arXiv subjects

Johannes Feist

Publications and source records attributed to Johannes Feist.

71 records · Page 4Linked to original sources

arXiv2016

Exploiting vibrational strong coupling to make an optical parametric oscillator out of a Raman laser

When the collective coupling of the rovibrational states in organic molecules and confined electromagnetic modes is sufficiently strong, the system enters into vibrational strong coupling, leading to the formation of hybrid light-matter quasiparticles. In this work we demonstrate theoretically how this hybridization in combination with stimulated Raman scattering can be utilized to widen the capabilities of Raman laser devices. We explore the conditions under which the lasing threshold can be diminished and the system can be transformed into an optical parametric oscillator. Finally, we show how the dramatic reduction of the many final molecular states into two collective excitations can be used to create an all-optical switch with output in the mid-infrared.

cond-mat.mes-hall↗

arXiv2016

Suppressing photochemical reactions with quantized light fields

Photoisomerization, i.e., a change of molecular structure after absorption of a photon, is one of the most fundamental photochemical processes. It can perform desirable functionality, e.g., as the primary photochemical event in human vision, where it stores electronic energy in the molecular structure, or for possible applications in solar energy storage and as memories, switches, and actuators; but it can also have detrimental effects, for example as an important damage pathway under solar irradiation of DNA, or as a limiting factor for the efficiency of organic solar cells. While photoisomerization can be avoided by shielding the system from light, this is of course not a viable pathway for approaches that rely on the interaction with external light (such as solar cells or solar energy storage). Here, we show that strong coupling of organic molecules to a confined light mode can be used to strongly suppress photoisomerization, and thus convert molecules that normally show fast photodegradation into photostable forms.

cond-mat.mes-hall↗

arXiv2015

Signatures of Vibrational Strong Coupling in Raman Scattering

In this Letter we analyze theoretically how the emergence of collective strong coupling between vibrational excitations and confined cavity modes affects Raman scattering processes. This work is motivated by recent experiments [Shalabney et al., Angew. Chemie 54, 7971 (2015)], which reported enhancements of up to three orders of magnitude in the Raman signal. By using different models within linear response theory, we show that the total Raman cross section is maintained constant when the system evolves from the weak-coupling limit to the strong-coupling regime. A redistribution of the Raman signal among the two polaritons is the main fingerprint of vibrational strong coupling in the Raman spectrum.

cond-mat.mes-hall↗

arXiv2015

Cavity-induced modifications of molecular structure in the strong coupling regime

In most theoretical descriptions of collective strong coupling of organic molecules to a cavity mode, the molecules are modeled as simple two-level systems. This picture fails to describe the rich structure provided by their internal rovibrational (nuclear) degrees of freedom. We investigate a first-principles model that fully takes into account both electronic and nuclear degrees of freedom, allowing an exploration of the phenomenon of strong coupling from an entirely new perspective. First, we demonstrate the limitations of applicability of the Born-Oppenheimer approximation in strongly coupled molecule-cavity structures. For the case of two molecules, we also show how dark states, which within the two-level picture are effectively decoupled from the cavity, are indeed affected by the formation of collective strong coupling. Finally, we discuss ground-state modifications in the ultra-strong coupling regime and show that some molecular observables are affected by the collective coupling strength, while others only depend on the single-molecule coupling constant.

quant-ph↗

arXiv2015

Harvesting Excitons Through Plasmonic Strong Coupling

Exciton harvesting is demonstrated in an ensemble of quantum emitters coupled to localized surface plasmons. When the interaction between emitters and the dipole mode of a metallic nanosphere reaches the strong coupling regime, the exciton conductance is greatly increased. The spatial map of the conductance matches the plasmon field intensity profile, which indicates that transport properties can be tuned by adequately tailoring the field of the plasmonic resonance. Under strong coupling, we find that pure dephasing can have detrimental or beneficial effects on the conductance, depending on the effective number of participating emitters. Finally, we show that the exciton transport in the strong coupling regime occurs on an ultrafast timescale given by the inverse Rabi splitting ($\sim10~$fs), orders of magnitude faster than transport through direct hopping between the emitters.

cond-mat.mes-hall↗

arXiv2015

Quantum theory of collective strong coupling of molecular vibrations with a microcavity mode

We develop a quantum mechanical formalism to treat the strong coupling between an electromagnetic mode and a vibrational excitation of an ensemble of organic molecules. By employing a Bloch-Redfield-Wangsness approach, we show that the influence of dephasing-type interactions, i.e., elastic collisions with a background bath of phonons, critically depends on the nature of the bath modes. In particular, for long-range phonons corresponding to a common bath, the dynamics of the "bright state" (the collective superposition of molecular vibrations coupling to the cavity mode) is effectively decoupled from other system eigenstates. For the case of independent baths (or short-range phonons), incoherent energy transfer occurs between the bright state and the uncoupled dark states. However, these processes are suppressed when the Rabi splitting is larger than the frequency range of the bath modes, as achieved in a recent experiment [Shalabney et al., Nat. Commun. 6, 5981 (2015)]. In both cases, the dynamics can thus be described through a single collective oscillator coupled to a photonic mode, making this system an ideal candidate to explore cavity optomechanics at room temperature.

cond-mat.mes-hall↗

arXiv2015

Extraordinary exciton conductance induced by strong coupling

We demonstrate that exciton conductance in organic materials can be enhanced by several orders of magnitude when the molecules are strongly coupled to an electromagnetic mode. Using a 1D model system, we show how the formation of a collective polaritonic mode allows excitons to bypass the disordered array of molecules and jump directly from one end of the structure to the other. This finding could have important implications in the fields of exciton transistors, heat transport, photosynthesis, and biological systems in which exciton transport plays a key role.

cond-mat.mes-hall↗

arXiv2014

Ab-initio nanoplasmonics: The impact of atomic structure

We present an ab-initio study of the hybridization of localized surface plasmons in a metal nanoparticle dimer. The atomic structure, which is often neglected in theoretical studies of quantum nanoplasmonics, has a strong impact on the optical absorption properties when sub-nanometric gaps between the nanoparticles are considered. We demonstrate that this influences the hybridization of optical resonances of the dimer, and leads to significantly smaller electric field enhancements as compared to the standard jellium model. In addition we show that the corrugation of the metal surface at a microscopic scale becomes as important as other well-known quantum corrections to the plasmonic response, implying that the atomic structure has to be taken into account to obtain quantitative predictions for realistic nanoplasmonic devices.

physics.optics↗

arXiv2014

Time delays for attosecond streaking in photoionization of neon

We revisit the time-resolved photoemission in neon atoms as probed by attosecond streaking. We calculate streaking time shifts for the emission of 2p and 2s electrons and compare the relative delay as measured in a recent experiment by Schultze et al. [Science 328, 1658 (2010)]. The B-spline R-matrix method is employed to calculate accurate Eisenbud-Wigner-Smith time delays from multi- electron dipole transition matrix elements for photoionization. The additional laser field-induced time shifts in the exit channel are obtained from separate, time-dependent simulations of a full streaking process by solving the time-dependent Schrödinger equation on the single-active-electron level. The resulting accurate total relative streaking time shifts between 2s and 2p emission lie well below the experimental data. We identify the presence of unresolved shake-up satellites in the experiment as a potential source of error in the determination of streaking time shifts.

physics.atom-ph↗

arXiv2014

Entanglement detection in coupled particle plasmons

When in close contact, plasmonic resonances interact and become strongly correlated. In this work we develop a quantum mechanical model, using the language of continuous variables and quantum information, for an array of coupled particle plasmons. This model predicts that when the coupling strength between plasmons approaches or surpasses the local dissipation, a sizable amount of entanglement is stored in the collective modes of the array. We also prove that entanglement manifests itself in far-field images of the plasmonic modes, through the statistics of the quadratures of the field, in what constitutes a novel family of entanglement witnesses. This protocol is so robust that it is indeed independent of whether our own model is correct. Finally, we estimate the amount of entanglement, the coupling strength and the correlation properties for a system that consists of two or more coupled nanospheres of silver, showing evidence that our predictions could be tested using present-day state-of-the-art technology.

cond-mat.mes-hall↗

arXiv2013

Nanoplasmonic near-field synthesis

The temporal response of resonances in nanoplasmonic structures typically converts an incoming few-cycle field into a much longer near-field at the spot where non-linear physical phenomena including electron emission, recollision and high-harmonic generation can take place. We show that for practically useful structures pulse shaping of the incoming pulse can be used to synthesize the plasmon-enhanced field and enable single-cycle driven nonlinear physical phenomena. Our method is demonstrated for the generation of an isolated attosecond pulse by plasmon-enhanced high harmonic generation. We furthermore show that optimal control techniques can be used even if the response of the plasmonic structure is not known a priori.

physics.atom-ph↗

arXiv2013

Photoionization of helium by attosecond pulses: extraction of spectra from correlated wave functions

We investigate the photoionization spectrum of helium by attosecond XUV pulses both in the spectral region of doubly excited resonances as well as above the double ionization threshold. In order to probe for convergence, we compare three techniques to extract photoelectron spectra from the wavepacket resulting from the integration of the time-dependent Schroedinger equation in a finite-element discrete variable representation basis. These techniques are: projection on products of hydrogenic bound and continuum states, projection onto multi-channel scattering states computed in a B-spline close-coupling basis, and a technique based on exterior complex scaling (ECS) implemented in the same basis used for the time propagation. These methods allow to monitor the population of continuum states in wavepackets created with ultrashort pulses in different regimes. Applications include photo cross sections and anisotropy parameters in the spectral region of doubly excited resonances, time-resolved photoexcitation of autoionizing resonances in an attosecond pump-probe setting, and the energy and angular distribution of correlated wavepackets for two-photon double ionization.

physics.atom-ph↗

arXiv2013

Single atom trapping and control inside a nanosize photonic crystal cavity

We analyze a possibility to trap, control and load a single atom inside a nanosize cavity formed in a photonic crystal. We consider a 1D nanobeam crystal having two nearly degenerate localized modes with mode maxima at the central air gap, forming a cavity with a mode volume <λ^{3}. For this system we found that an atom can be trapped by a mode detuned from an atomic transition and controled by the second resonant mode. We show that atomic motion can be cooled using cavity-enhanced rf Sisyphus cooling. We also discuss how an atom can be loaded inside the nanosize crystal air gap from short-wavelength optical tweezers.

quant-ph↗

arXiv2011

Attosecond streaking of correlated two-electron transitions in helium

We present fully ab initio simulations of attosecond streaking for ionization of helium accompanied by shake-up of the second electron. This process represents a prototypical case for strongly correlated electron dynamics on the attosecond timescale. We show that streaking spectroscopy can provide detailed information on the Eisenbud-Wigner-Smith time delay as well as on the infrared field dressing of both bound and continuum states. We find a novel contribution to the streaking delay that stems from the interplay of electron-electron and infrared-field interactions in the exit channel. We quantify all the contributions with attosecond precision and provide a benchmark for future experiments.

physics.atom-ph↗

arXiv2011

Probing scattering phase shifts by attosecond streaking

Attosecond streaking is one of the most fundamental processes in attosecond science allowing for a mapping of temporal (i.e. phase) information on the energy domain. We show that on the single-particle level attosecond streaking time shifts contain spectral phase information associated with the Eisenbud-Wigner-Smith (EWS) time delay, provided the influence of the streaking infrared field is properly accounted for. While the streaking phase shifts for short-ranged potentials agree with the associated EWS delays, Coulomb potentials require special care. We show that the interaction between the outgoing electron and the combined Coulomb and IR laser fields lead to a streaking phase shift that can be described classically.

physics.atom-ph↗

arXiv2011

Time-resolved photoemission by attosecond streaking: extraction of time information

Attosecond streaking of atomic photoemission holds the promise to provide unprecedented information on the release time of the photoelectron. We show that attosecond streaking phase shifts indeed contain timing (or spectral phase) information associated with the Eisenbud-Wigner-Smith time delay matrix of quantum scattering. However, this is only accessible if the influence of the streaking infrared (IR) field on the emission process is properly accounted for. The IR probe field can strongly modify the observed streaking phase shift. We show that the part of the phase shift ("time shift") due to the interaction between the outgoing electron and the combined Coulomb and IR laser fields can be described classically. By contrast, the strong initial-state dependence of the streaking phase shift is only revealed through the solution of the time-dependent Schrödinger equation in its full dimensionality. We find a time delay between the hydrogenic 2s and 2p initial states in He+ exceeding 20as for a wide range of IR intensities and XUV energies.

physics.atom-ph↗

arXiv2009

Electron correlation in two-photon double ionization of helium from attosecond to FEL pulses

We investigate the role of electron correlation in the two-photon double ionization of helium for ultrashort XUV pulses with durations ranging from a hundred attoseconds to a few femtoseconds. We perform time-dependent ab initio calculations for pulses with mean frequencies in the so-called "sequential" regime (photon energy above 54.4 eV). Electron correlation induced by the time correlation between emission events manifests itself in the angular distribution of the ejected electrons, which strongly depends on the energy sharing between them. We show that for ultrashort pulses two-photon double ionization probabilities scale non-uniformly with pulse duration depending on the energy sharing between the electrons. Most interestingly we find evidence for an interference between direct ("nonsequential") and indirect ("sequential") double photo-ionization with intermediate shake-up states, the strength of which is controlled by the pulse duration. This observation may provide a route toward measuring the pulse duration of FEL pulses.

physics.atom-ph↗