Seeded growth of single-crystal two-dimensional covalent organic frameworks

Science ◽  
2018 ◽  
Vol 361 (6397) ◽  
pp. 52-57 ◽  
Author(s):  
Austin M. Evans ◽  
Lucas R. Parent ◽  
Nathan C. Flanders ◽  
Ryan P. Bisbey ◽  
Edon Vitaku ◽  
...  
Keyword(s):  
Transient Absorption ◽  
Molecular Transport ◽  
Transient Absorption Spectroscopy ◽  
Two Dimensional ◽  
Covalent Organic Frameworks ◽  
Seeded Growth ◽  
Step Procedure ◽  
Structures And Properties ◽  
Powder Samples ◽  
2D Polymer

Polymerization of monomers into periodic two-dimensional networks provides structurally precise, layered macromolecular sheets that exhibit desirable mechanical, optoelectronic, and molecular transport properties. Two-dimensional covalent organic frameworks (2D COFs) offer broad monomer scope but are generally isolated as powders comprising aggregated nanometer-scale crystallites. We found that 2D COF formation could be controlled using a two-step procedure in which monomers are added slowly to preformed nanoparticle seeds. The resulting 2D COFs are isolated as single-crystalline, micrometer-sized particles. Transient absorption spectroscopy of the dispersed COF nanoparticles revealed improvement in signal quality by two to three orders of magnitude relative to polycrystalline powder samples, and suggests exciton diffusion over longer length scales than those obtained through previous approaches. These findings should enable a broad exploration of synthetic 2D polymer structures and properties.

Seeded Growth of Single-Crystal Two-Dimensional Covalent Organic Frameworks

2017 ◽  
Author(s):  
Austin M. Evans ◽  
Lucas R. Parent ◽  
Nathan C. Flanders ◽  
Ryan P. Bisbey ◽  
Edon Vitaku ◽  
...  
Keyword(s):  
Molecular Transport ◽  
Controlled Synthesis ◽  
Two Dimensional ◽  
Covalent Organic Frameworks ◽  
Seeded Growth ◽  
Covalent Bonds ◽  
Crystalline Materials ◽  
Step Procedure ◽  
Structures And Properties ◽  
2D Polymer

<div> <div> <div> <p>Polymerizing monomers into periodic two-dimensional (2D) networks provides structurally precise, atomically thin macromolecular sheets linked by robust, covalent bonds. These materials exhibit desirable mechanical, optoelectrotronic, and molecular transport properties derived from their designed structure and permanent porosity. 2D covalent organic frameworks (COFs) offer broad monomer scope, but are generally isolated as polycrystalline, insoluble powders with limited processability. Here we overcome this limitation by controlling 2D COF formation using a two- step procedure. In the first step, 2D COF nanoparticle seeds are prepared with approximate diameters of 30 nm. Next, monomers are slowly added to suppress new nucleation while promoting epitaxial growth on the existing seeds to sizes of several microns. The resulting COF nanoparticles are of exceptional and unprecedented quality, isolated as single crystalline materials with micron-scale domain sizes. These findings advance the controlled synthesis of 2D layered COFs and will enable a broad exploration of synthetic 2D polymer structures and properties. </p> </div> </div> </div>

Seeded Growth of Single-Crystal Two-Dimensional Covalent Organic Frameworks

2017 ◽  
Author(s):  
Austin M. Evans ◽  
Lucas R. Parent ◽  
Nathan C. Flanders ◽  
Ryan P. Bisbey ◽  
Edon Vitaku ◽  
...  
Keyword(s):  
Molecular Transport ◽  
Controlled Synthesis ◽  
Two Dimensional ◽  
Covalent Organic Frameworks ◽  
Seeded Growth ◽  
Covalent Bonds ◽  
Crystalline Materials ◽  
Step Procedure ◽  
Structures And Properties ◽  
2D Polymer

<div> <div> <div> <p>Polymerizing monomers into periodic two-dimensional (2D) networks provides structurally precise, atomically thin macromolecular sheets linked by robust, covalent bonds. These materials exhibit desirable mechanical, optoelectrotronic, and molecular transport properties derived from their designed structure and permanent porosity. 2D covalent organic frameworks (COFs) offer broad monomer scope, but are generally isolated as polycrystalline, insoluble powders with limited processability. Here we overcome this limitation by controlling 2D COF formation using a two- step procedure. In the first step, 2D COF nanoparticle seeds are prepared with approximate diameters of 30 nm. Next, monomers are slowly added to suppress new nucleation while promoting epitaxial growth on the existing seeds to sizes of several microns. The resulting COF nanoparticles are of exceptional and unprecedented quality, isolated as single crystalline materials with micron-scale domain sizes. These findings advance the controlled synthesis of 2D layered COFs and will enable a broad exploration of synthetic 2D polymer structures and properties. </p> </div> </div> </div>

Seeded Growth of Single-Crystal Two-Dimensional Covalent Organic Frameworks

2017 ◽  
Author(s):  
Austin M. Evans ◽  
Lucas R. Parent ◽  
Nathan C. Flanders ◽  
Ryan P. Bisbey ◽  
Edon Vitaku ◽  
...  
Keyword(s):  
Molecular Transport ◽  
Controlled Synthesis ◽  
Two Dimensional ◽  
Covalent Organic Frameworks ◽  
Seeded Growth ◽  
Covalent Bonds ◽  
Crystalline Materials ◽  
Step Procedure ◽  
Structures And Properties ◽  
2D Polymer

<div> <div> <div> <p>Polymerizing monomers into periodic two-dimensional (2D) networks provides structurally precise, atomically thin macromolecular sheets linked by robust, covalent bonds. These materials exhibit desirable mechanical, optoelectrotronic, and molecular transport properties derived from their designed structure and permanent porosity. 2D covalent organic frameworks (COFs) offer broad monomer scope, but are generally isolated as polycrystalline, insoluble powders with limited processability. Here we overcome this limitation by controlling 2D COF formation using a two- step procedure. In the first step, 2D COF nanoparticle seeds are prepared with approximate diameters of 30 nm. Next, monomers are slowly added to suppress new nucleation while promoting epitaxial growth on the existing seeds to sizes of several microns. The resulting COF nanoparticles are of exceptional and unprecedented quality, isolated as single crystalline materials with micron-scale domain sizes. These findings advance the controlled synthesis of 2D layered COFs and will enable a broad exploration of synthetic 2D polymer structures and properties. </p> </div> </div> </div>

scholarly journals Manipulation of hot carrier cooling dynamics in two-dimensional Dion–Jacobson hybrid perovskites via Rashba band splitting

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Jun Yin ◽  
Rounak Naphade ◽  
Partha Maity ◽  
Luis Gutiérrez-Arzaluz ◽  
Dhaifallah Almalawi ◽  
...  
Keyword(s):  
Transient Absorption ◽  
Phonon Scattering ◽  
Transient Absorption Spectroscopy ◽  
Band Model ◽  
Two Dimensional ◽  
Spintronic Devices ◽  
Hot Carrier ◽  
Band Splitting ◽  
Perovskite Materials ◽  
Spin Polarized

AbstractHot-carrier cooling processes of perovskite materials are typically described by a single parabolic band model that includes the effects of carrier-phonon scattering, hot phonon bottleneck, and Auger heating. However, little is known (if anything) about the cooling processes in which the spin-degenerate parabolic band splits into two spin-polarized bands, i.e., the Rashba band splitting effect. Here, we investigated the hot-carrier cooling processes for two slightly different compositions of two-dimensional Dion–Jacobson hybrid perovskites, namely, (3AMP)PbI4 and (4AMP)PbI4 (3AMP = 3-(aminomethyl)piperidinium; 4AMP = 4-(aminomethyl)piperidinium), using a combination of ultrafast transient absorption spectroscopy and first-principles calculations. In (4AMP)PbI4, upon Rashba band splitting, the spin-dependent scattering of hot electrons is responsible for accelerating hot-carrier cooling at longer delays. Importantly, the hot-carrier cooling of (4AMP)PbI4 can be extended by manipulating the spin state of the hot carriers. Our findings suggest a new approach for prolonging hot-carrier cooling in hybrid perovskites, which is conducive to further improving the performance of hot-carrier-based optoelectronic and spintronic devices.

scholarly journals Widely tunable cavity-enhanced ultrafast spectroscopy

2019 ◽  
Vol 205 ◽  
pp. 01024
Author(s):  
Myles C. Silfies ◽  
Yuning Chen ◽  
Henry Timmers ◽  
Abijith S. Kowligy ◽  
Alex Lind ◽  
...  
Keyword(s):  
Gas Phase ◽  
Absorption Spectroscopy ◽  
Ultrafast Spectroscopy ◽  
Transient Absorption ◽  
Transient Absorption Spectroscopy ◽  
Two Dimensional ◽  
Frequency Combs ◽  
Gas Phase Clusters ◽  
Uv Visible ◽  
Tunable Frequency

Generation of widely tunable frequency combs in the UV, visible, and infrared is discussed for use in cavity-enhanced transient absorption spectroscopy on gas-phase clusters. Progress towards cavity-enhanced two-dimensional spectroscopy is also presented.

scholarly journals Engineering of flat bands and Dirac bands in two-dimensional covalent organic frameworks (COFs): Relationships among molecular orbital symmetry, lattice symmetry, and electronic-structure characteristics

2022 ◽  
Author(s):  
Xiaojuan Ni ◽  
Hong Li ◽  
Feng Liu ◽  
Jean-Luc Bredas
Keyword(s):  
Electronic Structure ◽  
Molecular Orbital ◽  
Polymer Networks ◽  
Two Dimensional ◽  
Covalent Organic Frameworks ◽  
Orbital Symmetry ◽  
Structure Characteristics ◽  
Flat Bands ◽  
Lattice Symmetry ◽  
2D Polymer

Two-dimensional covalent organic frameworks (2D-COFs), also referred to as 2D polymer networks, display unusual electronic-structure characteristics, which can significantly enrich and broaden the fields of electronics and spintronics. In this...

UV Two-Dimensional Transient Absorption Spectroscopy

2012 ◽  
Author(s):  
Gerald Auböck ◽  
Cristina Consani ◽  
Frank van Mourik ◽  
Majed Chergui
Keyword(s):  
Absorption Spectroscopy ◽  
Transient Absorption ◽  
Transient Absorption Spectroscopy ◽  
Two Dimensional

scholarly journals Regulation of the luminescence mechanism of two-dimensional tin halide perovskites

2022 ◽  
Vol 13 (1) ◽  
Author(s):  
Tianju Zhang ◽  
Chaocheng Zhou ◽  
Xuezhen Feng ◽  
Ningning Dong ◽  
Hong Chen ◽  
...  
Keyword(s):  
Transient Absorption ◽  
Phonon Scattering ◽  
Potential Scattering ◽  
Transient Absorption Spectroscopy ◽  
Two Dimensional ◽  
Temperature Dependent ◽  
Control Engineering ◽  
Perovskite Materials ◽  
Halide Perovskites ◽  
Charged Defects

AbstractTwo-dimensional (2D) Sn-based perovskites are a kind of non-toxic environment-friendly luminescent material. However, the research on the luminescence mechanism of this type of perovskite is still very controversial, which greatly limits the further improvement and application of the luminescence performance. At present, the focus of controversy is defects and phonon scattering rates. In this work, we combine the organic cation control engineering with temperature-dependent transient absorption spectroscopy to systematically study the interband exciton relaxation pathways in layered A2SnI4 (A = PEA+, BA+, HA+, and OA+) structures. It is revealed that exciton-phonon scattering and exciton-defect scattering have different effects on exciton relaxation. Our study further confirms that the deformation potential scattering by charged defects, not by the non-polar optical phonons, dominates the excitons interband relaxation, which is largely different from the Pb-based perovskites. These results enhance the understanding of the origin of the non-radiative pathway in Sn-based perovskite materials.

scholarly journals Filling Exciton Trap-States in Two-Dimensional Tungsten Disulfide (WS2) and Diselenide (WSe2) Monolayers

Nanomaterials ◽  
2021 ◽  
Vol 11 (3) ◽  
pp. 770
Author(s):  
Zeynep Ezgi Eroglu ◽  
Dillon Contreras ◽  
Pouya Bahrami ◽  
Nurul Azam ◽  
Masoud Mahjouri-Samani ◽  
...  
Keyword(s):  
Transient Absorption ◽  
Decay Channel ◽  
Transition Metal Dichalcogenides ◽  
Tungsten Disulfide ◽  
Transient Absorption Spectroscopy ◽  
Two Dimensional ◽  
Trap States ◽  
Defect States ◽  
Femtosecond Transient Absorption ◽  
Exciton Decay

Two-dimensional transition metal dichalcogenides (2D-TMDs) hold a great potential to platform future flexible optoelectronics. The beating hearts of these materials are their excitons known as XA and XB, which arise from transitions between spin-orbit split (SOS) levels in the conduction and valence bands at the K-point. The functionality of 2D-TMD-based devices is determined by the dynamics of these excitons. One of the most consequential channels of exciton decay on the device functionality is the defect-assisted recombination (DAR). Here, we employ steady-state absorption and emission spectroscopies, and pump density-dependent femtosecond transient absorption spectroscopy to report on the effect of DAR on the lifetime of excitons in monolayers of tungsten disulfide (2D-WS2) and diselenide (2D-WSe2). These pump-probe measurements suggested that while exciton decay dynamics in both monolayers are driven by DAR, in 2D-WS2, defect states near the XB exciton fill up before those near the XA exciton. However, in the 2D-WSe2 monolayer, the defect states fill up similarly. Understanding the contribution of DAR on the lifetime of excitons and the partition of this decay channel between XA and XB excitons may open new horizons for the incorporation of 2D-TMD materials in future optoelectronics.

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