposited over the slits, provides the controlled dis-
sipative process of interaction responsible for the electron
localization.
The authors gratefully acknowledge useful discussions
with Professors M. Beleggia, G. F. Missiroli, and N. Sem-
prini Cesari as well as the skilful technical assistance of S.
Patuelli. They are also grateful to Professor E. Molinari for
encouraging comments.
1
R. P. Feynman, R. B. Leighton, and M. Sands, The Feynman Lectures on
Physics 共Addison-Wesley, Reading, 1966兲, Vol. 3, Chap. 1.
2
C. Jönsson, Z. Phys. 161, 454 共1961兲; Am. J. Phys. 42, 4 共1974兲.
3
S. Frabboni, G. C. Gazzadi, and G. Pozzi, Am. J. Phys. 75, 1053 共2007兲.
4
G. Möllenstedt and H. Düker, Z. Phys. A: Hadrons Nucl. 145, 377 共1956兲.
5
P. G. Merli, G. F. Missiroli, and G. Pozzi, Am. J. Phys. 44, 306 共1976兲.
6
A. Tonomura, J. Endo, T. Matsuda, T. Kawasaki, and H. Ezawa, Am. J.
Phys. 57, 117 共1989兲.
7
S. Frabboni, G. C. Gazzadi, and G. Pozzi, Appl. Phys. Lett. 93, 073108
共2008兲.
8
J. Summhammer, H. Rauch, and D. Tuppinger, Phys. Rev. A 36, 4447
共1987兲.
9
A. D. Cronin, J. Schmiedmayer, and D. E. Pritchard, Rev. Mod. Phys. 81,
1051 共2009兲.
10
I. L. Aleiner, N. S. Wingreen, and Y. Meir, Phys. Rev. Lett. 79, 3740
共1997兲.
11
E. Buks, R. Schuster, M. Heiblum, D. Mahalu, and V. Umansky, Nature
共London兲 391, 871 共1998兲.
12
P. L. Potapov, H. Lichte, J. Verbeeck, and D. van Dyck, Ultramicroscopy
106, 1012 共2006兲.
13
P. Sonnentag and F. Hasselbach, Phys. Rev. Lett. 98, 200402 共2007兲.
14
R. F. Egerton, Rep. Prog. Phys. 72, 016502 共2009兲.
15
S. Frabboni, G. C. Gazzadi, and A. Spessot, Appl. Phys. Lett. 89, 113108
共2006兲.
16
L. Reimer, Transmission Electron Microscopy: Physics of Image Forma-
tion and Microanalysis, 2nd ed. 共Springer, Berlin, 1989兲, Vol. 36.