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1$T$-TaSe$_2$ is a prototypical charge density wave (CDW) material for which electron-phonon coupling and associated lattice distortion play an important role in driving and stabilizing the CDW phase. Here, we investigate the lattice dynamics of bulk 1$T$-TaSe$_2$ using angle-resolved ultralow wavenumber Raman spectroscopy down to 10 cm$^{-1}$. Our high-resolution spectra allow us to identify at least 27 Raman-active modes in the commensurate (CCDW) phase. Contrary to other layered materials, we do not find evidence of interlayer breathing or shear modes, suggestive of $AA$ stacking in the bulk, or sufficiently weak interlayer coupling. Polarization dependence of the mode intensities allows the assignment of their symmetry, which is supported by first-principles calculations of the phonons for the bulk structure using density functional theory. A detailed temperature dependence in the range $T$ = 80 - 500 K allows us to identify soft modes associated with the CDW superlattice. Upon entering the incommensurate (ICCDW) phase above 473 K, we observe a dramatic loss of resolution of all modes, and significant linewidth broadening associated with a reduced phonon lifetime as the charge-order becomes incommensurate with the lattice., Comment: 8 pages, 3 figures, supplemental material

1$T$-TaSe$_2$ is widely believed to host a Mott metal-insulator transition in the charge density wave (CDW) phase according to the spectroscopic observation of a band gap that extends across all momentum space. Previous investigations inferred that the occurrence of the Mott phase is limited to the surface only of bulk specimens, but recent analysis on thin samples revealed that the Mott-like behavior, observed in the monolayer, is rapidly suppressed with increasing thickness. Here, we report combined time- and angle-resolved photoemission spectroscopy and theoretical investigations of the electronic structure of 1$T$-TaSe$_2$. Our experimental results confirm the existence of a state above $E_F$, previously ascribed to the upper Hubbard band, and an overall band gap of $\sim 0.7$ eV at $\overline{\Gamma}$. However, supported by density functional theory calculations, we demonstrate that the origin of this state and the gap rests on band structure modifications induced by the CDW phase alone, without the need for Mott correlation effects., Comment: Accepted by PRL

We discuss layout and performance of a high-resolution Stimulated Raman Loss spectrometer that has been newly developed for accurate studies of spectral lineshapes and line center frequencies of hydrogen isotopologues and in general of Raman active transitions. Thanks to the frequency comb calibration of the detuning between pump and Stokes lasers and to an active alignment of the two beams, the frequency accuracy is well below 100 kHz. Over the vertical axis the spectrometer benefits from shot-noise limited detection, signal enhancement via multipass cell, active flattening of the spectral baseline and measurement times of few seconds over spectral spans larger than 10 GHz. Under these conditions an efficient averaging of Raman spectra is possible over long measurement times with minimal distortion of spectral lineshapes. By changing the pump laser, transitions can be covered in a very broad frequency span, from 50 to 5000 $\mathrm{cm^{-1}}$, including both vibrational and rotational bands. The spectrometer has been developed for studies of fundamental and collisional physics of hydrogen isotopologues and has been recently applied to the metrology of the Q(1) 1-0 line of $\mathrm{H_2}$.

Nonlinear optics is of crucial importance in several fields of science and technology with applications in frequency conversion, entangled-photon generation, self-referencing of frequency combs, crystal characterization, sensing, and ultra-short light pulse generation and characterization. In recent years, layered materials and related heterostructures have attracted huge attention in this field, due to their huge nonlinear optical susceptibilities, their ease of integration on photonic platforms, and their 2D nature which relaxes the phase-matching constraints and thus offers a practically unlimited bandwidth for parametric nonlinear processes. In this review the most recent advances in this field, highlighting their importance and impact both for fundamental and technological aspects, are reported and explained, and an outlook on future research directions for nonlinear optics with atomically thin materials is provided.

Frequency combs have revolutionized optical frequency metrology, allowing one to determine highly accurate transition frequencies of a wealth of molecular species. Despite a recognized scientific interest, these progresses have only marginally benefited infrared-inactive transitions, due to their inherently weak cross-sections. Here we overcome this limitation by introducing stimulated-Raman-scattering metrology, where a frequency comb is exploited to calibrate the frequency detuning between the pump and Stokes excitation lasers. We apply this approach to molecular hydrogen to test quantum electrodynamics. We measure the transition frequency of the Q(1) fundamental line of H$_2$ around 4155 cm$^{-1}$ with few parts-per-billion uncertainty, which is comparable to the theoretical benchmark of ab initio calculations and more than a decade better than the experimental state of the art. Our comb-calibrated stimulated Raman scattering spectrometer extends the toolkit of optical frequency metrology as it can be applied, with simple technical changes, to many other infrared-inactive transitions, over a 50-5000 cm$^{-1}$ range that covers also purely rotational bands.

Spintronics is postulated on the possibility to employ the magnetic degree of freedom of electrons for computation and couple it to charges. In this view, the combination of the high-frequency of spin manipulations offered by antiferromagnets, with the wide tunability of the electronic properties peculiar of semiconductors provides a promising and intriguing platform. Here we explore this scenario in $\alpha$-MnTe, which is a semiconductor antiferromagnetically ordered at room temperature. Relying on a Raman mechanism and femtosecond laser pulses, we drive degenerate modes of coherent optical phonons, which modulate the chemical bonds involved in the super-exchange interaction. The spectrally-resolved measurements of the transient reflectivity reveal a coherent modulation of the band-gap at the frequency of 5.3 THz. The detection of the rotation of the polarisation, typically associated with magneto-optical effects, shows coherent and incoherent contributions. Modelling how the ionic motion induced by the phonons affects the exchange interaction in the material, we calculate the photoinduced THz spin dynamics: the results predict both a coherent and incoherent response, the latter of which is consistent with the experimental observation. Our work demonstrates that the same phonon modes modulate both the charge and magnetic degree of freedom, suggesting the resonant pumping of phonons as a viable way to link spin and charge dynamics even in nonlinear regimes.

Current precision experiments with single (anti)protons to test CPT symmetry progress at a rapid pace, but are complicated by the need to cool particles to sub-thermal energies. We describe a cryogenic Penning-trap setup for $^9$Be$^+$ ions designed to allow coupling of single (anti)protons to laser-cooled atomic ions for sympathetic cooling and quantum logic spectroscopy. We report on trapping and laser cooling of clouds and single $^9$Be$^+$ ions. We discuss prospects for a microfabricated trap to allow coupling of single (anti)protons to laser-cooled $^9$Be$^+$ ions for sympathetic laser cooling to sub-mK temperatures on ms time scales., Comment: Presented at the Eighth Meeting on CPT and Lorentz Symmetry, Bloomington, Indiana, May 12-16, 2019

The rate at which matter emits or absorbs light can be modified by its environment, as dramatically exemplified by the widely-studied phenomenon of superradiance. The reverse process, superabsorption, is harder to demonstrate due to the challenges of probing ultrafast processes, and has only been seen for small numbers of atoms. Its central idea - superextensive scaling of absorption meaning larger systems absorb faster - is also the key idea underpinning quantum batteries. Here we implement experimentally a paradigmatic model of a quantum battery, constructed of a microcavity enclosing a molecular dye. Ultrafast optical spectroscopy allows us to observe charging dynamics at femtosecond resolution to demonstrate superextensive charging rates and storage capacity, in agreement with our theoretical modelling. We find that decoherence plays an important role in stabilising energy storage. Our work opens new opportunities for harnessing collective effects in light-matter coupling for nanoscale energy capture, storage, and transport technologies., Comment: 42 pages, 20 figures, 3 tables

1$T$-TaSe$_{2}$ is host to coexisting strongly-correlated phases including charge density waves (CDWs) and an unusual Mott transition at low temperature. Here, we investigate coherent phonon oscillations in 1$T$-TaSe$_{2}$ using a combination of time- and angle-resolved photoemission spectroscopy (TR-ARPES) and time-resolved reflectivity (TRR). Perturbation by a femtosecond laser pulse triggers a modulation of the valence band binding energy at the $\Gamma$-point, related to the Mott gap, that is consistent with the in-plane CDW amplitude mode frequency. By contrast, TRR measurements show a modulation of the differential reflectivity comprised of multiple frequencies belonging to the distorted CDW lattice modes. Comparison of the temperature dependence of coherent and spontaneous phonons across the CDW transition shows that the amplitude mode intensity is more easily suppressed during perturbation of the CDW state by the optical excitation compared to other modes. Our results clearly identify the relationship of the in-plane CDW amplitude mode with the Mott phase in 1$T$-TaSe$_{2}$ and highlight the importance of lattice degrees of freedom., Comment: 7 pages, 4 figures, supplemental material

Black phosphorous (BP) is a layered semiconductor with high carrier mobility, anisotropic optical response and wide bandgap tunability. In view of its application in optoelectronic devices, understanding transient photo-induced effects is crucial. Here, we investigate by time- and angle-resolved photoemission spectroscopy BP in its pristine state and in the presence of Stark splitting, chemically induced by Cs ad-sorption. We show that photo-injected carriers trigger bandgap renormalization and a concurrent valence band attening caused by Pauli blocking. In the biased sample, photoexcitation leads to a long-lived (ns) surface photovoltage of few hundreds mV that counterbalances the Cs-induced surface band bending. This allows us to disentangle bulk from surface electronic states and to clarify the mechanism underlying the band inversion observed in bulk samples.

We present a transient absorption setup combining broadband detection over the visible-UV range with high temporal resolution ($\sim$20fs) which is ideally suited to trigger and detect vibrational coherences in different classes of materials. We generate and detect coherent phonons (CPs) in single layer (1L) MoS$_2$, as a representative semiconducting 1L-transition metal dichalcogenide (TMD), where the confined dynamical interaction between excitons and phonons is unexplored. The coherent oscillatory motion of the out-of-plane $A'_{1}$ phonons, triggered by the ultrashort laser pulses, dynamically modulates the excitonic resonances on a timescale of few tens fs. We observe an enhancement by almost two orders of magnitude of the CP amplitude when detected in resonance with the C exciton peak, combined with a resonant enhancement of CP generation efficiency. Ab initio calculations of the change in 1L-MoS$_2$ band structure induced by the $A'_{1}$ phonon displacement confirm a strong coupling with the C exciton. The resonant behavior of the CP amplitude follows the same spectral profile of the calculated Raman susceptibility tensor. This demonstrates that CP excitation in 1L-MoS$_2$ can be described as a Raman-like scattering process. These results explain the CP generation process in 1L-TMDs, paving the way for coherent all-optical control of excitons in layered materials in the THz frequency range.

We introduce a wide field hyperspectral microscope using the Fourier-transform approach. The interferometer is based on the Translating-Wedge-Based Identical Pulses eNcoding System (TWINS) [Opt. Lett. 37, 3027 (2012)], a common-path birefringent interferometer which combines compactness, intrinsic interferometric delay precision, long-term stability and insensitivity to vibrations. We describe three different implementations of our system: two prototypes designed to test different optical schemes and an add-on for a commercial microscope. We show high-quality spectral microscopy of the fluorescence from stained cells and powders of inorganic pigments, demonstrating that the device is suited to biology and materials science. We demonstrate the acquisition of a 1Mpixel hyperspectral image in 75 seconds in the spectral range from 400 to 1100 nm. We also introduce an acquisition method which synthesizes a tunable spectral filter, providing band-passed images by the measurement of only two maps., Comment: 16 pages, 11 figures

In Broadband Stimulated Raman Spectroscopy, the intrinsic limit given by the laser shot noise is seldom reached due to the electronic noise of the front-end amplifier and the intensity fluctuations of the laser source. In this paper we present a low-noise multi-channel acquisition system, with an integration-oriented design, able to compensate the common-mode fluctuations of the laser output power with the pseudo-differential structure and reach a sensitivity better than 10 ppm thanks to the lock-in technique., Comment: Post review version

We demonstrate quantum control of $^9$Be$^+$ ions directly implemented by an optical frequency comb. Based on numerical simulations of the relevant processes in $^9$Be$^+$ for different magnetic field regimes, we demonstrate a wide applicability when controlling the comb's spectral properties. We introduce a novel technique for the selective and efficient generation of a spectrally tailored narrow-bandwidth optical frequency comb near 313 nm. We experimentally demonstrate internal state control and internal-motional state coupling of $^9$Be$^+$ ions implemented by stimulated-Raman manipulation using a spectrally optimized optical frequency comb. Our pulsed laser approach is a key enabling step for the implementation of quantum logic and quantum information experiments in Penning traps., Comment: Includes supplementary material

Hot electrons dominate the ultrafast ($\sim$fs-ps) optical and electronic properties of metals and semiconductors and they are exploited in a variety of applications including photovoltaics and photodetection. We perform power-dependent third harmonic generation measurements on gated single-layer graphene and detect a significant deviation from the cubic power-law expected for a third harmonic generation process. We assign this to the presence of hot electrons. Our results indicate that the performance of nonlinear photonics devices based on graphene, such as optical modulators and frequency converters, can be affected by changes in the electronic temperature, which might occur due to increase of absorbed optical power or Joule heating.

We report stimulated Raman spectroscopy of the G phonon in both single and multi-layer graphene, through Coherent anti-Stokes Raman Scattering (CARS). The signal generated by the third order nonlinearity is dominated by a vibrationally non-resonant background (NVRB), which obscures the Raman lineshape. We demonstrate that the vibrationally resonant CARS peak can be measured by reducing the temporal overlap of the laser excitation pulses, suppressing the NVRB. We model the observed spectra, taking into account the electronically resonant nature of both CARS and NVRB. We show that CARS can be used for graphene imaging with vibrational sensitivity., Comment: 10 pages, 5 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

In monolayer Transition Metal Dichalcogenides (TMDs) the valence and conduction bands are spin split because of the strong spin-orbit interaction. In tungsten-based TMDs the spin-ordering of the conduction band is such that the so-called dark exciton, consisting of an electron and a hole with opposite spin orientation, has lower energy than the A exciton. A possible mechanism leading to the transition from bright to dark excitons involves the scattering of the electrons from the upper to the lower conduction band state in K. Here we exploit the valley selective optical selection rules and use two-color helicity-resolved pump-probe spectroscopy to directly measure the intravalley spin-flip relaxation dynamics of electrons in the conduction band of single-layer WS$_2$. This process occurs on a sub-ps time scale and it is significantly dependent on the temperature, indicative of a phonon-assisted relaxation. These experimental results are supported by time-dependent ab-initio calculations which show that the intra-valley spin-flip scattering occurs on significantly longer time scales only exactly at the K point. In a realistic situation the occupation of states away from the minimum of the conduction band leads to a dramatic reduction of the scattering time.

In this work, we report the first demonstration of a solution processable, optically switchable 1D photonic crystal by implementing phototunable doped metal oxide nanocrystals. The resulting device structure shows bi-photonic response with the photonic bandgap covering the visible spectral range and the plasmon resonance of the doped metal oxide the near infrared. By means of a facile photodoping process, we tuned the plasmonic response and switched effectively the optical properties of the photonic crystal, translating the effect from the near infrared to the visible. The ultrafast bandgap pumping induces a signal change in the region of the photonic stopband, with recovery times of several picoseconds, providing a step toward the ultrafast optical switching. Optical modeling uncovers the importance to understand largely the variations of the dielectric function of the photodoped material, and variations in the high frequency region of the Drude response are responsible for the strong switching in the visible after photodoping. Our device configuration offers unprecedented tunablility due to flexibility in device design, cover wavelength ranges from the visible to the near infrared. Our findings indicate a new protocol to modify the optical response of photonic devices by optical triggers only., Comment: 12 pages, 3 figures

The impulsive generation of two-magnon modes in antiferromagnets by femtosecond optical pulses, so-called femto-nanomagnons, leads to coherent longitudinal oscillations of the antiferromagnetic order parameter that cannot be described by a thermodynamic Landau-Lifshitz approach. We argue that this dynamics is triggered as a result of a laser-induced modification of the exchange interaction. In order to describe the oscillations we have formulated a quantum mechanical description in terms of magnon pair operators and coherent states. Such an approach allowed us to} derive an effective macroscopic equation of motion for the temporal evolution of the antiferromagnetic order parameter. An implication of the latter is that the photo-induced spin dynamics represents a macroscopic entanglement of pairs of magnons with femtosecond period and nanometer wavelength. By performing magneto-optical pump-probe experiments with 10 femtosecond resolution in the cubic KNiF$_3$ and the uniaxial K$_2$NiF$_4$ collinear Heisenberg antiferromagnets, we observed coherent oscillations at the frequency of 22 THz and 16 THz, respectively. The detected frequencies as a function of the temperature ideally fit the two-magnon excitation up to the N\'eel point. The experimental signals are described as dynamics of magnetic linear dichroism due to longitudinal oscillations of the antiferromagnetic vector., Comment: 25 pages, 10 figures

Optical harmonic generation occurs when high intensity light ($>10^{10}$W/m$^{2}$) interacts with a nonlinear material. Electrical control of the nonlinear optical response enables applications such as gate-tunable switches and frequency converters. Graphene displays exceptionally strong-light matter interaction and electrically and broadband tunable third order nonlinear susceptibility. Here we show that the third harmonic generation efficiency in graphene can be tuned by over two orders of magnitude by controlling the Fermi energy and the incident photon energy. This is due to logarithmic resonances in the imaginary part of the nonlinear conductivity arising from multi-photon transitions. Thanks to the linear dispersion of the massless Dirac fermions, ultrabroadband electrical tunability can be achieved, paving the way to electrically-tuneable broadband frequency converters for applications in optical communications and signal processing.

The equilibrium optical phonons of graphene are well characterized in terms of anharmonicity and electron-phonon interactions, however their non-equilibrium properties in the presence of hot charge carriers are still not fully explored. Here we study the Raman spectrum of graphene under ultrafast laser excitation with 3ps pulses, which trade off between impulsive stimulation and spectral resolution. We localize energy into hot carriers, generating non-equilibrium temperatures in the ~1700-3100K range, far exceeding that of the phonon bath, while simultaneously detecting the Raman response. The linewidth of both G and 2D peaks show an increase as function of the electronic temperature. We explain this as a result of the Dirac cones' broadening and electron-phonon scattering in the highly excited transient regime, important for the emerging field of graphene-based photonics and optoelectronics., Comment: 10 pages, 7 figures

Van der Waals heterostructures have emerged as promising building blocks that offer access to new physics, novel device functionalities, and superior electrical and optoelectronic properties. Applications such as thermal management, photodetection, light emission, data communication, high-speed electronics and light harvesting require a thorough understanding of (nanoscale) heat flow. Here, using time-resolved photocurrent measurements we identify an efficient out-of-plane energy transfer channel, where charge carriers in graphene couple to hyperbolic phonon polaritons in the encapsulating layered material. This hyperbolic cooling is particularly efficient, giving picosecond cooling times, for hexagonal BN, where the high-momentum hyperbolic phonon polaritons enable efficient near-field energy transfer. We study this heat transfer mechanism through distinct control knobs to vary carrier density and lattice temperature, and find excellent agreement with theory without any adjustable parameters. These insights may lead to the ability to control heat flow in van der Waals heterostructures.

Glasses are out-of-equilibrium systems aging under the crystallization threat. During ordinary glass formation, the atomic diffusion slows down rendering its experimental investigation impractically long, to the extent that a timescale divergence is taken for granted by many. We circumvent here these limitations, taking advantage of a wide family of glasses rapidly obtained by physical vapor deposition directly into the solid state, endowed with different "ages" rivaling those reached by standard cooling and waiting for millennia. Isothermally probing the mechanical response of each of these glasses, we infer a correspondence with viscosity along the equilibrium line, up to exapoise values. We find a dependence of the elastic modulus on the glass age, which, traced back to temperature steepness index of the viscosity, tears down one of the cornerstones of several glass transition theories: the dynamical divergence. Critically, our results suggest that the conventional wisdom picture of a glass ceasing to flow at finite temperature could be wrong., Comment: 4 figures and 1 supplementary figure

The understanding of how the sub-nanoscale exchange interaction evolves in macroscale correlations and ordered phases of matter, such as magnetism and superconductivity, requires to bridge the quantum and classical worlds. This monumental challenge has so far only been achieved for systems close to their thermodynamical equilibrium. Here we follow in real time the ultrafast dynamics of the macroscale magnetic order parameter triggered by the impulsive optical generation of spin excitations with the shortest possible nanometer-wavelength and femtosecond-period. Our experiments also disclose a possibility for the coherent control of these femtosecond nanomagnons, which are defined by the exchange energy. These findings open up novel opportunities for fundamental research on the role of short-wavelength spin excitations in magnetism and high-temperature superconductivity, since they provide a macroscopic probe of the femtosecond dynamics of sub-nanometer spin-spin correlations and, ultimately, of the exchange energy. With this approach it becomes possible to trace the dynamics of such short-range magnetic correlations for instance during phase transitions. Moreover, our work suggests that nanospintronics and nanomagnonics can employ phase-controllable spin waves with frequencies in the 20 THz domain.

Valleytronics targets the exploitation of the additional degrees of freedom in materials where the energy of the carriers may assume several equal minimum values (valleys) at non-equivalent points of the reciprocal space. In single layers of transition metal dichalcogenides (TMDs) the lack of inversion symmetry, combined with a large spin-orbit interaction, leads to a conduction (valence) band with different spin-polarized minima (maxima) having equal energies. This offers the opportunity to manipulate information at the level of the charge (electrons or holes), spin (up or down) and crystal momentum (valley). Any implementation of these concepts, however, needs to consider the robustness of such degrees of freedom, which are deeply intertwined. Here we address the spin and valley relaxation dynamics of both electrons and holes with a combination of ultrafast optical spectroscopy techniques, and determine the individual characteristic relaxation times of charge, spin and valley in a MoS$_{2}$ monolayer. These results lay the foundations for understanding the mechanisms of spin and valley polarization loss in two-dimensional TMDs: spin/valley polarizations survive almost two-orders of magnitude longer for holes, where spin and valley dynamics are interlocked, than for electrons, where these degrees of freedom are decoupled. This may lead to novel approaches for the integration of materials with large spin-orbit in robust spintronic/valleytronic platforms.

One of the pivotal questions in the physics of high-temperature superconductors is whether the low-energy dynamics of the charge carriers is mediated by bosons with a characteristic timescale. This issue has remained elusive since electronic correlations are expected to dramatically speed up the electron-boson scattering processes, confining them to the very femtosecond timescale that is hard to access even with state-of-the-art ultrafast techniques. Here we simultaneously push the time resolution and the frequency range of transient reflectivity measurements up to an unprecedented level that enables us to directly observe the 16 fs build-up of the effective electron-boson interaction in hole-doped copper oxides. This extremely fast timescale is in agreement with numerical calculations based on the t-J model and the repulsive Hubbard model, in which the relaxation of the photo-excited charges is achieved via inelastic scattering with short-range antiferromagnetic excitations., Comment: to appear in Nature Physics