When intense lightwaves accelerate electrons through a solid, the emerging high-order harmonic (HH) radiation offers key insights into the material
. Sub-optical-cycle dynamics-such as dynamical ...Bloch oscillations
, quasiparticle collisions
, valley pseudospin switching
and heating of Dirac gases
-leave fingerprints in the HH spectra of conventional solids. Topologically non-trivial matter
with invariants that are robust against imperfections has been predicted to support unconventional HH generation
. Here we experimentally demonstrate HH generation in a three-dimensional topological insulator-bismuth telluride. The frequency of the terahertz driving field sharply discriminates between HH generation from the bulk and from the topological surface, where the unique combination of long scattering times owing to spin-momentum locking
and the quasi-relativistic dispersion enables unusually efficient HH generation. Intriguingly, all observed orders can be continuously shifted to arbitrary non-integer multiples of the driving frequency by varying the carrier-envelope phase of the driving field-in line with quantum theory. The anomalous Berry curvature warranted by the non-trivial topology enforces meandering ballistic trajectories of the Dirac fermions, causing a hallmark polarization pattern of the HH emission. Our study provides a platform to explore topology and relativistic quantum physics in strong-field control, and could lead to non-dissipative topological electronics at infrared frequencies.
Harnessing the carrier wave of light as an alternating-current bias may enable electronics at optical clock rates
. Lightwave-driven currents have been assumed to be essential for high-harmonic ...generation in solids
, charge transport in nanostructures
, attosecond-streaking experiments
and atomic-resolution ultrafast microscopy
. However, in conventional semiconductors and dielectrics, the finite effective mass and ultrafast scattering of electrons limit their ballistic excursion and velocity. The Dirac-like, quasi-relativistic band structure of topological insulators
may allow these constraints to be lifted and may thus open a new era of lightwave electronics. To understand the associated, complex motion of electrons, comprehensive experimental access to carrier-wave-driven currents is crucial. Here we report angle-resolved photoemission spectroscopy with subcycle time resolution that enables us to observe directly how the carrier wave of a terahertz light pulse accelerates Dirac fermions in the band structure of the topological surface state of Bi
Te
. While terahertz streaking of photoemitted electrons traces the electromagnetic field at the surface, the acceleration of Dirac states leads to a strong redistribution of electrons in momentum space. The inertia-free surface currents are protected by spin-momentum locking and reach peak densities as large as two amps per centimetre, with ballistic mean free paths of several hundreds of nanometres, opening up a realistic parameter space for all-coherent lightwave-driven electronic devices. Furthermore, our subcycle-resolution analysis of the band structure may greatly improve our understanding of electron dynamics and strong-field interaction in solids.
The success of topological insulators (TI) in creating devices with unique functionalities is directly connected to the ability of coupling their helical spin states to well-defined perturbations. ...However, up to now, TI-based heterostructures always resulted in very disordered interfaces, characterized by strong mesoscopic fluctuations of the chemical potential that make the spin-momentum locking ill-defined over length scales of few nanometers or even completely destroy topological states. These limitations call for the ability to control topological interfaces with atomic precision. Here, we demonstrate that molecular self-assembly processes driven by inherent interactions among the constituents offer the opportunity to create well-defined networks at TIs surfaces. Even more remarkably, we show that the symmetry of the overlayer can be finely controlled by appropriate chemical modifications. By analyzing the influence of the molecules on the TI electronic properties, we rationalize our results in terms of the charge redistribution taking place at the interface. Overall, our approach offers a precise and fast way to produce tailor-made nanoscale surface landscapes. In particular, our findings make organic materials ideal TIs counterparts, because they offer the possibility to chemically tune both electronic and magnetic properties within the same family of molecules, thereby bringing us a significant step closer toward an application of this fascinating class of materials.
•Noncentrosymmetric crystals of RSc3(BO3)4 (R=La,Pr,Nd) were grown by TSSG from LiBO2-LiF flux.•RBO3 – ScBO3 diagrams (R=La, Pr and Nd) were refined by the solid-state synthesis and DSC ...methods.•Crystal structures were refined by single crystal x-ray analysis.•Luminescent spectra and second harmonic generation for grown crystals of RSc3(BO3)4 (R=La,Pr,Nd) were studied.
RBO3 – ScBO3 diagrams (R = La, Pr and Nd) were investigated by the solid state synthesis and DSC methods. In these systems the solid solutions based on RSc3(BO3)4, RBO3 and ScBO3 were identified. The single crystals of RSc3(BO3)4 were grown by spontaneous crystallization method from LiBO2-LiF flux. The borates containing Pr and Nd have typical luminescence in the red/IR range which correlated to Pr3+: 3P0 → 3H6, 1D2 → 3H4 (~ 620 nm), and 3P0 → 2F2, 1D2 → 3H5 (~ 655 nm) and Nd3+ electron transitions 4F3/2 → 4I9/2 (875 nm) and 4F3/2 → 4I11/2 (1055 nm). The luminescence intensity strongly depends on the concentration of the fluorophores. In addition the SHG efficiency (for radiation of Nd:YAG laser, 1064 nm) for grown PrSc3(BO3)4 crystals was found to be 1.85 times higher (deff) than for KDP revealing its high potential for various NLO applications.
We study ultrafast population dynamics in the topological surface state of SbFormula: see textTeFormula: see text in two-dimensional momentum space with time- and angle-resolved two-photon ...photoemission spectroscopy. Linearly polarized mid-infrared pump pulses are used to permit a direct optical excitation across the Dirac point. We show that this resonant excitation is strongly enhanced within the Dirac cone along three of the six Formula: see text-Formula: see text directions and results in a macroscopic photocurrent when the plane of incidence is aligned along a Formula: see text-Formula: see text direction. Our experimental approach makes it possible to disentangle the decay of transiently excited population and photocurent by elastic and inelastic electron scattering within the full Dirac cone in unprecedented detail. This is utilized to show that doping of SbFormula: see textTeFormula: see text by vanadium atoms strongly enhances inelastic electron scattering to lower energies, but only scarcely affects elastic scattering around the Dirac cone.
The recent focus on topological insulators is due to the scientific interest in the new state of quantum matter as well as the technology potential for a new generation of THz optoelectronics, ...spintronics and quantum computations. It is important to elucidate the dynamics of the Dirac fermions in the topologically protected surface state. Hence we utilized a novel ultrafast optical pump mid-infrared probe to explore the dynamics of Dirac fermions near the Dirac point. The femtosecond snapshots of the relaxation process were revealed by the ultrafast optics. Specifically, the Dirac fermion-phonon coupling strength in the Dirac cone was found to increase from 0.08 to 0.19 while Dirac fermions were away from the Dirac point into higher energy states. Further, the energy-resolved transient reflectivity spectra disclosed the energy loss rate of Dirac fermions at room temperature was about 1 meV/ps. These results are crucial to the design of Dirac fermion devices.
Phase pure Tb
1–
x
Yb
x
Al
3
(BO
3
)
4
(
x
= 0 – 1) crystalline powders were prepared by the combustion synthesis method. Down-conversion experiments under UV excitation of 375 nm revealed optimal ...concentration of Yb
x
= 0.5 providing intensive green luminescence with 24% of quantum efficiency. Also up-conversion luminescence via energy transfer from Yb
3+
to Tb
3+
using a low power IR diode laser operating at 980 nm was achieved. Here the most powerful green emission was obtained with
x
= 0.1.
Strong light fields have created opportunities to tailor novel functionalities of solids
. Floquet-Bloch states can form under periodic driving of electrons and enable exotic quantum phases
. On ...subcycle timescales, lightwaves can simultaneously drive intraband currents
and interband transitions
, which enable high-harmonic generation
and pave the way towards ultrafast electronics. Yet, the interplay of intraband and interband excitations and their relation to Floquet physics have been key open questions as dynamical aspects of Floquet states have remained elusive. Here we provide this link by visualizing the ultrafast build-up of Floquet-Bloch bands with time-resolved and angle-resolved photoemission spectroscopy. We drive surface states on a topological insulator
with mid-infrared fields-strong enough for high-harmonic generation-and directly monitor the transient band structure with subcycle time resolution. Starting with strong intraband currents, we observe how Floquet sidebands emerge within a single optical cycle; intraband acceleration simultaneously proceeds in multiple sidebands until high-energy electrons scatter into bulk states and dissipation destroys the Floquet bands. Quantum non-equilibrium calculations explain the simultaneous occurrence of Floquet states with intraband and interband dynamics. Our joint experiment and theory study provides a direct time-domain view of Floquet physics and explores the fundamental frontiers of ultrafast band-structure engineering.
•K7CaR2(B5O10)3 (where R-Nd,Yb) crystals were grown from new flux.•SHG efficiency for K7CaR2(B5O10)3 (where R-Nd,Yb) crystals is comparable to that of KDP.•Luminescent and absorption spectra for ...K7CaR2(B5O10)3 (where R-Nd,Yb) were measured.
Non-centrosymmetric borates K7CaR2(B5O10)3 have been synthesized by solid state reaction and successfully grown by the top seeded solution growth method using K2O-B2O3-CaF2 flux. IR, Raman, absorption spectra as well as data on melting temperature for the crystals were obtained. Optical properties like UV absorption edge and SHG intensity were compared with KH2PO4 (KDP) and K7CaY2(B5O10)3.
Hybrid organic/inorganic interfaces have been widely reported to host emergent properties that go beyond those of their single constituents. Coupling molecules to the recently discovered topological ...insulators, which possess linearly dispersing and spin-momentum-locked Dirac fermions, may offer a promising platform toward new functionalities. Here, we report a scanning tunneling microscopy and spectroscopy study of the prototypical interface between MnPc molecules and a Bi2Te3 surface. MnPc is found to bind stably to the substrate through its central Mn atom. The adsorption process is only accompanied by a minor charge transfer across the interface, resulting in a moderately n-doped Bi2Te3 surface. More remarkably, topological states remain completely unaffected by the presence of the molecules, as evidenced by the absence of scattering patterns around adsorption sites. Interestingly, we show that, while the HOMO and LUMO orbitals closely resemble those of MnPc in the gas phase, a new hybrid state emerges through interaction with the substrate. Our results pave the way toward hybrid organic–topological insulator heterostructures, which may unveil a broad range of exciting and unknown phenomena.
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