Yunhua Yao

Universal Near-Infrared and Mid-Infrared Optical Modulation for Ultrafast Pulse Generation Enabled by Colloidal Plasmonic Semiconductor Nanocrystals

Field effect relies on the nonlinear current-voltage relation in semiconductors; analogously, materials that respond nonlinearly to an optical field can be utilized for optical modulation. For instance, nonlinear optical (NLO) materials bearing a saturable absorption (SA) feature an on-off switching behavior at the critical pumping power, thus enabling ultrafast laser pulse generation with high peak power. SA has been observed in diverse materials preferably in its nanoscale form, including both gaped semiconductor nanostructures and gapless materials like graphene; while the presence of optical bandgap and small carrier density have limited the active spectral range and intensity. We show here that solution-processed plasmonic semiconductor nanocrystals exhibit superbroadband (over 400 THz) SA, meanwhile with large modulation depth (∼7 dB) and ultrafast recovery (∼315 fs). Optical modulators fabricated using these plasmonic nanocrystals enable mode-locking and Q-switching operation across the near-infrared and mid-infrared spectral region, as exemplified here by the pulsed lasers realized at 1.0, 1.5, and 2.8 μm bands with minimal pulse duration down to a few hundreds of femtoseconds. The facile accessibility and superbroadband optical nonlinearity offered by these nonconventional plasmonic nanocrystals may stimulate a growing interest in the exploiting of relevant NLO and photonic applications.

Laser polarization and phase control of up-conversion fluorescence in rare-earth ions

We theoretically and experimentally demonstrate the up-conversion fluorescence control via resonance-mediated two-photon absorption in rare-earth ions by varying both the laser polarization and phase. We show that both the laser polarization and phase can control the up-conversion fluorescence, and the up-conversion fluorescence intensity is decreased when the laser polarization changes from linear through elliptical to circular. We also show that the laser polarization will affect the control efficiency of the up-conversion fluorescence by varying the laser phase, and the circular polarization will reduce the control efficiency. Furthermore, we suggest that the control efficiency by varying the laser polarization and the effect of the laser polarization on the control efficiency by varying the laser phase can be artificially manipulated by controlling the laser spectral bandwidth. This optical control method opens a new opportunity to control the up-conversion fluorescence of rare-earth ions, which may have significant impact on the related applications of rare-earth ions.

Enhancing up-conversion luminescence of Er3+/Yb3+-codoped glass by two-color laser field excitation

Improving up-conversion luminescence efficiency of rare-earth ions is always a research hotspot because of its important applications in laser source, color display, photoelectric conversion and multiplexed biolabeling. Herein, we first utilize a combined two-color laser field with the laser wavelengths of 800 and 980 nm to further enhance the up-conversion luminescence in an Er3+/Yb3+-codoped glass sample. We show that the green up-conversion luminescence intensity by the combined two-color laser field can be greatly enhanced by comparing it with the sum of that induced by the two individual laser fields. We also show that the luminescence enhancement can be attributed to the cooperative up-conversion excitation process by the energy transfer from Yb3+ to Er3+ ions via the 980 nm laser field excitation and then the excited state absorption via the 800 nm laser field excitation. These studies present a clear physical picture for the up-conversion luminescence generation and enhancement in an Er3+/Yb3+-codoped glass sample, which are very helpful for properly designing the laser field to generate or improve the up-conversion luminescence efficiency in various lanthanide-codoped luminescent materials.

A Solution‐Processed Ultrafast Optical Switch Based on a Nanostructured Epsilon‐Near‐Zero Medium

Dynamical materials that capable of responding to optical stimuli have always been pursued for designing novel photonic devices and functionalities, of which the response speed and amplitude as well as integration adaptability and energy effectiveness are especially critical. Here we show ultrafast pulse generation by exploiting the ultrafast and sensitive nonlinear dynamical processes in tunably solution-processed colloidal epsilon-near-zero (ENZ) transparent conducting oxide (TCO) nanocrystals (NCs), of which the potential respond response speed is >2 THz and modulation depth is ~23% pumped at ~0.7 mJ/cm2, benefiting from the highly confined geometry in addition to the ENZ enhancement effect. These ENZ NCs may offer a scalable and printable material solution for dynamic photonic and optoelectronic devices.All the optical properties of materials are derived from dielectric function. In spectral region where the dielectric permittivity approaches zero, known as epsilon-near-zero (ENZ) region, the propagating light within the material attains a very high phase velocity, and meanwhile the material exhibits strong optical nonlinearity. The interplay between the linear and nonlinear optical response in these materials thus offers unprecedented pathways for all-optical control and device design. Here the authors demonstrate ultrafast all-optical modulation based on a typical ENZ material of indium tin oxide (ITO) nanocrystals (NCs), accessed by a wet-chemistry route. In the ENZ region, the authors find that the optical response in these ITO NCs is associated with a strong nonlinear character, exhibiting sub-picosecond response time (corresponding to frequencies over 2 THz) and modulation depth up to ≈160%. This large optical nonlinearity benefits from the highly confined geometry in addition to the ENZ enhancement effect of the ITO NCs. Based on these ENZ NCs, the authors successfully demonstrate a fiber optical switch that allows switching of continuous laser wave into femtosecond laser pulses. Combined with facile processibility and tunable optical properties, these solution-processed ENZ NCs may offer a scalable and printable material solution for dynamic photonic and optoelectronic devices.

Cu-Sn-S plasmonic semiconductor nanocrystals for ultrafast photonics

Here, we show that solution-processed Cu-Sn-S semiconductor nanocrystals (NCs) demonstrate a tunable localized surface plasmon resonance band in the near infrared region, where strong saturable absorption occurs. A saturable absorber based on these plasmonic NCs enables the construction of a stable mode-locked femtosecond fiber laser operating at the telecommunication band.

Realizing up-conversion fluorescence tuning in lanthanide-doped nanocrystals by femtosecond pulse shaping method

The ability to tune color output of nanomaterials is very important for their applications in laser, optoelectronic device, color display and multiplexed biolabeling. Here we first propose a femtosecond pulse shaping technique to realize the up-conversion fluorescence tuning in lanthanide-doped nanocrystals dispersed in the glass. The multiple subpulse formation by a square phase modulation can create different excitation pathways for various up-conversion fluorescence generations. By properly controlling these excitation pathways, the multicolor up-conversion fluorescence can be finely tuned. This color tuning by the femtosecond pulse shaping technique is realized in single material by single-color laser field, which is highly desirable for further applications of the lanthanide-doped nanocrystals. This femtosecond pulse shaping technique opens an opportunity to tune the color output in the lanthanide-doped nanocrystals, which may bring a new revolution in the control of luminescence properties of nanomaterials.

Femtosecond Laser-Induced Upconversion Luminescence in Rare-Earth Ions by Nonresonant Multiphoton Absorption.

The upconversion luminescence of rare-earth ions has attracted considerable interest because of its important applications in photoelectric conversion, color display, laser device, multiplexed biolabeling, and security printing. Previous studies mainly explored the upconversion luminescence generation through excited state absorption, energy transfer upconversion, and photon avalanche under the continuous wave laser excitation. Here, we focus on the upconversion luminescence generation through a nonresonant multiphoton absorption by using the intense femtosecond pulsed laser excitation and study the upconversion luminescence intensity control by varying the femtosecond laser phase and polarization. We show that the upconversion luminescence of rare-earth ions under the intense femtosecond laser field excitation is easy to be obtained due to the nonresonant multiphoton absorption through the nonlinear interaction between light and matter, which is not available by the continuous wave laser excitation in previous works. We also show that the upconversion luminescence intensity can be effectively controlled by varying the femtosecond pulsed laser phase and polarization, which can open a new technological opportunity to generate and control the upconversion luminescence of rare-earth ions and also can be further extended to the relevant application areas.

Polarization control of intermediate state absorption in resonance-mediated multi- photon absorption process

We theoretically and experimentally demonstrate the control of the intermediate state absorption in an (n + m) resonance-mediated multi-photon absorption process by the polarization-modulated femtosecond laser pulse. An analytical solution of the intermediate state absorption in a resonance-mediated multi-photon absorption process is obtained based on the time-dependent perturbation theory. Our theoretical results show that the control efficiency of the intermediate state absorption by the polarization modulation is independent of the laser intensity when the transition from the intermediate state to the final state is coupled by the single-photon absorption, but will be affected by the laser intensity when this transition is coupled by the non-resonant multi-photon absorption. These theoretical results are experimentally confirmed via a two-photon fluorescence control in (2 + 1) resonance-mediated three-photon absorption of Coumarin 480 dye and a single-photon fluorescence control in (1 + 2) resonance-mediated three-photon absorption of IR 125 dye.

Up-conversion luminescence polarization control in Er3＋-doped NaYF4 nanocrystals

We propose a femtosecond laser polarization modulation scheme to control the up-conversion (UC) luminescence in Er3+-doped NaYF4 nanocrystals dispersed in the silicate glass. We show that the UC luminescence can be suppressed when the laser polarization is changed from linear through elliptical to circular, and the higher repetition rate will yield the lower control efficiency. We theoretically analyze the physical control mechanism of the UC luminescence polarization modulation by considering on- and near-resonant two-photon absorption, energy transfer up-conversion, and excited state absorption, and show that the polarization control mainly comes from the contribution of near-resonant two-photon absorption. Furthermore, we propose a method to improve the polarization control efficiency of UC luminescence in rare-earth ions by applying a two-color femtosecond laser field.

Effect of two-color laser pulse intensity ratio on intense terahertz generation

We theoretically demonstrate the effect of the intensity ratio of the two-color laser field on the terahertz generation based on a transient photocurrent model. We show that the terahertz generation depends on the intensity ratio of the two-color laser field at a given total laser intensity, and the optimal intensity ratio for the maximum terahertz generation will decrease with the increase of the total laser intensity. We also show that the final ionization degree can be used to explain the optimal intensity ratio change at different laser intensities. Furthermore, we utilize the increasing rate of electron density and the electron drift velocity to illustrate the physical mechanism of the maximum terahertz radiation generation.