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1.
J Am Chem Soc ; 146(42): 29094-29103, 2024 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-39385061

RESUMO

Shortwave infrared (SWIR) light emitters and detectors are crucial in numerous applications. Conventionally, SWIR devices rely on epitaxially grown narrow bandgap semiconductors, such as InGaAs, which are expensive to fabricate and difficult to integrate with silicon complementary metal-oxide-semiconductors (CMOS). Colloidal quantum dots (CQDs) have emerged as low-cost alternatives to epitaxially grown semiconductors, offering integration with CMOS through solution-processing methods. However, the predominant SWIR-active CQD systems rely on heavy-metal-containing compositions (PbS and HgTe), hindering the adoption of CQD SWIR technology. InAs CQDs are promising substitutes in SWIR applications. However, synthesizing SWIR-active InAs CQDs is challenging, often constraining them to the visible or near-infrared regions. To achieve SWIR bandgaps, large InAs CQDs are typically required; such CQDs are prone to having surface traps that quench photogenerated charge carriers, adversely affecting device performance. Here, we report a two-step synthesis of surface-passivated SWIR-active InAs/ZnSe core/shell colloidal nanorod quantum dots (CNQDs). These surface-passivated CNQDs are highly emissive and tunable over the entire technologically important region (1200-1800 nm) of the SWIR window with photoluminescence quantum yields as high as 60%. Using these SWIR-active InAs/ZnSe CNQDs, we demonstrated an SWIR-active InAs CQD photodetector, achieving a record high external quantum efficiency of ∼15% at ∼1450 nm and a low dark current of ∼10-2 mA/cm2.

2.
J Am Chem Soc ; 146(6): 4144-4152, 2024 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-38315569

RESUMO

Circularly polarized light-emitting diodes (CP-LEDs) are critical for next-generation optical technologies, ranging from holography to quantum information processing. Currently deployed chiral luminescent materials, with their intricate synthesis and processing and limited efficiency, are the main bottleneck for CP-LEDs. Chiral metal nanoclusters (MNCs) are potential CP-LED materials, given their ease of synthesis and processability as well as diverse structures and excited states. However, their films are usually plagued by inferior electronic quality and aggregation-caused photoluminescence quenching, necessitating their incorporation into host materials; without such a scheme, MNC-based LEDs exhibit external quantum efficiencies (EQEs) < 10%. Herein, we achieve an efficiency leap for both CP-LEDs and cluster-based LEDs by using novel chiral MNCs with aggregation-induced emission enhancement. CP-LEDs using enantiopure MNC films attain EQEs of up to 23.5%. Furthermore, by incorporating host materials, the devices yield record EQEs of up to 36.5% for both CP-LEDs and cluster-based LEDs, along with electroluminescence dissymmetry factors (|gEL|) of around 1.0 × 10-3. These findings open a new avenue for advancing chiral light sources for next-generation optoelectronics.

3.
Angew Chem Int Ed Engl ; : e202416288, 2024 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-39291657

RESUMO

We present a series of newly developed donor-acceptor (D-A) polymers designed specifically for organic electrochemical transistors (OECTs) synthesized by a straightforward route. All polymers exhibited accumulation mode behavior in OECT devices, and tuning of the donor comonomer resulted in a three-order-of-magnitude increase in transconductance. The best polymer gFBT-g2T, exhibited normalized peak transconductance (gm,norm) of 298±10.4 S cm-1 with a corresponding product of charge-carrier mobility and volumetric capacitance, µC*, of 847 F V-1 cm-1 s-1 and a µ of 5.76 cm2 V-1 s-1, amongst the highest reported to date. Furthermore, gFBT-g2T exhibited exceptional temperature stability, maintaining the outstanding electrochemical performance even after undergoing a standard (autoclave) high pressure steam sterilization procedure. Steam treatment was also found to promote film porosity, with the formation of circular 200-400 nm voids. These results demonstrate the potential of gFBT-g2T in p-type accumulation mode OECTs, and pave the way for the use in implantable bioelectronics for medical applications.

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