SearcharxivSearch

arXiv subjects

Csaba Fábri

Publications and source records attributed to Csaba Fábri.

16 recordsLinked to original sources

Nuclear Spin Isomers and the Pauli Principle in Polaritonic Chemistry

The Pauli principle has far-reaching consequences in quantum physics. Here, we investigate, for the first time, its implications, together with nuclear spin isomerism, in polaritonic chemistry. The theory is developed for a single and a few molecules as well as for an ensemble of molecules. As an explicit and detailed example we first present an accurate numerical description of a realistic situation involving two $^{14}$NH$_3$ molecules, existing as ortho and para spin isomers, in an infrared plasmonic cavity. Then, we generalize the approach for molecular ensembles using analytical considerations based on the Tavis-Cummings model and simulate the transmission spectrum of a Fabry-Pérot cavity filled with $^{14}$NH$_3$ gas using quantum mechanics. These results are directly relevant for recent gas-phase experiments studying rovibrational polaritons in molecules. Our findings undoubtedly demonstrate that the Pauli principle and nuclear spin isomerism significantly reshape collective light-matter coupling involving molecules with identical nuclei.

physics.chem-ph

Polaritons of inherently interacting molecules

We investigate the absorption spectra of molecular ensembles strongly coupled to a Fabry-Pérot cavity and establish the microscopic origin of collective polaritonic bands. We show that long-range intermolecular interactions generate a large manifold of hybrid molecular-photonic states, even without disorder, vibrations, or thermal effects. The observed polariton bands are collective envelopes of these microscopic states, making photonic and molecular spectra strongly dependent on molecular arrangement. Our findings identify long-range intermolecular interactions as a key ingredient of molecular cavity QED.

physics.chem-ph

Efficient, direct calculation of reaction rate coefficients based on a partially rearranged rovibrational Hamiltonian. A full-dimensional case study of the H$_2$ + D $\rightarrow$ HD + H reaction

It is shown that an efficient, direct, and fully quantum mechanical calculation of thermal reaction rate coefficients requires a new, partially rearranged form of the numerically-constructed exact kinetic energy part of the rovibrational Hamiltonian expressed in internal coordinates. Using this Hamiltonian and an accurate, full-dimensional potential energy surface characterizing the H$_2$ + H exchange reaction, developed by Mielke, Garrett, and Peterson (J. Chem. Phys. 2002, 116, 4142), reaction rate coefficients in the temperature range of $75-800$ K have been computed for the H$_2$ + D $\rightarrow$ HD + H reaction. The paper puts particular emphasis on the exact treatment of overall molecular rotation and on nuclear spin symmetry.

physics.chem-ph

Light-induced nonadiabatic photodissociation of the NaH molecule including electron-rotation coupling

It is well established that electronic conical intersections (CIs) in molecular systems can be induced by laser light, even in diatomic molecules. The emergence of these light-induced degeneracies leads to strong coupling among electronic, vibrational, and photonic modes, which significantly influences ultrafast nuclear dynamics. In this work, we perform pump-probe numerical simulations on the NaH molecule, considering the first three singlet electronic states- (X1Σ+(X), A1Σ+(A) and B1Π(B)) -and including several light- induced degeneracies in the theoretical model. To elucidate the ultrafast molecular dynamics, the combined effects of multiple light-induced nonadiabatic couplings and rotational motion of the nuclei, together with the situation when the electronic angular momentum projected onto the diatomic axis couples with the angular momentum of the nuclei has been studied. We then calculate key dynamical observables such as dissociation probabilities, kinetic energy release spectra, and angular distributions of the photofragments within and above the linear regime.

physics.atm-clus

Indirect probing of light-induced nonadiabatic dynamics in lossy nanocavities

Light-induced nonadiabatic effects can arise from the interaction of a molecule with the quantized electromagnetic field of a Fabry--Pérot or plasmonic nanocavity. In this context, the quantized radiation field mixes the vibrational, rotational, and electronic degrees of freedom. In this work, we investigate the photodissociation dynamics of a rotating hydrogen molecule within a lossy plasmonic nanocavity. We highlight that, due to significant cavity loss, the dynamics are governed by an infinite number of light-induced conical intersections. We also examine the dissociation dynamics of fixed-in-space molecules by neglecting rotation, employing both the Lindblad master and non-Hermitian lossy Schrödinger equations. Additionally, we incorporate the effects of rotation within the parameter range of perfect agreement using the non-Hermitian lossy Schrödinger method. Furthermore, we show that in the absence of photon losses, there is a close correspondence between the classical Floquet description and the radiation field model.

physics.atm-clus

Impact of dipole self-energy on cavity-induced nonadiabatic dynamics

The coupling of matter to the quantized electromagnetic field of a plasmonic or optical cavity can be harnessed to modify and control chemical and physical properties of molecules. In optical cavities, a term known as the dipole self-energy (DSE) appears in the Hamiltonian to assure gauge invariance. The aim of this work is twofold. First, we introduce a method, which has its own merits and complements existing methods, to compute the DSE. Second, we study the impact of the DSE on cavity-induced nonadiabatic dynamics in a realistic system. For that purpose, various matrix elements of the DSE are computed as functions of the nuclear coordinates and the dynamics of the system after laser excitation is investigated. The cavity is known to induce conical intersections between polaritons, which gives rise to substantial nonadiabatic effects. The DSE is shown to slightly affect these light-induced conical intersections and, in particular, break their symmetry.

physics.chem-ph

Coupling Polyatomic Molecules to Lossy Nanocavities: Lindblad versus Schrödinger description

The use of cavities to impact molecular structure and dynamics has become popular. As cavities, in particular plasmonic nanocavities, are lossy and the lifetime of their modes can be very short, their lossy nature must be incorporated into the calculations. The Lindblad master equation is commonly considered as an appropriate tool to describe this lossy nature. This approach requires the dynamics of the density operator and is thus substantially more costly than approaches employing the Schrödinger equation for the quantum wave function when several or many nuclear degrees of freedom are involved. In this work we compare numerically the Lindblad and Schrödinger descriptions discussed in the literature for a molecular example where the cavity is pumped by a laser. The laser and cavity properties are varied over a range of parameters. It is found that the Schrödinger description adequately describes the dynamics of the polaritons and emission signal as long as the laser intensity is moderate and the pump time is not much longer than the lifetime of the cavity mode. Otherwise, it is demonstrated that the Schrödinger description gradually fails. We also show that the failure of the Schrödinger description can often be remedied by renormalizing the wave function at every step of the time propagation. The results are discussed and analyzed.

physics.chem-ph

Impact of Cavity on Molecular Ionization Spectra

Ionization phenomena are widely studied for decades. With the advent of cavity technology, the question arises how quantum light affects molecular ionization. As the ionization spectrum is recorded from the neutral ground state, it is usually possible to choose cavities which exert negligible effect on the neutral ground state, but have significant impact on the ion and the ionization spectrum. Particularly interesting are cases where the ion exhibits conical intersections between close-lying electronic states, which gives rise to substantial nonadiabatic effects. Assuming single-molecule strong coupling, we demonstrate that vibrational modes irrelevant in the absence of cavity play a decisive role when the molecule is in the cavity. Here, dynamical symmetry breaking is responsible for the ion-cavity coupling and high symmetry enables control of the coupling via molecular orientation relative to the cavity field polarization. Significant impact on the spectrum by the cavity is found and shown to even substantially increase for less symmetric molecules.

physics.chem-ph

Classical and quantum light-induced non-adiabaticity in molecular systems

The exchange of energy between electronic and nuclear motion is the origin of non-adiabaticity and plays an important role in many molecular phenomena and processes. Conical intersections (CIs) of different electronic potential energy surfaces lead to the most singular non-adiabaticity and have been intensely investigated. The coupling of light and matter induces conical intersections which are termed light-induced conical intersections (LICIs). There are two kinds of LICIs, those induced by classical (laser) light and those by quantum light like that provided by a cavity. The present work reviews the subject of LICIs, discussing the achievements made so far. Particular attention is paid to comparing classical and quantum LICIs, their similarities and differences and their relationship to naturally occurring CIs. In contrast to natural CIs, the properties of which are dictated by nature, the properties of their light-induced counterparts are controllable by choosing the frequency and intensity (or coupling to the cavity) of the external light source. This opens the door to inducing and manipulating various kinds of non-adiabatic effects. Several examples of diatomic and polyatomic molecules are presented covering both dynamics and spectroscopy. The computational methods employed are discussed as well. To our opinion, the young field of LICIs and their impact show much future potential.

physics.chem-ph

Practical guide to the statistical mechanics of molecular polaritons

A theoretical approach aimed at the quantum statistical mechanics of a molecular ensemble coupled to a lossless cavity mode is presented. A canonical ensemble is considered and an approximate formula is devised for the Helmholtz free energy correction due to cavity-molecule coupling, which enables the derivation of experimentally measurable thermodynamic quantities. The frequency of the cavity mode is assumed to lie in the infrared range. Therefore, the cavity couples to molecular vibrations and our treatment is restricted to the electronic ground state of the molecule. The method is tested for an analytically solvable model system of one-dimensional harmonic oscillators coupled to the cavity. The performance of the approximation and its range of validity are discussed in detail. It is shown that the leading-order correction to the Helmholtz free energy is proportional to the square of the collective coupling strength. We also demonstrate that the cavity mode does not have a significant impact on the thermodynamic properties of the system in the collective ultrastrong coupling regime (the collective coupling strength is comparable to the frequency of the cavity mode).

physics.chem-ph

Radiative Emission of Polaritons Controlled by Light-Induced Geometric Phase

Polaritons - hybrid light-matter states formed in cavity - strongly change the properties of the underlying matter. In optical or plasmonic nanocavities, polaritons decay by radiative emission of the cavity, which is accessible experimentally. Due to the interaction of a molecule with the quantized radiation field, polaritons exhibit light-induced conical intersections (LICIs) which dramatically influence the nuclear dynamics of molecular polaritons. We show that ultrafast radiative emission from the lower polariton is controlled by the geometric phase imposed by the LICI. This finding provides insight into the process of emission and, furthermore, allows one to compute these signals by augmenting the Born-Oppenheimer approximation for polaritons with a geometric phase term.

physics.chem-ph

Probing Light-Induced Conical Intersections by Monitoring Multidimensional Polaritonic Surfaces

The interaction of a molecule with the quantized electromagnetic field of a nano-cavity gives rise to light-induced conical intersections between polaritonic potential energy surfaces. We demonstrate for a realistic model of a polyatomic molecule that the time-resolved ultrafast radiative emission of the cavity enables to follow both nuclear wavepacket dynamics on and nonadiabatic population transfer between polaritonic surfaces without applying a probe pulse. The latter provides an unambiguous (and in principle experimentally accessible) dynamical fingerprint of light-induced conical intersections.

physics.chem-ph

The rovibrational Aharonov-Bohm effect

Another manifestation of the Aharonov-Bohm effect is introduced to chemistry, in fact to nuclear dynamics and high-resolution molecular spectroscopy. As demonstrated, the overall rotation of a symmetric-top molecule influences the dynamics of an internal vibrational motion in a way that is analogous to the presence of a solenoid carrying magnetic flux. To a good approximation, the low-energy rovibrational energy-level structure of the quasistructural molecular ion H5+ can be understood entirely in terms of this effect.

physics.chem-ph

Exactly solvable 1D model explains the low-energy vibrational level structure of protonated methane

A new one-dimensional model is proposed for the low-energy vibrational quantum dynamics of CH5+ based on the motion of an effective particle confined to a 60-vertex graph $Γ_{60}$ with a single edge length parameter. Within this model, the quantum states of CH5+ are obtained in analytic form and are related to combinatorial properties of $Γ_{60}$. The bipartite structure of $Γ_{60}$ gives a simple explanation for curious symmetries observed in numerically exact variational calculations on CH5+.

physics.chem-ph

Born-Oppenheimer approximation in optical cavities: from success to breakdown

The coupling of a molecule and a cavity induces non-adiabaticity in the molecule which makes the description of its dynamics complicated. For polyatomic molecules, reduced-dimensional models and the use of the Born-Oppenheimer approximation (BOA) may remedy the situation. It is demonstrated that contrary to expectation, BOA may even fail in a one-dimensional model and generally expected to fail in two- or more-dimensional models due to the appearance of conical intersections induced by the cavity.

physics.chem-ph

Striking light-induced nonadiabatic fingerprint in the low-energy vibronic spectra of polyatomic molecules

Nonadiabaticity, i.e., the effect of mixing electronic states by nuclear motion, is a central phenomenon in molecular science. The strongest nonadiabatic effects arise due to the presence of conical intersections of electronic energy surfaces. These intersections are abundant in polyatomic molecules. Laser light can induce in a controlled manner new conical intersections, called light-induced conical intersections, which lead to strong nonadiabatic effects similar to those of the natural conical intersections. These effects are, however, controllable and may even compete with those of the natural intersections. In this work we show that the standard low-energy vibrational spectrum of the electronic ground state can change dramatically by inducing nonadiabaticity via a light-induced conical intersection. This generic effect is demonstrated for an explicit example by full-dimensional high-level quantum calculations using a pump-probe scheme with a moderate-intensity pump laser and a weak probe laser.

physics.chem-ph