Identifying Strong-Field Effects in Indirect Photofragmentation Reactions

Abstract

Exploring molecular breakup processes induced by light-matter interactions has both fundamental and practical implications. However, it remains a challenge to elucidate the underlying reaction mechanism in the strong field regime, where the potentials of the reactant are modified dramatically. Here we perform a theoretical analysis combined with a time-dependent wavepacket calculation to show how a strong ultrafast laser field affects the photofragment products. As an example, we examine the photochemical reaction of breaking up the molecule NaI into the neutral atoms Na and I, which due to inherent nonadiabatic couplings are indirectly formed in a stepwise fashion via the reaction intermediate NaI*. By analyzing the angular dependencies of fragment distributions, we are able to identify the reaction intermediate NaI* from the weak to the strong field-induced nonadiabatic regimes. Furthermore, the energy levels of NaI* can be extracted from the quantum interference patterns of the transient photofragment momentum distribution.

Direct Signatures of Light-Induced Conical Intersections on the Field-Dressed Spectrum of Na2

“…Numerous theoretical and experimental studies have confirmed that LICIs have noticeable impact on different dynamical properties (like molecular alignment, photodissociation probability, etc...). [14][15][16][17][18][19] Furthermore, a strong effect in the angular distribution of the photofragments has been revealed that serves as a direct signature of the LICI. 18 The first experimental observation of LICIs in diatomic molecules was made by Bucksbaum et al.…”

Several recent developments in estimation and robust control of quantum systems

“…Since the computational complexity of quantum system identification algorithm usually exponentially increases with the number of qubits, it is expected to develop more efficient identification algorithms for quantum parameter identification. Other new directions for future research include the mechanism identification of physical process [38] and the identification of quantum networks [39], [40] where the network topology could be taken advantaged of.…”

Quantum Hamiltonian Identifiability via a Similarity Transformation Approach and Beyond

“…For Example 1,(14) is already in the Kalman canonical form and the minimal subsystem isẋ 1 = θ 1 x 1 + u, y = x 1 . Hence, θ 1 is identifiable and θ 2 is unidentifiable.…”