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2.  Demonstration of InAsSb/AlInSb Double Heterostructure Detectors for Room Temperature Operation in the 5–8 μm Wavelength Range
J.S. Wojkowski, H. Mohseni, J.D. Kim, and M. Razeghi
SPIE Conference, San Jose, CA, -- January 27, 1999 ...[Visit Journal]
We report the first demonstration of InAsSb/AlInSb double heterostructure detectors for room temperature operation. The structures were grown in a solid source molecular beam epitaxy reactor on semi-insulating GaAs substrate. The material was processed to 400x400 micrometer mesas using standard photolithography, etching, and metallization techniques. No optical immersion or surface passivation was used. The photovoltaic detectors showed a cutoff wavelength at 8 micrometer at 300 K. The devices showed a high quantum efficiency of 40% at 7 μm at room temperature. A responsivity of 300 mA/W was measured at 7 μm under a reverse bias of 0.25 V at 300 K resulting in a Johnson noise limited detectivity of 2x108 cm·Hz½/W. [reprint (PDF)]
 
2.  High power continuous wave operation of single mode quantum cascade lasers up to 5 W spanning λ∼3.8-8.3 µm
Quanyong Lu, Steven Slivken, Donghai Wu, and Manijeh Razeghi
Optics Express Vol. 28, Issue 10, pp. 15181-15188-- May 4, 2020 ...[Visit Journal]
In this work, we report high power continuous wave room-temperature operation single mode quantum cascade lasers in the mid-infrared spectral range from 3.8 to 8.3 µm. Single mode robustness and dynamic range are enhanced by optimizing the distributed feedback grating coupling design and the facet coatings. High power single mode operation is secured by circumventing the over-coupling issue and spatial hole burning effect. Maximum single-facet continuous-wave output power of 5.1 W and wall plug efficiency of 16.6% is achieved at room temperature. Single mode operation with a side mode suppression ratio of 30 dB and single-lobed far field with negligible beam steering is observed. The significantly increased power for single mode emission will boost the QCL applications in long-range free-space communication and remote sensing of hazardous chemicals. [reprint (PDF)]
 
2.  Type-II superlattice-based extended short-wavelength infrared focal plane array with an AlAsSb/GaSb superlattice etch-stop layer to allow near-visible light detection
Romain Chevallier, Arash Dehzangi, Abbas Haddadi, and Manijeh Razeghi
Optics Letters Vol. 42, Iss. 21, pp. 4299-4302-- October 17, 2017 ...[Visit Journal]
A versatile infrared imager capable of imaging the near-visible to the extended short-wavelength infrared (e-SWIR) is demonstrated using e-SWIR InAs/GaSb/AlSb type-II superlattice-based photodiodes. A bi-layer etch-stop scheme consisting of bulk InAs0.91Sb0.09 and AlAs0.1Sb0.9/GaSb superlattice layers is introduced for substrate removal from the hybridized back-side illuminated photodetectors. The implementation of this new technique on an e-SWIR focal plane array results in a significant enhancement in the external quantum efficiency (QE) in the 1.8–0.8μm spectral region, while maintaining a high QE at wavelengths longer than 1.8μm. Test pixels exhibit 100% cutoff wavelengths of ∼2.1 and ∼2.25μm at 150 and 300K, respectively. They achieve saturated QE values of 56% and 68% at 150 and 300K, respectively, under back-side illumination and without any anti-reflection coating. At 150K, the photodetectors (27μm×27μm area) exhibit a dark current density of 4.7×10−7  A/cm2 under a −50  mV applied bias providing a specific detectivity of 1.77×1012  cm·Hz1/2/W. At 300K, the dark current density reaches 6.6×10−2  A/cm2 under −50 mV bias, providing a specific detectivity of 5.17×109  cm·Hz1/2/W. [reprint (PDF)]
 
2.  Evaluating the size-dependent quantum efficiency loss in a SiO2-Y2O3 hybrid gated type-II InAs/GaSb long-infrared photodetector array
G. Chen , A. M. Hoang , and M. Razeghi
Applied Physics Letters 104 , 103509 (2014)-- March 14, 2014 ...[Visit Journal]
Growing Y2O3 on 20 nm SiO2 to passivate a 11 μm 50% cut-off wavelength long-wavelength infrared type-II superlattice gated photodetector array reduces its saturated gate bias (VGsat ) to −7 V. Size-dependent quantum efficiency (QE) losses are evaluated from 400 μm to 57 μm size gated photodiode. Evolution of QE of the 57 μm gated photodiode with gate bias and diode operation bias reveals different surface recombination mechanisms. At 77 K and VG,sat , the 57 μm gated photodiode exhibits QE enhancement from 53% to 63%, and it has 1.2 × 10−5 A/cm² dark current density at −200 mV, and a specific detectivity of 2.3 × 1012 Jones. [reprint (PDF)]
 
2.  AlGaN/AlN MOVPE heteroepitaxy: pulsed co-doping SiH4 and TMIn
Ilkay Demir, Yusuf Koçak, A. Emre Kasapoğlu, Manijeh Razeghi, Emre Gür and Sezai Elagoz
Semicond. Sci. Technol. 34 075028-- June 24, 2019 ...[Visit Journal]
We report a new growth approach pulsed co-doping growth of AlxGa1−xN (x > 0.5) epilayers on AlN/Al2O3 templates by metal organic vapor phase epitaxy (MOVPE). Using this approach SiH4 (silane) and TMIn (trimethylindium) supplied to the growth chamber alternately and pulsed during the growth of AlGaN epilayers. Structural and morphological quality of AlGaN epilayers were investigated by high resolution x-ray diffraction (HR-XRD), atomic force microscopy (AFM), Raman spectroscopy, and scanning electron microscopy (SEM) techniques. It has shown that higher crystalline quality with low full width at half maximum (FWHM) and smoother surface morphology with reduced hexagonal hillock density has been obtained by the pulsed co-doping growth approach. Volcano like hillock structures has been confirmed by Raman mapping. [reprint (PDF)]
 
2.  Recent performance records for mid-IR quantum cascade lasers
M. Razeghi; Y. Bai; S. Slivken; S. Kuboya; S.R. Darvish
Terahertz and Mid Infrared Radiation: Basic Research and Practical Applications, 2009. TERA-MIR International Workshop [5379656], (2009) -- November 9, 2009 ...[Visit Journal]
The wall plug efficiency of the mid-infrared quantum cascade laser in room temperature continuous wave operation is brought to 17%. Peak output power from a broad area (400 μm x 3 mm) device gives 120 W output power in pulsed mode operation at room temperature. Using a single-well-injector design, specifically made for low temperature operation, a record wall plug efficiency of 53% is demonstrated at 40 K. [reprint (PDF)]
 
2.  Room temperature terahertz quantum cascade laser sources with 215 μW output power through epilayer-down mounting
Q. Y. Lu, N. Bandyopadhyay, S. Slivken, Y. Bai, and M. Razeghi
Appl. Phys. Lett. 103, 011101 (2013)-- July 1, 2013 ...[Visit Journal]
We report room temperature terahertz (THz) quantum cascade laser sources with high power based on difference frequency generation. The device is Čerenkov phase matched and spectrally purified with an integrated dual-period distributed-feedback grating. Symmetric current injection and epilayer-down mounting of the device onto a patterned submount are used to improve the electrical uniformity and heat removal, respectively. The epilayer-down mounting also allows for THz anti-reflective coating to enhance the THz outcoupling efficiency. Single mode emission at 3.5 THz with a side-mode suppression ratio and output power up to 30 dB and 215  μW are obtained, respectively. [reprint (PDF)]
 
2.  Stability of far fields in double heterostructure and multiple quantum well InAsSb/InPAsSb/InAs midinfrared lasers
H. Yi, A. Rybaltowski, J. Diaz, D. Wu, B. Lane, Y. Xiao, and M. Razeghi
Applied Physics Letters 70 (24)-- June 16, 1997 ...[Visit Journal]
Far fields in perpendicular direction to the junction are investigated in double heterostructure (DH) and multiple quantum well (MQW) midwave-infrared InAsSb/InPAsSb/InAs lasers (λ = 3.2–3.6 μm). Strong broadening of the far fields in the DH lasers was observed with increases in temperature and/or current. On the contrary, MQW lasers with otherwise identical structure exhibit very stable far fields as narrow as 23° for all the operating conditions investigated. Our experiment and theoretical modeling suggest that these different behaviors of far fields in DH and MQW lasers are attributed to the refractive index fluctuation in the InAsSb laser active region. [reprint (PDF)]
 
2.  Intrinsic AlGaN photodetectors for the entire compositional range
D. Walker, X. Zhang, A. Saxler, P. Kung, J. Xu, and M. Razeghi
SPIE Conference, San Jose, CA, -- February 12, 1997 ...[Visit Journal]
AlxGa1-xN ultraviolet photoconductors with cut- off wavelengths from 365 nm to 200 nm have been fabricated and characterized. Various characteristics of the devices, such as photoresponse, voltage-dependent responsivity, frequency-dependent responsivity and noise spectral density, were measured and cross-referenced with optical, electrical and structural characteristics of the material to provide information about the mechanisms taking place during detection. The maximum detectivity reached 5.5 X 108 cm·Hz½/W at a modulating frequency of 14 Hz. The effective majority carrier lifetime in AlxGa1-xN materials, derived from frequency-dependent photoconductivity measurements, has been estimated to be from 6 to 35 msec. The frequency-dependent noise-spectrum shows that it is dominated by Johnson-noise at high frequencies for low Al-composition samples. [reprint (PDF)]
 
2.  Transport properties in n-type InSb films grown by metalorganic chemical vapor deposition
S.N. Song, J.B. Ketterson, Y.H. Choi, R. Sudharsanan, and M. Razeghi
Applied Physics Letters 63 (7)-- August 16, 1993 ...[Visit Journal]
We have measured the temperature and magnetic field dependence of the Hall mobility and transverse magnetoresistance in n-type InSb films epitaxially grown on GaAs substrates by metalorganic chemical vapor deposition. The films show a giant magnetoresistance: e.g., at 240 K the resistivity increases over 20 times at a magnetic field of 5 T; the low field coefficient of resistivity at 77 K is as high as 47.5 μ·Ω· cm/G. The Hall mobility decreases with magnetic field and saturates at higher fields. By taking the interface carrier transport into account, the observed field dependence of the Hall mobility and magnetoresistance may be understood based on a two-layer model. [reprint (PDF)]
 
2.  Passivation of Type-II InAs/GaSb superlattice photodetectors
A. Hood, Y. Wei, A. Gin, M. Razeghi, M. Tidrow, and V. Nathan
SPIE Conference, Jose, CA, Vol. 5732, pp. 316-- January 22, 2005 ...[Visit Journal]
Leakage currents limit the operation of high performance Type-II InAs/GaSb superlattice photodiode technology. Surface leakage current becomes a dominant limiting factor, especially at the scale of a focal plane array pixel (< 25 µm) and must be addressed. A reduction of the surface state density, unpinning the Fermi level at the surface, and appropriate termination of the semiconductor crystal are all aims of effective passivation. Recent work in the passivation of Type-II InAs\GaSb superlattice photodetectors with aqueous sulfur-based solutions has resulted in increased R0A products and reduced dark current densities by reducing the surface trap density. Additionally, photoluminescence of similarly passivated Type-II InAs/GaSb superlattice and InAs GaSb bulk material will be discussed. [reprint (PDF)]
 
2.  High power, high wall-plug efficiency, high reliability, continuous-wave operation quantum cascade lasers at Center for Quantum Devices
Razeghi, Manijeh
SPIE Proceedings Volume 11296, Optical, Opto-Atomic, and Entanglement-Enhanced Precision Metrology II; 112961C-- February 25, 2020 ...[Visit Journal]
Since the demonstration of the first quantum cascade laser (QCL) in 1997, QCLs have undergone considerable developments in output power, wall plug efficiency (WPE), beam quality, wavelength coverage and tunability. Among them, many world-class breakthroughs were achieved at the Center for Quantum Device at Northwestern University. In this paper, we will discuss the recent progress of our research and present the main contributions of the Center for Quantum Devices to the QCL family on high power, high wall-plug efficiency (WPE), continuous-wave (CW) and room temperature operation lasers. [reprint (PDF)]
 
2.  Aluminum nitride films on different orientations of sapphire and silicon
K. Dovidenko, S. Oktyabrsky, J. Narayan, and M. Razeghi
Journal of Applied Physics79 (5)-- March 1, 1996 ...[Visit Journal]
The details of epitaxial growth and microstrictural characteristics of AlN films grown on sapphire (0001), (1012) and Si (100), (111) substrates were investigated using plan‐view and cross‐sectional high‐resolution transmission electron microscopy and x‐ray diffraction techniques. The films were grown by metalorganic chemical vapor deposition using TMA1+NH3+N2 gas mixtures. Different degrees of epitaxy were observed for the films grown on α‐Al2O3 and Si substrates in different orientations. The epitaxial relationship for (0001) sapphire was found to be (0001)AlN∥(0001)sap with in‐plane orientation relationship of [0110]AlN∥[1210]sap. This is equivalent to a 30° rotation in the basal (0001) plane. For (1012) sapphire substrates, the epitaxial relationship was determined to be (1120)AlN∥(1012)sap with the in‐plane alignment of [0001]AlN∥[1011]sap. The AlN films on (0001) α‐Al2O3 were found to contain inverted domain boundaries and a/3〈1120〉 threading dislocations with the estimated density of 1010 cm−2. The density of planar defects (stacking faults) found in AlN films was considerably higher in the case of (1012) compared to (0001) substrates. Films on Si substrates were found to be highly textured c axis oriented when grown on (111) Si, and c axis textured with random in‐plane orientation on (100) Si. The role of thin‐film defects and interfaces on device fabrication is discussed. [reprint (PDF)]
 
2.  High-quality visible-blind AlGaN p-i-n photodiodes
E. Monroy, M. Hamilton, D. Walker, P. Kung, F.J. Sanchez, and M. Razeghi
Applied Physics Letters 74 (8)-- February 22, 1999 ...[Visit Journal]
We report the fabrication and characterization of AlxGa1−xN p-i-n photodiodes (0 < x < 0.15) grown on sapphire by low-pressure metalorganic chemical vapor deposition. The devices present a visible rejection of six orders of magnitude with a cutoff wavelength that shifts from 365 to 338 nm. Photocurrent decays are exponential for high load resistances, with a time constant that corresponds to the RC product of the system. For low load resistances, the transient response becomes non-exponential, with a decay time longer than the RC constant. This behavior is justified by the strong frequency dependence of the device capacitance. By an admittance analysis, we conclude that speed is not limited by deep levels, but by substitutional Mg capture and emission time. [reprint (PDF)]
 
2.  Quantum dot in a well infrared photodetectors for high operating temperature focal plane arrays
S. Tsao, T. Yamanaka, S. Abdollahi Pour, I-K Park, B. Movaghar and M. Razeghi
SPIE Proceedings, San Jose, CA Volume 7234-0V-- January 25, 2009 ...[Visit Journal]
InAs quantum dots embedded in InGaAs quantum wells with InAlAs barriers on InP substrate grown by metalorganic chemical vapor deposition are utilized for high operating temperature detectors and focal plane arrays in the middle wavelength infrared. This dot-well combination is unique because the small band offset between the InAs dots and the InGaAs well leads to weak dot confinement of carriers. As a result, the device behavior differs significantly from that in the more common dot systems that have stronger confinement. Here, we present energy level modeling of our QD-QW system and apply these results to interpret the detector behavior. Detectors showed high performance with D* over 1010 cm·Hz1/2W-1 at 150 K operating temperature and with high quantum efficiency over 50%. Focal plane arrays have been demonstrated operating at high temperature due to the low dark current observed in these devices. [reprint (PDF)]
 
2.  Scaling in back-illuminated GaN avalanche photodiodes
K. Minder, J.L. Pau, R. McClintock, P. Kung, C. Bayram, M. Razeghi and D. Silversmith
Applied Physics Letters, Vol. 91, No. 7, p. 073513-1-- August 13, 2007 ...[Visit Journal]
Avalanche p-i-n photodiodes of various mesa areas were fabricated on AlN templates for back illumination for enhanced performance through hole-initiated multiplication, and the effects of increased area on device performance were studied. Avalanche multiplication was observed in mesa sizes up to 14,063 µm^2 under linear mode operation. Uniform gain and a linear increase of the dark current with area were demonstrated. [reprint (PDF)]
 
2.  Quantum cascade laser: A tool for trace chemical detection
Allan J. Evans; Manijeh Razeghi
American Filtration and Separations Society - 20th Annual Conference and Exposition of the American Filtration and Separations Society 2:914-923 (2007)-- March 26, 2007
Laser-based trace chemical sensors are highly desired to enhance pollution filtering, health and safety monitoring, and filter efficiency monitoring for industrial processes. Limitations of current monitoring and sensing techniques are discussed and the benefits of mid-infrared spectroscopy using novel Quantum Cascade semiconductor Lasers (QCLs) are presented. These new techniques promise inexpensive, miniaturized sensors, capable of remote detection of trace chemicals in liquids, solids, and gasses with levels less than 1 part-per-billion. Applications of these techniques are discussed and the most recent developments of application-ready high power (> 100 mW), continuous-wave, mid-infrared QCLs operating above room temperature with lifetimes exceeding 12,000 hours are presented.
 
2.  High Power Quantum Cascade Lasers (QCLs) Grown by GasMBE
M. Razeghi and S. Slivken
SPIE Proceedings, International Conference on Solid State Crystals (ICSSC), Zakopane, Poland, -- October 14, 2002 ...[Visit Journal]
This paper is a brief summary of the technological development and state-of-the-art performance of quantum cascade lasers produced at the Centre for Quantum Devices. Laser design will be discussed, as well as experimental details of device fabrication. Recent work has focused on the development of high peak and average power QCLs emitting at room temperature and above. Scaling of the output is demonstrated by increasing the number of emitting regions in the waveguide core. At λ = 9 µm, over 7 W of peak power has been demonstrated at room temperature for a single diode, with an average power of 300 mW at 6% duty cycle. At shorter wavelengths, laser development includes the use of highly strain-balanced heterostructures in order to maintain a high conduction band offset and minimize leakage current. At λ = 6 µm, utilizing a high reflective coating and epilayer-down mounting of the laser, we have demonstrated 225 mW of average power from a single facet at room temperature. Lastly, these results are put in perspective of other reported results and possible future directions are discussed. [reprint (PDF)]
 
2.  LEO of III-Nitride on Al2O3 and Si Substrates
M. Razeghi, P. Kung, P. Sandvik, K. Mi, X. Zhang, V.P. Dravid, J. Freitas, and A. Saxler
SPIE Conference, San Jose, CA, -- January 26, 2000 ...[Visit Journal]
Lateral epitaxial overgrowth (LEO) has recently become the method of choice to reduce the density of dislocations in heteroepitaxial GaN thin films, and is thus expected to lead to enhanced performance devices. We present here the LEO growth and characterization of GaN films by low pressure metalorganic chemical vapor deposition. Various substrates were used, including basal plane sapphire and oriented Si substrates. The steps in the LEO growth technology will be briefly reviewed. The characterization results will be discussed in detail. The structural, electrical and optical properties of the films were assessed through scanning, atomic and transmission electron microscopy, x-ray diffraction, capacitance-voltage, deep level transient spectroscopy, photoluminescence, and scanning cathodoluminenscence measurements. Single-step and double- step LEO GaN was achieved on sapphire. Similarly high quality LEO grown GaN films were obtained on sapphire and silicon substrates. Clear and dramatic reduction in the density of defects are observed in LEO grown materials using the various characterization techniques mentioned previously. [reprint (PDF)]
 
2.  High quality AlN and GaN epilayers grown on (00*1) sapphire, (100) and (111) silicon substrates
P. Kung, A. Saxler, X. Zhang, D. Walker, T.C. Wang, I. Ferguson, and M. Razeghi
Applied Physics Letters 66 (22)-- May 29, 1995 ...[Visit Journal]
The growth of high quality AlN and GaN thin films on basal plane sapphire, (100), and (111) silicon substrates is reported using low pressure metalorganic chemical vapor deposition. X-ray rocking curve linewidths of about 100 and 30 arcsec were obtained for AlN and GaN on sapphire, respectively. Room‐temperature optical transmission and photoluminescence (of GaN) measurements confirmed the high quality of the films. The luminescence at 300 and 77 K of the GaN films grown on basal plane sapphire, (100), and (111) silicon was compared. [reprint (PDF)]
 
2.  Thermal Conductivity of InAs/GaSb Type II Superlattice
C. Zhou, B.M. Nguyen, M. Razeghi and M. Grayson
Journal of Electronic Materials, Vol. 41, No. 9, p. 2322-2325-- August 1, 2012 ...[Visit Journal]
The cross-plane thermal conductivity of a type II InAs/GaSb superlattice(T2SL) is measured from 13 K to 300 K using the 3x method. Thermal conductivity is reduced by up to two orders of magnitude relative to the GaSb bulk substrate. The low thermal conductivity of around 1 W/m K to 8 W/m K may serve as an advantage for thermoelectric applications at low temperatures, while presenting a challenge for T2SL interband cascade lasers and highpower photodiodes. We describe a power-law approximation to model nonlinearities in the thermal conductivity, resulting in increased or decreased peak temperature for negative or positive exponents, respectively. [reprint (PDF)]
 
2.  Surface leakage current reduction in long wavelength infrared type-II InAs/GaSb superlattice photodiodes
S. Bogdanov, B.M. Nguyen, A.M. Hoang, and M. Razeghi
Applied Physics Letters, Vol. 98, No. 18, p. 183501-1-- May 2, 2011 ...[Visit Journal]
Dielectric passivation of long wavelength infrared Type-II InAs/GaSb superlattice photodetectors with different active region doping profiles has been studied. SiO2 passivation was shown to be efficient as long as it was not put in direct contact with the highly doped superlattice. A hybrid graded doping profile combined with the shallow etch technique reduced the surface leakage current in SiO2 passivated devices by up to two orders of magnitude compared to the usual design. As a result, at 77 K the SiO(2) passivated devices with 10.5 μm cutoff wavelength exhibit an R0A of 120 Ω·cm², RmaxA of 6000 Ω·cm², and a dark current level of 3.5×10−5 A·cm−2 at −50 mV bias. [reprint (PDF)]
 
2.  Fabrication of nanostructured heterojunction LEDs using self-forming Moth-Eye Arrays of n-ZnO Nanocones Grown on p-Si (111) by PLD
D.J. Rogers; V.E. Sandana; F. Hosseini Teherani; M. Razeghi; H.-J. Drouhin
Proc. SPIE 7217, Zinc Oxide Materials and Devices IV, 721708 (February 17, 2009)-- February 17, 2009 ...[Visit Journal]
ZnO nanostructures were grown on Si (111) substrates using Pulsed Laser Deposition. The impact of growth temperature (Ts) and Ar pressure (PAr) on the morphology, crystal structure and photoluminescence was investigated. Various types of ZnO nanostructures were obtained. Self-forming arrays of vertically-aligned nanorods and nanocones with strong c-axis crystallographic orientation and good optical response were obtained at higher Ts. The nanocone, or "moth-eye" type structures were selected for LED development because of their graded effective refractive index, which could facilitate improved light extraction at the LED/air interface. Such moth-eye arrays were grown on p-type Si (111) substrates to form heteroj unction LEDs with the n-type ZnO nanocones acting as an active component of the device. These nanostructured LEDs gave rectifying I/V characteristics with a threshold voltage of about 6V and a blueish-white electroluminescence, which was clearly visible to the naked eye. [reprint (PDF)]
 
2.  Quantum Hall liquid-to-insulator transition in In1-xGaxAs/InP heterostructures
W. Pan, D. Shahar, D.C. Tsui, H.P. Wei, and M. Razeghi
Physical Review B 55 (23)-- June 15, 1997 ...[Visit Journal]
We report a temperature- and current-scaling study of the quantum Hall liquid-to-insulator transition in an In1-xGaxAs/InP heterostructure. When the magnetic field is at the critical field Bc, ρxx=0.86h/e². Furthermore, the transport near Bc scales as |B- Bc|T with κ=0.45±0.05, and as |B- Bc|I-b with b=0.23±0.05. The latter can be due to phonon emission in a dirty piezoelectric medium, or can be the consequence of critical behavior near Bc, within which z=1.0±0.1 and ν=2.1±0.3 are obtained from our data. [reprint (PDF)]
 
2.  Strain-Induced Metastable Phase Stabilization in Ga2O3 Thin Films
Yaobin Xu, Ji-hyeon Park, Zhenpeng Yao, Christopher Wolverton, Manijeh Razeghi, Jinsong Wu, and Vinayak P. Dravid
ACS Appl. Mater. Interfaces-- January 10, 2019 ...[Visit Journal]
It is well known that metastable and transient structures in bulk can be stabilized in thin films via epitaxial strain (heteroepitaxy) and appropriate growth conditions that are often far from equilibrium. However, the mechanism of heteroepitaxy, particularly how the nominally unstable or metastable phase gets stabilized, remains largely unclear. This is especially intriguing for thin film Ga2O3, where multiple crystal phases may exist under varied growth conditions with spatial and dimensional constraints. Herein, the development and distribution of epitaxial strain at the Ga2O3/Al2O3 film-substrate interfaces is revealed down to the atomic resolution along different orientations, with an aberration-corrected scanning transmission electron microscope (STEM). Just a few layers of metastable α-Ga2O3 structure were found to accommodate the misfit strain in direct contact with the substrate. Following an epitaxial α-Ga2O3 structure of about couple unit cells, several layers (4~5) of transient phase appear as the intermediate structure to release the misfit strain. Subsequent to this transient crystal phase, the nominally unstable κ-Ga2O3 phase is stabilized as the major thin film phase form. We show that the epitaxial strain is gracefully accommodated by rearrangement of the oxygen polyhedra. When the structure is under large compressive strain, Ga3+ ions occupy only the oxygen octahedral sites to form a dense structure. With gradual release of the compressive strain, more and more Ga3+ ions occupy the oxygen tetrahedral sites, leading to volumetric expansion and the phase transformation. The structure of the transition phase is identified by high resolution electron microscopy (HREM) observation, complemented by the density functional theory (DFT) calculations. This study provides insights from the atomic scale and their implications for the design of functional thin film materials using epitaxial engineering.
 

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