Showing 1–50 of 83 results for author: Heinz, T F

Moiré enabled spin pumping and preservation in MoSe2/WS2 heterobilayers

Authors: Leo Yu, Kateryna Pistunova, Sudipta Kundu, Jenny Hu, Kenji Watanabe, Takashi Taniguchi, Felipe H. da Jornada, Tony F. Heinz

Abstract: The spin degree of freedom is a fundamental quantum mechanical attribute with implications spanning from magnetism to quantum computing. Consequently, the relaxation of spin states for extended, Bloch electrons in solids has been studied for decades as it defines many of their properties and applications. We show that moiré patterns in layered materials can extend spin relaxation times by two orde… ▽ More The spin degree of freedom is a fundamental quantum mechanical attribute with implications spanning from magnetism to quantum computing. Consequently, the relaxation of spin states for extended, Bloch electrons in solids has been studied for decades as it defines many of their properties and applications. We show that moiré patterns in layered materials can extend spin relaxation times by two orders of magnitude to 1 millisecond and beyond. This is achieved by suppressing spin mixing for electrons in 2D semiconductor heterostructures, particularly in the MoSe2/WS2 system, as we elucidate both experimentally and theoretically. The extended longitudinal lifetime facilitates spin alignment over 50% using only nanowatt levels of optical power. Our findings highlight the potential of moiré engineering for future quantum sensing and information processing. △ Less

Submitted 2 June, 2026; originally announced June 2026.

Interfacial control of hot-carrier extraction and photostability in two-dimensional materials

Authors: Claudia Gollner, Mohammad Taghinejad, Chenyi Xia, Zhepeng Zhang, Fang Liu, Francesco Laudani, Annette Foelske, Mark L. Brongersma, Andrew J. Mannix, Tony F. Heinz, Aaron Lindenberg

Abstract: Two-dimensional transition metal dichalcogenides (TMDCs) are promising materials for next-generation optoelectronic devices, yet their implementation is hindered by limited sample stability and challenges in forming reliable electrical contacts. Here, by utilizing time-domain THz emission spectroscopy we directly probe charge carrier dynamics in monolayer WS2 on gold (Au) and fused silica (SiO2) a… ▽ More Two-dimensional transition metal dichalcogenides (TMDCs) are promising materials for next-generation optoelectronic devices, yet their implementation is hindered by limited sample stability and challenges in forming reliable electrical contacts. Here, by utilizing time-domain THz emission spectroscopy we directly probe charge carrier dynamics in monolayer WS2 on gold (Au) and fused silica (SiO2) as a function of interface morphology. For laser excitation above the band gap of WS2, we independently extract effective transport times for both electrons and holes and find that discontinuous WS2 contacts on rough Au generate larger net photocurrents than uniform, strongly coupled interfaces - a counterintuitive observation attributed to imbalanced electron and hole transfer from WS2 to Au. Crucially, we demonstrate that ultrafast charge extraction and separation suppress recombination-driven energy release and thereby prevent photo-induced degradation under ambient conditions, eliminating the need for encapsulation. These findings redefine interfacial design as a central control parameter for both performance and stability in 2D optoelectronic devices. △ Less

Submitted 8 May, 2026; originally announced May 2026.

Electric-field-tuned consecutive topological phase transitions between distinct correlated insulators in moire MoTe2/WSe2 heterobilayer

Authors: Xumin Chang, Zui Tao, Bowen Shen, Wanghao Tian, Jenny Hu, Kateryna Pistunova, Kenji Watanabe, Takashi Taniguchi, Tony F. Heinz, Tingxin Li, Kin Fai Mak, Jie Shan, Shengwei Jiang

Abstract: Consecutive topological phase transitions (TPTs) between strongly correlated electronic phases that differ simultaneously in symmetry breaking and topological order are of fundamental interest in condensed matter physics, yet are rarely realized experimentally. We report two consecutive electric-field-driven TPTs at half filling (nu = 1) in angle-aligned MoTe2/WSe2 moire heterobilayers. With incre… ▽ More Consecutive topological phase transitions (TPTs) between strongly correlated electronic phases that differ simultaneously in symmetry breaking and topological order are of fundamental interest in condensed matter physics, yet are rarely realized experimentally. We report two consecutive electric-field-driven TPTs at half filling (nu = 1) in angle-aligned MoTe2/WSe2 moire heterobilayers. With increasing out-of-plane displacement field, a geometrically frustrated Mott insulator evolves into a ferromagnetic quantum anomalous Hall (QAH) Mott insulator, i.e., a spin-polarized topological Mott insulator without an observable charge-gap closure, and subsequently into an antiferromagnetic, valley-coherent Mott insulator (VC-AFM) accompanied by a continuous charge-gap collapse and the emergence of a critical metallic state. Layer-resolved magnetic circular dichroism (MCD), magneto-transport, and compressibility measurements jointly determine the phase diagram. The high-field evolution of the antiferromagnetic state reveals a metamagnetic-like transition at a critical field B*, above which a Chern insulating transport response reappears. Our results establish the MoTe2/WSe2 moire platform as a tunable realization of an extended Kane-Mele-Hubbard model hosting sequential correlation-topology-intertwined transitions. △ Less

Submitted 17 February, 2026; originally announced February 2026.

Direct nanoscale mapping of band alignment in single-layer semiconducting lateral heterojunctions

Authors: Chakradhar Sahoo, Suman Kumar Chakraborty, A. Kousika, Alfred J. H. Jones, Manas Sharma, Thomas S. Nielsen, Zhihao Jiang, Ihsan A. Kolasseri, Subhadip Das, Matthew D. Watson, Cephise Cacho, Kenji Watanabe, Takashi Taniguchi, Yong P. Chen, Tony F. Heinz, Ananth Govind Rajan, Prasana K. Sahoo, Søren Ulstrup

Abstract: Atomic-scale control over band alignment in single-layer lateral heterostructures (LHSs) of dissimilar transition metal dichalcogenides (TMDCs) is critical for nextgeneration electronic, optoelectronic, and quantum technologies. However, direct experimental access to interfacial electronic states with nanometer precision remains a significant challenge. Here, we employ angle-resolved photoemission… ▽ More Atomic-scale control over band alignment in single-layer lateral heterostructures (LHSs) of dissimilar transition metal dichalcogenides (TMDCs) is critical for nextgeneration electronic, optoelectronic, and quantum technologies. However, direct experimental access to interfacial electronic states with nanometer precision remains a significant challenge. Here, we employ angle-resolved photoemission spectroscopy with nanoscale spatial resolution (nanoARPES) to directly map the epitaxial alignment and valence band evolution across MoSe2-WSe2 LHSs. By combining nanoARPES with spatially resolved photoluminescence, we correlate the evolution of the valence band maximum and exciton features across both atomically sharp and compositionally graded diffusive interfaces. We identified type-II band alignments governed by both material composition and interstitial-induced modifications of band offsets, in close agreement with density functional theory calculations. These results reveal fundamental mechanisms of electronic structure modulation at 1D TMDC heterointerfaces and provide a robust platform for tailored band engineering in van der Waals materials. △ Less

Submitted 3 February, 2026; originally announced February 2026.

Exciton-polaron Umklapp scattering in Wigner crystals

Authors: Erfu Liu, Matthew Wilson, Jenny Hu, Alexandra Zimmerman, Amal Mathew, Tianyi Ouyang, Ao Shi, Takashi Taniguchi, Kenji Watanabe, Tony F. Heinz, Yia-Chung Chang, Chun Hung Lui

Abstract: Strong Coulomb interactions in two-dimensional (2D) semiconductors give rise to tightly bound excitons, exciton polarons, and correlated electronic phases such as Wigner crystals (WCs), yet their mutual interplay remains poorly understood. Here we report the observation of multi-branch excitonic Umklapp scattering in both electron and hole WCs realized in ultraclean monolayer WSe$_2$, exhibiting e… ▽ More Strong Coulomb interactions in two-dimensional (2D) semiconductors give rise to tightly bound excitons, exciton polarons, and correlated electronic phases such as Wigner crystals (WCs), yet their mutual interplay remains poorly understood. Here we report the observation of multi-branch excitonic Umklapp scattering in both electron and hole WCs realized in ultraclean monolayer WSe$_2$, exhibiting exceptionally high melting temperatures (T$_c$ $\approx$ 20-30 K). Robust Wigner crystallization activates multiple finite-momentum optical resonances, including quasilinearly dispersing, light-like excitons and exciton polarons, extending far beyond the single excitonic Umklapp feature reported previously. Helicity-resolved magneto-optical measurements reveal a pronounced valley dependence of the scattering processes. Combined experiment and theory identify a polaron-induced brightening mechanism in which exciton polarons transfer oscillator strength from bright zero-momentum states to otherwise dark finite-momentum states, explaining the emergence of multiple Umklapp branches where conventional exciton-WC scattering is ineffective. These results establish WC polarons as a new quasiparticle paradigm and introduce polaron-induced Umklapp scattering as a general route to accessing finite-momentum many-body excitations in 2D quantum materials. △ Less

Submitted 24 January, 2026; v1 submitted 17 January, 2026; originally announced January 2026.

Terahertz field-induced giant symmetry modulations in a van der Waals antiferromagnet

Authors: Sheikh Rubaiat Ul Haque, Martin J. Cross, Sangeeta Rajpurohit, Jonah B. Haber, Christopher J. Ciccarino, Alexandra C. Zimmerman, Isabelle J. Sealey, Vadym Kulichenko, Monique Tie, Huaiyu Wang, Sharon S. Philip, Choongwon Seo, Jake D. Koralek, Luis Balicas, Mykhaylo Ozerov, Dmitry Smirnov, Liang Z. Tan, Felipe H. da Jornada, Tadashi Ogitsu, Matthias C. Hoffmann, Tony F. Heinz, Aaron M. Lindenberg

Abstract: Strong-field terahertz (THz) excitations enable dynamic control over electronic, lattice and symmetry degrees of freedom in quantum materials. Here, we uncover pronounced terahertz-induced symmetry modulations and coherent phonon dynamics in the van der Waals antiferromagnet MnPS3, in which inversion symmetry is broken by its antiferromagnetic spin configuration. Time-resolved second harmonic gene… ▽ More Strong-field terahertz (THz) excitations enable dynamic control over electronic, lattice and symmetry degrees of freedom in quantum materials. Here, we uncover pronounced terahertz-induced symmetry modulations and coherent phonon dynamics in the van der Waals antiferromagnet MnPS3, in which inversion symmetry is broken by its antiferromagnetic spin configuration. Time-resolved second harmonic generation measurements reveal long-lived giant oscillations in the antiferromagnetic phase, with amplitudes comparable to the equilibrium signal, driven by phonons involving percent-level atomic displacements relative to the equilibrium bond lengths. The temporal evolution of the rotational anisotropy patterns indicate a dynamic breaking of mirror symmetry, modulated by two vibrational modes at 1.7 THz and 4.5 THz, with the former corresponding to a hidden mode not observed in equilibrium spectroscopy. We show that these effects arise in part from a field-induced charge rearrangement mechanism that lowers the local crystal symmetry, and couples to the phonon modes. A long-lived field-driven response was uncovered with a complex THz polarization dependence which, in comparison to theory, indicates evidence for an antiferromagnetic-to-ferrimagnetic transition. Our results establish an effective field-tunable pathway for driving excitations otherwise weak in equilibrium, and for manipulating magnetism in low-dimensional materials via dynamical modulation of symmetry. △ Less

Submitted 1 October, 2025; originally announced October 2025.

Roadmap for Photonics with 2D Materials

Authors: F. Javier García de Abajo, D. N. Basov, Frank H. L. Koppens, Lorenzo Orsini, Matteo Ceccanti, Sebastián Castilla, Lorenzo Cavicchi, Marco Polini, P. A. D. Gonçalves, A. T. Costa, N. M. R. Peres, N. Asger Mortensen, Sathwik Bharadwaj, Zubin Jacob, P. J. Schuck, A. N. Pasupathy, Milan Delor, M. K. Liu, Aitor Mugarza, Pablo Merino, Marc G. Cuxart, Emigdio Chávez-Angel, Martin Svec, Luiz H. G. Tizei, Florian Dirnberger , et al. (123 additional authors not shown)

Abstract: Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combinat… ▽ More Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combination with layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary collection of those directions, where 2D materials contribute with polaritons of unique characteristics such as strong spatial confinement, large optical-field enhancement, long lifetimes, high sensitivity to external stimuli (e.g., electric and magnetic fields, heating, and strain), a broad spectral range from the far infrared to the ultraviolet, and hybridization with spin and momentum textures of electronic band structures. The explosion of photonics with 2D materials as a vibrant research area is producing breakthroughs, including the discovery and design of new materials and metasurfaces with unprecedented properties as well as applications in integrated photonics, light emission, optical sensing, and exciting prospects for applications in quantum information, and nanoscale thermal transport. This Roadmap summarizes the state of the art in the field, identifies challenges and opportunities, and discusses future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners. △ Less

Submitted 14 April, 2025; v1 submitted 6 April, 2025; originally announced April 2025.

Comments: 199 pages, 42 figures, 1154 references

Journal ref: ACS Photonics 12, 3961 (2025)

Nonresonant Raman control of ferroelectric polarization

Authors: Jiaojian Shi, Christian Heide, Haowei Xu, Yuejun Shen, Meredith Henstridge, Isabel Sedwick, Anudeep Mangu, Xinyue Peng, Shangjie Zhang, Mariano Trigo, Tony F. Heinz, Ju Li, Keith A. Nelson, Edoardo Baldini, Jian Zhou, Shambhu Ghimire, David A. Reis, Aaron M. Lindenberg

Abstract: Important advances have recently been made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light-matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant… ▽ More Important advances have recently been made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light-matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant Raman excitation of coherent modes has been experimentally observed and proposed for dynamic material control, but the resulting atomic excursion has been limited to perturbative levels. Here, this challenge is overcome by employing nonresonant ultrashort pulses with low photon energies well below the bandgap. Using mid-infrared pulses, ferroelectric reversal is induced in lithium niobate, and the large-amplitude mode displacements are characterized through femtosecond stimulated Raman scattering and second harmonic generation. This approach, validated by first-principle calculations, defines a novel method for synthesizing hidden phases with unique functional properties and manipulating complex energy landscapes at reduced energy consumption and ultrafast speeds. △ Less

Submitted 7 September, 2025; v1 submitted 15 November, 2024; originally announced November 2024.

Comments: 4 figures

Room-temperature valley-selective emission in Si-MoSe2 heterostructures enabled by high-quality-factor chiroptical cavities

Authors: Feng Pan, Xin Li, Amalya C. Johnson, Scott Dhuey, Ashley Saunders, Meng-Xia Hu, Jefferson P. Dixon, Sahil Dagli, Sze-Cheung Lau, Tingting Weng, Chih-Yi Chen, Jun-Hao Zeng, Rajas Apte, Tony F. Heinz, Fang Liu, Zi-Lan Deng, Jennifer A. Dionne

Abstract: Transition metal dichalcogenides possess valley pseudospin, enabling coupling between photon spin and electron spin for classical and quantum information processing. However, rapid valley-dephasing processes have impeded the development of scalable, high-performance valleytronic devices operating at room temperature. Here we demonstrate that a chiral resonant metasurface can enable room-temperatur… ▽ More Transition metal dichalcogenides possess valley pseudospin, enabling coupling between photon spin and electron spin for classical and quantum information processing. However, rapid valley-dephasing processes have impeded the development of scalable, high-performance valleytronic devices operating at room temperature. Here we demonstrate that a chiral resonant metasurface can enable room-temperature valley-selective emission in MoSe2 monolayers independent of excitation polarization. This platform provides circular eigen-polarization states with a high quality factor (Q-factor) and strong chiral near-field enhancement. The fabricated Si chiral metasurfaces exhibit chiroptical resonances with Q-factors up to 450 at visible wavelengths. We reveal degrees of circular polarization (DOP) reaching a record high of 0.5 at room temperature. Our measurements show that the high DOP can be attributed to the significantly increased chiroptical local density of states, which enhances valley-specific radiative transition rates by a factor of ~13. Our work could facilitate the development of ultracompact chiral classical and quantum light sources. △ Less

Submitted 23 November, 2025; v1 submitted 15 September, 2024; originally announced September 2024.

Chemically Tailored Growth of 2D Semiconductors via Hybrid Metal-Organic Chemical Vapor Deposition

Authors: Zhepeng Zhang, Lauren Hoang, Marisa Hocking, Jenny Hu, Gregory Zaborski Jr., Pooja Reddy, Johnny Dollard, David Goldhaber-Gordon, Tony F. Heinz, Eric Pop, Andrew J. Mannix

Abstract: Two-dimensional (2D) semiconducting transition-metal dichalcogenides (TMDCs) are an exciting platform for new excitonic physics and next-generation electronics, creating a strong demand to understand their growth, doping, and heterostructures. Despite significant progress in solid-source (SS-) and metal-organic chemical vapor deposition (MOCVD), further optimization is necessary to grow highly cry… ▽ More Two-dimensional (2D) semiconducting transition-metal dichalcogenides (TMDCs) are an exciting platform for new excitonic physics and next-generation electronics, creating a strong demand to understand their growth, doping, and heterostructures. Despite significant progress in solid-source (SS-) and metal-organic chemical vapor deposition (MOCVD), further optimization is necessary to grow highly crystalline 2D TMDCs with controlled doping. Here, we report a hybrid MOCVD growth method that combines liquid-phase metal precursor deposition and vapor-phase organo-chalcogen delivery to leverage the advantages of both MOCVD and SS-CVD. Using our hybrid approach, we demonstrate WS$_2$ growth with tunable morphologies - from separated single-crystal domains to continuous monolayer films - on a variety of substrates, including sapphire, SiO$_2$, and Au. These WS$_2$ films exhibit narrow neutral exciton photoluminescence linewidths down to 33 meV and room-temperature mobility up to 34 - 36 cm$^2$V$^-$$^1$s$^-$$^1$). Through simple modifications to the liquid precursor composition, we demonstrate the growth of V-doped WS$_2$, MoxW$_1$$_-$$_x$S$_2$ alloys, and in-plane WS$_2$-MoS$_2$ heterostructures. This work presents an efficient approach for addressing a variety of TMDC synthesis needs on a laboratory scale. △ Less

Submitted 6 March, 2024; originally announced March 2024.

Direct Exfoliation of Nanoribbons from Bulk van der Waals Crystals

Authors: Ashley P. Saunders, Victoria Chen, Jierong Wang, Amalya C. Johnson, Amy S. McKeown-Green, Helen J. Zeng, T. Kien Mac, Tuan Trinh, Tony F. Heinz, Eric Pop, Fang Liu

Abstract: Confinement of monolayers into quasi-one-dimensional atomically-thin nanoribbons could lead to novel quantum phenomena beyond those achieved in their bulk and monolayer counterparts. However, current experimental availability of nanoribbon species beyond graphene has been limited to bottom-up synthesis or top-down patterning. In this study, we introduce a versatile and direct lithography-free appr… ▽ More Confinement of monolayers into quasi-one-dimensional atomically-thin nanoribbons could lead to novel quantum phenomena beyond those achieved in their bulk and monolayer counterparts. However, current experimental availability of nanoribbon species beyond graphene has been limited to bottom-up synthesis or top-down patterning. In this study, we introduce a versatile and direct lithography-free approach to exfoliate a variety of bulk van der Waals (vdW) crystals into nanoribbons. Akin to the Scotch tape exfoliation in producing monolayers, this technique provides convenient access to a wide range of nanoribbons derived from their corresponding bulk crystals, including MoS2, WS2, MoSe2, WSe2, MoTe2, WTe2, ReS2, and hBN. The nanoribbons are single-crystalline, parallel-aligned, flat, and have high aspect ratio. We demonstrated the electrical, magnetic, and optical properties from the confinement, strain, and edge configurations of these nanoribbons. This versatile preparation technique will pave the way for future experimental investigation and broad applications in optoelectronic, sensing, electronic and quantum devices. △ Less

Submitted 17 February, 2024; originally announced February 2024.

Comments: 18 pages, 5 figures

Millimeter-scale exfoliation of hBN with tunable flake thickness

Authors: Amy S. McKeown-Green, Helen J. Zeng, Ashley P. Saunders, Jiayi Li, Jenny Hu, Jiaojian Shi, Yuejun Shen, Feng Pan, Jennifer A. Dionne, Tony F. Heinz, Stephen Wu, Fan Zheng, Fang Liu

Abstract: As a two-dimensional (2D) dielectric material, hexagonal boron nitride (hBN) is in high demand for applications in photonics, nonlinear optics, and nanoelectronics. Unfortunately, the high-throughput preparation of macroscopic-scale, high-quality hBN flakes with controlled thickness is an ongoing challenge, limiting device fabrication and technological integration. Here, we present a metal thin-fi… ▽ More As a two-dimensional (2D) dielectric material, hexagonal boron nitride (hBN) is in high demand for applications in photonics, nonlinear optics, and nanoelectronics. Unfortunately, the high-throughput preparation of macroscopic-scale, high-quality hBN flakes with controlled thickness is an ongoing challenge, limiting device fabrication and technological integration. Here, we present a metal thin-film exfoliation method to prepare hBN flakes with millimeter-scale dimension, near-unity yields, and tunable flake thickness distribution from 1-7 layers, a substantial improvement over scotch tape exfoliation. The single crystallinity and high quality of the exfoliated hBN are demonstrated with optical microscopy, atomic force microscopy, Raman spectroscopy, and second harmonic generation. We further explore a possible mechanism for the effectiveness and selectivity based on thin-film residual stress measurements, density functional theory calculations, and transmission electron microscopy imaging of the deposited metal films. We find that the magnitude of the residual tensile stress induced by thin film deposition plays a key role in determining exfoliated flake thickness in a manner which closely resembles 3D semiconductor spalling. Lastly, we demonstrate that our exfoliated, large-area hBN flakes can be readily incorporated as encapsulating layers for other 2D monolayers. Altogether, this method brings us one step closer to the high throughput, mass production of hBN-based 2D photonic, optoelectronic, and quantum devices. △ Less

Submitted 2 November, 2023; originally announced November 2023.

Comments: 21 pages, 5 figures, work completed at Stanford University

Quantum control of exciton wavefunctions in 2D semiconductors

Authors: Jenny Hu, Etienne Lorchat, Xueqi Chen, Kenji Watanabe, Takashi Taniguchi, Tony F. Heinz, Puneet A. Murthy, Thibault Chervy

Abstract: Excitons -- bound electron-hole pairs -- play a central role in light-matter interaction phenomena, and are crucial for wide-ranging applications from light harvesting and generation to quantum information processing. A long-standing challenge in solid-state optics has been to achieve precise and scalable control over the quantum mechanical state of excitons in semiconductor heterostructures. Here… ▽ More Excitons -- bound electron-hole pairs -- play a central role in light-matter interaction phenomena, and are crucial for wide-ranging applications from light harvesting and generation to quantum information processing. A long-standing challenge in solid-state optics has been to achieve precise and scalable control over the quantum mechanical state of excitons in semiconductor heterostructures. Here, we demonstrate a technique for creating tailored and tunable potential landscapes for optically active excitons in 2D semiconductors that enables in-situ wavefunction shaping at the nanoscopic lengthscale. Using nanostructured gate electrodes, we create localized electrostatic traps for excitons in diverse geometries such as quantum dots and rings, and arrays thereof. We show independent spectral tuning of multiple spatially separated quantum dots, which allows us to bring them to degeneracy despite material disorder. Owing to the strong light-matter coupling of excitons in 2D semiconductors, we observe unambiguous signatures of confined exciton wavefunctions in optical reflection and photoluminescence measurements. Our work introduces a new approach to engineering exciton dynamics and interactions at the nanometer scale, with implications for novel optoelectronic devices, topological photonics, and many-body quantum nonlinear optics. △ Less

Submitted 11 August, 2023; originally announced August 2023.

Achiral dielectric metasurfaces for spectral and polarization control of valley specific light emission from monolayer MoS2

Authors: Yin Liu, Sze Cheung Lau, Wen-Hui Sophia Cheng, Amalya Johnson, Qitong Li, Emma Simmerman, Ouri Karni, Jack Hu, Fang Liu, Mark L. Brongersma, Tony F. Heinz, Jennifer A. Dionne

Abstract: Excitons in two-dimensional transition metal dichalcogenides have a valley degree of freedom that can be optically accessed and manipulated for quantum information processing. Here, we integrate MoS2 with achiral silicon disk array metasurfaces to enhance and control valley-specific absorption and emission. Through the coupling to the metasurface Mie modes, the intensity and lifetime of the emissi… ▽ More Excitons in two-dimensional transition metal dichalcogenides have a valley degree of freedom that can be optically accessed and manipulated for quantum information processing. Here, we integrate MoS2 with achiral silicon disk array metasurfaces to enhance and control valley-specific absorption and emission. Through the coupling to the metasurface Mie modes, the intensity and lifetime of the emission of neutral excitons, trions and defect bound excitons can be enhanced, while the spectral shape can be modified. Additionally, we demonstrate the symmetric enhancement of the degree-of-polarization (DOP) of neutral exciton and trions via valley-resolved PL measurements, and find that the DOP can be as high as 24% for exciton emission and 34% for trion emission at 100K. These results can be understood by analyzing the near-field impact of metasurface resonators on both the chiral absorption of MoS2 emitters as well as the enhanced emission from the Purcell effect. Combining Si-compatible photonic design with large-scale (mm-scale) 2D materials integration, our work makes an important step towards on-chip valleytronic applications approaching room-temperature operation. △ Less

Submitted 5 June, 2023; v1 submitted 18 December, 2022; originally announced December 2022.

Atom-Specific Probing of Electron Dynamics in an Atomic Adsorbate by Time-Resolved X-ray Spectroscopy

Authors: Simon Schreck, Elias Diesen, Martina Dell'Angela, Chang Liu, Matthew Weston, Flavio Capotondi, Hirohito Ogasawara, Jerry LaRue, Roberto Costantini, Martin Beye, Piter S. Miedema, Joakim Halldin Stenlid, Jörgen Gladh, Boyang Liu, Hsin-Yi Wang, Fivos Perakis, Filippo Cavalca, Sergey Koroidov, Peter Amann, Emanuele Pedersoli, Denys Naumenko, Ivaylo Nikolov, Lorenzo Raimondi, Frank Abild-Pedersen, Tony F. Heinz , et al. (3 additional authors not shown)

Abstract: The electronic excitation occurring on adsorbates at ultrafast time scales from optical lasers that initiate surface chemical reactions is still an open question. Here, we report the ultrafast temporal evolution of X-ray absorption spectroscopy (XAS) and X-ray emission spectroscopy (XES) of a simple well known adsorbate prototype system, namely carbon (C) atoms adsorbed on a nickel (Ni(100)) surfa… ▽ More The electronic excitation occurring on adsorbates at ultrafast time scales from optical lasers that initiate surface chemical reactions is still an open question. Here, we report the ultrafast temporal evolution of X-ray absorption spectroscopy (XAS) and X-ray emission spectroscopy (XES) of a simple well known adsorbate prototype system, namely carbon (C) atoms adsorbed on a nickel (Ni(100)) surface, following intense laser optical pumping at 400 nm. We observe ultrafast (~100 fs) changes in both XAS and XES showing clear signatures of the formation of a hot electron-hole pair distribution on the adsorbate. This is followed by slower changes on a few ps time scale, shown to be consistent with thermalization of the complete C/Ni system. Density functional theory spectrum simulations support this interpretation. △ Less

Submitted 1 November, 2022; originally announced November 2022.

Comments: 33 pages, 12 figures. Submitted to Physical Review Letters

Floquet engineering of strongly-driven excitons in monolayer tungsten disulfide

Authors: Yuki Kobayashi, Christian Heide, Amalya C. Johnson, Fang Liu, David A. Reis, Tony F. Heinz, Shambhu Ghimire

Abstract: Interactions of quantum materials with strong-laser fields can induce exotic nonequilibrium electronic states. Monolayer transition-metal dichalcogenides, a new class of direct-gap semiconductors with prominent quantum confinement, offer exceptional opportunities toward Floquet engineering of quasiparticle electron-hole states, or excitons. Strong-field driving has a potential to achieve enhanced… ▽ More Interactions of quantum materials with strong-laser fields can induce exotic nonequilibrium electronic states. Monolayer transition-metal dichalcogenides, a new class of direct-gap semiconductors with prominent quantum confinement, offer exceptional opportunities toward Floquet engineering of quasiparticle electron-hole states, or excitons. Strong-field driving has a potential to achieve enhanced control of electronic band structure, thus a possibility to open a new realm of exciton light-matter interactions. However, experimental implementation of strongly-driven excitons has so far remained out of reach. Here, we use mid-infrared laser pulses below the optical bandgap to excite monolayer tungsten disulfide up to a field strength of 0.3 V/nm, and demonstrate strong-field light dressing of excitons in the excess of a hundred millielectronvolt. Our high-sensitivity transient absorption spectroscopy further reveals formation of a virtual absorption feature below the 1s-exciton resonance, which is assigned to a light-dressed sideband from the dark 2p-exciton state. Quantum-mechanical simulations substantiate the experimental results and enable us to retrieve real-space movies of the exciton dynamics. This study advances our understanding of the exciton dynamics in the strong-field regime, and showcases the possibility of harnessing ultrafast, strong-field phenomena in device applications of two-dimensional materials. △ Less

Submitted 31 October, 2022; originally announced November 2022.

Valley-coherent quantum anomalous Hall state in AB-stacked MoTe2/WSe2 bilayers

Authors: Zui Tao, Bowen Shen, Shengwei Jiang, Tingxin Li, Lizhong Li, Liguo Ma, Wenjin Zhao, Jenny Hu, Kateryna Pistunova, Kenji Watanabe, Takashi Taniguchi, Tony F. Heinz, Kin Fai Mak, Jie Shan

Abstract: Moiré materials provide fertile ground for the correlated and topological quantum phenomena. Among them, the quantum anomalous Hall (QAH) effect, in which the Hall resistance is quantized even under zero magnetic field, is a direct manifestation of the intrinsic topological properties of a material and an appealing attribute for low-power electronics applications. The QAH effect has been observed… ▽ More Moiré materials provide fertile ground for the correlated and topological quantum phenomena. Among them, the quantum anomalous Hall (QAH) effect, in which the Hall resistance is quantized even under zero magnetic field, is a direct manifestation of the intrinsic topological properties of a material and an appealing attribute for low-power electronics applications. The QAH effect has been observed in both graphene and transition metal dichalcogenide (TMD) moiré materials. It is thought to arise from the interaction-driven valley polarization of the narrow moiré bands. Here, we show surprisingly that the newly discovered QAH state in AB-stacked MoTe2/WSe2 moiré bilayers is not valley-polarized but valley-coherent. The layer- and helicity-resolved optical spectroscopy measurement reveals that the QAH ground state possesses spontaneous spin (valley) polarization aligned (anti-aligned) in two TMD layers. In addition, saturation of the out-of-plane spin polarization in both layers occurs only under high magnetic fields, supporting a canted spin texture. Our results call for a new mechanism for the QAH effect and highlight the potential of TMD moiré materials with strong electronic correlations and spin-orbit interactions for exotic topological states. △ Less

Submitted 15 August, 2022; originally announced August 2022.

Ultrahigh quality infrared polaritonic resonators based on bottom-up-synthesized van der Waals nanoribbons

Authors: Shang-Jie Yu, Yue Jiang, John A. Roberts, Markus A. Huber, Helen Yao, Xinjian Shi, Hans A. Bechtel, Stephanie N. Gilbert Corder, Tony F. Heinz, Xiaolin Zheng, Jonathan A. Fan

Abstract: van der Waals nanomaterials supporting phonon polariton quasiparticles possess unprecedented light confinement capabilities, making them ideal systems for molecular sensing, thermal emission, and subwavelength imaging applications, but they require defect-free crystallinity and nanostructured form factors to fully showcase these capabilities. We introduce bottom-up-synthesized α-MoO3 structures as… ▽ More van der Waals nanomaterials supporting phonon polariton quasiparticles possess unprecedented light confinement capabilities, making them ideal systems for molecular sensing, thermal emission, and subwavelength imaging applications, but they require defect-free crystallinity and nanostructured form factors to fully showcase these capabilities. We introduce bottom-up-synthesized α-MoO3 structures as nanoscale phonon polaritonic systems that feature tailorable morphologies and crystal qualities consistent with bulk single crystals. α-MoO3 nanoribbons serve as low-loss hyperbolic Fabry-Pérot nanoresonators, and we experimentally map hyperbolic resonances over four Reststrahlen bands spanning the far- and mid-infrared spectral range, including resonance modes beyond the tenth order. The measured quality factors are the highest from phonon polaritonic van der Waals structures to date. We anticipate that bottom-up-synthesized polaritonic van der Waals nanostructures will serve as an enabling high-performance and low-loss platform for infrared optical and optoelectronic applications. △ Less

Submitted 10 January, 2022; originally announced January 2022.

All-optical probe of three-dimensional topological insulators based on high-harmonic generation by circularly-polarized laser fields

Authors: Denitsa Baykusheva, Alexis Chacón, Jian Lu, Trevor P. Bailey, Jonathan A. Sobota, Hadas Soifer, Patrick S. Kirchmann, Costel R. Rotundu, Ctirad Uher, Tony F. Heinz, David A. Reis, Shambhu Ghimire

Abstract: We report the observation of a novel nonlinear optical response from the prototypical three-dimensional topological insulator Bi$_2$Se$_3$ through the process of high-order harmonic generation. We find that the generation efficiency increases as the laser polarization is changed from linear to elliptical, and it becomes maximum for circular polarization. With the aid of a microscopic theory and a… ▽ More We report the observation of a novel nonlinear optical response from the prototypical three-dimensional topological insulator Bi$_2$Se$_3$ through the process of high-order harmonic generation. We find that the generation efficiency increases as the laser polarization is changed from linear to elliptical, and it becomes maximum for circular polarization. With the aid of a microscopic theory and a detailed analysis of the measured spectra, we reveal that such anomalous enhancement encodes the characteristic topology of the band structure that originates from the interplay of strong spin-orbit coupling and time-reversal symmetry protection. Our study reveals a new platform for chiral strong-field physics and presents a novel, contact-free, all-optical approach for the spectroscopy of topological insulators. The implications are in ultrafast probing of topological phase transitions, light-field driven dissipationless electronics, and quantum computation. △ Less

Submitted 30 September, 2021; originally announced September 2021.

Comments: 21 pages, 5 figures

Journal ref: Nano Lett. 2021, 21, 21, 8970-8978

Moiré-localized interlayer exciton wavefunctions captured by imaging its electron and hole constituents

Authors: Ouri Karni, Elyse Barré, Vivek Pareek, Johnathan D. Georgaras, Michael K. L. Man, Chakradhar Sahoo, David R. Bacon, Xing Zhu, Henrique B. Ribeiro, Aidan L. O'Beirne, Jenny Hu, Abdullah Al-Mahboob, Mohamed M. M. Abdelrasoul, Nicholas S. Chan, Arka Karmakar, Andrew J. Winchester, Bumho Kim, Kenji Watanabe, Takashi Taniguchi, Katayun Barmak, Julien Madéo, Felipe H. da Jornada, Tony F. Heinz, Keshav M. Dani

Abstract: Interlayer excitons (ILXs) - electron-hole pairs bound across two atomically thin layered semiconductors - have emerged as attractive platforms to study exciton condensation, single-photon emission and other quantum-information applications. Yet, despite extensive optical spectroscopic investigations, critical information about their size, valley configuration and the influence of the moiré potent… ▽ More Interlayer excitons (ILXs) - electron-hole pairs bound across two atomically thin layered semiconductors - have emerged as attractive platforms to study exciton condensation, single-photon emission and other quantum-information applications. Yet, despite extensive optical spectroscopic investigations, critical information about their size, valley configuration and the influence of the moiré potential remains unknown. Here, we captured images of the time- and momentum-resolved distribution of both the electron and the hole that bind to form the ILX in a WSe2/MoS2 heterostructure. We thereby obtain a direct measurement of the interlayer exciton diameter of ~5.4 nm, comparable to the moiré unit-cell length of 6.1 nm. Surprisingly, this large ILX is well localized within the moiré cell to a region of only 1.8 nm - smaller than the size of the exciton itself. This high degree of localization of the interlayer exciton is backed by Bethe-Salpeter equation calculations and demonstrates that the ILX can be localized within small moiré unit cells. Unlike large moiré cells, these are uniform over large regions, thus allowing the formation of extended arrays of localized excitations for quantum technology. △ Less

Submitted 4 August, 2021; originally announced August 2021.

Comments: 4 figures

Experimental measurement of the intrinsic excitonic wavefunction

Authors: Michael K. L. Man, Julien Madéo, Chakradhar Sahoo, Kaichen Xie, Marshall Campbell, Vivek Pareek, Arka Karmakar, E Laine Wong, Abdullah Al-Mahboob, Nicholas S. Chan, David R. Bacon, Xing Zhu, Mohamed Abdelrasoul, Xiaoquin Li, Tony F. Heinz, Felipe H. da Jornada, Ting Cao, Keshav M. Dani

Abstract: An exciton, a two-body composite quasiparticle formed of an electron and hole, is a fundamental optical excitation in condensed-matter systems. Since its discovery nearly a century ago, a measurement of the excitonic wavefunction has remained beyond experimental reach. Here, we directly image the excitonic wavefunction in reciprocal space by measuring the momentum distribution of electrons photoem… ▽ More An exciton, a two-body composite quasiparticle formed of an electron and hole, is a fundamental optical excitation in condensed-matter systems. Since its discovery nearly a century ago, a measurement of the excitonic wavefunction has remained beyond experimental reach. Here, we directly image the excitonic wavefunction in reciprocal space by measuring the momentum distribution of electrons photoemitted from excitons in monolayer WSe2. By transforming to real space, we obtain a visual of the distribution of the electron around the hole in an exciton. Further, by also resolving the energy coordinate, we confirm the elusive theoretical prediction that the photoemitted electron exhibits an inverted energy-momentum dispersion relationship reflecting the valence band where the partner hole remains, rather than that of conduction-band states of the electron. △ Less

Submitted 25 November, 2020; originally announced November 2020.

Comments: 27 pages

Directly visualizing the momentum forbidden dark excitons and their dynamics in atomically thin semiconductors

Authors: Julien Madéo, Michael K. L. Man, Chakradhar Sahoo, Marshall Campbell, Vivek Pareek, E Laine Wong, Abdullah Al Mahboob, Nicholas S. Chan, Arka Karmakar, Bala Murali Krishna Mariserla, Xiaoqin Li, Tony F. Heinz, Ting Cao, Keshav M. Dani

Abstract: Resolving the momentum degree of freedom of excitons - electron-hole pairs bound by the Coulomb attraction in a photoexcited semiconductor, has remained a largely elusive goal for decades. In atomically thin semiconductors, such a capability could probe the momentum forbidden dark excitons, which critically impact proposed opto-electronic technologies, but are not directly accessible via optical t… ▽ More Resolving the momentum degree of freedom of excitons - electron-hole pairs bound by the Coulomb attraction in a photoexcited semiconductor, has remained a largely elusive goal for decades. In atomically thin semiconductors, such a capability could probe the momentum forbidden dark excitons, which critically impact proposed opto-electronic technologies, but are not directly accessible via optical techniques. Here, we probe the momentum-state of excitons in a WSe2 monolayer by photoemitting their constituent electrons, and resolving them in time, momentum and energy. We obtain a direct visual of the momentum forbidden dark excitons, and study their properties, including their near-degeneracy with bright excitons and their formation pathways in the energy-momentum landscape. These dark excitons dominate the excited state distribution - a surprising finding that highlights their importance in atomically thin semiconductors. △ Less

Submitted 1 May, 2020; originally announced May 2020.

Comments: 34 pages

Journal ref: Science, 04 Dec 2020: Vol. 370, Issue 6521, pp. 1199-1204

Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe2

Authors: Jie Gu, Valentin Walther, Lutz Waldecker, Daniel Rhodes, Archana Raja, James C. Hone, Tony F. Heinz, Stephane Kena-Cohen, Thomas Pohl, Vinod M. Menon

Abstract: Strong optical nonlinearities play a central role in realizing quantum photonic technologies. In solid state systems, exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. Here, the interaction between excitons forms the basis of the polaritonic nonlinearity. While the interaction between grou… ▽ More Strong optical nonlinearities play a central role in realizing quantum photonic technologies. In solid state systems, exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. Here, the interaction between excitons forms the basis of the polaritonic nonlinearity. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such ground state interactions is generally not sufficient to reach the regime of quantum nonlinear optics and strong single-polariton interactions. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities, as demonstrated with high-lying Rydberg states of cold atomic systems. Excitons in excited states have recently been observed in monolayer transition metal dichalcogenides. Here we demonstrate the formation of exciton-polaritons using the first excited excitonic state in monolayer tungsten diselenide (WSe2) embedded in a microcavity. Owing to the larger exciton size compared to their ground state counterpart, the realized polaritons exhibit an enhanced nonlinear response by more than an order of magnitude, as evidenced through a modification of the cavity Rabi splitting. The demonstration of excited exciton-polaritons in two-dimensional semiconductors and their enhanced nonlinear response presents the first step towards the generation of strong photon interactions in solid state systems, a necessary building block for quantum photonic technologies. △ Less

Submitted 28 December, 2019; originally announced December 2019.

Rigid band shifts in two-dimensional semiconductors through environmental screening

Authors: Lutz Waldecker, Archana Raja, Malte Rösner, Christina Steinke, Aaron Bostwick, Roland J. Koch, Chris Jozwiak, Takashi Taniguchi, Kenji Watanabe, Eli Rotenberg, Tim O. Wehling, Tony F. Heinz

Abstract: We investigate the effects of environmental dielectric screening on the electronic dispersion and the band gap in the atomically-thin, quasi two-dimensional (2D) semiconductor WS$_2$ using correlative angle-resolved photoemission and optical spectroscopies, along with first-principles calculations. We find the main effect of increased environmental screening to be a reduction of the band gap, with… ▽ More We investigate the effects of environmental dielectric screening on the electronic dispersion and the band gap in the atomically-thin, quasi two-dimensional (2D) semiconductor WS$_2$ using correlative angle-resolved photoemission and optical spectroscopies, along with first-principles calculations. We find the main effect of increased environmental screening to be a reduction of the band gap, with little change to the electronic dispersion of the band structure. These essentially rigid shifts of the bands results from the special spatial structure of the changes in the Coulomb potential induced by the dielectric environment in the 2D limit. Our results suggest dielectric engineering as a non-invasive method of tailoring the band structure of 2D semiconductors and provide guidance for understanding the electronic properties of 2D materials embedded in multilayer heterostructures. △ Less

Submitted 11 July, 2019; originally announced July 2019.

Comments: 5 pages, 3 figures

Journal ref: Phys. Rev. Lett. 123, 206403 (2019)

Revealing multiple classes of stable quantum emitters in hexagonal boron nitride with correlated cathodoluminescence, photoluminescence, and strain mapping

Authors: Fariah Hayee, Leo Yu, Jingyuan Linda Zhang, Christopher J. Ciccarino, Minh Nguyen, Ann F Marshall, Igor Aharonovich, Jelena Vučković, Prineha Narang, Tony F. Heinz, Jennifer A Dionne

Abstract: Single photon emitters (SPEs) in solids have emerged as promising candidates for quantum photonic sensing, communications, and computing. Defects in hexagonal boron nitride (hBN) exhibit high-brightness, room-temperature quantum emission, but their large spectral variability and unknown local structure significantly challenge their technological utility. Here, we directly correlate hBN quantum emi… ▽ More Single photon emitters (SPEs) in solids have emerged as promising candidates for quantum photonic sensing, communications, and computing. Defects in hexagonal boron nitride (hBN) exhibit high-brightness, room-temperature quantum emission, but their large spectral variability and unknown local structure significantly challenge their technological utility. Here, we directly correlate hBN quantum emission with the material's local strain using a combination of photoluminescence (PL), cathodoluminescence (CL) and nano-beam electron diffraction. Across 40 emitters and 15 samples, we observe zero phonon lines(ZPLs) in PL and CL ranging from 540-720 nm. CL mapping reveals that multiple defects and distinct defect species located within an optically-diffraction-limited region can each contribute to the observed PL spectra. Local strain maps indicate that strain is not required to activate the emitters and is not solely responsible for the observed ZPL spectral range. Instead, four distinct defect classes are responsible for the observed emission range. One defect class has ZPLs near 615 nm with predominantly matched CL-PL responses; it is not a strain-tuned version of another defect class with ZPL emission centered at 580 nm. A third defect class at 650 nm has low visible-frequency CL emission; and a fourth defect species centered at 705 nm has a small, ~10 nm shift between its CL and PL peaks. All studied defects are stable upon both electron and optical irradiation. Our results provide an important foundation for atomic-scale optical characterization of color centers, as well as a foundation for engineering defects with precise emission properties. △ Less

Submitted 1 July, 2019; v1 submitted 17 January, 2019; originally announced January 2019.

Anisotropic structural dynamics of monolayer crystals revealed by femtosecond surface x-ray scattering

Authors: I-Cheng Tung, Aravind Krishnamoorthy, Sridhar Sadasivam, Hua Zhou, Qi Zhang, Kyle L. Seyler, Genevieve Clark, Ehren M. Mannebach, Clara Nyby, Friederike Ernst, Diling Zhu, James M. Glownia, Michael E. Kozina, Sanghoon Song, Silke Nelson, Hiroyuki Kumazoe, Fuyuki Shimojo, Rajiv K. Kalia, Priya Vashishta, Pierre Darancet, Tony F. Heinz, Aiichiro Nakano, Xiaodong Xu, Aaron M. Lindenberg, Haidan Wen

Abstract: X-ray scattering is one of the primary tools to determine crystallographic configuration with atomic accuracy. However, the measurement of ultrafast structural dynamics in monolayer crystals remains a long-standing challenge due to a significant reduction of diffraction volume and complexity of data analysis, prohibiting the application of ultrafast x-ray scattering to study nonequilibrium structu… ▽ More X-ray scattering is one of the primary tools to determine crystallographic configuration with atomic accuracy. However, the measurement of ultrafast structural dynamics in monolayer crystals remains a long-standing challenge due to a significant reduction of diffraction volume and complexity of data analysis, prohibiting the application of ultrafast x-ray scattering to study nonequilibrium structural properties at the two-dimensional limit. Here, we demonstrate femtosecond surface x-ray diffraction in combination with crystallographic model-refinement calculations to quantify the ultrafast structural dynamics of monolayer WSe$_2$ crystals supported on a substrate. We found the absorbed optical photon energy is preferably coupled to the in-plane lattice vibrations within 2 picoseconds while the out-of-plane lattice vibration amplitude remains unchanged during the first 10 picoseconds. The model-assisted fitting suggests an asymmetric intralayer spacing change upon excitation. The observed nonequilibrium anisotropic structural dynamics in two-dimensional materials agrees with first-principles nonadiabatic modeling in both real and momentum space, marking the distinct structural dynamics of monolayer crystals from their bulk counterparts. The demonstrated methods unlock the benefit of surface sensitive x-ray scattering to quantitatively measure ultrafast structural dynamics in atomically thin materials and across interfaces. △ Less

Submitted 28 November, 2018; originally announced November 2018.

Optical models for thin layers

Authors: Yilei Li, Tony F. Heinz

Abstract: We provide a systematic study of the optical models for thin layers: the 3D model, the 2D model and the linearized 2D model. We show that the 2D model is applicable for layers with small optical thicknesses. Excellent agreement of the 2D model with the 3D model is demonstrated over broad spectral ranges from DC to near UV for representative van der Waals atomic layers and thin metal layers. The li… ▽ More We provide a systematic study of the optical models for thin layers: the 3D model, the 2D model and the linearized 2D model. We show that the 2D model is applicable for layers with small optical thicknesses. Excellent agreement of the 2D model with the 3D model is demonstrated over broad spectral ranges from DC to near UV for representative van der Waals atomic layers and thin metal layers. The linearized 2D model requires additionally weak optical response. Analytical expressions for the applicability and accuracies of the optical models are derived. We discuss the advantages and limitations of the models for the purpose of measuring their optical response functions. Further, we generalize the theory to take into account in-plane anisotropy, heterostructures, and stratified substrates. Implications of the 2D model for the correct analysis of transmission attenuation and implementations of half- and total-absorption layers are discussed. △ Less

Submitted 1 January, 2018; originally announced January 2018.

Ultrafast Graphene Light Emitter

Authors: Young Duck Kim, Yuanda Gao, Ren-Jye Shiue, Lei Wang, Ozgur Burak Aslan, Myung-Ho Bae, Hyungsik Kim, Dongjea Seo, Heon-Jin Choi, Suk Hyun Kim, Andrei Nemilentsau, Tony Low, Cheng Tan, Dmitri K. Efetov, Takashi Taniguchi, Kenji Watanabe, Kenneth L. Shepard, Tony F. Heinz, Dirk Englund, James Hone

Abstract: Ultrafast electrically driven nanoscale light sources are critical components in nanophotonics. Compound semiconductor-based light sources for the nanophotonic platforms have been extensively investigated over the past decades. However, monolithic ultrafast light sources with a small footprint remain a challenge. Here, we demonstrate electrically driven ultrafast graphene light emitters that achie… ▽ More Ultrafast electrically driven nanoscale light sources are critical components in nanophotonics. Compound semiconductor-based light sources for the nanophotonic platforms have been extensively investigated over the past decades. However, monolithic ultrafast light sources with a small footprint remain a challenge. Here, we demonstrate electrically driven ultrafast graphene light emitters that achieve light pulse generation with up to 10 GHz bandwidth, across a broad spectral range from the visible to the near-infrared. The fast response results from ultrafast charge carrier dynamics in graphene, and weak electron-acoustic phonon-mediated coupling between the electronic and lattice degrees of freedom. We also find that encapsulating graphene with hexagonal boron nitride (hBN) layers strongly modifies the emission spectrum by changing the local optical density of states, thus providing up to 460 % enhancement compared to the grey-body thermal radiation for a broad peak centered at 720 nm. Furthermore, the hBN encapsulation layers permit stable and bright visible thermal radiation with electronic temperatures up to 2,000 K under ambient conditions, as well as efficient ultrafast electronic cooling via near-field coupling to hybrid polaritonic modes. These high-speed graphene light emitters provide a promising path for on-chip light sources for optical communications and other optoelectronic applications. △ Less

Submitted 24 October, 2017; originally announced October 2017.

Comments: 18 pages, 4 figures

Journal ref: Nano Letters 18, 934 (2018)

Temperature Dependent Thermal Boundary Conductance of Monolayer MoS$_2$ by Raman Thermometry

Authors: Eilam Yalon, Özgür Burak Aslan, Kirby K. H. Smithe, Connor J. McClellan, Saurabh V. Suryavanshi, Feng Xiong, Aditya Sood, Christopher M. Neumann, Xiaoqing Xu, Kenneth E. Goodson, Tony F. Heinz, Eric Pop

Abstract: The electrical and thermal behavior of nanoscale devices based on two-dimensional (2D) materials is often limited by their contacts and interfaces. Here we report the temperature-dependent thermal boundary conductance (TBC) of monolayer MoS$_2$ with AlN and SiO$_2$, using Raman thermometry with laser-induced heating. The temperature-dependent optical absorption of the 2D material is crucial in suc… ▽ More The electrical and thermal behavior of nanoscale devices based on two-dimensional (2D) materials is often limited by their contacts and interfaces. Here we report the temperature-dependent thermal boundary conductance (TBC) of monolayer MoS$_2$ with AlN and SiO$_2$, using Raman thermometry with laser-induced heating. The temperature-dependent optical absorption of the 2D material is crucial in such experiments, which we characterize here for the first time above room temperature. We obtain TBC ~ 15 MWm$^-$$^2$K$^-$$^1$ near room temperature, increasing as ~ T$^0$$^.$$^6$$^5$ in the range 300 - 600 K. The similar TBC of MoS$_2$ with the two substrates indicates that MoS$_2$ is the "softer" material with weaker phonon irradiance, and the relatively low TBC signifies that such interfaces present a key bottleneck in energy dissipation from 2D devices. Our approach is needed to correctly perform Raman thermometry of 2D materials, and our findings are key for understanding energy coupling at the nanoscale. △ Less

Submitted 8 February, 2020; v1 submitted 20 October, 2017; originally announced October 2017.

Journal ref: ACS Applied Materials & Interfaces (2017)

Bright visible light emission from graphene

Authors: Young Duck Kim, Hakseong Kim, Yujin Cho, Ji Hoon Ryoo, Cheol-Hwan Park, Pilkwang Kim, Yong Seung Kim, Sunwoo Lee, Yilei Li, Seung-Nam Park, Yong Shim Yoo, Duhee Yoon, Vincent E. Dorgan, Eric Pop, Tony F. Heinz, James Hone, Seung-Hyun Chun, Hyeonsik Cheong, Sang Wook Lee, Myung-Ho Bae, Yun Daniel Park

Abstract: Graphene and related two-dimensional materials are promising candidates for atomically thin, flexible, and transparent optoelectronics. In particular, the strong light-matter interaction in graphene has allowed for the development of state-of-the-art photodetectors, optical modulators, and plasmonic devices. In addition, electrically biased graphene on SiO2 substrates can be used as a low-efficien… ▽ More Graphene and related two-dimensional materials are promising candidates for atomically thin, flexible, and transparent optoelectronics. In particular, the strong light-matter interaction in graphene has allowed for the development of state-of-the-art photodetectors, optical modulators, and plasmonic devices. In addition, electrically biased graphene on SiO2 substrates can be used as a low-efficiency emitter in the mid-infrared range. However, emission in the visible range has remained elusive. Here we report the observation of bright visible-light emission from electrically biased suspended graphenes. In these devices, heat transport is greatly minimised; thus hot electrons (~ 2800 K) become spatially localised at the centre of graphene layer, resulting in a 1000-fold enhancement in the thermal radiation efficiency. Moreover, strong optical interference between the suspended graphene and substrate can be utilized to tune the emission spectrum. We also demonstrate the scalability of this technique by realizing arrays of chemical-vapour-deposited graphene bright visible-light emitters. These results pave the way towards the realisation of commercially viable large-scale, atomically-thin, flexible and transparent light emitters and displays with low-operation voltage, and graphene-based, on-chip ultrafast optical communications. △ Less

Submitted 13 September, 2017; originally announced September 2017.

Comments: 63 page

Journal ref: Nature Nanotechnology 2015

Excitons in atomically thin transition metal dichalcogenides

Authors: Gang Wang, Alexey Chernikov, Mikhail M. Glazov, Tony F. Heinz, Xavier Marie, Thierry Amand, Bernhard Urbaszek

Abstract: Atomically thin materials such as graphene and monolayer transition metal dichalcogenides (TMDs) exhibit remarkable physical properties resulting from their reduced dimensionality and crystal symmetry. The family of semiconducting transition metal dichalcogenides is an especially promising platform for fundamental studies of two-dimensional (2D) systems, with potential applications in optoelectron… ▽ More Atomically thin materials such as graphene and monolayer transition metal dichalcogenides (TMDs) exhibit remarkable physical properties resulting from their reduced dimensionality and crystal symmetry. The family of semiconducting transition metal dichalcogenides is an especially promising platform for fundamental studies of two-dimensional (2D) systems, with potential applications in optoelectronics and valleytronics due to their direct band gap in the monolayer limit and highly efficient light-matter coupling. A crystal lattice with broken inversion symmetry combined with strong spin-orbit interactions leads to a unique combination of the spin and valley degrees of freedom. In addition, the 2D character of the monolayers and weak dielectric screening from the environment yield a significant enhancement of the Coulomb interaction. The resulting formation of bound electron-hole pairs, or excitons, dominates the optical and spin properties of the material. Here we review recent progress in our understanding of the excitonic properties in monolayer TMDs and lay out future challenges. We focus on the consequences of the strong direct and exchange Coulomb interaction, discuss exciton-light interaction and effects of other carriers and excitons on electron-hole pairs in TMDs. Finally, the impact on valley polarization is described and the tuning of the energies and polarization observed in applied electric and magnetic fields is summarized. △ Less

Submitted 10 November, 2017; v1 submitted 18 July, 2017; originally announced July 2017.

Comments: 28 pages, 8 figures, with updated references and corrected typos [Reviews of Modern Physics - in press]

Journal ref: Rev. Mod. Phys. 90, 21001 (2018)

Approaching the Intrinsic Photoluminescence Linewidth in Transition Metal Dichalcogenide Monolayers

Authors: Obafunso A. Ajayi, Jenny V. Ardelean, Gabriella D. Shepard, Jue Wang, Abhinandan Antony, Takeshi Taniguchi, Kenji Watanabe, Tony F. Heinz, Stefan Strauf, X. -Y. Zhu, James C. Hone

Abstract: Excitonic states in monolayer transition metal dichalcogenides (TMDCs) have been the subject of extensive recent interest. Their intrinsic properties can, however, be obscured due to the influence of inhomogeneity in the external environment. Here we report methods for fabricating high quality TMDC monolayers with narrow photoluminescence (PL) linewidth approaching the intrinsic limit. We find tha… ▽ More Excitonic states in monolayer transition metal dichalcogenides (TMDCs) have been the subject of extensive recent interest. Their intrinsic properties can, however, be obscured due to the influence of inhomogeneity in the external environment. Here we report methods for fabricating high quality TMDC monolayers with narrow photoluminescence (PL) linewidth approaching the intrinsic limit. We find that encapsulation in hexagonal boron nitride (h-BN) sharply reduces the PL linewidth, and that passivation of the oxide substrate by an alkyl monolayer further decreases the linewidth and also minimizes the charged exciton (trion) peak. The combination of these sample preparation methods results in much reduced spatial variation in the PL emission, with a full-width-at-half-maximum as low as 1.7 meV. Analysis of the PL line shape yields a homogeneous width of 1.43$\pm$0.08 meV and inhomogeneous broadening of 1.1$\pm$0.3 meV. △ Less

Submitted 20 February, 2017; originally announced February 2017.

Comments: 16 pages, 4 figures

Coulomb engineering of the bandgap in 2D semiconductors

Authors: Archana Raja, Andrey Chaves, Jaeeun Yu, Ghidewon Arefe, Heather M. Hill, Albert F. Rigosi, Timothy C. Berkelbach, Philipp Nagler, Christian Schüller, Tobias Korn, Colin Nuckolls, James Hone, Louis E. Brus, Tony F. Heinz, David R. Reichman, Alexey Chernikov

Abstract: The ability to control the size of the electronic bandgap is an integral part of solid-state technology. Atomically-thin two-dimensional crystals offer a new approach for tuning the energies of the electronic states based on the interplay between the environmental sensitivity and unusual strength of the Coulomb interaction in these materials. By engineering the surrounding dielectric environment,… ▽ More The ability to control the size of the electronic bandgap is an integral part of solid-state technology. Atomically-thin two-dimensional crystals offer a new approach for tuning the energies of the electronic states based on the interplay between the environmental sensitivity and unusual strength of the Coulomb interaction in these materials. By engineering the surrounding dielectric environment, we are able to tune the electronic bandgap in monolayers of WS2 and WSe2 by hundreds of meV. We exploit this behavior to present an in-plane dielectric heterostructure with a spatially dependent bandgap, illustrating the feasibility of our approach for the creation of lateral junctions with nanoscale resolution. This successful demonstration of bandgap engineering based on the non-invasive modification of the Coulomb interaction should enable the design of a new class of atomically thin devices to advance the limits of size and functionality for solid-state technologies. △ Less

Submitted 7 February, 2017; v1 submitted 3 February, 2017; originally announced February 2017.

Magnetic brightening and control of dark excitons in monolayer WSe2

Authors: Xiao-Xiao Zhang, Ting Cao, Zhengguang Lu, Yu-Chuan Lin, Fan Zhang, Ying Wang, Zhiqiang Li, James C. Hone, Joshua A. Robinson, Dmitry Smirnov, Steven G. Louie, Tony F. Heinz

Abstract: Monolayer transition metal dichalcogenide (TMDC) crystals, as direct-gap materials with unusually strong light-matter interaction, have attracted much recent attention. In contrast to the initial understanding, the minima of the conduction band are predicted to be spin split. Because of this splitting and the spin-polarized character of the valence bands, the lowest-lying excitonic states in WX2 (… ▽ More Monolayer transition metal dichalcogenide (TMDC) crystals, as direct-gap materials with unusually strong light-matter interaction, have attracted much recent attention. In contrast to the initial understanding, the minima of the conduction band are predicted to be spin split. Because of this splitting and the spin-polarized character of the valence bands, the lowest-lying excitonic states in WX2 (X=S, Se) are expected to be spin-forbidden and optically dark. To date, however, there has been no direct experimental probe of these dark band-edge excitons, which strongly influence the light emission properties of the material. Here we show how an in-plane magnetic field can brighten the dark excitonic states and allow their properties to be revealed experimentally in monolayer WSe2. In particular, precise energy levels for both the neutral and charged dark excitons were obtained and compared with ab-initio calculations using the GW-BSE approach. Greatly increased emission and valley lifetimes were observed for the brightened dark states as a result of their spin configuration. These studies directly probe the excitonic spin manifold and provide a new route to tune the optical and valley properties of these prototypical two-dimensional semiconductors. △ Less

Submitted 12 December, 2016; originally announced December 2016.

Comments: 10 pages, 4 figures

Journal ref: Nature Nanotechnology 12, 883-888 (2017)

Measurement of the optical dielectric function of transition metal dichalcogenide monolayers: MoS2, MoSe2, WS2 and WSe2

Authors: Yilei Li, Alexey Chernikov, Xian Zhang, Albert Rigosi, Heather M. Hill, Arend M. van der Zande, Daniel A. Chenet, En-Min Shih, James Hone, Tony F. Heinz

Abstract: We report a determination of the complex in-plane dielectric function of monolayers of four transition metal dichalcogenides: MoS2, MoSe2, WS2 and WSe2, for photon energies from 1.5 - 3 eV. The results were obtained from reflection spectra using a Kramers-Kronig constrained variational analysis. From the dielectric functions, we obtain the absolute absorbance of the monolayers. We also provide a c… ▽ More We report a determination of the complex in-plane dielectric function of monolayers of four transition metal dichalcogenides: MoS2, MoSe2, WS2 and WSe2, for photon energies from 1.5 - 3 eV. The results were obtained from reflection spectra using a Kramers-Kronig constrained variational analysis. From the dielectric functions, we obtain the absolute absorbance of the monolayers. We also provide a comparison of the dielectric function for the monolayers with the corresponding bulk materials. △ Less

Submitted 14 October, 2016; originally announced October 2016.

Journal ref: Phys. Rev. B 90, 205422 (2014)

Polaritons in layered 2D materials

Authors: Tony Low, Andrey Chaves, Joshua D. Caldwell, Anshuman Kumar, Nicholas X. Fang, Phaedon Avouris, Tony F. Heinz, Francisco Guinea, Luis Martin-Moreno, Frank Koppens

Abstract: In recent years, enhanced light-matter interactions through a plethora of dipole-type polaritonic excitations have been observed in two-dimensional (2D) layered materials. In graphene, electrically tunable and highly confined plasmon-polaritons were predicted and observed, opening up opportunities for optoelectronics, bio-sensing and other mid-infrared applications. In hexagonal boron nitride (hBN… ▽ More In recent years, enhanced light-matter interactions through a plethora of dipole-type polaritonic excitations have been observed in two-dimensional (2D) layered materials. In graphene, electrically tunable and highly confined plasmon-polaritons were predicted and observed, opening up opportunities for optoelectronics, bio-sensing and other mid-infrared applications. In hexagonal boron nitride (hBN), low-loss infrared-active phonon-polaritons exhibit hyperbolic behavior for some frequencies, allowing for ray-like propagation exhibiting high quality factors and hyperlensing effects. In transition metal dichalcogenides (TMDs), reduced screening in the 2D limit leads to optically prominent excitons with large binding energy, with these polaritonic modes having been recently observed with scanning near field optical microscopy (SNOM). Here, we review recent progress in state-of-the-art experiments, survey the vast library of polaritonic modes in 2D materials, their optical spectral properties, figures-of-merit and application space. Taken together, the emerging field of 2D material polaritonics and their hybrids provide enticing avenues for manipulating light-matter interactions across the visible, infrared to terahertz spectral ranges, with new optical control beyond what can be achieved using traditional bulk materials. △ Less

Submitted 7 July, 2017; v1 submitted 14 October, 2016; originally announced October 2016.

Journal ref: Nature Materials 16, 182--194 (2017)

Ultrafast Manipulation of Valley Pseudospin

Authors: Ziliang Ye, Dezheng Sun, Tony F. Heinz

Abstract: The coherent manipulation of spin and pseudospin underlies existing and emerging quantum technologies, including NMR, quantum communication, and quantum computation. Valley polarization, associated with the occupancy of degenerate, but quantum mechanically distinct valleys in momentum space, closely resembles spin polarization and has been proposed as a pseudospin carrier for the future quantum el… ▽ More The coherent manipulation of spin and pseudospin underlies existing and emerging quantum technologies, including NMR, quantum communication, and quantum computation. Valley polarization, associated with the occupancy of degenerate, but quantum mechanically distinct valleys in momentum space, closely resembles spin polarization and has been proposed as a pseudospin carrier for the future quantum electronics. Valley exciton polarization has been created in the transition metal dichalcogenide (TMDC) monolayers using excitation by circularly polarized light and has been detected both optically and electrically. In addition, the existence of coherence in the valley pseudospin has been identified experimentally. The manipulation of such valley coherence has, however, remained out of reach. Here we demonstrate an all-optical control of the valley coherence by means of the pseudomagnetic field associated with the optical Stark effect. Using below-bandgap circularly polarized light, we experimentally rotate the valley exciton pseudospin in monolayer WSe2 on the femtosecond time scale. Both the direction and speed of the rotation can be optically manipulated by tuning the dynamic phase of excitons in opposite valleys. This study completes the generation-manipulation-detection paradigm for valley pseudospin, enabling the platform of excitons in 2D materials for the control of this novel degree of freedom in solids. △ Less

Submitted 21 June, 2016; originally announced June 2016.

Comments: 9 pages, 4 figures

Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

Authors: Malte Selig, Gunnar Berghäuser, Archana Raja, Philipp Nagler, Christian Schüller, Tony F. Heinz, Tobias Korn, Alexey Chernikov, Ermin Malic, Andreas Knorr

Abstract: Atomically thin transition metal dichalcogenides (TMDs) are direct-gap semiconductors with strong light-matter and Coulomb interaction. The latter accounts for tightly bound excitons, which dominate the optical properties of these technologically promising materials. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in… ▽ More Atomically thin transition metal dichalcogenides (TMDs) are direct-gap semiconductors with strong light-matter and Coulomb interaction. The latter accounts for tightly bound excitons, which dominate the optical properties of these technologically promising materials. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. In a recent study, an experimental evidence for the existence of such dark states has been demonstrated, as well as their strong impact on the quantum efficiency of light emission in TMDs. Here, we reveal the microscopic origin of the excitonic coherence lifetime in two representative TMD materials (WS$_2$ and MoSe$_2$) within a joint study combining microscopic theory with optical experiments. We show that the excitonic coherence lifetime is determined by phonon-induced intra- and intervalley scattering into dark excitonic states. Remarkably, and in accordance with the theoretical prediction, we find an efficient exciton relaxation in WS$_2$ through phonon emission at all temperatures. △ Less

Submitted 11 May, 2016; originally announced May 2016.

Journal ref: Nature Communications 7, Article number: 13279 (2016)

Local polar fluctuations in lead halide perovskite crystals

Authors: Omer Yaffe, Yinsheng Guo, Liang Z. Tan, David A. Egger, Trevor Hull, Constantinos C. Stoumpos, Fan Zheng, Tony F. Heinz, Leeor Kronik, Mercouri G. Kanatzidis, Jonathan S Owen, Andrew M. Rappe, Marcos A. Pimenta, Louis E. Brus

Abstract: Hybrid lead-halide perovskites have emerged as an excellent class of photovoltaic materials. Recent reports suggest that the organic molecular cation is responsible for local polar fluctuations that inhibit carrier recombination. We combine low frequency Raman scattering with first-principles molecular dynamics (MD) to study the fundamental nature of these local polar fluctuations. Our observation… ▽ More Hybrid lead-halide perovskites have emerged as an excellent class of photovoltaic materials. Recent reports suggest that the organic molecular cation is responsible for local polar fluctuations that inhibit carrier recombination. We combine low frequency Raman scattering with first-principles molecular dynamics (MD) to study the fundamental nature of these local polar fluctuations. Our observations of a strong central peak in both hybrid (CH$_3$NH$_3$PbBr$_3$) and all-inorganic (CsPbBr$_3$) lead-halide perovskites show that anharmonic, local polar fluctuations are intrinsic to the general lead-halide perovskite structure, and not unique to the dipolar organic cation. MD simulations show that head-to-head Cs motion coupled to Br face expansion, on a few hundred femtosecond time scale, drives the local polar fluctuations in CsPbBr$_3$. △ Less

Submitted 10 February, 2017; v1 submitted 27 April, 2016; originally announced April 2016.

Journal ref: Phys. Rev. Lett. 118, 136001 (2017)

Valley Splitting and Polarization by the Zeeman Effect in Monolayer MoSe2

Authors: Yilei Li, Jonathan Ludwig, Tony Low, Alexey Chernikov, Xu Cui, Ghidewon Arefe, Young Duck Kim, Arend M. van der Zande, Albert Rigosi, Heather M. Hill, Suk Hyun Kim, James Hone, Zhiqiang Li, Dmitry Smirnov, Tony F. Heinz

Abstract: We have measured circularly polarized photoluminescence in monolayer MoSe2 under perpendicular magnetic fields up to 10 T. At low doping densities, the neutral and charged excitons shift linearly with field strength at a rate of $\mp$ 0.12 meV/T for emission arising, respectively, from the K and K' valleys. The opposite sign for emission from different valleys demonstrates lifting of the valley de… ▽ More We have measured circularly polarized photoluminescence in monolayer MoSe2 under perpendicular magnetic fields up to 10 T. At low doping densities, the neutral and charged excitons shift linearly with field strength at a rate of $\mp$ 0.12 meV/T for emission arising, respectively, from the K and K' valleys. The opposite sign for emission from different valleys demonstrates lifting of the valley degeneracy. The magnitude of the Zeeman shift agrees with predicted magnetic moments for carriers in the conduction and valence bands. The relative intensity of neutral and charged exciton emission is modified by the magnetic field, reflecting the creation of field-induced valley polarization. At high doping levels, the Zeeman shift of the charged exciton increases to $\mp$ 0.18 meV/T. This enhancement is attributed to many-body effects on the binding energy of the charged excitons. △ Less

Submitted 30 September, 2014; originally announced September 2014.

Journal ref: Phys. Rev. Lett. 113, 266804 (2014)

Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2

Authors: Alexey Chernikov, Timothy C. Berkelbach, Heather M. Hill, Albert Rigosi, Yilei Li, Ozgur B. Aslan, David R. Reichman, Mark S. Hybertsen, Tony F. Heinz

Abstract: We have experimentally determined the energies of the ground and first four excited excitonic states of the fundamental optical transition in monolayer WS2, a model system for the growing class of atomically thin two-dimensional semiconductor crystals. From the spectra, we establish a large exciton binding energy of 0.32 eV and a pronounced deviation from the usual hydrogenic Rydberg series of ene… ▽ More We have experimentally determined the energies of the ground and first four excited excitonic states of the fundamental optical transition in monolayer WS2, a model system for the growing class of atomically thin two-dimensional semiconductor crystals. From the spectra, we establish a large exciton binding energy of 0.32 eV and a pronounced deviation from the usual hydrogenic Rydberg series of energy levels of the excitonic states. We explain both of these results using a microscopic theory in which the non-local nature of the effective dielectric screening modifies the functional form of the Coulomb interaction. These strong but unconventional electron-hole interactions are expected to be ubiquitous in atomically thin materials. △ Less

Submitted 2 September, 2014; v1 submitted 17 March, 2014; originally announced March 2014.

Comments: published version

Journal ref: Phys. Rev. Lett. 113, 076802 (2014)

Atomically thin p-n junctions with van der Waals heterointerfaces

Authors: Chul-Ho Lee, Gwan-Hyoung Lee, Arend M. van der Zande, Wenchao Chen, Yilei Li, Minyong Han, Xu Cui, Ghidewon Arefe, Colin Nuckolls, Tony F. Heinz, Jing Guo, James Hone, Philip Kim

Abstract: Semiconductor p-n junctions are essential building blocks for modern electronics and optoelectronics. In conventional semiconductors, a p-n junction produces depletion regions of free charge carriers at equilibrium and built-in potentials associated with uncompensated dopant atoms. Carrier transport across the junction occurs by diffusion and drift processes defined by the spatial extent of this r… ▽ More Semiconductor p-n junctions are essential building blocks for modern electronics and optoelectronics. In conventional semiconductors, a p-n junction produces depletion regions of free charge carriers at equilibrium and built-in potentials associated with uncompensated dopant atoms. Carrier transport across the junction occurs by diffusion and drift processes defined by the spatial extent of this region. With the advent of atomically thin van der Waals (vdW) materials and their heterostructures, we are now able to realize a p-n junction at the ultimate quantum limit. In particular, vdW junctions composed of p- and n-type semiconductors each just one unit cell thick are predicted to exhibit completely different charge transport characteristics than bulk junctions. Here we report the electronic and optoelectronic characterization of atomically thin p-n heterojunctions fabricated using vdW assembly of transition metal dichalcogenides (TMDCs). Across the p-n interface, we observe gate-tuneable diode-like current rectification and photovoltaic response. We find that the tunnelling-assisted interlayer recombination of the majority carriers is responsible for the tunability of the electronic and optoelectronic processes. Sandwiching an atomic p-n junction between graphene layers enhances collection of the photoexcited carriers. The atomically scaled vdW p-n heterostructures presented here constitute the ultimate quantum limit for functional electronic and optoelectronic components. △ Less

Submitted 12 March, 2014; originally announced March 2014.

Comments: 29 pages, 3 figures in main & 10 figures in supplementary information

Journal ref: Nature Nanotech. 9, 676-681 (2014)

Tuning many-body interactions in graphene: The effects of doping on excitons and carrier lifetimes

Authors: Kin Fai Mak, Felipe H. da Jornada, Keliang He, Jack Deslippe, Nicholas Petrone, James Hone, Jie Shan, Steven G. Louie, Tony F. Heinz

Abstract: The optical properties of graphene are strongly affected by electron-electron (e-e) and electron-hole (e-h) interactions. Here we tune these many-body interactions through varying the density of free charge carriers. Measurements from the infrared to the ultraviolet reveal significant changes in the optical conductivity of graphene for both electron and hole doping. The shift, broadening, and modi… ▽ More The optical properties of graphene are strongly affected by electron-electron (e-e) and electron-hole (e-h) interactions. Here we tune these many-body interactions through varying the density of free charge carriers. Measurements from the infrared to the ultraviolet reveal significant changes in the optical conductivity of graphene for both electron and hole doping. The shift, broadening, and modification in shape of the saddle-point exciton resonance reflect strong screening of the many-body interactions by the carriers, as well as changes in quasi-particle lifetimes. Ab initio calculations by the GW Bethe-Salpeter equation (GW-BSE), which take into account modification of both the repulsive e-e and the attractive e-h interactions, provide excellent agreement with experiment. Understanding the optical properties and high-energy carrier dynamics of graphene over a wide range of doping is crucial for both fundamental graphene physics and for emerging applications of graphene in photonics. △ Less

Submitted 27 December, 2013; originally announced December 2013.

Comments: 11 pages, 4 figures, plus supplementary materials

Competing thermodynamic and dynamic factors select molecular assemblies on a gold surface

Authors: Thomas K. Haxton, Hui Zhou, Isaac Tamblyn, Daejin Eom, Zonghai Hu, Jeffrey B. Neaton, Tony F. Heinz, Stephen Whitelam

Abstract: Controlling the self-assembly of surface-adsorbed molecules into nanostructures requires understanding physical mechanisms that act across multiple length and time scales. By combining scanning tunneling microscopy with hierarchical ab initio and statistical mechanical modeling of 1,4-substituted benzenediamine (BDA) molecules adsorbed on a gold (111) surface, we demonstrate that apparently simple… ▽ More Controlling the self-assembly of surface-adsorbed molecules into nanostructures requires understanding physical mechanisms that act across multiple length and time scales. By combining scanning tunneling microscopy with hierarchical ab initio and statistical mechanical modeling of 1,4-substituted benzenediamine (BDA) molecules adsorbed on a gold (111) surface, we demonstrate that apparently simple nanostructures are selected by a subtle competition of thermodynamics and dynamics. Of the collection of possible BDA nanostructures mechanically stabilized by hydrogen bonding, the interplay of intermolecular forces, surface modulation, and assembly dynamics select at low temperature a particular subset: low free energy oriented linear chains of monomers, and high free energy branched chains. △ Less

Submitted 28 November, 2013; originally announced November 2013.

Comments: 6 pages, 4 figures

Journal ref: Phys. Rev. Lett. 111 265701 (2013)

Controlling the Spontaneous Emission Rate of Monolayer MoS$_2$ in a Photonic Crystal Nanocavity

Authors: Xuetao Gan, Yuanda Gao, Kin Fai Mak, Xinwen Yao, Ren-Jye Shiue, Arend van der Zande, Matthew Trusheim, Fariba Hatami, Tony F. Heinz, James Hone, Dirk Englund

Abstract: We report on controlling the spontaneous emission (SE) rate of a molybdenum disulfide (MoS$_2$) monolayer coupled with a planar photonic crystal (PPC) nanocavity. Spatially resolved photoluminescence (PL) mapping shows strong variations of emission when the MoS$_2$ monolayer is on the PPC cavity, on the PPC lattice, on the air gap, and on the unpatterned gallium phosphide substrate. Polarization d… ▽ More We report on controlling the spontaneous emission (SE) rate of a molybdenum disulfide (MoS$_2$) monolayer coupled with a planar photonic crystal (PPC) nanocavity. Spatially resolved photoluminescence (PL) mapping shows strong variations of emission when the MoS$_2$ monolayer is on the PPC cavity, on the PPC lattice, on the air gap, and on the unpatterned gallium phosphide substrate. Polarization dependences of the cavity-coupled MoS$_2$ emission show a more than 5 times stronger extracted PL intensity than the un-coupled emission, which indicates an underlying cavity mode Purcell enhancement of MoS$_2$ SE rate exceeding a factor of 70. △ Less

Submitted 3 October, 2013; originally announced October 2013.

Comments: 8 pages, 3 figures

Tunable electronic correlation effects in nanotube-light interactions

Authors: Yuhei Miyauchi, Zhengyi Zhang, Mitsuhide Takekoshi, Yuh Tomio, Hidekatsu Suzuura, Vasili Perebeinos, Vikram V. Deshpande, Chenguang Lu, Stéphane Berciaud, Philip Kim, James Hone, Tony F. Heinz

Abstract: Electronic many-body correlation effects in one-dimensional (1D) systems such as carbon nanotubes have been predicted to modify strongly the nature of photoexcited states. Here we directly probe this effect using broadband elastic light scattering from individual suspended carbon nanotubes under electrostatic gating conditions. We observe significant shifts in optical transition energies, as well… ▽ More Electronic many-body correlation effects in one-dimensional (1D) systems such as carbon nanotubes have been predicted to modify strongly the nature of photoexcited states. Here we directly probe this effect using broadband elastic light scattering from individual suspended carbon nanotubes under electrostatic gating conditions. We observe significant shifts in optical transition energies, as well as line broadening, as the carrier density is increased. The results demonstrate the differing role of screening of many-body electronic interactions on the macroscopic and microscopic length scales, a feature inherent to quasi-1D systems. Our findings further demonstrate the possibility of electrical tuning of optical transitions and provide a basis for understanding of various optical phenomena in carbon nanotubes and other quasi-1D systems in the presence of charge carrier doping. △ Less

Submitted 2 September, 2013; v1 submitted 25 August, 2013; originally announced August 2013.

Comments: 18 pages, 4 figures, plus supplemental material of 11 pages and 3 figures

Journal ref: Phys. Rev. B 92, 205407 (2015)

Intrinsic lineshape of the Raman 2D-mode in freestanding graphene monolayers

Authors: Stéphane Berciaud, Xianglong Li, Han Htoon, Louis E. Brus, Stephen K. Doorn, Tony F. Heinz

Abstract: We report a comprehensive study of the two-phonon inter-valley (2D) Raman mode in graphene monolayers, motivated by recent reports of asymmetric 2D-mode lineshapes in freestanding graphene. For photon energies in the range $1.53 \rm eV - 2.71 \rm eV$, the 2D-mode Raman response of freestanding samples appears as bimodal, in stark contrast with the Lorentzian approximation that is commonly used for… ▽ More We report a comprehensive study of the two-phonon inter-valley (2D) Raman mode in graphene monolayers, motivated by recent reports of asymmetric 2D-mode lineshapes in freestanding graphene. For photon energies in the range $1.53 \rm eV - 2.71 \rm eV$, the 2D-mode Raman response of freestanding samples appears as bimodal, in stark contrast with the Lorentzian approximation that is commonly used for supported monolayers. The transition between the freestanding and supported cases is mimicked by electrostatically doping freestanding graphene at carrier densities above $2\times 10^{11} \rm cm^{-2}$. This result quantitatively demonstrates that low levels of charging can obscure the intrinsically bimodal 2D-mode lineshape of monolayer graphene, which can be utilized as a signature of a quasi-neutral sample. In pristine freestanding graphene, we observe a broadening of the 2D-mode feature with decreasing photon energy that cannot be rationalized using a simple one-dimensional model based on resonant \textit{inner} and \textit{outer} processes. This indicates that phonon wavevectors away from the high-symmetry lines of the Brillouin zone must contribute to the 2D-mode, so that a full two-dimensional calculation is required to properly describe multiphonon-resonant Raman processes. △ Less

Submitted 30 May, 2013; originally announced May 2013.

Journal ref: Nano Lett., 13, 3517 (2013)

Tunable Infrared Phonon Anomalies in Trilayer Graphene

Authors: Chun Hung Lui, Emmanuele Cappelluti, Zhiqiang Li, Tony F. Heinz

Abstract: Trilayer graphene in both ABA (Bernal) and ABC (rhombohedral) stacking sequences is shown to exhibit intense infrared absorption from in-plane optical phonons. The feature, lying at ~1580 cm-1, changes strongly with electrostatic gating. For ABC-stacked graphene trilayers, we observed a large enhancement in phonon absorption amplitude, as well as softening of the phonon mode, as the Fermi level is… ▽ More Trilayer graphene in both ABA (Bernal) and ABC (rhombohedral) stacking sequences is shown to exhibit intense infrared absorption from in-plane optical phonons. The feature, lying at ~1580 cm-1, changes strongly with electrostatic gating. For ABC-stacked graphene trilayers, we observed a large enhancement in phonon absorption amplitude, as well as softening of the phonon mode, as the Fermi level is tuned away from charge neutrality. A similar, but substantially weaker effect is seen in samples with the more common ABA stacking order. The strong infrared response of the optical phonons and the pronounced variation with electrostatic gating and stacking-order reflect the interactions of the phonons and electronic excitations in the two systems. The key experimental findings can be reproduced within a simplified charged-phonon model that considers the influence of charging through Pauli blocking of the electronic transitions. △ Less

Submitted 21 January, 2013; originally announced January 2013.

Comments: 11 pages, 5 figures, supplemental material included

Journal ref: Phys. Rev. Lett. 110, 185504 (2013)

Grains and grain boundaries in highly crystalline monolayer molybdenum disulfide

Authors: Arend M. van der Zande, Pinshane Y. Huang, Daniel A. Chenet, Timothy C. Berkelbach, Youmeng You, Gwan-Hyoung Lee, Tony F. Heinz, David R. Reichman, David A. Muller, James C. Hone

Abstract: Recent progress in large-area synthesis of monolayer molybdenum disulfide, a new two-dimensional direct-bandgap semiconductor, is paving the way for applications in atomically thin electronics. Little is known, however, about the microstructure of this material. Here we have refined chemical vapor deposition synthesis to grow highly crystalline islands of monolayer molybdenum disulfide up to 120 u… ▽ More Recent progress in large-area synthesis of monolayer molybdenum disulfide, a new two-dimensional direct-bandgap semiconductor, is paving the way for applications in atomically thin electronics. Little is known, however, about the microstructure of this material. Here we have refined chemical vapor deposition synthesis to grow highly crystalline islands of monolayer molybdenum disulfide up to 120 um in size with optical and electrical properties comparable or superior to exfoliated samples. Using transmission electron microscopy, we correlate lattice orientation, edge morphology, and crystallinity with island shape to demonstrate that triangular islands are single crystals. The crystals merge to form faceted tilt and mirror boundaries that are stitched together by lines of 8- and 4- membered rings. Density functional theory reveals localized mid-gap states arising from these 8-4 defects. We find that mirror boundaries cause strong photoluminescence quenching while tilt boundaries cause strong enhancement. In contrast, the boundaries only slightly increase the measured in-plane electrical conductivity. △ Less

Submitted 9 January, 2013; originally announced January 2013.

High-Contrast Electro-Optic Modulation of a Photonic Crystal Nanocavity by Electrical Gating of Graphene

Authors: Xuetao Gan, Ren-Jye Shiue, Yuanda Gao, Kin Fai Mak, Xinwen Yao, Luozhou Li, Attila Szep, Dennis Walker Jr., James Hone, Tony F. Heinz, Dirk Englund

Abstract: We demonstrate a high-contrast electro-optic modulation of a photonic crystal nanocavity integrated with an electrically gated monolayer graphene. A high quality (Q) factor air-slot nanocavity design is employed for high overlap between the optical field and graphene sheet. Tuning of graphene's Fermi level up to 0.8 eV enables efficient control of its complex dielectric constant, which allows modu… ▽ More We demonstrate a high-contrast electro-optic modulation of a photonic crystal nanocavity integrated with an electrically gated monolayer graphene. A high quality (Q) factor air-slot nanocavity design is employed for high overlap between the optical field and graphene sheet. Tuning of graphene's Fermi level up to 0.8 eV enables efficient control of its complex dielectric constant, which allows modulation of the cavity reflection in excess of 10 dB for a swing voltage of only 1.5 V. We also observe a controllable resonance wavelength shift close to 2 nm around a wavelength of 1570 nm and a Q factor modulation in excess of three. These observations allow cavity-enhanced measurements of the graphene complex dielectric constant under different chemical potentials, in agreement with a theoretical model of the graphene dielectric constant under gating. This graphene-based nanocavity modulation demonstrates the feasibility of high-contrast, low-power frequency-selective electro-optic nanocavity modulators in graphene-integrated silicon photonic chips. △ Less

Submitted 2 November, 2012; originally announced November 2012.

Comments: 9 pages, 4 figures