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Tony Heinz

Publications and source records attributed to Tony Heinz.

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A cryogenic apparatus for coupling two-dimensional materials to a confocal multimode optical cavity

Two-dimensional van der Waals materials exhibit a variety of correlated electron phases, and optical driving offers a promising route toward manipulating them. For example, cavity-enhanced, continuous-wave (CW) Raman excitation has been suggested as a way to coherently and superradiantly populate phonons or charge density waves via material excitons. A steady-state phonon population may be sustained with sufficiently strong electron-phonon coupling to drive novel collective response. We describe an apparatus built to meet the requirements of such an experimental program: Namely, an ultrahigh-vacuum system housing a length-tunable confocal Fabry-P\'{e}rot cavity with an intracavity sample, both cryogenically cooled and stabilized against vibrations. A four-axis nanopositioner aligns the sample and supports electrical leads for sample carrier density modulation and transport measurements. Transmission through the multimode cavity enables in situ sample imaging for alignment; the sample is a transition metal dichalcogenide in this work. Operating near the confocal geometry concentrates the optical field into a localized supermode that substantially enhances light-matter coupling. This enhancement is preserved despite the millimeter-scale cavity length, which provides room for sample alignment and exchange.

quant-ph

Long-Range Fermi-Polaron Blockade in Monolayer MoSe$_2$

Strong optical nonlinearities at the few-photon level are a central goal for quantum photonics, yet they remain difficult to realize in solid-state systems. In doped two-dimensional semiconductors, coupling between excitons and a degenerate Fermi sea gives rise to exciton-Fermi polarons, many-body quasiparticles whose optical response is governed by fermionic correlations. Here, using femtosecond pump-probe transient absorption microscopy, we directly image the spatially resolved nonlinear optical response of exciton-Fermi polarons in monolayer MoSe$_2$. We observe a pronounced spatial suppression of resonant absorption associated with the attractive Fermi polaron, from which we extract an optical blockade radius that is more than ten times larger than that of the neutral exciton. Microscopic analysis indicates that this extended nonlinearity arises primarily from fermion-mediated interactions between exciton-Fermi polarons. Our results establish exciton-Fermi polarons in two-dimensional semiconductors as electrically tunable, strongly interacting optical quasiparticles, and identify them as a promising platform for ultralow-power nonlinear optical devices.

cond-mat.mes-hall

Transition Metal Dichalcogenide Excitons in Periodic Electrostatic Potentials: Center-of-Mass Models

Two-dimensional (2D) van-der-Waals materials are a promising platform for exciton state engineering. In this paper, we study the properties of excitons in 2D group VI transition-metal dichalcogenide (TMD) semiconductors that are modified by a periodic electrostatic potential through the quadratic Stark effect. Using a model that retains only center-of-mass and valley degrees-of-freedom, we find that electrostatic potentials can drive optical valley splitting up to 10meVs and induce valley selective exciton dispersion. We explain why both properties are sensitive to the rotational symmetry of the electrostatic trapping potential using a combination of numerical results and analytical approximations. An important consequence of valley-splitting is that the lowest exciton band is non-degenerate and has a linear dispersion around $\gamma$ that is expected to suppress thermal excitations, allowing true Bose condensation and superfluidity of excitons in two space dimensions.

cond-mat.str-el

Deterministic fabrication of graphene hexagonal boron nitride moir\'e superlattices

The electronic properties of moir\'e heterostructures depend sensitively on the relative orientation between layers of the stack. For example, near-magic-angle twisted bilayer graphene (TBG) commonly shows superconductivity, yet a TBG sample with one of the graphene layers rotationally aligned to a hexagonal Boron Nitride (hBN) cladding layer provided the first experimental observation of orbital ferromagnetism. To create samples with aligned graphene/hBN, researchers often align edges of exfoliated flakes that appear straight in optical micrographs. However, graphene or hBN can cleave along either zig-zag or armchair lattice directions, introducing a 30 degree ambiguity in the relative orientation of two flakes. By characterizing the crystal lattice orientation of exfoliated flakes prior to stacking using Raman and second-harmonic generation for graphene and hBN, respectively, we unambiguously align monolayer graphene to hBN at a near-0 degree, not 30 degree, relative twist angle. We confirm this alignment by torsional force microscopy (TFM) of the graphene/hBN moir\'e on an open-face stack, and then by cryogenic transport measurements, after full encapsulation with a second, non-aligned hBN layer. This work demonstrates a key step toward systematically exploring the effects of the relative twist angle between dissimilar materials within moir\'e heterostructures.

cond-mat.mes-hall

Giant room-temperature nonlinearities from a monolayer Janus topological semiconductor

Nonlinear optical materials possess wide applications, ranging from terahertz and mid-infrared detection to energy harvesting. Recently, the correlations between nonlinear optical responses and topological properties, such as Berry curvature and the quantum metric tensor, have stimulated great interest. Here, we report giant room-temperature nonlinearities in an emergent non-centrosymmetric two-dimensional topological material, the Janus transition metal dichalcogenides in the 1T' phase, which are synthesized by an advanced atomic-layer substitution method. High harmonic generation, terahertz emission spectroscopy, and second harmonic generation measurements consistently reveal orders-of-the-magnitude enhancement in terahertz-frequency nonlinearities of 1T' MoSSe (e.g., > 50 times higher than 2H MoS$_2$ for 18th order harmonic generation; > 20 times higher than 2H MoS$_2$ for terahertz emission). It is elucidated that such colossal nonlinear optical responses come from topological band mixing and strong inversion symmetry breaking due to the Janus structure. Our work defines general protocols for designing materials with large nonlinearities and preludes the applications of topological materials in optoelectronics down to the monolayer limit. This two-dimensional form of topological materials also constitute a unique platform for examining origin of the anomalous high-harmonic generation, with potential applications as building blocks for scalable attosecond sources.

cond-mat.mes-hall

X-ray Free Electron Laser Studies of Electron and Phonon Dynamics of Graphene Adsorbed on Copper

We report optical pumping and X-ray absorption spectroscopy experiments at the PAL free electron laser that directly probe the electron dynamics of a graphene monolayer adsorbed on copper in the femtosecond regime. By analyzing the results with ab-initio theory we infer that the excitation of graphene is dominated by indirect excitation from hot electron-hole pairs created in the copper by the optical laser pulse. However, once the excitation is created in graphene, its decay follows a similar path as in many previous studies of graphene adsorbed on semiconductors, i e. rapid excitation of SCOPS (Strongly Coupled Optical Phonons) and eventual thermalization. It is likely that the lifetime of the hot electron-hole pairs in copper governs the lifetime of the electronic excitation of the graphene.

cond-mat.mes-hall

Measurement of lateral and interfacial thermal conductivity of single- and bi-layer MoS2 and MoSe2 using refined optothermal Raman technique

Atomically thin materials such as graphene and semiconducting transition metal dichalcogenides (TMDCs) have attracted extensive interest in recent years, motivating investigation into multiple properties. In this work, we demonstrate a refined version of the optothermal Raman technique to measure the thermal transport properties of two TMDC materials, MoS2 and MoSe2, in single-layer (1L) and bi-layer (2L) forms. This new version incorporates two crucial improvements over previous implementations. First, we utilize more direct measurements of the optical absorption of the suspended samples under study and find values ~40% lower than previously assumed. Second, by comparing the response of fully supported and suspended samples using different laser spot sizes, we are able to independently measure the interfacial thermal conductance to the substrate and the lateral thermal conductivity of the supported and suspended materials. The approach is validated by examining the response of a suspended film illuminated in different radial positions. For 1L MoS2 and MoSe2, the room-temperature thermal conductivities are (84+/-17) W/mK and (59+/-18) W/mK, respectively. For 2L MoS2 and MoSe2, we obtain values of (77+/-25) W/mK and (42+/-13) W/mK. Crucially, the interfacial thermal conductance is found to be of order 0.1-1 MW/m2K, substantially smaller than previously assumed, a finding that has important implications for design and modeling of electronic devices.

cond-mat.mtrl-sci