arXiv subjects

Jiwoong Park

Publications and source records attributed to Jiwoong Park.

At least 37 records · Page 2Linked to original sources

arXiv2019

Low-loss composite photonic platform based on 2D semiconductor monolayers

Two dimensional materials such as graphene and transition metal dichalcogenides (TMDs) are promising for optical modulation, detection, and light emission since their material properties can be tuned on-demand via electrostatic doping. The optical properties of TMDs have been shown to change drastically with doping in the wavelength range near the excitonic resonances. However, little is known about the effect of doping on the optical properties of TMDs away from these resonances, where the material is transparent and therefore could be leveraged in photonic circuits. Here, we probe the electro-optic response of monolayer TMDs at near infrared (NIR) wavelengths (i.e. deep in the transparency regime), by integrating them on silicon nitride (SiN) photonic structures to induce strong light$-$matter interaction with the monolayer. We dope the monolayer to carrier densities of ($7.2 \pm 0.8$) $\times$ $10^{13} \textrm{cm}^{-2}$, by electrically gating the TMD using an ionic liquid. We show strong electro-refractive response in monolayer tungsten disulphide (WS$_2$) at NIR wavelengths by measuring a large change in the real part of refractive index $Δ$n = $0.53$, with only a minimal change in the imaginary part $Δ$k = $0.004$. The doping induced phase change ($Δ$n), compared to the induced absorption ($Δ$k) measured for WS$_2$ ($Δ$n/$Δ$k $\sim 125$), a key metric for photonics, is an order of magnitude higher than the $Δ$n/$Δ$k for bulk materials like silicon ($Δ$n/$Δ$k $\sim 10$), making it ideal for various photonic applications. We further utilize this strong tunable effect to demonstrate an electrostatically gated SiN-WS$_2$ phase modulator using a WS$_2$-HfO$_2$ (Hafnia)-ITO (Indium Tin Oxide) capacitive configuration, that achieves a phase modulation efficiency (V$_π$L) of 0.8 V $\cdot$ cm with a RC limited bandwidth of 0.3 GHz.

physics.app-ph↗

arXiv2019

Stacking, Strain, & Twist in 2D Materials Quantified by 3D Electron Diffraction

The field of two-dimensional (2D) materials has expanded to multilayered systems where electronic, optical, and mechanical properties change-often dramatically-with stacking order, thickness, twist, and interlayer spacing [1-5]. For transition metal dichalcogenides (TMDs), bond coordination within a single van der Waals layer changes the out-of-plane symmetry that can cause metal-insulator transitions [1, 6] or emergent quantum behavior [7]. Discerning these structural order parameters is often difficult using real-space measurements, however, we show 2D materials have distinct, conspicuous three-dimensional (3D) structure in reciprocal space described by near infinite oscillating Bragg rods. Combining electron diffraction and specimen tilt we probe Bragg rods in all three dimensions to identify multilayer structure with sub-Angstrom precision across several 2D materials-including TMDs (MoS2, TaSe2, TaS2) and multilayer graphene. We demonstrate quantitative determination of key structural parameters such as surface roughness, inter- & intra-layer spacings, stacking order, and interlayer twist using a rudimentary transmission electron microscope (TEM). We accurately characterize the full interlayer stacking order of multilayer graphene (1-, 2-, 6-, 12-layers) as well the intralayer structure of MoS2 and extract a chalcogen-chalcogen layer spacing of 3.07 +/- 0.11 Angstrom. Furthermore, we demonstrate quick identification of multilayer rhombohedral graphene.

cond-mat.mtrl-sci↗

arXiv2019

Spatiotemporal Mapping of Photocurrent in a Monolayer Semiconductor Using a Diamond Quantum Sensor

The detection of photocurrents is central to understanding and harnessing the interaction of light with matter. Although widely used, transport-based detection averages over spatial distributions and can suffer from low photocarrier collection efficiency. Here, we introduce a contact-free method to spatially resolve local photocurrent densities using a proximal quantum magnetometer. We interface monolayer MoS2 with a near-surface ensemble of nitrogen-vacancy centers in diamond and map the generated photothermal current distribution through its magnetic field profile. By synchronizing the photoexcitation with dynamical decoupling of the sensor spin, we extend the sensor's quantum coherence and achieve sensitivities to alternating current densities as small as 20 nA per micron. Our spatiotemporal measurements reveal that the photocurrent circulates as vortices, manifesting the Nernst effect, and rises with a timescale indicative of the system's thermal properties. Our method establishes an unprecedented probe for optoelectronic phenomena, ideally suited to the emerging class of two-dimensional materials, and stimulates applications towards large-area photodetectors and stick-on sources of magnetic fields for quantum control.

cond-mat.mtrl-sci↗

arXiv2018

θ-Tunable Photoluminescence from Interlayer Excitons in Twisted Bilayer Graphene

Using resonant 2-photon excitation of interlayer electrons in twisted bilayer graphene (tBLG), we resolve photoluminescence (PL) that tunes spectrally with stacking angle, θ. This weak signal is 4- 5$\times$ larger than the non-resonant background and is emitted from the interlayer band anti-crossing regions traditionally associated with van Hove singularity resonances. However, our observation of resonant PL emission with delayed ~1 ps electronic thermalization suggests interlayer carriers may instead form bound-excitons. Using both the 2-photon PL and intraband transient absorption spectra, we observe bright and dark state peak-splitting associated with an interlayer exciton binding energy ranging from 0.5 to 0.7 eV for θ = 8$^o$ to 17$^o$. These results support theoretical models showing interlayer excitons in tBLG are stabilized by a vanishing exciton-coupling strength to the metallic continuum states. This unexpected dual metal-exciton optical property of tBLG suggests possible θ-tuneable control over carrier thermalization, extraction and emission in optical graphene-based devices.

cond-mat.mes-hall↗

arXiv2018

Strain Mapping of Two-Dimensional Heterostructures with Sub-Picometer Precision

Next-generation, atomically thin devices require in-plane, one-dimensional heterojunctions to electrically connect different two-dimensional (2D) materials. However, the lattice mismatch between most 2D materials leads to unavoidable strain, dislocations, or ripples, which can strongly affect their mechanical, optical, and electronic properties. We have developed an approach to map 2D heterojunction lattice and strain profiles with sub-picometer precision and to identify dislocations and out-of-plane ripples. We collected diffraction patterns from a focused electron beam for each real-space scan position with a high-speed, high dynamic range, momentum-resolved detector - the electron microscope pixel array detector (EMPAD). The resulting four-dimensional (4D) phase space datasets contain the full spatially resolved lattice information of the sample. By using this technique on tungsten disulfide (WS2) and tungsten diselenide (WSe2) lateral heterostructures, we have mapped lattice distortions with 0.3 pm precision across multi-micron fields of view and simultaneously observed the dislocations and ripples responsible for strain relaxation in 2D laterally-epitaxial structures.

physics.app-ph↗

arXiv2018

Deep sub-Ångstrom imaging of 2D materials with a high dynamic range detector

Aberration-corrected optics have made electron microscopy at atomic-resolution a widespread and often essential tool for nanocharacterization. Image resolution is dominated by beam energy and the numerical aperture of the lens (α), with state-of-the-art reaching ~0.47 Å at 300 keV. Two-dimensional materials are imaged at lower beam energies to avoid knock-on damage, limiting spatial resolution to ~1 Å. Here, by combining a new electron microscope pixel array detector with the dynamic range to record the complete distribution of transmitted electrons and full-field ptychography to recover phase information from the full phase space, we increased the spatial resolution well beyond the traditional lens limitations. At 80 keV beam energy, our ptychographic reconstructions significantly improved image contrast of single-atom defects in MoS2, reaching an information limit close to 5α, corresponding to a 0.39 Å Abbe resolution, at the same dose and imaging conditions where conventional imaging modes reach only 0.98 Å.

cond-mat.mtrl-sci↗

arXiv2017

Absence of a Band Gap at Interface of a Metal and Highly Doped Monolayer $MoS_2$

High quality electrical contact to semiconducting transition metal dichalcogenides (TMDCs) such as $MoS_2$ is key to unlocking their unique electronic and optoelectronic properties for fundamental research and device applications. Despite extensive experimental and theoretical efforts reliable ohmic contact to doped TMDCs remains elusive and would benefit from a better understanding of the underlying physics of the metal-TMDC interface. Here we present measurements of the atomic-scale energy band diagram of junctions between various metals and heavily doped monolayer $MoS_2$ using ultra-high vacuum scanning tunneling microscopy (UHV-STM). Our measurements reveal that the electronic properties of these junctions are dominated by 2D metal induced gap states (MIGS). These MIGS are characterized by a spatially growing measured gap in the local density of states (L-DOS) of the $MoS_2$ within 2 nm of the metal-semiconductor interface. Their decay lengths extend from a minimum of ~0.55 nm near mid gap to as long as 2 nm near the band edges and are nearly identical for Au, Pd and graphite contacts, indicating that it is a universal property of the monolayer semiconductor. Our findings indicate that even in heavily doped semiconductors, the presence of MIGS sets the ultimate limit for electrical contact.

cond-mat.mtrl-sci↗

arXiv2017

Coherent Atomically-Thin Superlattices with Engineered Strain

Epitaxy forms the basis of modern electronics and optoelectronics. We report coherent atomically-thin superlattices, in which different transition metal dichalcogenide monolayers--despite large lattice mismatches--are repeated and integrated without dislocations. Grown by a novel omnidirectional epitaxy, these superlattices display fully-matched lattice constants across heterointerfaces while maintaining a surprisingly isotropic lattice structure and triangular symmetry. This strong epitaxial strain is precisely engineered via the nanoscale supercell dimensions, thereby enabling broad tuning of the optical properties and producing photoluminescence peak shifts as large as 250 meV. We present theoretical models to explain this coherent growth as well as the energetic interplay governing the flat-rippled configuration space in these strained monolayers. Such coherent superlattices provide novel building blocks with targeted functionalities at the atomically-thin monolayer limit.

cond-mat.mtrl-sci↗

arXiv2016

Atomically-thin Ohmic Edge Contacts Between Two-dimensional Materials

With the decrease of the dimensions of electronic devices, the role played by electrical contacts is ever increasing, eventually coming to dominate the overall device volume and total resistance. This is especially problematic for monolayers of semiconducting transition metal dichalcogenides (TMDs), which are promising candidates for atomically thin electronics. Ideal electrical contacts to them would require the use of similarly thin electrode materials while maintaining low contact resistances. Here we report a scalable method to fabricate ohmic graphene edge contacts to two representative monolayer TMDs - MoS2 and WS2. The graphene and TMD layer are laterally connected with wafer-scale homogeneity, no observable overlap or gap, and a low average contact resistance of 30 k$Ω$ $μ$m. The resulting graphene edge contacts show linear current-voltage (IV) characteristics at room temperature, with ohmic behavior maintained down to liquid helium temperatures.

cond-mat.mes-hall↗

arXiv2015

Strongly bound excitons dominate electronic relaxation in resonantly excited twisted bilayer graphene

When two sheets of graphene stack in a twisted bilayer graphene (tBLG) configuration, the resulting constrained overlap between interplanar 2p orbitals produce angle-tunable electronic absorption resonances. Using a novel combination of multiphoton transient absorption (TA) microscopy and TEM, we resolve the resonant electronic structure, and ensuing electronic relaxation inside single tBLG domains. Strikingly, we find that the transient electronic population in resonantly excited tBLG domains is enhanced many fold, forming a major electronic relaxation bottleneck. 2-photon TA microscopy shows this bottleneck effect originates from a strongly bound, dark exciton state lying 0.37 eV below the 1-photon absorption resonance. This stable coexistence of strongly bound excitons alongside free-electron continuum states has not been previously observed in a metallic, 2D material.

cond-mat.mes-hall↗

arXiv2014

Breaking of valley degeneracy by magnetic field in monolayer MoSe2

Using polarization-resolved photoluminescence spectroscopy, we investigate valley degeneracy breaking by out-of-plane magnetic field in back-gated monolayer MoSe$_2$ devices. We observe a linear splitting of $-0.22 \frac{\text{meV}}{\text{T}}$ between luminescence peak energies in $σ_{+}$ and $σ_{-}$ emission for both neutral and charged excitons. The optical selection rules of monolayer MoSe$_2$ couple photon handedness to the exciton valley degree of freedom, so this splitting demonstrates valley degeneracy breaking. In addition, we find that the luminescence handedness can be controlled with magnetic field, to a degree that depends on the back-gate voltage. An applied magnetic field therefore provides effective strategies for control over the valley degree of freedom.

cond-mat.mes-hall↗

arXiv2014

Van Hove Singularities and Excitonic Effects in the Optical Conductivity of Twisted Bilayer Graphene

We report a systematic study of the optical conductivity of twisted bilayer graphene (tBLG) across a large energy range (1.2 eV to 5.6 eV) for various twist angles, combined with first-principles calculations. At previously unexplored high energies, our data show signatures of multiple van Hove singularities (vHSs) in the tBLG bands, as well as the nonlinearity of the single layer graphene bands and their electron-hole asymmetry. Our data also suggest that excitonic effects play a vital role in the optical spectra of tBLG. Including electron-hole interactions in first-principles calculations is essential to reproduce the shape of the conductivity spectra, and we find evidence of coherent interactions between the states associated with the multiple vHSs in tBLG.

cond-mat.mes-hall↗

arXiv2014

The Valley Hall Effect in MoS2 Transistors

Electrons in 2-dimensional crystals with a honeycomb lattice structure possess a new valley degree of freedom (DOF) in addition to charge and spin. Each valley is predicted to exhibit a Hall effect in the absence of a magnetic field whose sign depends on the valley index, but to date this effect has not been observed. Here we report the first observation of this new valley Hall effect (VHE). Monolayer MoS2 transistors are illuminated by circularly polarized light which preferentially excites electrons into a specific valley, and a finite anomalous Hall voltage is observed whose sign is controlled by the helicity of the light. Its magnitude is consistent with theoretical predictions of the VHE, and no anomalous Hall effect is observed in bilayer devices due to the restoration of crystal inversion symmetry. Our observation of the VHE opens up new possibilities for using the valley DOF as an information carrier in next-generation electronics and optoelectronics.

cond-mat.mes-hall↗

arXiv2014

New Mechanism for Strongly Bound Excitons in Gapless Two-Dimensional Structures

Common wisdom asserts that bound excitons cannot form in high-dimensional (d>1) metallic structures because of their overwhelming screening and unavoidable resonance with nearby continuous bands. Strikingly, here we illustrate that this prevalent assumption is not quite true. A key ingredient that has been overlooked is that of viable decoherence that thwarts the formation of resonances. As an example of this general mechanism, we focus on an experimentally relevant material and predict bound excitons in twisted bilayer graphene, which is a two-dimensional gapless structure exhibiting metallic screening. The binding energies calculated by first-principles simulations are surprisingly large. The low-energy effective model reveals that these bound states are produced by a unique destructive coherence between two alike subband resonant excitons. In particular, this destructive coherent effect is not sensitive to the screening and dimensionality, and hence may persist as a general mechanism for creating bound excitons in various metallic structures, opening the door for excitonic applications based on metallic structures.

cond-mat.mes-hall↗

arXiv2013

Transient absorption and photocurrent microscopy show hot electron supercollisions describe the rate-limiting relaxation step in graphene

Using transient absorption (TA) microscopy as a hot electron thermometer we show disorder-assisted acoustic-phonon supercollisions (SCs) best describes the rate-limiting relaxation step in graphene over a wide range of lattice temperatures ($T_l=$5-300 K), Fermi energies ($E_F=\pm0.35$ eV), and optical probe energies (~0.3 - 1.1 eV). Comparison with simultaneously collected transient photocurrent, an independent hot electron thermometer, confirms the rate-limiting optical and electrical response in graphene are best described by the SC-heat dissipation rate model, $H=A(T^3_e- T^3_l)$. Our data further shows the electron cooling rate in substrate supported graphene is twice as fast as in suspended graphene sheets, consistent with SC-model prediction for disorder.

cond-mat.mtrl-sci↗

arXiv2013

Strain Solitons and Topological Defects in Bilayer Graphene

Spontaneous symmetry-breaking, where the ground state of a system has lower symmetry than the underlying Hamiltonian, is ubiquitous in physics. It leads to multiply-degenerate ground states, each with a different "broken" symmetry labeled by an order parameter. The variation of this order parameter in space leads to soliton-like features at the boundaries of different broken-symmetry regions and also to topological point defects. Bilayer graphene is a fascinating realization of this physics, with an order parameter given by its interlayer stacking coordinate. Bilayer graphene has been a subject of intense study because in the presence of a perpendicular electric field, a band gap appears in its electronic spectrum [1-3] through a mechanism that is intimately tied to its broken symmetry. Theorists have further proposed that novel electronic states exist at the boundaries between broken-symmetry stacking domains [4-5]. However, very little is known about the structural properties of these boundaries. Here we use electron microscopy to measure with nanoscale and atomic resolution the widths, motion, and topological structure of soliton boundaries and topological defects in bilayer graphene. We find that each soliton consists of an atomic-scale registry shift between the two graphene layers occurring over 6-11 nm. We infer the minimal energy barrier to interlayer translation and observe soliton motion during in-situ heating above 1000 °C. The abundance of these structures across a variety samples, as well as their unusual properties, suggests that they will have substantial effects on the electronic and mechanical properties of bilayer graphene.

cond-mat.mes-hall↗

arXiv2012

Photocurrent measurements of supercollision cooling in graphene

The cooling of hot electrons in graphene is the critical process underlying the operation of exciting new graphene-based optoelectronic and plasmonic devices, but the nature of this cooling is controversial. We extract the hot electron cooling rate near the Fermi level by using graphene as novel photothermal thermometer that measures the electron temperature ($T(t)$) as it cools dynamically. We find the photocurrent generated from graphene $p-n$ junctions is well described by the energy dissipation rate $C dT/dt=-A(T^3-T_l^3)$, where the heat capacity is $C=αT$ and $T_l$ is the base lattice temperature. These results are in disagreement with predictions of electron-phonon emission in a disorder-free graphene system, but in excellent quantitative agreement with recent predictions of a disorder-enhanced supercollision (SC) cooling mechanism. We find that the SC model provides a complete and unified picture of energy loss near the Fermi level over the wide range of electronic (15 to $\sim$3000 K) and lattice (10 to 295 K) temperatures investigated.

cond-mat.mes-hall↗

arXiv2011

Uniform Peak Optical Conductivity in Single-Walled Carbon Nanotubes

Recent measurements in single-walled carbon nanotubes show that, on resonance, all nanotubes display the same peak optical conductivity of approximately 8 $e^2/h$, independent of radius or chirality [Joh \emph{et al.}, \emph{Nature Nanotechnology} \textbf{6}, 51 (2011)]. We show that this uniform peak conductivity is a consequence of the relativistic band structure and strength of the Coulomb interaction in carbon nanotubes. We further construct a minimalist model of exciton dynamics that describes the general phenomenology and provides an accurate prediction of the numerical value of the peak optical conductivity. The work illustrates the need for careful treatment of relaxation mechanisms in modeling the optoelectronic properties of carbon nanotubes.

cond-mat.mes-hall↗