WO2015194359A1 - 電界発光素子の設計方法、その設計方法を用いて製造された電界発光素子、および、その設計方法を用いた電界発光素子の製造方法 - Google Patents
電界発光素子の設計方法、その設計方法を用いて製造された電界発光素子、および、その設計方法を用いた電界発光素子の製造方法 Download PDFInfo
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- H10K2102/301—Details of OLEDs
- H10K2102/302—Details of OLEDs of OLED structures
- H10K2102/3023—Direction of light emission
- H10K2102/3026—Top emission
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K2102/00—Constructional details relating to the organic devices covered by this subclass
- H10K2102/301—Details of OLEDs
- H10K2102/302—Details of OLEDs of OLED structures
- H10K2102/3023—Direction of light emission
- H10K2102/3031—Two-side emission, e.g. transparent OLEDs [TOLED]
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K2102/00—Constructional details relating to the organic devices covered by this subclass
- H10K2102/301—Details of OLEDs
- H10K2102/351—Thickness
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/80—Constructional details
- H10K50/805—Electrodes
- H10K50/81—Anodes
- H10K50/816—Multilayers, e.g. transparent multilayers
Definitions
- the present invention relates to a method for designing an electroluminescent element, an electroluminescent element manufactured using the design method, and a method for manufacturing an electroluminescent element using the design method.
- An electroluminescent element is composed of a photon generation layer sandwiched between a flat cathode and an anode, but in general, the anode is often a transparent electrode and the cathode is a metal reflective electrode.
- a metal electrode light is extracted from the transparent anode side and used as a single-sided light emitting device. Further, when both electrodes are transparent electrodes, a transparent light emitting element can be realized, and application to decorative lighting or the like is expected. On the other hand, not all the light emitted inside the photon generation layer is extracted, but the substrate mode in which the light is confined in the transparent substrate, the waveguide mode in which the light is confined in the photon generation layer and the transparent electrode, and the light in the metal electrode. There is a plasmon mode that is confined, which is a factor that limits the luminous efficiency of the device.
- the color and brightness of the light coming out are important, but the color and brightness of the light extracted outside are changed by the interference of the optical multilayer film and are difficult to control. A problem exists. Estimating the color and brightness of light extracted outside is important in applications.
- Non-Patent Document 1 As a method for designing the color coordinates, luminance, and the like of light that can be extracted to the outside, methods for calculating based on the photoluminescence spectrum of a light-emitting material are disclosed in JP 2010-147337 A (Patent Document 1) and JP 2009-054382 A. (Patent Document 2). Further, a detailed light extraction efficiency calculation method is disclosed in R. Meerheim et. Al., Appl. Phys. Lett., 97, 253305 (2010) (Non-Patent Document 1).
- Patent Documents 1 and 2 the external spectrum is calculated based on the photoluminescence spectrum, and there is a problem that the electroluminescence spectrum in the current injection state of the actual device cannot be accurately calculated.
- Non-Patent Document 1 it is necessary to assume the spectrum inside the photon generation layer, but details of how the ratio between the electron injection and the internal spectral intensity and the internal spectral shape are set to reduce errors in experiments and calculations. There is not enough explanation or explanation about the difference between the photoluminescence spectrum and the electroluminescence spectrum, and the difference between the experiment and the calculation remains.
- the present invention has been made in view of the above problems, and more accurately calculates an external emission spectrum output to the outside in a current injection state, and accurately estimates the amount and / or color of light extracted to the outside.
- An electroluminescent element design method, an electroluminescent element manufactured using the design method, and an electroluminescent element manufacturing method using the design method are provided.
- the photon generating layer sandwiched between the first functional layer and the second functional layer is provided between the first electrode and the second electrode which are transparent electrodes.
- the first transparent member, the first electrode, the first functional layer, the first based on the electroluminescence spectrum in the air or the first transparent member measured by passing a current through The thicknesses and the complex relative dielectric constants of the bifunctional layer, the photon generation layer, and the second electrode are obtained.
- the second electrode is a transparent electrode, and has a second transparent member on the opposite side of the second electrode from the side where the photon generation layer is provided, and the design variable is the above It further includes the complex relative dielectric constant and thickness of the second transparent member.
- an optical buffer layer is provided between at least one of the second electrode and the first transparent member, or between the second electrode and the second transparent member.
- the method further includes designing the thickness, complex relative dielectric constant, and structural constant of each film constituting the optical buffer film as design variables.
- the first optical fine structure that disturbs the amplitude and phase conditions of light is further included in any region between the transparent member and the photon generation layer, and the first optical fine structure is used as a design variable. It further includes designing the structural constant and complex dielectric constant of the structure.
- the interface between the first transparent member and the outside includes a second optical microstructure that disturbs the amplitude and phase conditions of light, and the structural constant of the second optical microstructure as a design variable and Includes complex dielectric constant.
- the electroluminescent device designed using the electroluminescent device design method according to the present invention is designed using any of the electroluminescent device design methods described above.
- the electroluminescent device design method based on the present invention the electroluminescent device manufactured based on the design variable obtained by any of the electroluminescent device design methods described above is inspected, and current drive characteristics are obtained. And measuring and analyzing the electroluminescence element measured and analyzed as a reference element, obtaining the design variable by the electroluminescent element design method according to any one of the above, based on the design variable, And a step of manufacturing an electroluminescent element.
- an external emission spectrum output to the outside in a current injection state can be calculated more accurately, and the amount and / or color of light extracted to the outside can be accurately estimated. It is possible to provide a design method of a light emitting element, an electroluminescent element manufactured using the design method, and a method of manufacturing an electroluminescent element using the design method.
- FIG. 1 is a block diagram showing the design method described in Patent Documents 1 and 2 described above.
- the conditions assumed in the calculation are (1) the photoluminescence (PL) spectrum of the luminescent material, and (2) the material, refractive index, and film thickness of the luminescent layer (S0).
- step 1 (S1) a PL spectrum is set based on the generated light intensity and the number of generated photons.
- S2 conditions for the position of the light emitting point, the film thickness, and the refractive index are set.
- S3 the light extraction efficiency is calculated.
- desired characteristics such as external light intensity, external photon number, LPW (lumen / W), EQE (external quantum efficiency) are calculated based on the results of S1 and S3.
- S3 and S4 are repeatedly executed (S5). Thereafter, when the desired characteristics are maximized in S6, calculation results such as a calculated value, light extraction efficiency, external light intensity, number of external photons, desired characteristics, and the like are obtained.
- FIG. 2 is a block diagram showing an outline of the design method of the electroluminescent element in the present embodiment.
- Conditions assumed in the calculation are (1) the external emission spectrum of the reference element, and (2) the material, refractive index, and film thickness of the light emitting layer (S00).
- step 11 (S11) an experimental value of the reference element is obtained from the generated light intensity and the number of generated photons.
- S12 the light extraction efficiency calculation value of the reference element is obtained.
- S13 the light emitting point position, film thickness, and refractive index conditions are set.
- S14 the light extraction efficiency is calculated.
- the ratio of the light extraction efficiency with the reference element is calculated based on the values and conditions obtained in S12 and S14.
- S16 desired characteristics such as external light intensity, external photon number, LPW, EQE and the like are calculated based on the experimental values and ratios obtained in S11 and S15.
- S14, S15, and S16 are repeatedly executed (S17). Thereafter, in S18, when the desired characteristics are maximized, calculation results such as calculated values, light extraction efficiency, external light intensity, number of external photons, desired characteristics, and the like are obtained.
- the electroluminescence spectrum actually measured externally in the reference element the light extraction efficiency calculated from the optical constant and the film thickness of the reference element, the optical constant of the analysis element, and
- This is a design method for calculating the external emission spectrum of the analysis element based on the light extraction efficiency calculated from the film thickness.
- the external emission spectrum output to the outside in the current injection state can be more accurately calculated, and the amount and / or color of the light extracted to the outside can be accurately estimated.
- a light emitting element design method can be realized.
- first electroluminescent element (First electroluminescent element)
- first electroluminescent device “a plurality of functional layers sandwiched between the transparent electrode and the second electrode and at least one photon generation layer are provided.
- a configuration example of an “electroluminescent device in which a transparent member is in contact with the surface of the transparent electrode opposite to the photon generation layer” will be described.
- 3 to 7 are first to fifth cross-sectional views showing a configuration example of the electroluminescent element in the present embodiment.
- the electroluminescent element 1A shown in FIG. 3 has an ITO (Indium Tin Oxide) electrode, a light emitting layer 14 and a second electrode 15 as a transparent electrode (first electrode) 13 on the first transparent member 10.
- Metal (Ag) reflective electrodes are formed in this order.
- the light emitting layer 14 includes a plurality of functional layers and a photon generation layer, and a transparent glass substrate is used for the first transparent member 10.
- the electroluminescent element 1B shown in FIG. 4 has a conductive resin 13a, a thin film Al (thin film metal electrode) 13b, and a conductive resin as the transparent electrode (first electrode) 13 as compared with the configuration of the electroluminescent element 1A.
- a laminated structure of 13c is used.
- the light emitting layer 14 is made of an organic material as compared with the structure of the electroluminescent element 1A.
- the light emitting layer includes a hole injection layer 14a and a hole transport layer 14b.
- the carrier balance in the photon generation layer 14c can be improved, and efficient light emission can be implement
- the electroluminescent element 1D shown in FIG. 6 has a configuration in which a thin film Ag is used for the transparent electrode 13, and the same effect as the electroluminescent element 1C can be obtained.
- a metal (Ag) reflective electrode can be used as the second electrode 15.
- the electroluminescent element 1C shown in FIGS. 5 and 6 is a bottom emission element.
- 3 to 6 exemplify an element (bottom emission element) that constitutes a functional layer on the first transparent member 10 using a transparent substrate, a configuration in which a reflective electrode is provided on an opaque member (top emission).
- the present embodiment is also applied to the device.
- FIG. 7 shows an electroluminescent element 1E which is a configuration example of a top emission element.
- a reflective electrode is provided as the second electrode 15 on the support substrate 16, the light emitting layer 14, the thin film Ag as the transparent electrode 13, and the sealing member as the first transparent member 10 on the second electrode 15, They are formed in this order.
- the light emitting layer 14 includes an electron injection layer 14e, an electron transport layer 14d, a photon generation layer 14c, a hole transport layer 14b, and a hole injection layer 14a from the second electrode 15 side.
- a transparent sealing member (first transparent member 10), an inert gas for sealing, or air is often provided on the transparent electrode 13.
- the transparent member of the present embodiment indicates a sealing member, an inert gas, or air.
- FIG. 8 to FIG. 10 are sixth to eighth cross-sectional views showing examples of the configuration of the electroluminescent element according to this embodiment.
- the electroluminescent element 1F shown in FIG. 8 includes an ITO electrode as the transparent electrode 13, a light emitting layer 14, an ITO electrode as the second electrode 15, and the second transparent member 17 on the first transparent member 10. They are formed in this order. By adopting this configuration, it is possible to realize a transparent light emitting element that is transparent on both sides and emits light on both sides or one side.
- the second transparent member 17 is made of, for example, ITO or a thin film metal electrode.
- the second transparent member 17 can be made of the same material as that of the first transparent member 10.
- a thin film metal film (Ag) is used as the second electrode 15 as compared with the configuration of the electroluminescent element 1F.
- a thin film metal film (Ag) is used for both the transparent electrode 13 and the second electrode 15 as compared with the configuration of the electroluminescent element 1F.
- FIG. 11 to FIG. 13 are ninth to thirteenth cross-sectional views showing examples of the configuration of the electroluminescent element according to the present embodiment.
- the electroluminescent element 1I shown in FIG. 11 has a conductive resin as the transparent electrode 13, a light emitting layer 14, a thin film metal film (Ag) as the second electrode 15, and an optical buffer layer 18 on the first transparent member 10.
- a thick multilayer metal film (Ag) is formed in this order as the dielectric multilayer film and the reflecting member 45.
- the electroluminescent element 1J shown in FIG. 12 has a dielectric multilayer film as a second optical buffer layer 19 between the first transparent member 10 and the transparent electrode 13 as compared with the configuration of the electroluminescent element 1I. Have. By adopting such a configuration, it is possible to optically design the color, the luminance ratio, and the light distribution of light emitted from both sides in the single-sided light emitting device.
- the electroluminescent element 1K shown in FIG. 13 includes a dielectric multilayer film as a second optical buffer layer 19 between the first transparent member 10 and the transparent electrode 13. In addition, it has a second transparent member instead of the reflecting member. By adopting such a configuration, it is possible to optically design the color, luminance ratio, and light distribution of light emitted from both sides in the double-sided light emitting device.
- the electroluminescent element 1L shown in FIG. 14 has an internal scattering layer between the first transparent member 10 and the thin film Ag as the transparent electrode 13 as compared with the configuration of the bottom emission element of the electroluminescent element 1D shown in FIG.
- a first optical microstructure 21 including is provided.
- the first optical fine structure 21 has a structure in which a smooth layer 21c is provided on a layer in which scattering particles as the light scattering layer 21b are held by a binder as the light scattering layer 21a.
- the thickness of the light scattering layer 21b is equal to the wavelength of light, and the size of the scattering particles has a fine structure that is several times less than the wavelength of light.
- the first optical microstructure 21 is provided between the second electrode 15 and the electron injection layer 14e as compared with the configuration of the electroluminescent element 1E shown in FIG. ing.
- the fine structure 21 includes a metal uneven structure 21d and a transparent conductive film 21e.
- the entire element above the second electrode 12 has a fine waveform, except for the first transparent member 10, as compared with the configuration of the electroluminescent element 1M shown in FIG. It is also a shape.
- an optical fine structure is provided on the second electrode 12 that is a reflective electrode, it is useful because plasmon mode loss absorbed by the electrode can be reduced.
- the above-described optical fine structure may be provided in the electroluminescent elements 1F to 1H, which are the transparent light emitting elements shown in FIGS.
- FIG. 17 is a fifteenth cross-sectional view illustrating a configuration example of the electroluminescent element according to the present embodiment.
- the second optical microstructure 31 is provided on the first transparent member 10 as compared with the configuration of the bottom emission element of the electroluminescent element 1D shown in FIG.
- a commercially available light extraction sheet can be used as the second optical microstructure 31.
- Specific examples of the structure include a structure in which the light scattering particles 31a are contained inside the transparent layer 31b and a structure in which the surface of the transparent member has irregularities, as illustrated.
- Examples of the structural constant in this case include surface unevenness height, width, unit structure period, or the size, density, and shape of scattering particles.
- FIG. 18 shows a configuration example of an electroluminescent element 1P including a plurality of photon generation layers.
- FIG. 18 is a cross-sectional view of the electroluminescent element 1P.
- the electroluminescent element 1P includes a transparent electrode 13, a light emitting layer 14A, a charge generating layer 14B, a second light emitting layer 14C, a charge generating layer 14D, a third light emitting layer 14E, and a reflective electrode on the transparent member 10. 45 are stacked in this order.
- a power source is connected between the transparent electrode 13 and the reflective electrode 45.
- Such an electroluminescent element can generate more light with the same current and is suitable for a highly efficient electroluminescent element.
- the electroluminescent element design method in this embodiment can be applied to such an electroluminescent element.
- the ratio of the light-emitting dopant in each light-emitting layer may be further included in the design variable.
- FIG. 19 shows an electroluminescent element 1Q configured so that a plurality of light emitting layers can be driven independently.
- FIG. 19 is a cross-sectional view of the electroluminescent element 1Q.
- the electroluminescent element 1Q includes a transparent electrode 13, a light emitting layer 14A, a second electrode (transparent electrode) 15, a second light emitting layer 14C, a third electrode (transparent electrode) 23, a first electrode on the transparent member 10.
- Three light emitting layers 14E and the reflective electrode 45 are laminated in this order.
- the power source 1 is provided between the transparent electrode 13 and the second electrode (transparent electrode) 15, and the power source 2 and the third electrode (second electrode) are provided between the second electrode (transparent electrode) 15 and the third light emitting layer 14E.
- a power source 3 is connected between the transparent electrode) 23 and the reflective electrode 45.
- an optical buffer layer may be included between the plurality of photon generation layers as shown in FIG. FIG. 20 is a cross-sectional view of the electroluminescent element 1R.
- the electroluminescent element 1R includes an optical buffer layer 41, a transparent electrode 13, a light emitting layer 14A, a second electrode (transparent electrode) 15, an optical buffer layer 42, and a third electrode (transparent electrode) on the transparent member 10. 23, second light emitting layer 14C, fourth electrode (transparent electrode) 24, optical buffer layer 43, fifth electrode (transparent electrode) 25, third light emitting layer 14E, sixth electrode (transparent electrode) 26
- the optical buffer layer 44 and the reflective electrode 45 are laminated in this order.
- Such a configuration makes it possible to arbitrarily control the spectrum and light distribution of the emitted light. Further, when such an optical buffer layer forms a microcavity at a specific wavelength, the emission rate of the specific wavelength can be increased.
- the electroluminescent device design method of the present embodiment including the optical buffer layer it is possible to efficiently design a configuration that realizes an electroluminescent device having a strong emission intensity at a desired wavelength and a desired angle. It becomes possible.
- the configuration including a plurality of light emitting layers may be applied to the double-sided light emitting element.
- an electroluminescent element that emits light on both sides and realizes a high efficiency or a desired spectrum can be efficiently designed.
- First transparent member 10 / second transparent member 17 The material which can be used as the 1st transparent member 10 or the 2nd transparent member 17 is illustrated.
- glass, plastic, etc. can be mentioned, but it is not limited to these.
- the transparent member preferably used include glass, quartz, and a transparent resin film.
- the glass examples include silica glass, soda lime silica glass, lead glass, borosilicate glass, and alkali-free glass. From the viewpoint of adhesion to the scattering layer, durability, and smoothness, the surface of these glass materials is subjected to physical treatment such as polishing, coatings made of inorganic or organic materials, A hybrid film combining the films can be formed.
- polyesters such as polyethylene terephthalate (PET) and polyethylene naphthalate (PEN), polyethylene, polypropylene, cellophane, cellulose diacetate, cellulose triacetate (TAC), cellulose acetate butyrate, cellulose acetate propionate ( CAP), cellulose esters such as cellulose acetate phthalate, cellulose nitrate or derivatives thereof, polyvinylidene chloride, polyvinyl alcohol, polyethylene vinyl alcohol, syndiotactic polystyrene, polycarbonate, norbornene resin, polymethylpentene, polyether ketone, polyimide , Polyethersulfone (PES), polyphenylene sulfide, polysulfone , Polyetherimide, polyetherketoneimide, polyamide, fluororesin, nylon, polymethylmethacrylate, acrylic or polyarylate, arton ((registered trademark) manufactured by JSR) or abortion ((registered trademark): product
- PET polyethylene
- Such coatings and hybrid coatings have a water vapor permeability (25 ⁇ 0.5 ° C., relative humidity 90 ⁇ 2% RH) measured by a method according to JIS K 7129-1992, of 0.01 g / (m 2 24h)
- the following gas barrier film also referred to as a barrier film or the like
- the oxygen permeability measured by a method according to JIS K 7126-1987 is 1 ⁇ 10 ⁇ 3 ml / (m 2 ⁇ 24 h ⁇ atm) or less
- the water vapor permeability is 1 ⁇ 10 ⁇ 5 g /
- a high gas barrier film of (m 2 ⁇ 24 h) or less is preferable.
- the material for forming the gas barrier film as described above may be any material that has a function of suppressing the intrusion of substances that cause deterioration of the element such as moisture and oxygen.
- silicon oxide, silicon dioxide, silicon nitride, the aforementioned polysilazane, or the like can be used.
- the method for forming the gas barrier film there is no particular limitation on the method for forming the gas barrier film.
- a polymerization method, a plasma CVD method, a laser CVD method, a thermal CVD method, a coating method, and the like can be used, but those obtained by atmospheric pressure plasma polymerization described in JP-A-2004-68143 and polysilazane (containing liquid) can be used.
- Particularly preferred is a material subjected to a modification treatment by irradiation with vacuum ultraviolet rays having a wavelength of 100 nm to 230 nm.
- Japanese Patent Laid-Open No. 2004-68143 discloses that the strength (kV / mm) of a high-frequency electric field applied from the first electrode is V1, and the high-frequency electric field applied from the second electrode is a thin film forming method using an atmospheric pressure plasma discharge processing apparatus.
- the strength (kV / mm) is V2 and the strength of the discharge start electric field (kV / mm) is IV, the relationship is V1 ⁇ IV> V2 or V1> IV ⁇ V2, and applied from the second electrode. It describes that a high frequency electric field having a power density of 1 W / cm 2 or more is applied to form a thin film.
- the design variables of the present embodiment related to the transparent member include the thickness of the member and the complex relative dielectric constant.
- the complex dielectric constant is calculated from the refractive index and the extinction constant using the formula (3) described later.
- the complex relative dielectric constant has a birefringence, it is defined as a tensor amount having a component in the three-dimensional axial direction. .
- Transparent electrode 13 / second electrode 15 The material used as the transparent electrode 13 or the 2nd electrode 15 is illustrated.
- a transparent thin film metal is particularly desirable because it has an effect of lowering the effective refractive index of the waveguide mode and facilitating scattering of the waveguide mode by the scattering layer.
- the transparent thin film metal layer is a light transmissive thin film made of a thin film metal. How thin the light can be transmitted can be expressed using the imaginary part of the refractive index. When the refractive index n and the extinction coefficient ⁇ are used, the phase change ⁇ and the transmittance T that occur when passing through a medium having a thickness d [m] can be expressed by the following equation (1).
- ⁇ is the wavelength of light in vacuum.
- Ld at which the light intensity is attenuated by e 1/2 from the equation (1) is expressed by the following equation (2).
- Transparent thin metal layer in order to have sufficient transmittance is preferably thinner than the distance L d of the formula (2).
- the transparent dielectric layer is a layer made of a dielectric.
- the definition of the dielectric will be described below. Whether the object is a metal that contains many free electrons and does not transmit much light, or a dielectric that contains few free electrons and transmits light, can be examined using the complex relative permittivity.
- the complex relative dielectric constant ⁇ c is an optical constant related to interface reflection, and is a physical quantity represented by the following formula (3) using the refractive index n and the extinction coefficient ⁇ .
- a medium having a negative real part of the complex relative dielectric constant is a metal
- a substance having a positive real part of the complex relative dielectric constant is a dielectric
- a material having a high electron transporting property tends to have a small refractive index n and a large extinction coefficient ⁇ .
- n is about 0.1
- the extinction coefficient ⁇ has a large value of 2 to 10
- the rate of change with respect to the wavelength is large. Therefore, even if the refractive index n is the same, the extinction coefficient ⁇ is greatly different, and the electron transport performance is often greatly different.
- a metal having a small refractive index n in order to lower the effective refractive index of the waveguide mode and a large extinction coefficient ⁇ in order to improve the response of electrons.
- aluminum (Al), silver (Ag), and calcium (Ca) are desirable.
- gold (Au) which has an advantage that is not easily oxidized can be considered.
- copper (Cu) is Another material which is characterized by good conductivity.
- platinum, rhodium, palladium, ruthenium, iridium, osmium, and the like are listed as materials that have good thermal and chemical properties and are not easily oxidized even at high temperatures and do not cause chemical reaction with the substrate material.
- an alloy using a plurality of metal materials may be used.
- MgAg and LiAl are often used as thin film transparent metal electrodes.
- a conductive resin that can be produced at low cost by using a coating method may be used for the transparent electrode.
- a fullerene derivative such as a perylene derivative or PCBM (phenyl C61 butyric acid methyl ester) can be considered.
- PCBM phenyl C61 butyric acid methyl ester
- the conductive resin material used as the hole transporting electrode is PEDOT (Poly (3,4-ethylenedioxythiophene)) / PSS (Poly (4-styrenesulfonate)), P3HT (Poly (3-hexylthiphene)), P3OT (Poly ( 3-octylthiophene), P3DDT ((Poly (3-dodecylthiophene-2,5-Diyl))), F8T2 (a copolymer of fluorene and bithiophene) and the like.
- PEDOT Poly (3,4-ethylenedioxythiophene)
- PSS Poly (4-styrenesulfonate
- P3HT Poly (3-hexylthiphene
- P3OT Poly ( 3-octylthiophene
- P3DDT ((Poly (3-dodecylthiophene-2,5-Diyl))
- F8T2 a copolymer
- a metal mesh, metal nanowire, metal nanoparticle or the like may be used in combination.
- the electronic conductivity of the electrode using the metal nanowire is increased, the average refractive index tends to be low, and the reflectance as viewed from the light emitting layer tends to be high.
- a transparent electrode material having a low reflectance as viewed from the light emitting layer is desirable because the light scattered in the waveguide mode can be efficiently extracted to the transparent substrate.
- a metal mesh, metal nanowire, or metal nanoparticle it has an effect of scattering the waveguide mode by the electrode itself and taking it out to the outside, which is desirable for realizing a highly efficient light-emitting element.
- the design variables of the present embodiment relating to the transparent electrode include the thickness of the member and the complex relative dielectric constant.
- the complex relative dielectric constant is calculated from the refractive index and the extinction constant using the formula (3), and when it has a birefringence, it is defined as a tensor amount having a component in the three-dimensional axial direction.
- a variable for determining the structure of each member and a complex relative dielectric constant are included in the design variables. For example, in the case of a metal mesh electrode, the height, width, period, material, combination of materials, etc. of the mesh can be included in the design variables.
- Photon generation layer 14c / functional layer When an organic material is used as the photon generation layer 14c or the functional layer, it typically has a refractive index of 1.6 to 1.8 in the visible light region.
- a material for the photon generation layer it is preferable to use an organometallic complex as a material for an organic EL element from the viewpoint of preferably obtaining effects such as improvement of external extraction quantum efficiency of the element and extension of emission lifetime.
- the metal involved in complex formation is preferably any one metal belonging to Groups 8 to 10 of the periodic table, Al or Zn, and in particular, the metal is Ir, Pt, Al or Zn. Is preferred.
- the design variables of the present embodiment relating to the photon generation layer include the thickness of the member and the complex relative dielectric constant.
- the complex relative dielectric constant is calculated from the refractive index and the extinction constant using the formula (3), and when it has a birefringence, it is defined as a tensor amount having a component in the three-dimensional axial direction.
- a variable for determining the structure of each member and a complex relative dielectric constant are included in the design variable.
- Reflective electrode (second electrode) 15 As the material of the reflective electrode, the metal materials exemplified as the material of the transparent thin film metal layer can be used. Other alloys and inks containing metal nanoparticles may be used. Further, a transparent electrode, a dielectric multilayer mirror, a metal uneven structure, and a photonic crystal may be used in combination with the reflective layer. When a dielectric multilayer mirror, a metal uneven structure, or a photonic crystal is used as a reflective layer, there is an advantage that plasmon loss in the reflective layer can be eliminated.
- the design variables of the present embodiment relating to the reflective electrode include the thickness of the member and the complex dielectric constant.
- the complex relative dielectric constant is calculated from the refractive index and the extinction constant using the formula (3), and when it has a birefringence, it is defined as a tensor amount having a component in the three-dimensional axial direction.
- a variable for determining the structure of each member and a complex relative dielectric constant are included in the design variable.
- Optical buffer layer As the optical buffer layer, in addition to the dielectric multilayer film, a photonic crystal structure can be used. In order to create a dielectric multilayer film or a photonic crystal structure, it is necessary to combine materials having a plurality of dielectric constants, and the dielectric material is preferably transparent at a wavelength at which light is generated in the photon generation layer.
- the resin material examples include vinyl chloride, acrylic, polyethylene, polypropylene, polystyrene, ABS, nylon, polycarbonate, polyethylene terephthalate, polyvinylidene fluoride, Teflon (registered trademark), polyimide, phenol resin, and a refractive index of 1.4 to There is 1.8.
- the design variables of the present embodiment relating to the optical buffer layer include the thickness and complex relative dielectric constant of each member constituting the buffer layer.
- the complex relative dielectric constant is calculated from the refractive index and the extinction constant using the formula (3), and when having a birefringence, it is defined as a tensor amount having a component in the three-dimensional axial direction.
- variables for determining the structure of each member and optical constants are included in the design variables.
- the film thickness and complex relative dielectric constant of each optical thin film constituting the dielectric multilayer film can be included in the design variables.
- the optical buffer layer is configured as a photonic crystal
- the dielectric structure of the unit cell of the photonic crystal and the complex relative dielectric constant of the material forming the unit cell can be included in the design variables.
- optical microstructure examples include a layer containing scattering particles, a layer having a concavo-convex structure, and a structure in which the entire light emitting layer has a corrugated structure.
- a design variable is composed of a variable for determining the size and shape of the structure and a complex relative dielectric constant of each structure.
- the complex relative dielectric constant is calculated from the refractive index and the extinction constant using the formula (3), and when it has a birefringence, it is defined as a tensor amount having a component in the three-dimensional axial direction.
- the light extraction efficiency is the number of photons extracted to the transparent member or air when the number of photons generated in the photon generation layer is 1.
- the calculation method disclosed in Patent Documents 1 and 2 shown in the background art hereinafter referred to as the calculation method in the background art
- the calculation method in the present embodiment is different in the following two points.
- the first difference between the calculation method in the background art and the calculation method in the present embodiment is that “in both the reference element and the desired analysis element, the light extraction efficiency from the photon generation layer to the transparent member or air is calculated.
- the ratio of the light extraction efficiency between the reference element and the analysis element is calculated, and the relationship between the thickness of each layer constituting the reference element and the analysis element and the complex relative permittivity of each layer and the ratio of the light extraction efficiency is calculated. It's a point to seek. This makes it possible to correct the difference between the photoluminescence spectrum and the electroluminescence spectrum caused by electron injection or the microcavity effect during the experiment.
- the second difference between the calculation method in the background art and the calculation method in the present embodiment is that “quantum optical analysis” is performed.
- the characteristic noticed in the present embodiment is various characteristics of external light at the time of electron injection.
- the calculation method in the background art is not explained, in order to calculate the characteristics at the time of electron injection, it is necessary to obtain the internal quantum efficiency by quantum optical analysis.
- a precise calculation is performed by calculating a change in the light emission rate due to the microcavity effect and solving a rate equation relating to light emission recombination.
- a rate equation related to luminescent recombination is written as the following equation (4).
- N exc is the exciton density in the photon generation layer
- N inj is the exciton injection density
- the light emission recombination probability ⁇ is calculated by the following equation (6).
- the calculation of the light emission recombination rate can be performed by combining the light emission lifetime unique to the material and the calculation method disclosed in Non-Patent Document 1.
- the analysis is performed by combining the light emission lifetime specific to the material and the existing electromagnetic field analysis methods such as the finite time difference method (FDTD method), the transfer matrix method, and the like.
- FDTD method finite time difference method
- the transfer matrix method and the like.
- ⁇ e is the electron-exciton conversion efficiency determined by the spin injection rule
- ⁇ is the luminescence recombination probability
- ⁇ OE is the “light extraction efficiency” to the transparent member or air, and includes quantum optical analysis It has become.
- the front spectrum S front ( ⁇ ) of the analysis element is calculated as the following equation (9) by the ratio G front ( ⁇ ) of the air total angle spectrum and the air front spectrum obtained by calculation.
- the calculation of the color coordinates and the luminous flux [lm] after the desired spectrum is obtained can be performed according to the definition of CIE.
- this calculation method can be applied not only to the full angle spectrum of air but also to the full angle spectrum inside the transparent member.
- a method for obtaining the full angle spectrum inside the transparent member by experiment there is a method in which a hemispherical lens sufficiently larger than the light emitting region is closely attached to the transparent member using matching oil and measured using an integrating sphere.
- a simple method is to perform exhaustive calculation within a desired range of design variables and achieve desired color coordinates or efficiency. In this case, a large number of levels can be calculated efficiently with a small number of levels when calculated based on the experimental design method.
- Each level is computationally efficient when it is computed in parallel by a plurality of cluster machines. In order to increase the calculation speed, it is desirable to perform parallel calculation using a graphic processor.
- optimization calculations It is desirable to combine the optimized algorithm with the steepest descent method, the conjugate gradient method, the linear programming method, the genetic algorithm, etc. regarding the desired characteristics. In optimization, it is desirable to perform optimization in consideration of robustness. As a specific robustness calculation method, it is desirable to perform a plurality of calculations for design variables in the vicinity of a certain level, evaluate by the magnitude of variation in desired characteristics, and select a level with small variation.
- FIG. 21 shows the procedure of the design method in the present embodiment.
- This design method mainly includes a current drive characteristic of the reference element and a part R100 for performing analysis, and an optimization loop 200 for the analysis element. Below, the design method of the essential part of the design method in this Embodiment is demonstrated.
- the design variable of the reference element is determined based on the film thickness, complex non-dielectric constant, structural constant, etc. (S110). Thereafter, a reference element is created (S120). Next, the reference element is measured (S130). Specifically, the measurement of the electroluminescence spectrum during current driving and the external quantum efficiency during current driving are measured. The measurement result of the reference element is input to S250 in the optimization loop R200 described later.
- the reference element is calculated based on the determination of the design variable of the reference element (S110) (S140). Specifically, the reference element is calculated using quantum optical analysis, electromagnetic field analysis, and ray tracing. The calculation result of the reference element is input to S240 in the optimization loop R200 described later.
- the design variable of the analysis element is determined based on the film thickness, complex non-dielectric constant, structural constant, etc. (S210). Thereafter, the analysis element is calculated (S220). Specifically, the analysis element is calculated using quantum optical analysis, electromagnetic field analysis, and ray tracing.
- the calculation result of the analysis element is obtained (S230). Specifically, the calculation results of the wavelength dependency of the relative light emission rate, the wavelength dependency of the light extraction efficiency, and the wavelength and angle dependency of the element emission intensity are obtained.
- the emission intensity ratio between the analysis element and the reference element is calculated. Specifically, the ratios of the wavelength dependency of the relative light emission rate, the wavelength dependency of the light extraction efficiency, and the wavelength and angle dependency of the device emission intensity are calculated.
- the electroluminescence spectrum of the analysis element is calculated (S250). Specifically, the wavelength dependence of the light extraction efficiency and the wavelength and angle dependence of the element emission intensity are calculated.
- desired characteristics of the analysis element are calculated (S260). Specifically, characteristics calculated from external quantum efficiency, front luminance, front color coordinates, angle dependency of color coordinates, light emission efficiency [lm / w], and other emission spectrum and its angle dependency, and power efficiency Value.
- the target value of the desired characteristic is compared with the analysis value, and the design variable is changed to approach the target value (S270).
- S270 random calculation, experimental design, steepest descent method, Newton method, conjugate gradient method, and genetic algorithm are used as calculation methods.
- the process returns to S210 again, the design variable of the analysis element is determined (S210), and the above optimization loop R200 is executed.
- This embodiment has a plurality of functional layers sandwiched between a transparent electrode and a second electrode and at least one photon generation layer, and is transparent on the surface of the transparent electrode opposite to the photon generation layer.
- the present invention relates to a method for designing an electroluminescent element in contact with a member.
- a typical example of the electroluminescence element is an organic EL electroluminescence element 100 as shown in FIG.
- the organic EL electroluminescent element 100 shown in FIG. 22 is provided with ITO (film thickness 150 nm) as a transparent electrode 113 on a glass substrate as a transparent member 110, and a first functional layer 114a and a photon generation layer 114c (by a vacuum evaporation method).
- the second functional layer 114e is provided. Thereafter, an Ag film (film thickness: 100 nm) as a reflective electrode was provided as the second electrode 15.
- the photon generation layer 114c was formed using a green phosphorescent material having an emission peak wavelength of 520 nm.
- the first functional layer 114a was provided with a hole injection layer, a hole transport layer, and an electron block layer (total 35 nm).
- the second functional layer 114e was provided with a hole blocking layer, an electron transport layer, and an electron injection layer (total xnm).
- the transparent member 110 is in contact with the surface of the transparent electrode 113 opposite to the photon generation layer 114c.
- the design variables in the design of the organic EL electroluminescent element 100 shown in FIG. 22 are the thicknesses of the transparent member 110, the transparent electrode 113, the first functional layer 114a, the second functional layer 114e, and the second electrode 115, And the complex relative dielectric constant, and the position and distribution of the light emitting points in the photon generation layer 114c.
- the purpose of the design method of the present embodiment is to realize a design that optimizes external characteristics during current driving.
- the external characteristic during current driving is an index as a desired characteristic shown in FIG. 29 to be described later, or an arbitrary index calculated using values in FIGS. 23 and 25 to 28 described later.
- Specific examples of indices include power efficiency, current efficiency, external quantum efficiency, front luminance, front color coordinates (x, y), front color temperature, color rendering, and angle dependency of color coordinates.
- the reference element can be created by a vacuum deposition method or the like.
- FIG. 23 summarizes the design variables used for the reference element. The design variable is composed of the film thickness and complex relative dielectric constant of each constituent member.
- the transparent substrate 110 is made of a glass substrate, has a film thickness of 700 micrometers (0.7 mm), and a complex relative dielectric constant of ⁇ 1.
- the transparent electrode 113 is made of ITO, has a film thickness of 150 nm, and a complex relative dielectric constant of ⁇ 2.
- the first functional layer 114a includes a hole injection layer, a hole transport layer, and an electron block layer, and has a film thickness of 35 nm and a complex relative dielectric constant of ⁇ 3.
- the photon generation layer 114c is composed of a light emitting layer, and has a film thickness of 20 nm and a complex relative dielectric constant of ⁇ 4.
- the second functional layer 114e includes a hole blocking layer, an electron transport layer, and an electron injection layer, and has a film thickness of 50 nm and a complex relative dielectric constant of ⁇ 5.
- the second electrode 115 is made of an Ag film, has a film thickness of 100 nm, and a complex relative dielectric constant of ⁇ 6. It is assumed that the position of the light emitting point is the center of the photon generation layer 114c and the distribution is concentrated at the center in a delta function.
- FIG. 24 shows an example of the configuration of an apparatus 1000 for measuring the external emission spectrum.
- the external emission spectrum of the reference element 100 may be a full angle spectrum measured using an integrating sphere 1100. Therefore, the reference element 100 is placed on the central portion of the integrating sphere 1100 using the platform 1200.
- the control device 1300 when measuring the spectrum of the reference element 100, it is preferable to record the number of photons for each wavelength in the control device 1300 using the spectroscope 1400. Further, the conditions (current and voltage) of the power supplied to the reference element 100 are recorded by the control device 1300 during measurement. In this way, the measurement data of the reference element 100 can be used for later analysis.
- FIG. 25 shows a specific example of measurement data.
- driving current (symbol I in , unit [A])
- driving voltage (symbol V in , unit [V])
- electroluminescence spectrum (symbol S EL1 ( ⁇ ), unit [/ S / nm])
- Element area (symbol S dev , unit [m 2 ])
- element temperature (symbol T dev , unit [K])
- front luminance (symbol I cd , unit [cd / m 2 ])
- front chromaticity x (symbol) x, unit dimensionless)
- front chromaticity y (symbol y, unit dimensionless)
- front color temperature (symbol T, unit [K]).
- the electroluminescence spectrum measured here is converted into the number of photons per unit time and unit wavelength.
- the electroluminescence spectrum measured in another unit can be converted into the number of photons per unit time and unit wavelength based on the measurement conditions.
- it can convert into an intensity spectrum by applying the energy per photon to the optical spectrum in units of the number of photons.
- Items to be calculated include relative emission recombination rate (parcel factor) wavelength dependence (symbol F 1 ( ⁇ ), unitless dimension, analysis method (quantum optical analysis / electromagnetic field analysis)), light extraction efficiency into air ( Symbol ⁇ Air1 ( ⁇ ), unit dimensionless, analysis method (electromagnetic field analysis, ray tracing)), angular distribution of air light intensity at a specific wavelength (symbol D Air1 ( ⁇ ), unit [/ sr], analysis method (electromagnetic field analysis) , Ray tracing)), light extraction efficiency to transparent member (symbol ⁇ Sub1 ( ⁇ ), unitless dimension, analysis method (electromagnetic field analysis, ray tracing)), and angular distribution of light intensity in transparent member at specific wavelength ( Symbol D Sub1 ( ⁇ ), unit [/ sr], analysis method (electromagnetic field analysis, ray tracing)).
- each analysis method can be calculated based on Patent Documents 1 and 2 and the electromagnetic field analysis method. It is assumed that the intensity angular distribution is standardized to be 1 when integrated over a solid angle (see Equation 11). In the case of designing an element that emits light on both sides, it is assumed that the standardization of Expression 11 is made for light emission in each direction.
- the parcel factor is the ratio of the light emission recombination rate to the light emission recombination rate of the light emitting material alone when there is a microcavity composed of a dielectric, metal, or the like in the periphery. ⁇ ). This completes the description of the measurement / analysis of the current drive characteristics of the reference element.
- the design variable of the element to be analyzed is determined (S210).
- the value of the design variable shown in FIG. 23 is changed.
- Specific methods of changing include a steepest descent method and a genetic algorithm that increase desired characteristics to be described later.
- This combination of input variables is vectorized, and the first loop is x [1], the second loop is x [2],..., And the Nth loop is x [N].
- Items calculated for the N-th loop analysis element include relative emission recombination rate (parcel factor) wavelength dependence (symbol F [N] ( ⁇ ), unitless dimension, analysis method (quantum optical analysis / electromagnetic field analysis) ), Light extraction efficiency into air (symbol ⁇ Air [N] ( ⁇ ), unitless dimension, analysis method (electromagnetic field analysis, ray tracing)), angular distribution of air light intensity at a specific wavelength (symbol D Air [N] ( ⁇ ), unit [/ sr], analysis method (electromagnetic field analysis, ray tracing)), light extraction efficiency to transparent member (symbol ⁇ Sub [N] ( ⁇ ), unit dimensionless, analysis method (electromagnetic field analysis, light ray) Tracking)), and angular distribution of light intensity in the transparent member at a specific wavelength (symbol D Sub [N] ( ⁇ ), unit [/ sr], analysis method (electromagnetic field analysis, ray tracing)).
- the light extraction efficiency represents the ratio of light generated in the photon generation layer to the air or the transparent member.
- EQE external quantum efficiency
- a ratio for calculating the electroluminescence spectrum of the analysis element is calculated using the measurement items measured at the time of current injection of the reference element shown in FIG. 25 (S240). In addition, the electroluminescence spectrum of the analysis element is calculated using the intensity ratio described above (S250). The items and symbols calculated here are defined as shown in FIGS.
- the items calculated for the analysis element of the N-th loop are the intensity ratio of energy in the air with the reference element (symbol G Air [N] ( ⁇ ), unit dimensionless), reference element and Intensity ratio (symbol G Sub [N] ( ⁇ ), unit dimensionless), electroluminescence spectrum calculation value (symbol S EL [N] ( ⁇ ), unit [/ s / nm]), In addition, the calculated value of electroluminescence spectrum in the transparent member (symbol S ELSub [N] ( ⁇ ), unit [/ s / nm]).
- the index values calculated for the analysis element of the N-th loop are power efficiency (symbol LPW [N], dimension [lm / W]), current efficiency (symbol LPA [N], dimension [lm] / A]), external quantum efficiency (symbol EQE [N], dimensionless), front luminance (symbol Y [N], dimension [cd / m 2 ]), front color coordinate x (symbol x [N], dimensionless) ), Front color coordinate y (symbol y [N], dimensionless), front color temperature (symbol T [N], [K]), front color rendering (symbol Ra [N], dimensionless), angle of color coordinate Dependency x (symbol x ⁇ [N] ( ⁇ ), dimensionless) and angle dependency y (symbol y ⁇ [N] ( ⁇ ), dimensionless) of color coordinates are included.
- the measurement of the reference element 100 shown in FIG. 24 is a measurement of the spectrum that appears in the air outside the element.
- the intensity ratio and the external emission spectrum calculation value shown in FIG. 28 are calculated by the equation (12) using the experimental electroluminescence spectrum shown in FIG.
- the intensity ratio of energy in the air between the reference element and the analysis element is calculated using the existing quantum optical analysis method, electromagnetic field analysis method, and ray tracing method shown in FIG.
- the electroluminescence spectrum of the analytical element is calculated using the measured value of the electroluminescence spectrum of the reference element (S130), the calculation result of the reference element (S140), and the calculation result of the analytical element (S230). (S240, S250). By calculating in this way, it becomes possible to accurately calculate the external emission electroluminescence spectrum at the time of current injection.
- the air in the arbitrary Nth calculation, or the external emission spectrum wavelength distribution inside the transparent member and the angular distribution of the light intensity are analyzed (S260). If the user is interested in the color coordinates of the emitted light, the color coordinates can be calculated by calculating according to the definition of CIE (International Commission on Illumination) using the calculated spectrum and angular distribution.
- CIE International Commission on Illumination
- the power efficiency of the analysis element can be calculated based on the driving conditions of the reference element shown in FIG. 25 and the calculation results shown in FIGS. Furthermore, by using the angle distribution characteristics shown in FIG. 27, the angle distribution of luminance and color coordinates can also be calculated.
- FIG. 29 lists indexes that can be calculated as desired characteristics.
- Desired characteristics are not limited to the indices listed in FIG. 29, but may include any indices calculated using the values listed in FIG. 23 and FIGS.
- Desired characteristics are not limited to the indices listed in FIG. 29, but may include any indices calculated using the values listed in FIG. 23 and FIGS.
- a design variable is slightly changed in the vicinity of a design variable and the variation of the index value is used as a new index value and optimization is performed to minimize the variation
- the design suitable for can be made.
- the color rendering properties of the color targets R1 to R15 may be independently evaluated as an index of the color rendering properties.
- the transparent substrate 110 is composed of a glass substrate, the film thickness is 700 micrometers (0.7 mm), and the complex relative dielectric constant is ⁇ 1.
- the transparent electrode 113 is made of ITO, has a film thickness of 150 nm, and a complex relative dielectric constant of ⁇ 2.
- the first functional layer 114a includes a hole injection layer, a hole transport layer, and an electron block layer, and has a film thickness of 37 nm and a complex relative dielectric constant of ⁇ 3.
- the photon generation layer 114c is composed of a light emitting layer, and has a film thickness of 20 nm and a complex relative dielectric constant of ⁇ 4.
- the second functional layer 114e includes a hole blocking layer, an electron transport layer, and an electron injection layer, and has a film thickness of 113 nm and a complex relative dielectric constant of ⁇ 5.
- the second electrode 115 is made of an Ag film, has a film thickness of 100 nm, and a complex relative dielectric constant of ⁇ 6.
- the (N + 1) th calculation is performed to bring the desired characteristic closer to the target value (S270).
- the iterative calculation algorithm include a steepest descent method, a conjugate gradient method, and a genetic algorithm that increase desired characteristics. Also, any existing optimization algorithm may be used.
- the optimization loop R200 is continued. The optimization loop R200 is terminated when it is determined that the desired characteristics are sufficiently close, or when the prescribed number of repetitions is completed.
- an evaluation function at the time of optimization and design an algorithm so that the evaluation function is minimized or maximized. For example, when optimization is performed to bring the front color coordinate (x, y) close to the target color coordinate (x target , y target ), an error of the color coordinate is determined as an evaluation function by the following equation (13), and the evaluation function is minimized. It is desirable to design the steepest descent method, conjugate gradient method, genetic algorithm, etc.
- design variables x [1], x [2]... X [N] are determined in advance based on the experimental design method, and parallel calculation is performed for combinations of N design variables. It is good to do.
- For parallel computation computation using a GPU (Graphics Processing Unit), computation using a cluster machine, computation using a multi-CPU, and the like are used.
- the element shown in FIG. 23 is used as the reference element, the desired characteristic is the front color coordinate (x, y) of the element, and the target front color coordinate is brought closer to the green coordinate (0.30, 0.60) of sRGB.
- the optimization calculation was performed as follows. As the design variable, the thicknesses of a plurality of functional layers were used. The experimental design was used as the optimization method, and multiple levels were calculated simultaneously by multi-CPU parallel calculation.
- FIG. 31 shows the optimization calculation results. Note that the level number N is reassigned in the order of large error.
- FIG. 31 shows that the combination x [256] of design variables has the smallest difference ⁇ xy among the calculated values and is a desirable combination of design variables.
- FIG. 30 shows a design variable x [256] as an optimization result. It can be seen that the reference element and the design variable in FIG. 23 are changed. Thus, by deriving the “relationship between the design variable and the desired characteristic”, it can be understood that the optimization for bringing the desired characteristic closer to the target value can be performed.
- FIG. 32 shows a flow when the design method in the above embodiment is applied to a method of manufacturing an electroluminescent element.
- the optimization loop R200 is once turned to output the optimum design.
- an electroluminescent element is manufactured based on the optimum design variable.
- the manufactured electroluminescent device is inspected, and current drive characteristics are measured and analyzed.
- the optimization loop R200 is turned again using the inspected electroluminescent element as a reference element to feed back to the manufacturing process. In this way, by applying the design method in the above embodiment to the manufacturing method, it becomes possible to stably manufacture an electroluminescent element having a desired characteristic value.
- the organic EL electroluminescent element 100 to be analyzed has a structure shown in FIG. 22, ITO (film thickness 150 nm) is provided as the transparent electrode 113 on the glass substrate as the transparent member 110, and the first functional layer is formed by vacuum deposition. 114a, a photon generation layer 114c (film thickness 20 nm), and a second functional layer 114e are provided. Thereafter, an Ag film (film thickness: 100 nm) as a reflective electrode was provided as the second electrode 15.
- the photon generation layer 114c was formed using a green phosphorescent material having an emission peak wavelength of 520 nm.
- the first functional layer 114a was provided with a hole injection layer, a hole transport layer, and an electron block layer (total 35 nm).
- the second functional layer 114e was provided with a hole blocking layer, an electron transport layer, and an electron injection layer (total xnm). Experiments and calculations were compared while changing the total film thickness from the hole blocking layer to the electron injection layer.
- FIG. 33 shows a result of comparison between the experimental results, the analysis method in the background art, and the analysis method in this example.
- FIG. 34 shows the error between experiment and analysis. It can be seen that the present example can calculate the experimental chromaticity and the external quantum efficiency more accurately. By using the analysis method of this embodiment, more accurate chromaticity and efficiency can be calculated. The same analysis can be applied to the analysis of the electroluminescent element of the single-sided light emitting element shown in FIGS.
- the design method of the present embodiment can be applied to the electroluminescent elements 1F to 1H which are the transparent light emitting elements shown in FIGS.
- the electroluminescent device design method of this embodiment for a transparent light emitting device, the amount and color of the light extracted outside both sides can be accurately estimated.
- the design method of the present embodiment can be applied to the electroluminescent elements 1I to 1J including the optical buffer layer shown in FIGS.
- By optimizing the design using the light emission efficiency improvement effect by the microcavity effect of the optical multilayer film by the design method of the present embodiment it is possible to design an element having the efficiency optimized with a desired color.
- the design method of the present embodiment can be applied to the electroluminescent elements 1K to 1M including the optical microstructure shown in FIGS.
- a light emitting element with high light emission efficiency and small emission intensity and small color shift can be realized.
- the design method of the present embodiment can be applied to the electroluminescent element 1O including the second optical fine structure shown in FIG.
- the electroluminescent elements 1A to 1O designed by applying the design method of the present embodiment shown in FIGS. 5 to 17 are useful as surface-emitting light sources capable of emitting a desired color with high efficiency. The same applies to the electroluminescent elements 1P to 1R shown in FIGS.
- the design method of the electroluminescent element in the background art calculates the external light spectrum of the electroluminescent element by current injection based on the photoluminescence spectrum, and calculates the external emission spectrum and calculation of the actual electroluminescent element.
- the emission spectrum and color coordinates of the electroluminescent device cannot be accurately calculated due to different external emission spectra.
- the efficiency and color coordinates are calculated accurately by calculating the external emission spectrum of the analysis element based on the external emission spectrum of the reference element.
- the efficiency and color coordinates are calculated accurately by calculating the external emission spectrum of the analysis element based on the external emission spectrum of the reference element.
- the external emission spectrum output to the outside in the current injection state can be calculated more accurately, and the amount and color of the light extracted to the outside can be accurately estimated.
- the present embodiment for a transparent light emitting element, it is possible to accurately estimate the amount and color of light extracted outside both sides.
- by optimizing the design using the light emission efficiency improvement effect by the microcavity effect of the optical multilayer film by the method of the present embodiment it is possible to design an electroluminescence device having the efficiency optimized with a desired color.
- an electroluminescent device with high light emission efficiency and small light emission intensity and color shift at each angle.
- the scattering efficiency of the substrate mode light using the design method of the present embodiment, it is possible to realize an electroluminescent device with high luminous efficiency and small luminous intensity and small color shift for each angle.
- an electroluminescent element designed using the design method of the present embodiment can achieve desired chromaticity with high efficiency.
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Abstract
Description
図1に上述した特許文献1および2に記載の設計方法をブロック図で示す。計算で仮定する条件は、(1)発光材料のフォトルミネッセンス(PL)スペクトル、および(2)発光層の材料、屈折率、膜厚である(S0)。ステップ1(S1)において、発生光強度および発生フォトン数により、PLスペクトルを設定する。S2において、発光点の位置、および、膜厚、屈折率の条件設定が行なわれる。S3において、光取出し効率が計算される。S4において、S1およびS3の結果に基づき、外部光強度、外部フォトン数、LPW(lumen/W)、EQE(external quantum efficiency:外部量子効率)等の所望の特性が計算される。所望の特性の最大化を求めるため、S3およびS4を繰り返し実行する(S5)。その後、S6において、所望の特性の最大化が得られた場合には、計算値、光取り出し効率、外部光強度、外部フォトン数、所望の特性等の計算結果が得られる。
『2.1 電界発光素子の構成』
本実施の形態における電界発光素子の構成について説明する。以下では有機電界発光素子を例に説明するが、本設計方法は有機電界発光素子の設計に限定されず、無機材料で構成される発光ダイオード(LED)等の設計にも用いることができる。
以下、図3から図7を参照して、第1の電界発光素子として、「透明電極と第2の電極との間に狭持された複数の機能層と少なくとも1層の光子発生層とを有し、透明電極の光子発生層とは反対側の面に透明部材が接している電界発光素子」の構成例について説明する。図3から図7は、本実施の形態における電界発光素子の構成例を示す第1から第5断面図である。
以下、図8から図10を参照して、第2の電界発光素子として、「第2の電極が透明電極でありかつ第2の電極の発光層が設けられる側と反対側に第2の透明部材を有する電界発光素子」の構成例について説明する。図8から図10は、本実施の形態における電界発光素子の構成例を示す第6から第8断面図である。
以下、図11から図13を参照して、第3の電界発光素子として、「透明電極と透明部材の間、もしくは第2の電極と第2の透明部材の間の少なくとも一方に光学多層膜を有する電界発光素子」の構成例について説明する。図11から図13は、本実施の形態における電界発光素子の構成例を示す第9から第13断面図である。
以下、図14から図16を参照して、第4の電界発光素子として、「透明部材と光子発生層との間に光の振幅および位相条件を乱す光学微細構造を含む電界発光素子」の構成例について説明する。図14から図16は、本実施の形態における電界発光素子の構成例を示す第12から第14断面図である。
以下、図17を参照して、第5の電界発光素子として、「透明部材と外部の界面に、光の振幅および位相条件を乱す第2の光学微細構造を含む電界発光素子」の構成例について説明する。図17は、本実施の形態における電界発光素子の構成例を示す第15断面図である。
以下に、上述した電界発光素子1A~1Nを構成する各種部材(材料)の詳細について説明する。
第1の透明部材10または第2の透明部材17として用いることのできる材料を例示する。たとえば、ガラス、プラスチック等を挙げることができるが、これらに限定されない。好ましく用いられる透明部材としては、ガラス、石英、透明樹脂フィルムを挙げることができる。
透明電極13、あるいは第2の電極15として用いられる材料を例示する。透明電極13としては、特に透明薄膜金属が、導波モードの実効屈折率を下げ、導波モードを散乱層で散乱させやすくする効果を持つので望ましい。透明薄膜金属層は薄膜金属で構成される光透過性を有する薄膜である。どの程度の薄さであれば光が透過するかは、屈折率の虚部を用いて表すことができる。屈折率nと消衰係数κを用いた場合、厚さd[m]の媒質を通過する際に生じる位相変化φと透過率Tとは、以下の式(1)で表すことができる。
光子発生層14cや機能層として有機材料を用いる場合には可視光の領域で典型的には1.6~1.8の間の屈折率を持つ。特に、光子発生層の材料は、素子の外部取りだし量子効率の向上、発光寿命の長寿命化等の効果を好ましく得る観点から、有機EL素子用材料として有機金属錯体を用いることが好ましい。さらに、錯体形成に係る金属が元素周期表の8族~10族に属するいずれか1種の金属、AlまたはZnであることが好ましく、特に上記金属が、Ir、Pt、AlまたはZnであることが好ましい。
反射電極の材料としては透明薄膜金属層の材料として例示した金属材料を用いることができる。その他の合金、金属ナノ粒子を含有したインクなどを用いてもよい。また、透明電極と誘電体多層膜ミラー、金属凹凸構造、フォトニック結晶を反射層と組み合わせて用いてもよい。誘電体多層膜ミラー、金属凹凸構造、フォトニック結晶を反射層として用いた場合には、反射層でのプラズモン損失をなくすことができる利点がある。
光学バッファ層としては誘電体多層膜のほか、フォトニック結晶構造を用いることができる。誘電体多層膜やフォトニック結晶構造を作成するためには、複数の誘電率を持つ材料を組み合わせる必要があり、誘電体材料は光子発生層で光が発生する波長において透明であることが望ましい。透明な材料としては、透明部材として用いられる材料を利用できる。具体的な材料としては、TiO2(屈折率n=2.5)、SiOx(屈折率n=1.4~3.5)などを用いることができる。その他の誘電体材料の例としては、ダイヤモンド、弗化カルシウム(CaF)、チッ化シリコン(Si3N4)などが例示できる。
光学微細構造としては、散乱粒子を含有する層、凹凸構造を有する層、発光層全体が波形構造を有する構造などが挙げられる。いずれの場合においても、構造の大きさや形を決めるための変数と、各構造の複素比誘電率から設計変数が構成される。なお、複素比誘電率は屈折率と消衰定数から式(3)を用いて計算され、複屈折率を有する場合は3次元の軸方向に成分をもつテンソル量として定義される。
本節においては、本実施の形態における光取り出し効率の計算方法について説明する。光取り出し効率は、光子発生層で発生した光子数を1とした場合に、透明部材あるいは空気に取り出される光子数である。具体的な計算方法については、背景技術で示した特許文献1、2に開示される計算方法(以下、背景技術における計算方法、と称する。)を用いることができるが、背景技術における計算方法と本実施の形態における計算方法とは、以下の2つの点で異なっている。
ここでは、図2を参照しながら、最適化計算の望ましい方法について説明する。電界発光素子の設計変数一つ一つに関して、『2.3 光取り出し効率と外部光の諸特性計算方法』で説明した方法で外部スペクトルを計算することにより外部量子効率、発光輝度、色座標が計算される。
『3.1 概要』
図21に本実施の形態における設計方法の手順を示す。この設計手法は主に基準素子の電流駆動特性ならびに解析を行う部分R100と、解析素子に対する最適化ループ200で構成される。以下では、本実施の形態における設計方法の本質的部分の設計方法について説明する。
(3.2.1 基準素子の設計変数決定、基準素子作成)
最初に基準素子の設計変数を決定する(S110)。典型的には各機能を実現するために最低必要な膜厚で作成するとよい。ここでは、図22に示した膜厚と、x=50nmを設定した例で説明する。基準素子は真空蒸着法等で作成できる。図23に、基準素子に用いた設計変数をまとめる。設計変数は各構成部材の膜厚と複素比誘電率とで構成される。
作成した基準素子(S120)の電極に電圧を印加し、外部発光スペクトルを測定する(S130)。図24に外部発光スペクトルを測定する装置1000の構成の一例を示す。基準素子100の外部発光スペクトルは積分球1100を用いて全角度スペクトルを測定するとよい。よって、基準素子100は、積分球1100の中心部に、台1200を用いて載置される。
図21に戻り、引き続き、基準素子の計算を実施する(S140)。基準素子の計算は量子光学解析、電磁場解析、光線追跡といった手法で構成され、それぞれ計算できる項目が異なる。ここでは、計算される項目と解析手法の選択について、図26にまとめる。
以下では、図21を参照しながら、最適化ループ内の各手順について説明する。
解析したい素子の設計変数を決定する(S210)。ここでは、図23に示した設計変数の値を変化させることとする。具体的な変化のさせ方としては、後述する所望の特性を上げるような最急降下法、遺伝的アルゴリズムが挙げられる。この入力変数の組み合わせをベクトル化して、1ループ目はx[1]、2ループ目はx[2]、・・・、Nループ目をx[N]とおくこととする。
次に、解析素子の計算を行なう(S220、S230)。ここで計算される項目は図26に示した基準素子の計算される項目と同じである。ただし、設計変数について1ループ目はx[1]、2ループ目はx[2]、・・・、Nループ目がx[N]と変化している点に注意する。ここではNループ目の解析結果について、図27に定めるように記号を決めるものとする。
図25に示す基準素子の電流注入時に測定された測定項目を用いて、解析素子のエレクトロルミネッセンススペクトルを計算するための比を計算する(S240)。また、上述の強度比を用いて解析素子のエレクトロルミネッセンススペクトルを計算する(S250)。ここで計算される項目と記号とを、図28および図29のように定義する。
上記、3.3.3説までの解析結果により、任意のN番目の計算における空気、あるいは透明部材内部における外部発光スペクトル波長分布と光強度の角度分布が解析されることになる(S260)。また、発光する光の色座標等に興味がある場合は、計算されたスペクトルと角度分布を用いて、CIE(国際照明委員会)の定義に従って計算することで色座標を計算できる。
これまでの説明により、設計変数をベクトルとしてまとめたN番目の設計変数x[N]が定まると、図30に例示される所望の特性が、基準素子の実験で求めたエレクトロルミネッセンススペクトルから計算される。
基準素子としては図23に示した素子を用い、所望の特性としては素子の正面色座標(x,y)とし、目標正面色座標をsRGBの緑座標(0.30,0.60)に近づけるように最適化計算を行なった。設計変数としては複数の機能層の膜厚を用いた。最適化手法には実験計画法を用い、マルチCPUによる並列計算によって複数水準を同時計算した。
図32に電界発光素子の製造方法に上記実施の形態における設計方法を適用した場合の流れを示す。[3.設計方法の詳細]で説明したように、いったん最適化ループR200を回し、最適設計を出力する。次に、その最適設計変数に基づいて電界発光素子の製造を行なう。その後、製造した電界発光素子を検査し、電流駆動特性を測定し解析する。
[5.1 片面発光素子]
以下では、本実施の形態の効果をより詳細に説明するために、有機電界発光素子の解析を例に説明する。解析する有機EL電界発光素子100は、図22に示す構造を有し、透明部材110としてのガラス基板上に、透明電極113としてITO(膜厚150nm)を設け、真空蒸着法によって第1機能層114a、光子発生層114c(膜厚20nm)、第2機能層114eを設ける。その後、第2の電極15として、反射電極であるAg膜(膜厚100nm)を設けた。なお、光子発生層114cは、発光ピーク波長が520nmである緑色の燐光発光材料を用いた。第1機能層114aは、正孔注入層、正孔輸送層、および電子ブロック層(合計35nm)を設けた。第2機能層114eは、正孔阻止層、電子輸送層、および電子注入層(合計xnm)を設けた。正孔阻止層から電子注入層までの総膜厚を変化させながら、実験と計算を比較した。
図8から図10に示した透明発光素子である電界発光素子1F~1Hに本実施の形態の設計方法は適用可能である。透明な発光素子について本実施の形態の電界発光素子の設計方法を実施することにより、両側の外部に取り出される光の量や色を正確に見積もることができる。
図11および図12に示した光学バッファ層を含む電界発光素子1I~1Jに本実施の形態の設計方法は適用可能である。光学多層膜のマイクロキャビティ効果による発光効率向上効果を利用した設計を本実施の形態の設計方法で最適化することにより、所望の色で効率を最適化した素子を設計できる。
図13から図16に示した光学微細構造を含む電界発光素子1K~1Mに本実施の形態の設計方法は適用可能である。導波モード光やプラズモン光の取り出し効率を本実施の形態の設計方法で設計することで、発光効率が高く、角度ごとの発光強度や色ずれの小さな発光素子を実現できる。
図17に示した第2の光学微細構造を含む電界発光素子1Oに本実施の形態の設計方法は適用可能である。基板モード光を効率良く散乱できる設計を実現することで、発光効率が高く、角度ごとの発光強度や色ずれの小さな発光素子を実現できる。
図5~図17に示した、本実施の形態の設計方法を適用して設計した電界発光素子1A~1Oは、高効率で所望の色を出せる面発光光源として有用である。また、図18~図20に示した電界発光素子1P~1Rも同様である。
Claims (7)
- 透明電極である第1の電極と第2の電極の間に、第1機能層および第2機能層に挟まれる光子発生層を有し、前記第1の電極の前記光子発生層が設けられる側とは反対側には第1の透明部材を有する電界発光素子の設計方法であって、
前記電界発光素子の構成を備える基準素子、および、前記電界発光素子の構成を備える所望の解析素子を準備し、
前記第1の透明部材、前記第1の電極、前記第1機能層、前記第2機能層、前記光子発生層、および、前記第2の電極の、それぞれの厚み、および、それぞれの複素比誘電率、並びに、前記光子発生層における発光点の位置、および、前記光子発生層における発光点の分布を設計変数として、量子光学解析、電磁場解析、および光線追跡を行ない、
前記基準素子と前記解析素子との両方において、前記光子発生層から前記透明部材または空気への光取り出し効率を計算して、前記基準素子と前記解析素子との「光取り出し効率の比」を算出し、さらに、
前記基準素子および前記解析素子をそれぞれ構成する前記各層の厚みおよび前記各層の複素比誘電率と前記「光取り出し効率の比」との関係を求め、
前記関係および前記基準素子に電流を流すことで測定される空気または前記第1の透明部材におけるエレクトロルミネッセンススペクトルに基づいて、設計変数として、前記第1の透明部材、前記第1の電極、前記第1機能層、前記第2機能層、前記光子発生層、および、前記第2の電極の、それぞれの前記厚み、および、それぞれの前記複素比誘電率を得る、電界発光素子の設計方法。 - 前記第2の電極は透明電極であり、かつ、前記第2の電極の前記光子発生層が設けられる側と反対側に第2の透明部材を有し、設計変数として前記第2の透明部材の複素比誘電率と厚みとをさらに含む、請求項1に記載の電界発光素子の設計方法。
- 前記第2の電極と前記第1の透明部材との間、または前記第2の電極と前記第2の透明部材との間の少なくともいずれか一方の間に光学バッファ層をさらに有し、
設計変数として前記光学バッファ膜を構成する各膜の厚み、複素比誘電率、および構造定数を設計することをさらに含む、請求項2に記載の電界発光素子の設計方法。 - 前記透明部材と前記光子発生層との間のいずれかの領域に光の振幅および位相条件を乱す第1の光学微細構造をさらに含み、
設計変数として前記第1の光学微細構造の構造定数および複素比誘電率を設計することをさらに含む、請求項1から請求項3のいずれか1項に記載の電界発光素子の設計方法。 - 前記第1の透明部材と外部との界面に、光の振幅および位相条件を乱す第2の光学微細構造を含み、
設計変数として前記第2の光学微細構造の構造定数および複素比誘電率を含む、請求項1から請求項4にいずれか1項に記載の電界発光素子の設計方法。 - 請求項1から請求項5のいずれか1項に記載の電界発光素子の設計方法を用いて設計された電界発光素子。
- 請求項1から請求項5のいずれか1項に記載の電界発光素子の設計方法により得られた前記設計変数の基づき製造された電界発光素子を検査し、電流駆動特性を測定および解析する工程と、
前記測定および解析された前記電界発光素子を基準素子として、請求項1から請求項5のいずれか1項に記載の電界発光素子の設計方法により前記設計変数を得て、前記設計変数に基づき、電界発光素子の製造を行なう工程と、
と備える、電界発光素子の製造方法。
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JP2004063349A (ja) * | 2002-07-30 | 2004-02-26 | Matsushita Electric Works Ltd | 白色有機電界発光素子、白色有機電界発光素子の設計方法 |
JP2006339050A (ja) * | 2005-06-02 | 2006-12-14 | Fuji Electric Holdings Co Ltd | 有機el発光素子光学シミュレータ、及び、そのプログラム |
JP2009054383A (ja) * | 2007-08-24 | 2009-03-12 | Panasonic Electric Works Co Ltd | 有機エレクトロルミネッセンス素子の設計方法及び有機エレクトロルミネッセンス素子 |
WO2014065084A1 (ja) * | 2012-10-26 | 2014-05-01 | コニカミノルタ株式会社 | 電界発光素子およびその電界発光素子を用いた照明装置 |
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US10115932B2 (en) | 2018-10-30 |
US20170179443A1 (en) | 2017-06-22 |
US20180138460A1 (en) | 2018-05-17 |
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US9893324B2 (en) | 2018-02-13 |
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