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Ultramicroscopy 164 (2016) 3145

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Ultramicroscopy
journal homepage: www.elsevier.com/locate/ultramic

Designs for a quantum electron microscope


P. Kruit a,n, R.G. Hobbs b, C-S. Kim b, Y. Yang b, V.R. Manfrinato b, J. Hammer c, S. Thomas c,
P. Weber c, B. Klopfer d, C. Kohstall d, T. Juffmann d, M.A. Kasevich d, P. Hommelhoff c,
K.K. Berggren b
a
Department of Imaging Physics, Delft University of Technology, Lorentzweg 1, 2628CJ Delft, The Netherlands
b
Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States
c
Department of Physics, Friedrich Alexander University Erlangen-Nrnberg (FAU), Staudtstrasse 1, d-91058 Erlangen, Germany
d
Department of Physics, Stanford University, Stanford, California 94305, United States

art ic l e i nf o a b s t r a c t

Article history: One of the astounding consequences of quantum mechanics is that it allows the detection of a target
Received 30 August 2015 using an incident probe, with only a low probability of interaction of the probe and the target. This
Received in revised form quantum weirdness could be applied in the eld of electron microscopy to generate images of beam-
24 February 2016
sensitive specimens with substantially reduced damage to the specimen. A reduction of beam-induced
Accepted 7 March 2016
damage to specimens is especially of great importance if it can enable imaging of biological specimens
Available online 10 March 2016
with atomic resolution. Following a recent suggestion that interaction-free measurements are possible
Keywords: with electrons, we now analyze the difculties of actually building an atomic resolution interaction-free
Transmission electron microscope electron microscope, or quantum electron microscope. A quantum electron microscope would require a
Radiation damage
number of unique components not found in conventional transmission electron microscopes. These
Interaction free measurement
components include a coherent electron beam-splitter or two-state-coupler, and a resonator structure to
Quantum interrogation
Quantum electron microscope allow each electron to interrogate the specimen multiple times, thus supporting high success prob-
abilities for interaction-free detection of the specimen. Different system designs are presented here,
which are based on four different choices of two-state-couplers: a thin crystal, a grating mirror, a
standing light wave and an electro-dynamical pseudopotential. Challenges for the detailed electron
optical design are identied as future directions for development. While it is concluded that it should be
possible to build an atomic resolution quantum electron microscope, we have also identied a number of
hurdles to the development of such a microscope and further theoretical investigations that will be
required to enable a complete interpretation of the images produced by such a microscope.
& 2016 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND
license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

1. Introduction minimum number of electrons Ne is required to form an image


with a specied signal-to-noise ratio. Atomic-scale imaging of
Electron microscopy (EM) has revolutionized our under- biological samples requires a lower bound Ne, which is already
standing of biomolecules, cells and biomaterials, by enabling their more than sufcient to cause damage. Consequently, resolution
analysis through imaging with (near-) atomic-scale resolution [1 must be sacriced in imaging biological specimens to avoid this
3]. Imaging biological systems at such high resolution has fa- damage. Presently, the attainable resolution for single objects by
cilitated the determination of structureproperty correlations that cryo-electron tomography is approximately 510 nm, which pre-
are key to our understanding of the biological function of such vents the production of atomically resolved images [5]. Sub-nan-
systems. However, the high-energy electrons typically used for ometer resolution is regularly achieved in cryo-electron tomo-
graphy through the use of sampling, where thousands of images
electron microscopy are known to cause damage to biological
with different projections of identical macromolecules are ac-
specimens due to inelastic scattering events that break chemical
quired and combined to generate the 3-D structure computa-
bonds (radiolysis), heat the specimen and even dislocate atoms
tionally [68]. However, this approach adds the requirement for
(knock-on damage) [4]. Specimen damage is related to the fact
the acquisition of thousands of images of identical structures as
that image information is shot-noise limited, meaning that a well as signicant computational effort. Moreover, the use of
sampling techniques does not address the fundamental problem,
n
Corresponding author. which is that a route toward atomically resolved images of in-
E-mail address: p.kruit@tudelft.nl (P. Kruit). dividual, isolated biological specimens, with negligible damage to

http://dx.doi.org/10.1016/j.ultramic.2016.03.004
0304-3991/& 2016 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
32 P. Kruit et al. / Ultramicroscopy 164 (2016) 3145

Fig. 1. An interaction-free measurement based on a MachZehnder interferometer. (a) An incident particle (photon/electron) enters the interferometer from the left and is
split into a superposition of two wave-packets by a 50/50 beam-splitter (S1). The two wave-packets then travel through the two arms of the interferometer via mirrors M1
and M2 respectively, before entering a second 50/50 beam-splitter (S2). The interferometer geometry is arranged such that a particle is never detected at detector 2 (D2) due
to deconstructive interference, while a particle is always detected at detector 1 (D1). (b) When an object is placed in the path of the lower arm of the interferometer,
deconstructive interference of the two-wave-packets is prevented, and a particle may now be detected at D2. In that case, the presence of the object has been determined by
detection of a particle that did not interact with the object.

the sample, is still lacking. The approach reported by Kwiat et al. [18] involved increasing the
Recent advances in quantum metrology [9] might allow us to reectivity of the beam-splitters, as ElitzurVaidman had pre-
overcome the resolution limits imposed by shot-noise. Instead, the viously suggested, thus reducing the intensity of the beam direc-
Heisenberg uncertainty principle limits resolution so that the ac- ted at the specimen of interest, while extending the system to
curacy of a measurement scales as 1/Ne, a Ne improvement over interrogate the specimen multiple times within a single mea-
the shot-noise limit. Recently, approaches implementing mea- surement. Kwiat et al. [18] proposed the use of a cavity to enable
surement techniques based on quantum mechanical phenomena the coherent evolution of intensity transfer between the sample
have been proposed that could reduce the electron dose to the and reference beams to achieve higher detection probabilities
specimen in a transmission electron microscope (TEM) [1012]. while simultaneously reducing the intensity at the specimen.
Here, we follow up on another idea rst reported by Elitzur and These higher detection probabilities have been experimentally
Vaidman [13], who proposed that an opaque object may be ob- demonstrated [18,22,23] and subsequently applied to imaging
served by detecting a photon that did not interact with that object systems [24]. These advanced IFM techniques yield a success
[14]. This concept, shown schematically in Fig. 1, uses a Mach probability of one, meaning that a single detected photon will be
Zehnder interferometer to perform an interaction-free measure- sufcient to determine the presence of an object in the path of the
ment (IFM). Here, a fully opaque object in the lower arm of the beam, and that no photon will be absorbed by the object. A par-
interferometer destroys interference in the system, and leads to tially absorbing object would result in a lower success probability
the detection of a photon at the dark output of the interferometer [25] and consequently reduced benet from the IFM approach.
(D2 in Fig. 1). Earlier concepts for such negative result experi- It should also be noted that an optical IFM relies on the su-
ments were proposed separately by Renninger and Dicke [15,16], perposition of a photon in two distinct states, as discussed below.
but the designs considered in our work stem from the Elitzur and It thus differs from other quantum imaging techniques such as
Vaidman scheme. While the experiment proposed by Elitzur and ghost imaging [26,27] or NOON state microscopy [28,29], that rely
Vaidman may achieve a truly interaction-free measurement for an on entanglement of two or more photons. Entanglement of pho-
ideal, fully opaque specimen, any measurement of a partially tons is technologically challenging and entanglement-enhanced
transparent specimen or a quantum system is not likely to fulll measurements often require post-selection of detection events, for
the requirements of an IFM and so we refer to such measurements
which an appropriate entangled state has been prepared. This
more generally here as quantum interrogations [17]. Various rea-
reduces the applicability of such techniques to low-damage mi-
lizations of such quantum interrogations have been achieved with
croscopy. An IFM neither requires entanglement, which has not
photons and shall be discussed later. Here, we show how this idea
yet been demonstrated for free electrons, nor post-selection
could be implemented in an electron microscope, not dissimilar to
and thus offers itself to implementation in low-damage electron
existing scanning transmission electron microscopes, to yield the
microscopy.
structure of a specimen with negligible exposure of the specimen,
The coherent evolution of intensity transfer between the
and thus reduced damage to the specimen. We will refer to such a
sample and reference beams in the scheme described by Kwiat
microscope as a quantum electron microscope (QEM), referring to
et al. may be represented by a quantum mechanical two-level
the essential quantum mechanical aspect of the interrogation
system such as a shallow electronic double well potential (Fig. 2
technique.
(a)). Thus, the scheme proposed by Kwiat et al. may be applicable
Fig. 1 illustrates the IFM scheme proposed by Elitzur and
to electrons as well as photons, as described by Putnam and Yanik
Vaidman [13] based on a MachZehnder interferometer. A probe
[30]. The two lowest energy eigenstates of a double-well potential
particle/wave, in this case a photon, is coherently split into two
are the symmetric state S and the antisymmetric state A , as
beams of equal amplitude by a 50/50 beam-splitter (S1), producing
shown in Fig. 2(a).
a sample beam and a reference beam. The two paths are re-
The state of an electron localized in the left (right) well of the
combined at a second 50/50 beam-splitter (S2) and, if the relative
double-well system can be dened as | reference ( | sample),
path length is chosen correctly, interference means that the pho-
ton will always exit this beam-splitter at the same output port which can be represented as a linear combination of the eigen-
(D1). However, when an object blocks the path of the sample- states: | reference= 1 (| S | A ), | sample= 1 (| S +| A ). The
2 2
beam, a photon can reach the other output port (D2) with a electron starts in the reference well and hence the initial state is
probability of . In this case, the presence of the object was de- the localized state | reference. Since this state is not an Eigenstate,
tected, although there was no interaction between the object and the state of the electron will change with time. According to the
the detected photon. This technique was conceptually extended to dynamics of a two-level system, the state will gradually evolve
success probabilities arbitrarily close to one using an approach back and forth between states | reference and | sample. Speci-
analogous to a discrete form of the quantum Zeno effect [1821]. cally, the electron population will gradually transfer back and forth
P. Kruit et al. / Ultramicroscopy 164 (2016) 3145 33

Fig. 2. (a) Double well potential. The two lowest energy eigenstates of this potential well are the symmetric state labeled S (dashed line) and the antisymmetric state
labeled A . (b) Plots of the probability of nding an electron in the reference and sample rings (see text), which contain the reference and sample wells respectively, as a
function of the number of circulations in those rings. The plots shown are for the case where an opaque object is absent from the sample ring (white pixel), or is present in
the sample ring (black pixel).

the right in Fig. 2(b), analogous to the quantum Zeno effect [19]. As
a result, determining the well/ring occupied by the electron will
reveal whether a transparent or opaque object exists in the path of
the sample ring. A full binary image of the specimen may be ob-
tained pixel-by-pixel, after N circulations, by scanning the sample
ring across the specimen, similar to a scanning electron micro-
scope (SEM) or a scanning transmission electron microscope
(STEM).
Recently, Putnam and Yanik [30] outlined a way to implement
this measurement principle using electrons. Their conceptual ap-
proach is based on using a double-well potential, where con-
tinuous coupling of the electron states is achieved by quantum
mechanical tunneling from one well to the other. They suggest an
implementation of the approach where the double potential well
is created in a ring-shaped hybrid Paul Penning trap for electrons.
A sample could be placed in one of the rings, as shown in Fig. 3.
We shall now consider the issue of damage to the sample
during the imaging procedure. Radiation damage can be shown to
scale with 1/No [25], where No is the number of circulations by the
electron in the ring required to fully tunnel from one ring to the
other i.e. for a complete transition from state | reference to state
| sample. The origin of the relationship between damage and No
may be understood by considering the process of transferring the
electron wavefunction from the | reference state to the | sample as
the transfer of 1/No of the amplitude from the reference beam to
the sample beam during each circulation. When a sample is pre-
sent and interacts with the wavefunction in the sample state, the
damage per circulation is then proportional to the intensity in the
Fig. 3. (a) Continuously coupled electron ring guides proposed by Putnam and
sample ring, that being 1/N2o . Consequently, the total damage after
Yanik. The gure shows an electron wave-packet circulating in the upper ring and
No circulations will be proportional to 1/ No . Thus, by making No
the inset shows Ueff the double-well potential that denes the electron rings la-
beled according to the states that occupy each, which are labeled |T and |B in the arbitrarily large, a quantum measurement can in principle be
gure, but shall be referred to as | reference and | sample respectively in this text. achieved with vanishing damage probability.
(b) A schematic description of the imaging mechanism. The grid in the path of the The description of the QEM as given above outlines a route
lower electron ring represents the object to be imaged, which consists of both
toward binary, black and white imaging, which may nd use in a
transparent and opaque pixels thus creating a binary image. A black (white) pixel in
the path of the lower ring prevents (allows) coherent evolution of the electron variety of biological imaging applications such as high-contrast
wave-packet from the upper ring to the lower ring after N circulations. Reprinted stained objects or materials infused with nanoparticles. One pro-
with permission from Putnam and Yanik [30]. Copyright 2009 The American Phy- blem with the interaction-free scheme of detection however, is
sical Society. that it is not immediately clear how one can obtain gray values in
an image, which is desirable in electron microscopy. A recent pa-
per from a number of the authors of this work concluded that
between the two wells. If we consider the double-well potential as grayscale imaging in the interaction-free scheme as described
being generated by a pair of coupled electron ring-resonators, then above is not possible without inducing damage to the sample,
the electron population will move between the reference well, albeit less damage than in conventional schemes for high-contrast
which is localized on the reference ring, and the sample well, specimen [25]. However, Facchi et al. [32] have suggested that
which is localized on the sample ring, with each circulation in grayscale imaging may be possible for largely opaque objects using
those rings as shown in the left plot of Fig. 2(b), [31]. However, if an imaging scheme referred to as quantum Zeno tomography.
an opaque object is placed in the path of the sample ring, it will Another problem, or perhaps opportunity, is the fact that an
destroy the coherent evolution of the electron state, and the electron microscope sample can also change the phase of the
electron will remain in the reference ring as shown in the plot on sample beam, which inuences the subsequent coupling between
34 P. Kruit et al. / Ultramicroscopy 164 (2016) 3145

Fig. 4. Modular design of the QEM system showing the layout and position of the resonator. The modular framework will enable compatibility with existing electron
microscopes, potentially allowing existing electron microscopes to operate in QEM-mode after installation of a resonator.

the reference beam and the sample beam. The issue of the electron In the next section, we shall describe the preliminary designs of
phase-shift in a QEM system was considered by Thomas et al. [25] quantum electron microscopes based on each of these four two-
but has not yet been analyzed in detail. In general, the eld of state-couplers.
interaction-free electron microscopy is so novel that the possibility
of grayscale imaging using such a technique has not yet been
completely eliminated, and will be the subject of further 2. Design based on a thin crystal coupler
investigation.
Putnam and Yanik [30] predicted an imaging resolution of Bragg diffraction from a crystalline sample can be used to co-
19 nm for their system consisting of a hybrid Paul-Penning trap herently split a beam of electrons. In fact, crystalline electron
using 100 keV electrons. Apart from the limited resolution, many beam-splitters were adopted in the rst electron interferometry
details of the system described by Putnam and Yanik present device developed by Marton in the 1950s, and have been im-
challenges for the construction of a proof-of-concept QEM, for plemented in a number of other electron interferometer devices
example, their system is based on charged particle trapping since then [3337], (thin crystals have since been replaced by
techniques, which are not commonly used in electron microscopy electron biprisms in electron interferometry instrumentation
and are less suitable for high-energy electrons, which are typically [38]). The dynamical theory of electron diffraction denes that the
required for imaging applications. In this work, we will describe a direct beam and the diffracted beams are coupled by the atomic
number of competing approaches toward the rst demonstration potential of the crystal, and hence that the intensity in the beams
of an operational QEM, with an emphasis upon the practical re- oscillates as a function of the crystal thickness [4,39,40]. Com-
quirements for a successful design. In particular we will consider monly observed thickness fringes in TEM images are caused by
systems based on four different electron-beam couplers to fulll this intensity oscillation between the direct beam and diffracted
the required coupling between the | reference and | sample states beams. Fig. 5 shows bright-eld and dark-eld TEM images of a
in the QEM. Here, we consider discrete coupler units as opposed to crystalline Si wedge. Bright-eld images are formed by collecting
the continuous coupler unit described by Putnam and Yanik. Dis- the direct-beam alone, using the objective aperture of the micro-
crete coupler units will enable greater compatibility with con- scope to isolate the direct-beam (000 in Fig. 5(c)). The dark-eld
ventional electron microscopy components, a key requirement for image shown here was formed by collecting one of the rst-order
the successful development of a QEM system. Below, we highlight diffracted beams. Thickness fringes can be observed at the edge of
the key components required in a QEM. the wedge and are caused by the reducing thickness of the Si
A QEM must have the following sub-units: crystal toward the lower edge shown in Fig. 5. The thickness var-
iation leads to intensity oscillations such that the intensity in the
1. A central electron-optical unit in which the electron beam can direct beam decreases as the intensity in the diffracted beams
travel repeatedly through the two-state coupler, which creates increases, thus leading to contrast variation in a bright-eld TEM
the necessary coupling between the reference and the sample image where only the direct-beam is collected by the objective
states. We call this the resonator. aperture to form an image (Fig. 5(a)). The inverse contrast can then
2. A two-state-coupler positioned within the resonator. be seen in the dark-eld image. This intensity oscillation is known
3. The resonator should also contain a sample holder and focusing as Pendellsung after the German for pendulum solution and is
unit to either create a small probe on the sample or to form a analogous to Rabi oscillations in two-level quantum systems dri-
magnied image of the sample depending on whether the mi- ven by an oscillating eld [41].
croscope is a scanning transmission microscope or an imaging Fig. 5(b) shows plots of the electron beam intensity for both the
transmission microscope. direct beam and the diffracted beam as a function of crystal
4. An electron source and beam-forming unit. thickness. The plots in Fig. 5(b) were produced by solving the
5. A unit that opens the resonator to allow the electron beam to HowieWhelan equations for the two-beam condition (see Fig. 5
enter. We call this unit the entrance barn door. (c)) [4]. The periodic oscillation of the electron beam intensity in
6. An exit barn door. both the direct, and the diffracted beams can be considered ana-
7. A detector unit. logous to the intensity oscillations in the reference and sample
beams of a QEM as described in Fig. 3. For the purpose of the
The modular design of the proposed QEM instrument is shown quantum interrogation in a QEM, we may replace the thick crystal
schematically in Fig. 4 below, and is applicable to all two-state- described by dynamical diffraction by a very thin crystal, and lead
coupler systems considered in this work. the same electron through it many times. The oscillatory behavior
While the coherent electron source and the electron detector should then be identical to that of a thick crystal if, by means of
are standard components of TEMs, a resonator and a coherent electron optics, we can reconstruct the electron wavefunction
two-state coupler are not. We have found that the design of an produced at the exit plane of the crystal, at the entrance plane of
operational QEM is to a large extent determined by the choice of the crystal, after a single pass through the resonator.
the two-state-coupler. So far we have identied four possible The calculated intensity oscillations shown in Fig. 5(b) were
couplers: (1) a transmission grating such as a thin crystal, (2) an based on the assumption that a perfect two-beam condition was
electron mirror patterned with a grating, (3) a radio frequency obtained where all of the electron-beam intensity is contained
potential well and (4) a standing light wave transmission grating. within the direct beam and a single diffracted beam. Moreover, we
P. Kruit et al. / Ultramicroscopy 164 (2016) 3145 35

Fig. 5. (a) Bright-eld and dark-eld TEM images of a crystalline Si wedge acquired under the two-beam condition with a o1104 oriented crystal and the direct beam and a
{220} beam strongly excited. Thickness fringes can be observed terminating at the edge of the wedge to the lower right of each image. (b) Plots of electron beam intensity as
a function of crystal thickness (t) for both the direct beam (reference beam in QEM) and the diffracted beam (sample beam in QEM) based on solutions to the HowieWhelan
t 2 sin2 (tseff ) 1
Eq. (4) which stipulate that Ig = =1 I0 seff = s2 + 2 , where Ig is the intensity of the diffracted beam, I0 is the intensity in the direct beam, t is sample
g (tseff )2 g

thickness, g is the extinction distance and s is a crystal-dependent parameter. If we consider a series of thin crystals with thickness tc in the path of the electron-beam, we
can observe a full intensity transfer from the direct-beam to the diffracted beam after N passes through that thin crystal. The plots in (b) show both the oscillatory nature of
the intensity transfer between the direct and diffracted beams known as the Pendellsung effect, and the point at which complete intensity transfer occurs (Ntc ), which
would be the point of operation for QEM. (c) Schematic representation of a typical two-beam diffraction condition for a thin crystalline sample. The gure shows the direct
beam (000) and diffracted beams (g(hkl)) for an incident electron beam at a {hkl} family of lattice planes that are oriented at the Bragg angle () with respect to the incident
beam. In this geometry, only one strong diffracted beam is formed.

assumed that any losses in intensity due to inelastic scattering distances (d-spacing) are desirable to increase the Bragg angle and
within the thin crystal coupler were negligible. Successful im- thus reduce the number of diffracted beams falling on the Ewald
plementation of this coupler in a resonator for a QEM system will sphere resulting in a cleaner two-beam condition. Additionally, we
depend upon satisfactory solutions to the following issues: (1) in- propose that an aperture placed near the sample plane would
tensity losses to other diffracted pathways should be eliminated or behave as an opaque pixel for any unwanted diffracted beams. As
blocked without too much impact on the intensity contained such, the aperture may function in a similar fashion to an opaque
within the reference and sample beams, (2) inelastic scattering at pixel as described in Fig. 1.
the crystal coupler needs to be minimized to reduce unwanted The second issue (2) concerns that of an inelastic scattering
intensity loss and (3) the relative phases of the sample and re- event within the sample beam or reference beam destroying the
ference beams need to be correct when they complete a circula- coherence between the two beams [42]. Inelastic scattering at the
tion in the resonator in order to achieve coherent coupling of the crystal coupler may be reduced through careful consideration of
two beams in subsequent circulations. While the issues high- the material and geometry of the coupler. The total inelastic
lighted here are challenging to overcome, in the following section scattering cross-section for electrons with  100 keV energy tends
we propose routes to address each of these issues during the to increase with increasing atomic number (Z) of the scattering
system design. material [40]. We may thus suppress the probability for inelastic
We propose to address issue (1) that of losses to higher order scattering by forming the coupler from a low-Z material such as
diffractive pathways by reducing the number of diffractive diamond or silicon. Diamond additionally possesses zone axes
pathways available for the beam to exit the crystal. The number of with short d-spacing values, supporting reduced losses to higher
diffractive pathways to exit the crystal coupler may be reduced by order diffraction pathways as described in (1) above. We may also
using a crystal with a zone axis consisting of closely spaced lattice decrease the total probability for inelastic scattering by reducing
planes. Crystals possessing zone axes with short interplanar the thickness of the crystal coupler. We note that the trend of
36 P. Kruit et al. / Ultramicroscopy 164 (2016) 3145

Fig. 6. Schematic drawing of the QEM system based on a thin crystalline coupler. (A) Electron source and beam forming optics. (B) Fast deector allows insertion of electron
pulse into the resonator. (C) Electron pulse is split at the coupler and a fraction of the electron-beam is focused onto the sample. (D) The sample and reference beams then
propagate within the ring resonator and are projected back onto the coupler. (E) After N circulations in the resonator the electron pulse is deected out of the resonator.
(F) Measurement of the intensity in the reference beam at a detector will then establish whether the pixel in the path of the sample beam is transparent or opaque.

reducing inelastic scattering by reducing the thickness may change using mirrors to create an electron cavity. We will consider the
for ultrathin ( o5 nm thick) crystals. Inelastic scattering mechan- storage-ring design here, as the thin crystal requires high-energy
isms such as surface and volume plasmon excitations are sup- electrons to maximize the mean-free-path of the electron traver-
pressed in ultrathin crystals, and retardation and interband tran- sing the crystal. A possible benet of the storage ring design is that
sitions may dominate the inelastic scattering process [43]. it can be combined with an electron energy-loss spectrometer
Nevertheless, the crystal thickness should be optimized to both (EELS) in a STEM to make use of the information in the inelastic
reduce inelastic scattering and achieve the desired intensity channel. Here, we assume operation in the STEM mode to keep the
splitting between the sample and reference beams. An intensity description as simple as possible; however, the principle could
splitting ratio of 99:1 between the reference beam and the sample also work in TEM mode, where many pixels are imaged simulta-
beam would necessitate 16 circulations in the resonator to achieve neously. A description of a system employing electron mirrors to
maximum intensity transfer between the reference and sample create a free-space electron cavity is described in the next section.
states according to the HowieWhelan equations, assuming a va- The layout of the electron optics required for the storage ring is
lue of zero for the crystal-dependent parameter seff. If we consider shown schematically in Fig. 6. Briey, the electron beam is formed
a o220 4 oriented Si crystal splitter, and 100 keV electrons in module [A], which consists of a high-brightness electron source
where g 75.7 nm, the HowieWhelan equations described above such as that commonly used in a high-resolution (S)TEM. The
allow us to calculate a suitable crystal thickness of 2.4 nm. Theo- beam is produced using an electron-optics system consisting of
retically Si crystals with thicknesses of t=n(75.7 nm)+2.4 nm , alignment optics, condenser lenses and apertures that select a
where n is an integer, could also achieve a similar splitting ratio. sufciently small section of phase space to create a beam that is
However, thicker crystals would lead to intensity loss, especially as almost fully coherent. Module [B] contains a fast beam-deection
the electron beam would have to pass through the crystal multiple system enabling injection of an electron bunch into the ring-re-
times (3). Correctly mapping the phase of the reference and sonator. The deection system should operate on a timescale sig-
sample beams back on to the crystal coupler after each circulation nicantly shorter than the circulation time of the electron bunch
in the resonator is equivalent to positioning the interference pat- in the ring-resonator. The circumference of the resonator would be
tern of the two beams with atomic resolution on the crystal lattice  1 m for typical STEM dimensions, thus giving a circulation time
of the crystal coupler. As a result, it is clear that the resonator of approximately 5 ns for a 200 keV electron propagating at ap-
should be installed in a tool capable of producing atomically re- proximately 2  108 m s  1. Upon entering the resonator the elec-
solved images of a crystal lattice i.e. a high-resolution TEM. The tron bunch is split at the crystal coupler such that one diffracted
high-resolution demands of re-imaging the sample and reference beam passes through the sample of interest. The sample is held in
beams on the coupler with the correct relative phase would be a conventional TEM sample holder residing in the immersion
reduced if an articial crystal could be produced with a typical objective lens. If we assume that the electron beam is tightly fo-
one-dimensional unit cell of say 10 nm. Although fabricating such cused at the sample plane (STEM-mode), this would suggest that
a structure is not impossible with modern techniques in multilayer the crystal coupler would be placed either, at the front focal plane,
growth or lithography, it may introduce other issues because of or at the back focal plane of the lens. In many microscopes, a
atomic scattering. More research in this direction is needed. diffraction aperture is placed in this position. Module [E] is a
The resonator may be formed using either a storage ring, or by mirror copy of module [B] and acts to deect the electron bunch
P. Kruit et al. / Ultramicroscopy 164 (2016) 3145 37

out of the resonator to a detection system. This module may also


contain magnication optics to further separate the direct beam
from the diffracted beams and to allow normal sample imaging
when the ring-resonator is deactivated. Module [D] contains
bending magnets and lenses to recirculate the sample and re-
ference beams back to the entrance plane of the coupler until the
number of circulations required for intensity transfer between the
reference and sample beams has been achieved.
One may wonder whether the addition of the resonator inu-
ences the resolution of the microscope or the longitudinal co-
herence of the beam. In the rst pass of the beam through the
sample, the resolution should be unaffected by the resonator, so
the resolution of a modern STEM should be obtained. The STEM
could even include an aberration corrector in section [C]. The Fig. 7. A plot of a cross-section through the potential surface simulated at a 1-m-
STEM objective lens usually demagnies the aberrations of the period grating to which a static eld of 30 kV/mm has been applied. The grating
condenser lenses such that they may be ignored. Similarly, we mesas have a square cross-section 100 nm in width and height. The potential dif-
assume that the aberrations of the resonator elements will also be ference between each of the equipotential lines shown in the plot is 1 V. The static
eld is generated by a bias potential applied between the grating surface and a
demagnied. However, after each pass, the aberrations Co of the
planar, grounded counter electrode parallel to, and above the grating surface. A
objective lens are added linearly to a value NCo, while the re- plane wave, such as that present in a collimated electron-beam, incident on such a
solution is proportional the square root of the total chromatic potential surface would diffract according to the grating equation producing a
aberration ( Cc ) and the 4th power root of the spherical aberra- linear array of diffraction spots in the back-focal plane of the collimating lens.

tion ( C1/4
s ). Thus, to achieve atomic resolution, an aberration cor-
rector will probably be required. One possibility is to insert a
grating will be at or above the energy of the incident electron, the
chromatic and spherical aberration corrector in the resonator by
electron will reect/diffract above the surface of the electrode and
using the properties of the non-rotational symmetry of the
will not directly interact with the solid surface of the mirror. This
deectors.
approach thus eliminates the probability for inelastic scattering at
If a crystal coupler is used, the exit wave of the coupler must be
the coupler. We call this device a grating mirror.
imaged onto the top surface of the crystal with sub-lattice re-
We consider diffraction from a sinusoidal grating mirror as
solution and accuracy. This resolution is easily obtained because
equivalent to diffraction at a transmission phase grating, where
the aperture angle of the beams at the coupler is small. The ac-
diffraction is a result of the position-dependent phase change of
curacy can be obtained by using deection and rotation optical the electron wave. A weak phase variation of (o o1) radians
elements. The mechanical and electronic drift of the interference yields an amplitude in the diffraction plane with a delta-function
pattern on the coupler should be much less than the lattice spa- on axis and the Fourier transform of the phase variation in the rest
cing during the time of N circulations ( 500 ns). Chromatic dis- of the plane. So if the phase variation is a periodic function, the
persion of the individual deectors in the resonator should be amplitude distribution also consists of delta functions with am-
mutually compensated. plitudes of the diffracted beams of the order of in magnitude
If the reference beam and the sample beam travel over different [44]. In the case of reection from a grating, the position-depen-
paths through the resonator, there is a risk of losing the ability to dent phase in the beam is introduced by the different path lengths
interfere because of a relative longitudinal shift of the wave- of the trajectories upon reecting from the surface. In a rst ap-
packets. This effect has not yet been analyzed in detail, but we proximation, we treat the whole electron mirror (decelerating
assume that it can be either eliminated or compensated. The same eld reection accelerating eld) as a pure phase grating. This
applies for the possible collapse through synchrotron radiation in means that we assume that when the diffracted beams exit from
the deectors. On the latter effect, let us note that only radiation the accelerating eld, they have not yet interfered with the re-
with sufciently short wavelength to distinguish between the ference beam to create amplitude contrast. So at the exit from the
paths of the reference beam and the sample beam will lead to mirror there is only a periodic phase variation on the exit wave. In
mutual decoherence. the far eld, the intensity distribution is then given by the Fourier
We conclude that a QEM based on a storage ring design transform of the exit waveform. This approximation should be
would be a complicated instrument, requiring many novel design accurate if the length over which the mirror eld acts is short
features. However, we have not found reasons why it would be compared to the length scale of the instrument. This approach
impossible to achieve atomic resolution in a quantum electron circumvents the difculty of applying diffraction theory in a si-
microscope with this design. tuation where the wavelength becomes innite, which occurs at
the position of reection. Now the diffraction angle may be de-
scribed by the grating equation.
3. Design based on diffractive electron mirror
n electron=d sin (1)

As we have seen in the previous section a diffractive element Here, n is the diffractive order, electron is the de Broglie wave-
such as a thin crystal may be employed as a coupler for a QEM length of the electron at the exit of the mirror, d is the period of
design. One drawback of the crystalline beam-splitter is that the the grating and is the angle of diffraction. The de Broglie wa-
electron beam has to pass through the crystal for diffraction to velength of a 5 keV electron is 17.4 pm, which results in a rst-
occur. An electron beam traversing a thin crystal will experience order diffraction angle of 17.4 rad for a grating with a period of
inelastic scattering resulting in a loss of signal. Consequently, we  1 m. It is apparent from the grating equation that a higher
propose to diffract an electron beam at a periodic surface potential energy electron beam or a larger grating period will result in a
generated by applying a high voltage to an electrode on which a smaller angle of diffraction and thus lower spatial separation of
topographical grating with a nanometer to micrometer scale per- the sample and reference beams in the resonator.
iod has been fabricated (Fig. 7). Since the potential applied to the For small phase changes, we expect that we can apply a local
38 P. Kruit et al. / Ultramicroscopy 164 (2016) 3145

WKB approximation since the changes are small on the scale of at mirror. A lens system focuses the reference beam through a
the wavelength. The phase change in going through the mirror is hole in the sample. A second lens system creates a parallel beam
then: onto the grating mirror. The reected and diffracted beams are
focused back on the plane of the sample. One rst-order diffracted
(x) = (2x,z

)
dz with=
h
2meU (x,z)
beam is focused on the sample. Higher order diffracted beams are
(2) blocked at this plane. During multiple passes through the re-
Here, the integral is taken over the path of the electron. Both sonator, the amplitude in the sample beam slowly increases. Ef-
the (z) and the length of the path of the electron are x-depen- fectively only half of the sample beam traverses the sample. The
dent. The potential U in the grating mirror is a solution of the sample is illuminated both from the top and from the bottom.
Laplace equation with a periodic boundary condition; After N cycles, the barn door is opened again and the bunch leaves
the resonator. Between the electron source and the barn door is a
2z 2x beam separator that deects the exiting electron bunch to a de-
U(x,z)=Ezz+Ue d cos
d (3) tector. Several sets of deectors will be necessary to steer the
In Eq. (3) above, d is the period of the sinusoidal potential beam correctly through the resonator. It is clear from Fig. 8 and the
variation with amplitude U at z 0 and Ez is the mirror eld. For grating equation that a shorter grating period and lower electron
a topographical grating with amplitude A, the surface acts as an energy give a larger separation of the reference beam and the
equipotential surface. At some distance from the surface, the effect sample beam and thus are preferential for ease of access to the
can be translated to a potential variation UAEz. Unfortunately, sample beam. However, as the grating period is reduced, so too is
the integral for the phase change when performed for this po- the amplitude of the surface potential modulation at the mirror. A
tential distribution does not have an analytical solution. None- reduced modulation of the potential will ultimately lead to a re-
theless, one can see that it is possible to choose for reection to duction in diffraction efciency. Likewise, a lower-energy electron
occur at an equipotential surface closer or further from the surface is more sensitive to stray elds in the resonator resulting in poorer
by tuning the potential of the mirror. With that, the intensity in imaging resolution. However, these are only considerations for the
very simple system shown in Fig. 8. The important parameter for a
the diffracted beams is tuned. In fact, preliminary numerical cal-
more complex system containing more lenses is the number of
culations show that the diffracted intensity is very sensitive to the
grating periods illuminated by the beam. A larger number of il-
choice of reection surface, which leads to the undesired effect of
luminated grating periods results in a sharper diffraction spot and
an electron-energy-dependent diffraction intensity. We have
thus improved resolution in the diffracted beam.
found that the grating period and potential gradient at the mirror
An example layout of a more complex microscope using a
surface must be large to minimize the effect of electron energy on
grating mirror is shown schematically in Fig. 9. The electron beam
diffraction intensity.
is formed in a module (A) which consists of a high-brightness
Fig. 8 shows a schematic drawing of a design for a microscope
with a resonator including the grating mirror. A barn door (see
next section for a detailed description) opens to allow an electron
bunch to enter the resonator and subsequently closes to act as a

Fig. 8. Schematic drawing of the QEM system based on a nanostructured electron Fig. 9. Schematic of a high-resolution QEM system based on a grating mirror
mirror coupler. The thick (blue) rays represent the reference electron-beam while coupler. (A) Electron source, entrance barn door and mirror (at high voltage).
the thin (red) rays represent the sample electron-beam. The sample is inserted into (B) Condenser lenses. (C) High-resolution immersion objective lens.
the path of one of the red rays at the crossover near the center of the resonator. The (D) Magnication lenses. (E) Grating mirror and exit barn door (at high voltage).
coupler at the base of the resonator is a diffractive mirror such as that shown in (F) Measurement of the intensity in the reference beam at a detector will then
Fig. 7. (For interpretation of the references to color in this gure legend, the reader establish whether the pixel in the path of the sample beam is transparent or
is referred to the web version of this article.) opaque.
P. Kruit et al. / Ultramicroscopy 164 (2016) 3145 39

electron source such as that commonly used in a high-resolution


(S)TEM. The beam is rst limited by apertures, which select a
sufciently small section of phase-space, to create a beam that is
almost fully coherent. As the electron energy is still low, this re-
gion is a suitable position for a barn door that upon closure acts as
an electron mirror. The beam is now accelerated and enters a
column similar to that in a conventional (S)TEM with condenser
lenses, alignment deectors, stigmators, a high-resolution objec-
tive lens and the sample holder (B,C). After the objective lens and a
few magnication lenses (D), there is a module in which the
grating mirror is held at the potential of the electron source (E). In
this module, the beam is decelerated towards the grating mirror. A
set of electrostatic deectors allows the beam to be deected to-
wards a hole in the mirror so that, after the required number of
bounces, the beam can exit the resonator. The beam is accelerated
again into the last module of the microscope. This module contains
the detector and may also contain magnication optics to further
separate the direct-beam from the diffracted beams, and to allow Fig. 10. A standing light wave as a beam-splitter in a QEM could either work in the
normal sample imaging when the resonator is deactivated. diffractive regime (A) or in the Bragg regime (B). The interference orders are se-
parated by 2k in momentum space.
The analysis of lens aberrations for this design is similar to that
discussed for the ring-resonator, so an aberration corrector would
also be very useful here. An interesting opportunity arises in this where Jn is the nth Bessel function of the rst kind.
system because we use mirrors located in a conjugate plane of the
objective lens back-focal plane. A mirror at that position can be
In the Bragg regime Up ( 2k2
2me )
, only two diffraction orders
couple [51] and they are again separated in momentum space by
used as aberration corrector for both spherical and chromatic
px =2k . The probability of nding an electron in each of the two
aberration.
In conclusion, a design of a QEM with a resonator between two diffraction orders will follow a Pendellsung with Pk=cos2 ( )
Up t
4
mirrors seems entirely feasible and considerably simpler than a
design with a ring-resonator. However, it relies on the as yet un-
and Pk=sin2 4( ) analogous to the solution obtained in the ori-
Up t

proven operation of the grating mirror. ginal QEM proposal [30]. Note that in a QEM there would be N
interactions between an electron and the standing light wave and
the argument in the above solutions would have to be replaced by
NUp t
4. Design based on a coupler using a standing wave of light . Also, the electrons have to encounter the standing light wave
4
k
at an angle = p in order to fulll energy and momentum
A coherent beam-splitter can also be realized via the diffraction z
conservation.
of electrons at a standing wave of light. This technique was ori-
In the diffractive regime, the setup would look like the one
ginally proposed by Kapitza and Dirac in 1933 [45] and was later
sketched in Fig. 6, with the standing light wave replacing the thin-
used to diffract electrons [46], atoms [47] and molecules [48]. A
crystal beam-splitter. Again, all higher diffraction orders would
review on the KapitzaDirac effect in electron matter wave optics
have to be blocked in order to avoid losses to the higher diffraction
has been prepared by Batelaan [49].
orders as discussed in Section 1 describing the design based on a
A beam-splitter made of light offers several advantages, most
thin-crystal coupler. One possible electron optical design for a
notably that there is no absorption and negligible inelastic scat-
beam-splitter operated in the Bragg regime is shown in Fig. 11.
tering of electrons. The required optics can be mounted far from
It is interesting to consider the laser intensity requirement for
the electron beam such that charging and patch potentials do not
such a beam-splitter. In the Bragg regime, the wavefunction of an
pose a serious problem. Also, as we will see in the following, the
electron is completely transferred from the reference beam to the
diffractive power of such a beam-splitter can simply be tuned by U t
(empty) sample beam if 40 = 2 . In the diffractive regime, a similar
varying the power of the laser and it would thus be possible to
alter the number of bounces required for a QEM measurement. statement can be made as the zeroth order Bessel function has its
U t
The KapitzaDirac effect can be described as the diffraction of rst zero at 0 2.4 . For an electron passing through a focused

electrons at the ponderomotive potential Up [50] of the standing Up r0
2
e2I 2 2c
Gaussian laser-beam of waist r0, we get Up (t) dt v
, where
light wave: Up= cos2 (kx) , where k= , = and I is the laser
2m0c2 2Ekin 2P
v= is the velocity of the electron. With I= , where P is the
intensity. This scattering can also be understood in a particle pic- m r2
0
ture, where absorption of a photon with momentum k and sti- total power of the continuous wave laser and after N interactions
mulated emission induced by a photon with momentum k leads our laser power requirement can be written as in Eq. (4).
to a total momentum transfer of 2k and a corresponding de- 0 c
2k
ection of the electron beam by an angle = p , where pz is the P=42r0 Ekin m 3
Ne2 (4)
z
longitudinal momentum of the electron.
It is thus tempting to choose a long laser wavelength, however
A beam-splitter for a QEM based on a standing light wave could
this would decrease the diffraction angle. Lower electron energies
be realized in two different regimes (see Fig. 10). For a strong
on the other hand will both decrease the power requirement and
ponderomotive potential Up 2m ( 2k2
e )
, in the so called diffractive increase the de Broglie wavelength of the electrons. For
= 532nm , Ekin=1keV and N=100 we get P3.7 kW for a focal waist
regime, this will lead to an interference pattern showing multiple
diffraction peaks [46], each corresponding to a transverse mo- of r0=10 m or P370 kW for a focal waist of r0=1 mm (the tran-
2k2
mentum transfer px =2nk , n . The probability of nding an sition from the diffractive to the Bragg regime Up= 2m is reached
e
electron in the nth diffraction peak will be given by In =J2n ( ),
U0 t

for r0=116 m ).
40 P. Kruit et al. / Ultramicroscopy 164 (2016) 3145

The demonstration of an electron beam-splitter is based on the


guiding techniques described above [57], which will enable the
coupling unit in this QEM approach. Fig. 12(a) shows the electrode
layout of the planar beam-splitter. The electric eld above the
guiding chip can be transformed from quadrupole to hexapole
symmetry along the horizontal y-direction by means of a tapered
central electrode. The hexapole symmetry of the electric eld
leads to the creation of a double-well pseudopotential with two
minima, separated by a potential barrier. The simulated pseudo-
potential is plotted in Fig. 12(b)(d), showing the transition from a
single to a double well. The separation of the double well can be
controlled by adjusting the width of the central electrode. Fur-
thermore, we have numerically optimized the shape of the chip
electrodes to provide a guiding potential that allows smooth beam
splitting, producing two spatially separated electron beams.
However, to implement the scheme proposed by Putnam and
Yanik using such a microwave guide with two arms, a few chal-
lenges have to be overcome. A single electron has to be coupled
into one of the arms, which is then supposed to provide a tight
connement and at the same time enable transfer of electron wave
amplitude into the second arm. To realize these two conicting
requirements (tight connement and coupling), we present a
modied scheme where the coupling potential between the two
arms is not constant. Thus our proposed electron guide is divided
into two sections, one of which enables coupling between the
Fig. 11. Conceptual design of a QEM with a standing light wave as the coupler resonator arms, while the other realizes a tight connement and
element. The electron beam enters the resonator off-axis, thus enabling the for- separates the two arms to allow encounters with the sample.
mation of a two-beam system. Fig. 14 shows a potential implementation of the QEM scheme
using the planar beam-splitter as a coupling element between two
electron resonators. The envisioned scheme uses electron wave
A standing light wave of this intensity can either be realized
packets that are laser-triggered from a metal nano-tip as a co-
with two counter propagating laser pulses or by enhancing a
herent source [58,59]. The electrons are coupled into the trans-
continuous wave laser in a cavity. In the Bragg regime, it might be
verse ground state of the lower arm of the beam-splitter potential
especially convenient to relax this laser power requirement by
(Fig. 13(b)). As described above, this localized reference state is
working with an elliptical beam prole that is compressed per-
actually a 50/50 superposition of the two lowest quantum states of
pendicular to the direction of the electron beam.
the double well potential.
Fig. 13(a) shows the energy levels of the two lowest states along
the beam-splitter chip. As the electron passes the junction of the
5. Design based on a double potential well coupler potential at yE35 mm (Point 4 in Fig. 13(b) and (c)), the conning
potential transforms from a double-well to a single-well trans-
The motion of slow electrons with kinetic energy on the order verse guiding potential. As a result, the electron, which is origin-
of several electronvolts can be precisely manipulated in free space ally in the ground state of the lower arm, now occupies a super-
using high-frequency electric elds. This capability allows the position of the two lowest energy states of the single-well po-
fabrication of 2-d traps for electrons based on the generation of tential. This superposition state alternates temporally between the
the necessary microwave elds by means of properly shaped two lowest Eigenstates. The frequency at which the electron's state
electrodes on a planar substrate [52,53]. The generation of mi- oscillates is proportional to the energy difference of the respective
crowave elds by means of a planar microwave chip provides ease states and may reach a frequency of up to E 2  58 MHz. At Ekin
of scalability and the exibility to engineer versatile guiding po- 1 eV, one period of this frequency corresponds to 10 cm of travel
tentials in the near-eld of the microwave excitation. This feature for the electron; however, the electron may be slowed to arbi-
makes surface-electrode structures ideally suited for the im- trarily low energies while conned above the chip.
plementation of a double-well potential as originally proposed by When the electron reaches the end of the chip at y 40 mm, it
Putnam and Yanik [30]. is reected by an electron mirror and driven back to the double-
The approach described here is based on a similar principle as well section of the guide, where the two minima are well sepa-
the Paul trap [54], which is widely used to trap and guide the rated. The superposition of the rst two eigenstates of a single well
motion of atomic ions [55]. In a 2-d Paul trap, the transverse is thus turned into a superposition of the rst two Eigenstates of a
connement of the guide relies on the formation of a time-aver- double-well, corresponding to a splitting of amplitudes between
aged harmonic pseudopotential resulting from a high-frequency the wells. Part of the amplitude from the reference state has been
electric quadrupole potential that oscillates in the gigahertz fre- transferred to the sample state. How the amplitude splits be-
quency range. Stable electron connement requires that the po- tween the two wells depends on the amount of time the electron
tential gradient experienced by the electron is nearly constant over remains in the single-well state, and hence the evolution of the
the amplitude of the electrons oscillation. A double-well pseu- superposition state during this time. Fig. 13(c) illustrates the
dopotential can be generated based on the same principles using a subsequent evolution of the wave-packet at several positions
microwave electric potential with hexapole instead of quadrupole along the guide. The part of the wave-packet that nally ends up in
symmetry. The hexapole symmetry is the lowest-order multipole the upper part of the potential ( sample state) is ejected from the
that supports two intersecting potential minima and hence creates guide, accelerated, and then focused onto the specimen or, if the
a beam-splitter [56]. specimen is transparent or absent, reected back by a second
P. Kruit et al. / Ultramicroscopy 164 (2016) 3145 41

Fig. 12. Electrode design of the planar electron beam-splitter and pseudopotential simulations. (a) The numerically optimized layout of the microwave driven electrodes is
shown in red. The blue areas are electrically grounded. The insets show the electric eld generated above the surface at three selected positions. (b) Cross-section normal to
the electrode plane at y 6.5 mm. A single pseudopotential minimum forms at a height of 450 mm above the substrate surface providing harmonic connement. (c) At
y 17 mm the additional central electrode, with a width of 160 mm, creates a double-well pseudopotential with a separation of 150 mm between the minima. A four-fold
magnied image is shown in the inset with a 50 times amplied color code. By increasing the width of the center electrode the separation of the double-well minima is
gradually increased. (d) At y30 mm the central electrode is 260 mm wide, leading to a separation of the minima of 400 mm. (For interpretation of the references to color in
this gure legend, the reader is referred to the web version of this article.)

mirror to be re-injected in into the guide. The other part of the beam entering the resonator, thus allowing all electrons to remain
wave-packet following the lower part of the potential ( reference in a paraxial condition during barn-door operation. Consequently,
state) is also ejected from the guide and reected by the closed these paraxial electrons will be less susceptible to the strong
barn-door without interaction with the specimen. By adjusting aberrations expected far from the optical axis of the barn-door.
the point where the electron gets reected inside the coupler, the The resonator round-trip time depends on the energy of the
time spent in the single well and thus the amplitude transfer from electrons and the geometry of the resonator, which depends on
the reference to the sample state can be adjusted. This control the period of the two-state coupler used for the specic design.
enables tuning the success probability of the quantum measure- We can perform a crude estimate for the design shown in Fig. 11
ment and thus the damage to the specimen. All the involved by assuming that at the sample plane, the distance between the
electron mirrors can be realized by electrostatic potentials. The reference beam and the sample beam should be at least x=5 mm,
barn door at the entrance to the resonator can be realized with in order to have sufcient access to sample beam. At constant
schemes as discussed in the preceding section. electron energy, the time for an electron to travel from the
m x
standing light wave to the sample plane will be > 2ek , which
5.1. Notes on the barn door amounts to 1.8 ns, where k=2/ , with =532 nm. This is in-
dependent of the longitudinal velocity of the electrons. The total
One challenge in building an electron resonator is coupling the round-trip time depends on the number of lens elements and the
electron into the resonator, and then out for detection. This can be potential-energy landscape within the resonator, but will be on
done by either lowering one of the dening potentials of the re- the order of 1030 ns for the resonator design shown in Fig. 11.
sonator at the moment the electron needs to enter/exit the re- This suggests that coupling of electrons into and out of the re-
sonator structure (see Fig. 15(a)), or by quickly decreasing/in- sonator should be controlled on a timescale of about 1 ns.
creasing the kinetic energy of the electron (see Fig. 15(b)), or by a While pulsed electrostatic ion traps have been realized with
pulsed deection of the electron beam (see Fig. 15(c)). All ap- gating times on the order of hundreds of nanoseconds [60], gating
proaches require this to be done on a timescale that is short times on the order of one nanosecond will require careful design
compared to the round-trip time of an electron in the resonator. and impedance matching of the electrodes.
Additionally, it is important to consider whether the electron For a two-state coupler based on a thin crystal, the round-trip
beam should enter the resonator as a focused beam or as a broad time could potentially be shorter due to the larger diffraction an-
collimated beam. Our preliminary designs consider a focused gle. Sub-nanosecond in-coupling and out-coupling of electrons
42 P. Kruit et al. / Ultramicroscopy 164 (2016) 3145

Fig. 13. Chip-based guided electron-beam coupler. (a) Energy level of the two lowest quantum states of the conning potential. (b) Numerically optimized beam-splitter
potential as coupler in the QEM scheme. The electron optics required to focus and reect the electron beam are shown in Fig. 14. See text for further explanation.
(c) Evolution of a wave-packet in the splitting potential. The blue curve shows the potential in transverse direction. The absolute value of an electron wavefunction is plotted
in red. (For interpretation of the references to color in this gure legend, the reader is referred to the web version of this article.)

might be realized using precisely timed THz [61] or optical control quantum principle of IFM. That principle has been realized already
[62] of electron trajectories and energies. for optical systems, but this paper contains the rst sketches of
modied electron microscopes in which quantum interrogations
or an IFM could be performed at atomic resolution. However, we
6. Discussion note that the principle of interaction-free imaging has thus far
only been shown to be capable of generating binary, black and
Acquiring atomic resolution, 3-d images of biological speci- white images. This imaging mechanism can be applied to high-
mens and macromolecules with negligible damage to the sample contrast samples consisting of pixels that are not fully opaque or
is presently one of the greatest challenges in electron microscopy. transparent. However, true grayscale imaging using a QEM is ex-
One approach toward meeting that challenge could be via the pected to result in specimen-damage comparable to that in normal
P. Kruit et al. / Ultramicroscopy 164 (2016) 3145 43

electron microscopy, an issue that was discussed recently in an- QEM if the number of round-trips is high. However, if the phase-
other paper from members of our collaboration [25]. If we con- shift is known or can be calculated, a commensurate phase-shift
sider real samples, this begs us to question how transparency is could intentionally be added to the reference beam to compensate
dened in electron microscopy. Samples can be opaque due to an for the phase-shift caused by the specimen. Consequently, there
interaction with the sample that destroys the coherence between may be potential for the development of additional operating
the reference and the sample beam, by large angle incoherent modes in the QEM system.
scattering for example. In addition to scattering, real specimens The designs of microscopes for interaction-free imaging pre-
also induce phase-shifts to the electron wave, which can alter the sented here are based on different ideas for a two-state-coupler:
a device that can bring electrons controllably from one state into
interference pattern produced at the coupler. In fact, it turns out
another state and back again by repeatedly passing the electrons
that a phase-shift results in a similar effect to an opaque pixel in a
through it. The four different types of couplers considered in this
work have been proven in principle to operate as electron beam-
splitters for coherent electron beams, however, their use to re-
combine spatially separated electron beams remains to be de-
monstrated. Consequently, the present discussion is intended to
help direct the development of such couplers. Note that we have
considered using an electron biprism as a coupler, since such a
device is able to direct part of a coherent electron wave function
into a separate beam, however we concluded that a biprism is not
able to slowly add more amplitude to a sample beam, which is a
requirement for the desired coupler. One of the problems we
foresee with the two-state couplers is that more than one (or two
as we need in some designs) side beam is created, thus disturbing
the principle. However, it may be expected that there is little
amplitude in these extra beams after one single interaction with
the coupler and thus, if these extra beams are blocked, very little
intensity will be lost from the experiment during each round-trip
in the resonator. The effect of small losses on such a measurement
has been discussed in a previous report by Kwiat et al. [17].
Another untested idea in the designs presented here is the
possibility of creating an electron resonator. Synchrotrons and
other particle accelerators prove that the injection of a particle
beam into a device that holds that particle for a long time is
Fig. 14. Schematic of a resonator system using the planar, on-chip, double-well possible; however, a design for such a device that is compatible
beam-splitter (green line centered above mirror). The chip acts as a coupling ele-
ment between the two arms of the electron resonator. The reference beam (thick
with present day electron microscopes is still outstanding. It is
blue line) enters the resonator through the barn door and is focused to the right clear that a compatible resonator device will require a fast
arm of the coupler (lower arm in Fig. 13(b)). The coupler reects the reference switching element to support both in-coupling and out-coupling
beam and transfers a small part of the amplitude into the sample beam (thin red of the electron-beam to and from the device. The design of a fast
line), which exits the left arm. Reference and sample beam are focused by the same
switching barn-door described here has been simulated and it
electron optics onto the (now closed) barn door plane, which also serves as the
sample plane in this scheme. Other optical designs where the sample is in eld free seems that the aberrations can be small enough to avoid dis-
space are also possible. (For interpretation of the references to color in this gure turbing the beam, but as we have stated a resonator has not yet
legend, the reader is referred to the web version of this article.) been demonstrated.

Fig. 15. Three concepts for coupling electrons in and out of the resonator structure: (A) At time 1 the potential V(z,t) on the entry barn door is lowered, such that the kinetic
energy of the electron is commensurate with entry to the resonator structure. After one reection from the exit barn door, the potential on the entry barn door has to be
raised sufciently to reect the electron. The electron can be out-coupled after multiple bounces at time 3 by lowering the potential applied to the exit barn door.
(B) Alternatively, the potentials on the resonator end caps can remain constant, if the kinetic energy of the electron is decreased sufciently at 1 and later increased again at
3. (C) Pulsed lateral deection constitutes another possibility to trap an electron within electrostatic resonator end caps.
44 P. Kruit et al. / Ultramicroscopy 164 (2016) 3145

If the proposed quantum electron microscopes are to achieve Acknowledgments


atomic resolution, it means that the focused electron probe should
be on the order of Angstroms in diameter and it should return to This research is funded by the Gordon and Betty Moore Foun-
exactly the same position after each cycle through the resonator. dation. The authors would like to thank M. F. Yanik, W. P. Putnam,
In the case of a thin crystal coupler, there is a greater challenge in J. Spence, F. Hasselbach and D. van Dyke for helpful discussions.
that the interference pattern of the reference beam and the sample
beam must be aligned to the atomic lattice that produced dif-
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