Applications In Optoelectronic Devices Research Articles

Theoretical insights into the structural and optoelectronic properties of the ternary cesium tetrafluoridobromate semiconductor CsBrF4

This work deals with the first theoretical study of structural, electronic, and optical properties of CsBrF4 ternary compound by using first-principle calculations. The calculated structural parameters and atomic positions are in accordance with the experimental ones declared in the literature. The obtained electronic properties signalize that this compound is a semiconductor material with a direct energy band gap. According to the investigated optical properties, the vast optical absorption range in the ultraviolet region indicates that CsBrF4 semiconductor could be useful for specific applications in ultraviolet optoelectronic devices; consequently, this theoretical study is the potential to support future experimental research.

Synthesis of Hybrid Tin-Based Perovskite Microcrystals for LED Applications.

Considerable focus on tin-based perovskites lies on substitution to leadhalide perovskites for the fabrication of eco-friendly optoelectronic devices.The major concern related to tin-based perovskite devices are mainly thestability and the efficiency. However, thinking on the final commercializationscope, other considerations such as precursor stability and cost are majorfactors to carry about. In this regard, this work presents a robust and facilesynthesis of 2D A2SnX4 (A = 4-fluorophenethylammonium(4-FPEA); X = I, Br, I/Br) and 3D FASnI3 perovskite microcrystals followinga developed synthesis strategy with low-cost starting materials. In thisdeveloped methodology, acetic acid is used as a solvent, which helps to protectfrom water by making a hydrophobic network over the perovskite surface, andhence provides sufficient ambient and long-term inert atmosphere stability ofthe microcrystals. Further, the microcrystals are recrystallized in thin filmsfor LED application, allowing the fabrication of orange, near-infrared and purered emitting LEDs. The two-step recrystallized devices show better performanceand stability in comparison to the reference devices made by using commercialprecursors. Importantly, the developed synthesis methodology is defined as ageneric method for the preparation of varieties of hybrid tin-based perovskitesmicrocrystals and application in optoelectronic devices.

Accelerated Discovery of Halide Perovskite Materials via Computational Methods: A Review

Halide perovskites have gained considerable attention in materials science due to their exceptional optoelectronic properties, including high absorption coefficients, excellent charge-carrier mobilities, and tunable band gaps, which make them highly promising for applications in photovoltaics, light-emitting diodes, synapses, and other optoelectronic devices. However, challenges such as long-term stability and lead toxicity hinder large-scale commercialization. Computational methods have become essential in this field, providing insights into material properties, enabling the efficient screening of large chemical spaces, and accelerating discovery processes through high-throughput screening and machine learning techniques. This review further discusses the role of computational tools in the accelerated discovery of high-performance halide perovskite materials, like the double perovskites A2BX6 and A2BB′X6, zero-dimensional perovskite A3B2X9, and novel halide perovskite ABX6. This review provides significant insights into how computational methods have accelerated the discovery of high-performance halide perovskite. Challenges and future perspectives are also presented to stimulate further research progress.

Covalent Bond Torsion-Enabled Unique Crystal-Phase Transformation of an Organic Semiconductor for Multicolor Light-Emitting Transistors.

High-mobility and color-tunable highly emissive organic semiconductors (OSCs) are highly promising for various optoelectronic device applications and novel structure-property relationship investigations. However, such OSCs have never been reported because of the great trade-off between mobility, emission color, and emission efficiency. Here, we report a novel strategy of molecular conformation-induced unique crystalline polymorphism to realize the high mobility and color-tunable high emission in a novel OSC, 2,7-di(anthracen-2-yl) naphthalene (2,7-DAN). Interestingly, 2,7-DAN has unique crystalline polymorphism, which has an almost identical packing motif but slightly different molecular conformation enabled by the small bond rotation angle variation between anthracene and naphthalene units. More remarkably, the subtle covalent bond rotation angle change leads to a big change in color emission (from blue to green) but does not significantly modify the mobility and emission efficiency. The carrier mobility of 2,7-DAN crystals can reach up to a reliable 17 cm2 V-1 s-1, which is rare for the reported high-mobility OSCs. Based on the unique phenomenon, high-performance light-emitting transistors with blue to green emission are simultaneously demonstrated in an OSC crystal. These results open a new way for designing emerging multifunctional organic semiconductors toward next-generation advanced molecular (atomic)-scale optoelectronics devices.

PbI2 Passivation of Three Dimensional PbS Quantum Dot Superlattices Toward Optoelectronic Metamaterials.

Lead chalcogenide colloidal quantum dots are one of the most promising materials to revolutionize the field of short-wavelength infrared optoelectronics due to their bandgap tunability and strong absorption. By self-assembling these quantum dots into ordered superlattices, mobilities approaching those of the bulk counterparts can be achieved while still retaining their original optical properties. The recent literature focused mostly on PbSe-based superlattices, but PbS quantum dots have several advantages, including higher stability. In this work, we demonstrate highly ordered 3D superlattices of PbS quantum dots with tunable thickness up to 200 nm and high coherent ordering, both in-plane and along the thickness. We show that we can successfully exchange the ligands throughout the film without compromising the ordering. The superlattices as the active material of an ion gel-gated field-effect transistor achieve electron mobilities up to 220 cm2 V-1 s-1. To further improve the device performance, we performed a postdeposition passivation with PbI2, which noticeably reduced the subthreshold swing making it reach the Boltzmann limit. We believe this is an important proof of concept showing that it is possible to overcome the problem of high trap densities in quantum dot superlattices enabling their application in optoelectronic devices.

Structural and optical properties of In-doped CdS nanostructures: A comprehensive study

This research offers a comprehensive exploration of the effects of In-doping on the characteristics of CdS nanopowders (NPs). The structural and morphological properties of In-doped CdS nanostructures were investigated, revealing significant changes induced by In-doping. X-ray diffraction (XRD) analysis verified the formation of CdS phase. Determination of crystallite size (D) demonstrated a decrease from 27.0 nm for undoped CdS to 23.0 nm for CdS doped with 12% In-doped. Field-emission scanning electron microscopy (FESEM) imaging showed grain-like structures with sizes of 20 – 35 nm, showing variations in particle size distribution with increasing In-dopant concentration. Photoluminescence (PL) analysis illustrated changes in PL intensity and emission peak wavelengths due to In-doping. PL intensity decreased after In-doping. Additionally, a blue-shift in emission peak wavelengths indicated changes in the bandgap energy of CdS induced by In-doping. UV-Vis spectroscopy assessed the optical properties, revealing shifts in absorption and transmission spectra du to In-doping. In-doping enhanced absorption within the 400 – 500 nm range while decreasing absorption within 600 – 1000 nm. Transmission spectra displayed increased transparency after In-doping, attributed to modifications in band structure and morphology. Reflectance spectra initially increased with In-dopant concentration within 400 – 500 nm, followed by a decrease, suggesting alterations in electronic and structural properties. Estimation of band gap energy (Eg) unveiled an increase in Eg for In-doped CdS nanostructures compared to undoped CdS, likely due to reduced crystallite size and the Burstein-Moss effect induced by In-dopant ions. Raman analysis revealed a shift in peak positions and changes in intensity after In-doping, with a decrease in the 2LO/LO ratio indicating a deterioration in crystalline quality after In-doping. Overall, this comprehensive investigation provides valuable insights into the structural, morphological, optical, and electrical properties of In-doped CdS nanostructures, pivotal for their promising applications in optoelectronic devices and photovoltaics.

Computational study to investigate effectiveness of titanium substitution in CaFeH3 perovskite-type hydride: An approach towards advanced hydrogen storage system

In recent years, there has been increased interest in hydrogen storage due to the numerous advantages hydrogen offers as an energy source. This study explores the structural, hydrogen storage, electronic, elastic, mechanical, and optical properties of Ca1-xTixFeH3 through DFT. After Ti substitution in the host material, structure phase transformation occurs: cubic → pseudo-cubic → cubic. Study compounds are thermodynamically stable and experimentally synthesizable according to the calculated negative formation energies. Gravimetric hydrogen storage capacities for different concentrations of Ti (x = 0, 0.11, 0.33, 0.55, 1) were calculated as 2.963, 2.938, 2.843, and 2.753 wt%, respectively. The investigation focuses on understanding the material's BS, Fermi level, and DOS, elucidating its metallic characteristics, and non-zero DOS at the Fermi level contributing to electrical and thermal conductivity. Elemental partial density of states reveals hybridization effects with Ti doping, affecting the valence band's atomic contributions. Using cubic symmetry, C11, C12, and C14 elastic constants were used to describe mechanical characteristics, and the Born criteria were met. Thus, mechanical stability was demonstrated for these compounds. Optical analyses exhibit changes concerning Ti concentrations and energy levels, including absorption spectra, conductivity, reflectivity, dielectric function, refractive index, energy loss function, and extinction coefficient. These findings shed light on the material's response to incident radiation and potential applications in hydrogen storage and optoelectronic devices.

Synthesis of multilayered h-BN film on the molten Ni–B and the influence of underneath W substrate

High-quality two-dimensional hexagonal boron nitride (h-BN) film with tens of layers has been used as a universal substrate and capping layer for the van der Waals devices. Various approaches have been carried out for the synthesis of multilayered h-BN. Among them, the metal flux method is reliable in yielding h-BN crystals with high crystalline quality. However, this time- and energy-demanding method hinders its scale application. Herein, inspired by the metal flux method, we reported the time-effective growth of high-quality multilayered h-BN film (ca. 20 nm) on a molten Ni–B layer wetting on W substrate with chemical vapor deposition method. The film exhibits an excellent stacking sequence and a full-width at half maximum of the Raman E2g peak narrow to 9.5 cm−1. Cross-sectional high-resolution transmission electron microscopy and in-situ x-ray diffraction spectroscopy were carried out to investigate the crystal structure evolution of Ni–B layer wetting on W substrate. It is found that the low surface tension caused by the spreading of Ni–B alloy on the W substrate and the presence of the Ni subsurface may be responsible for the formation of multilayered h-BN with excellent crystalline quality. Meanwhile, the W diffusion in Ni–B-based melt can hinder the formation of h-BN under certain growth conditions. The approach demonstrates the feasibility of large-scale growth of multilayered h-BN, paving the way to future applications in van der Waals electronic and optoelectronic devices.

Electronic and optical properties of As/Bi2Se3 van der Waals heterostructure: Ab initio insights

In this study, based on the first-principles calculations, we theoretically studied the electronic and optical properties of two dimensional (2D) As/Bi2Se3 van der Waals (vdW) heterostructure. The results show that all the materials exhibit semiconducting behavior with calculated band gaps of Eg = 1.71, 1.0, and 1.65 eV without spin-orbit coupling (SOC), for As monolayer, Bi2Se3 monolayer, and As/Bi2Se3 heterostructure respectively. Notably, the As/Bi2Se3 heterostructure demonstrates a type-II band alignment, facilitating the effective spatial separation of photogenerated carriers. This characteristic offers exciting opportunities for applications in efficient optoelectronic devices, photocatalysis, and solar energy conversion. The optical properties studies show that the heterostructure exhibits significant light absorption across the visible to ultraviolet light spectrum, making it a promising candidate for a wide array of optoelectronic devices.

Dependence of Ultrafast Electron Emission Characteristics of Graphene Cold Cathode on Femtosecond Photoexcitation Polarization Angle.

Ultrafast electron pulses, generated through femtosecond photoexcitation in nanocathode materials, introduce high-frequency characteristics and ultrahigh temporal-spatial resolution to vacuum micro-nano electronic devices. To advance the development of ultrafast electron sources sensitive to polarized light, we propose an ultrafast pulsed electron source based on a vertical few-layer graphene cold cathode. This source exhibits selective electron emission properties for varying polarization angles, with high switching ratios of 277 (at 0°) and 235 (at 90°). The electron emission of the graphene evolves from cosine to sine as the polarization angle increases from 0° to 90°. The variation of electron emission current with polarization angle is intrinsically related to light absorption, local field enhancement, and photothermal conversion efficiency. A physical mechanism model and semiempirical expression were presented to reveal the MPP and PTE mechanisms at different polarization angles. This tunable conversion between mechanisms indicates potential applications in tunable ultrafast optoelectronic devices.

Doctor Blade Casting of Thin Films Containing Different Concentrated Endemic Plant Extracts: Determination of Structure and Optical Properties

This study provides a thorough properties of the optical analysis of the thin films which produced from Astragalus tokatensis Fisch., Helichrysum noeanum Boiss. and Stachys huber-morathii R. Bhattacharjee extracts. Methanol extracts of plants were obtained via Soxhlet extractor. The highest extract yield (10.10%) was determined in H. noeanum. Doctor blade coating method is used to make thin film layer on glass substrate. The optical behavior of the deposited films is tested by means of he UV-vis-near IR absorbance and transmittance characterization. It is found that the maximum transmittance spectra reaches nearly to a value of 90 % for A. tokatensis sample. Significantly, all the samples display same optical absorbace spectra behavior. Energy band gaps of the films are presented based on Tauc relation and were found to be in the range between 3.68-3.81 eV. Besides, the analysis of functional groups available in the materials is broadly studied by Fourier transform infrared (FT-IR) spectroscopy. FT-IR measurement also confirms that all produced films have carbohydrate pattern. These findings demonstrate a cost-efficient approach for the production of thin films with plant extraction, and open a new perspective on the potential applications of optoelectronic devices.

DFT+U study of TlXBr3 (X = Sn, Ge) perovskites as next-generation materials for optoelectronics applications

The lead-free perovskite has gained increasing importance in optoelectronic device applications. In this study, we investigate the structural, electronic, optical, mechanical, thermodynamic, and thermoelectric properties of cubic phase TlSnBr3 and TlGeBr3 using the plane wave pseudopotential method based on density functional theory (DFT). To overcome constraints of the GGA-PBE technique, we implemented the LDA + U technique to solve on-site self-interaction errors. The Hubbard parameter 'U' was identified as a suitable solution for considering on-site self-interactions and calculating better electronic energy band gaps. The obtained lattice parameters are consistent with previous published results. Our findings indicate that both materials have a direct energy band gap, with values of 1.75 eV and 1.94 eV for TlSnBr3 and TlGeBr3, respectively. We also observe the existence of covalent and ionic bonding. The optical properties of these materials demonstrate high absorption coefficients and conductivity in the visible region. The mechanical properties are derived using the Voigt-Reuss-Hill approximation and suggest strong evidence of ductile behavior. Finally, the thermoelectric properties are evaluated by analyzing thermal to electrical conductivity, Seebeck coefficient, and Figure of merit criteria. Our comparative study of TlXBr3 (X = Sn, Ge) suggests that these compounds are promising candidate materials for photovoltaic and optoelectronic devices.

Photochromic luminescence of organic crystals arising from subtle molecular rearrangement

Photoluminescence (PL) colour-changing materials in response to photostimulus play an increasingly significant role in intelligent applications for their programmability. Nevertheless, current research mainly focuses on photochemical processes, with less attention to PL transformation through uniform aggregation mode adjustment. Here we show photochromic luminescence in organic crystals (e.g. dimethyl terephthalate) with PL varying from dark blue to purple, then to bright orange-red, and finally to red. This change is attributed to the emergence of clusters with red emission, which is barely achieved in single-benzene-based structures, thanks to the subtle molecular rearrangements prompted by light. Crucial to this process are the through-space electron interactions among molecules and moderate short contacts between ester groups. The irradiated crystals exhibit reversible PL transformation upon sufficient relaxation, showing promising applications in information storage and smart optoelectronic devices. This research contributes to the development of smart photochromic luminescent materials with significant PL colour transformations through molecular rearrangement.

Tunable Multicolor Emission and High Thermal Stability in Single‐Matrix Luminescent Crystals Based on Calcium Perovskites for Advanced Solid‐State Lighting Applications

AbstractThe development of environmentally friendly full‐inorganic luminescent materials with tunable emission properties and exceptional thermal stability is of paramount importance for applications in optoelectronic devices, solid‐state lighting, and anti‐counterfeiting technologies. In this study, a novel luminescent crystal based on calcium perovskites Cs2CaCl4·2H2O (CCCH) are explored using a hydrothermal method. Simultaneous co‐doping of CCCH with Sn2+ and Mn2+ yields the s‐p transition‐induced cyan light from Sn2+ and d‐d transition‐induced yellow light from Mn2+. It demonstrates effective energy transfer from self‐trapped exciton (STE) of matrix CCCH and s‐p transition of Sn2+ to Mn2+, synergizing composite white lights with tunable colors. Furthermore, the incorporation of Sn2+ into CCCH introduces a red shift from blue to cyan emission with a remarkable enhancement in luminescent intensity by a factor of 12 times. The crystal orbital Hamiltonian populations (─COHP) calculations revealed the crucial role of Mn2+ in lattice stability, as evidenced by the decomposition temperature exceeding 305 °C for CCCH:Sn2+,Mn2+ whereas 210 °C for undoped CCCH matrix. This research provides a comprehensive investigation of the luminescent properties of CCCH:Sn2+,Mn2+ crystal, holding significant promise for practical technological advancements in lighting and anti‐counterfeiting technologies.

Dynamic Dipole Moment of Luminescent Liquid Crystals Enabled Highly Efficient Active Waveguide Materials Design and Synthesis

AbstractOrganic optical waveguide materials have attracted considerable attention for their promising applications in photonic and optoelectronic devices. However, for most materials, excellent light‐loss properties at high temperature cannot be obtained due to many factors. Consequently, realizing efficient optical waveguide materials that perform well at elevated temperatures remains a significant challenge. In this study, relying on the luminescent properties and self‐assembly properties of luminescent liquid crystals (LLCs), successfully fabricated materials are present for highly efficient active optical waveguides. A systematically synthesized set of LLCs with different structures is named according to the substituent type and the position of the cyano group, namely α‐DECN, α‐DEEOCN, β‐DECN, and β‐DEEOCN. Notably, α‐DECN and β‐DECN reveal hexagonal columnar phase, while α‐DEEOCN and β‐DEEOCN exhibit smectic phase. Optical waveguide experiments have revealed that the obtained LLCs showed highly efficient optical waveguide behavior, where the lowest light loss reached 0.15 dB mm−1 at room temperature. Remarkably, these LLCs show even lower light loss at high temperatures, with the light loss reaching 0.11 dB mm−1 as the lowest point. Further experimental results indicate that this phenomenon is attributed to the change in the dipole moment of these molecules. This research forms a significant groundwork for advanced exploration in optical waveguide material.

Controlling structural, electronic and optical properties of cubic FASnI3 perovskites using biaxial strains in the presence of spin orbit coupling: A DFT analysis

There is a significant research focus on the utilization of organic-inorganic hybrid perovskite materials in the field of photovoltaics. The remarkable electronic and optical characteristics of organic-inorganic hybrid perovskites are prevalent in solar applications. In this study, the first-principles density functional theory (DFT) was used to investigate how strains affect the structural, electronic, and optical properties of the formamidinium tin tri-iodide (hereafter FASnI3) perovskite structure. The band structure analysis revealed that FASnI3 possesses semiconductor properties. A direct bandgap of 0.96 eV was found at the R-point for unstrained planar FASnI3 structure. The bandgap was reduced when compressive strains were applied. In contrast, the bandgap attained a higher value due to the increased tensile strains. Moreover, the optical properties, such as absorption coefficient, dielectric function and electron loss function, showed that FASnI3 structures have good photo-absorption ability. The dielectric constant exhibited a redshift in its peaks as the compressive strains were increased. However, the dielectric peaks exhibited a blueshift when subjected to the tensile strains. Additionally, for a deeper understanding of the band structure, the effect of spin-orbit coupling (SOC) was considered. The band gap of the FASnI3 perovskite structure was 0.75 eV when the SOC effect was considered. The strain is a crucial factor to consider for optimizing the performance of FASnI3 perovskite structure for their applications in optoelectronic devices.

Arylazopyrazole-modulated stable dual-mode phototransistors.

High-performance organic devices with dynamic and stable modulation are essential for building devices adaptable to the environment. However, the existing reported devices incorporating light-activated units exhibit either limited device stability or subpar optoelectronic properties. Here, we synthesize a new optically tunable polymer dielectric functionalized with photochromic arylazopyrazole units with a cis-isomer half-life of as long as 90 days. On this basis, stable dual-mode organic transistors that can be reversibly modulated are successfully fabricated. The trans-state devices exhibit high carrier mobility reaching 7.4 square centimeters per volt per second and excellent optical figures of merit, whereas the cis-state devices demonstrate stable but starkly different optoelectronic performance. Furthermore, optical image sensors are prepared with regulatable nonvolatile memories from 36 hours (cis state) to 108 hours (trans state). The achievement of dynamic light modulation shows remarkable prospects for the intelligent application of organic optoelectronic devices.

Ultranarrow Deep-Blue Luminescence of Perovskite Nanocrystals by A-Site Cation Control.

Metal-halide perovskite nanocrystals (NCs) are one of the most promising emitters for the application of display and nanolight sources. The full width at half-maximum (FWHM) of photoluminescence (PL) emission is essential for color purity, which however remains a difficulty to further reduce the FWHM of the perovskite NCs at room temperature. Here, we show the quasi-sphere perovskite NCs with narrow PL emission at a deep-blue wavelength of ∼430 nm; its PL FWHM reaches ∼11 nm at room temperature, owing to the monodispersion in size distribution as well as the symmetric quasi-sphere morphology of NCs releasing the fine structure splitting-induced inhomogeneous broadening. Through regulating A cations with respect to the ratio of FA (or MA)-to-Cs and Cs-to-Pb, the PL emission of the NCs could be tuned from ∼505 to ∼430 nm combined with varied morphologies from large cube to small quasi-sphere. Such spectroscopic and morphological discrepancies are supposed to be attributed to the different crystalline kinetics that is strongly dependent on the synthetic condition. To be specific, in the case of increasing FA (or MA)-to-Cs, the growth rate of CsPbBr3 and FAPbBr3 (or MAPbBr3) perovskites is determined by the reactivity of transient species, while in the case of decreasing the Cs-to-Pb ratio, the growth rate of perovskites is slowed down by the serious reduction of Cs+ in the precursor. This study provides an effective strategy to adjust the emission across from green to deep-blue color and promotes the perovskite NCs with a narrow FWHM, and tunable PL emission facilitates in application of optoelectronic devices.

Highly Stable Silver Nanowire Plasmonic Electrodes for Flexible Polymer Light-Emitting Devices.

Silver nanowire (AgNW) transparent electrodes are considered as a promising candidate for applications in flexible optoelectronic devices. However, it remains a great challenge to obtain flexible AgNW electrodes with excellent optoelectrical properties and mechanical flexibility. Here, highly stable Ag nanoparticle (AgNP)-enhanced plasmonic AgNW electrodes are demonstrated via the controllable in situ growth of AgNPs at the AgNW junctions and introduction of an l-histidine (l-His) wrapping layer. The flexible transparent electrodes of AgNW-AgNP/l-His possess a low sheet resistance (Rsh) of ∼17.5 Ω sq-1, a high transmittance of ∼92.5% (550 nm), and a robust mechanical stability (100,000 bending cycles). Benefiting from plasmon-coupling effects, flexible polymer light-emitting devices (FPLEDs) with AgNW-AgNP/l-His electrodes present a current efficiency (CE) of ∼14.8 cd A-1 and an external quantum efficiency (EQE) of ∼5.6%, constituting ∼80% and ∼75% increases compared to those of the reference devices with AgNW electrodes, respectively. Additionally, the laminated flexible transparent PLEDs (FT-PLEDs) are demonstrated by integrating polydimethylsiloxane/AgNW-AgNP anodes by a soft lamination process. The FT-PLEDs present a CE of ∼7.1 cd A-1 (cathode side: ∼3.9 cd A-1; anode side: ∼3.2 cd A-1) and an EQE of ∼2.7% (cathode side: ∼1.5%; anode side: ∼1.2%). Furthermore, the FPLEDs and FT-PLEDs exhibit robust mechanical durability, maintaining ∼89% and ∼86% of their initial luminance after 1000 bending cycles at a bending radius of 2 mm, respectively. This work opens up a new avenue for the development of high performance and stable flexible optoelectronic devices.

Insight into Interfacial Heat Transfer of β-Ga2O3/Diamond Heterostructures via the Machine Learning Potential.

β-Ga2O3 is an ultrawide-band gap semiconductor with excellent potential for high-power and ultraviolet optoelectronic device applications. Low thermal conductivity is one of the major obstacles to enable the full performance of β-Ga2O3-based devices. A promising solution for this problem is to integrate β-Ga2O3 with a diamond heat sink. However, the thermal properties of the β-Ga2O3/diamond heterostructures after the interfacial bonding have not been studied extensively, which are influenced by the crystal orientations and interfacial atoms for the β-Ga2O3 and diamond interfaces. In this work, molecular dynamics simulations based on machine learning potential have been adopted to investigate the crystal-orientation-dependent and interfacial-atom-dependent thermal boundary resistance (TBR) of the β-Ga2O3/diamond heterostructure after interfacial bonding. The differences in TBR at different interfaces are explained in detail through the explorations of thermal conductivity value, thermal conductivity spectra, vibration density of states, and interfacial structures. Based on the above explorations, a further understanding of the influence of different crystal orientations and interfacial atoms on the β-Ga2O3/diamond heterostructure was achieved. Finally, insightful optimization strategies have been proposed in the study, which could pave the way for better thermal design and management of β-Ga2O3/diamond heterostructures according to guidance in the selection of the crystal orientations and interfacial atoms of the β-Ga2O3 and diamond interfaces.