Investigations of the electronic, vibrational and structural properties of single and few-layer graphene

Single and few-layer graphene (SLG and FLG) have stimulated great scientific interest because of their distinctive properties and potential for novel applications. In this dissertation, we investigate the mechanical, electronic and vibrational properties of these remarkable materials by various techniques, including atomic-force microscopy (AFM) and Raman, infrared (IR), and ultrafast optical spectroscopy. With respect to its mechanical properties, SLG is known to be capable of undergoing significant mechanical deformation. We have applied AFM to investigate how the morphology of SLG is influenced by the substrate on which it is deposited. We have found that SLG is strongly affected by the morphology of the underlying supporting surface. In particular, SLG deposited on atomically flat surfaces of mica substrates exhibits an ultraflat morphology, with height variation essentially indistinguishable from that observed for the surface of cleaved graphite. One of the most distinctive aspects of SLG is its spectrum of electronic excitations, with its characteristic linear energy-momentum dispersion relation. We have examined the dynamics of the corresponding Dirac fermions by optical emission spectroscopy. By analyzing the spectra of light emission induced in the spectral visible range by 30-femtosecond laser pulses, we find that the charge carriers in graphene cool by the emission of strongly coupled optical phonons in a few 10's of femtoseconds and thermalize among themselves even more rapidly. The charge carriers and the strongly coupled optical phonons are thus essentially in thermal equilibrium with one another on the picosecond time scale, but can be driven strongly out of equilibrium with the other phonons in the system. Temperatures exceeding 3000 K are achieved for the subsystem of the charge carriers and optical phonons under femtosecond laser excitation. While SLG exhibits remarkable physical properties, its few-layer counterparts are also of great interest. In particular, FLG can exist in various crystallographic stacking sequences, which strongly influence the material's electronic properties. We have developed an accurate and convenient method of characterizing stacking order in FLG using the lineshape of the Raman 2D-mode. Raman imaging allows us to visualize directly the spatial distribution of Bernal (ABA) and rhombohedral (ABC) stacking in trilayer and tetralayer graphene. We find that 15% of exfoliated graphene trilayers and tetralayers are comprised of micrometer-sized domains of rhombohedral stacking, rather than of usual Bernal stacking. The accurate identification of stacking domains in FLG allows us to investigate the influence of stacking order on the material's electronic properties. In particular, we have studied by means of IR spectroscopy the possibility of opening a band gap by the application of a strong perpendicular electric field in trilayer graphene. We observe an electrically tunable band gap exceeding 100 meV in ABC trilayers, while no band gap is found for ABA trilayers. We have also studied the influence of layer thickness and stacking order on the Raman response of the out-of-plane vibrations in FLG. We observe a Raman combination mode that involves the layer-breathing vibrations in FLG. This Raman mode is absent in SLG and exhibits a lineshape that depends sensitively on both the material's layer thickness and stacking sequence

Observation of intervalley biexcitonic optical Stark effect in monolayer WS2

Coherent optical dressing of quantum materials offers technological advantages to control their electronic properties, such as the electronic valley degree of freedom in monolayer transition metal dichalcogenides (TMDs). Here, we observe a new type of optical Stark effect in monolayer WS2, one that is mediated by intervalley biexcitons under the blue-detuned driving with circularly polarized light. We found that such helical optical driving not only induces an exciton energy downshift at the excitation valley, but also causes an anomalous energy upshift at the opposite valley, which is normally forbidden by the exciton selection rules but now made accessible through the intervalley biexcitons. These findings reveal the critical, but hitherto neglected, role of biexcitons to couple the two seemingly independent valleys, and to enhance the optical control in valleytronics

Rdzeniowy zespół twarzowo-palcowy: częsty zespół w nietypowej lokalizacji

Background and purpose Cheiro-oral syndrome (COS) is an established neurological entity characterized by a sensory impairment confined to the mouth angle and ipsilateral finger(s)/ hand. The current understanding of localization is a concomitant involvement of the spinothalamic and trigeminothalamic tract between the cortex and pons. The cervical spinal cord has not been mentioned in this situation yet, and this unusual location may heretofore increase the risk of misdiagnosis. Material and methods Six patients who presented with unilateral COS due to cervical cord disorder are reported. Results All patients were women and their age ranged between 42 and 70 years. Their neurological deficits included unilateral paraesthesiae restricted to cheiro-oral distribution, positive radicular sign, and mild change of tendon reflex. Cervical spinal stenosis at middle/lower cervical spine with variable magnitude of cord compression and intrinsic cord damage was found. A diagnostic dilemma obviously arises from the lack of tangible neurological signs or typical pattern of myelopathy, in addition to the previous concept of cerebral involvement. A benign course ensued in all reported patients. Conclusions Cheiro-oral syndrome can be an early neurological sign for cervical cord disorder; it further suggests that it is a strong neurological but weak localizing sign. A reciprocal influence of multiple factors is considered to generate COS at the cervical cord. Therefore, an absence of brain pathology should lead to a thorough examination of the cervical cord in case of COS.Wstęp i cel pracy Zespół twarzowo-palcowy (ZTP) jest znanym zespołem neurologicznym, który cechuje się niedoczulicą ograniczoną do kącika ust i palców ręki lub ręki po tej samej stronie. Bieżący stan wiedzy dotyczący lokalizacji uszkodzenia w tym zespole wskazuje na jednoczesne zajęcie dróg rdzeniowo-wzgórzowej i trójdzielno-wzgórzowej pomiędzy mostem i korą mózgową. W tym kontekście nie wymieniano dotąd uszkodzenia rdzenia kręgowego w odcinku szyjnym, a taka nietypowa lokalizacja uszkodzenia może zwiększyć ryzyko błędnego rozpoznania miejsca uszkodzenia. Materiał i metody W pracy przedstawiono dane dotyczące 6 pacjentek z jednostronnym ZTP spowodowanym występowaniem nieprawidłowości w obrębie rdzenia kręgowego. Wyniki Zakres wieku pacjentek wynosił od 42 do 70 lat. Objawy neurologiczne obejmowały jednostronne parestezje ograniczone do obszaru twarzy i ręki, objaw korzeniowy i niewielkie nieprawidłowości w zakresie odruchów głębokich. Stwierdzono występowanie zwężenia kanału kręgowego w środkowej lub dolnej części odcinka szyjnego z uciskiem rdzenia kręgowego i uszkodzeniem wewnątrz rdzenia kręgowego. Wątpliwości diagnostyczne wynikały z braku typowych objawów neurologicznych mielopatii i stwierdzenia lokalizacji zmian nieodpowiadającej wcześniejszym opiniom na temat mózgowego pochodzenia zespołu. U wszystkich opisywanych pacjentek przebieg schorzenia był łagodny. Wnioski Zespół twarzowo-palcowy może być wczesnym objawem neurologicznym nieprawidłowości w obrębie rdzenia kręgowego. Stanowi istotny objaw neurologiczny, ale jego wartość lokalizacyjna jest niewielka. Powstawanie ZTP wskutek uszkodzenia rdzenia kręgowego wynika z wzajemnych oddziaływań wielu czynników. W razie braku uchwytnej patologii mózgu należy w przypadkach ZTP przeprowadzić szczegółowe badania rdzenia kręgowego w odcinku szyjnym

Large, valley-exclusive Bloch-Siegert shift in monolayer WS2

Coherent interaction with off-resonance light can be used to shift the energy levels of atoms, molecules, and solids. The dominant effect is the optical Stark shift, but there is an additional contribution from the so-called Bloch-Siegert shift that has eluded direct and exclusive observation in solids. We observed an exceptionally large Bloch-Siegert shift in monolayer tungsten disulfide (WS[subscript 2]) under infrared optical driving. By controlling the light helicity, we could confine the Bloch-Siegert shift to occur only at one valley, and the optical Stark shift at the other valley, because the two effects obey opposite selection rules at different valleys. Such a large and valley-exclusive Bloch-Siegert shift allows for enhanced control over the valleytronic properties of two-dimensional materials.United States. Department of EnergyUnited States. Dept. of Energy. Division of Materials Sciences and EngineeringGordon and Betty Moore Foundation (EPiQS Initiative Grant GBMF4540)Harvard University. Center for Integrated Quantum Materials (Grant DMR-1231319