PRPachaiyappan Rajamalli

Pachaiyappan Rajamalli

*This is an algorithmically generated author record based on publicly available information.

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Pachaiyappan Rajamalli has a total of 171 co-authors. Here are the top co-authors by number of shared publications:


Latest Publications

  • Realizing Locally Excited Intermediate Triplets via Naphthyl Unit in Donor‐Acceptor Based Thermally Activated Delayed Fluorescence Emitters for Efficient OLEDs

    by Nisha Yadav, Annette Mariya Tedy, Arun K. Manna, Pachaiyappan Rajamalli

    An in‐depth understanding of locally excited (LE) intermediate states is crucial in regulating the reverse intersystem crossing (RISC) process and overall efficiency of thermally activated delayed fluorescence (TADF) emitters, directing rational material synthesis. Herein, we investigated the effect of incorporating a low‐triplet‐energy naphthyl core at the acceptor, donor, and both positions through the design and synthesis of three donor‐acceptor (D‐A) emitters, with tunable optoelectronic properties. Doping 7 wt.% of NP‐ m DPA, 3BPy‐ m PNP, and NP‐ m PNP in 3,3′‐di(9 H ‐carbazol‐9‐yl)‐1,1′‐biphenyl ( m CBP) host resulted in the first excited singlet‐triplet energy gap (Δ E ST ) of 0.28, 0.31, and 0.42 eV. Temperature‐dependent transient photoluminescence (PL) measurements indicate robust TADF behavior in NP‐ m DPA and 3BPy‐ m PNP, while NP‐ m PNP exhibits weaker TADF accompanied by prominent phosphorescent fingerprints. In multi‐layer organic light‐emitting diodes (OLEDs) with an emissive layer (EML) comprising 7 wt.% of emitters in m CBP host, NP‐ m DPA exhibited an electroluminescence (EL) peak at 502 nm with the highest maximum external quantum efficiency (EQE max ) of 18.6%. In contrast, 3BPy‐ m PNP (505 nm) and NP‐ m PNP (492 nm) showed reduced EQE max of 12.6% and 5.1%. Detailed theoretical calculations reveal that incorporating a naphthyl unit in both D and A produces intermediate LE triplet states and improves RISC. Whereas, the naphthyl unit in only D or only A results in reduced Δ E ST and , enabling NP‐ m DPA to be the most efficient among the studied emitters.

  • Tuning the Acceptor Core in Cyano PyridineBased Framework to Realize Efficient TADF Emitters

    by Ashish K. Mazumdar, Bhaskar Chelleng, Svadha Devi, Gyana Prakash Nanda, Ganesh Manikandan, Pachaiyappan Rajamalli

    For next‐generation organic light‐emitting diode (OLED) displays and lighting, achieving stable, efficient deep‐blue and sky‐blue emission remains a challenge. Herein, we report a cyanopyridine‐based modular scaffold, an asymmetric dual core (2tCz2PyCN) that suppresses exciton loss to achieve sky‐blue emission, and an asymmetric single core analog (2tCzPyCN). The single core 2tCzPyCN exhibits deep blue emission ( λ max = 437 nm) with a CIE of (0.15, 0.14), asymmetric 2tCz2PyCN emitter exhibits sky‐blue emission ( λ max = 478 nm) with a CIE of (0.19, 0.38). The reduced conjugation in the single core 2tCzPyCN widens the energy gap, resulting in deep‐blue color (CIE y = 0.14), it also maximizes faster reverse intersystem crossing (RISC) through spin orbit coupling (SOC). The extended bipyridine core of 2tCz2PyCN lowers the excited state reorganization energy (0.82 vs. 0.94 eV), suppressing non‐radiative decay and raising the PLQY from 41.6% to 80.7%. The 2tCzPyCN‐based device achieves an EQE max of 8.80% in the deep blue region, whereas the asymmetric 2tCz2PyCN shows EQE max of 16.63% in the sky‐blue region. This work demonstrates that engineering the excited state via an asymmetric acceptor is a practical pathway for color tuning and developing efficient TADF emitters.

  • 3-Phenylisoquinoline Ligand-Driven Enhanced Triplet Emission in an Ir(III) Phosphor Enabling High-Efficiency in Orange and Hybrid White OLEDs

    by Md Intekhab Alam, Upasana Deori, Malati Das, Jyothis Dharaniyedath, Bhaskar Chelleng, Parthasarathy Gandeepan, Pachaiyappan Rajamalli

    We report the synthesis, photophysical properties, and electroluminescent performance of a Ir(3-phenylisoquinoline)3 (Ir(3-piq)3) complex. Single-crystal X-ray analysis reveals a distorted octahedral geometry with strong intermolecular interactions that enforce rigid molecular packing and abate nonradiative decay by reducing structural reorganization. Photophysical investigations reveal weak orange emission in solution and significantly enhanced emission in doped films. Optimized organic light-emitting diodes (OLEDs) achieve a low turn-on voltage of 2.5 V, a maximum external quantum efficiency (EQEmax) of 22.8%, and a brightness of 49616 cd/m2 with stable electroluminescence. Moreover, hybrid white OLEDs were fabricated by incorporating the blue TADF emitter, 3DPy-pDTC as an auxiliary dopant. The fabricated devices exhibit warm-white emission at 0.7 wt % doping of Ir(3-piq)3, delivering EQEmax of 17.7%. Notably, reducing the doping concentration of Ir(3-piq)3 to 0.5 wt % results in a well-balanced bright white emission with CIE co-ordinate of (0.29, 0.33) and achieves an EQEmax of 14.7%. These performances are attributed to efficient exciton utilization driven by synergistic phosphorescence and rapid reverse intersystem crossing in TADF emitters. Overall, this work demonstrates an effective strategy for achieving high-efficiency and stable orange emission in Ir-complexes and color-tunable hybrid white OLEDs through synergistic exciton management.


  • Open Access

    Tailoring B, N-embedded Helicenes towards Narrowband Circularly Polarized Organic Light-Emitting Diodes

    by Upasana Deori, Fangyuan Zhang, Suvendu Dey, Debranjan Hati, Prince Ravat, Pachaiyappan Rajamalli

    Owing to their inherently helical π-conjugated frameworks, helicenes are considered promising candidates for circularly polarized luminescence (CPL). Nonetheless, their implementation in circularly polarized organic light-emitting diodes (CP-OLEDs) remains limited due to difficulties in achieving both high color purity and external quantum efficiency (EQE). Recent advancements incorporate multi-resonance properties with boron-nitrogen units, which have shown significant improvements in this regard. Herein, a chiral emitter ( C 1 ) consisting of 1,4-B,N-embedded helical configuration is studied. C 1 exhibits narrowband fluorescence emission at 510 nm with a full width at half maxima (FWHM) of 23 nm in toluene and 26 nm in thin film. The resolved enantiomers show symmetric CPL, with a dissymmetry factor ( g lum ) of 1.0 × 10 –3 . The solution-processed CP-OLED based on C 1 exhibits external quantum efficiency (EQE) of 5.3%, delivering bright green emission centred at 514 nm with a FWHM of 28 nm. To further enhance the performance of the device, hyperfluorescent (HF) OLEDs are fabricated with C 1 acting as a terminal emitter and BPy-DTC as the TADF sensitizer. The maximum EQE of 13.5% is achieved, with a narrow FWHM of 39 nm. This work highlights the strong potential of helicene-based emitters for application in narrowband CP-OLEDs.

  • Rational Rigid‐Core Design Realizes Efficient and Color‐Pure Sky‐Blue MR‐TADF Emission in Boron‐Nitrogen Functionalized Dibenzo‐Xanthene

    by Thamodharan Viswanathan, Sabyasachi Maity, Upasana Deori, Nikhitha R., Nandish Sh, Sandhayarani Pal, Nisha Yadav, Anirban Mondal, Pachaiyappan Rajamalli

    In this work, we report the strategic incorporation of a rigid 14H‐dibenzo[a,j]xanthene ( DBX ) core into the BCz‐BN framework, leading to the development of a novel DBX‐BCz‐BN multi‐resonance (MR) thermally activated delayed fluorescence (TADF) emitter. This structural modification preserves the sky‐blue emission color while substantially narrowing the emission profile, reducing the full width at half maximum (FWHM) to 17 nm. In addition, the singlet–triplet energy gap (Δ E ST ) is lowered from 0.17 eV for BCz‐BN to 0.06 eV, thereby promoting more efficient reverse intersystem crossing (RISC) and improved exciton harvesting. As a result, the corresponding OLED device based on DBX‐BCz‐BN exhibits an external quantum efficiency (EQE) of 22.2%, while maintaining the same emission color. These results demonstrate that rigid‐core engineering via DBX incorporation is an effective strategy for achieving narrowband, efficient, and color‐pure sky‐blue TADF emitters.

  • Open Access

    Supramolecular engineering of non-planar bridged-ethers: blue to red emission tuning and solution-processed OLED fabrication

    by Shouvik Bhuin, Upasana Deori, Pandiyan Sivasakthi, Avanigadda Madhu Niharika, Pralok K. Samanta, Pachaiyappan Rajamalli, Manab Chakravarty

    Bridged oxo/thioethers are conjugated to a highly twisted molecular framework where alterations of the heteroatoms result in various molecular packing patterns, tuning blue-to-red emission, and are applied to afford a solution-processed yellow OLED.


  • Exploiting Ultrathin Layer to Realize Simultaneous High Electroluminescence Efficiency and Color Quality in Hybrid White Organic Light-Emitting Diodes

    by Upasana Deori, Vikash Kumar, Parthasarathy Gandeepan, Pachaiyappan Rajamalli

    Highly efficient white organic light-emitting diodes (WOLEDs) created by combining phosphorescent and thermally activated delayed fluorescence (TADF) emitters have advanced rapidly as cutting-edge technology for their potential applications in flat-panel displays and solid-state lighting. However, achieving high device performance while simultaneously ensuring a high white color quality remains a challenge. Here, we demonstrate efficient WOLEDs, fabricated by using a blue TADF emitter with an orange phosphor in a single emissive layer, enabling the generation of white light. The WOLEDs exhibit outstanding electroluminescent (EL) performance, achieving a maximum external quantum efficiency (EQE) of 31.8% and power efficiency (PE) of 56.8 lm W-1 and producing cold and warm white light by varying the concentration of the phosphor emitter. To further enhance the quality of white light without compromising the EL performance, a multilayer sandwich configuration was adopted by introducing an ultrathin (∼1 nm) layer of the efficient green TADF emitter BPyDTC between two white emissive layers. This design strategy resulted in a high-performance WOLED with a maximum EQE of 28.8% and a PE of 65.5 lm W-1, with EQE and PE values of 17.0% and 25.1 lm W-1at a luminance of 1000 cd m-2, respectively. The emission from all the layers effectively blends, achieving better coverage of the visible spectrum and generating white light with Commission Internationale de l'Eclairage, CIE coordinates of (0.38, 0.41).


  • A rigid xanthene–anthracene-based scaffold exhibiting ultra deep blue emission: multifunctional material as emitter and host for blue OLEDs

    by Nisha Yadav, Pachaiyappan Rajamalli

    Ultra-deep blue fluorescent emitters with Commission Internationale de L’Eclairage (CIE y ) < 0.08 are still in demand for achieving vibrant full-color displays.


  • Realizing high-efficiency TADF from a low-performing cyanopyridine emitter via symmetric coupling

    by Ashish Kumar Mazumdar, Bhaskar Chelleng, Svadha Devi, Gyana Prakash Nanda, Ganesh Manikandan, Pachaiyappan Rajamalli

    A novel dual core TADF emitter has been synthesized involving a symmetric coupling, demonstrating a minimal Δ E ST of 0.08 eV, an enhanced PLQY of 59.1% and a high EQE max of 15.02%, when compared to its single-core counterpart.


  • Design Strategy for Inducing Delayed Fluorescence via Molecular Flexibility: Structure -Property Relationships in Organic Emitters

    by Gyana Prakash Nanda, Suvendu Dey, Bahadur Sk, Rajan Suraksha, Anirban Mondal, Pachaiyappan Rajamalli

    Modification of the molecular structure can drastically change the photophysical properties of the luminogens, establishing these structure-property relationships provides a roadmap for the rational design of novel materials. In this...