Charge Transition Research Articles

The Physical Mechanism of Linear and Nonlinear Optical Properties of Nanographene-Induced Chiral Inversion.

Based on density functional theory (DFT) and wave function analysis, the ultraviolet and visible spectrophotometry (UV-Vis) spectra and Raman spectra of 1-meso and 1-rac obtained by the chiral separation of chiral nanographenes are theoretically investigated. The electron excitation properties of 1-meso and 1-rac are studied by means of transition density matrix (TDM) and charge density difference (CDD) diagrams. The intermolecular interaction is discussed based on an independent gradient model based on Hirshfeld partition (IGMH). The interaction of 1-meso and 1-rac with the external environment is studied using the electrostatic potential (ESP), and the electron delocalization degree of 1-meso and 1-rac is studied based on the magnetically induced current under the external magnetic field. Through the chiral separation of 1-rac, two enantiomers, 1-(P, P) and 1-(M, M), were obtained. The electrical-magnetic interaction of the molecule is revealed by analyzing the electron circular dichroism (ECD) spectra of 1-meso, 1-(P, P) and 1-(M, M), the transition electric dipole moment (TEDM) and the transition magnetic dipole moment (TMDM). It is found that 1-(P, P) and 1-(M, M) have opposite chiral properties due to the inversion of the structure.

Enhanced CO2 Electrolysis Through Mn Substitution Coupled with Ni Exsolution in Lanthanum Calcium Titanate Electrodes.

In this study, perovskite oxides La0.3Ca0.6Ni0.05MnxTi0.95- xO3- γ (x = 0, 0.05, 0.10) are investigated as potential solid oxide electrolysis cell cathode materials. The catalytic activity of these cathodes toward CO2 reduction reaction is significantly enhanced through the exsolution of highly active Ni nanoparticles, driven by applying a current of 1.2 A in 97% CO2 - 3% H2O. The performance of La0.3Ca0.6Ni0.05Ti0.95O3-γ is notably improved by co-doping with Mn. Mn dopants enhance the reducibility of Ni, a crucial factor in promoting the in situ exsolution of metallic nanocatalysts in perovskite (ABO3) structures. This improvement is attributed to Mn dopants enabling more flexible coordination, resulting in higher oxygen vacancy concentration, and facilitating oxygen ion migration. Consequently, a higher density of Ni nanoparticles is formed. These oxygen vacancies also improve the adsorption, desorption, and dissociation of CO2 molecules. The dual doping strategy provides enhanced performance without degradation observed after 133h of high-temperature operation, suggesting a reliable cathode material for CO2 electrolysis.

Unraveling the Photoluminescent Properties of Sb-Doped Cd-Based Inorganic Halides: A First-Principles Study.

Sb-doped Cd-based inorganic halides, with varying connections of CdCl6 octahedra ranging from 0D to 3D, exhibit a variety of photoluminescent properties. Single-band emission is observed in Sb-doped Rb4CdCl6 (0D) and Cs2CdCl4 (2D), while dual-band emission is seen in Sb-doped RbCdCl3 (1D) and CsCdCl3 (3D). Density-functional-based first-principles calculations were conducted. The results reveal that cation vacancies, acting as charge compensators, influence the luminescence properties of dopant centers. In CsCdCl3, the local cation vacancy VCd″ for Sb3+ at the Cd2+ site ([Sb□Cl9]6-) significantly modifies the photoluminescence property, accounting for the observed dual-band emission alongside the nonlocal compensation case. This effect is insignificant in Sb-doped Rb4CdCl6, RbCdCl3, and Cs2CdCl4, due to the large distances or high formation energies of Cd vacancies in these hosts. However, in Sb-doped RbCdCl3, two different potential energy minima, one that involves typical structure relaxation and the other that is off-center, lead to the observed dual-band emission. Furthermore, the shift of the charge transition level illustrates the different temperature dependences of the dual-band emission caused by the charge-compensating point defects. These insights not only enhance our understanding of luminescent materials based on halides containing ns2 dopants but also provide valuable guidance for the design and optimization of luminescent materials.

Metal‐Free Organic Dyes with Double Auxiliary Acceptors for High‐Performance Dye‐Sensitized Solar Cells

Dye‐sensitized solar cells (DSSCs) have continuously received attentions in the field of photovoltaics due to their charming properties and promising performance under the indoor dim‐light environment. Herein, two organic photosensitizers (GZ121 and GZ124) are designed with the insertion of double auxiliary acceptors in a donor‐acceptor‐π‐acceptor‐π‐acceptor (D‐A‐π‐A‐π‐A) design. The devices fabricated from these photosensitizers are investigated under one sun and dim‐light (300–6000 lux) conditions with N719 dye for comparison. The GZ124 dye achieves power conversion efficiencies (PCEs) of 9.43% (photocurrent density (Jsc) = 14.79 mA cm−2, photovoltage (Voc) = 0.85 V, and fill factor (FF) = 0.75) under one sun irradiation and 28.62% (Jsc = 0.99 mA cm−2, Voc = 0.68 V, and FF = 0.77) under dim‐light illumination at 6000 lux, which is far better than the reference N719 dye. Moreover, the PCE under dim light is ranked among the top as compared to DSSCs devices sensitized by a single dye. The GZ124 dye also demonstrates outstanding stability for more than 1000 h under prolonged one sun sensitization. The current studies affirm that the design of a D‐A‐π‐A‐π‐A structural framework by introducing double auxiliary acceptors in a single sensitizer is a promising approach to boost the performance of DSSCs.

The deep-acceptor nature of the chalcogen vacancies in 2D transition-metal dichalcogenides

Chalcogen vacancies in the semiconducting monolayer transition-metal dichalcogenides (TMDs) have frequently been invoked to explain a wide range of phenomena, including both unintentional p-type and n-type conductivity, as well as sub-band gap defect levels measured via tunneling or optical spectroscopy. These conflicting interpretations of the deep versus shallow nature of the chalcogen vacancies are due in part to shortcomings in prior first-principles calculations of defects in the semiconducting two-dimensional TMDs that have been used to explain experimental observations. Here we report results of hybrid density functional calculations for the chalcogen vacancy in a series of monolayer TMDs, correctly referencing the thermodynamic charge transition levels to the fundamental band gap (as opposed to the optical band gap). We find that the chalcogen vacancies are deep acceptors and cannot lead to n-type or p-type conductivity. Both the (0/−1) and (−1/−2) transition levels occur in the gap, leading to paramagnetic charge states S=1/2 and S = 1, respectively, in a collinear-spin representation. We discuss trends in terms of the band alignments between the TMDs, which can serve as a guide to future experimental studies of vacancy behavior.

Multifunctional In-MOF and Its S-Scheme Heterojunction toward Pollutant Decontamination via Fluorescence Detection, Physical Adsorption, and Photocatalytic REDOX.

A novel doubly interpenetrated indium-organic framework of 1 has been assembled by In3+ ions and highly conjugated biquinoline carboxylate-based bitopic connectors (H2L). The isolated 1 exhibits an anionic framework possessing channel-type apertures repleted with exposed quinoline N atoms and carboxyl O atoms. Owing to the unique architecture, 1 displays a durable photoluminescence effect and fluorescence quenching sensing toward CrO42-, Cr2O72-, and Cu2+ ions with reliable selectivity and anti-interference properties, fairly high detection sensitivity, and rather low detection limits. Ligand-to-ligand charge transition (LLCT) was identified as the essential cause of luminescence by modeling the ground state and excited states of 1 using DFT and TD-DFT. In addition, the negatively charged framework has the ability to rapidly capture single cationic MB, BR14, or BY24 and their mixture, including the talent to trap MB from the (MB + MO) system with high selectivity. Moreover, intrinsic light absorption capacity and band structure feature endow 1 with effective photocatalytic decomposition ability toward reactive dyes RR2 and RB13 under ultraviolet light. Notably, after further polishing the band structure state of 1 by constructing the S-scheme heterojunction of In2S3/1, highly efficient photocatalytic detoxification of Cr(VI) and degradation of reactive dyes have been fully achieved under visible light. This finding may open a new avenue for designing novel multifunctional MOF-based platforms to address some intractable environmental issues, i.e., detection of heavy metal ions, physical capture of pony-sized dyes, and photochemical decontamination of ultrastubborn reactive dyes and highly toxic Cr(VI) ions from water.

Substrate Doping and Defect Influence on P-Rich InP(001):H Surface Properties

Density-functional theory calculations on P-rich InP(001):H surfaces are presented. Depending on temperature, pressure and substrate doping, hydrogen desorption or adsorption will occur and influence the surface electronic properties. For p-doped samples, the charge transition levels of the P dangling bond defects resulting from H desorption will lead to Fermi level pinning in the lower half of the band gap. This explains recent experimental data. For n-doped substrates, H-deficient surfaces are the ground-state structure. This will lead to Fermi level pinning below the bulk conduction band minimum. Surface defects resulting from the adsorption of additional hydrogen can be expected as well, but affect the surface electronic properties less than H desorption.

Effect of temperature on lanthanide charge transition levels and vacuum referred binding energies

Location of lanthanide levels in the bandgap, vacuum referred binding energy (VRBE) in the lanthanide ground state and energy of lanthanide charge transition levels (CTLs) are just three different namings for the same concept. A concept of importance for the performance of lanthanide activated compounds. Energy differences of CTLs with the conduction band bottom and valence band top are important when it concerns e.g. lanthanide luminescence, charge carrier trapping, and valence stability. Effect of temperature on CTL energy or VRBE has so far never been addressed despite that luminescence application and thermoluminescence studies may span a temperature range from 10 K to 1000 K. In this work information on the bandgap (or energy of host exciton creation) around 10 K and at RT in compounds is gathered to demonstrate that bandgap decreases by 0.1 eV to 0.3 eV when temperature increases to RT. A similar decrease will be demonstrated for the energy of electron transfer from the VB to a trivalent lanthanide. The findings have consequences for VRBE-diagram construction, i.e. the experimental parameters for such construction should all apply to the same temperature. They also have consequences on how to relate luminescence thermal quenching energy barriers and TL derived electron and hole trap depths with a VRBE diagram. By proper evaluating the effects of temperature, accuracy of VRBE diagrams and consistency with luminescence and thermoluminescence data can be improved.

Improved Single-Shot Qubit Readout Using Twin rf-SET Charge Correlations

High-fidelity qubit readout is critical in order to obtain the thresholds needed to implement quantum error-correction protocols and achieve fault-tolerant quantum computing. Large-scale silicon qubit devices will have densely packed arrays of quantum dots with multiple charge sensors that are, on average, farther away from the quantum dots, entailing a reduction in readout fidelities. Here, we present a readout technique that enhances the readout fidelity in a linear SiMOS four-dot array by amplifying correlations between a pair of single-electron transistors, known as a twin SET. By recording and subsequently correlating the twin SET traces as we modulate the dot detuning across a charge transition, we demonstrate a reduction in the charge readout infidelity by over one order of magnitude compared to traditional readout methods. We also study the spin-to-charge conversion errors introduced by the modulation technique and conclude that faster modulation frequencies avoid relaxation-induced errors without introducing significant spin-flip errors, favoring the use of the technique at short integration times. This method not only allows for faster and higher-fidelity qubit measurements but it also enhances the signal corresponding to charge transitions that take place farther away from the sensors, enabling a way to circumvent the reduction in readout fidelities in large arrays of qubits. Published by the American Physical Society 2024

Study of a charge transition-driven resistive switching mechanism in TiO2-based random access memory via density functional theory.

The nature of the conducting filament (CF) with a high concentration of oxygen vacancies (VOs) in oxide thin film-based resistive random access memory (RRAM) remains unclear. The VOs in the CF have been assumed to be positively charged (VO2+) to explain the field-driven switching of RRAM, but VO2+ clusters in high concentration encounter Coulomb repulsion, rendering the CF unstable. Therefore, this study examined the oxidation state of VOs in the CF and their effects on the switching behavior via density functional theory calculations using a Pt/TiO2/Ti model system. It was concluded that the VOs in the CF are in a low oxidation state but are transformed to VO2+ immediately after release from the CF. In addition, the short-range interactions between VOs were confirmed to facilitate the rupture and rejuvenation of the CF by reducing the required activation energy. Finally, an improved switching model was proposed by considering the charge transition of VOs, providing a plausible explanation for the reported coexistence of two opposite bipolar switching polarities: the eight-wise and the counter-eight-wise polarities.

Field induced metamagnetic transition and mixed charge transfer Mott-Hubbard character in nanocrystalline FeCo2O4 spinel oxide: A combined study using experimental and first principles techniques

Unusual magnetic behavior of nanocrystalline FeCo2O4 (FCO) has been observed at different annealing temperatures. FCO nanoparticles have been prepared by co-precipitation method and the prepared sample annealed at different temperatures to vary its crystallite size. The powder x-ray diffraction analysis confirms the presence of pure spinel phase in the samples annealed at 900 ℃ and 1000℃. The increase in particle size with annealing temperature has been confirmed by field emission scanning electron microscopy (FESEM) analysis. High resolution x-ray photoelectron spectroscopy (HRXPS) analysis reveals the presence of mixed oxidation states of Fe+2/ Fe+3 and Co+3/Co+2 in the sample annealed at 900℃. The as-synthesized sample at 80 °C shows strong antiferromagnetic behavior due to their smaller particle size, but all the annealed samples have strong ferromagnetic behavior with large coercive field and remanence due to their larger particle size. We have observed a sharp rise in magnetization near small field values in the virgin curve and also the presence of virgin curve completely outside the main hysteresis loop in the M(H) curves measured at 5 K for the samples annealed at and above 1000 ℃ reveal the characteristic of first order nature of field induced metamagnetic transition. Structural parameters obtained after Rietveld refinement of powder x-ray diffraction pattern for sample annealed at 900 ℃ have been used for investigating the magnetic properties using first principles density functional theory. Our calculations using hybrid exchange-correlation functional, HSE06 captures the correct insulating ferromagnetic ground state and band gap for inverse spinel structure in broad agreement with our experimental results while calculations within GGA+U leads to a wrong half metallic ferromagnetic ground state. The partial density of states obtained for inverse spinel structure with HSE06 functional suggests a mixed charge transfer and Mott-Hubbard character in our system. We have explored the interplay among structural, magnetic and transport properties of FCO using experiment as well as first principles density functional theory.

Photothermal catalytic conversion of water and inert nitriles to amide activated by in-situ formed transition-metal-complex nanodots

Photothermal catalytic N-acetylation of aniline has been a promising strategy to synthesize amides, which combined the advantages of thermal catalysis and photocatalysis. Herein, we demonstrate a high-performance strategy to synthesize amides catalyzed by the in-situ formed first-row transition-metal (Fe, Co, Ni, Mn et al.) complexes nanodots (TMC NDs) under solar light excitation without using noble metals or strong acids. The dual-functional nitriles substrates acted as the ligands to coordinate with transition-metal salts affording photosensitive TMC NDs with high solar-to-thermal energy conversion efficiency. Intramolecular charge transitions reduced the energy barrier of nitriles activation by weakening CN bond and triggered near-field temperature rise via the electron–phonon scattering non-radiative pathway. The reaction system exhibited good tolerance to different functional groups, affording a series of amide derivatives. Such a dynamic coordination reaction mode and the in-situ formed TMC NDs opens new avenues toward solar-heat conversion via photon–phonon coupling in the field of chemical synthesis.

Macrocyclization-induce emission enhancement characteristics of benzothiadiazole-based macrocycles: A theoretical study

We present a comprehensive investigation into the molecular structures in the ground state and the first singlet excited state, intramolecular and intermolecular interactions, as well as the emission properties of monomers, dimers and macrocycles using density functional theory and time-dependent density functional theory. Our study aims to unveil the macrocyclization-induce emission enhancement principle for benzothiadiazole-based macrocycles. Compared with the typical π-π stacking of monomers, macrocycles exhibit the tighter stacking arrangement due to the presence of strong intramolecular and intermolecular hydrogen bond interactions and the rigid triangular geometry of macrocycle, which is conducive to the enhancement of emissions efficiency. The calculated oscillator strength of macrocycles in the first excited state is much higher than that of dimers composed of two monomers. Meanwhile, the large transition electric dipole moment is beneficial for enhancing the emission efficiency. Additionally, our study reveals an emission wavelength red-shift for macrocycles after “CH”/N substitution in the acceptor moiety, and the transition mode from LUMO to HOMO can be mainly attributed to intramolecular charge transition characters from acceptor to donor fragments. Our theoretical study might provide valuable insights for the design of innovative luminescent macrocycles with high emission efficiency.

Using transition density models to interpret experimental optical spectra of exciton-coupled cyanine (iCy3)2 dimer probes of local DNA conformations at or near functional protein binding sites.

Exciton-coupled chromophore dimers are an emerging class of optical probes for studies of site-specific biomolecular interactions. Applying accurate theoretical models for the electrostatic coupling of a molecular dimer probe is a key step for simulating its optical properties and analyzing spectroscopic data. In this work, we compare experimental absorbance and circular dichroism (CD) spectra of 'internally-labeled' (iCy3)2 dimer probes inserted site-specifically into DNA fork constructs to theoretical calculations of the structure and geometry of these exciton-coupled dimers. We compare transition density models of varying levels of approximation to determine conformational parameters of the (iCy3)2 dimer-labeled DNA fork constructs. By applying an atomistically detailed transition charge (TQ) model, we can distinguish between dimer conformations in which the stacking and tilt angles between planar iCy3 monomers are varied. A major strength of this approach is that the local conformations of the (iCy3)2 dimer probes that we determined can be used to infer information about the structures of the DNA framework immediately surrounding the probes at various positions within the constructs, both deep in the duplex DNA sequences and at sites at or near the DNA fork junctions where protein complexes bind to discharge their biological functions.

An estimator for the Coulomb repulsion parameter U to generate vacuum referred binding energy schemes for lanthanides in compounds

The U-value defined as the energy difference between the Eu4+/3+ and Eu3+/2+ charge transition levels (CTLs) is the most important parameter in constructing vacuum referred binding energy diagrams (VRBEs) with all the lanthanide CTLs with respect to the vacuum level of energy. The parameter is difficult to determine from experiment and the aim of this work is to establish a method to estimate the U-value from the average electronegativity of the cations in the compound. Since the U-value is controlled by the same physical processes, i.e., covalence and anion polarizability, as the centroid shift ϵc of the Ce3+ 5d configuration, one may estimate the U-value from that centroid shift. That method provides already good values for U for about 175 different compounds. Those U-values are compared with the average cation electronegativity χav, and relations will be established from which the U-value can be estimated with about ±0.1 eV accuracy from just the composition of the compound. It can be applied to all types of stoichiometric inorganic compounds like the halides (F, Cl, Br, I), chalcogenides (O, S, Se), and nitrides (N). The U-value complemented with the bandgap and the energy needed for electron transfer from the valence band top to a trivalent lanthanide dopant is then sufficient to construct a VRBE diagram with all lanthanide levels with respect to the vacuum level and the host valence and conduction bands.

High-temperature electrical breakdown and energy storage performance of ladderphane copolymer enhanced by molecular bondage and deep trapping

The advancement of renewable energy urgently needs dielectric capacitors with high energy storage performance at elevated temperatures. The energy loss and energy storage density are the core performance of these capacitors, which are determined by the conductivity and breakdown characteristics that are significantly influenced by the parameters such as trap characteristics, free volume, thermal expansion, and polymer chains displacement. Therefore, it is imperative to establish a quantitative correlation between microscopic parameters and energy storage performance of the ladderphanes for their substantial enhancement in energy storage density presently to elucidate this mechanism and further improve the performance. In this paper, the criterion of breakdown caused by the long displacement of polymer chains under the action of electric and thermal fields was proposed. Combining charge transport, heat transfer, and polymer chains motion, a joint simulation model of conductivity-breakdown-energy storage was established. The simulation results were consistent with the experimental results of high-temperature breakdown and energy storage. It was unveiled that the aggregate structure enhances the high-temperature breakdown and energy storage capabilities of ladderphane copolymer by restraining polymer chains motion and impeding charge transitions.

Case of the Bromine Vacancy in Cs4PbBr6.

Typically defect tolerance is equated with a lack of deleterious defects or with abundant defects creating only shallow levels. Here, we address the idea that deep defects, when unavoidable, do not guarantee harmful consequences. Using halogen vacancy as a common defect among halides, we explore its behavior in Cs4PbBr6. It is a large gap material (band gap of ∼4 eV) known for its green emission at ∼520 nm. We show that its Br-vacancy is indeed a deep defect as obtained from hybrid density functional calculations. An analysis of the configuration coordinate diagram corresponding to the defect's charge transition levels enables us to conclude that the nonradiative recombination cycle will be hampered by an extremely slow hole capture process. Therefore, Br-vacancy will not suppress light emission in Cs4PbBr6. Although this finding does not signal that all deep defects will behave similarly, it indicates that defect tolerance may be achievable despite their occurrence.

A new zero-dimensional (0D) hybrid bismuth (III) halide: Synthesis, crystal structure, thermal analysis, photophysical properties and DFT calculations

Low-dimensional organic-inorganic hybrid Bi(III) halides, with organic N, O-heterocycles, are promising solid-state photoluminescent materials, but are underexplored. In this work, we present the synthesis and characterization of a novel bismuth (III) hybrid salt, namely (C8H12NO)4[Bi2Cl10] (referred as (1)). (1) was synthesized using a solvent-evaporation method and extensively characterized using various techniques. The crystal structure of (1) was determined to be zero-dimensional (0D). In this structure, the individual bioctahedral [Bi2Cl10]4− dimers, which share edges, are completely isolated from each other. These dimers are separated by large 4-methoxybenzylammonium cations (C8H12NO)+. The latter are crucial for the crystal structural stability by balancing [Bi2Cl10]4-dimer charges and maintaining overall integrity. Solid-state diffuse reflectance UV–Vis spectrum demonstrates that (1) is a semiconductor with a band gap of 3.32 eV. Its photoluminescence spectrum exhibits intense blue emission when exposed to UV light, with CIE chromaticity coordinates of (0.22, 0.21). Theoretical calculations suggest that the emission with multiple centers originates both from a charge transition between (C8H12NO)+ and Bi2Cl104− ions and from excited-state proton transfer (ESPT) processes related to fluorescence properties. These ESPT processes occur through C–H…π and C–H…O intermolecular hydrogen bonding between the organic cations.

Syntheses, structures, photophysical properties and electroluminescent applications of dinuclear Copper(I) halide complexes containing 9-carbazolyl-substituted 1,2-Bis(diphenylphosphino)benzene

The studies on the photophysical properties of the copper(I) halide complexes based on rigid diphosphine ligands have attracted increasing attention. Here, six copper(I) halide complexes containing 9-carbazolyl-substituted 1,2-bis(diphenylphosphino)benzene, Cu2X2 (L1)2 and Cu2X2 (L2)2 [L1 = 1,2-bis(9-carbazolyl)-4,5-bis(diphenylphosphino)benzene, X = I (1), Br (2), Cl (3); L2 = 1-(9-carbazolyl)-3,4-bis(diphenylphosphino)benzene, X = I (4), Br (5), Cl (6)], were synthesized and characterized. In these complexes, two copper(I) centers are bridged by two halogen ligands to form a dinuclear structure with a four membered Cu2X2 ring. They exhibited efficient yellow green to yellowish orange delayed fluorescence in the powder state at ambient temperature, with peak wavelengths located between 548 and 602 nm (τ = 1.2–2.3 μs; Φ = 0.09–0.53). The introduction of one or two 9-carbazolyl substituents into the diphosphine resulted in the red shifting emission, shorter decay time and higher thermal stability of the complexes. The emission of the complexes originates from (metal + halide)-to-ligand and intraligand charge transitions. Organic light-emitting devices based on complex 1 exhibit yellow green luminescence with maximum external quantum efficiency of 12.0 % and current efficiency of 32.64 cd A−1.

Molecular engineering of tetraphenyl-based hole transporting materials to enhance photovoltaic properties of perovskite solar cells

Perovskite photovoltaic cells have lately gained appeal due to their excellent operational efficiency, photophysical properties, and high dielectric constant. Five novel hole transport materials namely TADM1–TADM5 were devised to improve power conversion efficiency (PCE) of Perovskite solar cells (PSCs). These molecules have tetraphenyl (TP) as a typical core, donor, and different acceptor units connected via a thiophene spacer. Under the framework of DFT theory, the B3LYP functional along with the 6–31 G basis set was utilized to study their geometries, molecular electrostatic potential, reorganization energies, the density of states, quantum chemical parameters, transition density matrix, binding energies, and charge transfer properties. All the designed HTMs (TADM1–TADM5) displayed excellent photovoltaic properties due to lower (Eg) varying (1.94–2.54 eV), small binding energies (0.04–0.36 eV), and high dipole moments (12.89 D to 26.93 D) that enhanced their electron charge transfer behavior. Small reorganization energy (RE) values for holes and electrons resulted in significant charge mobility. All the designed HTMs (TADM1-TADM5) have higher VOC (1.30–1.43 V) and power conversion efficiency (23.70–26.27%) than the reference molecule SMeTAD (20.94%). Consequently, all of the modelled molecules (TADM1-TADM5) demonstrate that using acceptor moieties is an effective method for achieving acceptable optoelectronic characteristics and outstanding efficiency.