Ultrastrong coupling in Super Yellow polymer microcavities and development of highly efficient polariton light-emitting diodes and light-emitting transistors.

We present detailed studies on exciton-photon coupling and polariton emission based on a poly(1,4-phenylenevinylene) copolymer, Super Yellow (SY), in a series of optical microcavities and optoelectronic devices, including light-emitting diode (LED) and light-emitting transistor (LET). We show that sufficiently thick SY microcavities can generate ultrastrong coupling with Rabi splitting energies exceeding 1 eV and exhibit spectrally narrow, nearly angle-independent photoluminescence following lower polariton (LP) mode dispersion. When the microcavity is designed with matched LP low-energy state and exciton emission peak for radiative pumping, the conversion efficiency from exciton to polariton emission can reach up to 80%. By introducing appropriate injection layers in a SY microcavity and optimizing the cavity design, we further demonstrate a high-performance ultrastrongly coupled SY LED with weakly dispersive electroluminescence along LP mode and a maximum external quantum efficiency (EQE) of 2.8%. Finally, we realize an ultrastrongly coupled LET based on vertical integration of a high-mobility ZnO transistor and a SY LED in a microcavity, which enables a large switching ratio, uniform emission in the ZnO pattern, and LP mode emission with a maximum EQE of 2.4%. This vertical LET addresses the difficulties of achieving high emission performance and precisely defining the emission area in typical planar LETs, and opens up the possibility of applying various strongly coupled emitters for advanced polariton devices and high-resolution applications.

Development of a highly efficient, strongly coupled organic light-emitting diode based on intracavity pumping architecture.

We report a highly efficient polariton organic light-emitting diode (POLED) based on an intracavity pumping architecture, where an absorbing J-aggregate dye film is used to generate polariton modes and a red fluorescent OLED is used for radiative pumping of emission from the lower polariton (LP) branch. To realize the device with large-area uniformity and adjustable coupling strength, we develop a spin-coating method to achieve high-quality J-aggregate thin films with controlled thickness and absorption. From systematic studies of the devices with different J-aggregate film thicknesses and OLED injection layers, we show that the J-aggregate film and the pump OLED play separate roles in determining the coupling strength and electroluminescence efficiency, and can be simultaneously optimized under a cavity design with a good LP-OLED emission overlap for effective radiative pumping. By increasing the absorption with thick J-aggregate film and improving the electron injection of pump OLED with Li2CO3 interlayer, we demonstrate the POLED with a large Rabi splitting energy of 192 meV and a maximum external quantum efficiency of 1.2%, a record efficiency of POLEDs reported so far. This POLED architecture can be generally applied for exploration of various organic materials to realize novel polariton devices and electrically pumped lasers.

Optical, structural, and mechanical properties of silicon oxynitride films prepared by pulsed magnetron sputtering.

Silicon oxynitride films were deposited by reactive pulsed magnetron sputtering. The optical, structural, and mechanical properties of silicon oxynitride films with different nitrogen proportions were analyzed via spectroscopy, atomic force microscopy, Twyman-Green interferometer, and nanoindentation. The refractive indices of the silicon oxynitride films were adjusted from 1.487 to 1.956 with the increase in nitrogen proportions. The surface roughness decreased from 1.33 to 0.97 nm with the increase in nitrogen proportions. The residual stress of the silicon oxynitride films was higher than for pure silicon nitride and silicon dioxide films. The hardness and Young's modulus increased from 13.51 to 19.74 GPa and 110.41 to 140.49 GPa with the increase in nitrogen proportions, respectively. The hardness and Young's modulus of antireflection coatings using silicon oxynitride film were 13.64 GPa and 102.11 GPa, respectively. Silicon oxynitride film could be used to improve the hardness of antireflective coatings.

Varying stress of SiOxCy thin films deposited by plasma polymerization.

SiOxCy thin films were deposited by plasma polymerization. The stress of the deposited SiOxCy thin films can be modified by adjusting the beam current, the anode voltage, and the flow rate of hexamethyldisiloxane (HMDSO) gas and oxygen. Reducing the beam current or increasing the flow rate of HMDSO gas increased the linear/cage structure ratio and turned the stress of the SiOxCy thin films from compressive to tensile. The linear/cage structure ratio can be adjusted by changing the composite parameter, W[FM]c/[FM]m, to control the stress of the deposited plasma polymer films. Multilayers of TiO2/SiO2/TiO2 were coated on a SiOxCy plasma polymer film herein, reducing their stress by 70% from 0.06 to 0.018 GPa. The refractive index is 1.55, and the absorption coefficient is less than 10-4 at 550 nm of the SiOxCy films. Superior optical performances of SiOxCy thin films make their use in optical thin films.

Optical properties and residual stress in Nb-Si composite films prepared by magnetron cosputtering.

This paper investigates Nb-Si metal composite films with various proportions of niobium in comparison to pure Nb films. Films were prepared by two-target RF-DC magnetron cosputtering deposition. The optical properties and residual stress were analyzed. A composition of Nb(0.74)Si(0.26) was chosen toward the design and fabrication of solar absorbing coatings having a high absorption in a broad wavelength range, a low residual stress, and suitable optical constants. The layer thicknesses and absorption characteristics of the Nb-Si composite films adhere more closely to the design than other coatings made of dielectric film materials.

Process dependence of morphology and microstructure of cyanine dye J-aggregate film: correlation with absorption, photo- and electroluminescence properties.

Cyanine dye J-aggregate films are a class of absorbing and luminescent materials which have been extensively applied in the polariton-based research. Here we systematically study the DEDOC cyanine dyes J-aggregate films made by layer-by-layer assembly and spin-coating processes to establish a clear correlation between the film structure and the absorption and luminescence properties. From detailed analyses of morphology, optical spectra, and light-emitting diode characteristics, we demonstrate that layer-by-layer assembled film has higher degrees of homogeneity and molecular packing quality than spin-coated film, leading to a higher absorption coefficient, more uniform luminescence, and a greater electroluminescence quantum efficiency with maximized thickness.

Optical constants of electrochromic films and contrast ratio of reflective electrochromic devices.

This study investigates the optical constants of WO3 electrochromic films and NiO ion-storage films in bleached and colored states and that of a Ta2O5 film used as an ion conductor. These thin films were all prepared by electron-beam evaporation and characterized using a spectroscopic ellipsometer. The spectra obtained using a spectrophotometer and those calculated from the optical constants agreed closely. An all-solid thin-film reflective electrochromic device was fabricated and discussed. Its mean contrast ratio of reflectance in the range of 400-700 nm was 37.91.

Adjustable exciton-photon coupling with giant Rabi-splitting using layer-by-layer J-aggregate thin films in all-metal mirror microcavities.

Developing of highly absorbing thin films is essential for exploration of light-matter interaction and polariton-based applications. We demonstrate here layer-by-layer assembled J-aggregate thin films of (DEDOC) cyanine dyes that have high absorption coefficient and controlled thicknesses, leading to adjustable exciton-photon coupling and Rabi splitting exceeding 400 meV at room temperature in all-metal mirror microcavities.

Thermal expansion coefficients of obliquely deposited MgF2 thin films and their intrinsic stress.

This study elucidates the effects of columnar angles and deposition angles on the thermal expansion coefficients and intrinsic stress behaviors of MgF2 films with columnar microstructures. The behaviors associated with temperature-dependent stresses in the MgF2 films are measured using a phase-shifting Twyman-Green interferometer with a heating stage and the application of a phase reduction algorithm. The thermal expansion coefficients of MgF2 films at various columnar angles were larger than those of glass substrates. The intrinsic stress in the MgF2 films with columnar microstructures was compressive, while the thermal stress was tensile. The thermal expansion coefficients of MgF2 films with columnar microstructures and their intrinsic stress evidently depended on the deposition angle and the columnar angle.

Optical properties and residual stress in aluminum nitride films prepared by alternating-current dual reactive magnetron sputtering.

Aluminum nitride films were deposited by alternating-current dual reactive magnetron sputtering. The influence of different nitrogen flow and working pressures at a sputtering power of 5 kW on the refractive index, extinction coefficient, crystalline structure, residual stress, and surface roughness of aluminum nitride films was discussed. The aluminum nitride film would have high refractive index, low extinction coefficient and small residual stress at suitable nitrogen flow rate and low working pressure.

Effect of thermal annealing on the optical properties and residual stress of graded-index-like films deposited by radio-frequency ion-beam sputtering.

Composite films of Ta-Si oxide and graded-index-like films have been realized by using radio-frequency ion-beam sputtering. The influence of thermal annealing on the optical properties and residual stress of single-layer composite films and graded-index-like films has been studied. The residual stress and optical properties of both types of films were more stable than that of the notch filters fabricated from a series of discrete quarter-wave layers made by alternatively stacking high and low index materials after annealing.

Residual stress in Ta2O5-SiO2 composite thin-film rugate filters prepared by radio frequency ion-beam sputtering.

Ta-Si oxide composite thin-film rugate filters were prepared by radio frequency ion-beam sputtering and their residual stress and substrate deflections were measured. The residual stress and substrate deflection of these composite film rugate filters were less than that of notch filters made from a series of discrete quarter-wave layers with alternate high and low indices because of the smooth modulation of composition and no interface structure of the rugate filter.

Residual stress in obliquely deposited MgF2 thin films.

MgF(2) films with a columnar microstructure are obliquely deposited on glass substrates by resistive heating evaporation. The columnar angles of the films increases with the deposition angle. Anisotropic stress does not develop in the films with tilted columns. The residual stresses in the films depend on the deposition and columnar angles in a columnar microstructure.

Investigation of thermal annealing of optical properties and residual stress of ion-beam-assisted TiO2 thin films with different substrate temperatures.

Titanium oxide films were prepared by ion-beam-assisted deposition on glass substrates at various substrate temperatures. The effect of the temperature of thermal annealing from 100 degrees C to 300 degrees C on the optical properties and residual stress was investigated. The influence on the stoichiometry and residual stress of titanium oxides deposited at different substrate temperature was discussed. The residual-stress was minimum and the extinction coefficient was maximum at an annealing temperature of 200 degrees C with a substrate temperature of 150 degrees C. However, when the substrate temperature was increased to 200 degrees C and 250 degrees C, the residual stress was minimum and the extinction coefficient was maximum at an annealing temperature of 250 degrees C. The spectra of x-ray photoelectron spectroscopy reveal that the films lost oxygen and slowly generated lower suboxides at the annealing temperature at which the residual stress was minimum and the extinction coefficient was maximum. As the annealing temperature increased above the temperature at minimum stress, the lower suboxides began to capture oxygen and form stable oxides. TiO2 films deposited at substrate temperatures of 200 degrees C and 250 degrees C were more stable than films deposited at 150 degrees C.

Effects of temperature on columnar microstructure and recrystallization of TiO2 film produced by ion-assisted deposition.

Titanium oxide thin films were deposited by electron-beam evaporation with ion-beam-assisted deposition. The effect of the substrate temperature and annealing temperature on the columnar microstructure and recrystallization of titanium oxide was studied. The values of the refractive index varied from 2.26 to 2.4, indicating that the different substrate temperatures affected the film density. X-ray diffraction revealed that all films were amorphous as deposited. At annealing temperatures from 100 degrees C to 300 degrees C, only the anatase phase was formed. As the substrate temperature increased from 150 degrees C to 200 degrees C to 250 degrees C, the recrystallization temperature fell from 300 degrees C through 250 degrees C to 200 degrees C. Changing the substrate temperature resulted in the formation of various types of columnar microstructure, as determined by scanning-electron microscopy. Different columnar structures resulted in different surface morphologies, as measured by atomic-force microscopy.

Effect of thermal annealing on the optical properties and residual stress of TiO2 films produced by ion-assisted deposition.

The effects of thermal annealing of titanium oxide films deposited by ion-beam assistance at annealing temperatures from 100 degrees C to 300 degrees C on the residual stress and optical properties of the films was investigated. The refractive indices and extinction coefficients increased gradually as the temperature was increased from 100 degrees C to 200 degrees C and then declined gradually as the temperature was increased further from 200 degrees C to 300 degrees C. The film lost oxygen and slowly generated lower suboxides as the annealing temperature was reduced below 200 degrees C, as determined by x-ray photoelectron spectroscopy (XPS). As the annealing temperature increased above 200 degrees C, the lower suboxides began to capture oxygen and form stable oxides. XPS measurements were made to verify both the binding energy associated with the Ti 2p line and the variation of the O 1s line. A Twyman-Green interferometer was employed for phase-shift interferometry to study the residual stress. The residual stress declined as the temperature was reduced from 100 degrees C to 200 degrees C because the lower suboxides reduced the stress in the film. Above 200 degrees C, the film began to capture oxygen, so the residual stress rose. At 300 degrees C, the film was no longer amorphous as the anatase was observed by x-ray diffraction.