Christina A. C. Garcia, Jennifer Coulter, and Prineha Narang. 1/23/2020. “Optoelectronic Response of Type-I Weyl Semimetals TaAs and NbAs from First Principles.” Physical Review Research, 2, 013073. Publisher's VersionAbstract
Weyl semimetals are materials with topologically nontrivial band structure both in the bulk and on the surface, hosting chiral nodes which are sinks and sources of Berry curvature. Weyl semimetals have been predicted, and recently measured, to exhibit large nonlinear optical responses. This discovery, along with their high mobilities, makes Weyl semimetals relevant to a broad spectrum of applications in optoelectronic, nanophotonic and quantum optical devices. While there is growing interest in understanding and characterizing the linear and nonlinear behavior of Weyl semimetals, an ab initio calculation of the linear optical and optoelectronic responses at finite temperature remains largely unexplored. Here, we specifically address the temperature dependence of the linear optical response in type-I Weyl semimetals TaAs and NbAs. We evaluate from first principles the scattering lifetimes due to electron-phonon and electron-electron interaction and incorporate these lifetimes in evaluating an experimentally relevant frequency-, polarization- and temperature-dependent complex dielectric function for each semimetal. From these calculations we present linear optical conductivity predictions which agree well where experiment exists (for TaAs) and guide the way for future measurements of type-I Weyl semimetals. Importantly, we also examine the optical conductivity's dependence on the chemical potential, a crucial physical parameter which can be controlled experimentally and can elucidate the role of the Weyl nodes in optoelectronic response. Through this work, we present design principles for Weyl optoelectronic devices that use photogenerated carriers in type-I Weyl semimetals.
Christopher J. Ciccarino, Johannes Flick, Isaac B. Harris, Matthew E. Trusheim, Dirk R. Englund, and Prineha Narang. 1/21/2020. “Strong Spin-Orbit Quenching via the Product Jahn-Teller Effect in Neutral Group IV Artificial Atom Qubits in Diamond.” arXiv. Publisher's VersionAbstract
Artificial atom qubits in diamond have emerged as leading candidates for a range of solid-state quantum systems, from quantum sensors to repeater nodes in memory-enhanced quantum communication. Inversion-symmetric group IV vacancy centers, comprised of Si, Ge, Sn and Pb dopants, hold particular promise as their neutrally charged electronic configuration results in a ground-state spin triplet, enabling long spin coherence above cryogenic temperatures. However, despite the tremendous interest in these defects, a theoretical understanding of the electronic and spin structure of these centers remains elusive. In this context, we predict the ground- and excited-state properties of the neutral group IV color centers from first principles. We capture the product Jahn-Teller effect found in the excited state manifold to second order in electron-phonon coupling, and present a non-perturbative treatment of the effect of spin-orbit coupling. Importantly, we find that spin-orbit splitting is strongly quenched due to the dominant Jahn-Teller effect, with the lowest optically-active 3Eu state weakly split into ms-resolved states. The predicted complex vibronic spectra of the neutral group IV color centers are essential for their experimental identification and have key implications for use of these systems in quantum information science.
Jennifer Coulter, Gavin B. Osterhoudt, Christina A. C. Garcia, Yiping Wang, Vincent Plisson, Bing Shen, Ni Ni, Kenneth S. Burch, and Prineha Narang. 12/24/2019. “Uncovering Electron-Phonon Scattering and Phonon Dynamics in Type-I Weyl Semimetals.” Physical Review B, 100, 220301(R). Publisher's VersionAbstract
Weyl semimetals are 3D phases of matter with topologically protected states that have remarkable macroscopic transport behaviors. As phonon dynamics and electron-phonon scattering play a critical role in the electrical and thermal transport, we pursue a fundamental understanding of the origin of these effects in type-I Weyl semimetals NbAs and TaAs. In the temperature-dependent Raman spectra of NbAs, we reveal a previously unreported Fano lineshape, a signature stemming from the electron-phonon interaction. Additionally, the temperature dependence of the A1 phonon linewidths in both NbAs and TaAs strongly deviate from the standard model of anharmonic decay. To capture the mechanisms responsible for the observed Fano asymmetry and the atypical phonon linewidth, we present first principles calculations of the phonon self-energy correction due to the electron-phonon interaction. Finally, we investigate the relationship between Fano lineshape, electron-phonon coupling, and locations of the Weyl points in these materials. Through this study of the phonon dynamics and electron-phonon interaction in these Weyl semimetals, we consider specific microscopic pathways which contribute to the nature of their macroscopic transport.
Dominik M. Juraschek, Quintin N. Meier, and Prineha Narang. 12/16/2019. “Parametric excitation of an optically silent Goldstone-like phonon mode.” arXiv. Publisher's VersionAbstract
It has recently been indicated that the hexagonal manganites exhibit Higgs- and Goldstone-like phonon modes that modulate the amplitude and phase of their primary order parameter. Here, we describe a mechanism by which a silent Goldstone-like phonon mode can be coherently excited, which is based on nonlinear coupling to an infrared-active Higgs-like phonon mode. Using a combination of first-principles calculations and phenomenological modeling, we describe the coupled Higgs-Goldstone dynamics in response to the excitation with a terahertz pulse. Besides theoretically demonstrating coherent control of crystallographic Higgs and Goldstone excitations, we show that the previously inaccessible silent phonon modes can be excited coherently with this mechanism.
Tomáš Neuman, Matthew Trusheim, and Prineha Narang. 12/12/2019. “Selective control of photon-mediated qubit-qubit interactions.” arXiv. Publisher's VersionAbstract
Quantum technologies such as quantum sensing, quantum imaging, quantum communications, and quantum computing rely on the ability to actively manipulate the quantum state of light and matter. Quantum emitters, such as color centers trapped in solids, are a useful platform for the realization of elementary building blocks (qubits) of quantum information systems. In particular, the modular nature of such solid-state devices opens up the possibility to connect them into quantum networks and create non-classical states of light shared among many qubits. The function of a quantum network relies on efficient and controllable interactions among individual qubits. In this context, we present a scheme where optically active qubits of differing excitation energies are mutually coupled via a dispersive interaction with a shared mode of an optical cavity. This generally off-resonant interaction is prohibitive of direct exchange of information among the qubits. However, we propose a scheme in which by acoustically modulating the qubit excitation energies it is in fact possible to tune to resonance a pre-selected pair of qubits and thus open a communication channel between them. This method potentially enables fast (∼ns) and parallelizable on-demand control of a large number of physical qubits. We develop an analytical and a numerical theoretical model demonstrating this principle and suggest feasible experimental scenarios to test the theoretical predictions.
Dominik M. Juraschek, Tomáš Neuman, Johannes Flick, and Prineha Narang. 11/30/2019. “Cavity control of nonlinear phononics.” arXiv. Publisher's VersionAbstract
Nonlinear interactions between phonon modes govern the behavior of vibrationally highly excited solids and molecules. Here, we demonstrate theoretically that optical cavities can be used to control the redistribution of energy from a highly excited coherent infrared-active phonon state into the other vibrational degrees of freedom of the system. The hybridization of the infrared-active phonon mode with the fundamental mode of the cavity induces a polaritonic splitting that we use to tune the nonlinear interactions with other vibrational modes in and out of resonance. We show that not only can the efficiency of the redistribution of energy be enhanced or decreased, but also the underlying scattering mechanisms may be changed. This work introduces the concept of cavity control to the field of nonlinear phononics, enabling nonequilibrium quantum optical engineering of new states of matter.
Dominik M. Juraschek, Prineha Narang, and Nicola A. Spaldin. 11/30/2019. “Phono-magnetic analogs to opto-magnetic effects.” arXiv. Publisher's VersionAbstract
The magneto-optical and opto-magnetic effects describe the interaction of light with a magnetic medium. The most prominent examples are the Faraday and Cotton-Mouton effects that modify the transmission of light through a medium, and the inverse Faraday and inverse Cotton-Mouton effects that can be used to coherently excite spin waves. Here, we introduce the phenomenology of the analog magneto-phononic and phono-magnetic effects, in which coherently excited vibrational quanta take the place of the light quanta. We show, using a combination of density functional theory and phenomenological modeling, that the effective magnetic fields exerted by these phono-magnetic effects on the spins of antiferromagnetic nickel oxide yield magnitudes comparable or larger than those of the opto-magnetic effects.
Bo Zhao, Cheng Guo, Christina A. C. Garcia, Prineha Narang, and Shanhui Fan. 11/19/2019. “Axion-Field-Enabled Nonreciprocal Thermal Radiation in Weyl Semimetals.” arXiv. Publisher's VersionAbstract
Objects around us constantly emit and absorb thermal radiation. The emission and absorption processes are governed by two fundamental radiative properties: emissivity and absorptivity.For reciprocal systems, the emissivity and absorptivity are restricted to be equal by Kirchhoff's law of thermal radiation. This restriction limits the degree of freedom to control thermal radiation and contributes to an intrinsic loss mechanism in photonic energy harvesting systems such assolar cells. Existing approaches to violate Kirchhoff's law typically utilize conventional magneto-optical effects in the presence of an external magnetic field. However, these approaches require either a strong magnetic field (~3T), or narrow-band resonances under a moderate magnetic field (~0.3T), because the non-reciprocity in conventional magneto-optical effects isusually weak in the thermal wavelength range. Here, we show that the axion electrodynamics in magnetic Weyl semimetals can be used to construct strongly nonreciprocal thermal emitters that near completely violate Kirchhoff's law over broad angular and frequency ranges, without requiring any external magnetic field. The non-reciprocity moreover is strongly temperature tunable, opening new possibilities for active non-reciprocal devices in controlling thermal radiation.
Gabriele Grosso, Hyowon Moon, Christopher J. Ciccarino, Johannes Flick, Noah Mendelson, Milos Toth, Igor Aharonovich, Prineha Narang, and Dirk R. Englund. 10/4/2019. “Low-temperature electron-phonon interaction of quantum emitters in hexagonal Boron Nitride.” arXiv. Publisher's VersionAbstract
Quantum emitters based on atomic defects in layered hexagonal Boron Nitride (hBN) have emerged as promising solid state 'artificial atoms' with atom-like photophysical and quantum optoelectronic properties. Similar to other atom-like emitters, defect-phonon coupling in hBN governs the characteristic single-photon emission and provides an opportunity to investigate the atomic and electronic structure of emitters as well as the coupling of their spin- and charge-dependent electronic states to phonons. Here, we investigate these questions using photoluminescence excitation (PLE) experiments at T=4K on single photon emitters in multilayer hBN grown by chemical vapor deposition. By scanning up to 250 meV from the zero phonon line (ZPL), we can precisely measure the emitter's coupling efficiency to different phonon modes. Our results show that excitation mediated by the absorption of one in-plane optical phonon increases the emitter absorption probability ten-fold compared to that mediated by acoustic or out-of-plane optical phonons. We compare these measurements against theoretical predictions by first-principles density-functional theory of four defect candidates, for which we calculate prevalent charge states and their spin-dependent coupling to bulk and local phonon modes. Our work illuminates the phonon-coupled dynamics in hBN quantum emitters at cryogenic temperature, with implications more generally for mesoscopic quantum emitter systems in 2D materials and represents possible applications in solid-state quantum technologies.
Prineha Narang, Christopher J. Ciccarino, Johannes Flick, and Dirk Englund. 9/30/2019. “Quantum Materials with Atomic Precision: Artificial Atoms in Solids: Ab Initio Design, Control, and Integration of Single Photon Emitters in Artificial Quantum Materials.” Advanced Functional Materials. Publisher's VersionAbstract
This Progress Report explores advances and opportunities in the atomic‐scale design, fabrication, and imaging of quantum materials toward creating artificial atoms in solids with tailored optoelectronic and quantum properties. The authors outline an “ab initio” approach to quantitatively linking first‐principles calculations and atomic imaging with atomic patterning, setting the stage for new designer quantum nanomaterials.
Georgios Varnavides, Adam S. Jermyn, Polina Anikeeva, and Prineha Narang. 9/3/2019. “Non-Equilibrium Phonon Transport Across Nanoscale Interfaces.” Physical Review B., 100, 115402. Publisher's VersionAbstract
Despite the ubiquity of applications of heat transport across nanoscale interfaces, including integrated circuits, thermoelectrics, and nanotheranostics, an accurate description of phonon transport in these systems remains elusive. Here we present a theoretical and computational framework to describe phonon transport with position, momentum and scattering event resolution. We apply this framework to a single material spherical nanoparticle for which the multidimensional resolution offers insight into the physical origin of phonon thermalization, and length-scale dependent anisotropy of steady-state phonon distributions. We extend the formalism to handle interfaces explicitly and investigate the specific case of semi-coherent materials interfaces by computing the coupling between phonons and interfacial strain resulting from aperiodic array of misfit dislocations. Our framework quantitatively describes the thermal interface resistance within the technologically relevant Si-Ge heterostructures. In future, this formalism could provide new insight into coherent and driven phonon effects in nanoscale materials increasingly accessible via ultrafast, THz and near-field spectroscopies.
Isaac Harris, Christopher J. Ciccarino, Johannes Flick, Dirk R. Englund, and Prineha Narang. 7/29/2019. “Group III Quantum Defects in Diamond are Stable Spin-1 Color Centers.” arXiv. Publisher's VersionAbstract
Color centers in diamond have emerged as leading solid-state artificial atoms for a range of quantum technologies, from quantum sensing to quantum networks. Concerted research activities are now underway to identify new color centers that combine stable spin and optical properties of the nitrogen vacancy (NV) with the spectral stability of the silicon vacancy (SiV) centers in diamond, with recent research identifying other group IV color centers with superior properties. In this Letter, we investigate a new class of diamond quantum emitters from first principles, the group III color centers, which we show to be thermodynamically stable in a spin-1, electric-field insensitive structure. From ab initio electronic structure methods, we characterize the product Jahn-Teller (pJT) effect present in the excited state manifold of these group III color centers, where we capture symmetry-breaking distortions associated with strong electron-phonon coupling. These predictions can guide experimental identification of group III vacancy centers and their use in applications in quantum information science and technology.
Siyuan Dai, Wenjing Fang, Nicholas Rivera, Yijing Stehle, Bor-Yuan Jiang, Jialang Shen, Roland Yingjie Tay, Christopher J. Ciccarino, Qiong Ma, Daniel Rodan‐Legrain, Pablo Jarillo‐Herrero, Edwin Hang Tong Teo, Michael M. Fogler, Prineha Narang, Jing Kong, and Dimitri N. Basov. 7/28/2019. “Phonon Polaritons in Monolayers of Hexagonal Boron Nitride.” Advanced Materials, 31, 37. Publisher's VersionAbstract
Phonon polaritons in van der Waals materials reveal significant confinement accompanied with long propagation length: important virtues for tasks pertaining to the control of light and energy flow at the nanoscale. While previous studies of phonon polaritons have relied on relatively thick samples, here reported is the first observation of surface phonon polaritons in single atomic layers and bilayers of hexagonal boron nitride (hBN). Using antenna‐based near‐field microscopy, propagating surface phonon polaritons in mono‐ and bilayer hBN microcrystals are imaged. Phonon polaritons in monolayer hBN are confined in a volume about one million times smaller than the free‐space photons. Both the polariton dispersion and their wavelength–thickness scaling law are altered compared to those of hBN bulk counterparts. These changes are attributed to phonon hardening in monolayer‐thick crystals. The data reported here have bearing on applications of polaritons in metasurfaces and ultrathin optical elements.
Johannes Flick and Prineha Narang. 7/10/2019. “Excited-State Nanophotonic and Polaritonic Chemistry with Ab initio Potential-Energy Surfaces.” arXiv. Publisher's VersionAbstract
Advances in nanophotonics, quantum optics, and low-dimensional materials have enabled precise control of light-matter interactions down to the nanoscale. Combining concepts from each of these fields, there is now an opportunity to create and manipulate photonic matter via strong coupling of molecules to the electromagnetic field. Towards this goal, here we introduce a first principles framework to calculate polaritonic excited-state potential-energy surfaces for strongly coupled light-matter systems. In particular, we demonstrate the applicability of our methodology by calculating the polaritonic excited-state manifold of a Formaldehyde molecule strongly coupled to an optical cavity. This proof-of-concept calculation shows how strong coupling can be exploited to alter photochemical reaction pathways by influencing avoided crossings. Therefore, by introducing an ab initio method to calculate excited-state potential-energy surfaces, our work opens a new avenue for the field of polaritonic chemistry.
Adam S. Jermyn, Giulia Tagliabue, Harry A. Atwater, William A. Goddard III, Prineha Narang, and Ravishankar Sundararaman. 7/8/2019. “Transport of hot carriers in plasmonic nanostructures.” Physical Review Materials, 3, 075201. Publisher's VersionAbstract
Plasmonic hot carrier devices extract excited carriers from metal nanostructures before equilibration and have the potential to surpass semiconductor light absorbers. However their efficiencies have so far remained well below theoretical limits, which necessitates quantitative prediction of carrier transport and energy loss in plasmonic structures to identify and overcome bottlenecks in carrier harvesting. Here, we present a theoretical and computational framework, nonequilibrium scattering in space and energy (NESSE), to predict the spatial evolution of carrier energy distributions that combines the best features of phase-space (Boltzmann) and particle-based (Monte Carlo) methods. Within the NESSE framework, we bridge first-principles electronic structure predictions of plasmon decay and carrier collision integrals at the atomic scale, with electromagnetic field simulations at the nano- to mesoscale. Finally, we apply NESSE to predict spatially-resolved energy distributions of photoexcited carriers that impact the surface of experimentally realizable plasmonic nanostructures at length scales ranging from tens to several hundreds of nanometers, enabling first-principles design of hot carrier devices.
Nicholas Rivera, Johannes Flick, and Prineha Narang. 5/16/2019. “Variational theory of non-relativistic quantum electrodynamics.” Physical Review Letters, 122, 193603. Publisher's VersionAbstract
The ability to achieve ultrastrong coupling between light and matter promises to bring about new means to control material properties, new concepts for manipulating light at the atomic scale, and new insights into quantum electrodynamics (QED). Thus, there is a need to develop quantitative theories of QED phenomena in complex electronic and photonic systems. In this Letter, we develop a variational theory of general non-relativistic QED systems of coupled light and matter. Essential to our Ansatz is the notion of an effective photonic vacuum whose modes are different than the modes in the absence of light-matter coupling. This variational formulation leads to a set of general equations that can describe the ground state of multielectron systems coupled to many photonic modes in real space. As a first step toward a new ab initio approach to ground and excited state energies in QED, we apply our Ansatz to describe a multilevel emitter coupled to many optical modes, a system with no analytical solution. We find a compact semianalytical formula which describes ground and excited state energies very well in all regimes of coupling parameters allowed by sum rules. Our formulation provides a nonperturbative theory of Lamb shifts and Casimir-Polder forces, as well as suggest new physical concepts such as the Casimir energy of a single atom in a cavity. Our method thus give rise to highly accurate nonperturbative descriptions of many other phenomena in general QED systems.
Toan Trong Tran, Blake Regan, Evgeny A. Ekimov, Zhao Mu, Yu Zhou, Wei-bo Gao, Prineha Narang, Alexander S. Solntsev, Milos Toth, Igor Aharonovich, and Carlo Bradac. 5/3/2019. “Anti-Stokes excitation of solid-state quantum emitters for nanoscale thermometry.” Science Advances, 5, 5, Pp. eaav9180. Publisher's VersionAbstract
Color centers in solids are the fundamental constituents of a plethora of applications such as lasers, light-emitting diodes, and sensors, as well as the foundation of advanced quantum information and communication technologies. Their photoluminescence properties are usually studied under Stokes excitation, in which the emitted photons are at a lower energy than the excitation ones. In this work, we explore the opposite anti-Stokes process, where excitation is performed with lower-energy photons. We report that the process is sufficiently efficient to excite even a single quantum system—namely, the germanium-vacancy center in diamond. Consequently, we leverage the temperature-dependent, phonon-assisted mechanism to realize an all-optical nanoscale thermometry scheme that outperforms any homologous optical method used to date. Our results frame a promising approach for exploring fundamental light-matter interactions in isolated quantum systems and harness it toward the realization of practical nanoscale thermometry and sensing.
Man-Nung Su, Christopher J. Ciccarino, Sushant Kumar, Pratiksha D. Dongare, Seyyed Ali Hosseini Jebeli, David Renard, Yue Zhang, Behnaz Ostovar, Wei-Shun Chang, Peter Nordlander, Naomi J. Halas, Ravishankar Sundararaman, Prineha Narang, and Stephan Link. 4/2/2019. “Ultrafast Electron Dynamics in Single Aluminum Nanostructures.” Nano Letters. Publisher's VersionAbstract
Aluminum nanostructures are a promising alternative material to noble metal nanostructures for several photonic and catalytic applications, but their ultrafast electron dynamics remain elusive. Here, we combine single-particle transient extinction spectroscopy and parameter-free first-principles calculations to investigate the non-equilibrium carrier dynamics in aluminum nanostructures. Unlike gold nanostructures, we find the sub-picosecond optical response of lithographically fabricated aluminum nanodisks to be more sensitive to the lattice temperature than the electron temperature. We assign the rise in the transient transmission to electron–phonon coupling with a pump-power-independent lifetime of 500 ± 100 fs and theoretically confirm this strong electron–phonon coupling behavior. We also measure electron–phonon lifetimes in chemically synthesized aluminum nanocrystals and find them to be even longer (1.0 ± 0.1 ps) than for the nanodisks. We also observe a rise and decay in the transient transmissions with amplitudes that scale with the surface-to-volume ratio of the aluminum nanodisks, implying a possible hot carrier trapping and detrapping at the native oxide shell–metal core interface.
Yuxin Yin, Jennifer Coulter, Christopher J. Ciccarino, and Prineha Narang. 3/21/2019. “A Theoretical Investigation of Charge Density Wave Instability in CuS2.” arXiv. Publisher's VersionAbstract
The existence of a charge density wave (CDW) in transition metal dichalcogenide CuS2 has remained undetermined since its first experimental synthesis nearly 50 years ago. Despite conflicting experimental literature regarding its low temperature structure, there exists no theoretical study of the phonon properties and lattice stability of this material. By studying the first-principles electronic structure and phonon properties of CuS2 at various electronic temperatures, we identify temperature-sensitive soft phonon modes which unveil a previously unreported Kohn anomaly at approximately 100K. Variation of the electronic temperature shows the presence of two distinct phases, characterized at low temperature by a 2×2×2 periodic charge modulation associated with the motion of the S2 dimers. Investigation of the Fermi surface presents a potential Fermi surface nesting vector related to the location of the Kohn anomaly and observed band splittings in the unfolded bandstructure. The combination of these results suggests a strong possibility of CDW order in CuS2. Further study of CuS2 in monolayer form finds no evidence of a CDW phase, as the identified bulk periodic distortions cannot be realized in 2D. This behavior sets this material apart from other transition metal dichalcogenide materials, which exhibit a charge density wave phase down to the 2D limit. As CDW in TMDC materials is considered to compete with superconductivity, the lack of CDW in monolayer CuS2 suggests the possibility of enhanced superconductivity relative to other transition metal dichalcogenides. Overall, our work identifies CuS2 as a previously unrealized candidate to study interplay of superconductivity, CDW order, and dimensionality.
Nicholas Rivera, Thomas Christensen, and Prineha Narang. 3/20/2019. “Phonon polaritonics in two-dimensional materials.” Nano Letters, 19, 4, Pp. 2653–2660. Publisher's VersionAbstract
Extreme confinement of electromagnetic energy by phonon polaritons holds the promise of strong and new forms of control over the dynamics of matter. To bring such control to the atomic-scale limit, it is important to consider phonon polaritons in two-dimensional (2D) systems. Recent studies have pointed out that in 2D, splitting between longitudinal and transverse optical (LO and TO) phonons is absent at the Γ point, even for polar materials. Does this lack of LO--TO splitting imply the absence of a phonon polariton in polar monolayers? Here, we derive a first-principles expression for the conductivity of a polar monolayer specified by the wavevector-dependent LO and TO phonon dispersions. In the long-wavelength (local) limit, we find a universal form for the conductivity in terms of the LO phonon frequency at the Γ point, its lifetime, and the group velocity of the LO phonon. Our analysis reveals that the phonon polariton of 2D is simply the LO phonon of the 2D system. For the specific example of hexagonal boron nitride (hBN), we estimate the confinement and propagation losses of the LO phonons, finding that high confinement and reasonable propagation quality factors coincide in regions which may be difficult to detect with current near-field optical microscopy techniques. Finally, we study the interaction of external emitters with two-dimensional hBN nanostructures, finding extreme enhancement of spontaneous emission due to coupling with localized 2D phonon polaritons, and the possibility of multi-mode strong and ultra-strong coupling between an external emitter and hBN phonons. This may lead to the design of new hybrid states of electrons and phonons based on strong coupling.