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When a laser beam induces surface tension gradient at the free surface of a liquid, a weak surface depression is expected and has been observed. Here we report giant depression and rupture in “optothermocapillary fluids” under the illumination of laser and sunlight. Computational fluid dynamics models were developed to understand the surface deformation and provided desirable physical parameters of the fluid for maximum deformation. New optothermocapillary fluids were created by mixing transparent lamp oil with different candle dyes. They can be cut open by sunlight and be patterned to different shapes and sizes using an ordinary laser show projector or a common laser pointer. Laser driving and elevation of optothermocapillary fluids, in addition to the manipulation of different droplets on their surface, were demonstrated as an efficient controlling method and platform for optofluidic operations. The fundamental understanding of light-induced giant depression and creation of new optothermocapillary fluids encourage the fundamental research and applications of optofluidics.

MoSe2–WSe2 heterostructures host strongly bound interlayer excitons (IXs), which exhibit bright photoluminescence (PL) when the twist angle is near 0° or 60°. Over the past several years, there have been numerous reports on the optical response of these heterostructures but no unifying model to understand the dynamics of IXs and their temperature dependence. Here we perform a comprehensive study of the temperature, excitation power, and time-dependent PL of IXs. We observe a significant decrease in PL intensity above a transition temperature that we attribute to a transition from localized to delocalized IXs. Astoundingly, we find a simple inverse relationship between the IX PL energy and the transition temperature, which exhibits opposite power-dependent behaviors for near 0° and 60° samples. We conclude that this temperature dependence is a result of IX–IX exchange interactions, whose effect is suppressed by the moiré potential trapping IXs at low temperature.

Two-dimensional (2D) material–organic interfaces offer a platform to realize hybrid materials with tunable optical properties that are determined by the interactions between the disparate materials...

Auger recombination in semiconductors is a many-body phenomenon in which recombination of electrons and holes is accompanied by excitation of other charge carriers. Being nonradiative, it is detrimental to light emission. The excess energy of the excited carriers is normally rapidly converted to heat, making Auger processes difficult to probe directly. Here, we employ a technique in which the Auger-excited carriers are detected by their ability to tunnel out of the semiconductor through a thin barrier, generating a current. We employ vertical van der Waals (vdW) heterostructures with monolayer WSe2 as the semiconductor and the wide band gap hexagonal boron nitride (hBN) as the tunnel barrier to preferentially transmit high-energy Auger-excited carriers to a graphite electrode. The unambiguous signatures of Auger processes are a rise in the photocurrent when excitons are created by resonant excitation, and negative differential photoconductance resulting from the shifts of the exciton resonances with voltage. We detect holes Auger-excited by both neutral and charged excitons, and find that the Auger scattering is surprisingly strong under weak excitation. The selective extraction of Auger carriers at low, controlled carrier densities that is enabled by vdW heterostructures illustrates an important addition to the techniques available for probing relaxation processes in 2D materials.

Over the past decade, excitonic effects in two-dimensional transition metal dichalcogenide semiconductors such as MoS2 and WSe2 have been intensely studied. Currently, there is significant interest in understanding how to control excitons in heterostructures and on-chip optical structures that have potential applications to excitonic and optical information processing devices. In this presentation, I will discuss our recent work exploring the nature of the moire trapping potential in MoSe2-WSe2 heterostructures, where the interlayer exciton photoluminescence exhibits a strong temperature dependence. I will also discuss our work demonstrating coupling between organic PTCDA molecular excitons and monolayer WSe2 excitons, which manifests as a ~20 times enhancement of the PTCDA Raman scattering efficiency. Finally, I will report on our recent studies on 2D semiconductor plasmonic structures composed of propagating surface plasmon polaritons (SPPs) coupled to monolayer WSe2 excitons. In our new “cross geometry” structures, we are able to explore the nonlinear exciton response of both co- and cross- propagating SPPs. In these devices, we observe a large (near unity) differential transmission response and population pulsation resonances that are dependent on the direction of SPP propagation.

For quantum technologies based on single excitons and spins, the deterministic placement and control of a single exciton is a long-standing goal. MoSe2-WSe2 heterostructures host spatially indirect interlayer excitons (IXs) which exhibit highly tunable energies and unique spin-valley physics, making them promising candidates for quantum information processing. Previous IX trapping approaches involving moir\'e superlattices and nanopillars do not meet the quantum technology requirements of deterministic placement and energy tunability. Here, we use a nanopatterned graphene gate to create a sharply varying electric field in close proximity to a MoSe2-WSe2 heterostructure. The dipole interaction between the IX and the electric field creates an ~20 nm trap. The trapped IXs show the predicted electric field dependent energy, saturation at low excitation power, and increased lifetime, all signatures of strong spatial confinement. The demonstrated architecture is a crucial step towards deterministic trapping of single IXs, which has broad applications to scalable quantum technologies.

The far-field linear and nonlinear optical response of excitons in two-dimensional (2D) semiconducting transitional metal dichalcogenides (TMDs), such as MoS2 and WSe2, have been the subject of intense investigation over the past decade. Here, we report on our experimental results measuring the linear and nonlinear response of surface plasmon polaritons (SPPs) propagating on metallic waveguides interacting with excitons in a single WSe2 monolayer. The WSe2 monolayer was encapsulated in hexagonal boron nitride and transferred on top of a metallic waveguide. The measurements were carried out at low temperature (below 11 K). We measured the linear absorption of SPPs by excitons, resulting in a 73 % attenuation of the transmitted probe. To determine the nonlinear response, we performed both optical pump-SPP probe and SPP pump-SPP probe experiments. For the SPP pump case, a differential transmission response exceeding 4 % was achieved. Time-resolved pump-probe measurements reveal a fast component of the nonlinear response of 290 fs with a slower 13.7 ps component, consistent with previous optical measurements. These plasmonic structures could open up new opportunities to probe fundamental light-matter interactions in 2D material-plasmonic heterostructures.

In crystalline systems, the electronic band structure determines the relationship between the crystal momentum and energy of an electron. In intrinsic semiconductors, the Fermi energy lies between two bands, where typically the highest valence band below the Fermi energy and lowest conduction band above the Fermi energy determine the electronic and optical physics. These extrema are referred to as crystal momentum space “valleys,” which are stable points in the band structure that electrons or holes can occupy. So that in addition to charge and spin, electrons in a crystalline solid also have a valley degree of freedom that determines the electron's position in crystal momentum space. The field of valleytronics seeks to use the electron's valley degree of freedom to encode and process information, analogous to charge in electronics or spin in spintronics. In this chapter, I will review the recent progress in 2D semiconductor valleytronics.

Alloying plays a central role in tailoring the material properties of 2D transition-metal dichalcogenides (TMDs). However, despite widespread reports, the details of the alloying mechanism in 2D TMDs have remained largely unknown and are yet to be further explored. Here, we combine a set of systematic experiments with ab initio density functional theory (DFT) calculations to unravel a defect-mediated mechanism for the alloying of monolayer TMD crystals. In our alloying approach, a monolayer MoSe2 film serves as a host crystal in which exchanging selenium (Se) atoms with sulfur (S) atoms yields a MoS2 xSe2(1- x) alloy. Our study reveals that the driving force required for the alloying of CVD-grown films with abundant vacancy-type defects is significantly lower than that required for the alloying of exfoliated films with fewer vacancies. Indeed, we show that pre-existing Se vacancies in the host MoSe2 lattice mediate the replacement of chalcogen atoms and facilitate the synthesis of MoS2 xSe2(1- x) alloys. Our DFT calculations suggest that S atoms can bind to Se vacancies and then diffuse throughout the host MoSe2 lattice via exchanging the position with Se vacancies, further supporting our proposed defect-mediated alloying mechanism. Beside native vacancy defects, we show that the existence of large-scale defects in CVD-grown MoSe2 films causes the fracture of alloys under the alloying-induced strain, while no such effect is observed in exfoliated MoSe2 films. Our study provides a deep insight into the details of the alloying mechanism and enables the synthesis of 2D alloys with tunable properties.

It is well known that an outward Marangoni convection from a low surface tension region will make the free surface of a liquid depressed. Here, we report that this established perception is only valid for thin liquid films. Using surface laser heating, we show that in deep liquids a laser beam pulls up the fluid above the free surface generating fountains with different shapes, and with decreasing liquid depth a transition from fountain to indentation with fountain-in-indentation is observed. High-speed imaging captures a transient surface depression before steady elevation is formed, and computational fluid dynamics simulations reveal the underlying flow patterns and quantify the depth-dependent and time-resolved surface deformations. Systematic investigation of the effect of laser parameters, surface tension and area of the fluid on its surface deformation further confirms that the laser fountain is a result of dynamic competition between outgoing Marangoni convection and the upward recirculation flow. Experiments and simulations also reveal that a smaller surface area can dramatically strengthen laser fountain. The discovery of laser fountain and the development of related experimental and simulation techniques have upended a century–old perception and opened up a new regime of interdisciplinary research and applications of Marangoni-induced interface phenomena.

A plasmonic modulator is a device that controls the amplitude or phase of propagating plasmons. In a pure plasmonic modulator, the presence or absence of a plasmonic pump wave controls the amplitude of a plasmonic probe wave through a channel. This control has to be mediated by an interaction between disparate plasmonic waves, typically requiring the integration of a nonlinear material. In this work, we demonstrate a 2D semiconductor nonlinear plasmonic modulator based on a WSe2 monolayer integrated on top of a lithographically defined metallic waveguide. We utilize the strong interaction between the surface plasmon polaritons (SPPs) and excitons in the WSe2 to give a 73 % change in transmission through the device. We demonstrate control of the propagating SPPs using both optical and SPP pumps, realizing a 2D semiconductor nonlinear plasmonic modulator, with an ultrafast response time of 290 fs., Plasmonic modulators have many possible applications in optical-frequency devices. Here the authors report a 2D semiconductor nonlinear plasmonic modulator enabled through strong interaction between the surface plasmon polaritons and excitons in a monolayer semiconductor integrated on top of a metallic waveguide.

We conduct ultrafast pump-probe spectroscopy in monolayer WS2 at high pump fluences to gain direct insight into interactions between a high density of carriers, defects, and phonons. We find that defects in the lattice play a major role in determining the relaxation dynamics by trapping the photoexcited carriers and acting as non-radiative recombination centers that emit phonons. In the high carrier density regime explored in our experiments, we observe substantial changes in the transient absorbance signal at unexpectedly long-time delays which we attribute to phonon-induced band gap modification. Our probe frequency dependent measurements and modeling indicate a renormalization of the bandgap by up to 23 meV. These results highlight the importance of defects and phonons for optical applications of monolayer transition metal dichalcogenides.

An upconversion from negatively charged to neutral excitons is observed in monolayer tungsten diselenide, which could provide a route for cooling two-dimensional semiconductors using lasers.

In monolayer semiconductor transition metal dichalcogenides, the exciton-phonon interaction is expected to strongly affect the photocarrier dynamics. Here, we report on an unusual oscillatory enhancement of the neutral exciton photoluminescence with the excitation laser frequency in monolayer MoSe2. The frequency of oscillation matches that of the M-point longitudinal acoustic phonon, LA(M). Oscillatory behavior is also observed in the steady-state emission linewidth and in timeresolved photoluminescence excitation data, which reveals variation with excitation energy in the exciton lifetime. These results clearly expose the key role played by phonons in the exciton formation and relaxation dynamics of two-dimensional van der Waals semiconductors., Published in npj 2D Materials and Applications. https://www.nature.com/articles/s41699-017-0035-1

Since the discovery of semiconducting monolayer transition metal dichalcogenides, a variety of experimental and theoretical studies have been carried out seeking to understand the intrinsic exciton population recombination and valley relaxation dynamics. Reports of the exciton decay time range from hundreds of femtoseconds to ten nanoseconds, while the valley depolarization time can exceed one nanosecond. At present, however, a consensus on the microscopic mechanisms governing exciton radiative and non-radiative recombination is lacking. The strong exciton oscillator strength resulting in up to ~ 20% absorption for a single monolayer points to ultrafast radiative recombination. However, the low quantum yield and large variance in the reported lifetimes suggest that non-radiative Auger-type processes obscure the intrinsic exciton radiative lifetime. In either case, the electron-hole exchange interaction plays an important role in the exciton spin and valley dynamics. In this article, we review the experiments and theory that have led to these conclusions and comment on future experiments that could complement our current understanding.

Atomically thin semiconductors, such as monolayer MoSe 2 and WSe 2 , have emerged as novel optoelectronic materials, with coupled spin-valley electronic physics and excitons that are strongly bound at room temperature. It has recently been shown that these materials can form the basis for atomically thin p-n junctions, transistors, light emitting diodes, and low threshold nanolasers. In this presentation, I will discuss optoelectronics and spin effects in heterostructures of MoSe 2 and WSe 2 , with type-II band alignment, with the lowest conduction band in the MoSe 2 layer, and the highest valence band in the WSe 2 layer. Upon optical excitation, electrons transfer to the MoSe 2 layer and holes transfer to the WSe 2 layer. Due to the strong attractive Coulomb interaction between these spatially separated layers can form interlayer excitons which have many similarities to the spatially indirect excitons of coupled GaAs quantum wells. However, unlike the coupled quantum well system, here the constituent electrons and holes are located in momentum space valleys on the edge of the Brillouin zone. The conduction and valence band valley alignment can be tuned by twist angle between layers to realize optically bright interlayer excitons with an optical selection rule allowing for optical control of the valley degree of freedom. I will discuss the dynamics and spin-valley effects of these bright interlayer excitons.

Semiconductor heterostructures are backbones for solid state based optoelectronic devices. Recent advances in assembly techniques for van der Waals heterostructures has enabled the band engineering of semiconductor heterojunctions for atomically thin optoelectronic devices. In two-dimensional heterostructures with type II band alignment, interlayer excitons, where Coulomb-bound electrons and holes are confined to opposite layers, have shown promising properties for novel excitonic devices, including a large binding energy, micron-scale in-plane drift-diffusion, and long population and valley polarization lifetime. Here, we demonstrate interlayer exciton optoelectronics based on electrostatically defined lateral p-n junctions in a MoSe2-WSe2 heterobilayer. Applying a forward bias enables the first observation of electroluminescence from interlayer excitons. At zero bias, the p-n junction functions as a highly sensitive photodetector, where the wavelength-dependent photocurrent measurement allows the direct observation of resonant optical excitation of the interlayer exciton. The resulting photocurrent amplitude from the interlayer exciton is about 200 times smaller compared to the resonant excitation of intralayer exciton. This implies that the interlayer exciton oscillator strength is two orders of magnitude smaller than that of the intralayer exciton due to the spatial separation of electron and hole to opposite layers. These results lay the foundation for exploiting the interlayer exciton in future 2D heterostructure optoelectronic devices., Nano Letters: http://pubs.acs.org/doi/pdf/10.1021/acs.nanolett.6b03398

Van der Waals heterostructures formed by two different monolayer semiconductors have emerged as a promising platform for new optoelectronic and spin/valleytronic applications. In addition to its atomically thin nature, a two-dimensional semiconductor heterostructure is distinct from its three-dimensional counterparts due to the unique coupled spin-valley physics of its constituent monolayers. Here, we report the direct observation that an optically generated spin-valley polarization in one monolayer can be transferred between layers of a two-dimensional MoSe2–WSe2 heterostructure. Using non-degenerate optical circular dichroism spectroscopy, we show that charge transfer between two monolayers conserves spin-valley polarization and is only weakly dependent on the twist angle between layers. Our work points to a new spin-valley pumping scheme in nanoscale devices, provides a fundamental understanding of spin-valley transfer across the two-dimensional interface, and shows the potential use of two-dimensional semiconductors as a spin-valley generator in two-dimensional spin/valleytronic devices for storing and processing information., Van der Waals heterostructures offer a platform for harnessing the spin-valley degree of freedom for information processing. Here, the authors transfer optically generated spin-valley polarization from one layer to another in a two-dimensional molybdenum diselenide–tungsten diselenide heterostructure.

Semiconductor technology is currently based on the manipulation of electronic charge; however, electrons have additional degrees of freedom, such as spin and valley, that can be used to encode and process information. Over the past several decades, there has been significant progress in manipulating electron spin for semiconductor spintronic devices, motivated by potential spin-based information processing and storage applications. However, experimental progress towards manipulating the valley degree of freedom for potential valleytronic devices has been limited until very recently. We review the latest advances in valleytronics, which have largely been enabled by the isolation of 2D materials (such as graphene and semiconducting transition metal dichalcogenides) that host an easily accessible electronic valley degree of freedom, allowing for dynamic control. The energy extrema of an electronic band are referred to as valleys. In 2D materials, two distinguishable valleys can be used to encode information and explore other valleytronic applications.

Single defects in monolayer WSe2 have been shown to be a new class of single photon emitters and have potential applications in quantum technologies. Whereas previous work relied on optical excitation of single defects in isolated WSe2 monolayers, in this work we demonstrate electrically driven single defect light emission by using both vertical and lateral van der Waals heterostructure devices. In both device geometries, we use few layer graphene as the source and drain and hexagonal boron nitride as the dielectric spacer layers for engineered tunneling contacts. In addition, the lateral devices utilize a split back gate design to realize an electrostatically defined p-i-n junction. At low current densities and low temperatures (∼5 K), we observe narrow spectral lines in the electroluminescence (EL) whose properties are consistent with optically excited defect bound excitons. We show that the emission originates from spatially localized regions of the sample, and the EL spectrum from single defects has a doublet with the characteristic exchange splitting and linearly polarized selection rules. All are consistent with previously reported single photon-emitters in optical measurements. Our results pave the way for on-chip and electrically driven single photon sources in two-dimensional semiconductors for quantum technology applications.

Stacking to prolong valley lifetime In the material MoSe 2 , which, like graphene, has a two-dimensional honeycomb crystal lattice, the electronic structure has two “valleys.” Electrons can be distinguished by the valley they reside in, making them act as potential information carriers. However, electrons easily lose this information by scattering into the other valley. Rivera et al. placed single layers of MoSe 2 and WSe 2 on top of each other and shone circularly polarized light on the structure. The light caused excitons—pairs of electrons and holes—to form so that the hole and electron came from the same valley but different layers. The valley-specific character of such excitons persisted far longer than would be possible in a single layer of either material. Science , this issue p. 688

We report charged exciton (trion) formation dynamics in doped monolayer transition metal dichalcogenides (TMDs), specifically molybdenum diselenide (MoSe2), using resonant two-color pump-probe spectroscopy. When resonantly pumping the exciton transition, trions are generated on a picosecond timescale through exciton-electron interaction. As the pump energy is tuned from the high energy to low energy side of the inhomogeneously broadened exciton resonance, the trion formation time increases by ~ 50%. This feature can be explained by the existence of both localized and delocalized excitons in a disordered potential and suggests the existence of an exciton mobility edge in TMDs. The quasiparticle formation and conversion processes are important for interpreting photoluminescence and photoconductivity in TMDs., 6 pages, 4 figures; accepted to PRB rapid

Nonlinear optical frequency conversion, in which optical fields interact with a nonlinear medium to produce new field frequencies, is ubiquitous in modern photonic systems. However, the nonlinear electric susceptibilities that give rise to such phenomena are often challenging to tune in a given material, and so far, dynamical control of optical nonlinearities remains confined to research labs as a spectroscopic tool. Here, we report a mechanism to electrically control second-order optical nonlinearities in monolayer WSe2, an atomically thin semiconductor. We show that the intensity of second-harmonic generation at the A-exciton resonance is tunable by over an order of magnitude at low temperature and nearly a factor of 4 at room temperature through electrostatic doping in a field-effect transistor. Such tunability arises from the strong exciton charging effects in monolayer semiconductors, which allow for exceptional control over the oscillator strengths at the exciton and trion resonances. The exciton-enhanced second-harmonic generation is counter-circularly polarized to the excitation laser, arising from the combination of the two-photon and one-photon valley selection rules that have opposite helicity in the monolayer. Our study paves the way towards a new platform for chip-scale, electrically tunable nonlinear optical devices based on two-dimensional semiconductors., Published in Nature Nanotechnology

Monolayer transition metal dichalcogenides, a new class of atomically thin semiconductors, possess optically coupled 2D valley excitons. The nature of exciton relaxation in these systems is currently poorly understood. Here, we investigate exciton relaxation in monolayer MoSe_{2} using polarization-resolved coherent nonlinear optical spectroscopy with high spectral resolution. We report strikingly narrow population pulsation resonances with two different characteristic linewidths of 1 and

Two-dimensional (2D) materials, such as graphene1, boron nitride2, and transition metal dichalcogenides (TMDs)3-5, have sparked wide interest in both device physics and technological applications at the atomic monolayer limit. These 2D monolayers can be stacked together with precise control to form novel van der Waals heterostructures for new functionalities2,6-9. One highly coveted but yet to be realized heterostructure is that of differing monolayer TMDs with type II band alignment10-12. Their application potential hinges on the fabrication, understanding, and control of bonded monolayers, with bound electrons and holes localized in individual monolayers, i.e. interlayer excitons. Here, we report the first observation of interlayer excitons in monolayer MoSe2-WSe2 heterostructures by both photoluminescence and photoluminescence excitation spectroscopy. The energy and luminescence intensity of interlayer excitons are highly tunable by an applied vertical gate voltage, implying electrical control of the heterojunction band-alignment. Using time resolved photoluminescence, we find that the interlayer exciton is long-lived with a lifetime of about 1.8 ns, an order of magnitude longer than intralayer excitons13-16. Our work demonstrates the ability to optically pump interlayer electric polarization and provokes the immediate exploration of interlayer excitons for condensation phenomena, as well as new applications in 2D light-emitting diodes, lasers, and photovoltaic devices., With Supplementary Materials

Engineering the electromagnetic environment of a nanometre-scale light emitter by use of a photonic cavity can significantly enhance its spontaneous emission rate, through cavity quantum electrodynamics in the Purcell regime. This effect can greatly reduce the lasing threshold of the emitter, providing a low-threshold laser system with small footprint, low power consumption and ultrafast modulation. An ultralow-threshold nanoscale laser has been successfully developed by embedding quantum dots into a photonic crystal cavity (PCC). However, several challenges impede the practical application of this architecture, including the random positions and compositional fluctuations of the dots, extreme difficulty in current injection, and lack of compatibility with electronic circuits. Here we report a new lasing strategy: an atomically thin crystalline semiconductor--that is, a tungsten diselenide monolayer--is non-destructively and deterministically introduced as a gain medium at the surface of a pre-fabricated PCC. A continuous-wave nanolaser operating in the visible regime is thereby achieved with an optical pumping threshold as low as 27 nanowatts at 130 kelvin, similar to the value achieved in quantum-dot PCC lasers. The key to the lasing action lies in the monolayer nature of the gain medium, which confines direct-gap excitons to within one nanometre of the PCC surface. The surface-gain geometry gives unprecedented accessibility and hence the ability to tailor gain properties via external controls such as electrostatic gating and current injection, enabling electrically pumped operation. Our scheme is scalable and compatible with integrated photonics for on-chip optical communication technologies.

Single quantum emitters (SQEs) are at the heart of quantum optics and photonic quantum information technologies. To date, all demonstrated solid-state single-photon sources are confined in three-dimensional materials. Here, we report a new class of SQEs based on excitons that are spatially localized by defects in two-dimensional tungsten-diselenide monolayers. The optical emission from these SQEs shows narrow linewidths of ~0.13 meV, about two orders of magnitude smaller than that of delocalized valley excitons. Second-order correlation measurements reveal strong photon anti-bunching, unambiguously establishing the single photon nature of the emission. The SQE emission shows two non-degenerate transitions, which are cross-linearly polarized. We assign this fine structure to two excitonic eigen-modes whose degeneracy is lifted by a large ~0.71 meV coupling, likely due to the electron-hole exchange interaction in presence of anisotropy. Magneto-optical measurements also reveal an exciton g-factor of ~8.7, several times larger than that of delocalized valley excitons. In addition to their fundamental importance, establishing new SQEs in 2D quantum materials could give rise to practical advantages in quantum information processing, such as efficient photon extraction and high integratability and scalability., Comment: 19 pages, 10 figures, including supplementary information

The electron spin state of a singly charged semiconductor quantum dot has been shown to form a suitable single qubit for quantum computing architectures with fast gate times. A key challenge in realizing a useful quantum dot quantum computing architecture lies in demonstrating the ability to scale the system to many qubits. In this Letter, we report an all optical experimental demonstration of quantum entanglement between a single electron spin confined to a single charged semiconductor quantum dot and the polarization state of a photon spontaneously emitted from the quantum dot's excited state. We obtain a lower bound on the fidelity of entanglement of $0.59\ifmmode\pm\else\textpm\fi{}0.04$, which is 84% of the maximum achievable given the timing resolution of available single photon detectors. In future applications, such as measurement-based spin-spin entanglement which does not require sub-nanosecond timing resolution, we estimate that this system would enable near ideal performance. The inferred (usable) entanglement generation rate is $3\ifmmode\times\else\texttimes\fi{}{10}^{3}\text{ }\text{ }{\mathrm{s}}^{\ensuremath{-}1}$. This spin-photon entanglement is the first step to a scalable quantum dot quantum computing architecture relying on photon (flying) qubits to mediate entanglement between distant nodes of a quantum dot network.

Optical Rabi oscillations are coherent population oscillations of a two-level system coupled by an electric dipole transition when driven by a strong nearly resonant optical field. In quantum dot structures, these measurements have typically been performed as a function of the total pulse area $\ensuremath{\int}{\ensuremath{\Omega}}_{0}(t)\phantom{\rule{0.16em}{0ex}}\mathrm{d}t$ where the pulse area varies as a function of Rabi frequency. Here, we report direct detection of the time-resolved coherent transient response of the resonance fluorescence to measure the time evolution of the optical Rabi oscillations in a single charged InAs quantum dot. We extract a decoherence rate consistent with the limit from the excited state lifetime.

We use coherent transient resonance fluorescence to follow the time evolution of Rabi oscillations in a semiconductor quantum dot. We obtain a lifetime limited decoherence rate.

Single electron spins confined to InAs quantum dots (QDs) can serve as qubits for quantum information applications. We report QD spin-photon entanglement useful for scaling a QD spin architecture via intermediate photonic qubits.

We demonstrate entanglement between an InAs quantum dot (QD) electron spin qubit and a photon. This valuable quantum information resource can be used to mediate spin-spin entanglement between distant nodes of a QD spin network.

The ability to harness spin polarization is critical for many semiconductor spin devices. It now seems that spin–orbit coupling with locally broken symmetry can enable a giant spin polarization in a semiconductor that is otherwise inversion symmetric.

The cytochrome b6f complex of oxygenic photosynthesis contains a single chlorophyll a (Chl a) molecule whose function is presently unknown. The singlet excited state of the Chl a molecule is quenched by the surrounding protein matrix, and thus the Chl a molecule in the b6f complex may serve as an exceptionally sensitive probe of the protein structure. For the first time, singlet excited-state dynamics were measured in well-diffracting crystals using femtosecond time-resolved optical pump-probe methodology. Lifetimes of the Chl a molecule in crystals of the cytochrome b6f complex having different space groups were 3-6 times longer than those determined in detergent solutions of the b6f. The observed differences in excited state dynamics may arise from small (1-1.5 A) changes in the local protein structure caused by crystal packing. The Chl a excited state lifetimes measured in the dissolved cytochrome b6f complexes from several different species are essentially the same, in spite of differences in the local amino acid sequences around the Chl a. This supports an earlier hypothesis that the short excited state lifetime of Chl a is critical for the function of the b6f complex.

A Schr¨ odinger representation approach is used to calculate the atom-field dynamics following spontaneous emission by an atom in its excited state to a superposition of its two ground-state sublevels, in the case where the frequency separation of the ground-state sublevels is large compared to the excited-state decay rate. The emitted radiation is incident on a broadband photodetector. Using a relatively simple model for the photodetector, we show how a measurement of a photo-signal leaves the atom in a coherent superposition of the two ground states. The relative phase between the two ground-state amplitudes can be interpreted in terms of the temporal phase acquired in the time interval between spontaneous emission (viewed as a quantum jump process) and detection. Alternatively, the phase can be associated with a spatial phase of the entangled atom-field system; the source atom is projected into a state containing this spatial phase when the emitted photon is detected.

We investigate the resonant nonlinear optical response of excitons in monolayer MoSe 2 , where we observe narrow population pulsation resonances. We investigate interlayer excitons in MoSe 2 -WSe 2 heterostructures, where we report long-lived valley polarization and spatial expansion.