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Chris Jozwiak

Publications and source records attributed to Chris Jozwiak.

106 records · Page 6Linked to original sources

A setup for extreme-ultraviolet ultrafast angle-resolved photoelectron spectroscopy at 50-kHz repetition rate

Time- and angle-resolved photoelectron spectroscopy (trARPES) is a powerful method to track the ultrafast dynamics of quasiparticles and electronic bands in energy and momentum space. We present a setup for trARPES with 22.3 eV extreme-ultraviolet (XUV) femtosecond pulses at 50-kHz repetition rate, which enables fast data acquisition and access to dynamics across momentum space with high sensitivity. The design and operation of the XUV beamline, pump-probe setup, and UHV endstation are described in detail. By characterizing the effect of space-charge broadening, we determine an ultimate source-limited energy resolution of 60 meV, with typically 80-100 meV obtained at 1-2e10 photons/s probe flux on the sample. The instrument capabilities are demonstrated via both equilibrium and time-resolved ARPES studies of transition-metal dichalcogenides. The 50-kHz repetition rate enables sensitive measurements of quasiparticles at low excitation fluences in semiconducting MoSe$_2$, with an instrumental time resolution of 65 fs. Moreover, photo-induced phase transitions can be driven with the available pump fluence, as shown by charge density wave melting in 1T-TiSe$_2$. The high repetition-rate setup thus provides a versatile platform for sensitive XUV trARPES, from quenching of electronic phases down to the perturbative limit.

physics.ins-det↗

Intrinsic Insulating Ground State in Transition Metal Dichalcogenide TiSe2

The transition metal dichalcogenide TiSe$_2$ has received significant research attention over the past four decades. Different studies have presented ways to suppress the 200~K charge density wave transition, vary low temperature resistivity by several orders of magnitude, and stabilize magnetism or superconductivity. Here we give the results of a new synthesis technique whereby samples were grown in a high pressure environment with up to 180~bar of argon gas. Above 100~K, properties are nearly unchanged from previous reports, but a hysteretic resistance region that begins around 80~K, accompanied by insulating low temperature behavior, is distinct from anything previously observed. An accompanying decrease in carrier concentration is seen in Hall effect measurements, and photoemission data show a removal of an electron pocket from the Fermi surface in an insulating sample. We conclude that high inert gas pressure synthesis accesses an underlying nonmetallic ground state in a material long speculated to be an excitonic insulator.

cond-mat.str-el↗

Emergence of a Metal-Insulator Transition and High Temperature Charge Density Waves in VSe2 at the Monolayer Limit

Emergent phenomena driven by electronic reconstructions in oxide heterostructures have been intensively discussed. However, the role of these phenomena in shaping the electronic properties in van der Waals heterointerfaces has hitherto not been established. By reducing the material thickness and forming a heterointerface, we find two types of charge-ordering transitions in monolayer VSe2 on graphene substrates. Angle-resolved photoemission spectroscopy (ARPES) uncovers that Fermi-surface nesting becomes perfect in ML VSe2. Renormalization group analysis confirms that imperfect nesting in three dimensions universally flows into perfect nesting in two dimensions. As a result, the charge density wave transition temperature is dramatically enhanced to a value of 350 K compared to the 105 K in bulk VSe2. More interestingly, ARPES and scanning tunneling microscopy measurements confirm an unexpected metal-insulator transition at 135 K, driven by lattice distortions. The heterointerface plays an important role in driving this novel metal-insulator transition in the family of monolayered transition metal dichalcogenides.

cond-mat.str-el↗

Electronic Structure of Exfoliated and Epitaxial Hexagonal Boron Nitride

Hexagonal boron nitride (hBN) is an essential component in van der Waals heterostructures as it provides high quality and weakly interacting interfaces that preserve the electronic properties of adjacent materials. While exfoliated flakes of hBN have been extensively studied using electron transport and optical probes, detailed experimental measurements of the energy- and momentum- dependent electronic excitation spectrum are lacking. Here, we directly determine the full valence band (VB) electronic structure of micron-sized exfoliated flakes of hBN using angle-resolved photoemission spectroscopy with micrometer spatial resolution. We identify the π- and σ-band dispersions, the hBN stacking order and determine a total VB bandwidth of 19.4 eV. We compare these results with electronic structure data for epitaxial hBN on graphene on silicon carbide grown in situ using a borazine precursor. The epitaxial growth and electronic properties are investigated using photoe- mission electron microscopy. Our measurements show that the fundamental electronic properties of hBN are highly dependent on the fabrication strategy.

cond-mat.mtrl-sci↗

Giant spin-splitting and gap renormalization driven by trions in single-layer WS$_2$/h-BN heterostructures

In two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs), new electronic phenomena such as tunable band gaps and strongly bound excitons and trions emerge from strong many-body effects, beyond spin-orbit coupling- and lattice symmetry-induced spin and valley degrees of freedom. Combining single-layer (SL) TMDs with other 2D materials in van der Waals heterostructures offers an intriguing means of controlling the electronic properties through these many-body effects via engineered interlayer interactions. Here, we employ micro-focused angle-resolved photoemission spectroscopy (microARPES) and in-situ surface doping to manipulate the electronic structure of SL WS$_2$ on hexagonal boron nitride (WS$_2$/h-BN). Upon electron doping, we observe an unexpected giant renormalization of the SL WS$_2$ valence band (VB) spin-orbit splitting from 430~meV to 660~meV, together with a band gap reduction of at least 325~meV, attributed to the formation of trionic quasiparticles. These findings suggest that the electronic, spintronic and excitonic properties are widely tunable in 2D TMD/h-BN heterostructures, as these are intimately linked to the quasiparticle dynamics of the materials.

cond-mat.mtrl-sci↗

The graphene/n-Ge(110) interface: structure, doping, and electronic properties

The implementation of graphene in semiconducting technology requires the precise knowledge about the graphene-semiconductor interface. In our work the structure and electronic properties of the graphene/$n$-Ge(110) interface are investigated on the local (nm) and macro (from $μ\mathrm{m}$ to mm) scales via a combination of different microscopic and spectroscopic surface science techniques accompanied by density functional theory calculations. The electronic structure of freestanding graphene remains almost completely intact in this system, with only a moderate $n$-doping indicating weak interaction between graphene and the Ge substrate. With regard to the optimization of graphene growth it is found that the substrate temperature is a crucial factor, which determines the graphene layer alignment on the Ge(110) substrate during its growth from the atomic carbon source. Moreover, our results demonstrate that the preparation routine for graphene on the doped semiconducting material ($n$-Ge) leads to the effective segregation of dopants at the interface between graphene and Ge(110). Furthermore, it is shown that these dopant atoms might form regular structures at the graphene/Ge interface and induce the doping of graphene. Our findings help to understand the interface properties of the graphene-semiconductor interfaces and the effect of dopants on the electronic structure of graphene in such systems.

cond-mat.mtrl-sci↗

Universal Mechanism of Band-Gap Engineering in Transition-Metal Dichalcogenides

Two-dimensional (2D) van-der-Waals semiconductors have emerged as a class of materials with promising device characteristics owing to the intrinsic bandgap. For realistic applications, the ideal is to modify the bandgap in a controlled manner by a mechanism that can be generally applied to this class of materials. Here, we report the observation of a universally tunable bandgap in the family of bulk 2H transition metal dichalcogenides (TMDs) by in situ surface doping of Rb atoms. A series of angle-resolved photoemission spectra unexceptionally shows that the bandgap of TMDs at the zone corners is modulated in the range of 0.8 ~ 2.0 eV, which covers a wide spectral range from visible to near infrared, with a tendency from indirect to direct bandgap. A key clue to understand the mechanism of this bandgap engineering is provided by the spectroscopic signature of symmetry breaking and resultant spin splitting, which can be explained by the formation of 2D electric dipole layers within the surface bilayer of TMDs. Our results establish the surface Stark effect as a universal mechanism of bandgap engineering based on the strong 2D nature of van-der-Waals semiconductors.

cond-mat.mtrl-sci↗

NaSn2As2: An Exfoliatable Layered van der Waals Zintl Phase

The discovery of new families of exfoliatable 2D crystals that have diverse sets of electronic, optical, and spin-orbit coupling properties, enables the realization of unique physical phenomena in these few-atom thick building blocks and in proximity to other materials. Herein, using NaSn2As2 as a model system, we demonstrate that layered Zintl phases having the stoichiometry ATt2Pn2 (A = Group 1 or 2 element, Tt = Group 14 tetrel element and Pn = Group 15 pnictogen element) and feature networks separated by van der Waals gaps can be readily exfoliated with both mechanical and liquid-phase methods. We identified the symmetries of the Raman active modes of the bulk crystals via polarized Raman spectroscopy. The bulk and mechanically exfoliated NaSn2As2 samples are resistant towards oxidation, with only the top surface oxidizing in ambient conditions over a couple of days, while the liquid-exfoliated samples oxidize much more quickly in ambient conditions. Employing angle-resolved photoemission spectroscopy (ARPES), density functional theory (DFT), and transport on bulk and exfoliated samples, we show that NaSn2As2 is a highly conducting 2D semimetal, with resistivities on the order of 10-6 Ω m. Due to peculiarities in the band structure, the dominating p-type carriers at low temperature are nearly compensated by the opening of n-type conduction channels as temperature increases. This work further expands the family of exfoliatable 2D materials to layered van der Waals Zintl phases, opening up opportunities in electronics and spintronics.

cond-mat.mtrl-sci↗

Massive Dirac fermions in a ferromagnetic kagome metal

The kagome lattice is a two-dimensional network of corner-sharing triangles known as a platform for exotic quantum magnetic states. Theoretical work has predicted that the kagome lattice may also host Dirac electronic states that could lead to topological and Chern insulating phases, but these have evaded experimental detection to date. Here we study the d-electron kagome metal Fe$_3$Sn$_2$ designed to support bulk massive Dirac fermions in the presence of ferromagnetic order. We observe a temperature independent intrinsic anomalous Hall conductivity persisting above room temperature suggestive of prominent Berry curvature from the time-reversal breaking electronic bands of the kagome plane. Using angle-resolved photoemission, we discover a pair of quasi-2D Dirac cones near the Fermi level with a 30 meV mass gap that accounts for the Berry curvature-induced Hall conductivity. We show this behavior is a consequence of the underlying symmetry properties of the bilayer kagome lattice in the ferromagnetic state with atomic spin-orbit coupling. This report provides the first evidence for a ferromagnetic kagome metal and an example of emergent topological electronic properties in a correlated electron system. This offers insight into recent discoveries of exotic electronic behavior in kagome lattice antiferromagnets and may provide a stepping stone toward lattice model realizations of fractional topological quantum states.

cond-mat.mtrl-sci↗

Spatially Resolved Electronic Properties of Single-Layer WS$_2$ on Transition Metal Oxides

There is a substantial interest in the heterostructures of semiconducting transition metal dichalcogenides (TMDCs) amongst each other or with arbitrary materials, through which the control of the chemical, structural, electronic, spintronic, and optical properties can lead to a change in device paradigms. A critical need is to understand the interface between TMDCs and insulating substrates, for example high-$κ$ dielectrics, which can strongly impact the electronic properties such as the optical gap. Here we show that the chemical and electronic properties of the single-layer (SL) TMDC, WS$_2$, can be transferred onto high-$κ$ transition metal oxide substrates TiO$_2$ and SrTiO$_3$. The resulting samples are much more suitable for measuring their electronic and chemical structures with angle-resolved photoemission than their native-grown SiO$_2$ substrates. We probe the WS$_2$ on the micron scale across 100-micron flakes, and find that the occupied electronic structure is exactly as predicted for freestanding SL WS$_2$ with a strong spin-orbit splitting of 420~meV and a direct band gap at the valence band maximum. Our results suggest that TMDCs can be combined with arbitrary multi-functional oxides, which may introduce alternative means of controlling the optoelectronic properties of such materials.

cond-mat.mtrl-sci↗

Spin-Polarized Surface Resonances Accompanying Topological Surface State Formation

Topological insulators host spin-polarized surface states born out of the energetic inversion of bulk bands driven by the spin-orbit interaction. Here we discover previously unidentified consequences of band-inversion on the surface electronic structure of the topological insulator Bi$_2$Se$_3$. By performing simultaneous spin, time, and angle-resolved photoemission spectroscopy, we map the spin-polarized unoccupied electronic structure and identify a surface resonance which is distinct from the topological surface state, yet shares a similar spin- orbital texture with opposite orientation. Its momentum- dependence and spin texture imply an intimate connection with the topological surface state. Calculations show these two distinct states can emerge from trivial Rashba-like states that change topology through the spin-orbit-induced band inversion. This work thus provides a compelling view of the coevolution of surface states through a topological phase transition, enabled by the unique capability of directly measuring the spin-polarized unoccupied band structure.

cond-mat.mtrl-sci↗

Influence of Optically Quenched Superconductivity on Quasiparticle Relaxation Rates in Bi2Sr2CaCu2O8+delta

We use time- and angle-resolved photoemission to measure quasiparticle relaxation dynamics across a laser-induced superconducting phase transition in Bi2Sr2CaCu2O8+delta. Whereas low-fluence measurements reveal picosecond dynamics, sharp femtosecond dynamics emerge at higher fluence. Analyses of data as a function of energy, momentum, and doping indicate that the closure of the near-nodal gap and disruption of macroscopic coherence are primary mechanisms driving this onset. The results demonstrate the important influence of transient electronic structure on relaxation dynamics, which is relevant for developing an understanding of nonequilibrium phase transitions.

cond-mat.str-el↗

Time- and Momentum-resolved Gap Dynamics in Bi2Sr2CaCu2O8+delta

We use time- and angle-resolved photoemission spectroscopy to characterize the dynamics of the energy gap in superconducting Bi2Sr2CaCu2O8+delta (Bi2212). Photoexcitation drives the system into a nonequilibrium pseudogap state: Near the Brillouin zone diagonal (inside the normal-state Fermi arc), the gap completely closes for a pump fluence beyond F = 15 μJ/cm^2; toward the Brillouin zone face (outside the Fermi arc), it remains open to at least 24 μJ/cm^2. This strongly anisotropic gap response may indicate multiple competing ordering tendencies in Bi2212. Despite these contrasts, the gap recovers with relatively momentum-independent dynamics at all probed momenta, which shows the persistent influence of superconductivity both inside and outside the Fermi arc.

cond-mat.str-el↗

Signatures of superconductivity and pseudogap formation in non-equilibrium nodal quasiparticles revealed by ultrafast angle-resolved photoemission

We use time- and angle-resolved photoemission to measure the nodal non-equilibrium electronic states in various dopings of Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$. We find that the initial pump-induced transient signal of these ungapped states is strongly affected by the onset of the superconducting gap at $T_c$, superconducting pairing fluctuations at $T_p$, and the pseudogap at $T^*$. Moreover, $T_p$ marks a suggestive threshold in the fluence-dependent transient signal, with the appearance of a critical fluence below $T_p$ that corresponds to the energy required to break apart all Cooper pairs. These results challenge the notion of a nodal-antinodal dichotomy in cuprate superconductors by establishing a new link between nodal quasiparticles and the cuprate phase diagram.

cond-mat.supr-con↗

Photoelectron spin-flipping and texture manipulation in a topological insulator

Recently discovered materials called three-dimensional topological insulators constitute examples of symmetry protected topological states in the absence of applied magnetic fields and cryogenic temperatures. A hallmark characteristic of these non-magnetic bulk insulators is the protected metallic electronic states confined to the material's surfaces. Electrons in these surface states are spin polarized with their spins governed by their direction of travel (linear momentum), resulting in a helical spin texture in momentum space. Spin- and angle-resolved photoemission spectroscopy (spin-ARPES) has been the only tool capable of directly observing this central feature with simultaneous energy, momentum, and spin sensitivity. By using an innovative photoelectron spectrometer with a high-flux laser-based light source, we discovered another surprising property of these surface electrons which behave like Dirac fermions. We found that the spin polarization of the resulting photoelectrons can be fully manipulated in all three dimensions through selection of the light polarization. These surprising effects are due to the spin-dependent interaction of the helical Dirac fermions with light, which originates from the strong spin-orbit coupling in the material. Our results illustrate unusual scenarios in which the spin polarization of photoelectrons is completely different from the spin state of electrons in the originating initial states. The results also provide the basis for a novel source of highly spin-polarized electrons with tunable polarization in three dimensions.

cond-mat.mtrl-sci↗

Widespread spin polarization effects in photoemission from topological insulators

High resolution spin- and angle-resolved photoemission spectroscopy (spin-ARPES) was performed on the three-dimensional topological insulator Bi$_2$Se$_3$ using a recently developed high-efficiency spectrometer. The topological surface state's helical spin structure is observed, in agreement with theoretical prediction. Spin textures of both chiralities, at energies above and below the Dirac point, are observed, and the spin structure is found to persist at room temperature. The measurements reveal additional unexpected spin polarization effects, which also originate from the spin-orbit interaction, but are well differentiated from topological physics by contrasting momentum and photon energy and polarization dependencies. These observations demonstrate significant deviations of photoelectron and quasiparticle spin polarizations. Our findings illustrate the inherent complexity of spin-resolved ARPES and demonstrate key considerations for interpreting experimental results.

cond-mat.mtrl-sci↗