Roopali Kukreja

Solvent additives and their effects on blend morphologies of bulk heterojunctions

Controlling the blend morphology is one of the ways to achieve high power conversion efficiency in organic bulk heterojunction (BHJ) photovoltaic devices. One simple yet effective method is “solvent additive” approach, which involves the addition of a small fraction of high boiling point solvent into the blend of donor/acceptor dissolved in another host solvent. Even though this method has been successfully applied in a number of polymer/fullerene BHJ devices, the selection rule of the choice of additive and the host solvent has yet to be fully established. In this work, we performed a systematic study of the effect of alkyl lengths of alkanedithiol additives on the nanoscale phase separation of P3HT:PC61BM blends and consequently, the power conversion efficiency (PCE) of the devices. The extent of the additive-induced phase separation is related to the additive boiling point and the degree of interaction between the additive and fullerene, as evident from grazing incidence X-ray diffractometry (GIXRD) and scanning transmission X-ray microscopy (STXM) data. We found that both the boiling point and the degree of interaction are correlated and should be considered simultaneously in the selection of the appropriate solvent additives. Lastly, PCE as high as 3.1% can be achieved in an optimally phase-separated blend due to an improvement in the charge dissociation and a decrease in bimolecular recombination.

Speed limit of the insulator–metal transition in magnetite

As the oldest known magnetic material, magnetite (Fe3O4) has fascinated mankind for millennia. As the first oxide in which a relationship between electrical conductivity and fluctuating/localized electronic order was shown, magnetite represents a model system for understanding correlated oxides in general. Nevertheless, the exact mechanism of the insulator-metal, or Verwey, transition has long remained inaccessible. Recently, three-Fe-site lattice distortions called trimerons were identified as the characteristic building blocks of the low-temperature insulating electronically ordered phase. Here we investigate the Verwey transition with pump-probe X-ray diffraction and optical reflectivity techniques, and show how trimerons become mobile across the insulator-metal transition. We find this to be a two-step process. After an initial 300 fs destruction of individual trimerons, phase separation occurs on a 1.5±0.2 ps timescale to yield residual insulating and metallic regions. This work establishes the speed limit for switching in future oxide electronics.

Direct observation and imaging of a spin-wave soliton with p−like symmetry

Spin waves, the collective excitations of spins, can emerge as nonlinear solitons at the nanoscale when excited by an electrical current from a nanocontact. These solitons are expected to have essentially cylindrical symmetry (that is, s-like), but no direct experimental observation exists to confirm this picture. Using a high-sensitivity time-resolved magnetic X-ray microscopy with 50 ps temporal resolution and 35 nm spatial resolution, we are able to create a real-space spin-wave movie and observe the emergence of a localized soliton with a nodal line, that is, with p-like symmetry. Micromagnetic simulations explain the measurements and reveal that the symmetry of the soliton can be controlled by magnetic fields. Our results broaden the understanding of spin-wave dynamics at the nanoscale, with implications for the design of magnetic nanodevices.

Photoinduced Enhancement of the Charge Density Wave Amplitude

Symmetry breaking and the emergence of order is one of the most fascinating phenomena in condensed matter physics. It leads to a plethora of intriguing ground states found in antiferromagnets, Mott insulators, superconductors, and density-wave systems. Exploiting states of matter far from equilibrium can provide even more striking routes to symmetry-lowered, ordered states. Here, we demonstrate for the case of elemental chromium that moderate ultrafast photoexcitation can transiently enhance the charge-density-wave (CDW) amplitude by up to 30% above its equilibrium value, while strong excitations lead to an oscillating, large-amplitude CDW state that persists above the equilibrium transition temperature. Both effects result from dynamic electron-phonon interactions, providing an efficient mechanism to selectively transform a broad excitation of the electronic order into a well-defined, long-lived coherent lattice vibration. This mechanism may be exploited to transiently enhance order parameters in other systems with coupled degrees of freedom.

Direct Observation of a Localized Magnetic Soliton in a Spin-Transfer Nanocontact.

We report the direct observation of a localized magnetic soliton in a spin-transfer nanocontact using scanning transmission x-ray microscopy. Experiments are conducted on a lithographically defined 150 nm diameter nanocontact to an ultrathin ferromagnetic multilayer with perpendicular magnetic anisotropy. Element-resolved x-ray magnetic circular dichroism images show an abrupt onset of a magnetic soliton excitation localized beneath the nanocontact at a threshold current. However, the amplitude of the excitation ≃25° at the contact center is far less than that predicted (⪅180°), showing that the spin dynamics is not described by existing models.

Generation mechanism of terahertz coherent acoustic phonons in Fe

T Henighan1,2,∗ M Trigo, S Bonetti, P Granitzka, D Higley, Z Chen, M P Jiang, R Kukreja, A Gray, A H Reid, E Jal, M C Hoffmann, M Kozina, S Song, M Chollet, D Zhu, P F Xu, J Jeong, K Carva, P Maldonado, P M Oppeneer, M G Samant, S S P. Parkin, D A Reis, and H A Dürr3† PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, California, USA Physics Department, Stanford University, Stanford, California, USA Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025. Van der Waals-Zeeman Institute, University of Amsterdam, 1018XE Amsterdam, The Netherlands Department of Photon Science and Applied Physics, Stanford University, Stanford, California, USA Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, California, USA IBM Almaden Research Center, 650 Harry Road, San Jose, California 95120, USA Max-Planck Institute for Microstructure Physics, 06120 Halle (Saale), Germany Charles University, Faculty of Mathematics and Physics, Department of Condensed Matter Physics, Ke Karlovu 5, CZ-12116 Prague 2, Czech Republic and Department of Physics and Astronomy, Uppsala University, P. O. Box 516, S-75120 Uppsala, Sweden (Dated: September 14, 2015)

X-ray Detection of Transient Magnetic Moments Induced by a Spin Current in Cu

We have used a MHz lock-in x-ray spectromicroscopy technique to directly detect changes in magnetic moment of Cu due to spin injection from an adjacent Co layer. The elemental and chemical specificity of x rays allows us to distinguish two spin current induced effects. We detect the creation of transient magnetic moments of 3×10^{-5}μ_{B} on Cu atoms within the bulk of the 28 nm thick Cu film due to spin accumulation. The moment value is compared to predictions by Motts two current model. We also observe that the hybridization induced existing magnetic moments at the Cu interface atoms are transiently increased by about 10% or 4×10^{-3}μ_{B} per atom. This reveals the dominance of spin-torque alignment over Joule heat induced disorder of the interfacial Cu moments during current flow.

Microwave soft x-ray microscopy for nanoscale magnetization dynamics in the 5–10 GHz frequency range

We present a scanning transmission x-ray microscopy setup combined with a novel microwave synchronization scheme for studying high frequency magnetization dynamics at synchrotron light sources. The sensitivity necessary to detect small changes in the magnetization on short time scales and nanometer spatial dimensions is achieved by combining the excitation mechanism with single photon counting electronics that is locked to the synchrotron operation frequency. Our instrument is capable of creating direct images of dynamical phenomena in the 5-10 GHz range, with high spatial resolution. When used together with circularly polarized x-rays, the above capabilities can be combined to study magnetic phenomena at microwave frequencies, such as ferromagnetic resonance (FMR) and spin waves. We demonstrate the capabilities of our technique by presenting phase resolved images of a ∼6 GHz nanoscale spin wave generated by a spin torque oscillator, as well as the uniform ferromagnetic precession with ∼0.1° amplitude at ∼9 GHz in a micrometer-sized cobalt strip.

Ultrafast reduction of the total magnetization in iron

Surprisingly, if a ferromagnet is exposed to an ultrafast laser pulse, its apparent magnetization is reduced within less than a picosecond. Up to now, the total magnetization, i.e., the average spin polarization of the whole valence band, was not detectable on a sub-picosecond time scale. Here, we present experimental data, confirming the ultrafast reduction of the total magnetization. Soft x-ray pulses from the free electron laser in Hamburg (FLASH) extract polarized cascade photoelectrons from an iron layer excited by a femtosecond laser pulse. The spin polarization of the emitted electrons is detected by a Mott spin polarimeter.

Phase separation in the nonequilibrium Verwey transition in magnetite

We present equilibrium and out-of-equilibrium studies of the Verwey transition in magnetite. In the equilibrium optical conductivity, we find a steplike change at the phase transition for photon energies below about 2 eV. The possibility of triggering a nonequilibrium transient metallic state in insulating magnetite by photo excitation was recently demonstrated by an x-ray study. Here we report a full characterization of the optical properties in the visible frequency range across the nonequilibrium phase transition. Our analysis of the spectral features is based on a detailed description of the equilibrium properties. The out-of-equilibrium optical data bear the initial electronic response associated to localized photoexcitation, the occurrence of phase separation, and the transition to a transient metallic phase for excitation density larger than a critical value. This allows us to identify the electronic nature of the transient state, to unveil the phase transition dynamics, and to study the consequences of phase separation on the reflectivity, suggesting a spectroscopic feature that may be generally linked to out-of-equilibrium phase separation.