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In the past two decades, various classes of topological materials have been discovered, spanning topological insulators, semimetals, and metals. While the observation and understanding of the topology of a material has been a primary focus so far, the precise and easy control of topology in a single material remains largely unexplored. Here, we demonstrate full experimental control over the topological Dirac nodal loop in the square-net material LaSb$_\mathrm{x}$Te$_\mathrm{2-x}$ by chemical substitution and electron doping. Using angle-resolved photoemission spectroscopy (ARPES), we show that changing the antimony concentration x from 0.9 to 1.0 in the bulk opens a gap as large as 400 meV in the nodal loop. Our symmetry analysis based on single-crystal X-ray diffraction and a minimal tight binding model establishes that the breaking of \textit{n} glide symmetry in the square-net layer is responsible for the opening of the gap. Remarkably, we can also realize this topological phase transition \textit{in situ} on the surface of LaSb$_\mathrm{x}$Te$_\mathrm{2-x}$ by chemical gating using potassium deposition, which enables the reversible switching of the topology from gapped to gapless nodal loop. The underlying control parameter for the structural and topological transition in the bulk and on the surface is the electron concentration. It opens a pathway towards applications in devices based on switching topology by electrostatic gating.

The 40-70 meV band-structure renormalization (so-called kink) in high-temperature cuprate superconductors - which has been mainly interpreted in terms of electron-boson coupling - is observed to be strongly suppressed both above the superconducting transition temperature and under optical excitation. We employ equilibrium and time- and angle-resolved photoemission spectroscopy, in combination with Migdal-Eliashberg simulations, to investigate the suppression of the near-nodal kink in Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$. We show that the $\sim$30$\%$ decrease of the kink strength across the superconducting-to-normal-state phase transition can be entirely accounted for by the filling of the superconducting gap, without additional consideration of temperature-dependent electron-boson coupling. Our findings demonstrate that consideration of changes in the density of states is essential to quantitatively account for the band structure renormalization effects in cuprates.

FeSe$_{1-x}$S$_x$ remains one of the most enigmatic systems of Fe-based superconductors. While much is known about the orthorhombic parent compound, FeSe, the tetragonal samples, FeSe$_{1-x}$S$_x$ with x>0.17, remain relatively unexplored. Here, we provide an in-depth investigation of the electronic states of tetragonal FeSe$_{0.81}$S$_{0.19}$, using scanning tunneling microscopy and spectroscopy (STM/S) measurements, supported by angle-resolved photoemission spectroscopy (ARPES) and theoretical modeling. We demonstrate that by analyzing modulations of the local density of states (LDOS) near and away from Fe vacancy defects separately, we can identify quasiparticle interference (QPI) signals originating from multiple regions of the Brillouin zone, including the bands at the M and A points. We also observe that QPI signals coexist with a much stronger LDOS modulation for states near the Fermi level whose period is independent of energy. Our measurements further reveal that this strong pattern appears in the STS measurements as short range stripe patterns that are locally two-fold symmetric. Since these stripe patterns coexist with four-fold symmetric QPI around Fe-vacancies, the origin of their local two-fold symmetry must be distinct from that of nematic states in orthorhombic samples. To further understand these stripe patterns, we explore several aspects related to them, such as the role of S and Fe vacancy defects, and whether they can be explained by QPI. We consider the possibility that the observed stripe patterns may represent incipient charge order correlations, similar to those observed in the cuprates.

In spintronic devices, the two main approaches to actively control the electrons' spin degree of freedom involve either static magnetic or electric fields. An alternative avenue relies on the application of optical fields to generate spin currents, which promises to bolster spin-device performance allowing for significantly faster and more efficient spin logic. To date, research has mainly focused on the optical injection of spin currents through the photogalvanic effect, and little is known about the direct optical control of the intrinsic spin splitting. Here, to explore the all-optical manipulation of a material's spin properties, we consider the Rashba effect at a semiconductor interface. The Rashba effect has long been a staple in the field of spintronics owing to its superior tunability, which allows the observation of fully spin-dependent phenomena, such as the spin-Hall effect, spin-charge conversion, and spin-torque in semiconductor devices. In this work, by means of time and angle-resolved photoemission spectroscopy (TR-ARPES), we demonstrate that an ultrafast optical excitation can be used to manipulate the Rashba-induced spin splitting of a two-dimensional electron gas (2DEG) engineered at the surface of the topological insulator Bi$_{2}$Se$_{3}$. We establish that light-induced photovoltage and charge carrier redistribution -- which in concert modulate the spin-orbit coupling strength on a sub-picosecond timescale -- can offer an unprecedented platform for achieving all optically-driven THz spin logic devices.

We present a method for producing high quality KCo2As2 crystals, stable in air and suitable for a variety of measurements. X-ray diffraction, magnetic susceptibility, electrical transport and heat capacity measurements confirm the high quality and an absence of long range magnetic order down to at least 2 K. Residual resistivity values approaching 0.25 $\mu\Omega$~cm are representative of the high quality and low impurity content, and a Sommerfeld coefficient $\gamma$ = 7.3 mJ/mol K$^2$ signifies weaker correlations than the Fe-based counterparts. Together with Hall effect measurements, angle-resolved photoemission experiments reveal a Fermi surface consisting of electron pockets at the center and corner of the Brillouin zone, in line with theoretical predictions and in contrast to the mixed carrier types of other pnictides with the ThCr2Si2 structure. A large, linear magnetoresistance of 200\% at 14~T, together with an observed linear and hyperbolic, rather than parabolic, band dispersions are unusual characteristics of this metallic compound and may indicate more complex underlying behavior., Comment: 9 pages, 4 figures

High-temperature superconducting cuprates exhibit an intriguing phenomenology for the low-energy elementary excitations. In particular, an unconventional temperature dependence of the coherent spectral weight (CSW) has been observed in the superconducting phase by angle-resolved photoemission spectroscopy (ARPES), both at the antinode where the d-wave paring gap is maximum, as well as along the gapless nodal direction. Here, we combine equilibrium and time-resolved ARPES to track the temperature dependent meltdown of the nodal CSW in Bi-based cuprates with unprecedented sensitivity. We find the nodal suppression of CSW upon increasing temperature to be ubiquitous across single- and double-layer Bi cuprates, and uncorrelated to superconducting and pseudogap onset temperatures. We quantitatively model both the lineshape of the nodal spectral features and the anomalous suppression of CSW within the Fermi-Liquid framework, establishing the key role played by the normal state electrodynamics in the description of nodal quasiparticles in superconducting cuprates., Comment: 6 pages, 3 figures; Supplementary Materials available upon request

With its direct correspondence to electronic structure, angle-resolved photoemission spectroscopy (ARPES) is a ubiquitous tool for the study of solids. When extended to the temporal domain, time-resolved (TR)-ARPES offers the potential to move beyond equilibrium properties, exploring both the unoccupied electronic structure as well as its dynamical response under ultrafast perturbation. Historically, ultrafast extreme ultraviolet (XUV) sources employing high-order harmonic generation (HHG) have required compromises that make it challenging to achieve a high energy resolution - which is highly desirable for many TR-ARPES studies - while producing high photon energies and a high photon flux. We address this challenge by performing HHG inside a femtosecond enhancement cavity (fsEC), realizing a practical source for TR-ARPES that achieves a flux of over 10$^{11}$ photons/s delivered to the sample, operates over a range of 8-40 eV with a repetition rate of 60 MHz. This source enables TR-ARPES studies with a temporal and energy resolution of 190 fs and 22 meV, respectively. To characterize the system, we perform ARPES measurements of polycrystalline Au and MoTe$_2$, as well as TR-ARPES studies on graphite., Comment: 11 pages, 5 figures

Graphene is a powerful playground for studying a plethora of quantum phenomena. One of the remarkable properties of graphene arises when it is strained in particular geometries and the electrons behave as if they were under the influence of a magnetic field. Previously, these strain-induced pseudomagnetic fields have been explored on the nano- and micrometer-scale using scanning probe and transport measurements. Heteroepitaxial strain, in contrast, is a wafer-scale engineering method. Here, we show that pseudomagnetic fields can be generated in graphene through wafer-scale epitaxial growth. Shallow triangular nanoprisms in the SiC substrate generate strain-induced uniform fields of 41 T. This enables the observation of strain-induced Landau levels at room temperature, as detected by angle-resolved photoemission spectroscopy, and confirmed by model calculations and scanning tunneling microscopy measurements. Our work demonstrates the feasibility of exploiting strain-induced quantum phases in two-dimensional Dirac materials on a wafer-scale platform, opening the field to new applications., Comment: Revised version as published in Science Advances

Electron interactions are pivotal for defining the electronic structure of quantum materials. In particular, the strong electron Coulomb repulsion is considered the keystone for describing the emergence of exotic and/or ordered phases of quantum matter as disparate as high-temperature superconductivity and charge- or magnetic-order. However, a comprehensive understanding of fundamental electronic properties of quantum materials is often complicated by the appearance of an enigmatic partial suppression of low-energy electronic states, known as the pseudogap. Here we take advantage of ultrafast angle-resolved photoemission spectroscopy to unveil the temperature evolution of the low-energy density of states in the electron-doped cuprate Nd$_{\text{2-x}}$Ce$_{\text{x}}$CuO$_{\text{4}}$, an emblematic system where the pseudogap intertwines with magnetic degrees of freedom. By photoexciting the electronic system across the pseudogap onset temperature T*, we report the direct relation between the momentum-resolved pseudogap spectral features and the spin-correlation length with an unprecedented sensitivity. This transient approach, corroborated by mean field model calculations, allows us to establish the pseudogap in electron-doped cuprates as a precursor to the incipient antiferromagnetic order even when long-range antiferromagnetic correlations are not established, as in the case of optimal doping., Comment: 17 pages, 3 figures

Time- and angle-resolved photoemission spectroscopy accesses the ultrafast evolution of quasiparticles and many-body interactions in solid-state systems. However, the momentum- and energy-resolved transient photoemission intensity may not be unambiguously related to the intrinsic relaxation dynamics of photoexcited electrons. In fact, interpretation of the time-dependent photoemission signal can be affected by the transient evolution of both the one-electron removal spectral function as well as the photoemission dipole matrix elements. Here we investigate the topological insulator Bi$_{1.1}$Sb$_{0.9}$Te$_2$S to demonstrate, by means of a careful probe-polarization study, the transient contribution of matrix elements to the time-resolved photoemission signal., Comment: 7 pages, 3 figures

The possibility of driving phase transitions in low-density condensates through the loss of phase coherence alone has far-reaching implications for the study of quantum phases of matter. This has inspired the development of tools to control and explore the collective properties of condensate phases via phase fluctuations. Electrically-gated oxide interfaces, ultracold Fermi atoms, and cuprate superconductors, which are characterized by an intrinsically small phase-stiffness, are paradigmatic examples where these tools are having a dramatic impact. Here we use light pulses shorter than the internal thermalization time to drive and probe the phase fragility of the Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$ cuprate superconductor, completely melting the superconducting condensate without affecting the pairing strength. The resulting ultrafast dynamics of phase fluctuations and charge excitations are captured and disentangled by time-resolved photoemission spectroscopy. This work demonstrates the dominant role of phase coherence in the superconductor-to-normal state phase transition and offers a benchmark for non-equilibrium spectroscopic investigations of the cuprate phase diagram., Comment: 24 pages, 9 figures, Main Text and Supplementary Information

We study the manipulation of the photoelectron spin-polarization in Bi$_2$Se$_3$ by spin- and angle-resolved photoemission spectroscopy. General rules are established that enable controlling the spin-polarization of photoemitted electrons via light polarization, sample orientation, and photon energy. We demonstrate the $\pm$100% reversal of a single component of the measured spin-polarization vector upon the rotation of light polarization, as well as a full three-dimensional manipulation by varying experimental configuration and photon energy. While a material-specific density-functional theory analysis is needed for the quantitative description, a minimal two-atomic-layer model qualitatively accounts for the spin response based on the interplay of optical selection rules, photoelectron interference, and topological surface-state complex structure. It follows that photoelectron spin-polarization control is generically achievable in systems with a layer-dependent, entangled spin-orbital texture., Comment: 5 pages, 4 figures. A high-resolution version with supplementary material can be found at: http://www.phas.ubc.ca/~quantmat/ARPES/PUBLICATIONS/Articles/BiSe_spin_ARPES.pdf

We present an analysis of two experimental approaches to controlling the directionality of molecular rotation with ultrashort laser pulses. The two methods are based on the molecular interaction with either a pair of pulses (a "double kick" scheme) or a longer pulse sequence (a "chiral pulse train" scheme). In both cases, rotational control is achieved by varying the polarization of and the time delay between the consecutive laser pulses. Using the technique of polarization sensitive resonance-enhanced multi-photon ionization, we show that both methods produce significant rotational directionality. We demonstrate that increasing the number of excitation pulses supplements the ability to control the sense of molecular rotation with quantum state selectivity, i.e. predominant excitation of a single rotational state. We also demonstrate the ability of both techniques to generate counter-rotation of molecular nuclear spin isomers (here, ortho- and para-nitrogen) and molecular isotopologues (here, 14N_2 and 15N_2)., Comment: 8 pages, 10 figures

We investigate experimentally the effect of quantum resonance in the rotational excitation of the simplest quantum rotor - a diatomic molecule. By using the techniques of high-resolution femtosecond pulse shaping and rotational state-resolved detection, we measure directly the amount of energy absorbed by molecules interacting with a periodic train of laser pulses, and study its dependence on the train period. We show that the energy transfer is significantly enhanced at quantum resonance, and use this effect for demonstrating selective rotational excitation of two nitrogen isotopologues, $ ^{14}N_2$ and $ ^{15}N_2$. Moreover, by tuning the period of the pulse train in the vicinity of a fractional quantum resonance, we achieve spin-selective rotational excitation of para- and ortho-isomers of $ ^{15}N_2$., Comment: 5 pages, 4 figures

Rabi oscillations of quantum population are known to occur in two-level systems driven by spectrally narrow laser fields. In this work we study Rabi oscillations induced by shaped broadband femtosecond laser pulses. Due to the broad spectral width of the driving field, the oscillations are initiated between a ground state and a coherent superposition of excited states, or a "wavepacket", rather than a single excited state. Our experiments reveal an intricate dependence of the wavepacket phase on the intensity of laser field. We confirm numerically that the effect is associated with the strong-field nature of the interaction, and provide a qualitative picture by invoking a simple theoretical model., Comment: 6 pages, 6 figures

Trains of ultrashort laser pulses separated by the time of rotational revival (typically, tens of picoseconds) have been exploited for creating ensembles of aligned molecules. In this work we introduce a chiral pulse train - a sequence of linearly polarized pulses with the polarization direction rotating from pulse to pulse by a controllable angle. The chirality of such a train, expressed through the period and direction of its polarization rotation, is used as a new control parameter for achieving selectivity and directionality of laser-induced rotational excitation. The method employs chiral trains with a large number of pulses separated on the time scale much shorter than the rotational revival (a few hundred femtosecond), enabling the use of conventional pulse shapers., Comment: 5 pages, 5 figures

We demonstrate a method of adiabatic population transfer from a single quantum state into a coherent superposition of states. The transfer is executed with femtosecond pulses, spectrally shaped in simple and intuitive manner, which does not require iterative feedback-controlled loops. In contrast to non-adiabatic methods of excitation, our approach is not sensitive to the exact value of laser intensity. We show that the population transfer is complete, and analyze the possibility of controlling the relative phases and amplitudes of the excited eigenstates. We discuss the limitations of the proposed control methods due to the dynamic level shifts and suggest ways of reducing their influence., Comment: Submitted to Phys. Rev. A. 9 pages, 9 figures

We propose and demonstrate the method of population transfer by piecewise adiabatic passage between two quantum states. Coherent excitation of a two-level system with a train of ultrashort laser pulses is shown to reproduce the effect of an adiabatic passage, conventionally achieved with a single frequency-chirped pulse. By properly adjusting the amplitudes and phases of the pulses in the excitation pulse train, we achieve complete and robust population transfer to the target state. The effect is demonstrated experimentally by observing piecewise excitation of Rubidium atoms from 5s_1/2 to 5p_1/2 electronic state. We show that similarly to the conventional adiabatic passage, the piecewise process is insensitive to the total excitation energy as long as the adiabaticity conditions are satisfied. The piecewise nature of the process suggests that robust and selective population transfer could be implemented in a variety of complex quantum systems beyond the two-level approximation., Comment: Submitted to Phys. Rev. Lett