Edbert Jarvis Sie

Valley-selective optical Stark effect in monolayer WS2

Breaking space-time symmetries in two-dimensional crystals can markedly influence their macroscopic electronic properties. Monolayer transition metal dichalcogenides (TMDs) are prime examples where the intrinsically broken crystal inversion symmetry permits the generation of valley-selective electron populations, even though the two valleys are energetically degenerate, locked by time-reversal symmetry. Lifting the valley degeneracy in these materials is of great interest because it would allow for valley-specific band engineering and offer additional control in valleytronic applications. Although applying a magnetic field should, in principle, accomplish this task, experiments so far have not shown valley-selective energy level shifts in fields accessible in the laboratory. Here, we show the first direct evidence of lifted valley degeneracy in the monolayer TMD WS2. By applying intense circularly polarized light, which breaks time-reversal symmetry, we demonstrate that the exciton level in each valley can be selectively tuned by as much as 18 meV through the optical Stark effect. These results offer a new way to control the valley degree of freedom, and may provide a means to realize new Floquet topological phases in two-dimensional TMDs.

Measurement of Intrinsic Dirac Fermion Cooling on the Surface of the Topological Insulator Bi2Se3 Using Time-Resolved and Angle-Resolved Photoemission Spectroscopy

We perform time- and angle-resolved photoemission spectroscopy of a prototypical topological insulator (TI) Bi(2)Se(3) to study the ultrafast dynamics of surface and bulk electrons after photoexcitation. By analyzing the evolution of surface states and bulk band spectra, we obtain their electronic temperature and chemical potential relaxation dynamics separately. These dynamics reveal strong phonon-assisted surface-bulk coupling at high lattice temperature and total suppression of inelastic scattering between the surface and the bulk at low lattice temperature. In this low temperature regime, the unique cooling of Dirac fermions in TI by acoustic phonons is manifested through a power law dependence of the surface temperature decay rate on carrier density.

Intervalley biexcitons and many-body effects in monolayer MoS 2

Interactions between two excitons can result in the formation of bound quasiparticles, known as biexcitons. Their properties are determined by the constituent excitons, with orbital and spin states resembling those of atoms. Monolayer transition metal dichalcogenides (TMDs) present a unique system where excitons acquire a new degree of freedom, the valley pseudospin, from which a novel intervalley biexciton can be created. These biexcitons comprise two excitons from different valleys, which are distinct from biexcitons in conventional semiconductors and have no direct analog in atomic and molecular systems. However, their valley properties are not accessible to traditional transport and optical measurements. Here, we report the observation of intervalley biexcitons in the monolayer TMD MoS2 using ultrafast pump-probe spectroscopy. By applying broadband probe pulses with different helicities, we identify two species of intervalley biexcitons with large binding energies of 60 and 40 meV. In addition, we also reveal effects beyond biexcitonic pairwise interactions in which the exciton energy redshifts at increasing exciton densities, indicating the presence of many-body interactions among them.

Large, Valley-Exclusive Bloch-Siegert Shift in Monolayer WS2

Going way off resonance Single atomic layers of transition metal dichalcogenide (TMD) materials have two nonequivalent valleys in their electronic structure. When researchers shine visible light on these monolayers, left-circularly polarized light modifies the electronic levels in one valley but not the other. Sie et al. studied the material WS2. They found that in the infrared regime, if the frequency of the light was far away from the resonance, energy levels in both valleys were affected. The so-called Bloch-Siegert effect could explain the energy shift in the “wrong” valley. The findings should be important for the manipulation of valleytronic properties of TMDs. Science, this issue p. 1066 Infrared pump-probe spectroscopy is used to measure coherent light-matter interactions in tungsten disulfide. 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 (WS2) 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.

Observation of Intervalley Biexcitonic Optical Stark Effect in Monolayer WS2

Coherent optical driving can effectively modify the properties of electronic valleys in transition metal dichalcogenides. 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 find 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.

Observation of Exciton Redshift–Blueshift Crossover in Monolayer WS2

We report a rare atom-like interaction between excitons in monolayer WS2, measured using ultrafast absorption spectroscopy. At increasing excitation density, the exciton resonance energy exhibits a pronounced redshift followed by an anomalous blueshift. Using both material-realistic computation and phenomenological modeling, we attribute this observation to plasma effects and an attraction-repulsion crossover of the exciton-exciton interaction that mimics the Lennard-Jones potential between atoms. Our experiment demonstrates a strong analogy between excitons and atoms with respect to interparticle interaction, which holds promise to pursue the predicted liquid and crystalline phases of excitons in two-dimensional materials.

Time-Resolved Absorption Spectroscopy

This dissertation work emphasizes on the exciton energy shift that is induced by femtosecond light pulses. At equilibrium, the exciton energy level in monolayer TMDs sits in the visible regime, e.g., E 0 = 2 eV in monolayer WS2. In order to detect this energy shift, we need a broadband probe pulse that is centered in the visible spectrum. White light continuum generation is a nonlinear optical process capable of producing such broadband light pulse between 500 and 700 nm (ℏω = 1.8 − 2.4 eV). In this chapter, we will discuss about time-resolved absorption spectroscopy setup (or simply transient absorption) that utilizes white light continuum to probe the exciton energy shift in monolayer TMDs. In the first section, we will show the overview of the transient absorption setup. In later sections, we will discuss in more details about (1) laser amplifier, (2) optical parametric amplifier, and (3) white light continuum generation. Finally, we will discuss about the data analysis based on the optical physics of monolayer materials on a transparent substrate.

Intervalley Biexcitons in Monolayer MoS 2

Interactions between two excitons can result in the formation of bound quasiparticles, known as biexcitons. Their properties are determined by the constituent excitons, with orbital and spin states resembling those of atoms. Monolayer transition metal dichalcogenides (TMDs) present a unique system where excitons acquire a new degree of freedom, the valley pseudospin, from which a novel intervalley biexciton can be created. These biexcitons comprise two excitons from different valleys, which are distinct from biexcitons in conventional semiconductors and have no direct analogue in atomic and molecular systems. However, their valley properties are not accessible to traditional transport and optical measurements. Here, we report the observation of intervalley biexcitons in the monolayer TMD MoS2 using ultrafast pump-probe spectroscopy [1]. By applying broadband probe pulses with different helicities, we identify two species of intervalley biexcitons with large binding energies of 60 and 40 meV. In addition, we also reveal effects beyond biexcitonic pairwise interactions in which the exciton energy redshifts at increasing exciton densities, indicating the presence of many-body interactions among them.

Lennard-Jones-Like Potential of 2D Excitons in Monolayer WS 2

In this chapter, we report a rare atom-like interaction between excitons in monolayer WS2, measured using ultrafast absorption spectroscopy. At increasing excitation density, the exciton resonance energy exhibits a pronounced redshift followed by an anomalous blueshift. Using both material-realistic computation and phenomenological modeling, we attribute this observation to plasma effects and an attraction-repulsion crossover of the exciton-exciton interaction that mimics the Lennard-Jones potential between atoms. Our experiment demonstrates a strong analogy between excitons and atoms with respect to inter-particle interaction, which holds promise to pursue the predicted liquid and crystalline phases of excitons in two-dimensional materials.

Intervalley Biexcitonic Optical Stark Effect in Monolayer WS 2

Coherent optical driving can effectively modify the properties of electronic valleys in transition metal dichalcogenides. 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 [1]. We find 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.