CsPbBr3nanowire polarized light-emitting diodes through mechanical rubbing

Article abstract of DOI:10.1039/c9cc10033d

Anisotropic films composed of aligned CsPbBr₃nanowires (NWs) have been successfully fabricated using a mechanical rubbing method. The films with a dense and uniform morphology show polarization photoluminescence (PL) behavior. Combined with an optimal device structure, a polarized light-emitting diode (LED) with a turn-on voltage as low as 6.5 V was obtained.

Full text of DOI:10.1039/c9cc10033d

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CsPbBr3 nanowire polarized light-emitting diodes through
mechanical rubbing
Received 00th January 20xx,
Accepted 00th January 20xx
Yaping Wei, ab Yinyan Xu, ab Qian Wang, ab Jianyue Wang, ac Hongbo Lu, *ab Jun Zhu, *ab
DOI: 10.1039/x0xx00000x
www.rsc.org/
 2 cm.25 However, most of available reports only investigated PL
polarization, and did not pay attention to electroluminescence (EL)
polarization. Nearly no electroluminescent application of this
material on polarized LEDs has been reported as far as we know.
Until now, a few methods have been used to obtain anisotropic
Anisotropic films composed of aligned CsPbBr3 nanowires (NWs)
have been successfully fabricated using a mechanical rubbing
method. The films with dense and uniform morphology show
polarization photoluminescence (PL) behavior. Combining with an
optimal device structure, a polarized light-emitting diode (LED)
with a turn-on voltage as low as 6.5 V was achieved.
films with good orientation for one-dimension inorganic
27
nanomaterials,
template-assisted assembly
mainly
containing
electrospinning,25,
and mechanical stretching.22, 23
13, 28, 29
Over the last several years, perovskite nanocrystals (NCs) have
drawn significant interests for their promising applications in
diverse fields, including light-emitting diodes (LEDs),1, 2 solar cells,3
photodetectors,4-6 lasers,7-9 and so on. Behind the many
applications is their excellent nature, such as superior
photoluminescence (PL) property, large absorption coefficient, long
carrier diffusion length, solution-processability, and low cost. Over
and above these features, anisotropic perovskite NCs can show
polarized emission10-14 that making it use for polarized LEDs.15 Since
a high degree of molecular alignment is essential to the generation
of polarized light, the fabrication of well-aligned anisotropic
perovskite NCs is a prerequisite for the practical use of perovskite in
polarized LEDs. Among a series of anisotropic perovskite NCs such
as nanoplatelets,16, 17 nanowires (NWs),18, 19 and nanorods (NRs),20
perovskite NWs may be the most promising one.
However, there are still many difficulties to integrate the fabricating
process of oriented anisotropic films into the LED preparing
process.
In this communication, we first synthesized CsPbBr3 NWs using
the hot-injection method and then prepared the anisotropic films
composed of oriented NWs by facile mechanical rubbing method.
CsPbBr3 NW polarized LEDs were achieved by optimizing the device
structure and the device performance was enhanced by improving
the morphology of anisotropic films.
There have been some reports on polarized PL properties of
anisotropic perovskite NCs recently.21-26 Wang et al studied the
polarization characteristics of full inorganic perovskite CsPbX3
quantum dots (QDs). The CsPbI3 QDs were observed to have a
degree of polarization up to 0.36 in hexane solvent and 0.40 in
film.11 Polarized fluorescent films have also been prepared using
perovskite NCs blended with polymers. By electrospinning
perovskite precursor solution mixed with polyvinylalcohol (PVA),
Meng et al achieved well-aligned MAPbBr3@PVA nanofibers with
the degree of polarization of 0.42 for the anisotropic film of 0.5 cm
Fig. 1 Schematic diagram of the preparing process of oriented
CsPbBr3 NW films by mechanical dry rubbing and mechanical wet
rubbing.
CsPbBr3 NWs were synthesized following the method reported
by Zhang et al19 and characterized using the UV-vis absorption
spectroscopy, PL spectroscopy, X-ray diffraction (XRD) and
transmission electron microscopy (TEM) (Fig. S1-3, Supplementary
Information). From the TEM images, most of CsPbBr3 NWs are 10
nm wide and present as bundles due to the strong ligand-ligand
intercalation.30 The synthesized CsPbBr3 NWs were dispersed in
hexane solvent for further application.
a National Engineering Lab of Special Display Technology, State Key Lab of
Advanced Display Technology, Academy of Opto-Electronic Technology, Hefei
University of Technology, 193 Tunxi Road, Hefei, 230009, China.
Email: bozhilu@hfut.edu.cn, jzhu@hfut.edu.cn
bAnhui Provincial Key Laboratory of Advance Functional Materials and Devices,
School of Chemistry and Chemical Engineering, Hefei University of Technology,
193 Tunxi Road, Hefei, 230009, China.
Mechanical rubbing method was employed here to achieve
oriented anisotropic films of CsPbBr3 NWs due to its easy process. It
was usually carried out by a cloth on a cylinder rotating in contact
CSchool of Electronic Science and Applied Physics, Hefei University of Technology,
193 Tunxi Road, Hefei, 230009, China.
†Electronic Supplementary Information (ESI) available: See
DOI: 10.1039/x0xx00000x
This journal is © The Royal Society of Chemistry 20xx
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with the polyimide film substrate. There have been some reports
The polarization PL properties were then VieinwvAertsictliegaOtnelinde.
that prepared anisotropic films composed of one-dimension Polarization of an incoherent light source iDsOcIh: a10ra.1c0t3e9r/iCze9dCCb1y00b3o3tDh
31
inorganic nanomaterials using mechanical rubbing method.15,
the contrast ratio (CR) and the degree of polarization (ρ). ρ can
Here we adopted two kinds of strategies for fabricating the theoretically take a value between 0 (unpolarized) and 1 (polarized),
oriented films, wet rubbing and dry rubbing, which are rubbing the CR and ρ are determined from the spectra using equations (1) and
drop-casted CsPbBr3 films using Chinese brush (Fig. 1) before and (2), respectively.
after the solvent is evaporated respectively. The alignment
direction of the NWs is random in the drop-casted CsPbBr3 films (Fig.
2a-b), while both wet rubbing (Fig. 2c-d) and dry rubbing (Fig. 2e-f)
produce oriented NWs whose direction is according with the
rubbing direction. The rubbed CsPbBr3 NW films are uniform and
densely packed (Fig. 2d, Fig. 2f). The film quality by facile
mechanical rubbing compares favorably with those obtained by
ρ = (I║ − I⊥)/( I║ + I⊥)
(1)
CR = I║/ I⊥
(2)
Here I║ and I⊥ represent the luminescent intensities when
the polarizer-axes are parallel and perpendicular to the rubbing
direction, respectively. It is calculated that the ρ and the CR value of
the PL for the dry-rubbed film are 0.5 and 3.0 respectively. The CR
value is near to that for the rubbed CdSe/CdS NR film, 3.5, which
was achieved by optimizing the substrate treatment and the
organic ligand ratio.31 Higher ρ and CR values have been reported in
some literature on lead halide perovskite PL research. For example,
well-aligned CsPbX3 (X = Br, Cl) NWs were synthesized using a vapor
phase van der Waals epitaxial method show a ρ up to 0.78.24
However, to the best of our knowledge, the ρ and CR value in our
complicated self-assembly at an air/liquid interface where
a
transferring process is needed for the film being integrated into
optoelectronic devices.29 The morphologies of the rubbed films are
slightly similar with the rubbed CdSe/CdS seeded-rod layer achieved
by a two-step process consisting of spin coating NRs followed by
mechanically rubbing using a rayon velvet fabric, despite that
CdSe/CdS seeded-rod size is much smaller (55 nm  5 nm or 67 nm
 5 nm).31 Although both wet rubbing and dry rubbing produced
oriented NW films, there are more grooves in the wet-rubbed film
when viewed in a large area (Fig. 2c). The groove size is 2-6 m and
results from the “soft” adhesion between the NW film and the
substrate. By comparison, the dry-rubbed film is more uniform and
less groove appears (Fig. 2e). The morphology difference between
the wet-rubbed and dry-rubbed films is also observed by crossing
section SEM and atomic force microscopy (AFM) measurement (Fig.
S4 and Fig. S5). Apparently, the grooves are unfavorable for the
charge transport and therefore the LED device performance, which
will be investigated in the following.
work are quite high among those for polarized PL based on lead
25, 26
halide perovskite NRs or NWs.21-23,
It is noted that the
drop-casted films without mechanical rubbing also showed a
certain ρ of 0.148 and the CR value was 1.3 (Fig. S6). The
polarization property was attributed to the self-orientation
behavior caused by the strong ligand-ligand van-der Waals
interaction.11, Similar polarization property has been found for
30
the drop-casted CsPbBr3 QD films.11 So it is believed that the origin
of polarization of CsPbBr3 NW films come from the synergistic effect
of NWs and mechanical rubbing. The luminescence photos for the
anisotropic CsPbBr3 NW films, through a linear polarizer (dashed
arrow) parallel (a) and perpendicular (b) were shown in Fig. S7.
Fig. 3 The PL spectra of anisotropic CsPbBr3 NW films for two
orthogonal directions.
In general, hole transport materials (HTMs) for LEDs should
have good hole mobility, excellent film-formation property and
appropriate HOMO-LUMO levels. The most commonly used HTM in
CsPbBr3 LEDs is PEDOT:PSS,32-37 which has a work function of 5.0 -
5.2 eV and is used as a buffer layer on top of ITO to obtain a stable,
pinhole free conductive layer for the device. The lead halide
perovskite LED based on PEDOT:PSS has exhibited a record external
quantum efficiency (EQE) that surpasses 20%.35 There is also a layer
of PVK or poly-TPD added to the PEDOT:PSS for hole transport and
Fig. 2 SEM images of drop-casted CsPbBr3 NW films without rubbing
(a,b) and after mechnical wet rubbing (c,d) or mechnical dry
rubbing (e,f).
electron blocking layer, which can reduce the hole injection
38-41
barrier.1,
Under wet rubbing, we adopted different device
structures and found that the performance of single-layer poly-TPD
2 | J. Name., 2012, 00, 1-3
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based device showed the best device performance. In Fig. 4c and 4d were reported for polarized LEDs based on one-dimension inorganic
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luminance-voltage (L-V) and current-voltage (J-V) characteristics of nanomaterial.15 A bias around 11 V was neDedOeI:d10to.10in39d/uCc9eCtCh1e00li3g3hDt
the CsPbBr3 NW LEDs are shown. The devices with poly-TPD, emission for polarized LED using rubbed CdSe/CdS quantum rods as
poly-TPD + PVK, PEDOT:PSS + poly-TPD as the HTMs delivered the emissive layer15. By assembling CdSe/CdS nanorods in smetic
optimal luminance. The corresponding turn-on voltages at 1 cd/m2 and nematic phases on the surface of water, forming a ordered
are 9.5 V, 9.5 V, 10 V respectively. The maximum brightness of 3.88 floating film, and integrating it into an electroluminescent device,
cd/m2 was reached at 11 V and at 293 mA/cm2 for the device use the resulted polarized LED delivered an onset voltage of around 9
single layer poly-TPD as the HTM. On one hand, the multi-layer V28. The fact is due to the different properties between conjugated
HTM structure is not conducive to the recombination of electrons polymers and inorganic NRs or NWs when the anisotropic films are
and holes in the luminescent layer. On the other hand, the electron formed. Some emissive conjugated polymers can take advantage of
mobility of TPBi is 3.3 × 10−5 cm2 V−1 s−1,42 the hole mobility of PVK, liquid-crystalline self-orientation properties and then form
poly-TPD are 1.0 × 10−6 and 1.0 × 10−4 cm2 V−1 s−1 respectively.40, 43 large-area smooth and uniform film on rubbed or photoaligned
In terms of hole mobility and charge balance, poly-TPD is better. alignment layer,45 while there are rather limited methods to
Furthermore, poly-TPD has a deeper HOMO energy than PEDOT: prepare uniform films composed of inorganic NRs or NWs. The
PSS and is more suitable for the hole injection into perovskite layer. mechanical dry rubbing method leads to anisotropic CsPbBr3 NW
From the J-V curves (Fig. 4d), the device also showed higher films with relatively uniform morphology. Combining with the
current.
optimal hole injection through the energy level alignment, the low
turn-on voltage was achieved. However, it is still higher than those
of CsPbBr3 LEDs using polycrystalline thin films or QD films as the
emissive layer1,32-40, typically a little higher than 2 V. Two factors are
considered as the cause. The first is the large film thickness here.
Most of the thicknesses for highly-efficient CsPbBr3 LEDs using
polycrystalline thin films32-35 are less than 300 nm and many
reported CsPbBr3 QD LEDs1,36-40 even use a QD monolayer with a
thickness less than 20 nm. Due to the difficulties for fabricating
oriented CsPbBr3 NW film, the thickness here is larger than 1 m.
The other factor that influences the turn-on voltage is the long
ligands for CsPbBr3 NWs. Replacing oleylamine and oleic acid with
shorter ligands such as ethyl acetate or butyl acetate has been
demonstrated to enhance the film conductivity and then decrease
the turn-on voltage in CsPbBr3 QD LEDs36-40. In general, the
dry-rubbed device exhibits higher efficiency and the highest EQE
approaches 0.08%. Further work to achieve anisotropic NW film
with higher quality is under progress.
Fig. 4 (a) Energy level alignment diagrams of CsPbBr3 NW LEDs. (b)
The schematic structure of CsPbBr3 NW LEDs. (c) Luminance-voltage
(L-V) characteristics and (d) Current density-voltage (J-V) curves of
wet-rubbed CsPbBr3 NW LED.
Fig. 6 (a) The EL spectra of dry-rubbed CsPbBr3 NW LEDs for two
orthogonal directions at a 6.5 V applied bias, inset shows the
photograph of working CsPbBr3 NW LED. (b) The CIE coordinates for
the EL spectrum of CsPbBr3 NW LED.
Fig. 5 (a) Luminance-current density-voltage (L-J-V) curves and (b)
EQE of wet-rubbed and dry-rubbed CsPbBr3 NW LEDs.
After determining the optimal device structure, different
rubbing methods are also found to be crucial to device performance.
With the optimal poly-TPD single layer HTM, the L-J-V
characteristics and the EQE of the devices prepared using the two
methods are showed in Fig. 5. The dry-rubbed device achieved a
maximum brightness of 3.5 cd/m2 at 5.17 mA/cm2 with a turn-on
voltage of 6.5 V. The turn-on voltage is much lower than that
prepared by wet rubbing because the grooves which will lead to
current leakage are reduced. Lower turn-on voltages less than 4 V
have been achieved for polarized LEDs based on oriented
conjugated polymers.44 However, turn-on voltages higher than 10 V
Fig. 6 shows the EL spectra of dry-rubbed CsPbBr3 NW LEDs for
the two orthogonal polarization directions and the trend is
according with the PL polarization. The emission peak is at 519 nm
and the full width at half maxima (FWHM) is 25 nm, well according
with the optical properties of CsPbBr3 NWs.46 The high-color-purity
green emission is consistent with that in Commission Internationale
del’ Enclairage (CIE).
Conclusions
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Gesquiere, S. T. Wu and Y. J. Dong, Nanoscale, 2018, 10, 15V4i3ew6-A1r5ti4c4le1O. nline
DOI: 10.1039/C9CC10033D
Zhang, J. Shi, W. N. Du, Y. F. Zhang, S. L. Chen, P. Gao, X. F. Liu, X. N.
Wang and Q. Zhang, Adv. Mater., 2018, 30, 1801805.
We have demonstrated the oriented alignment of CsPbBr3
NWs using mechanical rubbing. The deposition method is fast, facile,
and can be applied on relatively large substrates. The well-oriented
CsPbBr3 NWs films prepared in this study not only show PL
polarization, but also is used to prepare polarized LEDs. Among
them, the best device exhibits a turn-on voltage of 6.5 V and an EQE
of 0.08%. The results prove the great potential of polarized LEDs
based on CsPbBr3 NWs.
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We thank the supports by the National Key Research and
Development
Program
of
China
(2019YFE0101300,
2017YFE0133800) and the Distinguished Youth Foundation of Anhui
Province (1708085J09). The Key Lab of Photovoltaic and Energy
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acknowledged by the authors. The authors thank Dr. Yaohong
Zhang and Dr. Feng Liu for assistance with the AFM and crossing
section SEM measurements.
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4 | J. Name., 2012, 00, 1-3
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ChemComm
Journal Name
COMMUNICATION
TOC
View Article Online
DOI: 10.1039/C9CC10033D
CsPbBr3 nanowire polarized light-emitting diodes with low turn-on
voltage were achieved through mechanical rubbing combined with
an optimal device structure.
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