2 CHOLESTERIC LIQUID

CRYSTAL LASERS II

1.1 Introduction
1.2 Types Of CLC Laser
1.3 Lowering Threshold
1.4 Tunability
1.5 3D CLC Lasers
1.6 Conclusions
By Prof. Chia-Rong Lee
Liquid crystal Photonics lab.

1.4 Tunability
Wavelength tunability is one of the most attractive
features in CLC lasers. Since the DFB lasing occurs at
either or both of the edges of PBG, most of the cases
at the LWE, tuning of lasing wavelength is possible by
tuning the helical pitch.
There are many methods tuning the helical pitch:
(1) by changing temperature, (2) by applying electric
field, (3) by using light irradiation, and (4) by
applying mechanical strain (for polymer LC samples),
and (5) using spatial (position) tuning.

By Prof. Chia-Rong Lee

Liquid crystal Photonics lab.

1.4.1 Thermal Tuning

It is well known that the helical pitch in CLC sensitively
varies with temperature. Hence, thermal tuning was
achieved by many scientists even from the very
beginning.
(1) Quite wide range of tuning like 30-60 nm is possible
using single dye containing CLCs. However, the tuning
is not really continuous because of the surface pinning
of molecules.
* For the planar alignment (helical axis surface), surfaces
have to be homogeneously treated. Since the
molecular orientation at surfaces is fixed, number of
pitch is quantized to be multiple numbers of P/2.
By Prof. Chia-Rong Lee
Liquid crystal Photonics lab.

* If the helical structure with

pitch p was formed in the
sandwich cell of the thickness
d, the number of the helix
unit is d/p and is represented
by nd/ (by = np).
* When half the helix unit
disappears
due
to
the
elongation of the helical pitch,
the shift of the stop band
wavelength is given by,
(1.5)

By Prof. Chia-Rong Lee

Liquid crystal Photonics lab.

(2) To achieve real continuous tunability, devices with

helical axis parallel to the surface were examined.

By Prof. Chia-Rong Lee

Liquid crystal Photonics lab.

(3) A different method for continuously tuning lasing

wavelength was examined by Morris et al. They used
two different chiral dopants that exhibit opposing
dependences of the natural pitch on temperature
(dP/dT > 0 & dP/dT< 0). Tuning over 15 nm was
achieved using a 10 m thick cell. However, the
reason of the tunability in a cell, where the molecules
at both surfaces are fixed, is not clear. Moreover, the
cell quality might not be good judging from the wide
lasing emission peak (~2 nm).

By Prof. Chia-Rong Lee

Liquid crystal Photonics lab.

(4) Thermal tuning is also possible by using temperaturedependent chiral dopant solubility; that is, solubility of
chiral dopant increases with increasing temperature,
resulting in shorter pitch. Figure 1.14 shows the result.
Tuning over 60 nm was achieved.

By Prof. Chia-Rong Lee

Liquid crystal Photonics lab.

(5) Thermally tuning is also carried out in a defect-mode CLC

laser. Yoshida et al. fabricated a tunable single photonic
defect mode in a CLC based on inducing local
photopolymerization by two-photon excitation laser lithography.
The pitch elongated by a factor of about 20% and
became thermally stable after laser lithography, thus
creating a contrast in the pitch between the polymerized
and the unpolymerized regions, enabling the structure act
as a defect.
The author fabricated a structure with two polymerized
layers
sandwiching
an
unpolymerized
region
approximately ~0.7m wide, in which a single defect mode
was realized.
The defect mode wavelength was variable by 36 nm
upon heating the sample by 30oC and causing an
expansion of the polymer as well as a shortening of the
pitch in the unpolymerized region. These optical devices
may be used as tunable narrow bandpass filters or heat
By Prof. Chia-Rong Lee
sensors in integrated optical circuits.
Liquid crystal Photonics lab.

Tunable single photonic defectmode in cholesteric liquid

crystals
with
laser-induced
local modifications of helix

1.4.2 Electric Field Tuning

It is also well known that helical pitch can be tuned by
applying an electric field and is finally unwound under
sufficient field strength. However, again surface pinning
effect prevents the tuning of the helical pitch in cells
with the helical axis perpendicular to substrates.
(1) Yoshida et al. prepared wedge cells with the helical
axis parallel to substrates and examined the tunability
of lasing wavelength by applying an electric field. The
field strength linearly depends on the position. Using
such cells, position-dependent lasing wavelength
variation over 100 nm was obtained.

By Prof. Chia-Rong Lee

Liquid crystal Photonics lab.

Position sensitive, continuous wavelength

tunable laser based on photopolymerizable CLCs
with an in-plane helix alignment.

Materials: photopolymerizable CLC

(RMS03010, Merck), 1 wt %
photoinitiator
(irgacure 1850,Ciba),0.6wt%laserdye
(DCM).
Preparation: The sample was infiltrated
in a planarly rubbed wedge cell (width:
3.57.0m) cooled at 0.5oC/min from
the isotropic phase at 80oC to 25oC,
while applying a rectangular voltage of
30 V (1 kHz). This procedure allowed us
toobtainanin-plane helix alignment with
the helix axis lying in the direction parallel
to the rubbing direction.
Summary: TheChLC filmwithaninplane
helixalignmentisadvantageousoverthe
conventionalconfigurationthatit allows
continuous wavelength tuning and
emission of laser light in the cell plane
direction. Using photopolymerizable
materials is especially effective since a
freestanding film can be prepared, not
requiring any external voltage once it is
fabricated.
By Prof. Chia-Rong Lee
Liquid crystal Photonics lab.

(2) Electrotunability of the lasing wavelength of the defect

mode was also demonstrated using a layer of nematic
liquid crystal (NLC) inserted into dielectric multilayers
and CLC layers.
This is based on the fact that the wavelength of
defect modes continuously changes with the refractive
index of the defect layer. By applying an electric field, LC
molecules change the orientation, resulting in effective
refractive index.

By Prof. Chia-Rong Lee

Liquid crystal Photonics lab.

Electrically color-tunable defect mode

lasing in one-dimensional photonicband-gap system containing LC.

Fredericks
transition

By Prof. Chia-Rong Lee

Liquid crystal Photonics lab.

(3) (a) Another type of electrotuning was demonstrated by

Fuh et al. They used CLC with <0. By applying Edc along
the helical axis, the selective reflection band blue-shifts. By
applying an electric field of 150 V, lasing emission shifted
by 15 nm. The field-dependent helical pitch was attributed
to electrohydmdynamical effect.
(b) Similar but different observation was made by Park et
al. The sample used was NLCs embedded in helical
polymer networks consisting of photopolymerizable CLC.
With increasing E, transmittance spectra and color
viewed from substrate normal blue-shifts. The lasing peak
does not show any wavelength shift but just weakens.
With no E, lasing occurs in normal direction parallel to
helical axis. Surprisingly, under the field application, lasing
is generated to any angle up to 70 with the same
intensity as that in the normal direction. This phenomenon
was interpreted as a spatial undulation of helical axis by
Helfrich effect.

Electrically controllable omnidirectional

laser emission from a helical-polymer
network Composite film.

1.4.3 Phototuning
Several methods have been employed for wavelength tuning
by light irradiation.
Dispersing photoactive agents into the CLC matrix makes it
possible to adjust the pitch of the chiral structure by
irradiating the sample with UV light. Reports have shown that
wideband wavelength tuning can be achieved by adjusting
the exposure energy or time of the UV light. An increase in
tuning range has also been achieved by using two different
dyes, DCM and PM580, dissolved in a LC host.
Reversibility of phototunability can be achieved using
photochromic compounds with azobenzene substituents, in
which the transcis and cistrans conformation changes can
be induced using UV and visible light, respectively. Similar
optical tuning has been reported in defect-mode lasers
through a cistrans conformation change, resulting in a
contraction of the pitch in the defect layer relative to that of
the other two layers.

Light controllable tuning and switching

of lasing in CLCs (azo-chiral)

Azo-dyes

Trans-cis and cis-trans isomerization

h

120o

h, heat

N=N

N=N
Trans-isomer
(indark)

h > h

Cis-isomer

Curved cis-isomers have the ability to disturb LCs.

Matsui et al. have demonstrated based on numerical

analyses that the introduction and tuning of photonic
defect modes in the CLC can be realized by the local
deformation of the helix in the middle of the CLC layer.
The tuning of the defect mode can be performed by
both local elongation and shortening of the helix. By
elongation of the helix, defect modes show a red-shift,
and by shortening of the helix, defect modes show a
blue-shift. By controlling the degree of the modulation
of the HTP, a continuous shift of the defect modes can
be realized.

Their model can be applied to the optical control of the

defect mode in the CLC, and there is no need for a
complicated fabrication process such as an the
introduction of a isotropic thin layer, stacking of PCLC
films, and so on.
Based on this model, various applications can be
expected such as reversible tuning of the defect modes,
optical switches, and transient introduction and tuning
of the defect modes.
Such a spatially localized optical field can be attained
utilizing an interference of two laser beams. The tuning
of the defect modes can be realized on the basis of the
self-organizability of CLC. Utilizing these characteristics,
intelligent optical devices can be expected.

Tunable photonic defect

modes in a cholesteric liquid
crystal induced by optical
deformation of helix

1.4.4 Mechanical Tuning

Mechanical tuning has been reported for cholesteric
elastomers stretched laterally to contract the pitch.
Biaxial stretching of the elastomers gave a
corresponding change in pitch of up to 150 nm, resulting
in a change in laser wavelength from ~540 nm to 630
nm. Large shifts (~80 nm) in laser wavelength have
also been recently observed on biaxial stretching of a
chiral nematic polymer film.

Tunable Mirrorless Lasing

in CLC Elastomers
Blue

Green
Fig. 2. Change of R as function of the
thickness of the cholesteric LSCE due to
biaxial extension.

This result indicates that the pitch

deforms with the macroscopic
dimension of the network due to the
strong coupling between network
conformation
and
director
orientation.
Note that this effect does not
occur with liquid cholesteric
systems, i.e., low molar mass or
non-crosslinked polymeric LCs,
where the pitch stays (nearly)
constant with sample thickness.

Red

Fig. 1. Reflection appearance of the

CLC elastomer under white light
illumination as a function of biaxial
mechanical strain. The diameter of
the large circular sample chamber is
3.5 cm; the thickness of the
unstrained sample is 0.25 mm.

Fig. 3. Fluorescence spectrum of the

DCM dye and laser line in a dye-doped
LSCE sample.

Fig. 5. Laser emission from the DCMdoped LSCE sample.

1.4.5 Spatial Tuning

A variety of external stimuli have been employed to
control the helical pitch of CLCs. However, tunability is
generally restricted within a narrow wavelength range at
most 100 nm, and none of them supply tunability over the
whole visible range.
Chanishvili et al. and Huang et al. fabricated CLC
structures with a spatial helical pitch gradient and tried to
achieve lasing over a wide wavelength range.
(a) Chanishvili et al. used a spatial gradient of chiral
molecules, and succeeded in obtaining positiondependent lasing emission over the hole visible range.
Unfortunately, however, there was a small window,
where lasing was a possible. Moreover, six or more kinds
of dyes were necessary for wide-band sing.

Chiralconcentration
gradient

Lasing in dye-doped
cholesteric
liquid
crystals: two new
tuning strategies

Widely tunable ultraviolet-visible

liquid crystal laser

Smallwindow(nolasing)

(b) Huang et al. introduced temperature gradient across the

cell and used temperature-dependent chiral dopant solubility to
obtain the spatial-dependent pitch.
Since they used reactive monomers as a host and
polymerized, the pitch gradient was stable. However, the
tuning range was only 50nm because of the use of single
dye. Later, they succeeded in expanding the tunable
range to about 100 nm.

Spatially tunable laser emission in dyedoped photonic liquid crystals

Narrow tunable range partly originates from emission

bandwidth of the dye used. Actually, Chanishvili et al.
achieved a wide tunable range by using six or more dyes.
(c) Sonoyama et al. used two dyes, coumarin and DCM, and
succeeded in obtaining a wide tunable range covering the
whole visible range without a wavelength window showing no
lasing.
Necessary important points to obtaining a wide-banded
tunable DDCLC laser are summarized:
introduction of pitch gradient by temperature gradient,
introduction of concentration gradient of two dyes,
introduction of energy transfer between two dyes.

Lasing based on Frster transfer mechanism was

observedinCLCs usingcoumarin asasensitizer(energy
donor)andDOM asanemitter(energyacceptor).

spatial helical-pitch-gradient

Position-Sensitive Cholesteric
Liquid Crystal Dye Laser
Covering a Full Visible Range

31.0wt%chiral
dopant+
0.49wt%coumarin

20.8wt%chiral
dopant+0.49wt%
coumarin
+0.12wt%DCM

In the work of Sonoyama et al, the emission band of

coumarin dyes largely overlaps with the absorption band
of DCM dyes, so efficient energy transfer is expected.
Pumping light is absorbed by coumarin.
The gradients in both pitch and dye concentration are
important; at the shorter pitch region, emission of
coumarin cover this region, so the region must be rich in
coumarin. In the longer pitch region, on the contrary, the
wavelength corresponds to the emission of DCM. Hence,
this region must be rich in DCM. But at the same time, a
certain amount of coumarin is also necessary to absorb
pumping light. Finally, they succeeded in obtaining lasing
emission covering the whole visible range from 470 to
670nm by translating the cell with respect to a pumping
beam.

(d) Another important effort was to make the lasing device

temporally stable. Manabe et al. used photopolymerizable
CLCs and fixed the position dependent pitch and dye
concentration gradients by UV irradiation. Although the
pitch slightly blue shifted by polymerization, positiondependent lasing over a full visible range was preserved.
Toward practical application of cholesteric liquid crystals to tunable lasers

photocurable
CLC1+
0.4wt%C153

[photocurable CLC1
+0.1wt%DCM+
0.4wtC153]+
[photocurable
CLC2+NLC(2:1)+
0.1wt%DCM+
0.4wtC153]

Pump source: THG

pulseslightfroma
Nd:YAG
laser
converted
from
355 nm to 410 nm
through an optical
parametric
oscillator(OPO)

Pumpsource:THGpulseslight(355nm)
from a Nd:YAG laser using a different
prescriptionofmaterials.
28.8wt%
Chiral+
0.7wt%C460
+0.4wt%F555

22.3wt%
Chiral+
0.4wt%C460
+0.1wt%DCM

(e) Photopolymerized CLC lasers with a helical axis lying

within a substrate and with a pitch gradient were also
fabricated by Yoshida et al. In this case, the pitch
gradient was realized by applying an electric field across
wedged cells and fixed via photopolymerization. These
works opened the door of opportunity for a practical
application as disposable spatially-tunable dye lasers of a
film form.

(f) Lin et al. (C.-R. Lee group) developed a photoerasable

and photorewritable spatially-tunable laser using a DDCLC
with a photoisomerizable chiral dopant (AzoM). UV
illumination via a photomask with a transmittancegradient can create a pitch gradient in the cell such that
the lasing wavelength can be spatially tuned over a wide
band of 134nm.
The pitch gradient is generated by the UV-irradiationinduced gradient of the cis-AzoM concentration and
therefore the induced gradient of the cell HTP value,
resulting in the spatial tunability of the laser.
Furthermore,
the
laser
has
advantages
of
photoerasability and photorewritability. The spatial
tunability of the laser can undergo more than 100 cycles
of photoerasing and photorewriting processes without
decay or damage.

Prescription
ofDDCLC:
74.2wt%
NLC+
12.5wt%
chiral+12.6wt
%AZoM+
0.5wt%DCM+
0.2wt%P567+

Photoerasable and
photorewritable
spatially-tunable
laser based on a dyedoped cholesteric
liquid crystal with a
photoisomerizable
chiral
dopant

Fig. 4. (a) Two reversibly transformed

isomeric structures of AzoM in rod-like
trans- and bent cis-states and associated
isomerization reactions.

1.4.6 Multimode Lasing

We
sometimes
multiple lasing in

observed

(1) defect mode lasing from a

thick DDNLC defect layer
(100m)
inserted
between
PCLC layers
(2) simultaneous lasing of edge mode and defect mode
from a thin DDNLC defect layer (2m) inserted between
PCLC layers
(3) simultaneous lasing at both edges of PBG in a DDCL
(4) Frster couple system (donor C153+accepter P580 in CLC)
However, the wavelength range of multiple lasing
emission is limited within a very narrow range.

(5) Recently, Wang et al. obtained simultaneous nine lasing

peaks around a 600675 nm range. They prepared CLCs
doped with chiral dopant exceeding the dissolving limit.
As temperature increases, solubility increases and the
helical pitch becomes shorter. By increasing the cooling
rate, the number of defects and domains increases,
causing a multiple lasing.
(6) To achieve wide-range simultaneous multiwavelength lasing such as red (R), green (G), and
blue (B), a much sophisticated method to form widerange multiple reflection bands is demanded. Ha et al.
succeeded in obtaining RGB multiple reflection bands
using multilayered structures of single-pitch CLC layers
together with defect layers, and then in RGB
simultaneous lasing.

Simultaneous Red, Green, and

Blue Lasing Emissions in a
Single-Pitched
Cholesteric
Liquid-Crystal System

This
laser
is
unique
as
simultaneous RGB lasing occurs in a
single resonator using single-pitched
CLC with a single gain medium by a
single optical pumping. Furthermore,
each emission color of such lasings
could be controlled by adjusting
mixing ratios of two fluorescence
dyes in the gain medium and optical
pumping energies.

1.5 3D LC Lasers
Every LC laser mentioned so far has 1D cavity. One of
the 3D structures whose periodicity could be in the
visible range is obtained in the blue phase (BP).
The first lasing using a dye-doped BP was reported
by Cao et al. They actually observed different lasing
peaks from x, y, z directions.
Despite relatively low lasing threshold, the problem
of using BP is always the temperature range of the
phase. This problem was solved by Kikuchi et al. by
polymer stabilization. Using this technique, BP
temperature range becomes 60 K including room
temperature, although BP temperature range is usually
only 1 K or so. Using such polymer-stabilized BP, lasing
action was confirmed over 40 K.

Lasing in a 3D photonic
crystal of the liquid
crystal blue phase II

Laser Emission from a PolymerStabilized Liquid-Crystalline Blue Phase

In addition to the BP lasers, two types of LC 3D

resonators have been reported by Humar et al. Both
utilize LC droplets suspended in polymer matrices such as
polydimethyl-siloxane (PDMS).
Polymer dispersions of NLC droplets have been studied
extensively in the past, but individual droplets have never
been considered as tunable optical resonators.
(1) The first one is a microresonator of dye-doped NLC
droplets of about 10 m diameter. The POM observation
under crossed polarizers certifies the radial orientation of
the NLC director. When the NLC droplet was illuminated
at the edge by a focused laser beam, a bright spot was
observed at the other edge. In between, a light ring
along the circumference of the microcavity was clearly
visible. These observations clearly indicate whispering
gallery modes (WGMs). Actually, they succeeded in
observing spectra of WGMs circulating in a LC droplet.
From the line width (about 0.055 nm), Q factor of the
order of 12,000 was obtained.

Lasing has not been reported using WGMs of this droplet.

However, lasing capability using WGMs is well known
in other systems, so lasing in LC WGMs is surely
possible.
Moreover, by deforming the sphere slightly, highly
unidirectional lasing action would be possible, while
lasing emission of WGMs of perfect sphere always
emits tangentially. Another important aspect of the
WGMs from LC microdroplets is tunability. By applying
an electric field, director orientation in the droplet
changes as shown in Figure 1.20b and c. Linear and
reversible electrical tuning was obtained, and the
tuning range could be over 40 nm by choosing proper
LC materials.

Electrically
tunable
liquid
crystal optical microresonators

Figure 2 Spectrum of light circulating in a liquidcrystal

droplet. a,AsinglesetofWGMresonancesisobservedina
10.1 m droplet of E12 in PDMS, corresponding to the
lowestradialmodes(n=1)withTMpolarization.b,Inalarger
radial birefringent droplet (12.6 m) second radial modes
appearwithn=2.TheinsetshowsdetailsofaWGMspectral
line in a 53 mdiameter E12 droplet. The linewidth is
approximately0.055nm,andtheLCcavityQfactor isofthe
order of 12,000. This spectrum was measured using a high
resolutionmicroRamanspectrophotometer.

Advantages

simplicityofselfformation
surprisinglyhighQfactor
largeresponsetoexternal
stimuliincludinglowelectricfields
asvoltagetunableoptical
microdevices,surfacesensitive
sensors,tunablemicrocavity lasers
andsoftmatterphotoniccircuits.

(2) The second type of LC 3D resonator was formed by

using CLC microdroplets. By using glycerol, the director
is parallel to the interface of the droplet. Then, the
formation of 3D helical structure with radial helical
axes could be imagined. Lasing condition is the same
as that in 1D DFB CLC lasers.
Although the size of microdroplets cannot be
controlled, lasing wavelength is uniquely defined by
the helical pitch. An important point is that only dyes
located at the center of droplets contribute to the
lasing action (Figure 1.21), because the light emitted
at the center is confined three dimensionally due to the
radial helical axes; omnidirectional lasing emission
occurs toward all the radial directions. Temperaturedependent helical pitch can also be used for tuning the
laser light wavelength as in 1D DFB CLC lasers.

3D microlasers from self-assembled

cholesteric liquid-crystal microdroplets

Fig.5. (a)Lasingintensityfromasingle50
m CLCdroplet as a function of the angle
of rotation of the photodetector around
the axis of the cylindrical tube, containing
the microdroplets. (b) Lasing spectra as a
function of temperature. At higher
temperatures the laser line is shifted
outsidetheoptimumwavelengthregionof
thedyeused,sothelaseremissionceases.

1.6 Conclusions
It has been more than 30 years since the first observation
of CLC laser emission in 1980. This field has been
expanding rapidly particularly since Kopp et al. published
a paper.
In this chapter, we focused on the most typical LC lasers,
CLC microlasers. First, we described two kinds of CLC
microlasers. DFB and defect mode lasers. Next, extensive
efforts to lower the lasing threshold were summarized.
They are classified into 3 kinds of improvements --- cavity
structures, excitation conditions, and materials.
Methods for tuning lasing wavelength, which is the
most important feature of CLC lasers, were described. We
can use variations in temperature, electric field, and light
irradiation. Mechanical strain for polymer samples, spatial
tuning for wide wavelength tuning, and multiple lasing
over a wide wavelength range were also described.

The readers may also refer recent review article.

Tunability is not only for wavelength, but also possible
for polarization and directions, which I did not included
in this chapter.
3D lasing is the most recent topic and provides us with
promising devices. Much more application areas can be
expected in 3D lasers such as telecommunications,
optical computing, imaging devices, apparel and
decoration (), sensors, and biological imaging.