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In contrast to regular J- and H-aggregates, thin film squaraine aggregates usually have broad absorption spectra containing both J-and H-like features, which are favorable for organic photovoltaics. Despite being successfully applied in organic photovoltaics for years, a clear interpretation of these optical properties by relating them to specific excited states and an underlying aggregate structure has not been made. In this work, by static and transient absorption spectroscopy on aggregated n-butyl anilino squaraines, we provide evidence that both the red- and blue-shifted peaks can be explained by assuming an ensemble of aggregates with intermolecular dipole-dipole resonance interactions and structural disorder deriving from the four different nearest neighbor alignments-in sharp contrast to previous association of the peaks with intermolecular charge-transfer interactions. In our model, the next-nearest neighbor dipole-dipole interactions may be negative or positive, which leads to the occurrence of J- and H-like features in the absorption spectrum. Upon femtosecond pulse excitation of the aggregated sample, a transient absorption spectrum deviating from the absorbance spectrum emerges. The deviation finds its origin in the excitation of two-exciton states by the probe pulse. The lifetime of the exciton is confirmed by the band integral dynamics, featuring a single-exponential decay with a lifetime of 205 ps. Our results disclose the aggregated structure and the origin of red- and blue-shifted peaks and explain the absence of photoluminescence in squaraine thin films. Our findings underline the important role of structural disorder of molecular aggregates for photovoltaic applications.

We present time-resolved magneto-optical spectroscopy on the magnetic Mott-Hubbard-insulating Kitaev spin liquid candidate α-RuCl

We present time-resolved magneto-optical spectroscopy on the magnetic Mott-Hubbard-insulating Kitaev spin liquid candidate $\alpha$-RuCl$_3$ to investigate the nonequilibrium dynamics of its antiferromagnetically ordered zigzag groundstate after photoexcitation. A systematic study of the transient magnetic linear dichroism under different experimental conditions (temperature, external magnetic field, photoexcitation density) gives direct access to the dynamical interplay of charge excitations with the zigzag ordered state on ultrashort time scales. We observe a rather slow initial demagnetization (few to 10s of ps) followed by a long-lived non-thermal antiferromagnetic spin-disordered state (100$-$1000s of ps), which can be understood in terms of holons and doublons disordering the antiferromagnetic background after photoexcitation. Varying temperature and fluence in the presence of an external magnetic field reveals two distinct photoinduced dynamics associated with the zigzag and quantum paramagnetic disordered phases. The photo-induced non-thermal spin-disordered state shows universal compressed-exponential recovery dynamics related to the growth and propagation of zigzag domains on nanosecond time scales, which is interpreted within the framework of the Fatuzzo-Labrune model for magnetization reversal. The study of nonequilibrium states in strongly correlated materials is a relatively unexplored topic, but our results are expected to be extendable to a large class of Mott-Hubbard insulator materials with strong spin-orbit coupling.

The intermolecular charge transfer (CT) exciton in merocyanine: [6,6]-phenyl-C61-butyric acid methyl ester (PC61BM) system, induced by the molecular geometry is investigated. The CT state, localize...

ACS omega 5(11), 5824-5833 (2020). doi:10.1021/acsomega.9b03996, Published by ACS Publications, Washington, DC

We investigated the structural and magnetic properties of bare SrRuO3 (SRO) ultrathin films and SrRuO3/SrIrO3/SrZrO3 (SRO/SIO/SZO: RIZ) trilayer heterostructures between 10 and 80 K, by comparing macroscopic data using the magneto-optical Kerr effect (MOKE) and magneto-transport (anomalous Hall effect: AHE), with nanoscale fingerprints when applying noncontact scanning force microscopy (nc-SFM) and magnetic force microscopy (MFM). SRO and RIZ ultrathin films were epitaxially grown at 650 °C onto vicinal SrTiO3 (100) single-crystalline substrates to a nominal thickness of 4 and 4/2/2 unit cells (uc), respectively. Our correlated analysis allows associating topographic sample features of overgrown individual layers to their residual magnetization, as is shown here to be relevant for interpreting the macroscopic AHE data. Although the hump-like features in the AHE suggest a magnetically textured skyrmion phase to exist around 55 K associated with the topological Hall effect (THE), both our MOKE and MFM data ...

A key element to tailor the properties of magnetic multilayers is the coupling between the individual magnetic layers. In case of skyrmion hosting multilayers, coupling of skyrmions across the magnetic layers is highly desirable. Here the magnetic interlayer coupling was studied in epitaxial all-oxide heterostructures of ferromagnetic perovskite SrRuO$_3$ layers separated by spacers of the strong spin-orbit coupling oxide SrIrO$_3$. This combination of oxide layers is being discussed as a potential candidate system to host N\'{e}el skyrmions. First order reversal curve (FORC) measurements were performed in order to distinguish between magnetic switching processes of the individual layers and to disentangle the signal of soft magnetic impurities from the samples$'$ signal. Additionally, FORC investigations enabled to determine whether the coupling between the magnetic layers is ferromagnetic or antiferromagnetic. The observed interlayer coupling strength was weak for all the heterostructures, with SrIrO$_3$ spacers between 2 monolayers and 12 monolayers thick., Comment: 22 pages

Organic-inorganic hybrid materials have shown a remarkable and rapid development during the past decade because they can be tailored to obtain new device concepts with controlled physical properties. Here, we report on the electronic and magnetic properties of multilayer organic-inorganic hybrid films. Electrical transport properties arising from the pi electrons in the organic layer are characteristic of a metallic state at high temperature and evolve into a state described by two-dimensional variable range hopping when temperature decreases below 150 K. The intrinsic electronic behavior of the hybrid films was further studied via the optical properties in the IR range. The optical response confirms the metallic character of the hybrid films. In the second part, the magnetic properties are discussed. A long-range ferromagnetic order with an ordering temperature of similar to 1 K is revealed in the Gd-based hybrid film. The Cu-based hybrid film, however, shows more extended ferromagnetic exchange interactions than the Gd-based hybrid LB film.

Formation of magnetic order alters the character of spin excitations, which then affects transport properties. We investigate the photoexcited ultrafast spin dynamics in different magnetic phases in Néel-type skyrmion host GaV

The quadratic electro-optic effect (Kerr effect) is shown to be efficiently induced by a terahertz (THz) electric field in the quasi-two-dimensional (2D) material MnPS3. The waveform of the THz-induced response practically follows the intensity of the employed nearly single-cycle THz pulse. While neither THz-induced absorption nor the linear electro-optical effect are observed, we demonstrate that the THz electric field induces the refraction coefficient anisotropy experienced by light at the wavelength of 800 nm. In our experiment, the anisotropy results in polarization rotation of the light and corresponds to a nonlinear refractive index of the sample of approximately 13.1 × 10−14 W−1 cm2. This promotes the quasi-2D MnPS3 as a promising candidate for practical application in future ultrafast electro-optical devices.

The proposal that very small N\'eel skyrmions can form in ${\mathrm{SrRuO}}_{3}/{\mathrm{SrIrO}}_{3}$ epitaxial bilayers and that the electric field effect can be used to manipulate these skyrmions in gated devices strongly stimulated the recent research of ${\mathrm{SrRuO}}_{3}$ heterostructures. A strong interfacial Dzyaloshinskii-Moriya interaction was considered as the driving force for the formation of skyrmions in ${\mathrm{SrRuO}}_{3}/{\mathrm{SrIrO}}_{3}$ bilayers. Here, we investigated nominally symmetric heterostructures in which an ultrathin ferromagnetic ${\mathrm{SrRuO}}_{3}$ layer is sandwiched between large spin-orbit coupling ${\mathrm{SrIrO}}_{3}$ layers, for which the conditions are not favorable for the emergence of a net interfacial Dzyaloshinskii-Moriya interaction. Previously the formation of skyrmions in the asymmetric ${\mathrm{SrRuO}}_{3}/{\mathrm{SrIrO}}_{3}$ bilayers was inferred from anomalous Hall resistance loops showing humplike features that resembled topological Hall effect contributions. Symmetric ${\mathrm{SrIrO}}_{3}/{\mathrm{SrRuO}}_{3}/{\mathrm{SrIrO}}_{3}$ trilayers do not show hump anomalies in the Hall loops. However, the anomalous Hall resistance loops of symmetric multilayers, in which the trilayer is stacked several times, do exhibit the humplike structures, similar to the asymmetric ${\mathrm{SrRuO}}_{3}/{\mathrm{SrIrO}}_{3}$ bilayers. The origin of the Hall effect loop anomalies likely resides in unavoidable differences in the electronic and magnetic properties of the individual ${\mathrm{SrRuO}}_{3}$ layers rather than in the formation of skyrmions.

Magnetic interlayer coupling is a key ingredient in designing magnetic multilayers with functionalities that reach out to the realm of applications. In epitaxial ferromagnetic (FM) oxide multilayers, the magnetic interlayer coupling is, however, less studied and its prediction is often a challenging task. Ultrathin FM ${\mathrm{SrRuO}}_{3}$ epitaxial films with perpendicular magnetic anisotropy, interfaced with suitable oxides, may be susceptible of forming skyrmions. Hence, a strong FM interlayer coupling would be beneficial to achieve uniform switching behavior of a ${\mathrm{SrRuO}}_{3}$-based multilayer. Previous studies reported that the coupling of two ${\mathrm{SrRuO}}_{3}$ layers separated by a non-FM oxide spacer is at best weakly FM and the two FM layers switch at markedly different fields. Here we study the magnetic interlayer coupling between two FM ${\mathrm{SrRuO}}_{3}$ layers separated by ultrathin ${\mathrm{LaNiO}}_{3}$ in epitaxial heterostructures grown on ${\mathrm{SrTiO}}_{3}$(100) single crystals. We found that FM ${\mathrm{SrRuO}}_{3}$ layers separated by 2 monolayers (MLs) thick ${\mathrm{LaNiO}}_{3}$ show weak FM interlayer coupling of about $106\phantom{\rule{0.16em}{0ex}}\ensuremath{\mu}\mathrm{J}/{m}^{2}$ at 10 K. The coupling becomes strongly FM for four MLs thick (about 1.6 nm) ${\mathrm{LaNiO}}_{3}$ spacers and the two ${\mathrm{SrRuO}}_{3}$ layers reverse their magnetization at a common value of the perpendicular magnetic field. This is likely due to a transition of the ${\mathrm{LaNiO}}_{3}$ spacer from insulating to metallic, as its thickness increases.

We report on time-resolved mid-infrared-pump terahertz-transmission-probe studies of the topological-insulator materials ${({\mathrm{Bi}}_{1\ensuremath{-}x}{\mathrm{Sb}}_{x})}_{2}{\mathrm{Te}}_{3}$, in which by varying $x$ charge carriers are chemically tuned to be of $n$-type or $p$-type. Relaxation dynamics is found to be different in various aspects for transitions below or above the band gap, which are selectively excited by changing the pump-pulse energy. For the below-band-gap excitation, an exponential decay of the pump-probe signals is observed, which exhibits linear dependence on the pump-pulse fluence. In contrast, the relaxation dynamics for the above-band-gap excitation is characterized by a compressed exponential decay and nonlinear fluence dependence at high pump flunences, which reflects interaction of the excited nonequilibrium states.

Quadruple cation mixed halide perovskite, GA0.015Cs0.046MA0.152FA0.787Pb(I0.815Br0.185)3, single crystals were grown for the first time using an inverse temperature crystallization process. Solar cell devices in n-i-p stack configuration using thin films of the same materials showed power conversion efficiency above 20%. Complementary time-resolved spectroscopy confirmed that polycrystalline thin films and single crystals identically composed exhibit similar carrier dynamics in the picosecond range. Cooling of excited carriers and bandgap renormalization occur on the same time scale of 200–300 fs. The radiative recombination coefficient (1.2 × 10–9 cm3/s) is comparable to values reported for a GaAs semiconductor. At low excitation density, a long carrier lifetime of 3.2 μs was recorded possibly due to the passivation of recombination centers. This study clarifies discrepancies about the lifetime of hot carriers, the impact of radiative recombination, and the role of recombination centers on solar cell performance. The quadruple cation perovskites displayed short time dynamics with slow recombination of charge carriers. acceptedVersion

Harmonic generation is a general characteristic of driven nonlinear systems, and serves as an efficient tool for investigating the fundamental principles that govern the ultrafast nonlinear dynamics. Here, we report on terahertz-field driven high-harmonic generation in the three-dimensional Dirac semimetal Cd3As2 at room temperature. Excited by linearly-polarized multi-cycle terahertz pulses, the third-, fifth-, and seventh-order harmonic generation is very efficient and detected via time-resolved spectroscopic techniques. The observed harmonic radiation is further studied as a function of pump-pulse fluence. Their fluence dependence is found to deviate evidently from the expected power-law dependence in the perturbative regime. The observed highly non-perturbative behavior is reproduced based on our analysis of the intraband kinetics of the terahertz-field driven nonequilibrium state using the Boltzmann transport theory. Our results indicate that the driven nonlinear kinetics of the Dirac electrons plays the central role for the observed highly nonlinear response., The mechanism and scaling of high harmonic generation in solids is a highly compelling ongoing area of research. Here the authors show a non-perturbative behavior of HHG in terahertz regime from 3D Dirac semimetal, Cd3As2, at room temperature, and reveal the underlying nonlinear kinetics.

SrRuO3, a 4d ferromagnet with multiple Weyl nodes at the Fermi level, offers a rich playground to design epitaxial heterostructures and superlattices with fascinating magnetic and magnetotransport properties. Interfacing ultrathin SrRuO3 layers with large spin–orbit coupling 5d transition-metal oxides, such as SrIrO3, results in pronounced peaklike anomalies in the magnetic field dependence of the Hall resistivity. Such anomalies have been attributed either to the formation of Néel-type skyrmions or to modifications of the Berry curvature of the topologically nontrivial conduction bands near the Fermi level of SrRuO3. Here, epitaxial multilayers based on SrRuO3 interfaced with 5d perovskite oxides, such as SrIrO3 and SrHfO3, were studied. This work focuses on the magnetotransport properties of the multilayers, aiming to unravel the role played by the interfaces with 5d perovskites in the peaklike anomalies of the Hall resistance loops of SrRuO3 layers. Interfacing with large band gap insulating SrHfO3 layers did not influence the anomalous Hall resistance loops, while interfacing with the nominally paramagnetic semimetal SrIrO3 resulted in pronounced peaklike anomalies, which have been lately attributed to a topological Hall effect contribution as a result of skyrmions. This interpretation is, however, under strong debate and lately alternative causes, such as inhomogeneity of the thickness and the electronic properties of the SrRuO3 layers, have been considered. Aligned with these latter proposals, our findings reveal the central role played in the anomalies of the Hall resistivity loops by electronic inhomogeneity of SrRuO3 layers due to the interfacing with semimetallic 5d5 SrIrO3.

Atomically thin layer transition metal dichalcogenides have been intensively investigated for their rich optical properties and potential applications on nano-electronics. In this work, we study the incoherent phonon and exciton population dynamics in monolayer WS

The thermal metal-insulator phase transition in the -stacked (EDO-TTF)(2)PF6 charge transfer salt is of the Peierls type. It is related to geometrical reorganisations and charge ordering phenomena. We report that dimerising displacements are involved in the mechanism of this transition. By using periodic quantum chemical calculations, we find a double well potential in which dimerisation and charge localisation become manifest. By analysing the nuclear wavefunctions we discuss the mechanism of the phase transition in terms of thermal fluctuations.[GRAPHICS].

Trap-limited bimolecular recombination in poly(3-hexylthiophene) (P3HT) and [6,6]-phenyl-C61-butyric acid methyl ester (PC 61 BM) blend films has been investigated by using photo-induced charge extraction by linearly increasing voltage (photo-CELIV) method. The bimolecular recombination rate is strongly dependent on the photoexcitation density, the PC 61 BM composition and the thermal annealing process, but it slightly depends on the thickness of the blend film. The results show that the trap-limited bimolecular recombination is strongly affected by the distribution of the density of trap state (trap DOS). The higher trap-limited bimolecular recombination rate means the trap DOS centered at lower energy which is beneficial to charge carriers transportation, due to the lower activation energy and faster release rate. On the other hand, the trap-limited bimolecular recombination rate is mainly controlled by the slower species of charge carriers in the blend film when the transport of electrons and holes are strongly unbalanced, and the recombination rate will increase when the transport of electrons and holes becomes more balanced.

Monolayer transition metal dichalcogenides (TMDCs) hold the best promise for next generation optoelectronic and valleytronic devices. However, their actual performance is usually largely affected by the presence of inevitable defects. Therefore, a detailed understanding of the influence of defects on the dynamic properties is crucial for optimizing near future implementations. Here, the exciton population and valley scattering dynamics in a chemical vapor deposition grown large size monolayer WSe2 with naturally abundant vacancy and boundary defects were systematically investigated using polarization controlled heterodyned transient grating spectroscopy at different excitation wavelengths and temperatures. Slow and multi-exponential decay dynamics of the exciton population were observed while no sign of any micron scale diffusive transport was identified, consistent with the effect of exciton trapping by defects. In general, two different kinds of exciton species were identified: one with short population lifetime (∼10 ps) and extremely fast intervalley scattering dynamics (1 ns) and very slow intervalley scattering dynamics exceeding 100 ps. We assign the former to non-trapped excitons in the nanometer scale and the latter to defect-bound excitons. Temperature dependent intervalley scattering dynamics of the trapped excitons can be understood in terms of a two optical phonon dominated process at the K point in momentum space. Our findings highlight the importance of the intrinsic defects in monolayer TMDCs for manipulating exciton valley polarization and population lifetimes, which is key for future device applications.

The insulating and conducting phases of (EDO-TTF)(2)PF6 were studied by all electron, periodic Hartre-Fock and hybrid density functional calculations. Electronic properties, such as the electronic band structure, the density of states and the Fermi surface are discussed in relation to the metal-insulator transition in this material. The nature of conduction is confirmed in both phases from their band structures and density of states. The hybrid DFT band gaps are in good agreement with experiment. Interactions are discussed on the basis of band dispersion in the inter-stack, intra-stack and inter-sheet directions. We discuss the phase transition in terms of the Peierls mechanism and our results fully support this view.

The opening of a band gap in graphene nanoribbons induces novel optical and electronic properties, strongly enhancing their application potential in nanoscale devices. Knowledge of the optical excitations and associated relaxation dynamics are essential for developing and optimizing device designs and functionality. Here we report on the optical excitations and associated relaxation dynamics in surface aligned 7-atom wide armchair graphene nanoribbons as seen by time-resolved spontaneous Stokes and anti-Stokes Raman scattering spectroscopy. On the anti-Stokes side we observe an optically induced increase of the scattering intensity of the Raman active optical phonons which we assign to changes in the optical phonon populations. The optical phonon population decays with a lifetime of ∼2 ps, indicating an efficient optical-acoustic phonon cooling mechanism. On the Stokes side we observe a substantial decrease of the phonon peak intensities which we relate to the dynamics of the optically induced exciton population. The exciton population shows a multi-exponential relaxation on the hundreds of ps time scale and is independent of the excitation intensity, indicating that exciton-exciton annihilation processes are not important and the exsistence of dark and trapped exciton states. Our results shed light on the optically induced phonon and exciton dynamics in surface aligned armchair graphene nanoribbons and demonstrate that time-resolved spontaneous Raman scattering spectroscopy is a powerful method for exploring quasi-particle dynamics in low dimensional materials.

The tetradymite compound BiSbTeSe$_2$, is one of the most bulk-insulating three-dimensional topological insulators, which makes it important in the topological insulator research. It is a member of the solid-solution system Bi$_{2-x}$Sb$_x$Te$_{3-y}$Se$_y$, for which the local crystal structure, such as the occupation probabilities of each atomic site, is not well understood. We have investigated the temperature and polarization dependent spontaneous Raman scattering in BiSbTeSe$_2$, revealing a much higher number of lattice vibrational modes than predicted by group theoretical considerations for the space group R$\bar{3}$m corresponding to an ideally random solid-solution situation. The density functional calculations of phonon frequencies show a very good agreement with experimental data for parent material Bi$_2$Te$_3$, where no disorder effects were found. In comparison to Bi$_2$Te$_3$ the stacking disorder in BiSbTeSe$_2$, causes a discrepancy between theory and experiment. Combined analysis of experimental Raman spectra and DFT calculated phonon spectra for different types of atomic orders showed coexistence of different sequences of layers in the material and that those with Se in the center and a local order of Se-Bi-Se-Sb-Te, are the most favored., Comment: 6 pages, 4 figures, 2 tables

We study the absorption spectra of the yellow excitons in Cu$_2$O in high magnetic fields using polarization-resolved optical absorption measurements with a high frequency resolution. We show that the symmetry of the yellow exciton results in unusual selection rules for the optical absorption of polarized light and that the mixing of ortho- and para- excitons in magnetic field is important. Our calculation of the energies of the yellow exciton series in an arbitrary magnetic field gives an excellent fit to experimental data and allows us to understand the complex structure of excitonic levels and their magnetic field dependence, which resolves the old-standing disagreement between the results of optical absorption and cyclotron resonance measurements., 19 pages, 5 figures

In this paper we present a theoretical study of the nature of the ground state of the (EDO-TTF)(2)PF6 charge transfer salt by using ab initio quantum chemical theory for clusters in vacuum, for embedded clusters and for the periodic system. Exemplary for other organic charge transfer systems, we show that by using a relatively low level of theory it is possible to obtain a good understanding of the electronic structure of the ground state. An assessment is made of the proximity of the triplet, the open shell singlet and the closed shell singlet states of (EDO-TTF)(2)PF6. Our calculations reveal also that several charge ordered states are very close in energy. (C) 2015 Elsevier B.V. All rights reserved.

We report on the realization of charge selective CELIV (charge extraction by linearly increasing voltage) via the selective extraction of each charge carrier species in a SiO 2 inserted MIS (metal-insulator-semiconductor) structure. The experiments are performed in a typical active layer of P3HT (poly (3-hexylthiophene)):PCBM (phenyl C 61 -butyric acid methyl ester) with a composition ratio of 1:1. The presence of double CELIV peaks indicates the involvement of deep trap states in the charge transport process. Furthermore the difference in excitation intensity dependence between photo-excited holes and electrons suggests a difference in population probabilities of electrons and holes for shallow and deep trap states. Charge selective CELIV experiments also show that the simultaneous extraction of holes and electrons is not a simple linear superposition of the cases where they are extracted separately, indicating that a fraction of photo-excited charges populating shallow trap states can escape from the device.

Recently, Gao et al. reported being able to measure significant quantities of photogenerated charge up to one hour after it had been generated in an organic semiconductor device. The aim of this paper is twofold; (a) to provide conclusive experimental evidence to support the picture of device operation; and (b) to understand and demonstrate how changes to the device structure and materials can be used to tune the charge carrier lifetime. By tuning both the materials used, and the device structure we are able to observe a charge carrier life time of over 2 hours and still extract significant amounts of charge from the device after 5 hours. This is achieved by engineering the band structure of the device to control the spatial overlap of the stored photoexcited electron and hole populations and thus the recombination rate. By performing lifetime measurements as a function of charge carrier density and applied voltage we find the recombination rate has a 0th order dependence on carrier density, and elucidate the mechanisms responsible for these long charge carrier life times. This work is of technological significance for the development of organic electronic high sensitivity photodetectors and memory elements.

One-dimensional (1D) graphene nanoribbons (GNRs) are promising materials for future electronics and optoelectronics. Their versatility in electronic properties makes it possible to use them as an active element in devices with a tunable band gap. Different from graphene, armchair-edge GNRs (AGNRs) are semiconducting with a direct bandgap [1-3]. However, until now their photophysical characterization has not been addressed properly due to the metal substrate on which they are grown. The substrate hinders measurements such as transmission and photoluminescence (PL). Here we transfer AGNRs with a width of N = 7 atoms from Au(788) to insulating substrates using an alignment-preserving method and investigate their photoluminescence properties.

© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim A semiconductor-to-metal transition in N = 7 armchair graphene nanoribbons causes drastic changes in its electron and phonon system. By using angle-resolved photoemission spectroscopy of lithium-doped graphene nanoribbons, a quasiparticle band gap renormalization from 2.4 to 2.1 eV is observed. Reaching high doping levels (0.05 electrons per atom), it is found that the effective mass of the conduction band carriers increases to a value equal to the free electron mass. This giant increase in the effective mass by doping is a means to enhance the density of states at the Fermi level which can have palpable impact on the transport and optical properties. Electron doping also reduces the Raman intensity by one order of magnitude, and results in relatively small (4 cm−1) hardening of the G phonon and softening of the D phonon. This suggests the importance of both lattice expansion and dynamic effects. The present work highlights that doping of a semiconducting 1D system is strikingly different from its 2D or 3D counterparts and introduces doped graphene nanoribbons as a new tunable quantum material with high potential for basic research and applications.

In modern bulk heterojunction (BHJ) organic solar cells, blends of low-bandgap polymer and [70]PCBM acceptor are used in the active layer. In this combination, the polymer absorbs photons from the red and near-IR parts of the solar spectrum, while the blue and near-UV photons are harvested by [70]PCBM. As a result, both electron transfer from polymer to [70]PCBM and hole transfer from [70]PCBM to polymer are of utmost importance in free charge generation and have to be optimized simultaneously. Here we study electron and hole transfer processes in BHJ blends of two low-bandgap polymers, BTT-DPP and PCPDTBT, by ultrafast photoinduced spectroscopy (PIA). By tracking the PIA dynamics, we observed substantially different charge separation pathways in BHJs of the two polymers with [70]PCBM. From the photoinduced anisotropy dynamics, we demonstrated that in the PCPDTBT:[70]PCBM system both electron and hole transfer processes are highly efficient, while in the BTTBPP:[ 70]PCBM electron transfer is blocked due to the unfortunate energy level alignment leaving hole transfer the only pathway to free charge generation. Calculations at the density functional theory level are used to gain more insight into our findings. The presented results highlight the importance of the energy level alignment on the charge separation process.

Morphology of organic photovoltaic bulk heterojunctions (BHJs) – a nanoscale texture of the donor and acceptor phases – is one of the key factors influencing efficiency of organic solar cells. Detailed knowledge of the morphology is hampered by the fact that it is notoriously difficult to investigate by microscopic methods. Here we all-optically track the exciton harvesting dynamics in the fullerene acceptor phase from which subdivision of the fullerene domain sizes into the mixed phase (2–15 nm) and large (>50 nm) domains is readily obtained via the Monte-Carlo simulations. These results were independently confirmed by a combination of X-ray scattering, electron and atomic-force microscopies, and time-resolved photoluminescence spectroscopy. In the large domains, the excitons are lost due to the high energy disorder while in the ordered materials the excitons are harvested with high efficiency even from the domains as large as 100 nm due to the absence of low-energy traps. Therefore, optimizing of blend nanomorphology together with increasing the material order are deemed as winning strategies in the exciton harvesting optimization.

Atomically thin layer transition metal dichalcogenides have been intensively investigated for their rich optical properties and potential applications on nano-electronics. In this work, we study the incoherent phonon and exciton population dynamics in monolayer WS2 by time-resolved Resonance Raman scattering spectroscopy. Upon excitation of the exciton transition, both Stokes and anti-Stokes scattering strength of the optical and the longitudinal acoustic two phonon modes exhibit large reduction. Based on the assumption of quasi-equilibrium distribution, the hidden phonon population dynamics is retrieved, which shows an instant build-up and a relaxation lifetime of ∼4 ps at the exciton density ∼1012cm−2. A phonon temperature rises of ∼20 K was identified due to the exciton excitation and relaxation. The exciton relaxation dynamics extracted from the transient vibrational Raman response shows strong excitation density dependence, signaling an important bi-molecular contribution to the decay. These results provide significant knowledge on the thermal dynamics after optical excitation, enhance the understanding of the fundamental exciton dynamics in two-dimensional transition metal materials, and demonstrate that time-resolved Resonance Raman scattering spectroscopy is a powerful method for exploring quasi-particle dynamics in optical materials.

Recent experimental and theoretical work on hydrogen-like absorption spectra of excitons in external magnetic fields revealed new effects when the Coulomb interaction becomes comparable to the magnetic perturbation. We present a theoretical approach that allows for calculation of absorption spectra for any value of magnetic field. This approach opens the possibility to compute the optical functions i.e. reflectivity, transmission and absorption including the excitonic effects for various strength of external magnetic field.

Linear as well as time resolved absorption measurements were performed on 40 nm and 170 nm thick MAPbL films with PEDOT:PSS hole extraction layer, spin-coated on quartz substrate. From linear absorption measurements exciton binding energy of 18 – 19 meV and band gap of 1.60 - 1.62 eV was deduced. Transient absorption spectra after the excitation at 1.77 eV showed a strong difference in carrier recombination dynamics for the two MAPbI3 films of different thicknesses. From the analysis on the decay dynamics, hole population lifetime of 0.3 ns and 3.5 ns for 40 nm and 170 nm films, respectively, are determined. A numerical 1D diffusion model was used to model the carrier relaxation dynamics yielding hole diffusion constants of 0.025 - 0.030 cm2s−1, which results in a hole mobility of 1 cm2(Vs)−1 in these MAPbI3 films.