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Register a new userMolecular photodissociation enabled by ultrafast plasmon decay
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We propose a strategy for enabling photodissociation of a normally photostable molecule through coupling to a nanoparticle plasmon. The large possible coupling on the single-molecule level combined with the highly lossy nature of plasmonic modes, with lifetimes on the order of femtoseconds, opens an ultrafast decay channel for the molecule. For plasmon mode frequencies below the vertical photoexcitation energy of the molecule, the difference between excitation and emission energy is converted into vibrational energy on the molecular ground state in a Raman-like process. Under the correct conditions, this energy can be high enough to enable efficient photodissociation on the electronic ground state. We demonstrate the concept using numerical simulations of the Lindblad master equation for the hydrogen molecule in the vicinity of an aluminum nanoparticle, and explore the photodissociation efficiency as a function of various system parameters.
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Photodissociation is the dominant removal process of molecules in any region exposed to intense ultraviolet (UV) radiation. This includes diffuse and translucent interstellar clouds, dense photon-dominated regions, high velocity shocks, the surface layers of protoplanetary disks, and cometary and exoplanetary atmospheres. The rate of photodissociation depends on the cross sections for absorption into a range of excited electronic states, as well as on the intensity and shape of the radiation field at each position into the region of interest. Thus, an acccurate determination of the photodissociation rate of even a simple molecule like water or carbon monoxide involves many detailed considerations ranging from its electronic structure to its dissociation dynamics and the specifics of the radiation field that the molecule is exposed to. In this review chapter, each of these steps in determining photodissociation rates is discussed systematically and examples are provided.
We investigate the question whether Michelson type interferometry is possible if the role of the beam splitter is played by a spontaneous process. This question arises from an inspection of trajectories of atoms bouncing inelastically from an evanescent-wave (EW) mirror. Each final velocity can be reached via two possible paths, with a {it spontaneous} Raman transition occurring either during the ingoing or the outgoing part of the trajectory. At first sight, one might expect that the spontaneous character of the Raman transfer would destroy the coherence and thus the interference. We investigated this problem by numerically solving the Schrodinger equation and applying a Monte-Carlo wave-function approach. We find interference fringes in velocity space, even when random photon recoils are taken into account.
Ultrafast electron diffraction and time-resolved serial crystallography are the basis of the ongoing revolution in capturing at the atomic level of detail the structural dynamics of molecules. However, most experiments employ the classical ball-and-stick depictions, and the information of molecular quantum states, such as the density matrix, is missing. Here, we introduce a framework for the preparation and ultrafast coherent diffraction from rotational wave packets of molecules, and we establish a new variant of quantum state tomography for ultrafast electron diffraction to characterize the molecular quantum states. The ability to reconstruct the density matrix of molecules of arbitrary degrees of freedom will provide us with an unprecedentedly clear view of the quantum states of molecules, and enable the visualization of effects dictated by the quantum dynamics of molecules.
We use (1+1$$) resonance-enhanced multiphoton photodissociation (REMPD) to detect the population in individual rovibronic states of trapped HfF$^+$ with a single-shot absolute efficiency of 18%, which is over 200 times better than that obtained with fluorescence detection. The first photon excites a specific rotational level to an intermediate vibronic band at 35,000-36,500 cm$^{-1}$, and the second photon, at 37,594 cm$^{-1}$ (266 nm), dissociates HfF$^+$ into Hf$^+$ and F. Mass-resolved time-of-flight ion detection then yields the number of state-selectively dissociated ions. Using this method, we observe rotational-state heating of trapped HfF$^+$ ions from collisions with neutral Ar atoms. Furthermore, we measure the lifetime of the $^3Delta_1$ $v=0,, J=1$ state to be 2.1(2) s. This state will be used for a search for a permanent electric dipole moment of the electron.
We address the feasibility of imaging geometric and orbital structure of a polyatomic molecule on an attosecond time-scale using the laser induced electron diffraction (LIED) technique. We present numerical results for the highest molecular orbitals of the CO2 molecule excited by a near infrared few-cycle laser pulse. The molecular geometry (bond-lengths) is determined within 3% of accuracy from a diffraction pattern which also reflects the nodal properties of the initial molecular orbital. Robustness of the structure determination is discussed with respect to vibrational and rotational motions with a complete interpretation of the laser-induced mechanisms.
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