Two-dimensional (2D) semiconductors provide a unique opportunity for optoelectronics due to their layered atomic structure, electronic and optical properties. To date, a majority of the application-oriented research in this field has been focused on fieldeffect electronics as well as photodetectors and light emitting diodes. Here we present a perspective on the use of 2D semiconductors for photovoltaic applications. We discuss photonic device designs that enable light trapping in nanometer-thickness absorber layers, and we also outline schemes for efficient carrier transport and collection. We further provide theoretical estimates of efficiency indicating that 2D semiconductors can indeed be competitive with and complementary to conventional photovoltaics, based on favorable energy bandgap, absorption, external radiative efficiency, along with recent experimental demonstrations. Photonic and electronic design of 2D semiconductor photovoltaics represents a new direction for realizing ultrathin, efficient solar cells with applications ranging from conventional power generation to portable and ultralight solar power. *Corresponding author: haa@caltech.eduKeywords: Transition metal dichalcogenides, heterostructures, light-trapping, ShockleyQuessier, nanophotonics, 2D materials Since the isolation of graphene as the first free-standing two-dimensional (2D) material (from graphite), the class of layered 2D materials with weak van der Waals inter-planar bonding has expanded significantly. Two-dimensional materials now span a great diversity of atomic structure and physical properties. Prominent among these are the semiconductor chalcogenides of transition and basic metals (Mo, W, Ga, In, Sn, Re etc.) 1-3 , as well as layered allotropes of other p-block elements of the periodic table such as P, As, Te etc. 4 The availability of atomic layer thickness samples of stable, passivated, and dangling bond free semiconductor materials ushers in a new phase in solid state device design and optoelectronics.1, 5-8 A notable feature of the metal chalcogenide 2D semiconductors is the transition from an indirect bandgap in bulk to direct bandgap (Eg) in monolayer form, resulting in a high photoluminescence quantum yield (PL QY) [9][10] in turn corresponding to high radiative efficiency. This combined with the bandgap ranging from visible to near infrared part of the spectrum (1.1 to 2.0 eV) 1 makes the chalcogenides

We report experimental measurements for ultrathin (<15 nm) van der Waals heterostructures exhibiting external quantum efficiencies exceeding 50% and show that these structures can achieve experimental absorbance >90%. By coupling electromagnetic simulations and experimental measurements, we show that pn WSe/MoS heterojunctions with vertical carrier collection can have internal photocarrier collection efficiencies exceeding 70%.

We demonstrate near-unity, broadband absorbing optoelectronic devices using sub-15 nm thick transition metal dichalcogenides (TMDCs) of molybdenum and tungsten as van der Waals semiconductor active layers. Specifically, we report that near-unity light absorption is possible in extremely thin (<15 nm) van der Waals semiconductor structures by coupling to strongly damped optical modes of semiconductor/metal heterostructures. We further fabricate Schottky junction devices using these highly absorbing heterostructures and characterize their optoelectronic performance. Our work addresses one of the key criteria to enable TMDCs as potential candidates to achieve high optoelectronic efficiency.

Harnessing photoexcited “hot” carriers in metallic nanostructures could define a new phase of non-equilibrium optoelectronics for photodetection and photocatalysis. Surface plasmons are considered pivotal for enabling efficient operation of hot carrier devices. Clarifying the fundamental role of plasmon excitation is therefore critical for exploiting their full potential. Here, we measure the internal quantum efficiency in photoexcited gold (Au)–gallium nitride (GaN) Schottky diodes to elucidate and quantify the distinct roles of surface plasmon excitation, hot carrier transport, and carrier injection in device performance. We show that plasmon excitation does not influence the electronic processes occurring within the hot carrier device. Instead, the metal band structure and carrier transport processes dictate the observed hot carrier photocurrent distribution. The excellent agreement with parameter-free calculations indicates that photoexcited electrons generated in ultra-thin Au nanostructures impinge ballistically on the Au–GaN interface, suggesting the possibility for hot carrier collection without substantial energy losses via thermalization.

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Van der Waals materials and heterostructures that manifest strongly bound exciton states at room temperature also exhibit emergent physical phenomena and are of great promise for optoelectronic applications. Here, we demonstrate that nanostructured, multilayer transition metal dichalcogenides (TMDCs) by themselves provide an ideal platform for excitation and control of excitonic modes, paving the way to exciton-photonics. Hence, we show that by patterning the TMDCs into nanoresonators, strong dispersion and avoided crossing of exciton, cavity photons and plasmon polaritons with effective separation energy exceeding 410 meV can be controlled with great precision. We further observe that inherently strong TMDC exciton absorption resonances may be completely suppressed due to excitation of hybrid light-matter states and their interference. Our work paves the way to the next generation of integrated exciton optoelectronic nano-devices and applications in light generation, computing, and sensing.

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One-way propagation of light, analogous to the directional flow of electrons in the presence of electric potential difference, has been an important goal in the wave–matter interaction. Breaking time-reversal symmetry in photonic flows is faced with challenges different from those for electron flows. In recent years several approaches and methods have been offered towards achieving this goal. Here we investigate another systematic approach to design all-passive relatively high-throughput metastructures that exhibit nonreciprocal properties and achieve wave-flow isolation. Moreover, we build on those findings and propose a paradigm for a quasi-two-dimensional metastructure that mimics the nonreciprocal property of Faraday rotation without using any magnetic or electric biasing. We envision that the proposed approaches may serve as a building block for all-passive time-reversal symmetry breaking with potential applications for future nonreciprocal systems and devices