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This study revisits the electroabsorption (EA) spectrum of polyacetylene, as functions of the electric field strength, isomerization degree, and light polarization states. The EA spectrum of $cis$-$(CH)_x$ reveals an oscillatory feature that follows the Stark shift-related first derivative of the materials absorption spectrum that contains v(0-1) and v(0-2) sidebands of the excited $C=C$ stretching vibration that agrees well with the Raman spectrum. EA spectrum of $trans $-$(CH)_x$ does not match the first derivative of the materials absorption spectrum, and the phonon sideband frequency does not agree with the RS spectrum. EA spectrum of $trans $-$(CH)_x$ reveals a band below the first allowed $1B_u$ exciton. We interpret this feature as due to the electric field activated even-parity dark (forbidden) exciton, namely $mA_g$ ($m >1$), showing that the nonluminescent $trans $-$(CH)_x$ is due to the reverse order of the excited states, where a dark $mA_g$ exciton lies below the allowed $1B_u$ exciton. This agrees with the unusual phonon sideband in $trans $-$(CH)_x$ absorption, since the excited state attenuation caused by the fast internal conversion from $1B_u$ to $mA_g$ influences the apparent frequency that determines the phonon sideband. Consequently, from the EA and RS spectra we estimate the $1B_u$ lifetime in $trans $-$(CH)_x$ to be $\sim 30$ fs. Integrated EA spectrum of $trans $-$(CH)_x$ shows a traditional Huang-Rhys type series with a relaxation parameter, $S \sim 0.5$. This indicates that the EA spectrum of the $trans $ isomer is also determined by a Stark shift related to the first derivative of the absorption spectrum, but preferentially for the longest chains in the films chain lengths distribution. This is due to the $N^3$ response of the non-linear susceptibility, $\chi^{(3)}$ ($\sim$EA), dependence on the chain length having $N$ monomers.

Spin accumulation in semiconductor structures at room temperature and without magnetic fields is key to enable a broader range of opto-electronic functionality. Current efforts are limited due to inherent inefficiencies associated with spin injection into semiconductor structures. Here, we demonstrate spin injection across chiral halide perovskite/III-V interfaces achieving spin accumulation in a standard semiconductor III-V (AlxGa1-x)0.5In0.5P multiple quantum well (MQW) light emitting diode (LED). The spin accumulation in the MQW is detected via emission of circularly polarized light with a degree of polarization of up to ~15%. The chiral perovskite/III-V interface was characterized with X-ray photoemission spectroscopy (XPS), cross sectional scanning Kelvin probe force microscopy, and cross section transmission electron microscopy (TEM) imaging, showing a clean semiconductor/semiconductor interface where the fermi-level can equilibrate. These findings demonstrate chiral perovskite semiconductors can transform well-developed semiconductor platforms to ones that can also control spin.

In their Comment, Kimling and Kuschel (hereafter the commenters) challenge our original interpretation of the magneto-optical Kerr effect (MOKE) measurements using ultrasensitive Sagnac interferometer, claiming that the transverse spin-Seebeck effect (TSSE) is not the only contribution to the measured change in the Kerr rotation angle from a Ni80Fe20 (NiFe) ferromagnetic (FM) slab subjected to a lateral temperature gradient in the presence of a magnetic field. The authors assert that: (1) the TSSE, in general, has not been completely proven so far, and that the existing theories, in particular the phonon magnon drag model that we have used in our publication, in fact cannot explain the original work of Uchida et al. (2) The commenters based their critique on an estimate of the magnitude of the measured effect, arguing that to observe the TSSE that we originally claimed, the temperature gradient in our measurements should have been much larger than the value we measured. In this Reply, firstly, we summarize previous literature reports on the TSSE response in FM metallic systems. Secondly, we dispute the estimate of the necessary large temperature gradient made by the commenters. Importantly, the Kerr effect sensitivity to spin accumulation (via the TSSE response) has not been recognized by the commenters, in fact it was mistakenly assumed that the Kerr effect sensitivity to the spin accumulation by the TSSE is the same as the Kerr sensitivity to the bulk magnetization change due to the temperature change. In conclusion, we show that the TSSE is the only viable interpretation of our original measurements, and that the phonon-magnon drag model is indeed capable of explaining our results.

Three dimensional (3D) topological insulators (TIs) are an important class of materials with applications in electronics, spintronics and quantum computing. With the recent development of truly bulk insulating 3D TIs, it has become possible to realize surface dominated phenomena in electrical transport measurements e.g. the quantum Hall (QH) effect of massless Dirac fermions in topological surface states (TSS). However, to realize more advanced devices and phenomena, there is a need for a platform to tune the TSS or modify them e.g. gap them by proximity with magnetic insulators, in a clean manner. Here we introduce van der Waals (vdW) heterostructures in the form of topological insulator/insulator/graphite to effectively control chemical potential of the TSS. Two types of gate dielectrics, normal insulator hexagonal boron nitride (hBN) and ferromagnetic insulator Cr2Ge2Te6 (CGT) are utilized to tune charge density of TSS in the quaternary TI BiSbTeSe2. hBN/graphite gating in the QH regime shows improved quantization of TSS by suppression of magnetoconductivity of massless Dirac fermions. CGT/graphite gating of massive Dirac fermions in the QH regime yields half-quantized Hall conductance steps and a measure of the Dirac gap. Our work shows the promise of the vdW platform in creating advanced high-quality TI-based devices., Comment: 19 pages, 4 figures

Organic semiconductors find increasing importance in spin transport devices due to the modulation and control of their properties through chemical synthetic versatility. The organic materials are used as interlayers between two ferromagnet (FM) electrodes in organic spin valves (OSV), as well as for magnetic spin manipulation of metal-organic complexes at the molecular level. In the latter, specifically, the substrate-induced magnetic switching in a paramagnetic molecule has been evoked extensively, but studied by delicate surface spectroscopies. Here we present evidence of the substantial magnetic switching in a nanosized thin film of the paramagnetic molecule, tris(8-hydroxyquinoline)iron(III) (Feq3) deposited on a FM substrate, using the magnetoresistance response of electrical spin-injection in an OSV structure, and the inverse-spin-Hall effect induced by state-of-art pulsed microwave spin-pumping. We show that interfacial spin control at the molecular level may lead to a macroscopic organic spin transport device, thus, bridging the gap between organic spintronics and molecular spintronics.

The family of organometal trihalide perovskite (OTP), CH3NH3PbX3 (where X is halogen) has recently revolutionized the photovoltaics field and shows promise in a variety of optoelectronic applications. The characteristic spin properties of charge and neutral excitations in OTPs are influenced by the large spin-orbit coupling of the Pb atoms, which may lead to spin-based device applications. Here we report the first studies of pure spin-current and spin-aligned carrier injection in OTP spintronics devices using spin-pumping and spin-injection, respectively. We measure a relatively large inverse-spin-Hall effect using pulsed microwave excitation in OTP devices at resonance with a ferromagnetic substrate, from which we derive room temperature spin diffusion length, lambda_sd~9nm; and low-temperature giant magnetoresistance in OTP-based spin-valves from which we estimate lambda_sd~85nm.

Exploration of spin-currents in organic semiconductors (OSECs) induced by resonant microwave absorption in ferromagnetic substrates has been of great interest for potential spintronics applications. Due to the inherently weak spin-orbit coupling (SOC) of OSECs, their inverse spin Hall effect (ISHE) response is very subtle; limited by the microwave power applicable under continuous-wave (cw) excitation. Here we introduce a novel approach for generating significant ISHE signals using pulsed ferromagnetic resonance, where the ISHE is ~2-3 orders of magnitude larger compared to cw excitation. This strong ISHE enables us to investigate a variety of OSECs ranging from pi-conjugated polymers with strong SOC that contain intrachain platinum atoms, to weak SOC polymers, to C60 films, where the SOC is predominantly caused by the molecule surface curvature. The pulsed-ISHE technique offers a robust route for efficient injection and detection schemes of spin-currents at room temperature, and paves the way for spin-orbitronics in plastic materials.

The saga of the primary photoexcitations in $\pi$-conjugated polymers has been a source of extraordinary scientific curiosity that has lasted for more than three decades. From soliton excitations in trans-polyacetylene, to singlet and triplet excitons and polarons in other polymers, to charge transfer excitons in blends of polymers and fullerenes, the field has been rich with a variety of different photoexcitation species. Here we show the photogeneration of a novel primary intrachain photoexcitation species, namely the composite multi-exciton (CME) in $\pi$-conjugated donor-acceptor (DA)-copolymers used in organic photovoltaic (OPV) solar cells. We utilized the magnetic field response of the transient photoinduced absorption from sub-picosecond to millisecond to show in pristine DA-copolymer early photogeneration of the CME species that is composed of four coupled spin 1/2 particles, having unique optical and magnetic signatures. This species decomposes into two independent triplets in the microsecond time domain. Importantly in copolymer/fullerene blends the CME ionization generates photocarriers by a unique process that may enhance the photocurrent in OPV solar cells., Comment: 25 pages, 6 figures + Supplementary Information

Using first-principles calculations, we have systematically investigated the structural, electronic, and magnetic properties of facial (fac-) and meridional (mer-) tris(8-hydroxyquinoline)iron(III) (Feq3) molecules and their interaction with ferromagnetic substrate. Our calculation results show that for the isolated Feq3, mer-Feq3 is more stable than the fac-Feq3; and both Feq3 isomers have a high spin-state of 5 {\mu}B as the ground state when an on-site Hubbard-U term is included to treat the highly localized Fe 3d electrons; while the standard DFT calculations produce a low spin-state of 1 {\mu}B. These magnetic behaviors can be understood by the octahedral ligand field splitting theory. Furthermore, we found that fac-Feq3 has a stronger bonding to the Co surface than mer-Feq3 and an anti-ferromagnetic coupling was discovered between Fe and Co substrate, originating from the superexchange coupling between Fe and Co mediated by the interface oxygen and nitrogen atoms. These findings suggest that Feq3 molecular films may serve as a promising spin-filter material in spintronic devices.

Recently, much effort has been devoted to improve the efficiency of organic photovoltaic solar cells based on blends of donors and acceptors molecules in bulk heterojunction architecture. One of the major losses in organic photovoltaic devices has been recombination of polaron pairs at the donor/acceptor domain interfaces. Here, we present a novel method to suppress polaron pair recombination at the donor/acceptor domain interfaces and thus improve the organic photovoltaic solar cell efficiency, by doping the device active layer with spin 1/2 radical galvinoxyl. At an optimal doping level of 3 wt%, the efficiency of a standard poly(3-hexylthiophene)/1-(3-(methoxycarbonyl)propyl)-1-1-phenyl)(6,6)C61 solar cell improves by 18%. A spin-flip mechanism is proposed and supported by magneto-photocurrent measurements, as well as by density functional theory calculations in which polaron pair recombination rate is suppressed by resonant exchange interaction between the spin 1/2 radicals and charged acceptors, which convert the polaron pair spin state from singlet to triplet., Comment: 10 pages, 4 figures