Nanomolding of Metastable Mo 4P3 Mehrdad T Kiania Quynh P Sama Gangtae Jina Betül Pamukb Hyeuk Jin Hanac James L. Harta J. R. Stauffd Judy J Chaa

2025-05-02 0 0 722.95KB 10 页 10玖币

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Nanomolding of Metastable Mo4P3

Mehrdad T Kiania, Quynh P Sama, Gangtae Jina, Betül Pamukb, Hyeuk Jin Hana,c, James L.

Harta, J. R. Stauffd, Judy J Chaa

a) Department of Materials Science and Engineering, Cornell University, Ithaca, NY,

14853, USA

b) School of Applied and Engineering Physics, Cornell University, Ithaca, NY 14853, USA

c) Department of Environment and Energy Engineering, Sungshin Women's University,

Seoul 01133, South Korea

d) Department of Mechanical Engineering and Materials Science, Yale University, New

Haven, CT, 06520, USA

Abstract

Reduced dimensionality leads to emergent phenomena in quantum materials and there is a

need for accelerated materials discovery of nanoscale quantum materials in reduced dimensions.

Thermomechanical nanomolding is a rapid synthesis method that produces high quality single-

crystalline quantum nanowires with controlled dimensions over wafer-scale sizes. Herein, we

apply nanomolding to fabricate nanowires from bulk feedstock of MoP, a triple-point topological

metal with extremely high conductivity that is promising for low-resistance interconnects.

Surprisingly, we obtained single-crystalline Mo4P3 nanowires, a metastable phase at room

temperature in atmospheric pressure. We thus demonstrate nanomolding can create metastable

phases inaccessible by other nanomaterial syntheses and can explore a previously inaccessible

synthesis space at high temperatures and pressures. Furthermore, our results suggest that the

current understanding of interfacial solid diffusion for nanomolding is incomplete, providing

opportunities to explore solid-state diffusion at high-pressure and high-temperature regimes in

confined dimensions.

Introduction

One-dimensional (1D) material systems display emergent phenomena due to reduced

dimensionality and nanoscale confinement not present in higher dimensions, such as dislocation

starvation in nanopillars1, deviations in crystallization in metallic glasses2, and ballistic transport

in 1D van der Waals crystals3. In the context of quantum materials, realizing topological

superconductors for probing Majorana bound states4, maximizing topological surface states for

low dissipation microelectronics5 or catalysis6, and developing Josephson junctions with unusual

current-phase relations7 all rely on pristine 1D nanowire systems. Given the large predicted

number of topological quantum materials8, there are limited nanofabrication techniques that allow

for simultaneous morphological, crystallographic, and structural control of 1D nanowires over

wafer-scale distances. Traditional bottom up fabrication techniques such as chemical vapor

deposition or molecular beam epitaxy require extensive optimization and yet control of size and

defect structure is limited, while top-down lithographic approaches can achieve the desired size

but lack any control of defect structure and are severely limited with respect to material choice9.

In 2019, Liu et al. introduced the scalable fabrication method of thermomechanical

nanomolding (TMNM), where a bulk polycrystalline feedstock material is extruded through a

nanoporous mold at elevated temperatures (approximately 0.5Tm, where Tm is the melting point)

and pressures (>100 MPa)10. This process results in formation of single-crystalline, defect-free

nanowires with high aspect ratios11. The mold is etched away using a strong acid or base, and the

molded nanowires are separated from the bulk feedstock via sonication. TMNM holds several key

advantages over traditional synthesis methods, including the ability to produce single-crystalline

nanostructures from a polycrystalline feedstock due to re-orientation of the grains as they are

pressed through the mold12. Another major advantage of TMNM is its versatility as the library of

successfully nanomolded materials has expanded to include crystalline metals13, solid solutions10,

and ordered phases14.

The use of TMNM for 1D quantum materials has been unexplored. One particular issue is

that many quantum materials of interest possess covalent bonding, such as metal-phosphides15–18.

Molybdenum-phosphides such as MoP16,19, MoP220,17, and MoP415 exhibit unique quantum

transport effects arising from topologically protected surface states and MoP, a triple point

topological metal21, is a promising alternative to Cu due to its high carrier density, high electron

mobility, and low bulk resistivity. In Mo-P compounds, metallic bonding exists between Mo

atoms; however, the shortest atomic bond distances are between covalently bonded Mo and P

atoms22. Previous TMNM studies focused on metals or intermetallics with largely metallic

bonding13,14, which can make bond rearrangement during solid-state diffusion easier while certain

covalently bonded materials such as Si are not suitable for TMNM given their extremely low bulk

and surface diffusivities14.

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NanomoldingofMetastableMo4P3MehrdadTKiania,QuynhPSama,GangtaeJina,BetülPamukb,HyeukJinHana,c,JamesL.Harta,J.R.Stauffd,JudyJChaaa)DepartmentofMaterialsScienceandEngineering,CornellUniversity,Ithaca,NY,14853,USAb)SchoolofAppliedandEngineeringPhysics,CornellUniversity,Ithaca,NY14853,USAc)DepartmentofEn...

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Nanomolding of Metastable Mo 4P3 Mehrdad T Kiania Quynh P Sama Gangtae Jina Betül Pamukb Hyeuk Jin Hanac James L. Harta J. R. Stauffd Judy J Chaa

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