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Electronic correlation is of fundamental importance to high temperature superconductivity. While the low energy electronic states in cuprates are dominantly affected by correlation effects across the phase diagram, observation of correlation-driven changes in fermiology amongst the iron-based superconductors remains rare. Here we present experimental evidence for a correlation-driven reconstruction of the Fermi surface tuned independently by two orthogonal axes of temperature and Se/Te ratio in the iron chalcogenide family FeTe$_{1-x}$Se$_x$. We demonstrate that this reconstruction is driven by the de-hybridization of a strongly renormalized $d_{xy}$ orbital with the remaining itinerant iron 3$d$ orbitals in the emergence of an orbital-selective Mott phase. Our observations are further supported by our theoretical calculations to be salient spectroscopic signatures of such a non-thermal evolution from a strongly correlated metallic phase into an orbital-selective Mott phase in $d_{xy}$ as Se concentration is reduced., Comment: 25 pages, 5 figures, accepted version to appear in Communications Physics. arXiv admin note: text overlap with arXiv:2010.13913

Relaxation of photoexcited carriers in graphite is studied by TR-ARPES. Boltzmann rate-equations are used to model the observed non-thermal electron distributions, and several non-thermal phases in the fluence-delay phase space are identified with broad implications.

We report on the synthesis and electronic properties of epitaxial perovskite ${\mathrm{La}}_{1\text{\ensuremath{-}}x}{\mathrm{Sr}}_{x}\mathrm{Rh}{\mathrm{O}}_{3}$ thin films. Thin films with a Sr content ranging from $x=0$ to 0.5 have been grown using molecular beam epitaxy. Transport and x-ray photoemission spectroscopy data reveal an insulator-metal-insulator transition, accompanied by a $p$- to $n$-type carrier change observed in Hall measurements. Combined with theoretical calculations, we find that the addition of Sr does not directly dope carriers into the conduction band, but rather induces localized Rh $4d$ states within the $\mathrm{La}\mathrm{Rh}{\mathrm{O}}_{3}$ band gap. The bandwidth of the impurity band increases with Sr content, eventually causing the valence band (VB) and the localized Rh $4d$ band to overlap, which explains the first insulator-to-metal transition occurring at $x=0.35$. For Sr content $xg0.4$, possible cation ordering results in an increase of the gap between the VB and the Rh $4d$ band, leading to the second metal-to-insulator transition. We map out the electronic phase diagram of the Sr-doped $\mathrm{La}\mathrm{Rh}{\mathrm{O}}_{3}$ system and suggest strategies to engineer the electronic states in rhodate systems via delocalizing the ${\mathrm{Rh}}^{3+}$ states.

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

We study the relaxation of photoexcited electrons in graphite using TR-ARPES. Observed nonthermal electron distributions are modelled using Boltzmann rate-equations, leading to the identification of nonthermal phases in the fluence-delay phase space with broad implications.

Time- and angle-resolved photoemission spectroscopy (TR-ARPES) accesses the electronic structure of solids under optical excitation, and is a powerful technique for studying the coupling between electrons and collective modes. One approach to infer electron-boson coupling is through the relaxation dynamics of optically-excited electrons, and the characteristic timescales of energy redistribution. A common description of electron relaxation dynamics is through the effective electronic temperature. Such a description requires that thermodynamic quantities are well-defined, an assumption that is generally violated at early delays. Additionally, precise estimation of the non-thermal window -- within which effective temperature models may not be applied -- is challenging. We perform TR-ARPES on graphite and show that Boltzmann rate equations can be used to calculate the time-dependent electronic occupation function, and reproduce experimental features given by non-thermal electron occupation. Using this model, we define a quantitative measure of non-thermal electron occupation and use it to define distinct phases of electron relaxation in the fluence-delay phase space. More generally, this approach can be used to inform the non-thermal-to-thermal crossover in pump-probe experiments., Comment: 18 pages, 10 figures

Using a femtosecond extreme ultraviolet source with a narrow linewidth, we observe electrons in graphite scattering with the A 1 ' phonon from optically-populated initial states to well-defined final states, and extract the electron-phonon matrix element.

Topological magnets comprising 2D magnetic layers with Curie temperatures (TC ) exceeding room temperature are key for dissipationless quantum transport devices. However, the identification of a material with 2D ferromagnetic planes that exhibits an out-of-plane-magnetization remains a challenge. This study reports a ferromagnetic, topological, nodal-line, and semimetal MnAlGe composed of square-net Mn layers that are separated by nonmagnetic Al-Ge spacers. The 2D ferromagnetic Mn layers exhibit an out-of-plane magnetization below TC ≈ 503 K. Density functional calculations demonstrate that 2D arrays of Mn atoms control the electrical, magnetic, and therefore topological properties in MnAlGe. The unique 2D distribution of the Berry curvature resembles the 2D Fermi surface of the bands that form the topological nodal line near the Fermi energy. A large anomalous Hall conductivity of ≈700 S cm-1 is obtained at 2 K and related to this nodal-line-induced 2D Berry curvature distribution. The high transition temperature, large anisotropic out-of-plane magnetism, and natural heterostructure-type atomic arrangements consisting of magnetic Mn and nonmagnetic Al/Ge elements render nodal-line MnAlGe one of the few, unique, and layered topological ferromagnets that have ever been observed.

Ultrafast spectroscopies have become an important tool for elucidating the microscopic description and dynamical properties of quantum materials. In particular, by tracking the dynamics of non-thermal electrons, a material's dominant scattering processes -- and thus the many-body interactions between electrons and collective excitations -- can be revealed. Here we present a new method for extracting the electron-phonon coupling strength in the time domain, by means of time and angle-resolved photoemission spectroscopy (TR-ARPES). This method is demonstrated in graphite, where we investigate the dynamics of photo-injected electrons at the K point, detecting quantized energy-loss processes that correspond to the emission of strongly-coupled optical phonons. We show that the observed characteristic timescale for spectral-weight-transfer mediated by phonon-scattering processes allows for the direct quantitative extraction of electron-phonon matrix elements, for specific modes, and with unprecedented sensitivity., 19 pages, 4 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., Revised version as published in Science Advances

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

Monolayer graphene exhibits many spectacular electronic properties, with superconductivity being arguably the most notable exception. It was theoretically proposed that superconductivity might be induced by enhancing the electron-phonon coupling through the decoration of graphene with an alkali adatom superlattice [Profeta et al. Nat. Phys. 8, 131-134 (2012)]. While experiments have indeed demonstrated an adatom-induced enhancement of the electron-phonon coupling, superconductivity has never been observed. Using angle-resolved photoemission spectroscopy (ARPES) we show that lithium deposited on graphene at low temperature strongly modifies the phonon density of states, leading to an enhancement of the electron-phonon coupling of up to $\lambda\!\simeq\!0.58$. On part of the graphene-derived $\pi^*$-band Fermi surface, we then observe the opening of a $\Delta\!\simeq\!0.9$ meV temperature-dependent pairing gap. This result suggests for the first time, to our knowledge, that Li-decorated monolayer graphene is indeed superconducting with $T_c\!\simeq\!5.9 K$., Comment: Accepted. A high-resolution version with supplementary material can be found at http://qmlab.ubc.ca/ARPES/PUBLICATIONS/Articles/Graphene_Li.pdf

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

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 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, realizing a practical source for TR-ARPES that achieves a flux of over 1011 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 MoTe2, as well as TR-ARPES studies on graphite.

We perform time-resolved photoemission on the topological insulator Bi 2 Se 3 at 60 MHz repetition rate, with a 25 eV probe and a 1.2 eV pump, with demonstrated time and energy resolution of < 400 fs and < 25 meV, respectively.

Recent development of extreme ultraviolet (XUV) sources based on high harmonic generation (HHG) in femtosecond enhancement cavities (fsEC) has enabled generation of high photon ux ( 10 13 -10 14 photons/sec) in the XUV, at high repetition rates (> 50 MHz) and spanning the spectral region from 40 nm - 120 nm. Here we demonstrate the potential oered by this approach for angle-resolved photoemission spectroscopy by measuring the photoemission spectrum of Au using 8.3 and 25 eV photons with excellent resolution at rapid data rates.

spin-polarization. We demonstrate the � 100% reversal of a single component of the measured spinpolarizationvector upon the rotation of light polarization, as well as 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 yet fully generalized 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.

We characterize a new table-top, tunable XUV source spanning 8 to 25 eV based on a femtosecond enhancement cavity. This source is designed to investigate correlated electron systems with angle and time resolved photoemission spectroscopy.

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)., 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., 6 pages, 6 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., Submitted to Phys. Rev. Lett

The authors propose a new approach to vibration spectroscopy based on the coherent anti-Stokes Raman scattering of broadband ultrashort laser pulses. The proposed method reveals both the amplitude and the phase of molecular vibrations by utilizing the cross-correlation frequency resolved optical gating (XFROG) technique. The spectrum of the anti-Stokes pulse is measured as a function of the time delay between the laser-induced molecular vibrations and a well characterized broadband femtosecond probe pulse. The iterative XFROG algorithm provides a simultaneous complete characterization of molecular vibrations both in frequency and time domains with high resolution. They demonstrate experimentally the feasibility of the proposed method and show one of its potential applications in disentangling the time behavior of a mixture of vibrationally excited molecules. The technique of femtosecond pulse shaping is used for further improvement of accuracy and stability against noise.