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Daniel A. Rhodes

Publications and source records attributed to Daniel A. Rhodes.

26 records · Page 2Linked to original sources

Highly Confined In-plane Exciton-Polaritons in Monolayer Semiconductors

2D materials support unique excitations of quasi-particles that consist of a material excitation and photons called polaritons. Especially interesting are in-plane propagating polaritons which can be confined to a single monolayer and carry large momentum. In this work, we report the existence of a new type of in-plane propagating polariton, supported on monolayer transition-metal-dicalcogonide (TMD) in the visible spectrum, which has not yet been observed. This 2D in-plane exciton-polariton (2DEP) is described by the coupling of an electromagnetic light field with the collective oscillations of the excitons supported by monolayer TMDs. We expose the specific experimental conditions required for the excitation of the 2DEP and show that these can be created if the TMD is encapsulated with hexagonal-boron-nitride (hBN) and cooled to cryogenic temperatures. In addition, we compare the properties of the 2DEPs with those of surface-plasmons-polaritons (SPPs) at the same spectral range, and find that the 2DEP exhibit over two orders-of-magnitude larger wavelength confinement. Finally, we propose two configurations for the possible experimental observation of 2DEPs.

physics.optics↗

Diffusivity Reveals Three Distinct Phases of Interlayer Excitons in MoSe2/WSe2 Heterobilayers

Charge separated interlayer excitons in transition metal dichalcogenide (TMDC) heterobilayers are being explored for moiré exciton lattices and exciton condensates. The presence of permanent dipole moments and the poorly screened Coulomb interaction make many body interactions particularly strong for interlayer excitons. Here we reveal two distinct phase transitions for interlayer excitons in the MoSe2/WSe2 heterobilayer using time and spatially resolved photoluminescence imaging: from trapped excitons in the moiré-potential to the modestly mobile exciton gas as exciton density increases to ne/h ~ 1011 cm-2 and from the exciton gas to the highly mobile charge separated electron/hole plasma for ne/h > 1012 cm-2. The latter is the Mott transition and is confirmed in photoconductivity measurements. These findings set fundamental limits for achieving quantum states of interlayer excitons.

cond-mat.mes-hall↗

Odd- and even-denominator fractional quantum Hall states in monolayer WSe$_2$

Monolayer (ML) semiconducting transition-metal dichalcogenides (TMDs) represent a unique class of two-dimensional (2D) electron systems. Their atomically thin structure -- just like graphene -- facilitates gate-tunability, while the sizable band gap and strong spin-orbit coupling hold promise for properties beyond graphene. Measurements under large magnetic fields have revealed an unusual LL structure, distinct from other 2D electron systems. However, owing to limited sample quality and poor electrical contact, probing the lowest Landau levels (LLs) has been challenging, and observation of electron correlations within the fractionally filled LLs regime has not been possible. Here, through bulk electronic compressibility measurements, we investigate the LL structure of ML WSe$_2$ in the extreme quantum limit, and observe fractional quantum Hall (FQH) states in the lowest three LLs. The odd-denominator FQH sequences demonstrate a systematic evolution with the LL orbital index, which has not been observed in any other system but is consistent with generic theoretical expectations. In addition, we observe an even-denominator state in the second LL that is expected to host non-Abelian statistics. Our results suggest that the 2D semiconductors can provide an experimental platform that closely resembles idealized theoretical models in the quantum Hall regime.

cond-mat.mes-hall↗

Imaging strain-localized exciton states in nanoscale bubbles in monolayer WSe2 at room temperature

In monolayer transition metal dichalcogenides, quantum emitters are associated with localized strain that can be deterministically applied to create designer nano-arrays of single photon sources. Despite an overwhelming empirical correlation with local strain, the nanoscale interplay between strain, excitons, defects and local crystalline structure that gives rise to these quantum emitters is poorly understood. Here, we combine room-temperature nano-optical imaging and spectroscopy of excitons in nanobubbles of localized strain in monolayer WSe2 with atomistic structural models to elucidate how strain induces nanoscale confinement potentials that give rise to highly localized exciton states in 2D semiconductors. Nano-optical imaging of nanobubbles in low-defect monolayers reveal localized excitons on length scales of approximately 10 nm at multiple sites along the periphery of individual nanobubbles, which is in stark contrast to predictions of continuum models of strain. These results agree with theoretical confinement potentials that are atomistically derived from measured topographies of existing nanobubbles. Our results provide one-of-a-kind experimental and theoretical insight of how strain-induced confinement - without crystalline defects - can efficiently localize excitons on length scales commensurate with exciton size, providing key nanoscale structure-property information for quantum emitter phenomena in monolayer WSe2.

cond-mat.mes-hall↗

Magic continuum in twisted bilayer WSe2

Emergent quantum phases driven by electronic interactions can manifest in materials with narrowly dispersing, i.e. "flat", energy bands. Recently, flat bands have been realized in a variety of graphene-based heterostructures using the tuning parameters of twist angle, layer stacking and pressure, and resulting in correlated insulator and superconducting states. Here we report the experimental observation of similar correlated phenomena in twisted bilayer tungsten diselenide (tWSe2), a semiconducting transition metal dichalcogenide (TMD). Unlike twisted bilayer graphene where the flat band appears only within a narrow range around a "magic angle", we observe correlated states over a continuum of angles, spanning 4 degree to 5.1 degree. A Mott-like insulator appears at half band filling that can be sensitively tuned with displacement field. Hall measurements supported by ab initio calculations suggest that the strength of the insulator is driven by the density of states at half filling, consistent with a 2D Hubbard model in a regime of moderate interactions. At 5.1 degree twist, we observe evidence of superconductivity upon doping away from half filling, reaching zero resistivity around 3 K. Our results establish twisted bilayer TMDs as a model system to study interaction-driven phenomena in flat bands with dynamically tunable interactions.

cond-mat.mes-hall↗

Near-unity light absorption in a monolayer WS2 van der Waals heterostructure cavity

Excitons in monolayer transition-metal-dichalcogenides (TMDs) dominate their optical response and exhibit strong light-matter interactions with lifetime-limited emission. While various approaches have been applied to enhance light-exciton interactions in TMDs, the achieved strength have been far below unity, and a complete picture of its underlying physical mechanisms and fundamental limits has not been provided. Here, we introduce a TMD-based van der Waals heterostructure cavity that provides near-unity excitonic absorption, and emission of excitonic complexes that are observed at ultra-low excitation powers. Our results are in full agreement with a quantum theoretical framework introduced to describe the light-exciton-cavity interaction. We find that the subtle interplay between the radiative, non-radiative and dephasing decay rates plays a crucial role, and unveil a universal absorption law for excitons in 2D systems. This enhanced light-exciton interaction provides a platform for studying excitonic phase-transitions and quantum nonlinearities and enables new possibilities for 2D semiconductor-based optoelectronic devices.

physics.optics↗

Trion Species-Resolved Quantum Beats in MoSe2

Monolayer photonic materials offer a tremendous potential for on-chip optoelectronic devices. Their realization requires knowledge of optical coherence properties of excitons and trions that have so far been limited to nonlinear optical experiments carried out with strongly inhomogenously broadened material. Here we employ h-BN encapsulated and electrically gated MoSe2 to reveal coherence properties of trion-species directly in the linear optical response. Autocorrelation measurements reveal long dephasing times up to T2=1.16+-0.05 ps for positively charged excitons. Gate dependent measurements provide evidence that the positively-charged trion forms via spatially localized hole states making this trion less prone to dephasing in the presence of elevated hole carrier concentrations. Quantum beat signatures demonstrate coherent coupling between excitons and trions that have a dephasing time up to 0.6 ps, a two-fold increase over those in previous reports. A key merit of the prolonged exciton/trion coherences is that they were achieved in a linear optical experiment, and thus are directly relevant to applications in nanolasers, coherent control, and on-chip quantum information processing requiring long photon coherence.

cond-mat.mes-hall↗

Non-stoichiometry and Defects in the Weyl Semimetals TaAs, TaP, NbP, and NbAs

We report a structural study of the Weyl semimetals TaAs, TaP, NbP, and NbAs, utilizing diffraction techniques (single crystal x-ray diffraction and energy dispersive spectroscopy) and imaging techniques (transmission electron microscopy/scanning transmission electron microscopy). We observe defects of various degrees, leading to non-stoichiometric single crystals of all four semimetals. While TaP displays a large pnictide deficiency with composition TaP$_{0.83(3)}$, and stacking faults accompanied by anti-site disorder and site vacancies, TaAs displays transition metal deficiency with composition Ta$_{0.92(2)}$As and a high density of stacking faults. NbP also displays pnictide deficiency, yielding composition NbP$_{0.95(2)}$, and lastly, NbAs display very little deviation from a 1:1 composition, NbAs$_{1.00(3)}$, and is therefore recommended to serve as the model compound for these semimetals.

cond-mat.mtrl-sci↗