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Homogeneous mixed-valence (MV) behaviour is one of the most intriguing phenomena of f-electron systems. Despite extensive efforts, a fundamental aspect which remains unsettled is the experimental determination of the limiting cases for which MV emerges. Here we address this question for SmB6, a prototypical MV system characterized by two nearly-degenerate Sm2+ and Sm3+ configurations. By combining angle-resolved photoemission spectroscopy (ARPES) and x-ray absorption spectroscopy (XAS), we track the evolution of the mean Sm valence, vSm, in the SmxLa1-xB6 series. Upon substitution of Sm ions with trivalent La, we observe a linear decrease of valence fluctuations to an almost complete suppression at x = 0.2, with vSm ~ 2; surprisingly, by further reducing x, a re-entrant increase of vSm develops, approaching the value of vimp ~ 2.35 in the dilute-impurity limit. Such behaviour departs from a monotonic evolution of vSm across the whole series, as well as from the expectation of its convergence to an integer value for x â 0. Our ARPES and XAS results, complemented by a phenomenological model, demonstrate an unconventional evolution of the MV character in the SmxLa1-xB6 series, paving the way to further theoretical and experimental considerations on the concept of MV itself, and its influence on the macroscopic properties of rare-earth compounds in the dilute-to-intermediate impurity regime.
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We present the development of a versatile apparatus for 6.2 eV laser-based time and angle-resolved photoemission spectroscopy with micrometer spatial resolution (time-resolved µ-ARPES). With a combination of tunable spatial resolution down to â¼11 µm, high energy resolution (â¼11 meV), near-transform-limited temporal resolution (â¼280 fs), and tunable 1.55 eV pump fluence up to 3 mJ/cm2, this time-resolved µ-ARPES system enables the measurement of ultrafast electron dynamics in exfoliated and inhomogeneous materials. We demonstrate the performance of our system by correlating the spectral broadening of the topological surface state of Bi2Se3 with the spatial dimension of the probe pulse, as well as resolving the spatial inhomogeneity contribution to the observed spectral broadening. Finally, after in situ exfoliation, we performed time-resolved µ-ARPES on a â¼30 µm flake of transition metal dichalcogenide WTe2, thus demonstrating the ability to access ultrafast electron dynamics with momentum resolution on micro-exfoliated materials.
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PURPOSE: The early regression index (ERI) predicts treatment response in rectal cancer patients. Aim of current study was to prospectively assess tumor response to neoadjuvant chemo-radiotherapy (nCRT) of locally advanced esophageal cancer using ERI, based on MRI. MATERIAL AND METHODS: From January 2020 to May 2023, 30 patients with esophageal cancer were enrolled in a prospective study (ESCAPE). PET-MRI was performed: i) before nCRT (tpre); ii) at mid-radiotherapy, tmid; iii) after nCRT, 2-6 weeks before surgery (tpost); nCRT delivered 41.4 Gy/23fr with concurrent carboplatin and paclitaxel. For patients that skipped surgery, complete clinical response (cCR) was assessed if patients showed no local relapse after 18 months; patients with pathological complete response (pCR) or with cCR were considered as complete responders (pCR + cCR). GTV volumes were delineated by two observers (Vpre, Vmid, Vpost) on T2w MRI: ERI and other volume regression parameters at tmid and tpost were tested as predictors of pCR + cCR. RESULTS: Complete data of 25 patients were available at the time of the analysis: 3/25 with complete response at imaging refused surgery and 2/3 were cCR; in total, 10/25 patients showed pCR + cCR (pCR = 8/22). Both ERImid and ERIpost classified pCR + cCR patients, with ERImid showing better performance (AUC:0.78, p = 0.014): A two-variable logistic model combining ERImid and Vpre improved performances (AUC:0.93, p < 0.0001). Inter-observer variability in contouring GTV did not affect the results. CONCLUSIONS: Despite the limited numbers, interim analysis of ESCAPE study suggests ERI as a potential predictor of complete response after nCRT for esophageal cancer. Further validation on larger populations is warranted.
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Neoplasias Esofágicas , Imageamento por Ressonância Magnética , Terapia Neoadjuvante , Humanos , Neoplasias Esofágicas/terapia , Neoplasias Esofágicas/diagnóstico por imagem , Neoplasias Esofágicas/patologia , Masculino , Feminino , Estudos Prospectivos , Pessoa de Meia-Idade , Imageamento por Ressonância Magnética/métodos , Idoso , Quimiorradioterapia , Paclitaxel/administração & dosagem , Carboplatina/administração & dosagem , Resultado do Tratamento , Protocolos de Quimioterapia Combinada Antineoplásica/uso terapêutico , AdultoRESUMO
FeSe1-xSx remains one of the most enigmatic systems of Fe-based superconductors. While much is known about the orthorhombic parent compound, FeSe, the tetragonal samples, FeSe1-xSx with x > 0.17, remain relatively unexplored. Here, we provide an in-depth investigation of the electronic states of tetragonal FeSe0.81S0.19, using scanning tunneling microscopy and spectroscopy (STM/S) measurements, supported by angle-resolved photoemission spectroscopy (ARPES) and theoretical modeling. We analyze modulations of the local density of states (LDOS) near and away from Fe vacancy defects separately and identify quasiparticle interference (QPI) signals originating from multiple regions of the Brillouin zone, including the bands at the zone corners. 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. We explore several aspects related to the stripes, 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.
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The interplay between structural and electronic degrees of freedom in complex materials is the subject of extensive debate in physics and materials science. Particularly interesting questions pertain to the nature and extent of pre-transitional short-range order in diverse systems ranging from shape-memory alloys to unconventional superconductors, and how this microstructure affects macroscopic properties. Here we use neutron and X-ray diffuse scattering to uncover universal structural fluctuations in La2-xSrxCuO4 and Tl2Ba2CuO6+δ, two cuprate superconductors with distinct point disorder effects and with optimal superconducting transition temperatures that differ by more than a factor of two. The fluctuations are present in wide doping and temperature ranges, including compositions that maintain high average structural symmetry, and they exhibit unusual, yet simple scaling behaviour. The scaling regime is robust and universal, similar to the well-known critical fluctuations close to second-order phase transitions, but with a distinctly different physical origin. We relate this behaviour to pre-transitional phenomena in a broad class of systems with structural and magnetic transitions, and propose an explanation based on rare structural fluctuations caused by intrinsic nanoscale inhomogeneity. We also uncover parallels with superconducting fluctuations, which indicates that the underlying inhomogeneity plays an important role in cuprate physics.
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Quantum materials are notoriously sensitive to their environments, where small perturbations can tip a system toward one of several competing ground states. Graphene hosts a rich assortment of such competing phases, including a bond density wave instability ("Kekulé distortion") that couples electrons at the K/K' valleys and breaks the lattice symmetry. Here, we report observations of a ubiquitous Kekulé distortion across multiple graphene systems. We show that extremely dilute concentrations of surface atoms (less than three adsorbed atoms every 1000 graphene unit cells) can self-assemble and trigger the onset of a global Kekulé density wave phase. Combining complementary momentum-sensitive angle-resolved photoemission spectroscopy (ARPES) and low-energy electron diffraction (LEED) measurements, we confirm the presence of this density wave phase and observe the opening of an energy gap. Our results reveal an unexpected sensitivity of the graphene lattice to dilute surface disorder and show that adsorbed atoms offer an attractive route toward designing novel phases in two-dimensional materials.
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In spintronics, the two main approaches to actively control the electrons' spin involve static magnetic or electric fields. An alternative avenue relies on the use of optical fields to generate spin currents, which can bolster spin-device performance, allowing for faster and more efficient 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. To explore the optical manipulation of a material's spin properties, we consider the Rashba effect. Using time- and angle-resolved photoemission spectroscopy (TR-ARPES), we demonstrate that an optical excitation can tune the Rashba-induced spin splitting of a two-dimensional electron gas at the surface of Bi2Se3. We establish that light-induced photovoltage and charge carrier redistribution - which in concert modulate the Rashba spin-orbit coupling strength on a sub-picosecond timescale - can offer an unprecedented platform for achieving optically-driven spin logic devices.
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Superconductivity and charge density waves (CDWs) are competitive, yet coexisting, orders in cuprate superconductors. To understand their microscopic interdependence, a probe capable of discerning their interaction on its natural length and time scale is necessary. We use ultrafast resonant soft x-ray scattering to track the transient evolution of CDW correlations in YBa2Cu3O6+x after the quench of superconductivity by an infrared laser pulse. We observe a nonthermal response of the CDW order characterized by a near doubling of the correlation length within ≈1 picosecond of the superconducting quench. Our results are consistent with a model in which the interaction between superconductivity and CDWs manifests inhomogeneously through disruption of spatial coherence, with superconductivity playing the dominant role in stabilizing CDW topological defects, such as discommensurations.
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In strongly correlated systems the strength of Coulomb interactions between electrons, relative to their kinetic energy, plays a central role in determining their emergent quantum mechanical phases. We perform resonant x-ray scattering on Bi2Sr2CaCu2O8+δ, a prototypical cuprate superconductor, to probe electronic correlations within the CuO2 plane. We discover a dynamic quasi-circular pattern in the x-y scattering plane with a radius that matches the wave vector magnitude of the well-known static charge order. Along with doping- and temperature-dependent measurements, our experiments reveal a picture of charge order competing with superconductivity where short-range domains along x and y can dynamically rotate into any other in-plane direction. This quasi-circular spectrum, a hallmark of Brazovskii-type fluctuations, has immediate consequences to our understanding of rotational and translational symmetry breaking in the cuprates. We discuss how the combination of short- and long-range Coulomb interactions results in an effective non-monotonic potential that may determine the quasi-circular pattern.
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Charge density wave (CDW) order has been shown to compete and coexist with superconductivity in underdoped cuprates. Theoretical proposals for the CDW order include an unconventional d-symmetry form factor CDW, evidence for which has emerged from measurements, including resonant soft x-ray scattering (RSXS) in YBa2Cu3O6+x (YBCO). Here, we revisit RSXS measurements of the CDW symmetry in YBCO, using a variation in the measurement geometry to provide enhanced sensitivity to orbital symmetry. We show that the (0 0.31 L) CDW peak measured at the Cu L edge is dominated by an s form factor rather than a d form factor as was reported previously. In addition, by measuring both (0.31 0 L) and (0 0.31 L) peaks, we identify a pronounced difference in the orbital symmetry of the CDW order along the a and b axes, with the CDW along the a axis exhibiting orbital order in addition to charge order.
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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 nonthermal electrons, a material's dominant scattering processes can be revealed. Here, we present a method for extracting the electron-phonon coupling strength in the time domain, using time- and angle-resolved photoemission spectroscopy (TR-ARPES). This method is demonstrated in graphite, where we investigate the dynamics of photoinjected electrons at the [Formula: see text] point, detecting quantized energy-loss processes that correspond to the emission of strongly coupled optical phonons. We show that the observed characteristic time scale for spectral weight transfer mediated by phonon-scattering processes allows for the direct quantitative extraction of electron-phonon matrix elements for specific modes.
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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, enabling 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.
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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.
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Optimally doped cuprate are characterized by the presence of superconducting fluctuations in a relatively large temperature region above the critical transition temperature. We reveal here that the effect of thermal disorder, which decreases the condensate phase coherence at equilibrium, can be dynamically contrasted by photoexcitation with ultrashort midinfrared pulses. In particular, our findings reveal that light pulses with photon energy comparable to the amplitude of the superconducting gap and polarized in plane along the copper-copper direction can dynamically enhance the optical response associated with the onset of superconductivity. We propose that this effect can be rationalized by an effective d-wave BCS model, which reveals that midinfrared pulses result in a transient increase of the phase coherence.
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AIM: To assess whether there is a significant difference in perfusion parameters between benign and malignant prostatic lesions, focusing on semi-quantitative analysis of dynamic contrast-enhanced (DCE) magnetic resonance imaging (MRI) and presence of late gadolinium enhancement (LGE). MATERIAL AND METHODS: Three hundred and thirteen patients who underwent multiparametric MRI (mpMRI) of the prostate and with available corresponding histology (prostatectomy or biopsy) were selected retrospectively for this study. The MRI protocol consisted of multiplanar T2-and diffusion-weighted imaging, DCE and delayed axial T1 images. Images were reviewed independently by two radiologists for LGE assessment and Prostate Imaging - Reporting and Data System (PI-RADS) scoring. For each lesion, semi-quantitative analysis of DCE-MRI was performed and the following data were evaluated: time to peak, wash-in rate, wash-out rate, brevity of enhancement, and area under the curve. The presence or absence of LGE in delayed axial T1 images was assessed qualitatively. MRI results were compared to histology. The presence of significant prostate cancer was based both on Epstein criteria (SPC) and Gleason score (GS ≥7). RESULTS: SPC and Gleason score ≥7 tumours showed significant lower time to peak and brevity of enhancement (p<0.001) with higher wash-in rate (p=0.001). LGE was observed in 152/313 (49%) cases; among them 103/152 (68%) did not show SPC whereas 49/152 (32%) had SPC (p<0.001). The presence of LGE determined a risk reduction of SPC resulting as an independent predictor at multivariate analysis (logOR=-0.78, SE 0.33, p=0.02). CONCLUSION: Semi-quantitative perfusion analysis and LGE may help to predict the presence/absence of a significant prostate tumour and represent a promising tool to improve mpMRI diagnostic performance.
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Meios de Contraste , Gadolínio , Aumento da Imagem/métodos , Imageamento por Ressonância Magnética Multiparamétrica/métodos , Neoplasias da Próstata/diagnóstico por imagem , Adulto , Idoso , Idoso de 80 Anos ou mais , Humanos , Masculino , Pessoa de Meia-Idade , Próstata/diagnóstico por imagem , Reprodutibilidade dos TestesRESUMO
We report on the influence of spin-orbit coupling (SOC) in Fe-based superconductors via application of circularly polarized spin and angle-resolved photoemission spectroscopy. We combine this technique in representative members of both the Fe-pnictides (LiFeAs) and Fe-chalcogenides (FeSe) with tight-binding calculations to establish an ubiquitous modification of the electronic structure in these materials imbued by SOC. At low energy, the influence of SOC is found to be concentrated on the hole pockets, where the largest superconducting gaps are typically found. This effect varies substantively with the k_{z} dispersion, and in FeSe we find SOC to be comparable to the energy scale of orbital order. These results contest descriptions of superconductivity in these materials in terms of pure spin-singlet eigenstates, raising questions regarding the possible pairing mechanisms and role of SOC therein.
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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 interfaces1,2, ultracold Fermi atoms3,4 and cuprate superconductors5,6, 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 Bi2Sr2CaCu2O8+δ 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.
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Spin excitations in the overdoped high temperature superconductors Tl_{2}Ba_{2}CuO_{6+δ} and (Bi,Pb)_{2}(Sr,La)_{2}CuO_{6+δ} were investigated by resonant inelastic x-ray scattering (RIXS) as functions of doping and detuning of the incoming photon energy above the Cu-L_{3} absorption peak. The RIXS spectra at optimal doping are dominated by a paramagnon feature with peak energy independent of photon energy, similar to prior results on underdoped cuprates. Beyond optimal doping, the RIXS data indicate a sharp crossover to a regime with a strong contribution from incoherent particle-hole excitations whose maximum shows a fluorescencelike shift upon detuning. The spectra of both compound families are closely similar, and their salient features are reproduced by exact-diagonalization calculations of the single-band Hubbard model on a finite cluster. The results are discussed in the light of recent transport experiments indicating a quantum phase transition near optimal doping.
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The influence of the Mott physics on the doping-temperature phase diagram of copper oxides represents a major issue that is subject of intense theoretical and experimental effort. Here, we investigate the ultrafast electron dynamics in prototypical single-layer Bi-based cuprates at the energy scale of the O-2pâCu-3d charge-transfer (CT) process. We demonstrate a clear evolution of the CT excitations from incoherent and localized, as in a Mott insulator, to coherent and delocalized, as in a conventional metal. This reorganization of the high-energy degrees of freedom occurs at the critical doping pcr ≈0.16 irrespective of the temperature, and it can be well described by dynamical mean field theory calculations. We argue that the onset of the low-temperature charge instabilities is the low-energy manifestation of the underlying Mottness that characterizes the p < pcr region of the phase diagram. This discovery sets a new framework for theories of charge order and low-temperature phases in underdoped copper oxides.