Nonadiabatic molecular dynamics simulation of C2H22+ in a strong laser field*

Abstract

We investigate the alignment dependence of the strong laser dissociation dynamics of molecule C 2 H 2 2 + in the frame of real-time and real-space time-dependent density function theory coupled with nonadiabatic quantum molecular dynamics (TDDFT-MD) simulation. This work is based on a recent experiment study “ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene” [Wolter et al, Science 354, 308–312 (2016)]. Our simulations are in excellent agreement with the experimental data and the analysis confirms that the alignment dependence of the proton dissociation dynamics comes from the electron response of the driving laser pulse. Our results validate the ability of the TDDFT-MD method to reveal the underlying mechanism of experimentally observed and control molecular dissociation dynamics.

Non vertical ionization-dissociation model for strong IR induced dissociation dynamics of ${{D}_{2}}O^{2+}$

“…using a synchrotron light source at 57 eV. Furthermore, we discern that ( 13), ( 15), (16), and ( 18 We can summarize the dissociation yield CI, CII and CIII of 𝐷 2 𝑂 2+ from above analysis as:…”

“…The foundational concept of the SLIMIMES model is illustrated in Fig. within the duration of the laser pulse, with each fragment having the potential to be ionized during the photon-ionization-dissociation (PID) process [16,17].…”

“…The measurement and investigation of photon-induced electron-nuclei coupling dynamics, occurring on the femtosecond (fs) time scale, have long been a target of various time-resolved spectroscopies [1][2][3]. This coupling effect plays a crucial role in many strong laser-induced physics and chemistry processes, such as Photon-Induced Ionization Dissociation (PID) [4][5][6], especially in PID measurement schemes that use femtosecond (fs) strong infrared (IR) laser pulses [7][8][9][10][11][12][13][14][15][16][17].…”

“…However, fully understanding the detailed insights of PID dynamics induced by IR lasers in the molecular frame remains a challenge, as this process involves both electronic and nuclear motion. Solving the full electron and nuclei time-dependent Schrödinger equation (TDSE) is numerically unachievable so far [13][14][15][16][17]. This challenge is especially prominent for hydrogen bond dissociation, which can occur in as little as 8 to 10 fs [16,17].…”

“…Solving the full electron and nuclei time-dependent Schrödinger equation (TDSE) is numerically unachievable so far [13][14][15][16][17]. This challenge is especially prominent for hydrogen bond dissociation, which can occur in as little as 8 to 10 fs [16,17]. Within such a small time scale, the laser pulse does not end after dissociation, and the electrons of the fragments still have the possibility to further ionize to higher ionic states.…”