Stacking Mode-Driven Enhancement of Optoelectronic and Electrocatalytic Properties in Bilayer 2H MoS<sub>2</sub>

The stacking orientation of bilayer two-dimensional (2D) materials introduces an additional degree of freedom that can profoundly influence their electronic, optoelectronic, and electrochemical properties. While stacking-engineered phenomena such as ferroelectricity, superconductivity, and second harmonic generation have been widely studied in bilayer molybdenum disulfide (MoS<sub>2</sub>), their impact on functional device performance, particularly photoresponse and electrocatalysis, remains largely unexplored. Here, we investigate how the stacking configuration governs the optoelectronic and electrocatalytic behavior of bilayer MoS<sub>2</sub>, focusing on the two stable stacking orders: 2H and 3R synthesized via chemical vapor deposition (CVD). Photodetection measurements reveal that 2H stacked bilayer MoS<sub>2</sub> exhibits a remarkable two-orders-of-magnitude enhancement in photoresponsivity over its 3R counterpart, attributed to stronger interlayer coupling and more efficient charge transfer. Additionally, 2H MoS<sub>2</sub> demonstrates enhanced field-effect transistor (FET) characteristics and achieves twice the hydrogen evolution reaction (HER) activity compared to 3R MoS<sub>2</sub>. We employ scanning electrochemical cell microscopy (SECCM) to achieve spatially resolved mapping of electrocatalytic reactivity, offering the first direct nanoscale visualization of stacking-dependent HER activity. These findings underscore the crucial role of stacking orientation of atomic layers in tuning both optoelectronic and electrocatalytic properties, paving the way for stacking-engineered 2D materials in next-generation photodetectors and electrocatalytic devices.

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Publication Details

Journal
ACS Applied Materials & Interfaces
Published
2025-08-12
DOI
https://doi.org/10.1021/acsami.5c11713
Citations
2
Primary Topic
2D Materials and Applications
Type
article
Field-Weighted Citation Impact
1.04

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article

Stacking Mode-Driven Enhancement of Optoelectronic and Electrocatalytic Properties in Bilayer 2H MoS2

Irfan Haider Abidi, Jani Kotakoski, Cameron L. Bentley, Yuerui Lu et al.
2 citations
ACS Applied Materials & Interfaces
2D Materials and Applications
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article

Stacking Mode-Driven Enhancement of Optoelectronic and Electrocatalytic Properties in Bilayer 2H MoS2

Irfan Haider Abidi, Jani Kotakoski, Cameron L. Bentley, Yuerui Lu, N. Dissanayake, Sunil Singh Kushvaha, Enrico Della Gaspera, Vishnu Aggarwal, Pargam Vashishtha, Salvy P. Russo, Ajay Kumar Verma, Sumeet Walia, Jeffrey A. Davis, Jonathan O. Tollerud, Majid Panahandeh‐Fard, Jianfeng Mao, Balaji Kannan, Taimur Ahmed, Manoj Sehrawat, Sindhu Priya Giridhar, Clara Kofler, T. K. Gupta, Jake Limb
article en
2 citations

Abstract

The stacking orientation of bilayer two-dimensional (2D) materials introduces an additional degree of freedom that can profoundly influence their electronic, optoelectronic, and electrochemical properties. While stacking-engineered phenomena such as ferroelectricity, superconductivity, and second harmonic generation have been widely studied in bilayer molybdenum disulfide (MoS<sub>2</sub>), their impact on functional device performance, particularly photoresponse and electrocatalysis, remains largely unexplored. Here, we investigate how the stacking configuration governs the optoelectronic and electrocatalytic behavior of bilayer MoS<sub>2</sub>, focusing on the two stable stacking orders: 2H and 3R synthesized via chemical vapor deposition (CVD). Photodetection measurements reveal that 2H stacked bilayer MoS<sub>2</sub> exhibits a remarkable two-orders-of-magnitude enhancement in photoresponsivity over its 3R counterpart, attributed to stronger interlayer coupling and more efficient charge transfer. Additionally, 2H MoS<sub>2</sub> demonstrates enhanced field-effect transistor (FET) characteristics and achieves twice the hydrogen evolution reaction (HER) activity compared to 3R MoS<sub>2</sub>. We employ scanning electrochemical cell microscopy (SECCM) to achieve spatially resolved mapping of electrocatalytic reactivity, offering the first direct nanoscale visualization of stacking-dependent HER activity. These findings underscore the crucial role of stacking orientation of atomic layers in tuning both optoelectronic and electrocatalytic properties, paving the way for stacking-engineered 2D materials in next-generation photodetectors and electrocatalytic devices.

ACS Applied Materials & InterfacesVol. 17(34)
Australian National University (AU), University of Vienna (AT), La Trobe University (AU), Australian Regenerative Medicine Institute (AU), IEEE Computer Society (US), Optical Sciences (United States) (US), Monash University (AU), Swinburne University of Technology (AU), Council of Scientific and Industrial Research (IN), RMIT University (AU), Academy of Scientific and Innovative Research (IN)
Austrian Science Fund, Australian Research Council, Office of National Intelligence
Affordable and clean energy
Openalex Percentile: Top 23%
2D Materials and Applications
1.04
DOISourceOpenAlex
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