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In this report, we propose a novel technique for identifying and analyzing diverse nanoscale carbon allotropes using scanning electron micrographs. By precisely controlling the quenching rates of undercooled molten carbon through laser irradiation, we achieved the formation of microdiamonds, nanodiamonds, and Q-carbon films. However, standard laser irradiation without proper undercooling control leads to the formation of sparsely located diverse carbon polymorphs, hindering their discovery and classification through manual analyses. To address this challenge, we applied transfer-learning approaches using convolutional neural networks and computer vision techniques to achieve allotrope discovery even with sparse spatial presence. Our method achieved high accuracy rates of 92% for Q-carbon identification and 94% for distinguishing it from nanodiamonds. By leveraging scanning electron micrographs and precise undercooling control, our technique enables the efficient identification and characterization of nanoscale carbon structures. This research significantly contributes to the advancement of the field, providing automated tools for Q-materials and carbon polymorph identification. It opens up new opportunities for the further exploration of these materials in various applications. [ABSTRACT FROM AUTHOR]

Here, we aimed to achieve exposure of a nanodiamond layer to a high-energy excimer laser. The treatment was realized in high-vacuum conditions. The carbon, in the form of nanodiamonds (NDs), underwent high-temperature changes. The induced changes in carbon form were studied with Raman spectroscopy, X-ray photoelectron spectroscopy, and X-ray diffraction (XRD) and we searched for the Q-carbon phase in the prepared structure. Surface morphology changes were detected by atomic force microscopy (AFM) and scanning electron microscopy (SEM). NDs were exposed to different laser energy values, from 1600 to 3000 mJ cm−2. Using the AFM and SEM methods, we found that the NDs layer was disrupted with increasing beam energy, to create a fibrous structure resembling Q-carbon fibers. Layered micro-/nano-spheres, representing the role of diamonds, were created at the junction of the fibers. A Q-carbon structure (fibers) consisting of 80% sp3 hybridization was prepared by melting and quenching the nanodiamond film. Higher energy values of the laser beam (2000 and 3000 mJ cm−2), in addition to oxygen bonds, also induced carbide bonds characteristic of Q-carbon. Raman spectroscopy confirmed the presence of a diamond (sp3) phase and a low-intensity graphitic (G) peak occurring in the Q-carbon form samples. [ABSTRACT FROM AUTHOR]

We report formation of self-organized nanodiamond ring structures due to dynamical heterogeneity in super undercooled carbon, created by nanosecond laser melting of amorphous carbon layers. We envisage that diamond tetrahedra self-organize and lead to formation of string and ring structures on which nanodiamonds nucleate and grow. Denser ring structures are formed in Q-carbon due to higher undercooling and enhanced diamond nucleation. The average size is larger under heterogeneous nucleation compared to homogeneous nucleation due to lower critical size and free energy, allowing more time for growth. With nanosecond laser melting, growth velocities range 5–10 ms−1 and even higher for Q-carbon.

This work presents a theoretical study of the structural, optoelectronic, and magnetic properties of Q‑carbon, utilizing hybrid functionals within density functional theory (DFT) ab initio calculations. Moreover, experiments were conducted to measure structural parameters, dielectric functions, and magnetic properties, using various techniques. From the DFT simulations, structural, electronic, and optical properties have been simulated. The band gap energy was calculated using a hybrid approach, which combine HSE functional with different values of exact Hartree-Fock (HF) exchange (α). We propose a theoretical investigation of cubic and quasi-cubic forms of Q‑carbon. Our findings indicate that a non-cubic Q‑carbon cell is energetically more stable and possesses higher cell mass density and bulk modulus compared to a cubic cell. Calculations indicated that Q‑carbon exhibits semiconductor behavior; an indirect band gap of 3.10 eV and a direct band gap of about 3.4 eV was obtained for α = 0.44, in good agreement with experimental values. The density of states analysis allowed us to identify the p orbital of sp2 hybridized atoms as being prevalent on the top of the valence band and in the lowest energy conduction band states. Magnetic moment values of 0.37 μ B and 0.41 μ B was found in two sp2 bonded C atoms, in accordance with the experimental observation. Several optical properties were calculated. The theoretical findings are compatible with the experimental results shown here and available in the literature, with excellent agreement found between the calculated optical band gap and that obtained from absorption measurements. [Display omitted] • The study revealed 84 % sp3 carbon atoms, mass density of 3.14 g/cm3, bulk modulus of 306 GPa and mean bond length of 1.57 Å. • Ferromagnetic behavior is attributed to unpaired electrons resulted of the presence of sp2 and sp3 carbon atoms. • Q-carbon possess semiconductor behavior with indirect band gap of about 3.10 eV. • Hartree-Fock mixing parameter (α) of 0.44 best reproduces the experimental values for Q-carbon theoretical analysis. • Theoretical optical absorption of 3.60 eV is in excellent agreement with 3.70 eV obtained experimentally. [ABSTRACT FROM AUTHOR]

We describe the formation of highly uniform Quenched-carbon (Q-carbon) layers by plasma-enhanced chemical vapor deposition (PECVD) followed by low-energy Ar+ ion bombardment to achieve wafer-scale integration of Q-carbon films. After PECVD, 9 nm and 20 nm thick silicon-doped diamond-like carbon (Si-DLC) films showed complete conversion into Q-carbon using 250eV Ar+ ions via negative biasing. However, this conversion was only partial for 30 nm thick films. Detailed EELS, XPS, Raman, and EDS studies were carried out to confirm the formation of Q-carbon by this method. We discuss the mechanism of Q-carbon formation as a result of low-energy ion bombardment during PECVD of thin films. These ions during negative biasing are energetic enough to create Frenkel defects, which support the conversion of the three-fold coordinated sp2 carbon units in as-deposited carbon into sp3 bonded five-atom tetrahedron units in Q-carbon. This process enhances the atomic number density and fraction of sp3 bonded carbon. These diamond tetrahedra are randomly packed and provide easy nucleation sites for diamond. If the underlying substrate can provide an epitaxial template for diamond growth via domain matching epitaxy, then wafer-scale growth of diamond epitaxial films can be achieved for wafer-scale integration and next-generation novel device manufacturing from diamond-related materials. [Display omitted] • New method for the formation of uniform, wafer-scale silicon-doped Q-carbon (Si-Q-carbon). • Via low-energy ion bombardment, conversion of Si-DLC into Si-Q-carbon was performed. • Ion bombardment provided the energy for the formation of Frenkel pairs. • Frenkel pairs converted 3-fold coordinated sp2 carbon units Si-DLC into sp3 bonded 5-atom tetrahedron units in Si-Q-carbon. [ABSTRACT FROM AUTHOR]

The main aim of this study was to describe the treatment of carbon sheet with a high-energy excimer laser. The excimer modification changed the surface chemistry and morphology of carbon. The appearance of specific carbon forms and modifications have been detected due to exposure to laser beam fluencies up to 8 J cm−2. High fluence optics was used for dramatic changes in the carbon layer with the possibility of Q-carbon formation; a specific amorphous carbon phase was detected with Raman spectroscopy. The changes in morphology were determined with atomic force microscopy and confirmed with scanning electron microscopy, where the partial formation of the Q-carbon phase was detected. Energy dispersive spectroscopy (EDS) was applied for a detailed study of surface chemistry. The particular shift of functional groups induced on laser-treated areas was determined by X-ray photoelectron spectroscopy. For the first time, high-dose laser exposure successfully induced a specific amorphous carbon phase. [ABSTRACT FROM AUTHOR]

We have discovered that Q-carbon is extremely resistant to radiation damage under ion irradiations involving extreme atomic displacements and electronic excitations. Using 5 MeV Au + ions, the Q-carbon films on sapphire substrates were irradiated in the dose range 3.3–10 dpa (displacements-per-atom). After the ion irradiations, detailed studies on the atomic structure and bonding characteristics showed that atomic structure and bonding characteristics of amorphous Q-carbon remained essentially unchanged to 10 dpa of radiation damage, which is equivalent to over twenty years of neutron damage in a conventional reactor. There was an ion-beam mixed layer below the Q-carbon layer, whose thickness increased from 5 nm to 10 nm, as the dose increased from 3.3 to 10 dpa. This layer was found to be mostly amorphous with a mixture Al 2 O 3 and Al 4 C 3. This layer, formed as a result of enhanced forward scattering and ballistic ion beam mixing, exhibited composition consistent with detailed TRIM calculations. We also found that nanodiamonds (3 nm average size) embedded in Q-carbon grew to about 60 nm after 6.6 dpa and shrank to about 40 nm after 10 dpa. We discuss the mechanism for the growth and shrinkage of metastable phase of diamond under nonequilibrium ion irradiations. [Display omitted] [ABSTRACT FROM AUTHOR]

We present 1D, 2D and 3D structures of boron-doped Q-carbon with a higher superconducting transition temperature than the current value of 55 K in 25 at% B-doped amorphous Q-carbon. The higher transition temperature is predicted for 1D and 2D crystalline structures with increasing density of states near the Fermi level through dopant trapping in substitutional sites. We have synthesized 50at% B-doped Q-carbon where diamond tetrahedra are arranged randomly and packed with over 80% efficiency to generate an amorphous structure. Detailed EELS measurements show higher density of states near the Fermi level above 90 K and preliminary transport data show signature of Tc above 100 K.

We report formation of self-organized nanodiamond ring structures due to dynamical heterogeneity in super undercooled carbon, created by nanosecond laser melting of amorphous carbon layers. We envisage that diamond tetrahedra self-organize and lead to formation of string and ring structures on which nanodiamonds nucleate and grow. Denser ring structures are formed in Q-carbon due to higher undercooling and enhanced diamond nucleation. The average size is larger under heterogeneous nucleation compared to homogeneous nucleation due to lower critical size and free energy, allowing more time for growth. With nanosecond laser melting, growth velocities range 5–10 ms−1 and even higher for Q-carbon. Significant advancement in the creation of self-organized nanodiamond ring and string structures by laser processing at ambient pressure and temperature [ABSTRACT FROM AUTHOR]

This paper summarizes our research related to Q-carbon and Q-BN and direct conversion of carbon into diamond and h-BN into c-BN. Synthesis and processing of these materials are accomplished by nanosecond laser melting and subsequent quenching of amorphous carbon and nanocrystalline h-BN. Depending upon the degree of undercooling, molten carbon (or h-BN) can be converted into Q-carbon (or Q-BN) or diamond (or c-BN). The primary focus here is on the outstanding properties of these materials, including hardness greater than diamond, ferromagnetism, p- and n-type doping, NV nanodiamonds, high-temperature superconductivity in B-doped Q-carbon, enhanced field emission, superhard composite coatings, and future applications. IMPACT STATEMENT This research represents a fundamental breakthrough in the direct conversion of carbon into diamond at ambient temperatures and pressures in the air and their extraordinary properties.

We report on the synthesis of multifunctional microdiamonds by chemical vapor deposition (CVD) on 304 and 316 austenitic stainless steel (SS) substrates. The increase in wettability achieved by surface scratching and the structure of ultra-dense Q-carbon achieved high nucleation density and minimized strains in diamond films. Notably, these diamond films exhibit a high amount of twinning, leading to the formation of five-fold microdiamonds. The diamonds on scratched SS substrate and Q-carbon interlayer exhibit a full width at half maximum of 8.25 cm−1 and 11.5 cm−1, compared to 26 cm−1 on bare SS substrate. The diamond films grown on bare SS substrate exhibited cracking due to high tensile stress of 2.3 GPa, ascribed to thermal mismatch between SS and diamond. The electron backscattered diffraction investigations reveal iron inclusions in diamonds synthesized on bare SS substrates, which may create ferromagnetism in these diamonds. This route, compared to the ion beam implantation method using ferromagnetic ions, yields better samples. At 800 °C, 1012 Fe atoms/cm2s are transferred from the SS substrate into the diamonds. The dominant growth orientation for these CVD diamonds was determined to be <110> out of plane. These multifunctional microdiamonds are useful for biomedical, electronic, and tribological applications. Image 1 [ABSTRACT FROM AUTHOR]

The versatility of the arrangement of C atoms with the formation of different allotropes and phases has led to the discovery of several new structures with unique properties. Carbon nanomaterials are currently very attractive nanomaterials due to their unique physical, chemical, and biological properties. One of these is the development of superconductivity, for example, in graphite intercalated superconductors, single-walled carbon nanotubes, B-doped diamond, etc. Not only various forms of carbon materials but also carbon-related materials have aroused extraordinary theoretical and experimental interest. Hybrid carbon materials are good candidates for high current densities at low applied electric fields due to their negative electron affinity. The right combination of two different nanostructures, CNF or carbon nanotubes and nanoparticles, has led to some very interesting sensors with applications in electrochemical biosensors, biomolecules, and pharmaceutical compounds. Carbon materials have a number of unique properties. In order to increase their potential application and applicability in different industries and under different conditions, they are often combined with other types of material (most often polymers or metals). The resulting composite materials have significantly improved properties.

We report the spectroscopic demonstration of the shallow-level energy states in the recently discovered B-doped Q-carbon Bardeen-Cooper-Schrieffer (BCS) high-temperature superconductor. The Q-carbon is synthesized by ultrafast melting and quenching, allowing for high B-doping concentrations which increase the superconducting transition temperature (T c) to 36 K (compared to 4 K for B-doped diamond). The increase in T c is attributed to the increased density of energy states near the Fermi level in B-doped Q-carbon, which give rise to superconducting states via strong electron-phonon coupling below T c. These shallow-level energy states, however, are challenging to map due to limited spatial and energy resolution. Here, we use ultrahigh energy resolution monochromated electron energy-loss spectroscopy (EELS), to detect and visualize the newly formed shallow-level energy states (vibrational modes) near the Fermi level (ranging 30–100 meV) of the B-doped Q-carbon. With this study, we establish the significance of high-resolution EELS in understanding the superconducting behavior of BCS superconducting C-based materials, which demonstrate a phenomenal enhancement in the presence of shallow-level energy states. Image 1 [ABSTRACT FROM AUTHOR]

We present 1D, 2D and 3D structures of boron-doped Q-carbon with a higher superconducting transition temperature than the current value of 55 K in 25 at% B-doped amorphous Q-carbon. The higher transition temperature is predicted for 1D and 2D crystalline structures with increasing density of states near the Fermi level through dopant trapping in substitutional sites. We have synthesized 50at% B-doped Q-carbon where diamond tetrahedra are arranged randomly and packed with over 80% efficiency to generate an amorphous structure. Detailed EELS measurements show higher density of states near the Fermi level above 90 K and preliminary transport data show signature of Tc above 100 K. Novel 1D, 2D and 3D structures of boron-doped Q-carbon with higher Tc than current BCS record of 55K by increasing B-concentration and the density of states near the Fermi level. [ABSTRACT FROM AUTHOR]

• Q-carbon exhibits exciting functional properties and robust mechanical strength. • The surface of the Q-carbon can be functionalized by doping it with silicon. • Si-doped Q-carbon is hydrophilic and highly resistant to biofilm formation. • Q-carbon has potential applications in advanced biomedical devices. Q-carbon, an allotrope of carbon, exhibits exciting functional properties and robust mechanical strength. We propose that the surface of the Q-carbon can be functionalized by doping it with silicon to enhance its performance as a potential implant material. As such, a coating of silicon-doped Q-carbon (Si-Q-carbon) is shown to minimize the formation of biofilm, thus reducing the risk of microbial infection. We report the formation of Si-Q-carbon coatings of varied thicknesses (10nm and 20nm) through the plasma-enhanced chemical vapor deposition technique. The surface composition and the bonding characteristics of the thin films were evaluated by Raman spectroscopy, XPS, and EELS studies, which showed that the thinnest sample (10nm) has a high sp3 content of ∼85%. Furthermore, wettability and surface energy calculations were undertaken to investigate the surface characteristics of the coatings. The 10nm sample was found to be more hydrophilic with a water contact angle of 75.3° (± 0.6°). The antibacterial activity of Si-Q-carbon coatings was investigated using a Staphylococcus epidermidis agar plating technique, and the adhesion of bacteria was explained in terms of the surface properties of the thin films. We demonstrate that the Si-Q-carbon coating with the highest sp3 content is hydrophilic and showed a 57% reduction in adhered biofilm relative to a glass control. We envisage the potential application of Q-carbon in arthroplasty devices with enhanced mechanical strength and resistance to periprosthetic joint infections. [ABSTRACT FROM AUTHOR]

Q-carbon, a quenched form of carbon, is a recently discovered carbon structure that has tremendous properties, compatibility, and potential for use in device fabrication and other electronic and mechanical applications. However, the non-equilibrium nature of the synthesis process and a very small window of growth parameters have limited the formation of Q-carbon to only low thermal conductive substrates. This study aims to overcome these limitations through extensive tuning of the parameters of diamond-like-carbon (DLC), the base structure required for the formation of Q-carbon. The as-deposited DLC films demonstrate I D /I G ratios ranging from 0.12 to 1.67, which are obtained through the optimization of laser energy density, rep rate, and deposition temperature during pulsed laser deposition. Utilizing Simulation of Laser Interaction with Materials, pulsed laser annealing (PLA) was used to directly transform the DLC films into Q-carbon while varying the PLA energy density from 0.3 J/cm2 to 1.2 J/cm2. Findings of Q-carbon formation on sapphire using different DLC films assisted in the preparation of a roadmap for overcoming the substrate limitations for Q-carbon formation. Further, Q-carbon is formed on AlN substrates for the direct deposition of diamond films without the requirement of a non-carbon interfacial layer or nanodiamond seeding layer. The large-area and uniform diamond growth on Q-carbon shows well-faceted and five-fold twinned growth with a 70 % improvement in the residual compressive stress of diamond on AlN. Such a method of diamond deposition on AlN provides the opportunity to address the thermal management issues in wide- and ultra-wide bandgap high-power electronic devices. [Display omitted] • The sp2-sp3 carbon composition in the DLC films is entirely tunable using PLD. • Q-carbon is formed on sapphire using different DLC films by controlling laser fluence. • Low thermal conductive substrate limitation of Q-carbon formation has been overcome. • DLC precursor and PLA parameters are crucial for any Q-carbon formation. • Diamond is deposited on AlN using a Q-carbon interlayer for thermal management. [ABSTRACT FROM AUTHOR]

This article presents a study on preparing and characterising Q-carbon structures through ultrafast cooling of annealed amorphous carbon using a nanosecond KrF excimer laser. The experiments were conducted under high vacuum conditions. Different Q-carbon structures resembling fibers, clusters, microdots, and combinations of clusters with nanodots were successfully prepared by varying the beam energy density (ranging from 0.6 to 1.8 J cm−2) during the pulsed laser annealing process. The resulting changes in surface morphology were analysed using atomic force microscopy (AFM) and scanning electron microscopy (SEM). Additionally, the modified forms of carbon were investigated through energy-dispersive spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy. The findings reveal that increasing the beam energy density during the pulsed laser annealing process led to a corresponding increase in the percentage of sp3 hybridisation in the samples. The highest sp3 content, reaching 83 %, was observed in the sample with the highest energy value of 1.8 J cm−2, where the fastest undercooling occurred. In addition, we evaluated the antibacterial potential of the prepared sample (1.0 J) using two bacterial strains, one gram-positive of S. aureus and one gram-negative of E. coli. [Display omitted] [ABSTRACT FROM AUTHOR]

Abstract While hot-filament assisted chemical vapor deposition (HFCVD) is a well-established technique to synthesize diamond thin films using microdiamond seeds, the quality of grown diamond thin films is often compromised due to the presence of contaminants, i.e. graphitic entities and the eroded tungsten filament remnants, at the film-substrate interface. Here, we present a novel approach to form high-quality, contamination-free diamond thin films with HFCVD using Q-carbon precursor. The Q-carbon is a metastable phase which is formed by nanosecond laser melting of amorphous carbon and rapid quenching from the superundercooled state and consists of ∼75% sp3 and rest sp2 hybridized carbon. Using Q-carbon seeds in HFCVD, we demonstrate the growth of polycrystalline diamond film with a clean interface without any tungsten filament impurities. With large-area vibrational Raman mode analysis, we also observe a significant reduction in the presence of overall graphitic entities in the diamond film. With the realization of such a high-quality interface, we present a pathway to fabricate significantly improved diamond coatings and solid-state devices. Graphical abstract Image 1 [ABSTRACT FROM AUTHOR]

This paper summarizes our research related to Q-carbon and Q-BN and direct conversion of carbon into diamond and h-BN into c-BN. Synthesis and processing of these materials are accomplished by nanosecond laser melting and subsequent quenching of amorphous carbon and nanocrystalline h- BN. Depending upon the degree of undercooling, molten carbon (or h-BN) can be converted into Q-carbon (or Q-BN) or diamond (or c-BN). The primary focus here is on the outstanding properties of these materials, including hardness greater than diamond, ferromagnetism, p- and n-type doping,NV nanodiamonds, high-temperature superconductivity in B-doped Q-carbon, enhanced field emission, superhard composite coatings, and future applications. [ABSTRACT FROM AUTHOR]

We report field electron emission investigations in Q-carbon composite structures formed by pulsed laser annealing of amorphous carbon layers. Under the optimum fabrication conditions, a dense microstructured morphology of Q-carbon was obtained, which is important for local electric field enhancement in field-emission device applications. The turn-on field required to draw an emission current density of 1 μA/cm 2 is found to be 2.4 V/μm. The Q-carbon films show good electron emission stability as a function of time up to 4 h. The microstructure and morphology of the field emitting Q-carbon films was analyzed by a variety of techniques, including field emission scanning electron microscope, Raman spectroscopy, and atomic force microscopy. Our results show a very high emission current density value of ~30 μA/cm 2 at an applied electric field of 2.65 V/μm, which is hysteresis-free and stable. The generated emission current has been found to have low fluctuations (<4%) and shows no generation of defects during repeated emission measurements on the sample. Our findings thus hold a great promise for the development of Q-carbon films in applications ranging from field emitters and frictionless motors to heterostructures for novel micro and nano-electronic devices. [ABSTRACT FROM AUTHOR]

A newly discovered quenched form of carbon, widely known as Q-carbon, thin films are synthesized by the direct conversion of the amorphous carbon layer using the nanosecond pulsed laser annealing technique, and its corrosion-resistant properties, that is, potentiodynamic polarization (PDP) and electrochemical impedance spectroscopy technique, are investigated. The unique microstructure and the existence of defects (sp 2 content) in sp 3 -rich Q-carbon are highly desirable for efficient corrosion-resistant performance. The sp 3 percentage of the as-grown Q-carbon is measured to be ∼80.5% from the D and G peaks of the Raman and C-1S X-ray photoelectron spectrum. The anti-corrosion properties with inhibition durability of Q-carbon thin films are systematically investigated in various concentrations of Na 2 SO 4 solutions, and the corrosion potential, corrosion current, and corrosion rate of Q-carbon are determined to be -253 V, 30.1 × 10 -5 A/cm 2 , and 0.00528, respectively, for 1 M Na 2 SO 4 solution. Both series and contact resistance decrease from 5498.6 and 821.1 Ω to 698.8 and 124.3 Ω with an increase of Na 2 SO 4 concentration from 0.1 to 1 M, respectively. The small shift of PDP curves toward more negative potential, the shrinkage of the radius of semicircular arcs in the Nyquist plot ( Z″ vs Z' ), and negligible loss in corrosion resistance (∼78%) are observed for Q-carbon thin film at the immersion time up to 48 h. The unique sp 2 -sp 3 ratio, shorter bond length, compact atomic arrangement, and minimum porosity, along with the high adhesion strength, due to the ultrafast solid-liquid-solid growth route, of Q-carbon thin film on the substrate signify it as a better alternative compared to the existing corrosion-resistant materials.

The versatility of the arrangement of C atoms with the formation of different allotropes and phases has led to the discovery of several new structures with unique properties. Carbon nanomaterials are currently very attractive nanomaterials due to their unique physical, chemical, and biological properties. One of these is the development of superconductivity, for example, in graphite intercalated superconductors, single-walled carbon nanotubes, B-doped diamond, etc. Not only various forms of carbon materials but also carbon-related materials have aroused extraordinary theoretical and experimental interest. Hybrid carbon materials are good candidates for high current densities at low applied electric fields due to their negative electron affinity. The right combination of two different nanostructures, CNF or carbon nanotubes and nanoparticles, has led to some very interesting sensors with applications in electrochemical biosensors, biomolecules, and pharmaceutical compounds. Carbon materials have a number of unique properties. In order to increase their potential application and applicability in different industries and under different conditions, they are often combined with other types of material (most often polymers or metals). The resulting composite materials have significantly improved properties. [ABSTRACT FROM AUTHOR]

Q-carbon is a densely packed metastable phase of carbon formed by ultrafast quenching of carbon melt in a super-undercooled state. After quenching, diamond tetrahedra are randomly packed with >80% packing efficiency. This discovery has opened a pathway to fabricate various interesting heterostructures following the highly nonequilibrium route of nanosecond pulsed laser annealing. In the present work, we demonstrate the evolution of Q-carbon/α-carbon and Q-carbon/diamond heterostructures with atomically sharp interfaces, controlled via varying solidification rates of the undercooled C melt. This structure consists of ultrahard Q-carbon (∼80% sp 3 and rest sp 2 ) with an overlayer of soft α-carbon (∼40% sp 3 ) on the inert c-Al 2 O 3 substrate. Using high-resolution scanning transmission electron microscopy and Raman spectroscopy analysis, we present the formation of the highly dense Q-carbon/α-carbon bilayer structure with distinctly different atomic and electronic structures. The laser-solid interaction simulations coupled with atomistic ab initio modeling further confirm the conversion of C melt into Q-carbon by achieving maximum undercooling near the substrate and further into α-carbon with a decrease in regrowth velocity (<6 m/s) away from the substrate. We present details of the evolution of heterointerfaces formed from carbon melt for designing heterostructures far from equilibrium for various functional applications by using pulsed laser processing.