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Ultrafast optical control over nanoscale charge currents is increasingly important for emerging integrated optoelectronics and other applications. Here, we introduce versatile new hybrid nanoplasmonic-graphene sources of tailored picosecond photocurrents and demonstrate bias-free, continuously-polarization-rotatable terahertz emission.

We used femtosecond optical spectroscopy to study ultrafast spin and orbital ordering dynamics in the antiferromagnetic Mott insulator α-Sr2CrO4. This chromate system possesses multiple spin and orbital ordered phases, and therefore could enable us to study the unique interplay between these collective phases through their non-equilibrium response to photoexcitation. Here, by varying the pump photon energy, we selectively drove inter-site spin hopping between neighboring Cr t2g orbitals and charge transfer-type transitions between oxygen 2p and Cr eg orbitals. The resulting transient reflectivity dynamics revealed temperature-dependent anomalies across the Neel temperature for spin ordering as well as the transition temperatures linked to different types of orbital order. Our results reveal distinct relaxation timescales for spin and orbital orders in α-Sr2CrO4 and provide experimental evidence for the phase transition at TO, possibly related to antiferro-type orbital ordering.

We investigate the static and ultrafast magneto-optical response of the hexagonal chiral helimagnet $Cr_{1/3}NbS_{2}$ above and below the helimagnetic ordering temperature. The presence of a magnetic easy plane contained within the crystallographic ab-plane is confirmed, while degenerate optical pump-probe experiments reveal significant differences in the dynamic between the parent, $NbS_{2}$, and Cr-intercalated compounds. Time resolved magneto-optical Kerr effect measurements show a two-step demagnetization process, where an initial, sub-ps relaxation and subsequent buildup ($\tau > 50$ ps) in the demagnetization dynamic scale similarly with increasing pump fluence. Despite theoretical evidence for partial gapping of the minority spin channel, suggestive of possible half metallicity in $Cr_{1/3}NbS_{2}$, such a long demagnetization dynamic likely results from spin lattice-relaxation as opposed to minority state blocking. However, comparison of the two-step demagnetization process in $Cr_{1/3}NbS_{2}$ with other 3d intercalated transition metal dichalcogenides reveals a behavior that is unexpected from conventional spin-lattice relaxation, and may be attributed to the complicated interaction of local moments with itinerant electrons in this material system.

We demonstrate perturbative optical harmonic generation up to fifth order in the topological chiral crystal RhSi under femtosecond mid-infrared excitation, with particularly strong third harmonic responses that may be linked to Berry curvature contributions.

Controlling the photoexcited properties and behavior of hybrid perovskites by halide doping has the potential to impact a wide range of emerging technologies, including solar cells and radiation detectors. Crystalline samples of methylammonium lead bromide substituted with chlorine (MAPbBr

X-ray ptychography is a rapidly developing coherent diffraction imaging technique that provides nanoscale resolution on extended field-of-view. However, the requirement of coherence and the scanning mechanism limit the throughput of ptychographic imaging. In this paper, we propose X-ray ptychography using multiple illuminations instead of single illumination in conventional ptychography. Multiple locations of the sample are simultaneously imaged by spatially separated X-ray beams, therefore, the obtained field-of-view in one scan can be enlarged by a factor equal to the number of illuminations. We have demonstrated this technique experimentally using two X-ray beams focused by a house-made Fresnel zone plate array. Two areas of the object and corresponding double illuminations were successfully reconstructed from diffraction patterns acquired in one scan, with image quality similar with those obtained by conventional single-beam ptychography in sequence. Multi-beam ptychography approach increases the imaging speed, providing an efficient way for high-resolution imaging of large extended specimens.

Symmetry plays a central role in conventional and topological phases of matter, making the ability to optically drive symmetry change a critical step in developing future technologies that rely on such control. Topological materials, like the newly discovered topological semimetals, are particularly sensitive to a breaking or restoring of time-reversal and crystalline symmetries, which affect both bulk and surface electronic states. While previous studies have focused on controlling symmetry via coupling to the crystal lattice, we demonstrate here an all-electronic mechanism based on photocurrent generation. Using second-harmonic generation spectroscopy as a sensitive probe of symmetry change, we observe an ultrafast breaking of time-reversal and spatial symmetries following femtosecond optical excitation in the prototypical type-I Weyl semimetal TaAs. Our results show that optically driven photocurrents can be tailored to explicitly break electronic symmetry in a generic fashion, opening up the possibility of driving phase transitions between symmetry-protected states on ultrafast time scales., 28 pages, 15 figures, 4 Tables

Weyl semimetals have been the focus of intense experimental and theoretical investigation, due to their broad appeal in fundamental science and applied technology alike. More recently, several studies have centered on the nonlinear optical properties of these materials, where it is believed that characteristic features of Weyl physics can be observed. To date, these studies have been limited to static or quasi-static measurements, but new and important insights can come about through extending these nonlinear optical spectroscopies into the time domain. To do so, we use terahertz (THz) emission spectroscopy and time-resolved second harmonic generation (TR-SHG) spectroscopy to provide a contact free measure of ultrafast photocurrent dynamics in the transition metal monopnictide family of type-I Weyl semimetals. On the basis of our data, we are able to clearly distinguish between helicity-dependent photocurrents generated within the ab-plane and polarization-independent photocurrents flowing along the non-centrosymmetric c-axis. Such findings are consistent with earlier static photocurrent experiments, and demonstrate on the basis of both the physical constraints imposed by symmetry and the temporal dynamics intrinsic to current generation and decay that optically induced photocurrents in TaAs are inherent to the underlying crystal symmetry. Such generality in the microscopic origin of photocurrent generation in the transition metal monopnictide family of Weyl semimetals makes these materials promising candidates as next generation sources or detectors in the mid-IR and THz frequency ranges.

A light-induced topological phase transition is realized in the Dirac semimetal ZrTe5 by coherently driving symmetry-breaking phonons.

We utilized ultrafast X-ray diffraction to investigate optically induced strain waves in the Weyl semimetal TaAs, revealing real-time structural oscillations originating from quasilongitudinal and quasi-shear acoustic phonon modes.

The chiral helimagnet Cr1/3NbS2 hosts exotic spin textures, whose influence on the magneto-transport properties make this material an ideal candidate for future spintronic applications. To date, the interplay between macroscopic magnetic and transport degrees of freedom is believed to result from a reduction in carrier scattering following spin order. Here, we present electronic structure measurements across the helimagnetic transition temperature TC that challenges this view. We show that the Fermi surface is comprised of strongly hybridized Nb- and Cr-derived electronic states, and that spectral weight close to the Fermi level increases anomalously as the temperature is lowered below TC. These findings are rationalized on the basis of first principle density functional theory calculations, which reveal a large nearest-neighbor exchange energy, suggesting the interaction between local spin moments and hybridized Nb- and Cr-derived itinerant states to go beyond the perturbative interaction of Ruderman-Kittel-Kasuya-Yosida, suggesting instead a mechanism rooted in a Hund’s exchange interaction.

We measure effect of strain on Auger recombination from compositional and applied biaxial stress using time-resolved photoluminescence and pump-probe spectroscopy. Results suggest that straining by composition, but not external stress, can tune the Auger coefficient.

Ultrashort terahertz (THz) pulses are a powerful tool for both probing and controlling novel phenomena in quantum materials. This is particularly useful in Dirac materials, since these materials exhibit novel magnetic and lattice excitations that can potentially be used to control their properties. Here, the use of ultrashort THz pulses to reveal the circular photogalvanic effect in the Weyl semimetal TaAs and probe magnetoplasmon modes in graphene nanoribbons will be examined. We performed THz emission spectroscopy on the (112) and (001) surfaces of the Weyl semimetal TaAs. Our data enables us to clearly distinguish between helicity-dependent photocurrents generated within the ab-plane and polarization-independent photocurrents flowing along the non-centrosymmetric c-axis. Such findings are in excellent agreement with previous static photocurrent measurements. However, by considering both the physical constraints imposed by symmetry and the temporal dynamics intrinsic to current generation and decay, we can attribute these transient photocurrents to the underlying crystal symmetry of these materials. We also used terahertz (THz) magneto-optical spectroscopy to demonstrate how a periodic array of graphene micro-ribbons can be used to control the transmission spectrum and polarization state of a THz pulse whose electric field is oriented along the pattern’s axis of periodicity (perpendicular to the long axis of the ribbons). Our results demonstrate that graphene micro-ribbon arrays are a powerful system for controlling the coupling between light and magnetoplasmonic modes. This enables the tailoring of THz transmission profiles and polarization states using applied magnetic fields.

We investigate polarization-dependent ultrafast photocurrents in the Weyl semimetal TaAs using terahertz (THz) emission spectroscopy. Our results reveal that highly directional, transient photocurrents are generated along the non-centrosymmetric c-axis regardless of incident light polarization, while helicity-dependent photocurrents are excited within the ab-plane. This is consistent with earlier static photocurrent experiments, and demonstrates on the basis of both the physical constraints imposed by symmetry and the temporal dynamics intrinsic to current generation and decay that optically induced photocurrents in TaAs are inherent to the underlying crystal symmetry of the transition metal monopnictide family of Weyl semimetals.

We investigate polarization-dependent ultrafast photocurrents in theWeyl semimetal TaAs using terahertz (THz) emission spectroscopy. Our results reveal that highly directional, transient photocurrents are generated along the non-centrosymmetric c-axis regardless of incident light polarization, while helicity-dependent photocurrents are excited within the ab-plane. Such findings are consistent with earlier static photocurrent experiments, and demonstrate on the basis of both the physical constraints imposed by symmetry and the temporal dynamics intrinsic to current generation and decay that optically induced photocurrents in TaAs are inherent to the underlying crystal symmetry. Such generality in the microscopic origin of photocurrent generation in the transition metal monopnictide family of Weyl semimetals makes these materials promising candidates as next generation sources or detectors in the mid-IR and terahertz frequency ranges.

We differentiate the effect of strain induced by lattice-mismatched growth from strain induced by mechanical deformation on cubic nonradiative Auger recombination in narrow-gap GaInAsSb/GaSb quantum well (QW) heterostructures. The typical reduction in the Auger coefficient observed with lattice-mismatched growth appears to be due to the concomitant compositional change rather than the addition of strain, with implications for mid-IR semiconductor laser design. We induced a range of internal compressive strain in five samples from −0.90% to −2.07% by varying the composition during the growth and mechanically induced a similar range of internal strain in analogous quantum well membrane samples. We performed time-resolved photoluminescence and differential reflectivity measurements to extract the carrier recombination dynamics, taken at 300 K with carrier densities from 2.7 × 10 18 cm−3 to 1.4 × 10 19 cm−3. We observed no change with strain in the cubic Auger coefficient of samples that were strained mechanically, but we did observe a trend with strain in samples that were strained by the QW alloy composition. Measured Auger coefficients ranged from 3.0 × 1 0 − 29 cm6 s−1 to 3.0 × 1 0 − 28 cm6 s−1.

The recent discovery of the soliton lattice, and the intriguing interplay between magnetic and transport degrees of freedom, make the chiral helimagnet Cr1/3NbS2 a very promising material both for technological applications, and for elucidating the connection between non-trivial spin textures and the microscopic interactions allowed in a crystalline lattice lacking in inversion symmetry. In this talk, we present recent results of photoemission and time-resolved optical spectroscopy on Cr1/3NbS2. Most notably, the data reveal that the Fermi surface is partially composed of Cr states, and that such states may give rise to a possible half metallicity as suggested by the characteristically long demagnetization dynamic measured from time-resolved magneto-optical Kerr effect (MOKE). Finally, it will be discussed how these findings are inconsistent with a description of magnetism and magnetotransport in this material based solely on spin ordering arguments.

We performed time-resolved second harmonic generation (SHG) spectroscopy on the Weyl semimetal TaAs. These measurements reveal a potential transient photoinduced state as well as an ultrafast dependence of the SHG signal on pump polarization.

Methyl ammonium lead bromide (MAPbBr3) crystals, possible replacements for silicon in many photonic applications, were probed with transient reflectivity spectroscopy, revealing faster carrier cooling dynamics and slower recombination dynamics with increased chlorine doping.