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Register a new userAmbient Effects on Photogating in MoS2 Photodetectors
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Atomically thin transition metal dichalcogenides (TMDs) are ideal candidates for ultrathin optoelectronics that is flexible and semitransparent. Photodetectors based on TMDs show remarkable performance, with responsivity and detectivity higher than 10^3 A/W and 10^12 Jones, respectively, but they are plagued by response times as slow as several tens of seconds. Although it is well established that gas adsorbates such as water and oxygen create charge traps and significantly increase both the responsivity and the response time, the underlying mechanism is still unclear. Here we study the influence of adsorbates on MoS2 photodetectors under ambient conditions, vacuum and illumination at different wavelengths. We show that, for wavelengths sufficiently short to excite electron-hole pairs in the MoS2, light illumination causes desorption of water and oxygen molecules. The change in the molecular gating provided by the physisorbed molecules is the dominant contribution to the device photoresponse in ambient conditions.
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Adsorbate engineering is a promising route for controlling the electronic properties of monolayer transition-metal dichalcogenide materials. Here, we study shallow bound states induced by charged adatoms on MoS$_2$ using large-scale tight-binding simulations with screened adatom potentials obtained from ab initio calculations. The interplay of unconventional screening in two-dimensional systems and multivalley effects in the transition-metal dichalcogenide (TMDC) band structure results in a rich diversity of bound impurity states. We present results for impurity state wavefunctions and energies, as well as for the local density of states in the vicinity of the adatom which can be measured using scanning tunnelling spectroscopy. We find that the presence of several distinct valleys in the MoS$_2$ band structure gives rise to crossovers of impurity states at critical charge strengths, altering the orbital character of the most strongly bound state. We compare our results to simpler methods, such as the 2D hydrogen atom and effective mass theory, and we discuss limitations of these approaches.
Interactions between two excitons can result in the formation of bound quasiparticles, known as biexcitons. Their properties are determined by the constituent excitons, with orbital and spin states resembling those of atoms. Monolayer transition metal dichalcogenides (TMDs) present a unique system where excitons acquire a new degree of freedom, the valley pseudospin, from which a novel intervalley biexciton can be created. These biexcitons comprise two excitons from different valleys, which are distinct from biexcitons in conventional semiconductors and have no direct analogue in atomic and molecular systems. However, their valley properties are not accessible to traditional transport and optical measurements. Here, we report the observation of intervalley biexcitons in the monolayer TMD MoS2 using ultrafast pump-probe spectroscopy. By applying broadband probe pulses with different helicities, we identify two species of intervalley biexcitons with large binding energies of 60 meV and 40 meV. In addition, we also reveal effects beyond biexcitonic pairwise interactions in which the exciton energy redshifts at increasing exciton densities, indicating the presence of many-body interactions among them.
We present flexible photodetectors (PDs) for visible wavelengths fabricated by stacking centimetre-scale chemical vapour deposited (CVD) single layer graphene (SLG) and single layer CVD MoS2, both wet transferred onto a flexible polyethylene terephthalate substrate. The operation mechanism relies on injection of photoexcited electrons from MoS2 to the SLG channel. The external responsivity is 45.5A/W and the internal 570A/W at 642nm. This is at least two orders of magnitude higher than bulk-semiconductor flexible membranes and other flexible PDs based on graphene and layered materials. The photoconductive gain is up to 4x10^5. The photocurrent is in the 0.1-100 uA range. The devices are semi-transparent, with just 8% absorption at 642nm and work stably upon bending to a curvature of 6cm. These capabilities and the low voltage operation (<1V) make them attractive for wearable applications.
Graphene is an ideal material for hot-electron bolometers, due to its low heat capacity and weak electron-phonon coupling. Nanostructuring graphene with quantum dot constrictions yields detectors with extraordinarily high intrinsic responsivity, higher than 1x10^9 V/W at 3K. The sensing mechanism is bolometric in nature: the quantum confinement gap causes a strong dependence of the electrical resistance on the electron temperature. Here we show that this quantum confinement gap does not impose a limitation on the photon energy for light detection and these quantum dot bolometers work in a very broad spectral range, from terahertz, through telecom to ultraviolet radiation, with responsivity independent of wavelength. We also measure the power dependence of the response. Although the responsivity decreases with increasing power, it stays higher than 1x10^8 V/W in a wide range of absorbed power, from 1 pW to 0.4 nW.
The discovery of graphene has put the spotlight on other layered materials including transition metal dichalcogenites (TMD) as building blocks for novel heterostructures assembled from stacked atomic layers. Molybdenum disulfide, MoS2, a semiconductor in the TMD family, with its remarkable thermal and chemical stability and high mobility, has emerged as a promising candidate for post-silicon applications such as switching, photonics, and flexible electronics. Since these rely on controlling the position of the Fermi energy (EF), it is crucial to understand its dependence on doping and gating. Here we employed scanning tunneling microscopy (STM) and spectroscopy (STS) with gating capabilities to measure the bandgap and the position of EF in MoS2, and to track its evolution with gate voltage. For bulk samples, the measured bandgap (~1.3eV) is comparable to the value obtained by photoluminescence, and the position of EF (~0.35eV) below the conduction band, is consistent with n-doping reported in this material. Using topography together with spectroscopy we traced the source of the n-doping in bulk MoS2 samples to point defects, which we attribute to S vacancies. In contrast, for thin films deposited on SiO2, we found significantly higher levels of n-doping that cannot be attributed to S vacancies. By combining gated STS with transport measurements in a field effect transistor (FET) configuration, we demonstrate that the higher levels of n-doping in thin film samples is due to charge traps at the sample-substrate interface.
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