CN109423696B - Growing device of multilayer organic single crystal structure - Google Patents

Growing device of multilayer organic single crystal structure Download PDF

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CN109423696B
CN109423696B CN201710736116.5A CN201710736116A CN109423696B CN 109423696 B CN109423696 B CN 109423696B CN 201710736116 A CN201710736116 A CN 201710736116A CN 109423696 B CN109423696 B CN 109423696B
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后藤修
陈默
曾兴为
魏潇赟
孟鸿
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Peking University Shenzhen Graduate School
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    • CCHEMISTRY; METALLURGY
    • C30CRYSTAL GROWTH
    • C30BSINGLE-CRYSTAL GROWTH; UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL; PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; APPARATUS THEREFOR
    • C30B29/00Single crystals or homogeneous polycrystalline material with defined structure characterised by the material or by their shape
    • C30B29/54Organic compounds
    • CCHEMISTRY; METALLURGY
    • C30CRYSTAL GROWTH
    • C30BSINGLE-CRYSTAL GROWTH; UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL; PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; APPARATUS THEREFOR
    • C30B23/00Single-crystal growth by condensing evaporated or sublimed materials

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Abstract

The invention relates to a growth device of a multilayer organic single crystal structure, which utilizes various organic semiconductor materials to grow the multilayer organic single crystal structure such as pn junction, heterojunction, quantum well, multi-quantum well and the like. The equipment is characterized in that: 1. at least two temperature control regions for sublimation of the material and growth of a single crystal, respectively; 2. the two temperature control areas are adjacent and parallel, and the temperature can be quickly and independently regulated and controlled; 3. after the growth of the first layer of single crystal is finished, the replacement of the source material can be finished without the contact of the surface of the single crystal and air, and the subsequent growth of the second layer of single crystal is carried out.

Description

Growing device of multilayer organic single crystal structure
Technical Field
The invention relates to the technical field of organic semiconductor materials, in particular to a growth device with a multilayer organic single crystal structure.
Background
The pn junction is a key structure for preparing photoelectric and electronic semiconductor devices such as a Solar Cell (SC), a Light Emitting Diode (LED), a Laser Diode (LD), a bipolar transistor and the like. At present, the expected next generation of photoelectric devices, Organic Light Emitting Diodes (OLEDs), have been mass produced, applied to the manufacture of televisions and display screens, and gradually come into people's lives. However, other devices than OLEDs, such as Organic Solar Cells (OSCs), Organic Lasers (OLDs), etc., are still in the development stage of basic research and intensive understanding.
Compared with organic polycrystalline materials, the organic single crystal materials eliminate grain boundary interference and have highly ordered structures, so that the intrinsic carrier transmission characteristics of the materials can be reflected, and field effect transistors (TFTs) prepared by taking organic single crystal films as active layers are widely applied to the performance research of the materials. Because of the great technical difficulty in growing multilayer single crystal structures, the current research still hasMainly focusing on device structures based on single-layer single-crystal thin films. Pioneer pioneering work has revealed an explosion in the field of organic semiconductors and unlimited possibility in the future, rubrene (rubrene) being representative of high-performance p-type organic semiconductor material, whose single-crystal TFT has a mobility as high as 40cm2/Vs,[1]And has anisotropic transmission characteristics.[2,3]In addition, the diffusion length of excitons in rubrene single crystals can reach several micrometers, while the diffusion length in corresponding polycrystals is only several nanometers.[4]The advantages of mobility and exciton diffusion length make the organic single crystal pn junction an ideal unit for the preparation of high performance Organic Solar Cells (OSCs). It has been reported in the literature that organic single crystal SC structures can be grown using mixed solutions of n-type and p-type materials.[5,6]Although this method succeeds in obtaining a double-layer single crystal structure, the device efficiency is extremely low, and more importantly, the size and thickness control of the single crystal thin film cannot be achieved. If one could develop methods of growing single crystal p-i-n structures, including heterostructures, one could design and fabricate devices with properties comparable to inorganic materials using organic materials. However, due to the lack of suitable manufacturing equipment, it is still difficult to obtain a full single crystal structure with precisely controllable interface and thickness.
At present, there are many research institutes devoted to the preparation of single crystal PN junctions and heterojunctions, however there are few successful cases reported in the literature. The subject group of Japan studied using a single crystal tetracene[3]Or pentacene[4-5]Film as substrate, growing C60The mechanism of (2). They used a vacuum evaporation apparatus to grow C by changing the substrate temperature60However, the second film obtained is not monocrystalline. Other groups of subjects tried to study the characteristics of organic pn junctions, but also failed to successfully grow a second layer single crystal on an organic single crystal substrate. In this case, Wavingping, Briseno and co-workers used copper (F) hexadecafluoro phthalocyanine16CuPc, n-type material) and copper phthalocyanine (CuPc, p-type material), and the organic single crystal pn junction nanobelt is obtained by a vapor phase epitaxial growth method.[6]They used the pre-grown copper phthalocyanine single crystal nanobelt as a template for epitaxial growth, induced the hexadecafluoro copper phthalocyanine to form a one-dimensional single crystal heterojunction, and studiedThe performance of the organic solar cell based on the single crystal heterojunction is studied. Although this work completed the challenge of growing organic single crystal heterojunctions, it was not systematically studied in greater depth. Therefore, a new set of methods for growing single crystal pn, heterojunctions and multilayer structures must be developed. Reference to the literature
[1]J.Takeya,M.Yamagishi,Y.Tominari,R.Hirahara,Y.Nakazawa,T.Nishikawa,T.Kawase,T.Shimoda,S.Ogawa,Appl.Phys.Lett.90,102120(2007).
[2]V.C.Sundar,J.Zaumseil,V.Podzorov,E.Menard,R.L.Willett,T.Someya,M.E.Gershenson,J.A.Rogers,Science 303,1644(2004).
[3]C.Reese and Z.Bao,Adv.Mater.19,4535(2007).
[4]H.Najafov,B.Lee,Q.Zhou,L.C.Feldman,and V.Podzorov,Nature Mater.9,938(2010).
[5]C.Fan,A.P.Zoombelt,H.Jiang,W.Fu,J.Wu,W.Yuan,Y.Wang,H.Li,H.Chen,and Z.Bao,Adv.Mater.2013,25,5762–5766.
[6]H.Li,C.Fan,W.Fu,H.L.Xin,and H.Chen,Angew.Chem.54,956–960(2015).
[7]Y.Zhang,H.Dong,Q.Tang,W.Chen,S.Ferdous,S.C.B.Mannsfeld,W.Hu,A.L.Briseno,J.Am.Chem.Soc.132,11580-11584(2010).
Disclosure of Invention
The technical problems to be solved by the invention include: provides a growing device of a multilayer organic single crystal structure, which solves the problem of difficult formation of the multilayer organic single crystal structure in the prior art.
The technical scheme for solving the problems comprises the following steps: the growth device comprises a vapor phase growth unit placed under the protection of inert gas atmosphere, wherein the vapor phase growth unit comprises an air inlet sealing head and an airflow sleeve detachably connected with the air inlet sealing head, and a source material sublimation area and a growth area are arranged in the airflow sleeve.
In the growth device with the multilayer organic single crystal structure, the region where the air inlet end enclosure is connected with the airflow sleeve is a source material introducing region, and the connection between the air inlet end enclosure and the airflow sleeve is opened to replace materials.
In the growth device with the multilayer organic single crystal structure, a first O-shaped ring is arranged at the joint of the airflow sleeve and the air inlet end enclosure, and a first water cooling system is arranged near the first O-shaped ring.
In the growth device with the multilayer organic single crystal structure, the vapor phase growth unit further comprises an air outlet end enclosure, and one end, far away from the air inlet end enclosure, of the airflow sleeve is connected with the air outlet end enclosure.
In the growth device with the multilayer organic single crystal structure, the airflow sleeve is detachably connected with the air outlet end enclosure, a second O-shaped ring is arranged at the joint of the airflow sleeve and the air outlet end enclosure, and a second water cooling system is arranged near the second O-shaped ring.
In the growth device of the multilayer organic single crystal structure, the source material sublimation area and the growth area are arranged at intervals, the interval distance is more than 5mm, and the temperature is controlled by using independent resistance heating plates respectively.
In the growth device of the multilayer organic single crystal structure provided by the invention, the source material sublimation area and the growth area can slide along the track and are fixed at a specific position.
The growth device of the multilayer organic single crystal structure further comprises a flow guide part covering the source material sublimation area and the growth area from the upper part, the top of the flow guide part is slightly inclined, the opening of the flow guide part is large, the outlet of the flow guide part is small, and the internal airflow is directly blown to the substrate.
In the growth device of the multilayer organic single crystal structure, the bottom of the drainage piece extends out of a cover plate, and the cover plate is arranged in at least one part of a gap between the source material sublimation area and the growth area.
In the growth device of the multilayer organic single crystal structure provided by the invention, a first carrier gas introducing pipe and a second carrier gas introducing pipe are arranged on the gas inlet sealing head, the gas flow direction of the first carrier gas introducing pipe is parallel to the radial extension direction of the gas flow sleeve, and the gas flow direction of the second carrier gas introducing pipe is vertical to the radial extension direction of the gas flow sleeve.
The implementation of the invention has the following beneficial effects: the device has compact structure, the vapor phase growth unit is isolated from the air, and when the vapor phase growth unit is opened to replace materials, the materials and the single crystal do not need to be contacted with the air. Each temperature control area uses an independent resistance heating plate to control the temperature, so that no temperature distribution exists in the surface, and the rapid and accurate regulation and control of the temperature can be ensured. Since the vapor of the source material is directly blown toward the substrate, the source material loss of the apparatus is less compared to the conventional physical vapor transport apparatus.
Drawings
The invention will be further described with reference to the accompanying drawings and examples, in which:
FIG. 1 is a schematic diagram of a conventional physical vapor transport apparatus;
FIG. 2 is a schematic structural view of a growth apparatus for a multi-layered organic single crystal structure according to the present invention;
FIG. 3 is a schematic structural view of a vapor phase growth unit of a growth apparatus for a multi-layered organic single crystal structure according to the present invention;
FIG. 4 is a schematic structural diagram of a flow guide of a growth apparatus for a multilayer organic single crystal structure according to the present invention;
FIG. 5 is a saturation (unsaturation) curve of a rubrene single crystal;
FIG. 6 is a rubrene single crystal grown using a growth apparatus of a multi-layered organic single crystal structure of the present invention; (a) the sublimation temperature of the source material is 300 ℃, and the temperature of the growth area is 200 ℃; (b) the sublimation temperature of the source material is 330 ℃, and the temperature of the growth area is 220 ℃; (c) the sublimation temperature of the source material is 320 ℃, and the temperature of the growth zone is 210 ℃.
Detailed Description
The following examples are intended to illustrate embodiments of this aspect and should not be construed as limiting the scope of the invention.
Fig. 1 shows a schematic diagram of a conventional physical vapor transport apparatus. The design of this apparatus is based on a material purification apparatus with two temperature controlled zones, a source material sublimation zone (temperature labeled T1) and a growth zone (temperature labeled T2, T2< T1). Nitrogen and/or argon are used as carrier gases to transport saturated vapors of the source material from the sublimation zone to the growth zone. The substrate is placed in a growth zone and, under supersaturated conditions, the vapor of the source material precipitates a single crystal on the substrate. Such devices were initially used to purify the source material by sublimation, so the growth zone had a larger temperature profile and the furnace was longer.
Growing multilayer structures with this apparatus will cause the following problems:
(1) after one layer of single crystal growth is complete, the quartz furnace must be opened to replace the source material to grow a second layer of single crystals (of a different material). The existing gas purification device has a long furnace body and is inconvenient to put into a glove box protected by nitrogen. Thus, opening the furnace body will result in the single crystal surface being exposed to air. Contamination of the single crystal surface with air will destroy the interface between the two layers of single crystal.
(2) If an existing gas purification apparatus is used, the inner tube should have a diameter of at least 1 inch in order to place the substrate in the inner tube. However, due to the large temperature distribution in the inner tube, the high temperature source material vapor will move along the upper wall of the inner tube, and almost all of the single crystal will be deposited on the upper wall of the inner tube, rather than on the substrate placed at the lower portion of the inner tube, and the single crystal cannot be efficiently collected.
(3) The existing gas purification device adopts resistance wires for heating, and the horizontal direction and the radius direction of a furnace body have large temperature distribution, so that the temperature of a growth area is difficult to accurately and quickly control.
In order to reproducibly obtain a single crystal with a good interface, it is necessary to avoid the surface of the source material and the single crystal thin film from contacting with moisture in the air, and therefore, the apparatus is to be placed under an inert gas atmosphere, and the vapor growth unit should be small and compact.
Fig. 2 is a schematic structural diagram of a growth apparatus of a multi-layer organic single crystal structure according to the present invention, as shown in fig. 2, the growth apparatus has at least two temperature control regions for sublimation of a material and growth of a single crystal, respectively, the two temperature control regions are adjacent and parallel (the minimum distance is 5 mm), the temperature of each temperature control region can be rapidly and independently controlled, and the vapor phase growth unit 100 is placed under the protection of an inert gas atmosphere, so that the source material can be replaced without contacting the inside tube furnace with moisture in the air. For convenience of description, the following "vapor growth unit 100 furnace" and "furnace" refer to the vapor growth unit 100 unless otherwise specified.
The vapor growth unit 100 includes a gas inlet head 120 (see fig. 3) and a gas flow sleeve 110 detachably connected to the gas inlet head 120, and a source material sublimation region 140 and a growth region 150 are disposed in the gas flow sleeve 110. The principle of the growth of the organic single crystal is similar to that of the traditional physical meteorological transmission equipment. To reduce the volume of the furnace of the vapor growth unit 100, the source material sublimation zone 140 and the growth zone 150 are positioned adjacent and parallel. To control the temperature quickly and accurately, a resistive heating plate system is used. Through the design, the problem that the furnace body is long and is inconvenient to integrally carry out inert gas atmosphere protection can be solved.
In the present invention, it is preferable that the region where the air inlet cap 120 is connected to the gas flow sleeve 110 is the source material introduction region 160, and the connection between the air inlet cap 120 and the gas flow sleeve 110 is opened to replace the material. Since the vapor phase growth unit 100 is entirely placed under the atmosphere of inert gas, for example, the vapor phase growth unit 100 is directly placed in the glove box 200 filled with inert gas, the glove box 200 isolates the furnace body from air, and when the furnace body is opened to replace materials, the materials and the single crystal do not need to be in contact with air.
FIG. 3 is a schematic structural view of a vapor phase growth unit of a growth apparatus for a multi-layered organic single crystal structure according to the present invention, in which a source material sublimation region 140 and a growth region 150 are spaced apart from each other by a distance greater than 5mm, and the temperature is controlled by using independent resistance heating plates, respectively. To facilitate operation, the sublimation zone 140 and growth zone 150 may slide along the track and may be fixed at specific locations. The whole heating surface of the heating plate has uniform temperature, no temperature distribution in the surface, and rapid and accurate regulation and control of the temperature can be ensured.
The first O-ring 121 (see fig. 2) is disposed at the connection position of the airflow sleeve 110 and the air inlet sealing head 120, and because the temperature of the source material needs to be raised to be close to 400 ℃ to ensure the sublimation of the material, in order to avoid damaging the first O-ring 121, a first water cooling system 170 (see fig. 2) is installed near the first O-ring 121.
Similarly, the vapor phase growth unit 100 further includes an air outlet end enclosure 130, the air outlet end enclosure 130 is located at one end of the air flow sleeve 110 far away from the air inlet end enclosure 120, that is, two sections of the air flow sleeve 110 are respectively connected to the air inlet end enclosure 120 and the air outlet end enclosure 130, so that a rather isolated air flow region is formed inside the air flow sleeve 110, which is convenient for growth of the multilayer organic single crystal structure. Preferably, the gas flow sleeve 110 is detachably connected to the gas outlet sealing head 130, a second O-ring 131 (see fig. 2) is disposed at the connection position of the gas flow sleeve 110 and the gas outlet sealing head 130, and a second water cooling system 180 (see fig. 2) is installed near the second O-ring 131 to avoid damage.
To solve the temperature distribution problem of the inner tube, we have prepared a flow guide 160 as shown in fig. 4, and the flow guide 160 may be a quartz fitting. The assembly covers the source material sublimation zone 140 and the growth zone 150 from above. The fitting top 161 is slightly angled so that its opening 162 is large and the outlet 163 is small, and the internal gas flow can be directed toward the substrate 164.
Preferably, the bottom of the flow director 160 extends beyond a cover plate 165, and the cover plate 165 is disposed in at least a portion of the space separating the source material sublimation zone 140 and the growth zone 150. The bottom is partially covered to avoid diffusion of the sublimated source material gases from the sublimation zone and the gap with the growth zone 150 to the outer tube. Since the vapor of the source material is directly blown toward the substrate 164, the source material loss of the apparatus is less compared to the conventional physical vapor transport apparatus.
Preferably, with reference to fig. 2 to 4, the inlet end enclosure 120 is provided with a first carrier gas inlet pipe 122 and a second carrier gas inlet pipe 123, the gas flow direction of the first carrier gas inlet pipe 122 is substantially parallel to the radial extension direction of the gas flow sleeve 110, and the gas flow direction of the second carrier gas inlet pipe 123 forms an angle with the radial extension direction of the gas flow sleeve 110. Most preferably, the gas flow direction of the first carrier gas introduction pipe 122 is parallel to the radial extension direction of the gas flow sleeve 110, the gas flow direction of the second carrier gas introduction pipe 123 is perpendicular to the radial extension direction of the gas flow sleeve 110, and the second carrier gas introduction pipe 123 is disposed at the upper portion of the gas inlet end socket 120, so that the carrier gas blown by the second carrier gas introduction pipe 123 is ejected downward. Thus, the carrier gas enters the flow sleeve 110, and the direction of the flow coincides with the direction of the inclination of the top of the flow guide 160. Not only promotes the internal gas flow to be directly blown to the substrate, but also ensures the carrier gas flow of the gas flow sleeve 110.
Example structural details of the growth apparatus
(1) Source material sublimation zone
The apparatus may use at least two source materials. The melting point of most organic micromolecules is lower than 400 ℃, and the source material can be heated to be close to 400 ℃ by using a resistance heating system so as to ensure the sublimation of the material. The gas flow sleeve may be separated from the apparatus when the source material is replaced. The air in the system can be quickly replaced by inert carrier gas (nitrogen or argon) by using a vacuum pump. The technical difficulty is that when the equipment works, the temperature of the furnace body needs to be controlled to be about 400 ℃, and the O-shaped ring(s) (used at the connection part of the airflow sleeve and the equipment)
Figure BDA0001388161960000071
7075) The maximum heat resistant temperature is only 327 ℃. Therefore, we introduce a water cooling system near the O-ring to avoid damage.
(2) Source material introduction region
Multiple connections are required at the source material introduction zone, however, for the reasons previously mentioned, connections with O-rings must be avoided, and therefore we have used a metal connection 190(Swagelok, SS-6BW-1/4or 3/8, max. refractory temperature 483 ℃, structure see fig. 1). Similarly, a similar metal connection port 190 is used on the outlet seal 130.
(3) Growth zone
There are two temperature control zones within the airflow sleeve. The source material sublimation zone 140 and the growth zone 150 are covered by the same piece of flow guide 160, for example using a quartz fitting. The top of the flow-directing member 160 is an inclined plane that forms an angle with the direction of the gas flow and is placed in the gas flow sleeve 110 to ensure that the gas flow is directed towards the substrate.
Example 2 Single Crystal growth Process for rubrene
We explain the single crystal growth process in this device using rubrene, a typical organic small molecule material.
The principle of single crystal growth by vapor phase method can be explained by a saturation (supersaturation) curve showing the relationship between the state of the material and the temperature at a certain gas partial pressure. By using the device, the growth rule of the rubrene single crystal is obtained, as shown in fig. 5. The temperature of the source material is raised to obtain saturated vapor, and the partial pressure can be determined by a saturation curve according to the sublimation temperature of the source material under the condition that the flow rate of the carrier gas is unchanged. When the saturated vapor of the source material reaches the growth region 150 with the carrier gas, the partial pressure is constant and the temperature will decrease to the growth region 150 temperature. If the gas reaches a supersaturated state (below the supersaturation curve), the supersaturated fraction develops nuclei. It was found experimentally that when the temperature of the growth zone 150 is set above the corresponding supersaturation temperature, no single crystal is formed; when the growth zone 150 temperature is equal to the corresponding supersaturation temperature, a small number of larger volume single crystals may be formed; when the growth zone 150 temperature is below the corresponding supersaturation temperature, a large number of small single crystals may be formed.
Furthermore, it was found experimentally that the growth zone 150 temperature can affect the morphology of the single crystal, as shown in FIG. 6. At low temperatures (T2 ═ 200 ℃ C.), the single crystals are in the form of flakes, while at high temperatures (T2 ≥ 210 ℃ C.), the single crystals are in the form of needles or rods.
The apparatus is currently used to grow a single crystal in the form of a plate having an area of about 100. mu. m.times.200. mu.m and a thickness of about 60 nm. The crystallization process can be controlled by further optimizing the growth conditions of the single crystal (sublimation temperature of the source material, growth temperature, flow rate of the carrier gas, etc.) to obtain single crystals of different morphology and size for subsequent pn junction preparation.
While the present invention has been described with reference to the embodiments shown in the drawings, the present invention is not limited to the embodiments, which are illustrative and not restrictive, and it will be apparent to those skilled in the art that various changes and modifications can be made therein without departing from the spirit and scope of the invention as defined in the appended claims.

Claims (6)

1. The growth device of the multilayer organic single crystal structure is characterized by comprising a vapor phase growth unit placed under the protection of inert gas atmosphere, wherein the vapor phase growth unit comprises a gas inlet end enclosure and a gas flow sleeve detachably connected with the gas inlet end enclosure, and a source material sublimation area and a growth area are arranged in the gas flow sleeve; the area where the air inlet end enclosure is connected with the airflow sleeve is a source material introducing area, and the connection between the air inlet end enclosure and the airflow sleeve is opened to replace materials; the top of the drainage piece is slightly inclined, so that the opening of the drainage piece is large, the outlet of the drainage piece is small, and the internal airflow is directly blown to the substrate;
a cover plate extends from the bottom of the drainage piece and is arranged in at least one part of the gap between the source material sublimation area and the growth area; the air inlet sealing head is provided with a first carrier gas inlet pipe and a second carrier gas inlet pipe, the airflow direction of the first carrier gas inlet pipe is parallel to the radial extension direction of the airflow sleeve, and the airflow direction of the second carrier gas inlet pipe is perpendicular to the radial extension direction of the airflow sleeve.
2. The growth device of a multilayer organic single crystal structure according to claim 1, wherein a first O-ring is arranged at the joint of the gas flow sleeve and the gas inlet end enclosure, and a first water cooling system is arranged near the first O-ring.
3. The growth device of a multilayer organic single crystal structure according to claim 1, wherein the vapor phase growth unit further comprises an air outlet end enclosure, and one end of the air flow sleeve, which is far away from the air inlet end enclosure, is connected with the air outlet end enclosure.
4. The growth device of a multilayer organic single crystal structure according to claim 3, wherein the gas flow sleeve is detachably connected with the gas outlet end enclosure, a second O-shaped ring is arranged at the joint of the gas flow sleeve and the gas outlet end enclosure, and a second water cooling system is arranged near the second O-shaped ring.
5. A growth apparatus of a multi-layered organic single-crystal structure according to claim 1, wherein the source material sublimation zone and the growth zone are spaced apart by a distance greater than 5mm, and the temperature is controlled using separate resistance heating plates, respectively.
6. A growth apparatus for multi-layered organic single-crystal structure according to claim 5, wherein the source material sublimation zone and the growth zone are slidable along a rail and fixed at a specific site.
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