Driven by functionality and purity demand for applications of inorganic nanoparticle colloids in optics, biology, and energy, their surface chemistry has become a topic of intensive research interest. Consequently, ligand-free colloids are ideal reference materials for evaluating the effects of surface adsorbates from the initial state for application-oriented nanointegration purposes. After two decades of development, laser synthesis and processing of colloids (LSPC) has emerged as a convenient and scalable technique for the synthesis of ligand-free nanomaterials in sealed environments. In addition to the high-purity surface of LSPC-generated nanoparticles, other strengths of LSPC include its high throughput, convenience for preparing alloys or series of doped nanomaterials, and its continuous operation mode, suitable for downstream processing. Unscreened surface charge of LSPC-synthesized colloids is the key to achieving colloidal stability and high affinity to biomolecules as well as support materials,...

Laser Synthesis and Processing of Colloids: Fundamentals and Applications

Preface 1. Planck's radiation law and the Einstein coefficients 2. Quantum mechanics of the atom-radiation interaction 3. Classical theory of optical fluctuations and coherence 4. Quantization of the radiation field 5. Single-mode quantum optics 6. Multimode and continuous-mode quantum optics 7. Optical generation, attenuation and amplification 8. Resonance fluorescence and light scattering 9. Nonlinear quantum optics Index

The quantum theory of light.

In light of the talent in synthesis of highly active metal and oxide catalysts, a newly emerging technique ― laser synthesis and processing in liquids (LSPC) ― is gaining increasing attention for catalytic applications, such as water splitting, fuel cells and photodegradation of organic pollutants. The advantages of using LSPC-synthesized metal catalysts have been reviewed elsewhere [Chem. Rev. 2017, 117, 3990-4113]. In this review, we discuss the current challenging issues about the material properties (surface chemistry and particle evolution) of the LAL/LPL-synthesized metal catalysts. Main focus is put on the advantages of LSPC in surfactant-free defect engineering of oxide NPs. Compared to other techniques (e.g., hydrogenation), LSPC provides a unique platform to simultaneously introduce oxygen vacancies and surface disorders to oxide (e.g., TiO2) nanomaterials, thus allowing the band gap narrowing from both conduction band (CB) and valence band (VB) directions. The defect-rich oxides have versatile uses, such as either directly applied as photocatalysts and as building blocks to construct supported, doped and ternary oxide photocatalysts for electrochemical and photocatalytic applications. The LSPC-synthesized catalysts are promising to be applied as the commercial catalysts in light of their higher activities than those of the current Pt/C and P25 TiO2 commercial catalysts.

Recent Advances in Surfactant-Free, Surface Charged and Defect-Rich Catalysts Developed by Laser Ablation and Processing in Liquids

The rapid development of the computational methods based on density functional theory, on the one hand, and of time-, energy-, and momentum-resolved spectroscopy, on the other hand, allows today an unprecedently detailed insight into the processes governing hot-electron relaxation dynamics, and, in particular, into the role of the electron-phonon coupling. Instead of focusing on the development of a particular method, theoretical or experimental, this review aims to treat the progress in the understanding of the electron-phonon coupling which can be gained from both, on the basis of recently obtained results. We start by defining several regimes of hot electron relaxation via electron-phonon coupling, with respect to the electron excitation energy. We distinguish between energy and momentum relaxation of hot electrons, and summarize, for several semiconductors of the IV and III-V groups, the orders of magnitude of different relaxation times in different regimes, on the basis of known experimental and numerical data. Momentum relaxation times of hot electrons become very short around 1 eV above the bottom of the conduction band, and such ultrafast relaxation mechanisms are measurable only in the most recent pump-probe experiments. Then, we give an overview of the recent progress in the experimental techniques allowing to obtain detailed information on the hot-electron relaxation dynamics, with the main focus on time-, energy-, and momentum-resolved photoemission experiments. The particularities of the experimental approach developed by one of us, which allows to capture time-, energy-, and momentum-resolved hot-electron distributions, as well as to measure momentum relaxation times of the order of 10 fs, are discussed. We further discuss the main advances in the calculation of the electron-phonon scattering times from first principles over the past ten years, in semiconducting materials. Ab initio techniques and efficient interpolation methods provide the possibility to calculate electron-phonon scattering times with high precision at reasonable numerical cost. We highlight the methods of analysis of the obtained numerical results, which allow to give insight into the details of the electron-phonon scattering mechanisms. Finally, we discuss the concept of hot electron ensemble which has been proposed recently to describe the hot-electron relaxation dynamics in GaAs, the applicability of this concept to other materials, and its limitations. We also mention some open problems.

https://iopscience.iop.org/article/10.1088/1361-648X/aad487/pdf

Hot electron relaxation dynamics in semiconductors: assessing the strength of the electron–phonon coupling from the theoretical and experimental viewpoints

Pulsed laser melting in liquid (PLML) has emerged as a facile approach to synthesize submicron spheres (SMSs) for various applications. Typically lasers with long pulse durations in the nanosecond regime are used. However, recent findings show that during melting the energy absorbed by the particle will be dissipated promptly after laser-matter interaction following the temperature decrease within tens of nanoseconds and hence limiting the efficiency of longer pulse widths. Here, the feasibility to utilize a picosecond laser to synthesize Ge SMSs (200~1000 nm in diameter) is demonstrated by irradiating polydisperse Ge powders in water and isopropanol. Through analyzing the educt size dependent SMSs formation mechanism, we find that Ge powders (200~1000 nm) are directly transformed into SMSs during PLML via reshaping, while comparatively larger powders (1000~2000 nm) are split into daughter SMSs via liquid droplet bisection. Furthermore, the contribution of powders larger than 2000 nm and smaller than 200 nm to form SMSs is discussed. This work shows that compared to nanosecond lasers, picosecond lasers are also suitable to produce SMSs if the pulse duration is longer than the material electron-phonon coupling period to allow thermal relaxation.

Germanium Sub-Microspheres Synthesized by Picosecond Pulsed Laser Melting in Liquids: Educt Size Effects

We develop a theory of energy relaxation in semiconductors and insulators highly excited by the long-acting external irradiation. We derive the equation for the non-equilibrium distribution function of excited electrons. The solution for this function breaks up into the sum of two contributions. The low-energy contribution is concentrated in a narrow range near the bottom of the conduction band. It has the typical form of a Fermi distribution with an effective temperature and chemical potential. The effective temperature and chemical potential in this low-energy term are determined by the intensity of carriers' generation, the speed of electron-phonon relaxation, rates of inter-band recombination, and electron capture on the defects. In addition, there is a substantial high-energy correction. This high-energy “tail” largely covers the conduction band. The shape of the high-energy “tail” strongly depends on the rate of electron-phonon relaxation but does not depend on the rates of recombination and trapping. We apply the theory to the calculation of a non-equilibrium distribution of electrons in an irradiated GaN. Probabilities of optical excitations from the valence to conduction band and electron-phonon coupling probabilities in GaN were calculated by the density functional perturbation theory. Our calculation of both parts of distribution function in gallium nitride shows that when the speed of the electron-phonon scattering is comparable with the rate of recombination and trapping then the contribution of the non-Fermi “tail” is comparable with that of the low-energy Fermi-like component. So the high-energy contribution can essentially affect the charge transport in the irradiated and highly doped semiconductors.

/pdf/electron-phonon-relaxation-and-excited-electron-distribution-420uqm09bx.pdf

Electron-phonon relaxation and excited electron distribution in gallium nitride

We propose a first-principle method for evaluations of the time-dependent electron distribution function of excited electrons in the conduction band of semiconductors. The method takes into account the excitations of electrons by external source and the relaxation to the bottom of conduction band via electron-phonon coupling. The methods permits calculations of the non-equilibrium electron distribution function, the quasi-stationary distribution function with steady-in-time source of light, the time of setting of the quasi-stationary distribution and the time of energy loss via relaxation to the bottom of conduction band. The actual calculations have been performed for titanium dioxide in the anatase structure and zinc oxide in the wurtzite structure. We find that the quasi-stationary electron distribution function for ZnO is a fermi-like curve that rises linearly with increasing excitation energy whereas the analogous curve for anatase consists of a main peak and a shoulder. The calculations demonstrate that the relaxation of excited electrons and the setting of the quasi-stationary distribution occur within the time no more than 500 fsec for ZnO and 100 fsec for anatase. 
We also discuss the applicability of the effective phonon model with energy-independent electron-phonon transition probability. We find that the model only reproduces the trends in changing of the characteristic times whereas the precision of such calculations is not high. The rate of energy transfer to phonons at the quasi-stationary electron distribution also have been evaluated and the effect of this transfer on the photocatalyses has been discussed. We found that for ZnO this rate is about 5 times less than in anatase.

Electron-phonon relaxation and excited electron distribution in zinc oxide and anatase

We propose a first-principles method for evaluations of the time-dependent electron distribution function of excited electrons in the conduction band of semiconductors. The method takes into account the excitations of electrons by an external source and the relaxation to the bottom of the conduction band via electron–phonon coupling. The methods permit calculations of the non-equilibrium electron distribution function, the quasi-stationary distribution function with a steady-in-time source of light, the time of setting of the quasi-stationary distribution and the time of energy loss via relaxation to the bottom of the conduction band. The actual calculations have been performed for titanium dioxide in the anatase structure and zinc oxide in the wurtzite structure. We find that the quasi-stationary electron distribution function has a peak near the bottom of the conduction band and a tail whose maximum energy rises linearly with increasing energy of excitation. The calculations demonstrate that the relaxation of excited electrons and the setting of the quasi-stationary distribution occur within a time of no more than 500 fs for ZnO and 100 fs for anatase. We also discuss the applicability of the effective phonon model to energy-independent electron–phonon transition probability. We find that the model only reproduces the trends in the change of the characteristic times whereas the precision of such calculations is not high. The rate of energy transfer to phonons at the quasi-stationary electron distribution also have been evaluated and the effect of this transfer on the photocatalysis has been discussed. We found that for ZnO this rate is about five times less than in anatase.

/pdf/electron-phonon-relaxation-and-excited-electron-distribution-hbd7d5hkdc.pdf

Electron-phonon relaxation and excited electron distribution in zinc oxide and anatase.

We develop a theory of energy relaxation in semiconductors and insulators highly excited by the long-acting external irradiation. We derive the equation for the non-equilibrium distribution function of excited electrons. The solution for this function breaks up into the sum of two contributions. The low-energy contribution is concentrated in a narrow range near the bottom of the conduction band. It has the typical form of a Fermi distribution with an effective temperature and chemical potential. The effective temperature and chemical potential in this low-energy term are determined by the intensity of carriers' generation, the speed of electron-phonon relaxation, rates of inter-band recombination and electron capture on the defects. In addition, there is a substantial high-energy correction. This high-energy 'tail' covers largely the conduction band. The shape of the high-energy 'tail' strongly depends on the rate of electron-phonon relaxation but does not depend on the rates of recombination and trapping. We apply the theory to the calculation of a non-equilibrium distribution of electrons in irradiated GaN. Probabilities of optical excitations from the valence to conduction band and electron-phonon coupling probabilities in GaN were calculated by the density functional perturbation theory. Our calculation of both parts of distribution function in gallium nitride shows that when the speed of electron-phonon scattering is comparable with the rate of recombination and trapping then the contribution of the non-Fermi 'tail' is comparable with that of the low-energy Fermi-like component. So the high-energy contribution can affect essentially the charge transport in the irradiated and highly doped semiconductors.

/pdf/electron-phonon-relaxation-and-excited-electron-distribution-4b3cggafqt.pdf

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Electron-phonon relaxation and excited electron distribution in gallium nitride

Electron-phonon relaxation and excited electron distribution in zinc oxide and anatase

Electron-phonon relaxation and excited electron distribution in zinc oxide and anatase.

Electron-phonon relaxation and excited electron distribution in gallium nitride