skip to main content


Title: Direct Imprinting of Quasi‐3D Nanophotonic Structures into Colloidal Quantum‐Dot Devices
Abstract

Three‐dimensional (3D) subwavelength nanostructures have emerged and triggered tremendous excitement because of their advantages over the two‐dimensional (2D) counterparts in fields of plasmonics, photonic crystals, and metamaterials. However, the fabrication and integration of 3D nanophotonic structures with colloidal quantum dots (CQDs) faces several technological obstacles, as conventional lithographic and etching techniques may affect the surface chemistry of colloidal nanomaterials. Here, the direct fabrication of functional quasi‐3D nanophotonic structures into CQD films is demonstrated by one‐step imprinting with well‐controlled precision in both vertical and lateral directions. To showcase the potential of this technique, diffraction gratings, bilayer wire‐grid polarizers, and resonant metal mesh long‐pass filters are imprinted on CQD films without degrading the optical and electrical properties of CQD. Furthermore, a dual‐diode CQD detector into an unprecedented mid‐wave infrared two‐channel polarization detector is functionalized by embedding an imprinted bilayer wire‐grid polarizer within the CQDs. The results show that this approach offers a feasible pathway to combine quasi‐3D nanostructures with colloidal materials‐based optoelectronics and access a new level of light manipulation.

 
more » « less
NSF-PAR ID:
10373680
Author(s) / Creator(s):
 ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Materials
Volume:
32
Issue:
9
ISSN:
0935-9648
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Photodetectors based on colloidal quantum dots (CQDs) and single layer graphene (SLG) have shown high responsivity due to the synergy of strong light absorption from CQDs and high mobility from SLG. However, it is still challenging to achieve high-density and small-footprint devices on a chip to meet the demand for their integration into electronic devices. Even though there are numerous approaches to pattern the chemically fragile CQD films, usually they require non-conventional approaches such as stamping and surface modification that may be non-compatible with semiconductor processing. In this study, we show that conventional lithography and dry etching can be used to pattern QD active films by employing a graphene monolayer passivation/protective layer that protects the surface ligands of CQDs. This protective layer avoids damage induced by lithography process solvents that deteriorate the carrier mobility of CQDs and therefore the photoresponse. Herein we report patterning of CQDs using conventional UV photolithography, achieving reproducible five-micron length PbS CQDs/SLG photodetectors with a responsivity of 10 8 A W −1 . We have also fabricated thirty-six PbS CQDs/SLG photodetectors on a single chip to establish micron size photodetectors. This process offers an approach to pattern QDs with conventional UV lithography and dry etching semiconductor technology to facilitate their integration into current semiconductor commercial technology. 
    more » « less
  2. Abstract

    Halide perovskite colloidal quantum dots (CQDs) have recently emerged as a promising candidate for CQD photovoltaics due to their superior optoelectronic properties to conventional chalcogenides CQDs. However, the low charge separation efficiency due to quantum confinement still remains a critical obstacle toward higher‐performance perovskite CQD photovoltaics. Available strategies employed in the conventional CQD devices to enhance the carrier separation, such as the design of type‐Ⅱ core–shell structure and versatile surface modification to tune the electronic properties, are still not applicable to the perovskite CQD system owing to the difficulty in modulating surface ligands and structural integrity. Herein, a facile strategy that takes advantage of conjugated small molecules that provide an additional driving force for effective charge separation in perovskite CQD solar cells is developed. The resulting perovskite CQD solar cell shows a power conversion efficiency approaching 13% with an open‐circuit voltage of 1.10 V, short‐circuit current density of 15.4 mA cm−2, and fill factor of 74.8%, demonstrating the strong potential of this strategy toward achieving high‐performance perovskite CQD solar cells.

     
    more » « less
  3. Three-dimensional (3D) nanostructures play a crucial role in nanophotonics, lasers, and optical systems. This article reports on the fabrication of 3D nanostructures consisting of opal structures that are spatially aligned to an array of holes defined in the photoresist. The proposed method uses colloidal lithography to pattern a hexagonal array of holes, which are then used to direct the subsequent 3D assembly of colloidal particles. This approach allows the 3D opal structures to be aligned with the 2D array of holes, which can enhance spatial-phase coherence and reduce defects. The polymer patterns can be used as a sacrificial template for atomic layer deposition and create free-standing nanolattices. The final structure consists of a combination of nanolattice, upon which controlled deposition of opal structures is achieved. These structures result in nanostructured materials with high porosity, which is essential to create low-index materials for nanophotonics. A thick layer of titanium oxide with high refractive index is deposited over nanolattices to demonstrate the mechanical stability of underlying structures. These nanolattice structures with precisely controlled height can serve as a low-index layer and can find applications in Bragg reflectors, nanophotonics, and optical multilayers.

     
    more » « less
  4. Colloidal quantum dots (CQDs) provide wide spectral tunability and high absorption coefficients owing to quantum confinement and large oscillator strengths, which along with solution processability, allow a facile, low-cost, and room-temperature deposition technique for the fabrication of photonic devices. However, many solution-processed CQD photodetector devices demonstrate low specific-detectivity and slow temporal response. To achieve improved photodetector characteristics, limiting carrier recombination and enhancing photogenerated carrier separation are crucial. In this study, we develop and present an alternate vertical-stack photodetector wherein we use a solution-processed quantum dot photoconversion layer coupled to an amorphous selenium (a-Se) wide-bandgap charge transport layer that is capable of exhibiting single-carrier hole impact ionization and is compatible with active-matrix readout circuitry. This a-Se chalcogenide transport layer enables the fabrication of high-performance and reliable solution-processed quantum dot photodetectors, with enhanced charge extraction capabilities, high specific detectivity (D* ∼ 0.5–5 × 1012 Jones), fast 3 dB electrical bandwidth (3 dB BW ∼ 22 MHz), low dark current density (JD ∼ 5–10 pA/cm2), low noise current (in ∼ 20–25 fW/Hz1/2), and high linear dynamic range (LDR ∼ 130–150 dB) across the measured visible electromagnetic spectrum (∼405–656 nm). 
    more » « less
  5. Modern high-throughput nanopatterning techniques, such as nanoimprint lithography, make it possible to fabricate arrays of nanostructures (features with dimensions of 10’s to 100’s of nm) over large area substrates (cm2to m2scale) such as Si wafers, glass sheets, and flexible roll-to-roll webs. The ability to make such large-area nanostructure arrays (LNAs) has created an extensive design space, enabling a wide array of applications including optical devices, such as wire-grid polarizers, transparent conductors, color filters, and anti-reflection surfaces, and building blocks for electronic components, such as ultracapacitors, sensors, and memory storage architectures. However, existing metrology methods will have trouble scaling alongside fabrication methods. Scanning electron microscopy (SEM) and atomic force microscopy (AFM), for instance, have micron scale fields of view (FOV) that preclude comprehensive characterization of LNAs, which may be manufactured at m2per minute rates. Scatterometry approaches have larger FOVs (typically 100’s of µm to a few mm), but traditional scatterometry systems measure samples one point at a time, which also makes them too slow for large-scale LNA manufacturing. In this work, we demonstrate parallelization of the traditional spectroscopic scatterometry approach using hyperspectral imaging, increasing the throughput of the technique by a factor of 106-107. We demonstrate this approach by using hyperspectral imaging and inverse modeling of reflectance spectra to derive 3-dimensional geometric data for Si nanopillar array structures over both mm and cm-scale with µm-scale spatial resolution. This work suggests that geometric measurements for a variety of LNAs can be performed with the potential for high speed over large areas which may be critical for future LNA manufacturing.

     
    more » « less