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Motional narrowing implies narrowing induced by motion, for example, in nuclear resonance, the thermally induced random motion of the nuclei in an inhomogeneous environment leads to counter-intuitive narrowing of the resonance line. Similarly, the excitons in monolayer semiconductors experience magnetic inhomogeneity: the electron-hole spin-exchange interaction manifests as an in-plane pseudo-magnetic field with a periodically varying orientation inside the exciton band. The excitons undergo random momentum scattering and pseudospin precession repeatedly in this inhomogeneous magnetic environment - typically resulting in fast exciton depolarization. On the contrary, we show that such magnetic inhomogeneity averages out at high scattering rate due to motional narrowing. Physically, a faster exciton scattering leads to a narrower pseudospin distribution on the Bloch sphere, implying a nontrivial improvement in exciton polarization. The in-plane nature of the pseudo-magnetic field enforces a contrasting scattering dependence between the circularly and linearly polarized excitons - providing a spectroscopic way to gauge the sample quality., Comment: Accepted in Nano Letters

In the recent past, significant research efforts have been put forth to fabricate low-cost noble metal-free substrates for surface-enhanced Raman spectroscopy (SERS) applications. Here we propose semiconducting TiO2 multi-leg nanotubes (TiO2 MLNTs, with and without the gold nanoparticle coating) as SERS substrates. TiO2 MLNTs show unique multi-leg morphology compared to the conventional non-multi-leg tubes and possess better light-harvesting properties. TiO2 MLNTs are fabricated with a simple and versatile single-step electrochemical anodization method. Remarkable high SERS sensitivity is observed towards the detection of Methylene blue (MB), up to nM concentration (E.F. ~104). The same is attributed to the resonantly matched photonic absorption edge of TiO2 MLNTs with the wavelength of incident laser probe light. On the other hand, gold nanoparticle-coated TiO2 MLNTs demonstrated further enhancement in SERS sensitivity (E.F. ~105, for nM of MB) facilitated by the synergy that exists between the plasmonic modes (LSPRs) of Au and the photonic absorption mode of TiO2 MLNTs.

The broadening and polarization of excitonic luminescence in monolayer TMDs largely suffer from inhomogeneity and temperature - an unresolved problem to date. In this work, through few-layer-graphene encapsulation of monolayer WS$_2$, we reduce the inter-excitonic energy separation, which then can have a narrow resonance with a specific phonon mode of our choice. The resulting single-step exciton relaxation with the resonating phonon mode significantly suppresses the inhomogeneous broadening, allowing us to achieve the narrowest exciton linewidth of 1.06 meV (which translates to 0.19 meV after deconvolution with the excitation laser linewidth). The single-phonon resonance helps to achieve a high quantum efficiency despite graphene encapsulation. The technique is powerful in tuning the exciton polarization during relaxation by choosing a specific resonating phonon mode. For example, the valley coherence (polarization) improves from $\sim$68% ($\sim$40%) to $\sim$90% ($\sim$75%) on resonance with 2$A_1$' and $A_1$' modes respectively. We further demonstrate a strong polarization reversal on resonance with a chiral phonon mode. Strikingly, the above features remain robust against temperature (up to 200 K) and sample age (few months in ambient condition). The findings will lead to clean excitonic measurements without requiring cryogenic cooling.

Strong Coulomb interaction in monolayer semiconductors allows them to host optically active large many-body states, such as the five-particle state, charged biexciton. Strong nonlinear light absorption by the charged biexciton under spectral resonance, coupled with its charged nature, makes it intriguing for nonlinear photodetection - an area that is hitherto unexplored. Using the high built-in vertical electric field in an asymmetrically designed few-layer graphene encapsulated 1L-WS$_2$ heterostructure, here we report a large, highly nonlinear photocurrent arising from the strong absorption by two charged biexciton species under zero external bias (self-powered mode). Time-resolved measurement reveals that the generated charged biexcitons transfer to the few-layer graphene in a timescale of sub-5 ps, indicating an ultrafast intrinsic limit of the photoresponse. By using single- and two-color photoluminescence excitation spectroscopy, we show that the two biexcitonic peaks originate from bright-dark and bright-bright exciton-trion combinations. Such innate nonlinearity in the photocurrent due to its biexcitonic origin, coupled with the ultrafast response due to swift inter-layer charge transfer, exemplifies the promise of manipulating many-body effects in monolayers towards viable optoelectronic applications.

Strong Coulomb interaction in monolayer transition metal dichalcogenides can facilitate nontrivial many-body effects among excitonic complexes. Many-body effects like exciton-exciton annihilation (EEA) have been widely explored in this material system. However, a similar effect for charged excitons (or trions), that is, trion-trion annihilation (TTA), is expected to be relatively suppressed due to repulsive like-charges, and has not been hitherto observed in such layered semiconductors. By a gate-dependent tuning of the spectral overlap between the trion and the charged biexciton through an "anti-crossing"-like behaviour in monolayer WS$_2$, here we present an experimental observation of an anomalous suppression of the trion emission intensity with an increase in gate voltage. The results strongly correlate with time-resolved measurements, and are inferred as a direct evidence of a nontrivial TTA resulting from non-radiative Auger recombination of a bright trion, and the corresponding energy resonantly promoting a dark trion to a charged biexciton state. The extracted Auger coefficient for the process is found to be tunable ten-fold through a gate-dependent tuning of the spectral overlap.

The monolayers of semiconducting transition metal dichalcogenides host strongly bound excitonic complexes and are an excellent platform for exploring many-body physics. Here we demonstrate a controlled kinetic manipulation of the five-particle excitonic complex, the charged biexciton, through a systematic dependence of the biexciton peak on excitation power, gate voltage, and temperature using steady-state and time-resolved photoluminescence (PL). With the help of a combination of the experimental data and a rate equation model, we argue that the binding energy of the charged biexciton is less than the spectral separation of its peak from the neutral exciton. We also note that while the momentum-direct radiative recombination of the neutral exciton is restricted within the light cone, such restriction is relaxed for a charged biexciton recombination due to the presence of near-parallel excited and final states in the momentum space.

Moir\'e superlattice-induced sub-bands in twisted van der Waals homo- and hetero-structures govern their optical and electrical properties, rendering additional degrees of freedom such as twist angle. Here, we demonstrate the moir\'e superlattice effects on the intralayer excitons and trions in a twisted bilayer of MoS$_2$ of H-type stacking at marginal twist angles. We identify the emission from localized and multiple delocalized sub-bands of intralayer moir\'e excitons and show their electrical modulation by the corresponding trion formation. The electrical control of the oscillator strength of the moir\'e excitons also results in a strong tunability of resonant Raman scattering. We find that the gate-induced doping significantly modulates the electronic moir\'e potential, however leaves the excitonic moir\'e confinement unaltered. This effect, coupled with variable moir\'e trap filling by tuning the optical excitation density, allows us to delineate the different phases of localized and delocalized moir\'e trions. We demonstrate that the moir\'e excitons exhibit strong valley coherence that changes in a striking non-monotonic W-shape with gating due to motional narrowing. These observations from the simultaneous electrostatic control of quasiparticle-dependent moir\'e potential will lead to exciting effects of tunable many-body phenomena in moir\'e superlattices.

Medical professionals evaluating alternative treatment plans for a patient often encounter time varying confounders, or covariates that affect both the future treatment assignment and the patient outcome. The recently proposed Counterfactual Recurrent Network (CRN) accounts for time varying confounders by using adversarial training to balance recurrent historical representations of patient data. However, this work assumes that all time varying covariates are confounding and thus attempts to balance the full state representation. Given that the actual subset of covariates that may in fact be confounding is in general unknown, recent work on counterfactual evaluation in the static, non-temporal setting has suggested that disentangling the covariate representation into separate factors, where each either influence treatment selection, patient outcome or both can help isolate selection bias and restrict balancing efforts to factors that influence outcome, allowing the remaining factors which predict treatment without needlessly being balanced., Comment: Accepted in Workshop on "The Neglected Assumptions in Causal Inference" at ICML 2021 (July)

In monolayer transition metal dichalcogenide semiconductors, valley coherence degrades rapidly due to a combination of fast scattering and inter-valley exchange interaction. This leads to a sub-picosecond valley coherence time, making coherent manipulation of exciton a highly challenging task. Using monolayer MoS2 sandwiched between top and bottom graphene, here we demonstrate fully valley coherent excitons by observing ~100% degree of linear polarization in steady state photoluminescence. This is achieved in this unique design through a combined effect of (a) suppression in exchange interaction due to enhanced dielectric screening, (b) reduction in exciton lifetime due to a fast inter-layer transfer to graphene, and (c) operating in the motional narrowing regime. We disentangle the role of the key parameters affecting valley coherence by using a combination of calculation (solutions of Bethe-Salpeter and Maialle-Silva-Sham equations) and a careful choice of design of experiments using four different stacks with systematic variation of screening and exciton lifetime. To the best of our knowledge, this is the first report in which the excitons are found to be valley coherent in the entire lifetime in monolayer semiconductors, allowing optical readout of valley coherence possible.