Diffraction Signatures Research Articles

Is a Bent Crystal Still a Single Crystal?

The mention of the word "crystal" invokes images of minerals, gems, and rocks, all of which are inevitably solid, hard, and durable entities with well-defined smooth faces and straight edges. With the discovery in the first half of the 20th century that many molecular crystals are soft and can be deformed in a similar way as rubber or plastic, this perception is changing, and both the concept and formal definition of what a crystal is may require reinterpretation. The seemingly naïve question posed in the title of this Minireview does not have a simple answer. Here, we discuss how the effects of the elastic and plastic deformation of molecular crystals on the diffraction signature give primary evidence of their degree of crystallinity. In most cases, the definition of a crystal holds for both elastically and plastically deformed crystals and, unless there is significant or complete physical separation of the crystal during the deformation, they can safely be considered (deformed) single crystals with a high concentration of defects.

The dynamic spectral signatures from lunar occultation: A simulation study

Lunar occultation, which occurs when the Moon crosses sight-lines to distant sources, has been studied extensively through apparent intensity pattern resulting from Fresnel diffraction, and has been successfully used to measure angular sizes of extragalactic sources. However, such observations till date have been mainly over narrow bandwidth, or averaged over the observing band, and the associated intensity pattern in time has rarely been examined in detail as a function of frequency over a wide band. Here, we revisit the phenomenon of lunar occultation with a view to study the associated intensity pattern as a function of both time and frequency. Through analytical and simulation approach, we examine the variation of intensity across the dynamic spectra, and look for chromatic signatures which could appear as discrete dispersed signal tracks, when the diffraction pattern is adequately smoothed by a finite source size. We particularly explore circumstances in which such diffraction pattern might closely follow the interstellar dispersion law followed by pulsars and transients, such as the Fast Radio Bursts (FRBs), which remain a mystery even after a decade of their discovery. In this paper, we describe details of this investigation, relevant to radio frequencies at which FRBs have been detected, and discuss our findings, along with their implications. We also show how a band-averaged light curve suffers from temporal smearing, and consequent reduction in contrast of intensity variation, with increasing bandwidth. We suggest a way to recover the underlying diffraction signature, as well as the sensitivity improvement commensurate with usage of large bandwidths.

Competition between Exceptionally Long‐Range Alkyl Sidechain Ordering and Backbone Ordering in Semiconducting Polymers and Its Impact on Electronic and Optoelectronic Properties

Intra- and intermolecular ordering greatly impact the electronic and optoelectronic properties of semiconducting polymers. Despite much prior efforts regarding molecular packing, the interrelationship between ordering of alkyl sidechains and conjugated backbones has not been fully detailed. We report here the discovery of a highly ordered alkyl sidechain phase in six representative semiconducting polymers, determined from distinct spectroscopic and diffraction signatures. The sidechain ordering exhibits unusually large coherence lengths of at least 70 nm, induces torsional/twisting backbone disorder, and results in a vertically layered multilayer nanostructure with ordered sidechain layers alternating with disordered backbone layers. Calorimetry and in-situ variable temperature scattering measurements in a model system PBnDT-FTAZ clearly delineate this competition of ordering that prevents the simultaneous long-range order of both moieties. The long-range sidechain ordering can be exploited as a transient state to fabricate PBnDT-FTAZ films with an atypical edge-on texture and 2.5x improved OFET mobility. The observed influence of ordering between the moieties implies that improved molecular design could produce synergistic rather than destructive ordering effects. Given the large sidechain coherence lengths observed, such synergistic ordering should greatly improve the coherence length of backbone ordering and thereby improve electronic and optoelectronic properties such as charge transport and exciton diffusion lengths.

Soil Development under Continuous Agriculture at the Morrow Plots Experimental Fields from X-ray Diffraction Profile Modelling

Impact of continuous cropping on clay mineralogy was assessed on a collection of unfertilized soil samples from the Morrow Plots experimental fields covering 110 years of long crop rotations. Evolution of mineralogy was quantitatively determined by fitting X-ray diffraction (XRD) patterns from four size fractions (50–2, 2–0.2, 0.2–0.05 and <0.05 µm) of the surface horizon (0–20 cm). The mineralogy of the three clay subfractions (2–0.2 µm, 0.2–0.05 µm and <0.05 µm) consists mainly of coexisting illite-smectite-chlorite whose compositions range from discrete illite (in the 2–0.2 µm subfraction) to discrete smectite (in the <0.05 µm subfraction). Mixed layers of similar compositions were used to fit XRD data from all clay subfractions. With decreasing size fractions, both the size of the coherent scattering domains and the proportion of illite-rich mixed layers decrease, thus accounting for the higher cation exchange measured in the <0.05 µm subfraction compared to other clay subfractions. The analysis of fine clay subfractions (<0.2 µm or lower) provided key information and constraints to a complete and accurate description of the bulk <2 µm fraction. Additional constraints derived from chemical treatments (K-saturation and heating) proved to be especially useful to propose a reliable structure model for these fine clay subfractions because of their weakly modulated diffraction signature. Mineralogy of all subfractions considered is essentially stable over the studied period (1904–2014), with the relative proportion of the different clay layer types (illite, smectite, kaolinite, chlorite) showing no significant evolution in the bulk <2 µm fraction. A century of continuous cropping thus results essentially in an increase of fine clay particles (<0.05 µm) and a decrease of the 0.2–0.05 µm subfraction, indicative of clay mineral dissolution and consistent with observed increase of cation exchange capacity with time. The relative proportion of the bulk <2 µm fraction is nearly constant over the studied period, indicative of minimal export of clay phases.

New Calcium Hydrides with Mixed Atomic and Molecular Hydrogen

Two new polyhydrides of calcium have been synthesized at high pressures and high temperatures and characterized by Raman spectroscopy, infrared spectroscopy, and synchrotron X-ray diffraction. Above 20 GPa and 700 K, we synthesize a phase having a monoclinic (C2/m) structure with Ca2H5 composition, which is characterized by a distinctive vibration at 3789 cm–1 at 25 GPa. The observed Raman spectrum is in close agreement with first-principles calculations of a Ca2H5 structure characterized by a lattice containing a central layer of H2 molecules oriented along the (100) direction. At higher pressures (e.g., 116 GPa and 1600 K), we synthesize another phase, which has the composition of CaH4 and a denser body-centered tetragonal structure. This weakly metallic phase also contains molecular-like H2 units, and its spectroscopic as well as diffraction signatures match closely with those predicted from first-principles calculations. This phase is observed to persist on decompression to 60 GPa at room temperature. The elongation of the H–H bond in these hydrides is a result of the Ca–H2 interaction, analogous to what occurs in molecular compounds, where H2 binds side-on to a d-element, such as in Kubas complex.

A novel method to remove the background from x-ray diffraction signal

The first step that is required to extract the correct information from a two-dimensional (2D) diffraction signature is to remove the background accurately. However, direct background subtraction inevitably overcorrects the signal as it does not take into account the attenuation by the sample. Other traditional background removal methods, such as the rolling ball technique, can separate sharp diffraction peaks of crystalline materials from their background. These methods are unsuitable for biological tissue, which is amorphous and does not have sharp diffraction peaks. This technical note proposes a novel method that combines peak fitting and experimental results to estimate the background for 2D XRD signals.

Cassini UVIS solar occultations by Saturn’s F ring and the detection of collision-produced micron-sized dust

We present an analysis of eleven solar occultations by Saturn’s F ring observed by the Ultraviolet Imaging Spectrograph (UVIS) on the Cassini spacecraft. In four of the solar occultations we detect an unambiguous signal from diffracted sunlight that adds to the direct solar signal just before or after the occultations occur. The strongest detection was a 10% increase over the direct signal that was enabled by the accidental misalignment of the instrument’s pointing. We compare the UVIS data with images of the F ring obtained by the Cassini Imaging Science Subsystem (ISS) and find that in each instance of an unambiguous diffraction signature in the UVIS data, the ISS data shows that there was a recent disturbance in that region of the F ring. Similarly, the ISS images show a quiescent region of the F ring for all solar occultations in which no diffraction signature was detected. We therefore conclude that collisions in the F ring produce a population of small ring particles that can produce a detectable diffraction signal immediately interior or exterior to the F ring. The clearest example of this connection comes from the strong detection of diffracted light in the 2007 solar occultation, when the portion of the F ring that occulted the Sun had suffered a large collisional event, likely with S/2004 S 6, several months prior. This collision was observed in a series of ISS images (Murray et al., 2008).Our spectral analysis of the data shows no significant spectral features in the F ring, indicating that the particles must be at least 0.2 µm in radius. We apply a forward model of the solar occultations, accounting for the effects of diffracted light and the attenuated direct solar signal, to model the observed solar occultation light curves. These models constrain the optical depth, radial width, and particle size distribution of the F ring. We find that when the diffraction signature is present, we can best reproduce the occultation data using a particle population with an average effective particle size of less than 300 µm, while occultations without clear diffraction signals are best modeled using a population with an effective particle size larger than 400 µm.

Correlation of X-ray diffraction signatures of breast tissue and their histopathological classification

This pilot study examines the correlation of X-ray diffraction (XRD) measurements with the histopathological analysis of breast tissue. Eight breast cancer samples were investigated. Each sample contained a mixture of normal and cancerous tissues. In total, 522 separate XRD measurements were made at different locations across the samples (8 in total). The resulting XRD spectra were subjected to principal component analysis (PCA) in order to determine if there were any distinguishing features that could be used to identify different tissue components. 99.0% of the variation between the spectra were described by the first two principal components (PC). Comparing the location of points in PC space with the classification determined by histopathology indicated correlation between the shape/magnitude of the XRD spectra and the tissue type. These results are encouraging and suggest that XRD could be used for the intraoperative or postoperative classification of bulk tissue samples.

Fourier-Based Diffraction Analysis of Live Caenorhabditis elegans.

This manuscript describes how to classify nematodes using temporal far-field diffraction signatures. A single C. elegans is suspended in a water column inside an optical cuvette. A 632 nm continuous wave HeNe laser is directed through the cuvette using front surface mirrors. A significant distance of at least 20-30 cm traveled after the light passes through the cuvette ensures a useful far-field (Fraunhofer) diffraction pattern. The diffraction pattern changes in real time as the nematode swims within the laser beam. The photodiode is placed off-center in the diffraction pattern. The voltage signal from the photodiode is observed in real time and recorded using a digital oscilloscope. This process is repeated for 139 wild type and 108 "roller" C. elegans. Wild type worms exhibit a rapid oscillation pattern in solution. The "roller" worms have a mutation in a key component of the cuticle that interferes with smooth locomotion. Time intervals that are not free of saturation and inactivity are discarded. It is practical to divide each average by its maximum to compare relative intensities. The signal for each worm is Fourier transformed so that the frequency pattern for each worm emerges. The signal for each type of worm is averaged. The averaged Fourier spectra for the wild type and the "roller" C. elegans are distinctly different and reveal that the dynamic worm shapes of the two different worm strains can be distinguished using Fourier analysis. The Fourier spectra of each worm strain match an approximate model using two different binary worm shapes that correspond to locomotory moments. The envelope of the averaged frequency distribution for actual and modeled worms confirms the model matches the data. This method can serve as a baseline for Fourier analysis for many microscopic species, as every microorganism will have its unique Fourier spectrum.

Fourier-Based Diffraction Analysis of Live <em>Caenorhabditis elegans</em>

This manuscript describes how to classify nematodes using temporal far-field diffraction signatures. A single C. elegans is suspended in a water column inside an optical cuvette. A 632 nm continuous wave HeNe laser is directed through the cuvette using front surface mirrors. A significant distance of at least 20-30 cm traveled after the light passes through the cuvette ensures a useful far-field (Fraunhofer) diffraction pattern. The diffraction pattern changes in real time as the nematode swims within the laser beam. The photodiode is placed off-center in the diffraction pattern. The voltage signal from the photodiode is observed in real time and recorded using a digital oscilloscope. This process is repeated for 139 wild type and 108 "roller" C. elegans. Wild type worms exhibit a rapid oscillation pattern in solution. The "roller" worms have a mutation in a key component of the cuticle that interferes with smooth locomotion. Time intervals that are not free of saturation and inactivity are discarded. It is practical to divide each average by its maximum to compare relative intensities. The signal for each worm is Fourier transformed so that the frequency pattern for each worm emerges. The signal for each type of worm is averaged. The averaged Fourier spectra for the wild type and the "roller" C. elegans are distinctly different and reveal that the dynamic worm shapes of the two different worm strains can be distinguished using Fourier analysis. The Fourier spectra of each worm strain match an approximate model using two different binary worm shapes that correspond to locomotory moments. The envelope of the averaged frequency distribution for actual and modeled worms confirms the model matches the data. This method can serve as a baseline for Fourier analysis for many microscopic species, as every microorganism will have its unique Fourier spectrum.

High-pressure melting behavior of tin up to 105 GPa

The melting curve of Sn initially rises steeply as a function of pressure but exhibits a decrease in slope ($d{T}_{m}/dP$) above 40 GPa to become nearly flat above 50 GPa. Previous studies have argued that a body-centered tetragonal (bct) to cubic (bcc) phase transition occurs in this range at room temperature. However, our investigations have shown that the phase behavior is more complex in this region with orthorhombic (bco) splitting of reflections occurring in the x-ray diffraction pattern above 32 GPa and coexisting diffraction signatures of bco and bcc structures are observed between 40 and 70 GPa. Here we have documented the simultaneous presence of bco and bcc reflections up to the melting point, negating the possibility that their coexistence might indicate a kinetically hindered first-order phase transformation. In this paper we have extended the observation of Sn melting relations into the megabar ($Pg100$ GPa) range using the appearance of liquid diffuse scattering in x-ray diffraction patterns and discontinuities during thermal signal processing to diagnose the occurrence of melting. Both techniques yield consistent results that indicate the melting line maintains the same low slope up to the highest pressure examined and does not flatten. The results below approximately 40 GPa agree well with the melting relations produced recently using a multiphase equation of state fitted to available or assumed data. Above this pressure the experimental melting points lie increasingly below the predicted crystal-liquid phase boundary, but above the flat melting from past studies, indicating that the thermodynamic properties of the body-centered ``$\ensuremath{\gamma}$''-Sn structure remain to be clarified.

On the issues of resolving a low melting combination as a definite eutectic or an elusive cocrystal: A critical evaluation

Cocrystals and eutectics are different yet related crystalline multi-component adducts with diverse applications in pharmaceutical and materials fields. Recently, they were shown to be alternate products of cocrystallization experiments. Whereas a cocrystal shows distinct diffraction, spectroscopic and thermal signatures as compared to parent components, the hallmark of a eutectic is its low melting nature. However, in certain cases, there can be a problem when one resorts to design a cocrystal and assess its formation vis-à-vis a eutectic. In the absence of a gold standard method to make a cocrystal, it is often difficult to judge how exhaustive should the cocrystallization trials be to ensure the accomplishment of a desired/putative cocrystal. Further, a cocrystal can manifest with intermolecular interactions and/or crystal structure similar to that of its parent compounds such that the conventional diffraction and spectroscopic techniques will be of little help to conclusively infer the formation of cocrystal in the lack of single crystals. Such situations combined with low melting behavior of a combination brings the complication of resolving the combination as a cocrystal or eutectic since now both the adducts share common features. Based on the curious case of Caffeine–Benzoic acid combination, this study aims to unfold the intricate issues related to the design, formation and characterization of cocrystals and eutectics for a way forward. The utility of heteronuclear seeding methodology in establishing a given combination as a cocrystal-forming one or a eutectic-forming one in four known systems is appraised. The notion of mutual exclusivity of cocrystal and eutectic from cocrystallization and issues related to their structural organization and manifestation are discussed. The potential of hetero seeding in facilitating the formation of a putative cocrystal and thus establishing a given combination as a cocrystal-forming one or a eutectic-forming one is appraised.

Linewidth Reconstruction Employing a Radial Basis Function Network in Optical Scatterometry

This paper applied a radial basis function network (RBFN) in coherent Fourier scatterometry (CFS) to reconstruct the linewidth of periodic line/space (L/S) patterns. The fast, nondestructive, and repeatable measurement capability of CFS enables its integration with intelligent lithography systems. Two steps to reconstruct the linewidth of the L/S patterns were performed in this paper. The first step was to use the finite difference time domain numerical electromagnetic tool to rigorously establish the library of modeled diffraction signatures by using the L/S patterns. Each modeled signature was converted to an intensity vector as the training data to construct the RBFN. The trained RBFN has a simple architecture consisting of three layers: input, hidden, and output layers. The second step was to collect the experimental signatures and feed them into the trained RBFN model to predict the linewidth of L/S patterns. This paper used the transverse electric polarized incident beam at the wavelength of 632 nm in the experimental setup of the CFS. Five L/S patterns were used to test the constructed RBFN. The experimental results indicated that the maximal difference was 13 nm between the CFS and the atomic force microscopy (AFM) measurements for the sample D with an L/S of 200 nm. The minimum difference was 2 nm for the sample A with an L/S of 140 nm. The correlation coefficient between the CFS and AFM metrology measurement running through five samples was 0.972. The high correlation between the CFS with the proposed RBFN measurements and the AFM revealed the potential to implement the radial basis learning kernel in optical metrology to achieve intelligent lithography.

LOW COST MICROSCOPY FOR THREE DIMENSIONAL IMAGING USING DIGITAL INLINE HOLOGRAPHIC PRINCIPLE

Optical microscopy is reached a new level in terms of resolution, 3 - D imaging capability, flexibility of imaging different samples which increase imaging complexity and the cost.. Though established labs can afford high - end microscopes, it remains a concern in rural areas where clinics and patients cannot afford much. Semi - portable microscopy based on inline holographic setup is demonstrated where depth information as 3rd dimension can also be accessed. This setup contains only light emitting diode (LED), pinhole and charge coup led device (CCD) camera. Since laser source gives rise to speckle noise and it is also cost constraint for developing a low cost microscopy, thus it is replaced with incoherent LED source. This setup is also known as ‘lensless holography’ because there is no use of lens for imaging. In conventional inline holographic setup the sample is placed closed to the pinhole which will restrict field of view (FOV) and diffraction signature of one particle (cell) will overlap w ith other. To avoid overlap of diffractio n signatures and to increase FOV sample was placed close to CCD sensor. To test the working of microscopy agarose microbeads were used. Optimization algorithm is used for reconstruction of object field from recorded hologram.. Thus both amplitude as well a s the phase images of the microbeads is reconstructed. Instead of using microscopic objective to focus sample, autofocus algorithm is used to calculate the focused plane

Diffraction signatures of fracture intersections

Fractured rock causes diffractions, which are often discarded as noise in ground-penetrating radar (GPR) and seismic data. Most fractures are too thin, too steep, and their displacement is too small to be imaged by reflections, and diffractions are the only detectable signal. To decipher the information about fracture geometry and distribution contained in diffractions, we compare 3D synthetic ray-Born modeling with high-density 3D GPR data and outcrop observations from the Cassis Quarry in Southern France. Our results reveal how the intersection between two fractures is the basic geologic element producing a recordable diffraction. In this new model, two intersecting fractures are represented by one finite-length line diffractor. The intersection of three fractures is a 3D cross composed of three line diffractors. Fractures extending over several meters in the outcrop display linear clusters of diffraction circles in unmigrated GPR time slices. Such large-scale fracture intersections are composed of many aligned short subwavelength line diffractors due to fracture roughness and variations of fracture opening. The shape irregularities and amplitude variations of composite diffraction signatures are a consequence of the geometry and spacing of the intersecting fractures generating them. With three simple base-type intersecting fracture models (horizontal dip, gentle dip, and steep dip), the fracture network geometry can be directly deciphered from the composite diffraction signatures visible on unmigrated time slices. The nonrandom distribution of diffractions is caused by fracture trends and patterns providing information about fracture dip, spacing, and continuity of fractured domains. With the similarity law, the diffraction phenomena observed in GPR data are very similar in character to those seen on the seismic scale with the wavelength as the scaling link. GPR data serve as a proxy to decipher seismic diffractions.

The chemical instability of Na2IrO3 in air

We report that Na2IrO3, which has a layered honeycomb iridium oxide sublattice interleaved by Na planes, decomposes in laboratory air while maintaining the same basic crystal structure. The decomposition reaction was monitored by time-dependent powder X-ray diffraction under different ambient atmospheres, through which it was determined that it occurs only in the simultaneous presence of both CO2 and H2O. A hydrated sodium carbonate is the primary decomposition product along with altered Na2IrO3. The diffraction signature of the altered Na2IrO3 is quite similar to that of the pristine material, which makes the detection of decomposition difficult in a sample handled under ordinary laboratory conditions. The decomposed samples show a significantly decreased magnetic susceptibility and the disappearance of the low temperature antiferromagnetic transition considered to be characteristic of the phase. Samples that have never been exposed to air after synthesis display a previously unreported magnetic transition at 5K.

Differentiating veatchite polytypes using X-ray powder diffraction

Veatchite polytypes were properly identified from several localities relying solely on micro powder diffraction data. Diagnostic differences in their respective calculated patterns gave reliable identification results when compared with measured data. This permitted the confirmation of co-existing veatchite-1A and -2M on the same specimen from the Billie Mine, Inyo County, California as flat elongated crystals (-1A) and flat rhombic plates (-2M), respectively. On the specimen from the Sterling Borax Mine (Lang), type-locality for veatchite-2M, the polytype veatchite-1A was confirmed from radiating rhombic plates. From the type specimen for veatchite-1A (rhombic plates), collected from the borate deposit in Emet, Turkey, an additional unknown polytype of this mineral was discovered, but lacks suitable material for a complete characterization. At the Penobsquis deposit near Sussex in New Brunswick, Canada, only veatchite-2M was encountered. The area between 20 and 25°2θ holds the following diffraction signatures: -1A (two sets of double peaks at approximately 21.5 and 24.5°2θ), -1M (single peaks at 20 and 23°2θ) and -2M (double peaks at 20 and 23°2θ). The unknown polytype from Emet, Turkey differs from polytype-1A in that same range by having single peaks at the 21.5 and 24.5° instead of double peaks.

Laser-induced orbital projection and diffraction of O-2 with velocity map imaging

In a velocity map imaging spectrometer, we measured the electron momentum distributions from the ionization of O molecules with 800 nm wavelength, 40 fs laser pulses at a peak intensity of W cm. The molecules were aligned at 0, 45 and 90 relative to the laser polarization prior to ionization. We show that for all alignments the low momentum region – populated by direct electrons which do not recollide with the parent ion – is consistent with the ionized orbital being filtered and projected onto the continuum electron wave packet. In the high momentum region – populated by rescattered electrons – we observe that the pattern created by diffraction of the recolliding wave packet by the ion core disappears as the alignment gets closer to the laser field axis. We find that a two-slit diffraction model agrees well with the results for molecules aligned at 90, but only partially predicts the decrease in the diffraction signature for smaller alignment angles.

High-pressure structural transformations of Sn up to 138 GPa: Angle-dispersive synchrotron x-ray diffraction study

The high-pressure behavior of elemental Sn has been studied by angle-dispersive synchrotron x-ray diffraction up to 138 GPa under quasihydrostatic conditions at room temperature. The data confirm the occurrence of a first-order phase transition at 10.8 GPa between $\ensuremath{\beta}$-Sn (Sn-II) ($I{4}_{1}/amd$) and a further body-centered-tetragonal polymorph ($\ensuremath{\gamma}$-Sn or Sn-III) ($I4/mmm$). Above 32 GPa, this phase exhibits a distortion into a new body-centered-orthorhombic (bco) modification ($Immm$). Beyond 70 GPa, the structure becomes body-centered cubic (bcc) ($Im\ensuremath{-}3m$). There is a region of coexistence where the bcc reflections are observed to appear superimposed on the bco pattern above 40 GPa and the two diffraction signatures coexist until 70 GPa. We examined this possible existence of a kinetically hindered first-order phase transition between the two polymorphs by performing density functional theory (DFT) calculations with an emphasis on the potential energy in response to axial ($c/a,b/a$) distortions at constant volume. The DFT results suggest a slightly different interpretation of the structural transformations. At low pressure, the global minimum energy is always centered around $b/a=1$, and there is no indication of transformation to a bco structure. However, any small strains in the $c/a$ ratio in the system would provide an orthorhombic distortion of the observed magnitude. Such strains could be induced due to slight deviations from hydrostatic conditions in the experimental study. Concerning the possible bco-bcc phase transitions, the DFT calculations reveal an energy surface with a barrier developed between solutions with different $c/a$ values over the pressure range of interest. Crucially, the calculated barrier heights are low, and they disappear in the region of the observed phase transformation. The DFT results indicate a mechanically softened material that may exhibit localized domain structures in response to even slightly nonhydrostatic stress conditions.

Optimization of low temperature GaN buffer layers for halide vapor phase epitaxy growth of bulk GaN

We have studied growth and self-separation of bulk GaN on c-oriented Al2O3 using low temperature (LT) GaN buffer layers. By studying the X-ray diffraction (XRD) signature for the asymmetric and symmetric reflections versus the LT-GaN thickness and V/III precursor ratio, we observe that the peak width of the reflections is minimized using a LT buffer thickness of ∼100–300nm. It was observed that the V/III precursor ratio has a strong influence on the morphology. In order to obtain a smooth morphology, the V/III precursor ratio has to be more than 17 during the growth of the buffer layer. By using an optimized LT buffer layer for growth of a 20μm thick GaN layer, we obtain a XRD peak with a full width at half maximum of ∼400 and ∼250arcs for (002) and (105) reflection planes, respectively, and with a dark pit density of ∼2.2×108cm−2. For layers thicker than 1mm, the GaN was spontaneously separated and by utilizing this process, thick free freestanding 2″ GaN substrates were manufactured.