2024 New's Items

Theory of mechanical exfoliation of van der Waals bonded layered materials

Sun H
Sahin O
Javey A
Ager JW
Chrzan DC
2024

A theoretical framework for analyzing the mechanical exfoliation of 2D materials at finite temperature is introduced. As an example, this framework, based on transition-state theory and calculation of the reaction pathway, is applied to the mechanical exfoliation of multilayer MoS2. The theory predicts that altering the bonding of the top layer to the bulk through straining or twisting and slowly exfoliating at low temperatures will enhance the yield of the monolayer material.

Ion diffusion retarded by diverging chemical susceptibility

Cai Y
Wang Z
Wan J
Li J
Guo R
Ager JW
Javey A
Zheng H
Jiang J
Wu J
2024

For first-order phase transitions, the second derivatives of Gibbs free energy (specific heat and compressibility) diverge at the transition point, resulting in an effect known as super-elasticity along the pressure axis, or super-thermicity along the temperature axis. Here we report a chemical analogy of these singularity effects along the atomic doping axis, where the second derivative of Gibbs free energy (chemical susceptibility) diverges at the transition point, leading to an anomalously high energy barrier for dopant diffusion in co-existing phases, an effect we coin as super-...

Meter-scale van der Waals films manufactured via one-step roll printing

Lee K
Higashitarumizu N
Wang S
Kim C
Ho CY
Oh JW
Zan G
Madsen M
Lee TW
Chrzan DC
Park C
2024

A weak van der Waals (vdW) force in layered materials enables their isolation into thin flakes through mechanical exfoliation while sustaining their intrinsic electronic and optical properties. Here, we introduce a universal roll-printing method capable of producing vdW multilayer films on wafer-to-meter scale. This process uses sequential exfoliation and transfer of layered materials from the powder sources to target substrates through a repeated rolling of a cylindrical metal drum. We achieve uniformly coated films with a library of vdW powders on various mechanically rigid and...

Direct Heterogeneous Integration of Molybdenum Disulfide via Spin-on Molecular Chemistry

Balushi ZA
Im H
Gupta A
Lu D
Buckingham M
Ma K
Nemsak S
Higashitarumizu N
Rahman IR
Liang J
Wan J
2024
Two-dimensional (2D) semiconductors, such as molybdenum disulfide (MoS2), are emerging as key materials for next-generation electronics, addressing challenges in the miniaturization of silicon-based technologies. Despite progress in scaling-up 2D materials, integrating them into functional devices remains challenging, particularly in the context of three-dimensional integration. Here, we present a scalable method for growing high-quality mono- to few-layer MoS2 on large wafers using a spin-on precursor, molybdenum ethyl xanthate. This approach facilitates the formation of a metastable...

Black Phosphorus for Mid-Infrared Optoelectronics: Photophysics, Scalable Processing, and Device Applications

Higashitarumizu N
Wang S
Wang S
Kim H
Bullock J
Javey A
2024

High efficiency mid-infrared (λ = 3–8 μm) light emitters and photodetectors are pivotal for advancing next-generation optoelectronics. However, narrow-bandgap semiconductors face fundamental challenges such as pronounced nonradiative carrier recombination and thermally generated noise, which impede device performance. Recently, two-dimensional layered black phosphorus (BP) and its alloys have attracted substantial interest for mid-infrared device applications, demonstrating superior performance relative to conventional III–V and II–VI semiconductors with similar bandgaps. In this review,...

Low Contact Resistance WSe2 p-Type Transistors with Highly Stable, CMOS-Compatible Dopants

Kim I
Higashitarumizu N
Rahman IR
Wang S
Kim HM
Geng J
Prabhakar RR
Ager III JW
Javey A
2024

High contact resistance has been a bottleneck in developing high-performance transition-metal dichalcogenide (TMD) based p-type transistors. We report degenerately doped few-layer WSe2 transistors with contact resistance as low as 0.23 ± 0.07 kΩ·μm per contact by using platinum(IV) chloride (PtCl4) as the p-type dopant, which is composed of ions compatible with the complementary metal-oxide-semiconductor (CMOS) fabrication process. Top-gated devices with a gate length of 200 nm showed good switching behaviors, implying that the dopant diffusion into the gate stack...

Colloidal Dispersions of Sterically and Electrostatically Stabilized PbS Quantum Dots: Structure Factors, Second Virial Coefficients, and Film-Forming Properties

Ahhyun Jeong
Joshua Portner
Christian P. N. Tanner
Justin C. Ondry
Chenkun Zhou
Zehan Mi
Youssef A. Tazoui
Byeongdu Lee
Vivian R. K. Wall
Naomi S. Ginsberg
Dmitri V. Talapin
2024

Electrostatically stabilized nanocrystals (NCs) and, in particular, quantum dots (QDs) hold promise for forming strongly coupled superlattices due to their compact and electronically conductive surface ligands. However, studies of the colloidal dispersion and interparticle interactions of electrostatically stabilized sub-10 nm NCs have been limited, hindering the optimization of their colloidal stability and self-assembly. In this study, we employed small-angle X-ray scattering (SAXS) experiments to investigate the interparticle interactions and arrangement of PbS QDs with thiostannate...

Reversible Electron-Beam Patterning of Colloidal Nanoparticles at Fluid Interfaces

Jonathan G. Raybin
Ethan J. Dunsworth
Veronica Guo
Naomi S. Ginsberg
2024

The directed self-assembly of colloidal nanoparticles (NPs) using external fields guides the formation of sophisticated hierarchical materials but becomes less effective with decreasing particle size. As an alternative, electron-beam-driven assembly offers a potential avenue for targeted nanoscale manipulation, yet remains poorly controlled due to the variety and complexity of beam interaction mechanisms. Here, we investigate the beam–particle interaction of silica NPs pinned to the fluid–vacuum interface of ionic liquid droplets. In these experiments, scanning electron microscopy of...

Anion and Cation Migration at 2D/3D Halide Perovskite Interfaces

R. F. Moral
C. A. R. Perini
T. Kodalle
A. Kim
F. Babbe
N. Harada
J. Hajhemati
P. Schulz
N. S. Ginsberg
S. Aloni
C. P. Schwartz
J. P. Correa-Baena
C. M. Sutter-Fella
2024

This study explores the ionic dynamics in 2D/3D perovskite solar cells, which are known for their improved efficiency and stability. The focus is on the impact of halide choice in 3D perovskites treated with phenethylammonium halide salts (PEAX, X = Br and I). Our findings reveal that light and heat drive ionic migration in these structures, with PEA+ species diffusing into the 3D film in PEABr-treated samples. Mixed-halide 3D perovskites show halide interdiffusion, with bromine migrating to the surface and iodine diffusing into the film. Cathodoluminescence microscopy reveals...

In Situ Coherent X-ray Scattering Reveals Polycrystalline Structure and Discrete Annealing Events in Strongly-Coupled Nanocrystal Superlattices

M. J. Hurley*
C. P. T. Tanner*
J. Portner
J. K. Utterback
I. Coropceanu
A. Das, J. D. Slivka
A. Fluerasu
Y. Sun, S. Song
L. M. Hamerlynck
A. H. Miller
P. Bhattacharyya
D. V. Talapin
G. J. Williams
G. J. Williams
S. W. Teitelbaum
2024

Solution-phase bottom up self-assembly of nanocrystals into superstructures such as ordered superlattices is an attractive strategy to generate functional materials of increasing complexity, including very recent advances that incorporate strong interparticle electronic coupling. While the self-assembly kinetics in these systems have been elucidated and related to the product characteristics, the weak interparticle bonding interactions suggest the superstructures formed could continue to order within the solution long after the primary nucleation and growth have occurred, even though...