Ambipolar Performance Research Articles

Improvement of C-shaped pocket TFET with sandwiched drain for ambipolar performance and analog/RF performance

A novel structure of tunneling field effect transistor device (CSP-SD-TFET) is proposed, which adds a sandwiched drain to the C-shaped pocket TFET (CSP-TFET). This structure can increase the resistance of the drain, share the lateral electric field at the tunneling junction between the channel and the drain, reduce the lateral electric field at the tunneling junction, and suppress the generation of ambipolar current. The DC and analog/RF characteristics of CSP-SD-TFET are simulated and analyzed by Sentaurus TCAD, and the sandwiched structure parameters of the drain are optimized. The results show that the sandwiched drain structure suppresses the ambipolar current and on-state current, so the parameters of the sandwiched drain structure need to be a compromise between low ambipolar current and high on-state current. The optimized CSP-SD-TFET device has good DC characteristics, such as low average subthreshold swing SSavg (12.2mV/dec), high on/off current ratio Ion/Ioff (2.5 × 1011), high on-state current Ion (9.02 × 10−4 A/μm) and low ambipolar current Iamb (5.41 × 10−17A/μm). The RF performance of the CSP-SD-TFET, such as the cut-off frequency fT (1 × 1011 Hz) and gain-bandwidth product GBP (5.66 × 1010 Hz), are improved. It can be seen that the CSP-SD-TFET device not only has good DC characteristics but also improves analog/RF characteristics.

Ambipolar performance improvement of the C-shaped pocket TFET with dual metal gate and gate–drain underlap

Dual-metal gate and gate–drain underlap designs are introduced to reduce the ambipolar current of the device based on the C-shaped pocket TFET(CSP-TFET). The effects of gate work function and gate–drain underlap length on the DC characteristics and analog/RF performance of CSP-TFET devices, such as the on-state current (I on), ambipolar current (I amb), transconductance (g m), cut-off frequency (f T) and gain–bandwidth product (GBP), are analyzed and compared in this work. Also, a combination of both the dual-metal gate and gate–drain underlap designs has been proposed for the C-shaped pocket dual metal underlap TFET (CSP-DMUN-TFET), which contains a C-shaped pocket area that significantly increases the on-state current of the device; this combination design substantially reduces the ambipolar current. The results show that the CSP-DMUN-TFET demonstrates an excellent performance, including high I on (9.03 × 10−9 A/μm), high I on/I off (∼1011), low SSavg (∼13 mV/dec), and low I amb (2.15 × 10−2 A/μm). The CSP-DMUN-TFET has the capability to fully suppress ambipolar currents while maintaining high on-state currents, making it a potential replacement in the next generation of semiconductor devices.

Cross-dipole π-π stacking of crossed perylene diimides with D-A-D structures by crystal engineering towards ambipolar charge transport performance and aggregation-induced emission

A cross-dipole π-π close-stacking of 1,7-diphenylazophenol (AZO) perylene diimides (PDI, AZO-PDIs) formed in a single-crystal integrating good ambipolar charge transport and aggregation-induced emission (AIE) behaviors has been unveiled. The weak electron donating and moderate steric hindrance of AZOs endows AZO-PDIs with crossed Donor-Acceptor-Donor (D-A-D) structures, which facilitates the charge injection of both electrons and holes and a distinct cross-dipole π-π close-packing with the distance of only 3.29 Å. Accordingly, the wave function overlaps and electronic coupling of PDI cores are significantly enhanced to provide a quasi-1D charge transport channel, resulting in ambipolar performance with the hole and electron mobility of 6.74 cm2 V−1 s−1 and 5.96 cm2 V−1 s−1 respectively. The average conductivity of 0.5 S m−1 has further confirmed the good charge transport properties of the single crystals. Moreover, it also exhibits AIE behaviors due to the weak transition dipole resonance induced by the cross-dipole stacking of a large rotation angle (79.8°) and restriction of intramolecular rotation of the bulk AZOs. This work initially provides a promising strategy for achieving both charge transport and AIE performance on account of D-A-D molecules with crossed conformations at the molecular level and efficient π-overlaps induced by cross-dipole stacking at the supramolecular level.

Buckybowl and its chiral hybrids featuring eight-membered rings and helicene units.

Here we report the synthesis of a novel buckybowl (7) with a high bowl-to-bowl inversion barrier (ΔG‡ = 38 kcal mol-1), which renders the rate of inversion slow enough at room temperature to establish two chiral polycyclic aromatic hydrocarbons (PAHs). By strategic fusion of eight-membered rings to the rim of 7, the chiral hybrids 8 and 9 are synthesized and display helicity and positive and negative curvature, allowing the enantiomers to be configurationally stable and their chiroptical properties are thoroughly examined. Computational and experimental studies reveal the enantiomerization mechanisms for the chiral hybrids and demonstrate that the eight-membered ring strongly affects the conformational stability. Because of its static and doubly curved conformation, 9 shows a high binding affinity towards C60. The OFET performance of 7-9 could be tuned and the hybrids show ambipolar characteristics. Notably, the 9·C60 cocrystal exhibits well-balanced ambipolar performance with electron and hole mobilities of up to 0.19 and 0.11 cm2 V-1 s-1, respectively. This is the first demonstration of a chiral curved PAH and its complex with C60 for organic devices. Our work presents new insight into buckybowl-based design of PAHs with configurational stability and intriguing optoelectronic properties.

High performance ambipolar semiconductor of pyridine-capped diketopyrrolopyrrole-porphyrin oligomers: Roles of thiophen substitution and oligomer length

Series of seven donor-acceptor pyridine-capped diketopyrrolopyrrole − 5,15-diacetylenyl-10,20-diaryl-porphyrinato zinc oligomers nPyDPP-PAr [n = 1–3, Ar = methyl-benzothiophene (BT) or methyl thiophene (T) or methylbenzene (B)] were designed. Density functional theory calculations were performed to theoretically study the molecular geometry, electronic structure, and charge transport properties of the seven donor-acceptor compounds. The effects of oligomer length and different Ar groups on the crystal packing mode and charge transport properties were systematically studied. Thiophen substitution reduces the electron injection barrier, diminishes the reorganization energy, enlarges the charge transfer integral, and therefore shows three-to-one role for ambipolar semiconductor with large charge transfer mobility. Extending the π-conjugated backbone not only improves the semiconductor performance, but also makes the ambipolar performance more balanced. 3PyDPP-PT and 3PyDPP-PBT show high hole/electron transfer mobility as high as 8.28/7.90 cm2 V−1 s−1 and 9.00/9.79 cm2 V−1 s−1, respectively.

Source pocket-engineered hetero-gate dielectric SOI Tunnel FET with improved performance

In this paper, we have studied and proposed a planar Tunnel FET device with source side SiGe pocket and hetero-gate dielectric structure that works by utilizing quantum mechanical Band-to-Band tunnelling (BTBT) mechanism. Simulation results obtained using a calibrated SILVACO TCAD device simulator show that the device exhibits good ambipolar performance because of the hetero-gate dielectric and the use of source pocket leads to steep point subthreshold swing of 4.90 mV/dec., an average subthreshold swing of 25.31 mV/dec. and a threshold voltage of 0.23 V. For including the hetero-gate dielectric, the variation in drain current values with high-κ dielectric length is analysed. The change in transfer characteristics with pocket parameters including pocket length and pocket doping is also reported. A 4 nm Si0.7Ge0.3 n+ pocket with doping concentration of 5 × 1019 cm−3 is found to show the maximum ON-OFF current ratio of 5.23 × 1011. This paper also performs a comparative study between different TFET structures and the analysis clearly highlights the potential of proposed Source Pocket-Engineered Hetero Gate Dielectric (SPE-HGD) TFET device for low-power and energy-efficient applications.

Synthesis and characterization of naphthalene derivatives for two-component heterojunction-based ambipolar field-effect transistors complemented with copper hexadecafluorophthalocyanine (F16CuPc).

In order to develop organic semiconductor materials with good performance, herein, a series of naphthalene derivatives were designed and synthesized by a “building-blocks approach” connected through α-bond, double bond, and triple bond, respectively. Thin-film transistors were fabricated in single-component and two-component modes based on these naphthalene derivatives by combining the F16CuPc as the n-type material. The ambipolar performance was investigated by adjusting the device preparation procedure with the hole and electron mobility of up to 10−2 cm2 V−1 s−1. Furthermore, the electrical performance was also improved to 0.73 cm2 V−1 s−1 using the two-component bilayer configuration.

A nonchlorinated solvent-processed polymer semiconductor for high-performance ambipolar transistors.

Ambipolar polymer semiconductors are potentially serviceable for logic circuits, light-emitting field-effect transistors (LFETs) and polymer solar cells (PSCs). Although several high-performance ambipolar polymers have been developed, their optoelectronic devices are generally processed from toxic chlorinated solvents. To achieve the commercial applications of organic FETs (OFETs), the polymers should be processed from nonchlorinated solvents, instead of chlorinated solvents. However, most conjugated polymers show poor solubility in nonchlorinated solvents. It is of great importance to develop ambipolar polymers that can be processed from nonchlorinated solvents. Here, we develop a nonchlorinated solvent processed polymer named poly[7-fluoro-N, N′-di(4-decyltetradecyl)-7′-azaisoindigo-6′,6″-(thieno[3,2-b]thiophene-2,5-diyl)-7‴-fluoro-N″, N‴-di(4-decyltetradecyl)-7″-azaisoindigo-6,6‴-([2,2″-bithiophene]-5,5″-diyl)] (PITTI-BT) by designing a monomer with a large molar mass. The polymer displays good solubility in p-xylene (PX). Well-aligned films of PITTI-BT are achieved by an off-center spin-coating (SC) method. Based on the high-quality films, the OFETs fabricated from PX solution achieve record ambipolar performance with hole and electron mobilities of 3.06 and 2.81 cm2 V−1 s−1, respectively. The combination of nonchlorinated solvents and good alignment process offers an effective and eco-friendly approach to obtain high-performance ambipolar transistors.

Organic (TPyP)Eu2[Pc(OPh)8]2/CdS self-assembled hybrid nano-transistors with high ambipolar performance

A new organic/inorganic hybrid bicomponent nanomaterial was obtained by quasi-Langmuir-Shafer (QLS) method with a mixed (phthalocyaninato)-(porphyrinato) europium complex (TPyP)Eu2[Pc(OPh)8]2 and the inorganic material CdS. The conductivity of the (TPyP)Eu2[Pc(OPh)8]2/CdS hybrid film (1.9 × 10−7 S cm−1) was greatly improved compared to the (TPyP)Eu2[Pc(OPh)8]2 film (6 × 10−10 S cm−1). In good contrast, the (TPyP)Eu2[Pc(OPh)8]2/CdS bicomponent thin film transistor devices constructed by QLS method revealed excellent ambipolar performance, much larger hole mobility (0.09 cm2 V−1 s−1; on/off ratio of 104) and electron mobility (0.01 cm2 V−1 s−1; on/off ratio of 103) when compared with single-component (TPyP)Eu2[Pc(OPh)8] film that showed 6.9 × 10−7 cm2 V−1 s−1 hole mobility (on/off ratio of 102) and 3.07 × 10−5 cm2 V−1 s−1 electron mobility (on/off ratio of 102). In addition, SEM and AFM results also showed that the bicomponent film had a uniform particle size distribution and a dense film structure. These properties could reduce the obstacles and carrier traps in the film and stabilize its electrical properties, which could greatly facilitate the transport of electrons and holes. The research work opens a new way for the preparation of stable, high-performance ambipolar OTFT devices in the air through molecular design and device assembly technology.

Theoretical insights on the high and differential charge transfer performance of dithienyl-diketopyrrolopyrrole-based polymers as ambipolar semiconductors

Diketopyrrolopyrrole (DPP)-containing polymers are among the highest mobility semiconductors for field-effect transistor applications. The molecular geometries, electronic structures and charge transport properties as ambipolar organic semiconductors of two series of total 24 donor–acceptor dithienyl-diketopyrrolopyrrole-based oligomers mDTDPPAr and nBDTDPPAr (m = 1–4, n = 1–2, Ar = TT, BT, BDT, TVT) are investigated theoretically through density functional theory and classical Marcus charge transfer theory. The effects of oligomer length form = 1–4, different Ar groups, and different Ar position on the structures and charge transfer properties are systematically studied. It was found that expanding π-conjugate backbone is a viable method to improve their semiconductor performance. Oligomers 4DTDPPTT, 4DTDPPBT, 4DTDPPTVT possess prominent ambipolar semiconductors properties with charge transfer mobilities of 9.62, 10.73, 12.60 cm2 V−1 s−1 for hole and of 7.54, 8.06, 15.56 cm2 V−1 s−1 for electron, respectively. 4DTDPPBDT exhibits large but unbalanced ambipolar performance with hole/electron transfer mobilities of 10.86/20.17 cm2 V−1 s−1 due to the special conjugation of BDT. Changing the order and position of donor and acceptor units has less significant influence on charge transfer mobility. Anisotropic mobilities are also studied to clarify the different charge transfer directions.

Tuning the Charge Carrier Polarity of Organic Transistors by Varying the Electron Affinity of the Flanked Units in Diketopyrrolopyrrole‐Based Copolymers

AbstractFine‐tuning of the charge carrier polarity in organic transistors is an important step toward high‐performance organic complementary circuits and related devices. Here, three new semiconducting polymers, namely, pDPF‐DTF2, pDPSe‐DTF2, and pDPPy‐DTF2, are designed and synthesized using furan, selenophene, and pyridine flanking group‐based diketopyrrolopyrrole cores, respectively. Upon evaluating their electrical properties in transistor devices, the best performance has been achieved for pDPSe‐DTF2 with the highest and average hole mobility of 1.51 and 1.22 cm2 V−1 s−1, respectively. Most intriguingly, a clear charge‐carrier‐polarity change is observed when the devices are measured under vacuum. The pDPF‐DTF2 polymer exhibits a balanced ambipolar performance with the µh/µe ratio of 1.9, whereas pDPSe‐DTF2 exhibits p‐type dominated charge carrier transport properties with the µh/µe ratio of 26.7. Such a charge carrier transport change is due to the strong electron‐donating nature of the selenophene. Furthermore, pDPPy‐DTF2 with electron‐withdrawing pyridine flanking units demonstrates unipolar n‐type charge transport properties with an electron mobility as high as 0.20 cm2 V−1 s−1. Overall, this study demonstrates a simple yet effective approach to switch the charge carrier polarity in transistors by varying the electron affinity of flanking groups of the diketopyrrolopyrrole unit.

Solution-processable (Pc′)Eu(Pc′)Eu[TP(OH)PP]/rGO bilayer heterojunction organic transistors with exceptional excellent ambipolar performance

For the purpose of fabricating next generation of microelectronics and photonics, the transistor that simultaneously provides high-efficiency charge transport and air-stable ambipolar performance becomes highly desired. In this paper, the bilayer heterojunction field-effect transistors, named as t-Pc-1/rGO (HFET-1) and t-Pc-2/rGO (HFET-2), are constructed for the first time by using a simple two-step solution-processing approach, in which the high conductive reduced graphene oxide (rGO) film as the sub-layer and the film of ambipolar sandwich mixed (phthalocyaninato)(porphyrinato) europium triple-deckers (Pc′)Eu(Pc′)Eu[TP(OH)PP] {Pc′ = Pc, [Pc(OPh)8]} (t-Pc-1, t-Pc-2) as the top layer, respectively. The resulting bilayer heterojunction devices exhibit significantly improved air-stable ambipolar performance with the carrier mobilities of ca. 107 to 108 fold higher than those of pristine triple-deckers, and the Ion/Ioff of 102 to 103 fold higher than that of the single-component rGO device. In particular, due to the heterojunction effect in an “accumulation mode”, the device HFET-2 shows the ultrahigh and balanced mobilities between hole, 30.9 cm2 V−1 s−1, and electron, 39.6 cm2 V−1 s−1, with the optimized ON/OFF ratio of 103 for both carriers, representing the best result for ambipolar OFET devices reported thus far.

Solution-processable small molecules for bulk heterojunction ambipolar thin-film transistors and complementary-like inverters

Solution-processable thioalkylated bithiophene derivatives with different lengths of side chains (SBT-n; n = 10, 12, 14, 16, 18) have been synthesized and characterized as p-channel organic semiconductors for thin-film transistors (TFTs). Based on a combination of the highest performing SBT derivative (SBT-14) and quinoidals (DTTRQs) as p- and n-channel materials, solution-processed small-molecular bulk heterojunction (BHJ) ambipolar thin-film transistors were fabricated, and the resulting devices showed air-stable and high ambipolar performance with well-balanced electron and hole mobilities as high as 0.70 cm2 V−1 s−1 and 0.21 cm2 V−1 s−1, respectively. Furthermore, complementary-like inverters comprising two ambipolar thin-film transistors were demonstrated, which exhibited a high voltage gain of up to 81. Our study clearly demonstrated that side chain engineering of small molecular organic semiconductors had a significant influence on the electrical performance of TFTs and BHJ transistors, as well as complementary-like inverters.

Optimization of Line-Tunneling Type L-Shaped Tunnel Field-Effect-Transistor for Steep Subthreshold Slope

The L-shaped tunneling field-effect-transistor (LTFET) has been recently introduced to overcome the thermal subthreshold limit of conventional metal-oxide-semiconductor field-effect-transistors (MOSFET). In this work, the shortcomings of the LTFET was investigated. It was found that the corner effect present in the LTFET effectively degrades its subthreshold slope. To avoid the corner effect, a new type of device with dual material gates is presented. The new device, termed the dual-gate (DG) LTEFT (DG-LTFET), avoids the corner effect and results in a significantly improved subthreshold slope of less than 10 mV/dec, and an improved ON/OFF current ratio over the LTFET. The DG-LTFET was evaluated for different device parameters and bench-marked against the LTFET. This work presents the optimum configuration of the DG-LTFET in terms of device dimensions and doping levels to determine the best subthreshold, ON current, and ambipolar performance.

Air-stable, transparent flexible ambipolar organic thin film transistors based on CuPc-F16CuPc bi-channel structure

We report the fabrication of air-stable, transparent flexible ambipolar organic thin film transistors based on CuPc and F16CuPc bi-channel films deposited under 10−1 Pa, by using graphene gate electrode, fluoropolymer Cytop dielectric layer, and Au source/drain electrodes on polyethylene terephthalate substrates. The devices show outstanding air-stability and high optical transparency of above 75% with electron and hole mobilities up to 0.031 and 0.029 cm2/V·s, respectively. The excellent ambipolar performance, along with the outstanding air-stability and high optical transparency, make CuPc-F16CuPc bi-channel transistors as a promising candidate for organic integrated circuits.

Medium band gap polymer based solution-processed high-κ composite gate dielectrics for ambipolar OFET

The authors present a novel ambipolar organic filed-effect transistors (OFETs) composed of a hybrid dielectric thin film of Ta2O5:PMMA nanocomposite material, and solution processed poly(selenophene, benzotriazole and dialkoxy substituted [1,2-b:4, 5-b′] dithiophene (P-SBTBDT)-based organic semiconducting material as the active layer of the device. We find that the Ta2O5:PMMA insulator shows n-type conduction character, and its combination with the p-type P-SBTBDT organic semiconductor leads to an ambipolar OFET device. Top-gated OFETs were fabricated on glass substrate consisting of interdigitated ITO electrodes. P-SBTBDT-based material was spin coated on the interdigitated ITO electrodes. Subsequently, a solution processed Ta2O5:PMMA nanocomposite material was spin coated, thereby creating the gate dielectric layer. Finally, as a gate metal, an aluminum layer was deposited by thermal evaporation. The fabricated OFETs exhibited an ambipolar performance with good air-stability, high field-induced current and relatively high electron and hole mobilities although Ta2O5:PMMA nanocomposite films have slightly higher leakage current compared to the pure Ta2O5 films. Dielectric properties of the devices with different ratios of Ta2O5:PMMA were also investigated. The dielectric constant varied between 3.6 and 5.3 at 100 Hz, depending on the Ta2O5:PMMA ratio.

Balanced Ambipolar Organic Field-Effect Transistors by Polymer Preaggregation.

Ambipolar organic field-effect transistors (OFETs) based on heterojunction active films still suffer from an imbalance in the transport of electrons and holes. This problem is related to an uncontrolled phase separation between the donor and acceptor organic semiconductors in the thin films. In this work, we have developed a concept to improve the phase separation in heterojunction transistors to enhance their ambipolar performance. This concept is based on preaggregation of the donor polymer, in this case poly(3-hexylthiophene) (P3HT), before solution mixing with the small-molecular-weight acceptor, phenyl-C61-butyric acid methyl ester (PCBM). The resulting heterojunction transistor morphology consists of self-assembled P3HT fibers embedded in a PCBM matrix, ensuring balanced mobilities reaching 0.01 cm2/V s for both holes and electrons. These are the highest mobility values reported so far for ambipolar OFETs based on P3HT/PCBM blends. Preaggregation of the conjugated polymer before fabricating binary blends can be regarded as a general concept for a wider range of semiconducting systems applicable in organic electronic devices.

Gate engineered heterostructure junctionless TFET with Gaussian doping profile for ambipolar suppression and electrical performance improvement

This study investigates a junctionless tunnel field-effect transistor with a dual material gate and a heterostructure channel/source interface (DMG-H-JLTFET). We find that using the heterostructure interface improves device behavior by reducing the tunneling barrier width at the channel/source interface. Simultaneously, the dual material gate structure decreases ambipolar current by increasing the tunneling barrier width at the drain/channel interface. The performance of the device is analyzed based on the energy band diagram at on, off, and ambipolar states. Numerical simulations demonstrate improvements in ION, IOFF, ION/IOFF, subthreshold slope (SS), transconductance and cut-off frequency and suppressed ambipolar behavior. Next, the workfunction optimization of dual material gate is studied. It is found that if appropriate workfunctions are selected for tunnel and auxiliary gates, the JLTFET exhibits considerably improved performance. We then study the influence of Gaussian doping distribution at the drain and the channel on the ambipolar performance of the device and find that a Gaussian doping profile and a dual material gate structure remarkably reduce ambipolar current. Gaussian doped DMG-H-JLTFET, also exhibits enhanced IOFF, ION/IOFF, SS and a low threshold voltage without degrading IOFF.

Controlled morphology of self-assembled microstructures via solvent-vapor annealing temperature and ambipolar OFET performance based on a tris(phthalocyaninato) europium derivative

A novel homoleptic sandwich-type tris[2,3,9,10,16,17,23,24-octa(naphthoxy)phthalocyaninato] europium triple-decker complex Eu2[Pc(ONh)8]3 (1), having a low-lying LUMO energy level of – 4.0 eV and relatively narrow HOMO–LUMO separation of 1.13 eV, was designed and successfully synthesized. The OFET devices fabricated from this compound using a solution-based quasi-Langmuir-Shäfer (QLS) method display air-stable ambipolar performance with the carrier mobilities of (2.5 ± 0.5) × 10−6 cm2 V−1 s−1 for holes and (2.3 ± 0.3) × 10−6 cm2 V−1 s−1 for electrons, indicating its ambipolar semiconducting nature. Upon the o-dichlorobenzene (DCB) solvent vapor annealing at the temperature of 60, 80, 100, and 120 °C, a fine combination of the “oriented attachment” with Ostwald ripening process under controlled SVA environments leads to the growth of the first two-dimensional (2D) micro-sheet microstructures with tunable morphology including the fragment-like irregular polygons, quasi-four-corner sheets, squares, and clovers, respectively, from the nanoparticles of the pristine QLS film. This in turn results in the tunable OFET device performance with the carrier mobilities changing as a result of the morphologies and crystallinities. The best result was achieved for the most crystalline 2D squares-based devices with the carrier mobilities of 0.11 ± 0.03 cm2 V−1 s−1 for holes and 0.06 ± 0.02 cm2 V−1 s−1 for electrons.

How methoxy groups change nature of the thiophene based heterocyclic chalcones from p-channel to ambipolar transport semiconducting materials

Chalcone derivatives gained significant consideration from scientific community due to their potential applications ranging from better biological activity to the efficient semiconducting properties. Present investigation deals with the in-depth study of three chalcone derivatives (2E)-1-(2,5-Dimethyl-3-thienyl)-3-(2-methoxyphenyl)prop-2-en-1-one (1), (2E)-3-(3,4-Dimethoxyphenyl)-1-(2,5-dimethylthiophen-3-yl)prop-2-en-1-one (2), and (E)-1-(2,5-Dimethyl-3-thienyl)-3-(2,4,5-trimethoxyphenyl)prop-2-en-1-one (3) highlighting their optoelectronic, charge transport (CT) and nonlinear optical (NLO) response. The ground and excited state geometries are optimized by applying density functional theory (DFT) and time dependent DFT, respectively. The effect of electron donating groups on the frontier molecular orbitals, absorption and emission wavelengths are investigated and discussed thoroughly using the quantum chemical calculations. The comprehensive intra-molecular charge transfer (ICT) is perceived from the occupied orbitals to the unoccupied molecular orbitals. A novel structure-property relationship is established on the basis of their calculated electronic structures, frontier orbitals and density of states. The electro-optical and nonlinear optical (NLO) properties are finely tuned in the chalcone derivatives comprising of di- and tri-methoxy groups at peripheral. The nature of the p-type and ambipolar charge transport behavior of the compounds 1–3 is limelighted on the basis of their ionization potentials, electron affinities, reorganization energies, transfer integrals and intrinsic mobility. The mono- and di-substituted methoxy chalcone derivatives show the ambipolar performance owing to the better transfer integral and intrinsic mobility values for hole and electron. Whilst tri-methoxy at peripheral would lead the p-channel characteristics due to the balanced reorganization energy (hole and electron) and superior hole transfer integrals leads to higher hole intrinsic mobility.