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Using light to control transient phases in quantum materials is an emerging route to engineer new properties and functionality, with both thermal and non-thermal phases observed out of equilibrium. Transient phases are expected to be heterogeneous, either through photo-generated domain growth or by generating topological defects, and this impacts the dynamics of the system. However, this nanoscale heterogeneity has not been directly observed. Here we use time- and spectrally resolved coherent X-ray imaging to track the prototypical light-induced insulator-to-metal phase transition in vanadium dioxide on the nanoscale with femtosecond time resolution. We show that the early-time dynamics are independent of the initial spatial heterogeneity and observe a 200 fs switch to the metallic phase. A heterogeneous response emerges only after hundreds of picoseconds. Through spectroscopic imaging, we reveal that the transient metallic phase is a highly orthorhombically strained rutile metallic phase, an interpretation that is in contrast to those based on spatially averaged probes. Our results demonstrate the critical importance of spatially and spectrally resolved measurements for understanding and interpreting the transient phases of quantum materials.The intermediate states in photo-excited phase transitions are expected to be inhomogeneous. However, ultrafast X-ray imaging shows the early part of the metal–insulator transition in VO2 is homogeneous but then becomes heterogeneous.

To pinpoint the electronic and structural mechanisms that affect intrinsic and extrinsic performance limits of 2D material devices, it is of critical importance to resolve the electronic properties on the mesoscopic length scale of such devices under operating conditions. Herein, angle‐resolved photoemission spectroscopy with nanoscale spatial resolution (nanoARPES) is used to map the quasiparticle electronic structure of a twisted bilayer graphene device. The dispersion and linewidth of the Dirac cones associated with top and bottom graphene layers are determined as a function of spatial position on the device under both static and operating conditions. The analysis reveals that microscopic rotational domains in the two graphene layers establish a range of twist angles from 9.8° to 12.7°. Application of current and electrostatic gating lead to strong electric fields with peak strengths of 0.75 V/μm at the rotational domain boundaries in the device. These proof‐of‐principle results demonstrate the potential of nanoARPES to link mesoscale structural variations with electronic states in operating device conditions and to disentangle such extrinsic factors from the intrinsic quasiparticle dispersion. Nanoscale angle‐resolved photoemission spectroscopy is applied to map the electronic structure of a twisted bilayer graphene device during the application of current and an electrostatic gate voltage. Rotational domains are found to strongly affect the measured linewidth of the top and bottom Dirac cones and lead to a spatially inhomogeneous electric field during operation of the device.

Reliable methods to individually track large numbers of cells in real time are urgently needed to advance our understanding of important biological processes like cancer metastasis, neuronal network development and wound healing. It has recently been suggested to introduce microscopic whispering gallery mode lasers into the cytoplasm of cells and to use their characteristic, size-dependent emission spectrum as optical barcode but so far there is no evidence that this approach is generally applicable. Here, we describe a method that drastically improves intracellular delivery of resonators for several cell types, including mitotic and non-phagocytic cells. In addition, we characterize the influence of resonator size on the spectral characteristics of the emitted laser light and identify an optimum size range that facilitates tagging and tracking of thousands of cells simultaneously. Finally, we observe that the microresonators remain internalized by cells during cell division, which enables tagging several generations of cells.

Heterostructures composed of the intrinsic magnetic topological insulator MnBi\\(_2\\)Te\\(_4\\) and its non-magnetic counterpart Bi\\(_2\\)Te\\(_3\\) host distinct surface electronic band structures depending on the stacking order and exposed termination. Here, we probe the ultrafast dynamical response of MnBi\\(_2\\)Te\\(_4\\) and MnBi\\(_4\\)Te\\(_7\\) following near-infrared optical excitation using time- and angle-resolved photoemission spectroscopy, and disentangle surface from bulk dynamics based on density functional theory slab calculations of the surface-projected electronic structure. We gain access to the out-of-equilibrium charge carrier populations of both MnBi\\(_2\\)Te\\(_4\\) and Bi\\(_2\\)Te\\(_3\\) surface terminations of MnBi\\(_4\\)Te\\(_7\\), revealing an instantaneous occupation of states associated with the Bi\\(_2\\)Te\\(_3\\) surface layer followed by carrier extraction into the adjacent MnBi\\(_2\\)Te\\(_4\\) layers with a laser fluence-tunable delay of up to 350 fs. The ensuing thermal relaxation processes are driven by phonon scattering with significantly slower relaxation times in the magnetic MnBi\\(_2\\)Te\\(_4\\) septuple layers. The observed competition between interlayer charge transfer and intralayer phonon scattering demonstrates a method to control ultrafast charge transfer processes in MnBi\\(_2\\)Te\\(_4\\)-based van der Waals compounds.

X-ray photoelectron diffraction is a powerful tool for determining the structure of clean and adsorbate-covered surfaces. Extending the technique into the ultrafast time domain will open the door to studies as diverse as the direct determination of the electron-phonon coupling strength in solids and the mapping of atomic motion in surface chemical reactions. Here we demonstrate time-resolved photoelectron diffraction using ultrashort soft X-ray pulses from the free electron laser FLASH. We collect Se 3d photoelectron diffraction patterns over a wide angular range from optically excited Bi\\(_2\\)Se\\(_3\\) with a time resolution of 140 fs. Combining these with multiple scattering simulations allows us to track the motion of near-surface atoms within the first 3 ps after triggering a coherent vibration of the A\\(_{1g}\\) optical phonons. Using a fluence of 4.2 mJ/cm\\(^2\\) from a 1.55 eV pump laser, we find the resulting coherent vibrational amplitude in the first two interlayer spacings to be on the order of 1 pm.

Using light to control transient phases in quantum materials is an emerging route to engineer new properties and functionality, with both thermal and non-thermal phases observed out of equilibrium. Transient phases are expected to be heterogeneous, either through photo-generated domain growth or by generating topological defects, and this impacts the dynamics of the system. However, this nanoscale heterogeneity has not been directly observed. Here we use time- and spectrally resolved coherent X-ray imaging to track the prototypical light induced insulator-to-metal phase transition in vanadium dioxide on the nanoscale with femtosecond time resolution. We show that the early-time dynamics are independent of the initial spatial heterogeneity and observe a 200 fs switch to the metallic phase. A heterogeneous response emerges only after hundreds of picoseconds. Through spectroscopic imaging, we reveal that the transient metallic phase is a highly orthorhombically strained rutile metallic phase, an interpretation that is in contrast to those based on spatially averaged probes. Our results demonstrate the critical importance of spatially and spectrally resolved measurements for understanding and interpreting the transient phases of quantum materials.

Screening in reduced dimensions has strong consequences on the electronic properties in van der Waals semiconductors, impacting the quasiparticle band gap and exciton binding energy. Screening in these materials is typically treated isotropically, yet black phosphorus exhibits in-plane electronic anisotropy seen in its effective mass, carrier mobility, excitonic wavefunctions, and plasmonic dispersion. Here, we use the adsorption of individual potassium atoms on the surface of black phosphorus to vary the near-surface doping over a wide range, while simultaneously probing the dielectric screening via the ordering of the adsorbed atoms. Using scanning tunneling microscopy, we visualize the role of strongly anisotropic screening which leads to the formation of potassium chains with a well-defined orientation and spacing. We quantify the mean interaction potential utilizing statistical methods and find that the dimensionality and anisotropy of the screening is consistent with the presence of a band-bending induced confinement potential near the surface. We corroborate the observed behavior with coverage-dependent studies of the electronic structure with angle-resolved photoemission.

The presence of an electrical transport current in a material is one of the simplest and most important realisations of non-equilibrium physics. The current density breaks the crystalline symmetry and can give rise to dramatic phenomena, such as sliding charge density waves [1], insulator-to-metal transitions [2,3] or gap openings in topologically protected states [4]. Almost nothing is known about how a current influences the electron spectral function, which characterizes most of the solid's electronic, optical and chemical properties. Here we show that angle-resolved photoemission spectroscopy with a nano-scale light spot (nanoARPES) provides not only a wealth of information on local equilibrium properties, but also opens the possibility to access the local non-equilibrium spectral function in the presence of a transport current. Unifying spectroscopic and transport measurements in this way allows non-invasive local measurements of the composition, structure, many-body effects and carrier mobility in the presence of high current densities.