Optoelectronic Applications Research Articles

Orientation-Dependent Photoconductivity of Quasi-2D Nanocrystal Self-Assemblies: Face-Down, Edge-Up Versus Randomly Oriented Quantum Wells.

Here, strongly orientation-dependent lateral photoconductivity of a CdSe monolayer colloidal quantum wells (CQWs) possessing short-chain ligands is reported. A controlled liquid-air self-assembly technique is utilized to deliberately engineer the alignments of CQWs into either face-down (FO) or edge-up (EO) orientation on the substrate as opposed to randomly oriented (RO) CQWs prepared by spin-coating. Adapting planar configuration metal-semiconductor-metal (MSM) photodetectors, it is found that lateral conductivity spans ≈2 orders of magnitude depending on the orientation of CQWs in the film in the case of utilizing short ligands. The long native ligands of oleic acid (OA) are exchanged with short-chain ligands of 2-ethylhexane-1-thiol (EHT) to reduce the inter-platelet distance, which significantly improved the photoresponsivity from 4.16, 0.58, and 4.79 mA W-1 to 528.7, 6.17, and 94.2mAW-1, for the MSM devices prepared with RO, FO, and EO, before and after ligands exchange, respectively. Such CQW orientation control profoundly impacts the photodetector performance also in terms of the detection speed (0.061 s/0.074 s for the FO, 0.048 s/0.060 s for the EO compared to 0.10 s/0.16 s for the RO, for the rise and decay time constants, respectively) and the detectivity (1.7×1010, 2.3×1011, and 7.5×1011 Jones for the FO, EO, and RO devices, respectively) which can be further tailored for the desired optoelectronic device applications. Attributed to charge transportation in colloidal films being proportional to the number of hopping steps, these findings indicate that the solution-processed orientation of CQWs provides the ability to tune the photoconductivity of CQWs with short ligands as another degree of freedom to exploit and engineer their absorptive devices.

Influence of Pressure on Structural, Electronic, Optical, and Elastic Properties of Lead-Free Chalcogen Perovskite LaLuS3 via First-Principles Calculations: Implications for Optoelectronic Applications

Abstract Chalcogen perovskites have garnered increasing attention as promising materials for optoelectronic applications. In this study, we employed the first-principles method to investigate the structural, electronic, optical, and elastic properties of LaLuS3 under hydrostatic pressure at various levels. Through a thorough analysis of the calculated electronic structures, we observed that LaLuS3 exhibits direct band gaps, with the magnitudes of these gaps changing as the pressure varied. Specifically, the band gaps decrease by 2.19 eV, 2.025 eV, 1.365 eV, and 0.6043 eV at hydrostatic pressures of 0%, 10%, 20%, and 30% GPa, respectively. Furthermore, we observed shifts in the conduction band minimum and valence band maximum positions, indicating the potential of LaLuS3 for perovskite-based devices. This suggests that external pressure can serve as a powerful tool for designing new functional materials with intriguing properties. Our investigation also revealed promising optical properties of LaLuS3 under high pressures, further affirming its potential for optoelectronic and solar cell applications. The optical functions of the material are enhanced with increasing pressure, particularly in the ultraviolet range, highlighting its suitability for a wide range of optoelectronic devices. Moreover, while maintaining mechanical stability, hydrostatic pressure exerts a significant influence on the mechanical properties of LaLuS3. Lastly, our calculations on anisotropy demonstrate that applied pressure can enhance the anisotropic nature of LaLuS3. This comprehensive study underscores the efficacy of hydrostatic pressure as a systematic approach to modifying the photovoltaic performance of halide perovskites.

Computational and experimental investigations on structural, electronic and optical properties of scheelite compounds

Abstract Oxide of tungstate has consistently been pursued for use in optoelectronic applications. This study details the synthesis of AWO4 (A=Ba, Sr and Ca) using a high-temperature solid-state method. Additionally, theoretical calculations highlight its electronic structure, density of states, photoelectric properties, and vibrational modes. The X-ray diffraction of AWO4 (A=Ba, Sr and Ca) was meticulously introduced by the utilization of Rietveld for refinement. The refined lattice parameters substantially verified AWO4 (A=Ba, Sr and Ca) as a tetragonal system of scheelite with the spatial group of I41/a, and demonstrated significant alteration with the discrepancy in the radius of alkaline earth metal (A-site) ions. The electronic configuration and optical attributes of AWO4 (A=Ba, Sr and Ca) possessing scheelite-like structure were explored using density functional theory (DFT) based computational techniques. The theoretical blueprint was derived by optimizing the structure based on defects. The postulated optical bandgap energy confirms the occurrence of direct electronic transitions at Brillouin region G points. Calculations suggested the direct band gaps of BaWO4, SrWO4, and CaWO4 at 4.385, 3.123 and 3.813 eV. This was attributed to the energy levels produced by O and A-site atoms in the valence band, and W and O atoms in the conduction band. An examination of the polarization effect and uneven electronic charge distribution between [CaO8]6- and [WO4]2- clusters brought about by structural defects in AWO4 (A=Ba, Sr and Ca) was performed. Moreover, advanced investigations have been conducted on the elastic constants and mechanical durability of AWO4 (A=Ba, Sr and Ca). This research extensively calculated the elastic moduli of various matrices utilizing DFT. The critical Pugh's ratio value was found to be>1.75, it indicated that AWO4 (A=Ba, Sr and Ca) has significant potential as a resilient material.

Defect Engineering and Emission Tuning of Wide-Bandgap MAPbCl3 Perovskite.

Lead-chloride perovskites are promising candidates for optoelectronic applications, such as visible-blind UV photodetection. It remains unclear how the deep defects in this wide-bandgap material impact the carrier recombination dynamics. In this work, we study the defect properties of MAPbCl3 (MA = CH3NH3) based on photoluminescence (PL) measurements. Our investigations show that apart from the intrinsic emission, four sub-bandgap emissions emerge, which are very likely to originate from the radiative recombination of excitons bound to several intrinsic vacancy and interstitial defects. The intensity of various emission features can be tuned by adjusting the type and ratio of precursors used during synthesis. Our study not only provides important insights into the defect property and carrier recombination mechanism in this class of material but also demonstrates efficient strategies for defect passivation and engineering, paving the way for further development of lead-chloride perovskite-based optoelectronic devices.

Tuning optical properties of palgraphyne under biaxial mechanical strain: A density functional theory investigation

Palgraphyne is a two-dimensional material of carbon atoms with sp2 and sp hybridization. The influence of the biaxial mechanical strain on its optical properties is studied based on density functional theory calculations. It is observed that palgraphyne exhibits anisotropic behavior for photons with parallel and perpendicular polarizations. The dielectric constant of palgraphyne is higher than graphene. It has been found that biaxial tensile and compressive strains lead to an increase and decrease in the dielectric constant, respectively. The absorption spectra of palgraphyne sheet across the infrared to ultraviolet regions suggest that it has the potential to be a valuable material for utilization as absorber. Additionally, the reflection and transmission constants indicate that the sheet displays high transparency specially in the ultraviolet region. The peaks of optical quantities including dielectric constant, absorption coefficient, optical coefficient, reflection and transmission constants are moved to lower and higher energies under tensile and compressive strains, respectively. The anticipated results could make palgraphyne a candidate for optoelectronic applications.

Theoretically designed M@diaza[2.2.2]cryptand complexes: the role of non-covalent interactions in promoting NLO properties of organic electrides

ABSTRACT Organic excess electron compounds with significant nonlinear optical (NLO) properties are widely employed in optoelectronic applications. Herein, single-alkali metals with diaza[2.2.2] cryptand (M@crypt,M=Li, Na, and K) are investigated for optoelectronic and NLO properties by using the density functional theory. Thermodynamic and kinetic stabilities of present complexes are computed through interaction energy (Eint) and ab-initio molecular dynamic (AIMD) simulations. M@crypt complexes carry excess electrons and mimic molecular electrides. Quantum theory of atoms in molecules (QTAIM) analysis and reduced density gradient (RDG) spectra demonstrate the roles of the weak van der Waals (vdW) interactions between metal and complexant. The remarkable hyperpolarizability (βo) value up to 1.41 × 106 au may be credited to the presence of loosely bound excess electrons. The hyper Rayleigh scattering hyperpolarizability (βHRS) is recorded up to 1.31 × 106 au for the K@crypt. Furthermore, frequency-dependent first-order and second-order hyperpolarizability is more prominent at the applied frequency of ω = 0.042823 au. The electron localizing function (ELF) and localized orbital locator (LOL) analysis further disclose the nature of interaction between alkali metal and complexant. The TD-DFT method is adopted to get excited state parameters and absorbance properties. An electron density difference map (EDDM) is exploited to evaluate the orbital contributions in excited states. Hence, the studied electride may become a promising candidate for NLO materials. We anticipate that the present work will provide insight into further development of molecular electride for optoelectronic applications.

Twin Irida Graphene: A Carbon Material with Optoelectronic Features

AbstractA novel allotrope structure of carbon named twin irida graphene composed of 3‐16‐8 carbon rings is proposed. Its structural, mechanical, electronic, and optical characteristics are explored by density functional theory. It is shown that twin irida graphene has an energetically favorable structure. Its dynamical and thermal stabilities at room temperature are also examined and confirmed. The in‐plane stiffness of twin irida graphene is less than graphene. It is a metal and maintains this property even against the external strain and applied electric field. This sheet exhibits an anisotropy response to the incident photon with different polarizations. The potential of sheet for use in energy storage and absorption systems is indicated by its high dielectric constant and optical absorption. The reflection constants as well as the transmission constants of twin irida graphene indicate its transparency, mostly in the high‐energy region. Thus, twin irida graphene is a suitable material for use in optoelectronic applications due to its structural and physical characteristics.

Electric pulse-tuned piezotronic effect for interface engineering

Investigating interface engineering by piezoelectric, flexoelectric and ferroelectric polarizations in semiconductor devices is important for their applications in electronics, optoelectronics, catalysis and many more. The interface engineering by polarizations strongly depends on the property of interface barrier. However, the fixed value and uncontrollability of interface barrier once it is constructed limit the performance and application scenarios of interface engineering by polarizations. Here, we report a strategy of tuning piezotronic effect (interface barrier and transport controlled by piezoelectric polarization) reversibly and accurately by electric pulse. Our results show that for Ag/HfO2/n-ZnO piezotronic tunneling junction, the interface barrier height can be reversibly tuned as high as 168.11 meV by electric pulse, and the strain (0–1.34‰) modulated current range by piezotronic effect can be switched from 0–18 nA to 44–72 nA. Moreover, piezotronic modification on interface barrier tuned by electric pulse can be up to 148.81 meV under a strain of 1.34‰, which can totally switch the piezotronic performance of the electronics. This study provides opportunities to achieve reversible control of piezotronics, and extend them to a wider range of scenarios and be better suitable for micro/nano-electromechanical systems.

Achieving broadband NIR-I to NIR-II emission in layer-structured Mg4Nb2O9:Cr3+,Yb3+ phosphor for multifunctional applications

Broadband near-infrared (NIR) phosphor-converted light-emitting diodes (pc-LEDs) have garnered unprecedented attention in photonic, optoelectronic and biological applications. Here, an efficient broadband NIR phosphor Mg4Nb2O9:Cr3+ was achieved. Excited by 455 nm blue light, the Mg4Nb2O9:Cr3+ phosphor exhibited a maximum peak at 863 nm with a relatively wide full width at half maximum (FWHM) of approximately 178 nm and the internal quantum efficiency (IQE) was measured to be 94 %. The observed broadband emission in the NIR range can be attributed to two distinct Cr3+ centers within the Mg4Nb2O9 structure, namely Mg2+ and Mg2+-Mg2+ dimer, which was confirmed through luminescence, decay kinetic analysis and density function theory (DFT) calculations. To further broaden the NIR emission, Yb3+ was co-doped with Cr3+ in Mg4Nb2O9. Benefited from the efficient energy transfer from Cr3+ to Yb3+, the codoped Mg4Nb2O9:Cr3+, Yb3+ shows a bandwidth of 223 nm and IQE of 86.4 %. The pc NIR-LED device incorporating this phosphor achieved a NIR output power of 131.6 mW at input current of 400 mA, with a photoelectric conversion efficiency of 44.2 %. Finally, the constructed NIR-LED demonstrated multifunctional applications in non-destructive detection and information encryption.

Strain engineering of electronic, mechanical, and optical properties of orthorhombic III–V group monolayers by first principles calculations

Using first principles calculations, we systematically investigated the effects of strain engineering on the electronic, mechanical, and optical properties of two-dimensional (2D) orthorhombic III–V group materials, including BN, BP, BAs, AlN, AlP, and GaN. It is shown that all the III–V orthorhombic monolayers exhibit excellent mechanical anisotropy for Young’s modulus, Shear modulus, and Poisson’s ratio, especially for the AlN and GaN monolayers. AlN, AlP, and GaN are predicted to be indirect bandgap semiconductors, with their bandgap of 0.70, 0.15, and 0.53 eV, respectively. And BN is demonstrated to be a direct bandgap semiconductor (0.63 eV). Under uniaxial tensile strains, their electronic structures have non-monotonic anisotropic variations and these monolayers can be effectively modulated from metal to semiconductor, experiencing indirect–direct bandgap transitions. In addition, all the orthorhombic III–V materials exhibit highly anisotropic light-harvesting performances and the optical absorbance can be efficiently tailored with tensile strains applied along a- and b-directions. The strong optical absorptions in the visible light regions suggested that AlN, BN, and GaN may be optically tunable 2D materials for component absorbance layers for solar cell applications. The excellent anisotropic and tunable electronic, mechanical, and optical performances indicate that the orthorhombic III–V monolayers are promising candidates for potential applications of optoelectronics and photovoltaics.

Single Crystal Growth and Transport Properties of Narrow Band Gap Semiconductor RhP2

Abstract Here, we report the growth of high-quality single crystals of RhP2, and systematically study its structure and physical properties by transport, magnetism, and heat capacity measurements. Single-crystal X-ray diffraction revealed RhP2 adopts a monoclinic structure with the cell parameters a=5.7347(10) Å, b=5.7804(11) Å, and c=5.8222(11) Å, space group P21/c (No. 14). The electrical resistivity ρ(T) measurements indicate that RhP2 exhibits a narrow band gap behavior with the activation energies of 223.1 m eV and 27.4 m eV for two distinct regions, respectively. The temperature-dependent Hall effect measurements show electron domain transport behavior with a low charge carrier concentration. We found that RhP2 has a high mobility μe~210 cm2v-1s-1 with carrier concentrations ne~3.3×1018 cm-3 at 300 K with a narrow band gap feature. The high mobility μe reached a maximum of approximately 340 cm2v-1s-1 with carrier concentrations ne~2×1018 cm-3 at 100 K. No magnetic phase transitions were observed from the susceptibility χ(T) and specific heat Cp(T) measurements of RhP2. Our results not only offer effective potential as a material platform for studying exotic physical properties and electron band structures but also motivate further exploration of their potential photovoltaic and optoelectronic applications.

Delocalized, asynchronous, closed-loop discovery of organic laser emitters.

Contemporary materials discovery requires intricate sequences of synthesis, formulation, and characterization that often span multiple locations with specialized expertise or instrumentation. To accelerate these workflows, we present a cloud-based strategy that enabled delocalized and asynchronous design-make-test-analyze cycles. We showcased this approach through the exploration of molecular gain materials for organic solid-state lasers as a frontier application in molecular optoelectronics. Distributed robotic synthesis and in-line property characterization, orchestrated by a cloud-based artificial intelligence experiment planner, resulted in the discovery of 21 new state-of-the-art materials. Gram-scale synthesis ultimately allowed for the verification of best-in-class stimulated emission in a thin-film device. Demonstrating the asynchronous integration of five laboratories across the globe, this workflow provides a blueprint for delocalizing-and democratizing-scientific discovery.

Mn2+ Mediated Spin‐Exchange Enables CsPbBr3 Nanoplatelets to Function as Highly Efficient Triplet Sensitizers for Triplet‐Triplet Annihilation Upconversion

AbstractPerovskite nanoplatelets (NPls) have emerged as a new generation of nanomaterials that are promising for optoelectronic applications due to their large absorption and fast yet efficient emission. Particularly, they are also potential triplet sensitizers for triplet‐triplet annihilation upconversion (TTA‐UC), provided that the fast intrinsic decay of exciton can be circumvented. Herein, doping the CsPbBr3 NPls with Mn2+ (Mn2+: CsPbBr3 NPls) can efficiently convert fast‐decay triplet exciton to a long‐lived excited state of Mn2+ through Dexter‐type spin‐allowed energy transfer, enabling simultaneous large absorption and long‐lived excited state are demonstrated. Additionally, similar to the exciton‐to‐Mn2+ energy transfer, Mn2+‐to‐triplet state of annihilator energy transfer is also spin‐allowed and thus highly efficient. These pave the way for using Mn2+: CsPbBr3 NPls as triplet sensitizers. The superior triplet sensitization ability of Mn2+: CsPbBr3 NPls is demonstrated by using 9,10‐diphenylanthracene molecules (DPA) as representative annihilators. 93% quenching of Mn2+ emission and considerably accelerated decay of Mn2+ are observed after the addition of a trace amount of DPA. TTA‐UC measurement demonstrates that benefitted from the long‐lived excited state of Mn2+, the normalized upconversion photoluminescence quantum yield is ≈10% with an energy threshold being as low as ≈0.35 W cm−2. The results shed new light on using Mn2+: CsPbBr3 NPls as a triplet sensitizer.

Enhancing mid-infrared surface phonon polariton modes: optimization of structural parameters in Nb-doped SrTiO3 with hole array structures for advanced infrared sensors

This study utilized the finite difference time domain method to investigate the mid infrared surface phonon polaritons and localized surface phonon resonances in undoped and niobium (Nb)-doped SrTiO3 (STO) with planar and holes array structures. Research has shown that Nb-doped STO operates in the Reststrahlen band of 8.06–18.48 µm, providing a wider spectral response than undoped STO (12.58–18.26 µm) and effectively covering the atmospheric window of long wave infrared. This indicates that the increase in virtual permittivity has the least impact on spectral broadening, indicating that the new infrared sensor technology has broad prospects. The optimization of structural parameters, including the period, filling factor, and depth of STO holes array, as well as the response to changes in incident light angle, is crucial for guiding the design of high-performance optoelectronic devices. In addition, this study explored the excitation of four resonant modes within a holes array and analyzed their relationship with array parameters to enhance the design of optoelectronic applications.

Recent progress of group III-V materials-based nanostructures for photodetection.

Due to the suitable bandgap structure, efficient conversion rates of photon to electron, adjustable optical bandgap, high electron mobility/aspect ratio, low defects, and outstanding optical and electrical properties for device design, III-V semiconductors have shown excellent properties for optoelectronic applications, including photodiodes, photodetectors, solar cells, photocatalysis, etc. In particular, III-V nanostructures have attracted considerable interest as a promising photodetector platform, where high-performance photodetectors can be achieved based on the geometry-related light absorption and carrier transport properties of III-V materials. However, the detection range from Ultraviolet to Terahertz including broadband photodetectors of III-V semiconductors still have not been more broadly development despite significant efforts to obtain the high performance of III-V semiconductors. Therefore, the recent development of III-V photodetectors in a broad detection range from Ultraviolet to Terahertz, and future requirements are highly desired.
In this review, the recent development of photodetectors based on III-V semiconductor with different detection range is discussed. First, the bandgap of III-V materials and synthesis methods of III-V nanostructures are explored, subsequently, the detection mechanism and key figures-of-merit for the photodetectors are introduced, and then the device performance and emerging applications of photodetectors are provided. Lastly, the challenges and future research directions of III-V materials for photodetectors are presented.&#xD.

Computational study of lattice dynamics and mechanical properties of AlxIn1-xPySbzAs1-y-z/InP under the effect of composition

For the first time, the composition dependence of pentanary AlInPSbAs alloy is described. The effect of composition on the polarity (∝p), mechanical parameters have been calculated for the AlxIn1-xPySbzAs1-y-z alloy. The impact of composition on the internal strain parameter (ζ), bond-bending force constant (α), bond-stretching force constant (β), and sound velocity (v) has been reported. Results from experiments and the investigated properties of the new alloy show a high degree of agreement. In this work, the density function theory (DFT) and the empirical pseudo-potential approach (EPM) with the virtual crystal approximation (VCA) have been used. The outcomes are expected to be used in optoelectronic applications and in understanding the mechanical properties of AlxIn1-xPySbzAs1-y-z alloy.

Structural, optoelectronic, and magnetic behaviors of Li2BeTM( TM= V, Cr, Mn, Fe)Se4 compounds using DFT investigations

Abstract In this work, we provide computational investigations of the electronic, the optical and the magnetic properties of the Li2BeTMSe4(TM = V, Cr, Mn, Fe) compounds using the first-principle calculations based on the density functional theory. In this respect, we employ the generalized gradient approximation corrected by the Tran-Balaha modified Becke-Johnson exchange potential to obtain more accurate results. Among these outcomes, we first examine the electronic properties such as the band energy dispersion and the state densities. Regarding this, the Li2BeTMSe4 quaternary family is found to have an indirect band gap of 1.910 eV, 1.905 eV, 2.223 eV and 1.278 eV for TM= V, Cr, Mn, and Fe, respectively. Further, an examination of the optical properties reveals that the computed optical absorption spectra cover a broad energy range in the visible and the ultraviolet spectrum. Motivated by spintronic applications, we additionally determine the total and the local magnetic moments. Then, we compute the associated Curie temperature via a linear relation with the total magnetic moments. Among others, the Li2BeTMSe4(TM= V, Cr, Mn, Fe) materials involve acceptable temperatures showing potential applications for high temperature nano-devices activities. Comparing the obtained findings with the available ones, the acquired results indicate that the Li2BeTMSe4(TM = V, Cr, Mn, Fe) materials exhibit a wide range of applications in solar cells, optoelectronics, and other fields.

Highly Efficient and Thermally Stable Broadband NIR Phosphors with Superlong Afterglow Performance and their Multifunctional Applications

AbstractNear‐infrared (NIR) phosphor‐converted light‐emitting diodes (pc‐LEDs) are considered as promising next‐generation light sources for optoelectronic and biomedical applications. Nevertheless, NIR phosphors with large bandwidths, long emission peaks, high external quantum efficiencies (EQEs) and valuable thermal stabilities are challenging to develop. Herein, this study reports a novel gallium germanate host, Ga3Al3Ge2O13 (GAGO), with a large bandgap and rigid host lattice for Cr3+ ion doping. The blue LED excitable GAGO:0.012Cr3+ phosphor can produce broadband NIR emission with a maximum intensity at 816 nm and a full‐width at half‐maximum (FWHM) of 187 nm. Notably, the phosphor also exhibits an excellent EQE of 35.8% and perfect thermal stability (I423 K/I298 K = 67.4%). Moreover, an attractive NIR afterglow duration of more than 24 h is achieved in the GAGO:0.004Cr3+ phosphor. The type and origin of the traps are discussed, and a possible long persistent luminescent (LPL) mechanism is proposed. Finally, an NIR pc‐LED based on a GAGO:0.012Cr3+ phosphor is fabricated. The results demonstrate that the obtained phosphors show great potential for use in night vision, nondestructive detection, bioimaging and information encryption. This study provides new insight into the development of broadband NIR luminescent materials with high efficiency, good thermal stability and extraordinary afterglow performance.

Exploring the Mn doped BaTe alloy for spintronics and energy harvesting applications

In the present study, the ferromagnetic semiconductor behavior of Mn doped BaTe is reported along with their physical properties. The calculations are done by full potential linearized augmented plane wave (FP-LAPW) approach within spin-polarized density functional theory (SP-DFT). Formation energies were computed to satisfy the stability of reported alloys. The spin-polarization is included in the calculations to study the electronic (band structure (BS), density of states (DOS)) and magnetic characteristics. Ba1−xMnxTe elucidates the magnetic semiconductor nature with direct band gap (Eg) in both spin channels while indirect Eg (1.66 eV) is observed for pure BaTe compound. Stable ferromagnetic (FM) states are vindicated owing to the p-d hybridization which are contributors in inducing magnetic moments (μ B) at interstitial and non-magnetic sites. The optical parameters (reflectivity, absorption coefficient, refraction, optical conductivity and dielectric function) were computed within an energy range of 0–10 eV. Thermoelectric (TE) features are also figured using Boltaz-Trap code in terms of thermal and electrical conductivity, figure of merit, Seebeck coefficient and power factor. The analysis of optical parameters suggests that the considered alloys is active within visible to UV-range, having potential applications in optoelectronic, photovoltaic and thermoelectric applications.

Indolo[3,2-a]carbazoles as Engineered Materials for Optoelectronic Applications: Synthesis, Structural Insights, and Computational Screening.

The biological and medicinal importance of indolocarbazoles has been known for the past several decades. However, in recent times, these compounds have been emerging as potential candidates for optoelectronic applications, although several challenges are associated with their synthesis. We report here a Pd(II)-catalyzed process for the synthesis of indolo[3,2-a]carbazoles. The reaction proceeded under neat conditions and in the presence of aqueous nonmetallic oxidant TBHP, and the products were purified directly after the completion of the reaction. Also, the possibility of employing the present method for reaction with gram-scale feed was investigated. A detailed single-crystal analysis of several indolo[3,2-a]carbazoles revealed how the molecular arrangement can be tuned by altering the functionalization. Finally, the developed molecules were screened computationally to assess their potential for possible use as hole transport materials (HTMs) for organic light-emitting diodes (OLEDs).