@article{ZeuschnerWangDebetal.2022, author = {Zeuschner, Steffen Peer and Wang, Xi-Guang and Deb, Marwan and Popova, Elena and Malinowski, Gregory and Hehn, Michel and Keller, Niels and Berakdar, Jamal and Bargheer, Matias}, title = {Standing spin wave excitation in Bi}, series = {Physical review : B, Condensed matter and materials physics}, volume = {106}, journal = {Physical review : B, Condensed matter and materials physics}, number = {13}, publisher = {American Physical Society}, address = {College Park}, issn = {2469-9950}, doi = {10.1103/PhysRevB.106.134401}, pages = {9}, year = {2022}, abstract = {Based on micromagnetic simulations and experimental observations of the magnetization and lattice dynamics after the direct optical excitation of the magnetic insulator Bi : YIG or indirect excitation via an optically opaque Pt/Cu double layer, we disentangle the dynamical effects of magnetic anisotropy and magneto-elastic coupling. The strain and temperature of the lattice are quantified via modeling ultrafast x-ray diffraction data. Measurements of the time-resolved magneto-optical Kerr effect agree well with the magnetization dynamics simulated according to the excitation via two mechanisms: the magneto-elastic coupling to the experimentally verified strain dynamics and the ultrafast temperature-induced transient change in the magnetic anisotropy. The numerical modeling proves that, for direct excitation, both mechanisms drive the fundamental mode with opposite phase. The relative ratio of standing spin wave amplitudes of higher-order modes indicates that both mechanisms are substantially active.}, language = {en} } @article{ZeuschnerParpiievPezeriletal.2019, author = {Zeuschner, Steffen and Parpiiev, Tymur and Pezeril, Thomas and Hillion, Arnaud and Dumesnil, Karine and Anane, Abdelmadjid and Pudell, Jan-Etienne and Willig, Lisa and R{\"o}ssle, Matthias and Herzog, Marc and von Reppert, Alexander and Bargheer, Matias}, title = {Tracking picosecond strain pulses in heterostructures that exhibit giant magnetostriction}, series = {Structural Dynamics}, volume = {6}, journal = {Structural Dynamics}, number = {2}, publisher = {AIP Publishing LLC}, address = {Melville, NY}, issn = {2329-7778}, doi = {10.1063/1.5084140}, pages = {9}, year = {2019}, abstract = {We combine ultrafast X-ray diffraction (UXRD) and time-resolved Magneto-Optical Kerr Effect (MOKE) measurements to monitor the strain pulses in laser-excited TbFe2/Nb heterostructures. Spatial separation of the Nb detection layer from the laser excitation region allows for a background-free characterization of the laser-generated strain pulses. We clearly observe symmetric bipolar strain pulses if the excited TbFe2 surface terminates the sample and a decomposition of the strain wavepacket into an asymmetric bipolar and a unipolar pulse, if a SiO2 glass capping layer covers the excited TbFe2 layer. The inverse magnetostriction of the temporally separated unipolar strain pulses in this sample leads to a MOKE signal that linearly depends on the strain pulse amplitude measured through UXRD. Linear chain model simulations accurately predict the timing and shape of UXRD and MOKE signals that are caused by the strain reflections from multiple interfaces in the heterostructure.}, language = {en} } @misc{ZeuschnerParpiievPezeriletal.2019, author = {Zeuschner, Steffen and Parpiiev, Tymur and Pezeril, Thomas and Hillion, Arnaud and Dumesnil, Karine and Anane, Abdelmadjid and Pudell, Jan-Etienne and Willig, Lisa and R{\"o}ssle, Matthias and Herzog, Marc and von Reppert, Alexander and Bargheer, Matias}, title = {Tracking picosecond strain pulses in heterostructures that exhibit giant magnetostriction}, series = {Postprints der Universit{\"a}t Potsdam : Mathematisch-naturwissenschaftliche Reihe}, journal = {Postprints der Universit{\"a}t Potsdam : Mathematisch-naturwissenschaftliche Reihe}, number = {706}, issn = {1866-8372}, doi = {10.25932/publishup-42845}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-428457}, pages = {9}, year = {2019}, abstract = {We combine ultrafast X-ray diffraction (UXRD) and time-resolved Magneto-Optical Kerr Effect (MOKE) measurements to monitor the strain pulses in laser-excited TbFe2/Nb heterostructures. Spatial separation of the Nb detection layer from the laser excitation region allows for a background-free characterization of the laser-generated strain pulses. We clearly observe symmetric bipolar strain pulses if the excited TbFe2 surface terminates the sample and a decomposition of the strain wavepacket into an asymmetric bipolar and a unipolar pulse, if a SiO2 glass capping layer covers the excited TbFe2 layer. The inverse magnetostriction of the temporally separated unipolar strain pulses in this sample leads to a MOKE signal that linearly depends on the strain pulse amplitude measured through UXRD. Linear chain model simulations accurately predict the timing and shape of UXRD and MOKE signals that are caused by the strain reflections from multiple interfaces in the heterostructure.}, language = {en} } @article{ZeuschnerMatternPudelletal.2021, author = {Zeuschner, S. P. and Mattern, M. and Pudell, Jan-Etienne and von Reppert, A. and R{\"o}ssle, M. and Leitenberger, Wolfram and Schwarzkopf, J. and Boschker, J. E. and Herzog, Marc and Bargheer, Matias}, title = {Reciprocal space slicing}, series = {Structural Dynamics}, volume = {8}, journal = {Structural Dynamics}, publisher = {AIP Publishing LLC}, address = {Melville, NY}, issn = {2329-7778}, doi = {10.1063/4.0000040}, pages = {11}, year = {2021}, abstract = {An experimental technique that allows faster assessment of out-of-plane strain dynamics of thin film heterostructures via x-ray diffraction is presented. In contrast to conventional high-speed reciprocal space-mapping setups, our approach reduces the measurement time drastically due to a fixed measurement geometry with a position-sensitive detector. This means that neither the incident (ω) nor the exit (2θ) diffraction angle is scanned during the strain assessment via x-ray diffraction. Shifts of diffraction peaks on the fixed x-ray area detector originate from an out-of-plane strain within the sample. Quantitative strain assessment requires the determination of a factor relating the observed shift to the change in the reciprocal lattice vector. The factor depends only on the widths of the peak along certain directions in reciprocal space, the diffraction angle of the studied reflection, and the resolution of the instrumental setup. We provide a full theoretical explanation and exemplify the concept with picosecond strain dynamics of a thin layer of NbO2.}, language = {en} } @misc{ZeuschnerMatternPudelletal.2021, author = {Zeuschner, S. P. and Mattern, M. and Pudell, Jan-Etienne and von Reppert, A. and R{\"o}ssle, M. and Leitenberger, Wolfram and Schwarzkopf, J. and Boschker, J. E. and Herzog, Marc and Bargheer, Matias}, title = {Reciprocal space slicing}, series = {Postprints der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe}, journal = {Postprints der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe}, number = {1137}, issn = {1866-8372}, doi = {10.25932/publishup-49976}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-499761}, pages = {13}, year = {2021}, abstract = {An experimental technique that allows faster assessment of out-of-plane strain dynamics of thin film heterostructures via x-ray diffraction is presented. In contrast to conventional high-speed reciprocal space-mapping setups, our approach reduces the measurement time drastically due to a fixed measurement geometry with a position-sensitive detector. This means that neither the incident (ω) nor the exit (2θ) diffraction angle is scanned during the strain assessment via x-ray diffraction. Shifts of diffraction peaks on the fixed x-ray area detector originate from an out-of-plane strain within the sample. Quantitative strain assessment requires the determination of a factor relating the observed shift to the change in the reciprocal lattice vector. The factor depends only on the widths of the peak along certain directions in reciprocal space, the diffraction angle of the studied reflection, and the resolution of the instrumental setup. We provide a full theoretical explanation and exemplify the concept with picosecond strain dynamics of a thin layer of NbO2.}, language = {en} } @article{ZamponiAnsarivonKorffSchmisingetal.2009, author = {Zamponi, Flavio and Ansari, Zunaira and von Korff Schmising, Clemens and Rothhardt, Philip and Zhavoronkov, Nickolai and Woerner, Michael and Elsaesser, Thomas and Bargheer, Matias and Trobitzsch-Ryll, Timo and Haschke, Michael}, title = {Femtosecond hard X-ray plasma sources with a kilohertz repetition rate}, issn = {0947-8396}, doi = {10.1007/s00339-009-5171-9}, year = {2009}, abstract = {Laser-driven plasma sources of femtosecond hard X-ray pulses have found widespread application in ultrafast X- ray diffraction. The recent development of plasma sources working at kilohertz repetition rates has allowed for diffraction experiments with strongly improved sensitivity, now revealing subtle fully reversible changes of the geometry of crystal lattices. We provide a brief review of this development and present a novel plasma source with an optimized mechanical and optical design, providing a high flux of several 10(10) photons/s at the Cu-K alpha energy of 8.04 keV and a pulse duration of a parts per thousand currency sign300 fs. First experiments, including the generation of Debye-Scherrer diffraction patterns from Si powder, demonstrate the high performance of this source.}, language = {en} } @article{WoernervonKorffSchmisingBargheeretal.2009, author = {Woerner, Michael and von Korff Schmising, Clemens and Bargheer, Matias and Zhavoronkov, Nickolai and Vrejoiu, Ionela and Hesse, Dietrich and Alexe, Marin and Elsaesser, Thomas}, title = {Ultrafast structural dynamics of perovskite superlattices}, issn = {0947-8396}, doi = {10.1007/s00339-009-5174-6}, year = {2009}, abstract = {Femtosecond x-ray diffraction provides direct insight into the ultrafast reversible lattice dynamics of materials with a perovskite structure. Superlattice (SL) structures consisting of a sequence of nanometer-thick layer pairs allow for optically inducing a tailored stress profile that drives the lattice motions and for limiting the influence of strain propagation on the observed dynamics. We demonstrate this concept in a series of diffraction experiments with femtosecond time resolution, giving detailed information on the ultrafast lattice dynamics of ferroelectric and ferromagnetic superlattices. Anharmonically coupled lattice motions in a SrRuO3/PbZr0.2Ti0.8O3 (SRO/ PZT) SL lead to a switch-off of the electric polarizations on a time scale of the order of 1 ps. Ultrafast magnetostriction of photoexcited SRO layers is demonstrated in a SRO/SrTiO3 (STO) SL.}, language = {en} } @article{WilligvonReppertDebetal.2019, author = {Willig, Lisa and von Reppert, Alexander and Deb, Marwan and Ganss, F. and Hellwig, O. and Bargheer, Matias}, title = {Finite-size effects in ultrafast remagnetization dynamics of FePt}, series = {Physical review : B, Condensed matter and materials physics}, volume = {100}, journal = {Physical review : B, Condensed matter and materials physics}, number = {22}, publisher = {American Physical Society}, address = {College Park}, issn = {2469-9950}, doi = {10.1103/PhysRevB.100.224408}, pages = {6}, year = {2019}, abstract = {We investigate the ultrafast magnetization dynamics of FePt in the L1(0) phase after an optical heating pulse, as used in heat-assisted magnetic recording. We compare continuous and nano-granular thin films and emphasize the impact of the finite size on the remagnetization dynamics. The remagnetization speeds up significantly with increasing external magnetic field only for the continuous film, where domain-wall motion governs the dynamics. The ultrafast remagnetization dynamics in the continuous film are only dominated by heat transport in the regime of high magnetic fields, whereas the timescale required for cooling is prevalent in the granular film for all magnetic field strengths. These findings highlight the necessary conditions for studying the intrinsic heat transport properties in magnetic materials.}, language = {en} } @article{vonReppertWilligPudelletal.2018, author = {von Reppert, Alexander and Willig, Lisa and Pudell, Jan-Etienne and Roessle, M. and Leitenberger, Wolfram and Herzog, Marc and Ganss, F. and Hellwig, O. and Bargheer, Matias}, title = {Ultrafast laser generated strain in granular and continuous FePt thin films}, series = {Applied physics letters}, volume = {113}, journal = {Applied physics letters}, number = {12}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/1.5050234}, pages = {5}, year = {2018}, abstract = {We employ ultrafast X-ray diffraction to compare the lattice dynamics of laser-excited continuous and granular FePt films on MgO (100) substrates. Contrary to recent results on free-standing granular films, we observe in both cases a pronounced and long-lasting out-of-plane expansion. We attribute this discrepancy to the in-plane expansion, which is suppressed by symmetry in continuous films. Granular films on substrates are less constrained and already show a reduced out-of-plane contraction. Via the Poisson effect, out-of-plane contractions drive in-plane expansion and vice versa. Consistently, the granular film exhibits a short-lived out-of-plane contraction driven by ultrafast demagnetization which is followed by a reduced and delayed expansion. From the acoustic reflections of the observed strain waves at the film-substrate interface, we extract a 13\% reduction of the elastic constants in thin 10 nm FePt films compared to bulk-like samples. (C) 2018 Author(s).}, language = {en} } @article{vonReppertSarhanSteteetal.2016, author = {von Reppert, Alexander and Sarhan, Radwan Mohamed and Stete, Felix and Pudell, Jan-Etienne and Del Fatti, N. and Crut, A. and Koetz, Joachim and Liebig, Ferenc and Prietzel, Claudia Christina and Bargheer, Matias}, title = {Watching the Vibration and Cooling of Ultrathin Gold Nanotriangles by Ultrafast X-ray Diffraction}, series = {The journal of physical chemistry : C, Nanomaterials and interfaces}, volume = {120}, journal = {The journal of physical chemistry : C, Nanomaterials and interfaces}, publisher = {American Chemical Society}, address = {Washington}, issn = {1932-7447}, doi = {10.1021/acs.jpcc.6b11651}, pages = {28894 -- 28899}, year = {2016}, abstract = {We study the vibrations of ultrathin gold nanotriangles upon optical excitation of the electron gas by ultrafast X-ray diffraction. We quantitatively measure the strain evolution in these highly asymmetric nano-objects, providing a direct estimation of the amplitude and phase of the excited vibrational motion. The maximal strain value is well reproduced by calculations addressing pump absorption by the nanotriangles and their resulting thermal expansion. The amplitude and phase of the out-of-plane vibration mode with 3.6 ps period dominating the observed oscillations are related to two distinct excitation mechanisms. Electronic and phonon pressures impose stresses with different time dependences. The nanosecond relaxation of the expansion yields a direct temperature sensing of the nano-object. The presence of a thin organic molecular layer at the nanotriangle/substrate interfaces drastically reduces the thermal conductance to the substrate.}, language = {en} } @article{vonReppertPudellKocetal.2016, author = {von Reppert, Alexander and Pudell, Jan-Etienne and Koc, A. and Reinhardt, M. and Leitenberger, Wolfram and Dumesnil, K. and Zamponi, Flavio and Bargheer, Matias}, title = {Persistent nonequilibrium dynamics of the thermal energies in the spin and phonon systems of an antiferromagnet}, series = {Structural dynamics}, volume = {3}, journal = {Structural dynamics}, publisher = {American Institute of Physics}, address = {Melville}, issn = {2329-7778}, doi = {10.1063/1.4961253}, pages = {11}, year = {2016}, abstract = {We present a temperature and fluence dependent Ultrafast X-Ray Diffraction study of a laser-heated antiferromagnetic dysprosium thin film. The loss of antiferromagnetic order is evidenced by a pronounced lattice contraction. We devise a method to determine the energy flow between the phonon and spin system from calibrated Bragg peak positions in thermal equilibrium. Reestablishing the magnetic order is much slower than the cooling of the lattice, especially around the Neel temperature. Despite the pronounced magnetostriction, the transfer of energy from the spin system to the phonons in Dy is slow after the spin-order is lost. (C) 2016 Author(s).}, language = {en} } @article{vonReppertPuddellKocetal.2016, author = {von Reppert, Alexander and Puddell, J. and Koc, A. and Reinhardt, M. and Leitenberger, Wolfram and Dumesnil, K. and Zamponi, Flavio and Bargheer, Matias}, title = {Persistent nonequilibrium dynamics of the thermal energies in the spin and phonon systems of an antiferromagnet}, series = {Structural dynamics}, volume = {3}, journal = {Structural dynamics}, publisher = {AIP Publishing LLC}, address = {Melville, NY}, issn = {2329-7778}, doi = {10.1063/1.4961253}, year = {2016}, abstract = {We present a temperature and fluence dependent Ultrafast X-Ray Diffraction study of a laser-heated antiferromagnetic dysprosium thin film. The loss of antiferromagnetic order is evidenced by a pronounced lattice contraction. We devise a method to determine the energy flow between the phonon and spin system from calibrated Bragg peak positions in thermal equilibrium. Reestablishing the magnetic order is much slower than the cooling of the lattice, especially around the N{\´e}el temperature. Despite the pronounced magnetostriction, the transfer of energy from the spin system to the phonons in Dy is slow after the spin-order is lost.}, language = {en} } @misc{vonReppertPuddellKocetal.2016, author = {von Reppert, Alexander and Puddell, J. and Koc, A. and Reinhardt, M. and Leitenberger, Wolfram and Dumesnil, K. and Zamponi, Flavio and Bargheer, Matias}, title = {Persistent nonequilibrium dynamics of the thermal energies in the spin and phonon systems of an antiferromagnet}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-98710}, pages = {11}, year = {2016}, abstract = {We present a temperature and fluence dependent Ultrafast X-Ray Diffraction study of a laser-heated antiferromagnetic dysprosium thin film. The loss of antiferromagnetic order is evidenced by a pronounced lattice contraction. We devise a method to determine the energy flow between the phonon and spin system from calibrated Bragg peak positions in thermal equilibrium. Reestablishing the magnetic order is much slower than the cooling of the lattice, especially around the N{\´e}el temperature. Despite the pronounced magnetostriction, the transfer of energy from the spin system to the phonons in Dy is slow after the spin-order is lost.}, language = {en} } @article{vonReppertMatternPudelletal.2020, author = {von Reppert, Alexander and Mattern, Maximilian and Pudell, Jan-Etienne and Zeuschner, Steffen Peer and Dumesnil, Karine and Bargheer, Matias}, title = {Unconventional picosecond strain pulses resulting from the saturation of magnetic stress within a photoexcited rare earth layer}, series = {Structural Dynamics}, volume = {7}, journal = {Structural Dynamics}, number = {024303}, publisher = {AIP Publishing LLC}, address = {Melville, NY}, issn = {2329-7778}, doi = {10.1063/1.5145315}, pages = {13}, year = {2020}, abstract = {Optical excitation of spin-ordered rare earth metals triggers a complex response of the crystal lattice since expansive stresses from electron and phonon excitations compete with a contractive stress induced by spin disorder. Using ultrafast x-ray diffraction experiments, we study the layer specific strain response of a dysprosium film within a metallic heterostructure upon femtosecond laser-excitation. The elastic and diffusive transport of energy to an adjacent, non-excited detection layer clearly separates the contributions of strain pulses and thermal excitations in the time domain. We find that energy transfer processes to magnetic excitations significantly modify the observed conventional bipolar strain wave into a unipolar pulse. By modeling the spin system as a saturable energy reservoir that generates substantial contractive stress on ultrafast timescales, we can reproduce the observed strain response and estimate the time- and space dependent magnetic stress. The saturation of the magnetic stress contribution yields a non-monotonous total stress within the nanolayer, which leads to unconventional picosecond strain pulses.}, language = {en} } @misc{vonReppertMatternPudelletal.2020, author = {von Reppert, Alexander and Mattern, Maximilian and Pudell, Jan-Etienne and Zeuschner, Steffen Peer and Dumesnil, Karine and Bargheer, Matias}, title = {Unconventional picosecond strain pulses resulting from the saturation of magnetic stress within a photoexcited rare earth layer}, series = {Postprints der Universit{\"a}t Potsdam : Mathematisch Naturwissenschaftliche Reihe}, journal = {Postprints der Universit{\"a}t Potsdam : Mathematisch Naturwissenschaftliche Reihe}, number = {899}, issn = {1866-8372}, doi = {10.25932/publishup-46935}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-469350}, pages = {15}, year = {2020}, abstract = {Optical excitation of spin-ordered rare earth metals triggers a complex response of the crystal lattice since expansive stresses from electron and phonon excitations compete with a contractive stress induced by spin disorder. Using ultrafast x-ray diffraction experiments, we study the layer specific strain response of a dysprosium film within a metallic heterostructure upon femtosecond laser-excitation. The elastic and diffusive transport of energy to an adjacent, non-excited detection layer clearly separates the contributions of strain pulses and thermal excitations in the time domain. We find that energy transfer processes to magnetic excitations significantly modify the observed conventional bipolar strain wave into a unipolar pulse. By modeling the spin system as a saturable energy reservoir that generates substantial contractive stress on ultrafast timescales, we can reproduce the observed strain response and estimate the time- and space dependent magnetic stress. The saturation of the magnetic stress contribution yields a non-monotonous total stress within the nanolayer, which leads to unconventional picosecond strain pulses.}, language = {en} } @article{TchoumbaKwamenRoessleLeitenbergeretal.2019, author = {Tchoumba Kwamen, Christelle Larodia and R{\"o}ssle, Matthias and Leitenberger, Wolfram and Alexe, Marin and Bargheer, Matias}, title = {Time-resolved X-ray diffraction study of the structural dynamics in an epitaxial ferroelectric thin Pb(Zr0.2Ti0.8)O-3 film induced by sub-coercive fields}, series = {Applied physics letters}, volume = {114}, journal = {Applied physics letters}, number = {16}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/1.5084104}, pages = {5}, year = {2019}, abstract = {The electric field-dependence of structural dynamics in a tetragonal ferroelectric lead zirconate titanate thin film is investigated under subcoercive and above-coercive fields using time-resolved X-ray diffraction. The domain nucleation and growth are monitored in real time during the application of an external field to the prepoled thin film capacitor. We propose the observed broadening of the in-plane peak width of the symmetric 002 Bragg reflection as an indicator of the domain disorder and discuss the processes that change the measured peak intensity. Subcoercive field switching results in remnant disordered domain configurations. Published under license by AIP Publishing.}, language = {en} } @misc{SteteSchossauKoopmanetal.2018, author = {Stete, Felix and Schossau, Phillip Gerald and Koopman, Wouter-Willem Adriaan and Bargheer, Matias}, title = {Size Dependence of the Coupling Strength in Plasmon-Exciton Nanoparticles}, series = {Quantum Nano-Photonics}, journal = {Quantum Nano-Photonics}, publisher = {Springer}, address = {Dordrecht}, isbn = {978-94-024-1546-9}, issn = {1871-465X}, doi = {10.1007/978-94-024-1544-5_26}, pages = {381 -- 383}, year = {2018}, abstract = {The coupling between molecular excitations and nanoparticles leads to promising applications. It is for example used to enhance the optical cross-section of molecules in surface enhanced Raman scattering, Purcell enhancement or plasmon enhanced dye lasers. In a coupled system new resonances emerge resulting from the original plasmon (ωpl) and exciton (ωex) resonances as ω±=12(ωpl+ωex)±14(ωpl-ωex)2+g2---------------√, (1) where g is the coupling parameter. Hence, the new resonances show a separation of Δ = ω+ - ω- from which the coupling strength can be deduced from the minimum distance between the two resonances, Ω = Δ(ω+ = ω-).}, language = {en} } @article{SteteSchossauBargheeretal.2018, author = {Stete, Felix and Schossau, Phillip and Bargheer, Matias and Koopman, Wouter-Willem Adriaan}, title = {Size-Dependent coupling of Hybrid Core-Shell Nanorods}, series = {The journal of physical chemistry : C, Nanomaterials and interfaces}, volume = {122}, journal = {The journal of physical chemistry : C, Nanomaterials and interfaces}, number = {31}, publisher = {American Chemical Society}, address = {Washington}, issn = {1932-7447}, doi = {10.1021/acs.jpcc.8b04204}, pages = {17976 -- 17982}, year = {2018}, abstract = {Owing to their ability of concentrating electromagnetic fields to subwavelength mode volumes, plasmonic nanoparticles foster extremely high light-matter coupling strengths reaching far into the strong-coupling regime of light matter interaction. In this article, we present an experimental investigation on the dependence of coupling strength on the geometrical size of the nanoparticle. The coupling strength for differently sized hybrid plasmon-core exciton-shell nanorods was extracted from the typical resonance anticrossing of these systems, obtained by controlled modification of the environment permittivity using layer-by-layer deposition of polyelectrolytes. The observed size dependence of the coupling strength can be explained by a simple model approximating the electromagnetic mode volume by the geometrical volume of the particle. On the basis of this model, the coupling strength for particles of arbitrary size can be predicted, including the particle size necessary to support single-emitter strong coupling.}, language = {en} } @article{SteteKoopmanBargheer2017, author = {Stete, Felix and Koopman, Wouter-Willem Adriaan and Bargheer, Matias}, title = {Signatures of strong coupling on nanoparticles}, series = {ACS Photonics}, volume = {4}, journal = {ACS Photonics}, publisher = {American Chemical Society}, address = {Washington}, issn = {2330-4022}, doi = {10.1021/acsphotonics.7b00113}, pages = {1669 -- 1676}, year = {2017}, abstract = {In the strong coupling regime, exciton and plasmon excitations are hybridized into combined system excitations. The correct identification of the coupling regime in these systems is currently debated, from both experimental and theoretical perspectives. In this article we show that the extinction spectra may show a large peak splitting, although the energy loss encoded in the absorption spectra clearly rules out the strong coupling regime. We investigate the coupling of J-aggregate excitons to the localized surface plasmon polaritons on gold nanospheres and nanorods by fine-tuning the plasmon resonance via layer-by-layer deposition of polyelectrolytes. While both structures show a characteristic anticrossing in extinction and scattering experiments, the careful assessment of the systems' light absorption reveals that strong coupling of the plasmon to the exciton is not present in the nanosphere system. In a phenomenological model of two classical coupled oscillators, a Fano-like regime causes only the resonance of the light-driven oscillator to split up, while the other one still dissipates energy at its original frequency. Only in the strong-coupling limit do both oscillators split up the frequencies at which they dissipate energy, qualitatively explaining our experimental finding.}, language = {en} } @misc{SteteKoopmanBargheer2018, author = {Stete, Felix and Koopman, Wouter-Willem Adriaan and Bargheer, Matias}, title = {Signatures of strong coupling on nanoparticles}, series = {Quantum Nano-Photonics}, journal = {Quantum Nano-Photonics}, publisher = {Springer}, address = {Dordrecht}, isbn = {978-94-024-1546-9}, issn = {1871-465X}, doi = {10.1007/978-94-024-1544-5_53}, pages = {445 -- 447}, year = {2018}, abstract = {The electromagnetic coupling of molecular excitations to plasmonic nanoparticles offers a promising method to manipulate the light-matter interaction at the nanoscale. Plasmonic nanoparticles foster exceptionally high coupling strengths, due to their capacity to strongly concentrate the light-field to sub-wavelength mode volumes. A particularly interesting coupling regime occurs, if the coupling increases to a level such that the coupling strength surpasses all damping rates in the system. In this so-called strong-coupling regime hybrid light-matter states emerge, which can no more be divided into separate light and matter components. These hybrids unite the features of the original components and possess new resonances whose positions are separated by the Rabi splitting energy h Omega. Detuning the resonance of one of the components leads to an anticrossing of the two arising branches of the new resonances omega(+) and omega(-) with a minimal separation of Omega = omega(+) - omega(-).}, language = {en} }