CN113675358A - Method for improving efficiency of green phosphorescent OLED device based on exciplex host of B4PYMPM - Google Patents
Method for improving efficiency of green phosphorescent OLED device based on exciplex host of B4PYMPM Download PDFInfo
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- H10K50/12—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers comprising dopants
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Abstract
The invention discloses a method for improving the efficiency of a green phosphorescent OLED device based on an exciplex main body of B4PYMPM, wherein the exciplex main body with intermolecular TADF effect is formed by co-evaporating the B4PYMPM with stronger electron transmission capability and mCP, so that the energy transfer process of a light-emitting layer is optimized, the concentration of excitons in the light-emitting layer is dispersed, the electron transmission capability of the light-emitting layer is enhanced, the transmission balance of carriers of the light-emitting layer is improved, the current efficiency, the power efficiency and the external quantum efficiency of the device are obviously improved, the turn-on voltage of the device is reduced, and the efficiency roll-off of the device is smaller. According to the invention, the materials of the electron transport layer and the hole transport layer are combined to form the exciplex main body, so that the performance of the green phosphorescent OLED device is greatly improved on the premise of not increasing the energy level barrier.
Description
Technical Field
The invention relates to a method for improving the efficiency of a green phosphorescent OLED device based on an exciplex co-host of B4PYMPM, wherein the B4PYMPM with stronger electron transmission capability is doped into a host material mCP of the green phosphorescent OLED device to form the exciplex co-host, and the intermolecular TADF effect of the exciplex can effectively improve the exciton utilization rate, so that the method is an effective method for preparing the green phosphorescent OLED device with simple structure and high efficiency. .
Background
In the OLED device, excited states generated after recombination of electrons of a cathode and holes of an anode comprise a singlet excited state and a triplet excited state, the theoretical ratio of the singlet excited state to the triplet excited state is 1:3, the traditional fluorescent material can only utilize singlet excitons, and 75% of triplet excitons are wasted; phosphorescent materials, while capable of 75% internal quantum efficiency, are too costly to fabricate due to the need for expensive heavy metal atoms. TADF (Thermally Activated Delayed Fluorescence) can convert triplet excitons into singlet excitons by Reverse Intersystem Crossing (RISC) due to a small energy gap between singlet energy levels and triplet energy levels, thereby achieving 100% internal quantum efficiency, but generally has very strict requirements on the structure of a device, and both an electron donor and an acceptor are present in an organic molecule having TADF characteristics. An exciplex formed by combining a single electron donor and acceptor material can achieve the same effect as intramolecular TADF in a simpler manner. According to the invention, the exciplex is formed as a co-host by selecting the electron material and the hole material with a proper energy level relation through co-evaporation, so that the device has higher performance.
Disclosure of Invention
The invention aims to make up the defects of the prior art and provides a method for improving the efficiency of a green phosphorescent OLED device based on an exciplex co-host of B4 PYMPM. According to the invention, the OLED device with excellent performance is prepared through reasonable device structure design, and the method specifically comprises the following steps: proper energy level matching among all functional layers, matching of carrier transmission rate of a main material, proper doping concentration of a luminescent material and the like. According to the invention, the B4PYMPM with strong electron transmission capability is used as a co-host material and added into the light-emitting layer of the green phosphorescent OLED device to form the exciplex with the intermolecular TADF effect, so that the transmission balance of current carriers can be improved, and the efficiency of the green phosphorescent OLED device is improved.
The invention is realized by the following technical scheme:
a method for improving the efficiency of a green phosphorescent OLED device based on an exciplex host of B4PYMPM, the green phosphorescent OLED device comprising an emission layer of the exciplex host, the emission layer being composed of two host materials doped with a guest emitting material, 4,6-Bis (3, 5-Bis (pyridin-4-yl) phenyl) -2-methylpyrimidine (4, 6-Bis (3,5-di (pyridine-4-yl) phenyl) -2-methylpyrimidine,4,6-Bis (3, 5-di-4-pyridylphenyl) -2-methylpyrimidine, B4 PYMPM) being added to the emission layer of the green phosphorescent OLED device as a common host material.
The light emitting layer of the green phosphorescent OLED device adopts N, N' -dicarbazolyl-3,5-benzene (mCP) with strong hole transport capacity and B4PYMPM with strong electron transport capacity to form an exciplex as a co-host, and the green phosphorescent material fac-Ir (ppy)3As guest doping material.
Host material mCP and B4PYMPM doped guest luminescent material fac-Ir (ppy)330nm in total, wherein the mass ratio of the host material mCP to the B4PYMPM is 1:1, and the guest doping material fac-Ir (ppy)3The concentration of (B) varies within the range of 1wt% to 9 wt%.
Host materials mCP and B4PYMPM, and guest dopant material fac-Ir (ppy)330nm in total, wherein the mass ratio of the host material mCP to the B4PYMPM is 1:1, and the guest doping material fac-Ir (ppy)3The concentration of (B) is 7 wt%.
Host material mCP and B4PYMPM doped guest luminescent material fac-Ir (ppy)3Co-evaporated on green phosphorusAnd a light emitting layer is formed on the ITO glass substrate of the optical OLED device.
To prepare a high efficiency green phosphorescent OLED device, we prepared devices a, B for efficiency testing, where B is the control. The preparation method of the devices A and B comprises the following steps:
and a device A:
(ITO/MoO3(10nm)/TAPC(30nm)/mCP(15nm)/mCP:B4PYMPM:fac-Ir(ppy)3,1:1:7wt%(30 nm)/B4PYMPM(40 nm)/LiF(1 nm)/Al(100 nm))；
the operation steps are as follows:
(1) ultrasonic cleaning of the ITO glass substrate;
(2) drying the cleaned ITO glass substrate by nitrogen, and then drying by a hot bench;
(3) carrying out ultraviolet ozone treatment on the ITO glass substrate;
(4) placing the ITO glass substrate subjected to ultraviolet ozone treatment on a customized substrate frame, then placing the ITO glass substrate into a coating machine, and vacuumizing the coating machine;
(5) then MoO is respectively coated on the ITO glass substrate3(10 nm), TAPC (30nm), mCP (15 nm), EML (30nm), B4PYMPM (40nm), LiF (1nm) and Al (100nm), wherein the EML is a light-emitting layer, the thickness is 30nm, the mass ratio of two host materials mCP and B4PYMPM of the light-emitting layer is 1:1, and a guest doping material fac-Ir (ppy)3The proportion is 7wt%, and then the coating machine is started to take out the prepared device after the coating machine is cooled to a proper temperature;
(6) packaging the prepared device;
(7) testing the performance of the prepared device;
device B as control:
(ITO/MoO3(10nm)/TAPC(30nm)/mCP(15nm)/mCP:7wt%fac-Ir(ppy)3 (30nm)/B4PYMPM(40nm)/LiF(1nm)/Al(100nm))；
the operation steps are as follows:
(1) repeating the steps (1), (2), (3) and (4) of the device A;
(2) respectively plating MoO on the ITO glass substrate3（10 nm），TAPC（30 nm），mCP（15 nm），EML（30 nm), B4PYMPM (40nm), LiF (1nm), Al (100nm), wherein EML is a light-emitting layer with the thickness of 30nm, and a green phosphorescent material fac-Ir (ppy)3The proportion of (B) is 7 wt%. After the coating is finished, opening the coating machine to take out the device after the coating machine is cooled to a proper temperature;
(3) packaging the prepared device;
(4) testing the performance of the prepared device;
the principle of the invention is as follows:
in the green phosphorescent device, mCP with strong hole transport capability and B4PYMPM with strong electron transport capability are simultaneously used as main materials to be evaporated together to form an exciplex main body, and the exciplex main body has intermolecular TADF (TADF) characteristics, effectively utilizes triplet excitons and theoretically realizes 100% internal quantum efficiency. Because the electron transmission rate of the B4PYMPM and the hole transmission rate of the mCP are in the same order of magnitude, the luminescent center can be well limited in the luminescent layer, so that the exciton quenching phenomenon caused by exciton diffusion and exciton aggregation at the interface is reduced; meanwhile, the density of excitons can be dispersed by adopting a host-guest doping mode, so that the phenomenon of exciton quenching under high brightness is reduced; and the introduced B4PYMPM with stronger electron transport capacity is used as a main body, so that the transport balance of the current carrier of the luminous layer can be improved. By comparing the efficiency of the green phosphorescent OLED device with and without the B4PYMPM as the main body, the efficiency of the green phosphorescent OLED device with the B4PYMPM with stronger electron transfer capability as the main body is greatly improved.
The invention has the advantages that:
according to the invention, B4PYMPM with strong electron transmission capability is added into the light emitting layer of the green phosphorescent OLED device as another main material, and is co-evaporated with mCP to form an exciplex main body with an intermolecular TADF effect, so that the energy transfer process of the light emitting layer is optimized, the concentration of excitons in the light emitting layer is dispersed, the transmission balance of carriers of the light emitting layer is improved, and an exciton recombination region is limited in the center of the light emitting layer, so that the current efficiency, the power efficiency and the external quantum efficiency of the device are remarkably improved, the brightness of the device is improved by nearly three times, the starting voltage of the device is reduced, and the efficiency roll-off of the device is more stable.
Drawings
The energy level diagram of the device of fig. 1.
Fig. 2 is a block diagram of a device.
Fig. 3 is a graph of power efficiency versus luminance versus current efficiency for the device.
Fig. 4 external quantum efficiency-luminance plot of the device.
Detailed Description
Referring to fig. 1 and 2, a method for improving efficiency of a green phosphorescent OLED device based on an exciplex host of B4PYMPM, which includes an emission layer having an exciplex as a host, the emission layer being formed of two host materials doped with guest emitting materials, 4,6-Bis (3, 5-Bis (pyridin-4-yl) phenyl) -2-methylpyrimidine (4, 6-Bis (3,5-di (pyridine-4-yl) phenyl) -2-methylpyrimidine,4,6-Bis (3, 5-di-4-pyridylphenyl) -2-methylpyrimidine, B4 PYMPM) being added to the emission layer of the green phosphorescent OLED device as a common host material to form the exciplex.
N, N-dicarbazolyl-3, 5-benzene (N, N' -dicarbazolyl-3, 5-bezene, mCP) with strong hole transport capability and 4,6-Bis (3, 5-Bis (pyridin-4-yl) phenyl) -2-methylpyrimidine (4, 6-Bis (3,5-di (pyridine-4-yl) phenyl) -2-methylpyrimidine,4,6-Bis (3, 5-di-4-pyridylphenylphenyl) -2-methylpyrimidine and B4 PYMPM) with strong electron transport capability are selected to be co-evaporated to form exciplex as a co-host, and a green phosphorescent material fac-Ir (ppy)3As guest doping material.
Host material mCP and B4PYMPM doped guest luminescent material fac-Ir (ppy)330nm in total, wherein the mass ratio of the host material mCP to the B4PYMPM is 1:1, and the guest doping material fac-Ir (ppy)3The concentration range of (A) varies between 1wt% and 9 wt%.
Host material mCP and B4PYMPM doped guest luminescent material fac-Ir (ppy)330nm in total, wherein the mass ratio of the host material mCP to the B4PYMPM is 1:1, and the guest doping material fac-Ir (ppy)3The concentration of (B) is 7 wt%.
Host material mCP and B4PYMPM doped guest luminescent material fac-Ir (ppy)3And co-evaporating to form a light-emitting layer on the ITO glass substrate of the green phosphorescent OLED device.
The following provides a detailed description of embodiments of the invention. The embodiment provides a detailed implementation mode and a specific operation process based on the technical scheme of the invention. The scope of the present invention includes, but is not limited to, the following examples.
Referring to fig. 1, 2, 3, 4, to prepare device a:
(ITO/MoO3(10nm)/TAPC(30nm)/mCP(15nm)/mCP:B4PYMPM:fac-Ir(ppy)31:1:7wt% (30nm)/B4PYMPM (40nm)/LiF (1nm)/Al (100nm)) structure, we performed the following steps:
(1) and cleaning the ITO substrate:
putting the ITO glass substrate into a beaker filled with ITO cleaning solution diluted by pure water, putting the beaker into an ultrasonic cleaning instrument for ultrasonic treatment for 30 min, and then replacing the pure water for ultrasonic treatment for 10 min.
(2) And heating and drying:
after the ITO substrate was cleaned, water on the ITO glass substrate was blown clean with nitrogen gas, and then heated at 120 degrees for 10min on a hot stage.
(3) And ultraviolet ozone treatment:
after the steps (1) and (2), processing the ITO substrate for 10-20min by using an ultraviolet light cleaning machine to remove organic matter residues on the surface of the ITO substrate, increase the number of hydroxyl groups on the surface of the ITO substrate and effectively improve the work function of the surface of the ITO simultaneously.
(4) After the ITO glass substrate is treated in the steps (1), (2) and (3), the ITO substrate treated by ultraviolet ozone is placed on a substrate frame, then the ITO glass substrate is placed into an evaporation chamber of an EvoVac ultrahigh vacuum film coating machine, a valve of the chamber is closed, and then the evaporation chamber is vacuumized. When the vacuum degree of the chamber is increased to 5.5X 10-6The Torr may start evaporation. And then, sequentially evaporating each functional layer of the device: MoO3(hole injection layer), TAPC (hole transport layer), mCP (hole transport layer), EML (light emitting layer), B4PYMPM (electron transport layer), LiF (electron injection layer), and Al (cathode), each film layer having a thickness of 10 nm, 30nm, 15 nm, 30nm, 40nm, 1nm, and 100nm, respectively. The rates other than the light-emitting layer are respectively1A/s, 1.2A/s, 0.4A/s, 1A/s; the light-emitting layer is made of host material mCP, B4PYMPM and guest doping material fac-Ir (ppy)3Co-evaporation, the evaporation rate is 0.8A/s: 1.2A/s: 0.13A/s, and the mass ratio of host material mCP and B4PYMPM is 1: guest dopant material fac-Ir (ppy)3Is 7 wt%. And after the coating is finished, opening the coating machine after the chamber of the coating machine is cooled to a proper temperature, and taking out the prepared device.
(5) And packaging the device:
and taking out the evaporated device, adhering the glass cover plate coated with the ultraviolet curing glue and the device substrate in a glove box with water and oxygen content lower than 1 ppm by using a manufactured clamp, shielding the organic layer, and irradiating for 3 min under ultraviolet light for curing. After ultraviolet light exposure, a barrier separated from the atmospheric environment is formed, and the barrier can effectively prevent water-oxygen in the air from entering the device and avoiding reaction with the device;
(6) and carrying out performance test on the packaged device:
as shown in fig. 3 and 4, in the current-voltage-luminance characteristic test, a test system composed of a Keithley 2400 power supply meter and a Topcon SR-UL1R spectroradiometer is used to collect the relevant data (voltage, current, luminance and spectrum) of the OLED device; the External Quantum Efficiency (EQE) of all devices was calculated from the current density, brightness and spectral data obtained from the above tests. None of the devices were subjected to any packaging process prior to all device testing. All tests were done at room temperature in a dark room.
For the preparation of control device B:
(ITO/MoO3(10nm)/TAPC(30nm)/ mCP (15nm)/ mCP:fac-Ir(ppy)37wt% (30nm)/B4PYMPM (40nm)/LiF (1nm)/Al (100nm)) structure, the steps of the invention are as follows:
(1) and repeating the steps (1), (2) and (3) of preparing the device A.
(2) After the ITO glass substrate is treated in the steps (1), (2) and (3), the ITO glass substrate treated by ultraviolet ozone is placed on a customized substrateAnd (3) putting the wafer frame into an evaporation chamber of an EvoVac ultrahigh vacuum coating machine, closing a valve of the chamber, and vacuumizing the evaporation chamber. When the vacuum degree of the chamber is increased to 5.5X 10-6The Torr may start evaporation. And then, sequentially evaporating each functional layer of the device: MoO3 (hole injection layer), TAPC (hole transport layer), mCP (hole transport layer), EML (light emitting layer), B4PYMPM (electron transport layer), LiF (electron injection layer), and Al (cathode), each having a thickness of 10 nm, 30nm, 15 nm, 30nm, 40nm, 1nm, and 100nm, respectively. The rates except the luminescent layer are respectively 1A/s, 1.2A/s, 0.4A/s and 1A/s; the light emitting layer is made of a host material mCP and a guest doping material fac-Ir (ppy)3Co-evaporation at a rate of 1.2A/s: 0.1A/s, and a guest doping material fac-Ir (ppy)3Is 7 wt%. And after the coating is finished, opening the coating machine to take out the device after the chamber of the coating machine is cooled to a proper temperature.
(3) And packaging the device:
and taking out the evaporated device, adhering the glass cover plate coated with the ultraviolet curing glue and the device substrate in a glove box with water and oxygen content lower than 1 ppm by using a manufactured clamp, shielding the organic layer, and irradiating for 3 min under ultraviolet light for curing. After ultraviolet light exposure, a barrier separated from the atmospheric environment is formed, and the barrier can effectively prevent water-oxygen in the air from entering the device and avoiding reaction with the device;
(4) and carrying out performance test on the packaged device:
in the current-voltage-brightness characteristic test, a test system consisting of a Keithley 2400 power supply meter and a Topcon SR-UL1R spectroradiometer is adopted to collect related data (voltage, current, brightness and spectrum) of an OLED device; the External Quantum Efficiency (EQE) of all devices was calculated from the current density, brightness and spectral data obtained from the above tests. None of the devices were subjected to any packaging process prior to all device testing. All tests were done at room temperature in a dark room.
The electroluminescence property parameter pairs of the green phosphorescent devices a and B are shown in table 1.
TABLE 1
| Device | Von(V) | CEmax(cd/A) | PEmax(lm/W) | EQEmax(%) | Lmax(cd/m2) |
| A | 3.10 | 87.21 | 78.82 | 25.02 | 66255 |
| B | 3.20 | 69.24 | 62.15 | 19.54 | 29094 |
Note:
Von(V): starting voltage; CEmax(cd/A): maximum current efficiency; PE (polyethylene)max(lm/W): maximum power efficiency; EQEmax(%): most preferablyLarge external quantum efficiency; l ismax(cd/m2): the maximum brightness.
Claims (6)
1. A method for improving the efficiency of a green phosphorescent OLED device based on an exciplex host of B4PYMPM is characterized in that: the green phosphorescent OLED device comprises an emitting layer with an exciplex host, and 4,6-Bis (3, 5-Bis (pyridin-4-yl) phenyl) -2-methylpyrimidine (4, 6-Bis (3,5-di (pyridine-4-yl) phenyl) -2-methylpyrimidine,4,6-Bis (3, 5-di-4-pyridylphenylphenyl) -2-methylpyrimidine, B4 PYMPM) is added into the emitting layer of the green phosphorescent OLED device to form the exciplex.
2. The method of claim 1, wherein the green phosphorescent OLED device based on the exciplex host of B4PYMPM has improved efficiency, and the method comprises: the luminescent layer is formed by doping two host materials with guest luminescent materials.
3. The method of claim 2, wherein the green phosphorescent OLED device based on the exciplex host of B4PYMPM has improved efficiency, and the method comprises: the light emitting layer of the green phosphorescent OLED device adopts N, N-dicarbazolyl-3, 5-benzene (N, N' -dicarbazolyl-3, 5-benzone, mCP) with strong hole transport capability and B4PYMPM with strong electron transport capability to form an exciplex as a co-host, and the guest doping material adopts a green phosphorescent material fac-Ir (ppy)3。
4. The method of claim 3, wherein the green phosphorescent OLED device based on the exciplex host of B4PYMPM has improved efficiency, and the method comprises: the host material mCP and the B4PYMPM doped guest luminescent material fac-Ir (ppy)330nm in total, wherein the mass ratio of the host material mCP to the B4PYMPM is 1:1, and the guest doping material fac-Ir (ppy)3In the range of 1wt% to 9 wt%.
5. The green phosphorescent OL based on exciplex host of B4PYMPM of claim 4The method for improving the efficiency of the ED device is characterized by comprising the following steps: the host material mCP and the B4PYMPM doped guest luminescent material fac-Ir (ppy)330nm in total, wherein the mass ratio of the host material mCP to the B4PYMPM is 1:1, and the guest doping material fac-Ir (ppy)3The concentration of (B) is 7 wt%.
6. The method of claim 5, wherein the green phosphorescent OLED device based on the exciplex host of B4PYMPM has improved efficiency, and the method comprises: an exciplex formed between the host material mCP and the B4PYMPM is re-doped with a guest material fac-Ir (ppy)3And co-evaporating to form a light-emitting layer on the ITO glass substrate of the green phosphorescent OLED device.
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