Communication

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A Compact Full 2π Flexoelectro-Optic Liquid Crystal Phase

Modulator
Xiuze Wang, Julian A. J. Fells, Yuping Shi, Taimoor Ali, Chris Welch, Georg H. Mehl,
Timothy D. Wilkinson, Martin J. Booth, Stephen M. Morris,* and Steve J. Elston

modulators (SLMs). While optical MEMS-

Wavefront shaping, which is often achieved using liquid crystal (LC) spatial based phase modulators generally exhibit
light modulators, is particularly important for a wide range of applications very fast response times, they are often
including laser microfabrication and micromanipulation, microscopy, and characterized by a low number of pixels,
making it more challenging to accurately
quantum optics. In this work, results are presented for the first integrated LC
compensate for higher order aberrations.[6]
phase modulator that combines a flexoelectro-optic LC layer (that behaves LC materials, on the other hand, can
as a switchable λ/2 waveplate) with a polymerized reactive mesogen layer exhibit a variety of electro-optic effects. By
(which acts as a λ/4 waveplate) and a mirrored substrate that creates a combining the merits of high-performance
double-pass geometry. For a flexoelectro-optic LC layer that exhibits switching complementary metal oxide semicon-
ductor (CMOS) technology with the various
angles of ±45° at a voltage of ±85 V a full 2π phase modulation is observed
electro-optical properties of LC materials,
when driven by a 1 kHz waveform. Experimental results are also compared LC-based SLM technologies are able to sup-
with modeling using Jones calculus of the amplitude and phase variation port a large number of pixels to provide
when the LC and the polymer layer deviate from their desired waveplate high resolution across a wave-front in a
conditions. The development and demonstration of an integrated device is compact technology. This high-resolution is
particularly significant for applications where size and cost are critical factors a key advantage of LC-based SLMs in com-
parison with other technologies. However,
such as in LiDAR for the Space and Automotive industries, respectively.
the technology often suffers from either
slow response times (nematic LC) or binary
phase modulation (chiral smectic C).[7–10]
Applications such as holography, beam steering and shaping, Approaches based upon 2D materials have been considered
aberration correction, and super-resolution optical microscopy as an alternative candidate for phase modulation technology.[11–14]
rely heavily upon technologies such as optical phase modula- As examples, an 8π phase range all-optical phase modulator has
tors.[1–5] Several technologies exist that can be used to modu- been reported which relies on using a strong photothermal
late the phase of light, such as optical microelectromechanical effect in phosphorene[11] whereas an antimonene-based optical
systems (MEMS) and liquid crystal (LC)-based spatial light modulator has been developed that can provide fast phase (up
to 16π) and intensity modulation at the same time.[14] However,
these technologies still have their limitations such as relatively
X. Wang, Dr. J. A. J. Fells, Y. Shi, T. Ali, Prof. M. J. Booth, slow response times (e.g., milliseconds) or relatively high pump
Prof. S. M. Morris, Prof. S. J. Elston
Department of Engineering Science powers, which may not be desirable for some practical applica-
University of Oxford tions. Developing new types of phase modulators that possess
Parks Road, Oxford OX1 3PJ, UK fast response, analog phase modulation, and low driving voltage
E-mail: stephen.morris@eng.ox.ac.uk is particularly important for applications such as beam-steering
Dr. C. Welch, Prof. G. H. Mehl in optical communications[3] and real-time holography.[15]
Department of Chemistry
University of Hull
Flexoelectro-optic chiral nematic LCs have been shown to
Hull HU6 7RX, UK be a promising candidate for phase modulation owing to the
Prof. T. D. Wilkinson fast-switching times and the analog control of the tilt angle of
Department of Engineering the optic axis.[16] The flexoelectro-optic effect can be observed
University of Cambridge when an electric field is applied perpendicular to the helical
9 JJ Thomson Avenue, Cambridge CB3 0FA, UK axis, resulting in a deflection of the optic axis from the unper-
The ORCID identification number(s) for the author(s) of this article turbed helical axis in a plane that is orthogonal to the applied
can be found under https://doi.org/10.1002/admt.202000589.
field direction.[17–22] For conventional devices with transverse
© 2020 The Authors. Advanced Materials Technologies published by Wiley- electrodes, a uniform lying helix (ULH) geometry is required
VCH GmbH. This is an open access article under the terms of the Creative to ensure that the field direction is orthogonal to the helix axis.
Commons Attribution License, which permits use, distribution and repro-
duction in any medium, provided the original work is properly cited.
The response time of the flexoelectro-optic effect can be of the
order of 100s of microseconds when the pitch of the chiral
DOI: 10.1002/admt.202000589 nematic LC is short (<500 nm).

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Recent work has shown that the flexoelectro-optic effect not precisely measured, but the thickness of the region where
can be used to achieve full 2π phase modulation when chiral the device shows the appropriate phase modulation has been
nematic LCs with large tilt angles (>45°) of the optic axis are estimated from the results presented in this paper (vide infra).
combined with a λ/4 waveplate and a reflector that both pre- The silver layer on the bottom substrate has two functions in
serves the handedness of circularly polarized light and creates the device: 1) it acts as a reflector for the incoming light so
a double-pass geometry.[23,24] The optical field component of as to increase the modulation depth by creating a double-pass
the light at the output of the device (Eout) after passing through through the LC layer, and 2) it acts as the bottom electrode,
all of the optical components can be expressed in terms of the which together with the top ITO electrode, facilitates the appli-
input optical field component (Ein) as Eout = Ein e+4iϕ, where the cation of an electric field across the chiral nematic LC layer so
total phase change is four times the switching angle, ϕ. There- as to initiate flexoelectro-optic switching.
fore, a 45° tilt angle, which equates to ϕ = ±45° (as the optic axis An experimental challenge that is encountered when fab-
tilts in opposite directions for opposite polarities of the applied ricating the proof-of-concept device is the necessity for the
electric field), leads to a 2π phase modulation. polymer and LC layers to form λ/4 and λ/2 waveplates, respec-
Achieving full 2π phase modulation has been made possible tively, at the desired wavelength. This requires precise control
by the development of LC compounds such as 4′,4′-(heptane- of the thickness of the layers, which is non-trivial. To relax the
1,7-diyl)bis(([1′,1″-biphenyl]-4″-carbo-nitrile)) (CB7CB), which constraints on the thickness, the polymer and LC layers were
exhibits switching angles in excess of ±45° when it is doped with fabricated so that each layer formed a wedge shape (as illus-
a small concentration of high twisting power chiral dopant.[25–29] trated in Figure 2). The subsequent orientations of the wedged
A drawback with the configurations described in refs. [23] polymer and LC layers were orthogonal to each other, allowing
and [24], however, is that numerous optical components were a region to be found where the polymer and LC layers function
required, which makes the current arrangement impractical for as a λ/4 waveplate and a λ/2 waveplate, respectively.
many device applications as the overall thickness is rather large. The purpose of the wedge-shaped design of the PF layer
For example, in ref. [23] an LC cell with a nominal gap of 5 µm and the LC layer was to enable the correct thicknesses to be
was used as the tunable λ/2 waveplate and standard bench-top found. However, this also meant that there were many different
optical components in the form of λ/4 waveplates and mirrors thickness combinations across the device. Deviation from the
were needed to build the phase modulation system. Furthermore, desired waveplate conditions results in both phase error and
the numerous free-space components result in multiple inter- variation in the amplitude loss and to demonstrate this experi-
faces and therefore unwanted reflection losses. Before this tech- mentally light was passed through a region of the device in
nology can be deployed into real systems, the optical components which neither the thickness of the PF layer nor the LC layer
need to be integrated into a compact package so that the overall correspond to their correct values for achieving a λ/4 and λ/2
device thickness is comparable with existing SLM devices. waveplate, respectively. Toward this end, the integrated device
In this paper, a prototype-integrated phase modulator exhib- was placed on a Michelson interferometer as shown in Figure 3
iting the desired phase modulation of 2π with a frame rate of and the measured phase and normalized amplitude loss varia-
1 kHz is demonstrated by combining a flexoelectro-optic LC tion from this region of the device where the waveplate condi-
layer, a birefringent polymer film (which acts as the λ/4 wave- tions were not satisfied, as determined from the interference
plate), and a mirror all in one compact package. The reduction fringe images using MATLAB, are presented in Figure 4.
of the individual components into a single device represents The flexoelectro-optic LC layer was modeled as a waveplate
an important step forward in terms of development toward the with an optic axis in a plane that is normal to the incident
realization of a flexoelectro-optic optical phase modulator. beam. The optical field at the output, Eout, of the integrated
The basic structure of the integrated device is illustrated in system including the linear polarizer and λ/4 waveplate (the
Figure 1. Briefly, the device consists of (omitting the alignment components in the dashed blue line in Figure 3) is given by
layers) a 100-nm thick silver layer that is coated onto a glass
substrate, a reactive mesogen polymer film (PF) that acts as a  π  π π  π 
E out = PQ 1 −  D (−ϕ ) Q 2 −  MQ 2   D (ϕ ) Q 1   PE in (1)
λ/4 waveplate, a tunable flexoelectro-optic LC layer that behaves  4  4 4 4
as a λ/2 waveplate, and a top glass substrate that is coated with
indium tin oxide (ITO). The total thickness of the device was where Ein is the Jones vector for a vertically polarized light at
π 
the input, P is a vertically aligned linear polarizer, Q 1   is the
4
Jones matrix for a λ/4 waveplate at π/4 to the vertical, D(ϕ) is
the Jones matrix of the flexoelectro-optic LC layer with a retard-
ance, δ, and optic axis that is oriented at an angle, ϕ, to the ver-
π 
tical axis and Q 2   is the Jones matrix for the PF layer, which
4
has a retardance of ξ to allow deviation from the optimum λ/4
waveplate condition, and M is the Jones matrix for a mirror.
Note that in the terms after the mirror (i.e., terms to the left of
M in Equation (1)) the orientation angles of the waveplates are
Figure 1.  Device architecture of the “integrated” flexoelectro-optic LC reversed because the system has a mirror symmetry configura-
modulator. tion and the light is now propagating in the opposite direction.

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Figure 2.  Schematic illustrating the key steps in the procedure for fabricating the integrated device and the formation of wedge-shaped geometries for
the polymer retarder (blue layer) and flexoelectro-optic LC (red layer) layers to achieve λ/4 and λ/2 waveplate behavior, respectively. The color scheme
used for the different layers is the same as that used in Figure 1.

In this example of a non-optimal region of the device, there PF layer set to ξ  =  0.38 waves and the retardance of the LC
is almost a 50% variation in the amplitude across the full range layer set to δ = 0.8 waves. With these values of ξ and δ, both the
of switching angles (±45°). The red dash lines in Figure 4 shows simulated phase and loss variation show close correlation with
simulated results from Equation (1), with the retardance of the the experimental data. Although there is a significant deviation
from the ideal values of ξ = 0.25 waves and δ = 0.5 waves, the

Figure 3.  Michelson interferometer arrangement to measure the phase

and intensity response of the integrated LC optical phase modulator: (SH)
shutter; (NDX) neutral density filter of optical density X; (VND) variable
neutral density filter; (PC) personal computer; (PS) power supply; (AMP) Figure 4.  Experimental (blue lines) and modeling (red dashed lines)
voltage amplifier; (TC) temperature controller; (CAM) CCD camera; (DUT) results for the amplitude loss variation and the phase error as a function
device under test; (P) linear polarizer; (Q1) λ/4 waveplate; (L1) lens; (LC) of the absolute angle of the optic-axis of the flexoelectro-optic device rela-
liquid crystal layer; (PF) reactive mesogen polymer film; (S) silvered sub- tive to the vertical axis. These results are an example case of when the
strate; (M) mirror; (BS) non-polarizing beam splitter. The components PF was not a precise λ/4 waveplate and the switchable LC layer does not
highlighted by the red-dashed line represent the integrated device (ID). fulfil the condition of a λ/2 waveplate.

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flexoelectro-optic tilt angle that is not linear with voltage at high

amplitudes and small drifts in environmental temperature,
which lead to measurement error. Nevertheless, the results
show that by combining a reactive mesogen polymer film with
a chiral nematic layer operated in a flexoelectro-optic mode it
is possible to achieve full 2π modulation of the optical phase
when subjected to 1 kHz switching frequencies.
There are important key characteristics of the phase modu-
lator which we can comment on. One is the optical efficiency
of the device, which was found to be around 20% to 40%,
depending upon the ULH alignment quality. The relatively
low efficiency is due to scattering from non-uniformities in the
lying helix alignment of the LC phase modulation layer, but it is
anticipated that the maximum efficiency could be significantly
improved through the use of high-quality ULH alignments
Figure 5.  Experimentally determined phase for the integrated LC optical such as those formed using solvent-assisted processes.[30] Addi-
phase modulator presented in this work (measured using the Michelson
interferometer presented in Figure  3). The main plot shows the optical
tionally, we can consider the Figure-of-Merit (FoM) for the mod-
phase shift as a function of the applied peak-to-peak voltage (Vpp). The ulator, as introduced by Khoo and Wu.[31] For nematic-based
red solid data points represent experimental measurements where the devices this parameter can be defined as
RM polymer and LC layers function as λ/4 and λ/2 waveplates, respec-
K 11 ( ∆n )
2
tively, and the dashed line is a line of best fit. The inset contains an upper
fringe pattern and a lower fringe pattern. Each fringe pattern corresponds FoM = (2)
to a specific voltage level and the phase difference can be obtained by
γ1
comparing the position of the upper and lower fringe patterns.
where K11 is the LC splay elastic constant, Δn is the optical ani-
sotropy, and γ1 is the rotational viscosity. Unfortunately, this
device still functions as a phase modulator, but at the expense definition does not relate directly to the electro-optic effect that
of unwanted amplitude modulation and a reduction in linearity we employ in this study. However, if we note that the switching
of the phase response. time of a nematic layer of thickness d can be characterized as
Figure 5, on the other hand, shows experimental results for
light passing through an optimal area of the integrated device, γ 1d 2
τ= (3)
where the thickness of the LC layer is close to that required for K 11π 2
a λ/2 waveplate (nominally 5 µm) and the thickness of the PF
is close to that required for a λ/4 waveplate (7  µm). Example then we can re-write the FoM as
images of the interference fringes captured on the CCD can
1 ( ∆n·d )
2
be seen in the inset of the figure. In this exemplar case, the
FoM = · (4)
phase range was found to be almost 2π when the applied peak- τ π2
to-peak voltage reached 170 Vpp (±85 V). The response time was
not directly measured for this integrated device (it was faster For our device Δn · d is close to a half-wave at λ = 632.8 nm.
than the frame-rate of the CCD camera). However, from the The switching time varies with voltage, but is typically around
measurement of the switching times for the same mixture in 0.5  ms. Putting these values into Equation  (4) leads to an FoM
a commercially-available glass test cell (Instec, 5 µm-thickness), of 20 µm2 s−1. By way of comparison, for a standard nematic
the response time was estimated to be around 500 µs. Here material, such as the eutectic mixture, E7, the FoM is found to
the voltage required to achieve 2π is found to be substantially be approximately 4 µm2 s−1. However, care must be taken when
larger than that observed in our previous studies: it should be making such a comparison because the electro-optic mechanisms
noted that even though the voltage is relatively large, for this used are fundamentally different in the two cases. For example, in
switching range the ULH helix does not unwind, and there- the nematic case the “switch-on” time is controlled by γ1/(ΔεE2),
fore the changes in the birefringence are small).[23,24] The pri- where Δε is the dielectric anisotropy and E is the applied electric
mary reason for this higher driving voltage requirement is that field, whereas the “switch-off” time is controlled by γ1d2/K11,[32]
the thickness of the device is considerably greater than that so the switch-on time is field dependent and the switch-off time
employed in previous studies as the electric field was applied is device thickness dependent. In contrast, for flexoelectro-optic
not just across the LC layer but also the λ/4 polymer retarder switching, the response time is controlled by γ1p2/(K11  + K33),
and the numerous alignment layers. To confirm that this was where p is the helix pitch and K33 is the bend elastic constant, so
the case, the LC mixture was also filled into a commercially the switching time is independent of electric field, but strongly
available glass cell (5  µm-thickness, Instec). In this case, a dependent on the helical pitch of the material. Nevertheless, in
driving voltage of ±34 V was required to achieve ±45° switching. both cases, Equation (4) illustrated that the FoM depends on the
The results presented in Figure 5 also show that the depend- ratio of the square of the required retardation to the switching
ence of the phase modulation on the applied voltage follows an time, and in that sense, comparing the metrics is useful.
almost linear behavior. However, a small deviation from line- There are two key operational bandwidths which can be
arity is observed and is believed to be the combined result of a considered in this experiment. One is the optical spectral

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bandwidth over which the device can be operated, the other is substrate using spin-coating (2000 rpm, 1 min), which was subsequently
the electro-optic switching speed bandwidth. The device is nor- aligned through exposure to a polarized UV light source (λ  = 365  nm,
power density = 5 mW cm−2 and the curing time was 10 mins).[33]
mally designed to operate at a specific wavelength (in our case
The two substrates were then assembled to form a wedge-cell by
λ = 633 nm) where the LC layer with appropriate thickness will using 6  µm spacer beads on one side of the glass substrate and no
work as a half-waveplate and the RM layer in front of the mirror spacer beads on the other side (the actual wedge spacing was not
is a quarter-wave thick. Variation in the wavelength (over a measured). For the λ/4 polymer retarder, a reactive mesogen (RM) LC
spectral bandwidth) will effectively result in errors in the phase mixture (98 wt% RM257 and 2  wt% IRG819) was opted for, which was
modulation and variation in the intensity when switching. The capillary filled into the glass cell before being placed on a hot-stage
effect of this can be seen in Figure  4. This is shown here as that was set to a temperature of 80 °C. Following this, the sample was
exposed to UV light for 40 min at a power density of 100 cm−2 to cross-
“non ideal” conditions in the layer thicknesses, but is equivalent link the RM layer. The device was then soaked in water for one day to
to changing the wavelength to around 400  nm. As noted, the dissolve the SD1 layer so that the upper substrate could be removed,
electro-optic switching speed for the material used in this study leaving a reflective substrate coated with a λ/4 waveplate (3).
was around 500 µs, leading to a 1 kHz bandwidth (assuming an An ITO glass substrate with a photo-aligned SD1 film was prepared
equal duty-cycle switching waveform). while a layer of SD1 was also coated on the top of the polymer film on
This work has successfully demonstrated an integrated LC the mirrored substrate to promote the alignment of the chiral nematic
LC. During the process, it was found that the SD1 does not easily spread
optical phase modulator based on the flexoelectro-optic effect of
on top of the polymer film. In order to improve its wettability for SD1,
a chiral nematic LC aligned in the ULH mode which exhibits a the top surface of the polymer film was treated in a UV Ozone Cleaner
2π phase range with a frame rate of 1 kHz with the assistance of (Ossila E511) for 5 min, which ensured that the SD1 could be coated
an additional λ/4 waveplate placed before the integrated device, onto it. The two substrates (one was the SD1-coated RM layer substrate
which comprises an LC layer consisting of chiral nematic LC and and the other was the SD1-coated ITO substrate) were then assembled
a birefringent polymer film. Although the precise thickness of the to form a cell with a wedge geometry in two orthogonal directions:
one axis consisted of a wedge in the polymer layer (y-axis) whereas
whole device was not determined, the approximate thickness of
the glass substrates were assembled in such a way as to form a wedge
the “working” region can be estimated from the driving voltages. along the x-axis. Once constructed, the cell was then filled with the
As noted above, a driving voltage of ±34 V is required to achieve chiral nematic mixture, CB7CB + 3  wt% BDH1281 (high twisting power
±45° switching across a 5  µm thick layer of material. Therefore, chiral dopant supplied from Merck Ltd.) to form the integrated device
our required driving voltage of ±85  V for the integrated device (4). The LC mixture was found to exhibit a right-handed chiral nematic
suggests an overall thickness for the LC layer and waveplate of phase between 106 and 113 °C (on heating). The pitch (p) of the mixture
around 12.5  µm. The operating condition for this device is cur- was found to be approximately p  ≈ 210  nm, which was estimated from
the spectral position of the reflection band, measured using a UV–vis
rently ±85 V at a temperature of 108 °C but could be reduced with spectrometer (Agilent 8454), and the refractive indices quoted in ref. [34]
further material optimization, such as the mixtures presented in at the measurement temperature. The quality of the ULH texture was
the work of Varanytsia and Chien.[25,26] Additionally, the device we investigated using polarizing optical microscopy and was found to be
developed shows a response time that is quite fast for analogue similar to that reported in previously published work.[29] The full device
phase modulation, with potential operational speeds of more than stack showing the orthogonal wedge directions is shown in (5).
1 kHz. This integrated device has substantial potential in spatial Phase Modulation Measurements: The phase modulator device was
placed in a Michelson interferometer to measure the optical phase
light modulator technology, enabling full 2π phase modulation
shift as shown in Figure  3. The light source was a continuous wave
with low-intensity modulation to be achieved. Development into Helium–Neon (He–Ne) laser (Uniphase 1125P) that generated light at
a pixelated spatial light modulator would have a range of appli- a wavelength of 632.8  nm. The input light first passed through a non-
cations in optical wave-front engineering and optical light-beam polarizing beam-splitter (Newport 05BC16NP) via the aid of mirrors
steering in areas such as optical communications. before being split into two components. One of the output beams from
the beam-splitter (the signal beam) passed through the integrated device
and is reflected back toward the beam-splitter. As the chiral nematic
phase of the device was at elevated temperatures (between T = 106 and
113  °C), a temperature-controlled hot-stage was required to allow it to
Experimental Section be operated in the chiral nematic phase. The LC layer was aligned in
Device Fabrication: The procedure employed to fabricate the device the ULH geometry (with SD1 working as the alignment layer) by cooling
is presented schematically in Figure  2. A glass substrate (1  mm-thick) from the isotropic phase in the presence of an electric field (≈2 V µm−1)
was first cleaned using acetone and a UV Ozone Cleaner (Ossila Corp.) and mechanically rubbing the device with a blunt instrument to promote
and then coated with a silver film that was approximately 100  nm-thick the lying helix alignment. Monodomains of ULH alignment were found
using thermal evaporation (Syskey Technology Corp.) (1). The thermal to be 150 × 150 µm2 in size, in accordance with the results presented in a
evaporator was situated in a glove box (MBraun Labstar) and subjected previous study for a comparable LC layer (in this experimental device the
to a nitrogen atmosphere and an internal pressure of 2  × 10−6 Torr. The ULH alignment was not stabilized by a polymer network).[29] Before the
deposition was performed at a rate of 0.1  nm s−1, which was monitored integrated LC device, a linear polarizer and λ/4 waveplate were included
using a quartz-oscillation thickness monitor. The silver was deposited to generate circularly polarized light before a lens L1 focused the
through a shadow mask resulting in an active area of approximately incoming light into a monodomain region of the device. The other
21 mm × 23 mm. After deposition of the silver coating, a thin poly-vinyl output beam (the reference beam) was directed toward two mirrors to
alcohol (PVA) layer (PVA was dissolved into water to form a 0.5 wt% PVA reflect the light back with a small angle offset so as to generate clear
solution in water) was deposited on top of the silver film using a spin- interference fringes at the CCD camera. The fringes were captured by
coating process at a rate of 1000 rpm for 2 min before being mechanically using a collection lens to image directly onto a CCD camera (Thorlabs
rubbed with a rubbing machine to form the first of two uniaxial alignment DCU224C, 1280  × 1024, 8-bit color). The fringe period was estimated
layers for the polymer λ/4 retarder (2). For the other alignment layer, a from the small angle introduced between the signal and reference beams
second glass substrate was prepared and a thin film of the sulfonic of the Michelson interferometer to be approximately 30 µm, resulting in
photoalignment material, SD1, was deposited onto the bare glass a number of fringes across any individual ULH domain.

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