ABSTRACT
In quantum materials, degeneracies and frustrated interactions can have a profound impact on the emergence of long-range order, often driving strong fluctuations that suppress functionally relevant electronic or magnetic phases1-7. Engineering the atomic structure in the bulk or at heterointerfaces has been an important research strategy to lift these degeneracies, but these equilibrium methods are limited by thermodynamic, elastic and chemical constraints8. Here we show that all-optical, mode-selective manipulation of the crystal lattice can be used to enhance and stabilize high-temperature ferromagnetism in YTiO3, a material that shows only partial orbital polarization, an unsaturated low-temperature magnetic moment and a suppressed Curie temperature, Tc = 27 K (refs. 9-13). The enhancement is largest when exciting a 9 THz oxygen rotation mode, for which complete magnetic saturation is achieved at low temperatures and transient ferromagnetism is realized up to Tneq > 80 K, nearly three times the thermodynamic transition temperature. We interpret these effects as a consequence of the light-induced dynamical changes to the quasi-degenerate Ti t2g orbitals, which affect the magnetic phase competition and fluctuations found in the equilibrium state14-20. Notably, the light-induced high-temperature ferromagnetism discovered in our work is metastable over many nanoseconds, underscoring the ability to dynamically engineer practically useful non-equilibrium functionalities.
ABSTRACT
Crystal lattice fluctuations, which are known to influence phase transitions of quantum materials in equilibrium, are also expected to determine the dynamics of light-induced phase changes. However, they have only rarely been explored in these dynamical settings. Here we study the time evolution of lattice fluctuations in the quantum paraelectric SrTiO3, in which mid-infrared drives have been shown to induce a metastable ferroelectric state. Crucial in these physics is the competition between polar instabilities and antiferrodistortive rotations, which in equilibrium frustrate the formation of long-range ferroelectricity. We make use of high-intensity mid-infrared optical pulses to resonantly drive the Ti-O-stretching mode at 17 THz, and we measure the resulting change in lattice fluctuations using time-resolved X-ray diffuse scattering at a free-electron laser. After a prompt increase, we observe a long-lived quench in R-point antiferrodistortive lattice fluctuations. Their enhancement and reduction are theoretically explained by considering the fourth-order nonlinear phononic interactions to the driven optical phonon and third-order coupling to lattice strain, respectively. These observations provide a number of testable hypotheses for the physics of light-induced ferroelectricity.
ABSTRACT
Nonlinear optical techniques at visible frequencies have long been applied to condensed matter spectroscopy. However, because many important excitations of solids are found at low energies, much can be gained from the extension of nonlinear optics to mid-infrared and terahertz frequencies. For example, the nonlinear excitation of lattice vibrations has enabled the dynamic control of material functions. So far it has only been possible to exploit second-order phonon nonlinearities at terahertz field strengths near one million volts per centimetre. Here we achieve an order-of-magnitude increase in field strength and explore higher-order phonon nonlinearities. We excite up to five harmonics of the A1 (transverse optical) phonon mode in the ferroelectric material lithium niobate. By using ultrashort mid-infrared laser pulses to drive the atoms far from their equilibrium positions, and measuring the large-amplitude atomic trajectories, we can sample the interatomic potential of lithium niobate, providing a benchmark for ab initio calculations for the material. Tomography of the energy surface by high-order nonlinear phononics could benefit many aspects of materials research, including the study of classical and quantum phase transitions.
ABSTRACT
INTRODUCTION: Microcirculatory alterations are key mechanisms in sepsis pathophysiology leading to tissue hypoxia, edema formation, and organ dysfunction. Hyperspectral imaging (HSI) is an emerging imaging technology that uses tissue-light interactions to evaluate biochemical tissue characteristics including tissue oxygenation, hemoglobin content and water content. Currently, clinical data for HSI technologies in critical ill patients are still limited. METHODS AND ANALYSIS: TIVITA® Tissue System was used to measure Tissue oxygenation (StO2), Tissue Hemoglobin Index (THI), Near Infrared Perfusion Index (NPI) and Tissue Water Index (TWI) in 25 healthy volunteers and 25 septic patients. HSI measurement sites were the palm, the fingertip, and a suprapatellar knee area. Septic patients were evaluated on admission to the ICU (E), 6 h afterwards (E+6) and three times a day (t3-t9) within a total observation period of 72 h. Primary outcome was the correlation of HSI results with daily SOFA-scores. RESULTS: Serial HSI at the three measurement sites in healthy volunteers showed a low mean variance expressing high retest reliability. HSI at E demonstrated significantly lower StO2 and NPI as well as higher TWI at the palm and fingertip in septic patients compared to healthy volunteers. StO2 and TWI showed corresponding results at the suprapatellar knee area. In septic patients, palm and fingertip THI identified survivors (E-t4) and revealed predictivity for 28-day mortality (E). Fingertip StO2 and THI correlated to SOFA-score on day 2. TWI was consistently increased in relation to the TWI range of healthy controls during the observation time. Palm TWI correlated positively with SOFA scores on day 3. DISCUSSION: HSI results in septic patients point to a distinctive microcirculatory pattern indicative of reduced skin oxygenation and perfusion quality combined with increased blood pooling and tissue water content. THI might possess risk-stratification properties and TWI could allow tissue edema evaluation in critically ill patients. CONCLUSION: HSI technologies could open new perspectives in microcirculatory monitoring by visualizing oxygenation and perfusion quality combined with tissue water content in critically ill patients - a prerequisite for future tissue perfusion guided therapy concepts in intensive care medicine.
Subject(s)
Hyperspectral Imaging , Microcirculation , Perfusion Imaging , Point-of-Care Testing , Sepsis/diagnostic imaging , Skin/blood supply , Spectroscopy, Near-Infrared , Adult , Aged , Aged, 80 and over , Biomarkers/metabolism , Body Water/metabolism , Case-Control Studies , Critical Illness , Female , Hemoglobins/metabolism , Humans , Hyperspectral Imaging/instrumentation , Male , Middle Aged , Organ Dysfunction Scores , Oxygen/metabolism , Perfusion Imaging/instrumentation , Pilot Projects , Point-of-Care Systems , Predictive Value of Tests , Prospective Studies , Regional Blood Flow , Sepsis/metabolism , Sepsis/physiopathology , Skin/metabolism , Spectroscopy, Near-Infrared/instrumentation , Time FactorsABSTRACT
Intravascular fluid administration belongs to the cornerstones of perioperative treatment with a substantial impact on surgical outcome especially with respect to major abdominal surgery. By avoidance of hypovolemia and hypervolemia, adequate perioperative fluid management significantly contributes to the reduction of insufficient tissue perfusion as a determinant of postoperative morbidity and mortality. The effective use of intravascular fluids requires detailed knowledge of the substances as well as measures to guide fluid therapy. Fluid management already starts preoperatively and should be continued in the postoperative setting (recovery room, peripheral ward) considering a patient-adjusted and surgery-adjusted hemodynamic monitoring. Communication between all team members participating in perioperative care is essential to optimize fluid management.
Subject(s)
Fluid Therapy , Hemodynamic Monitoring , Abdomen/surgery , Humans , Hypovolemia/prevention & control , Perioperative CareABSTRACT
Terahertz-frequency optical pulses can resonantly drive selected vibrational modes in solids and deform their crystal structures. In complex oxides, this method has been used to melt electronic order, drive insulator-to-metal transitions and induce superconductivity. Strikingly, coherent interlayer transport strongly reminiscent of superconductivity can be transiently induced up to room temperature (300 kelvin) in YBa2Cu3O6+x (refs 9, 10). Here we report the crystal structure of this exotic non-equilibrium state, determined by femtosecond X-ray diffraction and ab initio density functional theory calculations. We find that nonlinear lattice excitation in normal-state YBa2Cu3O6+x at above the transition temperature of 52 kelvin causes a simultaneous increase and decrease in the Cu-O2 intra-bilayer and, respectively, inter-bilayer distances, accompanied by anisotropic changes in the in-plane O-Cu-O bond buckling. Density functional theory calculations indicate that these motions cause drastic changes in the electronic structure. Among these, the enhancement in the character of the in-plane electronic structure is likely to favour superconductivity.
ABSTRACT
Measuring how the magnetic correlations evolve in doped Mott insulators has greatly improved our understanding of the pseudogap, non-Fermi liquids and high-temperature superconductivity. Recently, photo-excitation has been used to induce similarly exotic states transiently. However, the lack of available probes of magnetic correlations in the time domain hinders our understanding of these photo-induced states and how they could be controlled. Here, we implement magnetic resonant inelastic X-ray scattering at a free-electron laser to directly determine the magnetic dynamics after photo-doping the Mott insulator Sr2IrO4. We find that the non-equilibrium state, 2 ps after the excitation, exhibits strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. These two-dimensional (2D) in-plane Néel correlations recover within a few picoseconds, whereas the three-dimensional (3D) long-range magnetic order restores on a fluence-dependent timescale of a few hundred picoseconds. The marked difference in these two timescales implies that the dimensionality of magnetic correlations is vital for our understanding of ultrafast magnetic dynamics.
Subject(s)
Iridium/chemistry , Magnetic Fields , Molecular Dynamics Simulation , Strontium/chemistry , SuperconductivityABSTRACT
We report on the generation of high-energy (1.9 µJ) far-infrared pulses tunable between 4 and 18 THz frequency. Emphasis is placed on tunability and on minimizing the bandwidth of these pulses to less than 1 THz, as achieved by difference-frequency mixing of two linearly chirped near-infrared pulses in the organic nonlinear crystal DSTMS. As the two near-infrared pulses are derived from amplification of the same white light continuum, their carrier envelope phase fluctuations are mutually correlated, and hence the difference-frequency THz field exhibits absolute phase stability. This source opens up new possibilities for the control of condensed matter and chemical systems by selective excitation of low-energy modes in a frequency range that has, to date, been difficult to access.
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We report on the generation of narrowband carrier-envelope phase stable mid-infrared (MIR) pulses between 10 and 15 µm. High pulse energies and narrow bandwidths are required for the selective nonlinear excitation of collective modes of matter that is not possible with current sources. We demonstrate bandwidths of <2% at 12.5 µm wavelength through difference frequency generation between two near-infrared (NIR) pulses, which are linearly chirped. We obtain a reduction in bandwidth by one order of magnitude, compared to schemes that make use of transform-limited NIR pulses. The wavelength of the narrowband MIR pulse can be tuned by changing the optical delay between the two chirped NIR pulses.
ABSTRACT
We report on the demonstration of ultrafast optical reversal of the ferroelectric polarization in LiNbO_{3}. Rather than driving the ferroelectric mode directly, we couple to it indirectly by resonant excitation of an auxiliary high-frequency phonon mode with femtosecond midinfrared pulses. Because of strong anharmonic coupling between these modes, the atoms are directionally displaced along the ferroelectric mode and the polarization is transiently reversed, as revealed by time-resolved, phase-sensitive, second-harmonic generation. This reversal can be induced in both directions, a key prerequisite for practical applications.
ABSTRACT
We employ time-resolved resonant x-ray diffraction to study the melting of charge order and the associated insulator-to-metal transition in the doped manganite Pr_{0.5}Ca_{0.5}MnO_{3} after resonant excitation of a high-frequency infrared-active lattice mode. We find that the charge order reduces promptly and highly nonlinearly as function of excitation fluence. Density-functional theory calculations suggest that direct anharmonic coupling between the excited lattice mode and the electronic structure drives these dynamics, highlighting a new avenue of nonlinear phonon control.
ABSTRACT
We study the response of the one-dimensional charge density wave in K_{0.3}MoO_{3} to different types of excitation with femtosecond optical pulses. We compare direct excitation of the lattice at midinfrared frequencies with injection of quasiparticles across the low energy charge density wave gap and with charge transfer excitation in the near infrared. For all three cases, we observe a fluence threshold above which the amplitude-mode oscillation frequency is softened and the mode becomes increasingly damped. We show that all the data can be collapsed onto a universal curve in which the melting of the charge density wave occurs abruptly at a critical lattice excursion. These data highlight the existence of a universal stability limit for a charge density wave, reminiscent of the Lindemann criterion for the melting of a crystal lattice.
ABSTRACT
Selective optical excitation of a substrate lattice can drive phase changes across heterointerfaces. This phenomenon is a nonequilibrium analogue of static strain control in heterostructures and may lead to new applications in optically controlled phase change devices. Here, we make use of time-resolved nonresonant and resonant x-ray diffraction to clarify the underlying physics and to separate different microscopic degrees of freedom in space and time. We measure the dynamics of the lattice and that of the charge disproportionation in NdNiO_{3}, when an insulator-metal transition is driven by coherent lattice distortions in the LaAlO_{3} substrate. We find that charge redistribution propagates at supersonic speeds from the interface into the NdNiO_{3} film, followed by a sonic lattice wave. When combined with measurements of magnetic disordering and of the metal-insulator transition, these results establish a hierarchy of events for ultrafast control at complex-oxide heterointerfaces.
ABSTRACT
Static strain in complex oxide heterostructures has been extensively used to engineer electronic and magnetic properties at equilibrium. In the same spirit, deformations of the crystal lattice with light may be used to achieve functional control across heterointerfaces dynamically. Here, by exciting large-amplitude infrared-active vibrations in a LaAlO3 substrate we induce magnetic order melting in a NdNiO3 film across a heterointerface. Femtosecond resonant soft X-ray diffraction is used to determine the spatiotemporal evolution of the magnetic disordering. We observe a magnetic melt front that propagates from the substrate interface into the film, at a speed that suggests electronically driven motion. Light control and ultrafast phase front propagation at heterointerfaces may lead to new opportunities in optomagnetism, for example by driving domain wall motion to transport information across suitably designed devices.
ABSTRACT
CONSPECTUS: Driving phase changes by selective optical excitation of specific vibrational modes in molecular and condensed phase systems has long been a grand goal for laser science. However, phase control has to date primarily been achieved by using coherent light fields generated by femtosecond pulsed lasers at near-infrared or visible wavelengths. This field is now being advanced by progress in generating intense femtosecond pulses in the mid-infrared, which can be tuned into resonance with infrared-active crystal lattice modes of a solid. Selective vibrational excitation is particularly interesting in complex oxides with strong electronic correlations, where even subtle modulations of the crystallographic structure can lead to colossal changes of the electronic and magnetic properties. In this Account, we summarize recent efforts to control the collective phase state in solids through mode-selective lattice excitation. The key aspect of the underlying physics is the nonlinear coupling of the resonantly driven phonon to other (Raman-active) modes due to lattice anharmonicities, theoretically discussed as ionic Raman scattering in the 1970s. Such nonlinear phononic excitation leads to rectification of a directly excited infrared-active mode and to a net displacement of the crystal along the coordinate of all anharmonically coupled modes. We present the theoretical basis and the experimental demonstration of this phenomenon, using femtosecond optical spectroscopy and ultrafast X-ray diffraction at a free electron laser. The observed nonlinear lattice dynamics is shown to drive electronic and magnetic phase transitions in many complex oxides, including insulator-metal transitions, charge/orbital order melting and magnetic switching in manganites. Furthermore, we show that the selective vibrational excitation can drive high-TC cuprates into a transient structure with enhanced superconductivity. The combination of nonlinear phononics with ultrafast crystallography at X-ray free electron lasers may provide new design rules for the development of materials that exhibit these exotic behaviors also at equilibrium.
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We use midinfrared pulses with stable carrier-envelope phase offset to drive molecular vibrations in the charge transfer salt ET-F_{2}TCNQ, a prototypical one-dimensional Mott insulator. We find that the Mott gap, which is probed resonantly with 10 fs laser pulses, oscillates with the pump field. This observation reveals that molecular excitations can coherently perturb the electronic on-site interactions (Hubbard U) by changing the local orbital wave function. The gap oscillates at twice the frequency of the vibrational mode, indicating that the molecular distortions couple quadratically to the local charge density.
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We report femtosecond resonant soft x-ray diffraction measurements of the dynamics of the charge order and of the crystal lattice in nonsuperconducting, stripe-ordered La1.875Ba0.125CuO4. Excitation of the in-plane Cu-O stretching phonon with a midinfrared pulse has been previously shown to induce a transient superconducting state in the closely related compound La1.675Eu0.2Sr0.125CuO4. In La1.875Ba0.125CuO4, we find that the charge stripe order melts promptly on a subpicosecond time scale. Surprisingly, the low temperature tetragonal (LTT) distortion is only weakly reduced, reacting on significantly longer time scales that do not correlate with light-induced superconductivity. This experiment suggests that charge modulations alone, and not the LTT distortion, prevent superconductivity in equilibrium.
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We investigate the order parameter dynamics of the stripe-ordered nickelate, La(1.75)Sr(0.25)NiO(4), using time-resolved resonant x-ray diffraction. In spite of distinct spin and charge energy scales, the two order parameters' amplitude dynamics are found to be linked together due to strong coupling. Additionally, the vector nature of the spin sector introduces a longer reorientation time scale which is absent in the charge sector. These findings demonstrate that the correlation linking the symmetry-broken states does not unbind during the nonequilibrium process, and the time scales are not necessarily associated with the characteristic energy scales of individual degrees of freedom.
ABSTRACT
BACKGROUND AND RESEARCH QUESTION: In case of events such as a cyber attack or a mass casualty incident, ad hoc measures have to be taken in hospitals. As part of the critical infrastructure, hospitals are required by law to prepare, update and exercise alarm and emergency plans for various special situations. The processes and instruments involved for emergency response are defined in the hospital alert and emergency planning. The present study aims to explain with which resources and for which special situations hospitals are prepared. METHODS: A prospective, exploratory, anonymous survey of hospitals in Germany was conducted. Hospitals with both internal medicine and surgery departments were included. Out of 2497 hospitals listed in the German Hospital Directory ( www.deutsches-krankenhaus-verzeichnis.de ), 1049 met the inclusion criteria. After correcting for hospital groups with shared administrations, 850 employees were identified and contacted by email. Quality and risk management managers were asked about resources, risks, and content of their own hospital alert and emergency planning using a standardized questionnaire. The survey was conducted using the online platform EFS Survey (Tivian XI GmbH, Cologne) via www.unipark.de . Access to the survey was via a nonpersonalized hyperlink. Apart from the size and type of hospital surveyed, no data were collected that would allow identification of an individual person. RESULTS: Of the participating hospitals 45% (nâ¯= 43) were primary care hospitals, 24% (nâ¯= 23) were specialty care hospitals, 10% (nâ¯= 9) were nonuniversity maximum care hospitals, and 21% (nâ¯= 20) were university maximum care hospitals. In total 95 hospitals participated in the survey, of which 98% (nâ¯= 93) reported having a hospital alert and emergency plan. Preparation for individual scenarios varied widely. Of the participating hospitals 45% (nâ¯= 43) reported having been the target of cyber attacks with an emphasis on maximum care hospitals (55%, nâ¯= 11 of 20). Technical redundancy for computer systems is available in 67% (nâ¯= 63) of participating hospitals, while independent means of communication exist in 50% (nâ¯= 47) of hospitals. A physician-staffed crisis and disaster management unit existed in 60% (nâ¯= 56) of the surveyed hospitals. At least a part time position for planning issues was installed in 12 hospitals. CONCLUSION: Most participating hospitals are aware of the need for a hospital alert and emergency plan and have various scenario-specific plans in place. Especially mass casualty events, fire and hospital evacuation scenarios are uniformly covered among participating hospitals; however, gaps appear to exist not only for chemical, biological or radionuclear situations but also especially in the area of extreme weather events and infrastructure failures. Only about two thirds of all participating hospitals have contingency plans for water supply and/or heating failures. An important limitation of the study is the comparatively low response rate of 12.9% (nâ¯= 95 of 850). While primary care hospitals were underrepresented in the study, 32% of Germany's larger hospitals (>â¯800 beds) participated. In the future, there is a particular need to engage enough medical staff in the area of hospital alert and emergency planning and refunding of these measures by hospitals.
Subject(s)
Disaster Planning , Mass Casualty Incidents , Humans , Emergency Service, Hospital , Prospective Studies , Surveys and Questionnaires , Hospitals, University , Safety ManagementABSTRACT
We report on ultrafast optical experiments in which femtosecond midinfrared radiation is used to excite the lattice of complex oxide heterostructures. By tuning the excitation energy to a vibrational mode of the substrate, a long-lived five-order-of-magnitude increase of the electrical conductivity of NdNiO(3) epitaxial thin films is observed as a structural distortion propagates across the interface. Vibrational excitation, extended here to a wide class of heterostructures and interfaces, may be conducive to new strategies for electronic phase control at THz repetition rates.