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Attosecond physics

Attosecond physics, also known as attophysics, or more generally attosecond science, is a branch of physics that deals with light–matter interaction phenomena wherein attosecond photon pulses are used to investigate dynamical processes in matter with unprecedented temporal resolution.

Introduction
. The period of this states superposition (1s-2p) is around 400 as. Motivation The natural time scale of electron motion in atoms, molecules, and solids is the attosecond (1 as= 10−18 s). For simplicity, consider a quantum particle in superposition between ground-level, of energy \epsilon_0 , and the first excited level, of energy \epsilon_1 : :|\Psi\rangle=c_g|\psi_g\rangle+c_e|\psi_e\rangle with c_e and c_g chosen as the square roots of the quantum probability of observing the particle in the corresponding state. : |\psi_g(t)\rangle= |0\rangle e^{-\frac{i\epsilon_0}{\hbar} t} \qquad |\psi_e(t)\rangle =|1\rangle e^{-\frac{i\epsilon_1}{\hbar}t} are the time-dependent ground |0\rangle and excited state |1\rangle respectively, with \hbar the reduced Planck constant. The expectation value of a generic hermitian and symmetric operator, \hat{P}, can be written as P(t)=\langle\Psi|\hat{P}|\Psi\rangle, as a consequence the time evolution of this observable is: :P(t)=|c_g|^2\langle0|\hat{P}|0\rangle+|c_e|^2\langle1|\hat{P}|1\rangle+2c_ec_g\langle0|\hat{P}|1\rangle\cos\left(\frac{\epsilon_1-\epsilon_0}{\hbar}t \right) While the first two terms do not depend on time, the third, instead, does. This creates a dynamic for the observable P(t) with a characteristic time, T_c, given by T_c=\frac{2\pi \hbar}{\epsilon_1-\epsilon_0}. in hydrogen atoms. The color bar indicates the angular density (orientation of the wavepacket) as a function of the polar angle from 0 to π (x-axis), at which one can find the particle, and time (y-axis). As a consequence, for energy levels in the range of \epsilon_1-\epsilon_0 \approx 10 eV, which is the typical electronic energy range in matter, Generation of attosecond pulses To generate a traveling pulse with an ultrashort time duration, two key elements are needed: bandwidth and central wavelength of the electromagnetic wave. From Fourier analysis, the more the available spectral bandwidth of a light pulse, the shorter, potentially, is its time duration. There is, however, a lower-limit in the minimum duration exploitable for a given pulse central wavelength. This limit is the optical cycle. Thus, a smaller time duration requires the use of shorter, and more energetic wavelength, even down to the soft-X-ray (SXR) region. For this reason, standard techniques to create attosecond light pulses are based on radiation sources with broad spectral bandwidths and central wavelength located in the XUV-SXR range. The most common sources that fit these requirements are free-electron lasers (FEL) and high harmonic generation (HHG) setups. Physical observables and experiments Once an attosecond light source is available, one has to drive the pulse towards the sample of interest and, then, measure its dynamics. The most suitable experimental observables to analyze the electron dynamics in matter are: • Angular asymmetry in the velocity distribution of molecular photo-fragment. • Quantum yield of molecular photo-fragments. • XUV-SXR spectrum transient absorption. • XUV-SXR spectrum transient reflectivity. • Photo-electron kinetic energy distribution. are used to image ultra-fast processes occurring in matter.|325x325px The general strategy is to use a pump-probe scheme to "image" through one of the aforementioned observables the ultra-fast dynamics occurring in the material under investigation. Few-femtosecond IR-XUV/SXR attosecond pulse pump-probe experiments As an example, in a typical pump-probe experimental apparatus, an attosecond (XUV-SXR) pulse and an intense (10^{11}-10^{14} W/cm2) low-frequency infrared pulse with a time duration of few to tens femtoseconds are collinearly focused on the studied sample. At this point, by varying the delay of the attosecond pulse, which could be pump/probe depending on the experiment, with respect to the IR pulse (probe/pump), the desired physical observable is recorded. The subsequent challenge is to interpret the collected data and retrieve fundamental information on the hidden dynamics and quantum processes occurring in the sample. This can be achieved with advanced theoretical tools and numerical calculations. By exploiting this experimental scheme, several kinds of dynamics can be explored in atoms, molecules and solids; typically light-induced dynamics and out-of-equilibrium excited states within attosecond time-resolution. == Quantum mechanics foundations ==
Quantum mechanics foundations
Attosecond physics typically deals with non-relativistic bounded particles and employs electromagnetic fields with a moderately high intensity (10^{11}-10^{14} W/cm2). This fact allows to set up a discussion in a non-relativistic and semi-classical quantum mechanics environment for light–matter interaction. Atoms Resolution of time dependent Schrödinger equation in an electromagnetic field The time evolution of a single electronic wave function in an atom, |\psi(t)\rangle is described by the Schrödinger equation (in atomic units): :\hat{H}|\psi(t)\rangle=i\dfrac{\partial}{\partial t}|\psi(t)\rangle \quad (1.0) where the light–matter interaction Hamiltonian, \hat{H} , can be expressed in the length gauge, within the dipole approximation, as: :\hat{H}=\frac{1}{2}\hat{\textbf{p}}^2+V_{C}+ \hat{\textbf{r}}\cdot\textbf{E}(t) where V_C is the Coulomb potential of the atomic species considered; \hat{\textbf{p}}, \hat{\textbf{r}} are the momentum and position operator, respectively; and \textbf{E}(t) is the total electric field evaluated in the neighbor of the atom. The formal solution of the Schrödinger equation is given by the propagator formalism: :|\psi(t)\rangle=e^{-i\int_{t_0}^{t}\hat{H}dt'}|\psi (t_0)\rangle \qquad(1.1) where |\psi (t_0)\rangle, is the electron wave function at time t=t_0. This exact solution cannot be used for almost any practical purpose. However, it can be proved, using Dyson's equations that the previous solution can also be written as: :|\psi(t)\rangle=-i\int_{t_0}^{t}dt'\Big[ e^{-i\int_{t'}^{t}\hat{H}(t)dt}\hat{H}_I(t')e^{-i\int_{t_0}^{t'}\hat{H}_0(t)dt}|\psi(t_0)\rangle \Big]+e^{-i\int_{t_0}^{t}\hat{H}_0(t)dt}|\psi(t_0)\rangle \qquad(1.2) where, :\hat{H}_0=\frac{1}{2}\hat{\textbf{p}}^2+V_{C} is the bounded Hamiltonian and :\hat{H}_I=\hat{\textbf{r}}\cdot\textbf{E}(t) is the interaction Hamiltonian. The formal solution of Eq. (1.0), which previously was simply written as Eq. (1.1), can now be regarded in Eq. (1.2) as a superposition of different quantum paths (or quantum trajectory), each one of them with a peculiar interaction time t' with the electric field. In other words, each quantum path is characterized by three steps: • An initial evolution without the electromagnetic field. This is described by the left-hand side \hat{H}_0 term in the integral. • Then, a "kick" from the electromagnetic field, \hat{H}_I(t') that "excite" the electron. This event occurs at an arbitrary time that uni-vocally characterizes the quantum path t' . • A final evolution driven by both the field and the Coulomb potential, given by \hat{H} . In parallel, you also have a quantum path that do not perceive the field at all, this trajectory is indicated by the right-hand side term in Eq. (1.2). This process is entirely time-reversible, i.e. can also occur in the opposite order. For strong-field interaction problems, where ionization may occur, one can imagine to project Eq. (1.2) in a certain continuum state (unbounded state or free state) |\textbf{p}\rangle, of momentum \textbf{p} , so that: :c_{\textbf{p}}(t)=\langle\textbf{p}|\psi(t)\rangle=-i\int_{t_0}^{t}dt'\langle \textbf{p}|e^{-i\int_{t'}^{t}\hat{H}(t)dt}\hat{H}_I(t')e^{-i\int_{t_0}^{t'}\hat{H}_0(t)dt}|{\psi(t_0)}\rangle +\langle \textbf{p} |e^{-i\int_{t_0}^{t}\hat{H}_0(t)dt}|\psi(t_0)\rangle \quad (1.3) where |c_{\textbf{p}}(t)|^2 is the probability amplitude to find at a certain time t, the electron in the continuum states |\textbf{p}\rangle. If this probability amplitude is greater than zero, the electron is photoionized. For the majority of application, the second term in (1.3) is not considered, and only the first one is used in discussions, is currently used to describe the behavior of atoms (and molecules) in intense laser fields. SFA is the starting theory for discussing both high harmonic generation and attosecond pump-probe interaction with atoms. The main assumption made in SFA is that the free-electron dynamics is dominated by the laser field, while the Coulomb potential is regarded as a negligible perturbation. This fact re-shapes equation (1.4) into: :a_{\textbf{p}}^{SFA}(t)=-i\int_{t_0}^{t}dt'\langle \textbf{p}|e^{-i\int_{t'}^{t}\hat{H}_{V}(t)dt}\hat{H}_I(t')e^{-i\int_{t_0}^{t'}\hat{H}_0(t)dt}|{\psi(t_0)}\rangle \quad (1.4) where, \hat{H}_V=\frac{1}{2}(\hat{\textbf{p}}+\textbf{A}(t))^2 is the Volkov Hamiltonian, here expressed for simplicity in the velocity gauge, with \textbf{A}(t) , \textbf{E}(t)=-\frac{\partial \textbf{A}(t)}{\partial t} , the electromagnetic vector potential. At this point, to keep the discussion at its basic level, lets consider an atom with a single energy level |0\rangle, ionization energy I_P and populated by a single electron (single active electron approximation). We can consider the initial time of the wave function dynamics as t_0=-\infty, and we can assume that initially the electron is in the atomic ground state |0\rangle. So that, :\hat{H}_0|0\rangle=-I_P|0\rangle and |\psi(t)\rangle=e^{-i\int_{-\infty}^{t'}\hat{H}_0dt}|0\rangle=e^{I_Pt'}|0\rangle Moreover, we can regard the continuum states as plane-wave functions state, \langle\textbf{r}|\textbf{p}\rangle=(2\pi)^{-\frac{3}{2}}e^{i\textbf{p}\cdot{\textbf{r}}} . This is a rather simplified assumption, a more reasonable choice would have been to use as continuum state the exact atom scattering states. The time evolution of simple plane-wave states with the Volkov Hamiltonian is given by: :\langle\textbf{p}|e^{-i\int_{t'}^{t}\hat{H}_{V}(t)dt}=\langle\textbf{p}+\textbf{A}(t)|e^{-i\int_{t'}^{t}(\textbf{p}+\textbf{A}(t))^2dt} here for consistency with Eq. (1.4) the evolution has already been properly converted into the length gauge. As a consequence, the final momentum distribution of a single electron in a single-level atom, with ionization potential I_P, is expressed as: a_{\textbf{p}}(t)^{SFA}=-i\int_{-\infty}^{t} \textbf{E}(t')\cdot \textbf{d}[\textbf{p}+\textbf{A}(t')] e^{+i(I_Pt'-S(t,t'))}dt' \quad (1.5) where, :\textbf{d}[\textbf{p}+\textbf{A}(t')]=\langle\textbf{p}+\textbf{A}(t')|\hat{\textbf{r}}|0 \rangle is the dipole expectation value (or transition dipole moment), and :S(t,t')=\int_{t'}^{t}\frac{1}{2}(\textbf{p}+\textbf{A}(t))^2dt is the semiclassical action. The result of Eq. (1.5) is the basic tool to understand phenomena like: • The high harmonic generation process, which is typically the result of strong field interaction of noble gases with an intense low-frequency pulse, • Attosecond pump-probe experiments with simple atoms. • The debate on tunneling time. Weak attosecond pulse-strong-IR-fields-atoms interactions Attosecond pump-probe experiments with simple atoms is a fundamental tool to measure the time duration of an attosecond pulse and to explore several quantum proprieties of matter. == Techniques ==
Techniques
Here are listed and discussed some of the most common techniques and approaches pursued in attosecond research centers. Metrology with photo-electron spectroscopy (FROG-CRAB) A daily challenge in attosecond science is to characterize the temporal proprieties of the attosecond pulses used in any pump-probe experiments with atoms, molecules or solids. The most used technique is based on the frequency-resolved optical gating for a complete reconstruction of attosecond bursts (FROG-CRAB). developed in 1991 for picosecond-femtosecond pulse characterization, to the attosecond field. Complete reconstruction of attosecond bursts (CRAB) is an extension of FROG and it is based on the same idea for the field reconstruction. In other words, FROG-CRAB is based on the conversion of an attosecond pulse into an electron wave-packet that is freed in the continuum by atomic photoionization, as already described with Eq.(1.7). The role of the low-frequency driving laser pulse( e.g. infra-red pulse) is to behave as gate for the temporal measurement. Then, by exploring different delays between the low-frequency and the attosecond pulse a streaking trace (or streaking spectrogram) can be obtained. The reconstruction of both the low-frequency field and the attosecond pulse from a streaking trace is typically achieved through iterative algorithms, such as: • Principal component generalized projections algorithm (PCGPA). • Volkov transform generalized projection algorithm (VTGPA). • extended ptychographic iterative engine (ePIE). == See also ==
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