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Title: Spatiotemporal Mapping of a Photocurrent Vortex in Monolayer MoS2 Using Diamond Quantum Sensors

Journal Article · · Physical Review. X
ORCiD logo [1]; ORCiD logo [2];  [3];  [2]; ORCiD logo [4];  [5]; ORCiD logo [6]
  1. Univ. of Chicago, IL (United States); Boston College, Chestnut Hill, MA (United States)
  2. Univ. of Chicago, IL (United States)
  3. Univ. of Chicago, IL (United States); Cornell Univ., Ithaca, NY (United States)
  4. Univ. of Chicago, IL (United States). James Franck Inst.
  5. Univ. of Chicago, IL (United States); Univ. of Chicago, IL (United States). James Franck Inst.
  6. Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States). Center for Molecular Engineering

Photocurrents are central to understanding and harnessing the interaction of light with matter. Here, we introduce a contact-free method to spatially resolve photocurrent distributions using proximal quantum magnetometers. We interface monolayer MoS2 with a near-surface ensemble of nitrogen-vacancy centers in diamond and map the generated photothermal current distribution through its magnetic-field profile. By synchronizing pulsed photoexcitation with dynamical decoupling of the sensor spin, we extend the sensor's quantum coherence and resolve time-dependent, two-dimensional current densities as small as 20 nA/mu m, with a projected sensitivity of 200 nA/mu m root Hz). Our spatially resolved measurements reveal that optical excitation can generate micron-sized photocurrent vortices in MoS2, manifesting a photo-Nernst effect exceeding that of gate-tuned graphene at comparable magnetic fields. We further probe the rise time of the photocurrents and show that thermal diffusion determines its spatial variation. These spatiotemporal capabilities establish an optically accessed, local probe for optoelectronic phenomena, ideally suited to the emerging class of two-dimensional materials, for which making contacts is challenging and can alter the intrinsic material properties.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
Air Force Office of Scientific Research (AFOSR); Air Force Research Laboratory (AFRL); National Science Foundation (NSF); US Army Research Office (ARO); US Office of Naval Research (ONR); USDOE
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1595950
Journal Information:
Physical Review. X, Journal Name: Physical Review. X Journal Issue: 1 Vol. 10; ISSN 2160-3308
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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