From 7190ebedfd8854782a5f413a2aab09d2abf3ca7f Mon Sep 17 00:00:00 2001 From: Felipe Herrera Date: Thu, 19 Dec 2024 11:31:09 -0300 Subject: [PATCH] updated Thu program and added Fri talk and speaker files --- _layouts/program.html | 201 ++++++++++++++---- .../{Annette Carroll.md => AnnetteCarroll.md} | 0 _speakers/ConstanzaToninelli.md | 2 +- _speakers/DavidLeitner copy.md | 7 + _speakers/FelipeRecabal.md | 6 + _speakers/HerbertDiaz.md | 6 + .../{MattSheldon.md => MatthewSheldon.md} | 0 _speakers/MichaelShatruk.md | 6 + _speakers/MichelineSoley.md | 7 + _speakers/RuthTichauer.md | 7 + _speakers/josesanzvicario.md | 7 + _talks/AnnetteCarroll.md | 13 ++ _talks/constanzatoninelli.md | 26 +++ _talks/davidleitner.md | 18 ++ _talks/dennisclougherty.md | 19 ++ _talks/feliperecabal.md | 24 +-- _talks/giacomovaltolina.md | 18 +- _talks/herbertdiaz.md | 9 + _talks/janetanders.md | 21 ++ _talks/josesanzvicario.md | 15 ++ _talks/marissaweichman.md | 21 +- _talks/markusraschke.md | 21 +- _talks/matthewsheldon.md | 18 ++ _talks/michaelshatruk.md | 12 ++ _talks/michelinesoley.md | 17 ++ _talks/niclasmueller.md | 18 ++ _talks/ruthtichauer.md | 46 ++-- _talks/taoli.md | 17 ++ 28 files changed, 462 insertions(+), 120 deletions(-) rename _speakers/{Annette Carroll.md => AnnetteCarroll.md} (100%) create mode 100644 _speakers/DavidLeitner copy.md create mode 100644 _speakers/FelipeRecabal.md create mode 100644 _speakers/HerbertDiaz.md rename _speakers/{MattSheldon.md => MatthewSheldon.md} (100%) create mode 100644 _speakers/MichaelShatruk.md create mode 100644 _speakers/MichelineSoley.md create mode 100644 _speakers/RuthTichauer.md create mode 100644 _speakers/josesanzvicario.md create mode 100644 _talks/AnnetteCarroll.md create mode 100644 _talks/constanzatoninelli.md create mode 100644 _talks/davidleitner.md create mode 100644 _talks/dennisclougherty.md create mode 100644 _talks/herbertdiaz.md create mode 100644 _talks/janetanders.md create mode 100644 _talks/josesanzvicario.md create mode 100644 _talks/matthewsheldon.md create mode 100644 _talks/michaelshatruk.md create mode 100644 _talks/michelinesoley.md create mode 100644 _talks/niclasmueller.md create mode 100644 _talks/taoli.md diff --git a/_layouts/program.html b/_layouts/program.html index e401499..046ae24 100644 --- a/_layouts/program.html +++ b/_layouts/program.html @@ -580,49 +580,178 @@

Thursday 19

-
+ + +
  • + 09:40 - 10:00 +
    -
  • - 14:00 - 17:00 + +
    Non-canonical steady state of two coupled oscillators in the strong coupling regime
    +     + +
    Felipe Recabal
    +     + +
    • - -
    Invited and Contributed Talks
    -     - - +
  • + 10:00 - 10:40 +
    + + +
    Towards quantum control of complex cold molecules inside a cavity
    +     + +
    Giacomo Valtolina
    +     +
    +
    • + +
  • + 10:40 - 11:20 +
    Coffee Break
    +
    • + + +
  • + 11:20 - 12:00 +
    + + +
    Organic Molecules in Solids for Photonic Quantum Technologies
    +     + +
    Costanza Toninelli
    +     +
    +
    • + +
  • + 12:00 - 12:40 +
    + + +
    Impact of system-bath coupling on a quantum system's steady state
    +     + +
    Janet Anders
    +     +
    +
    • + +
  • + 12:40 - 14:00 +
    Lunch Break
    +
    • + + +
  • + 14:00 - 14:40 +
    + + +
    Plasmonic Platforms for Polaritonic Chemistry
    +     + +
    Matthew Sheldon
    +     +
    +
    • + + +
  • + 14:40 - 15:00 +
    + + +
    High-Symmetry Lanthanide Complexes as Clock-Transition Qubits
    +     + +
    Michael Shatruk
    +     +
    +
    • + + +
  • + 15:00 - 15:20 +
    + + +
    Variational Quantum Eigensolver for Estimating the Equilibrium Configuration of Molecules
    +     + +
    Herbert Díaz
    +     +
    +
    • + +
  • + 15:20 - 16:00 +
    Coffee Break
    +
    • + + + +
  • + 16:00 - 16:40 +
    + + +
    A Tale of Two Methods for Simulating Molecular Polaritons
    +     + +
    Tao Li
    +     +
    +
    • + + +
  • + 16:40 - 17:00 +
    + + +
    Variational approach to atom-membrane dynamics
    +     + +
    Dennis Clougherty
    +     +
    +
    • + + + +
  • + 17:00 - 17:20 +
    + + +
    Modelling Light-Matter Interactions with Atomic Resolution
    +     + +
    Ruth Tichauer
    +     +
    +
  • - 18:20 - 20:00 -
    Conference Dinner
    + 18:30 - 20:00 +
    Conference Dinner
    • diff --git a/_speakers/Annette Carroll.md b/_speakers/AnnetteCarroll.md similarity index 100% rename from _speakers/Annette Carroll.md rename to _speakers/AnnetteCarroll.md diff --git a/_speakers/ConstanzaToninelli.md b/_speakers/ConstanzaToninelli.md index 55a5c1e..a655070 100644 --- a/_speakers/ConstanzaToninelli.md +++ b/_speakers/ConstanzaToninelli.md @@ -1,6 +1,6 @@ --- name: Constanza Toninelli -first_name: Constanza +first_name: Costanza last_name: Toninelli asociation: University of Florence status: invited diff --git a/_speakers/DavidLeitner copy.md b/_speakers/DavidLeitner copy.md new file mode 100644 index 0000000..717ff99 --- /dev/null +++ b/_speakers/DavidLeitner copy.md @@ -0,0 +1,7 @@ +--- +name: Dennis Clougherty +first_name: Dennis +last_name: Clougherty +asociation: University of Vermont +#status: invited +--- diff --git a/_speakers/FelipeRecabal.md b/_speakers/FelipeRecabal.md new file mode 100644 index 0000000..46964e0 --- /dev/null +++ b/_speakers/FelipeRecabal.md @@ -0,0 +1,6 @@ +--- +name: Felipe Recabal +first_name: Felipe +last_name: Recabal +asociation: Universidad de Santiago de Chile +--- \ No newline at end of file diff --git a/_speakers/HerbertDiaz.md b/_speakers/HerbertDiaz.md new file mode 100644 index 0000000..48717bd --- /dev/null +++ b/_speakers/HerbertDiaz.md @@ -0,0 +1,6 @@ +--- +name: Herbert Diaz +first_name: Herbert +last_name: Díaz +asociation: Pontificia Universidad Católica de Chile +--- \ No newline at end of file diff --git a/_speakers/MattSheldon.md b/_speakers/MatthewSheldon.md similarity index 100% rename from _speakers/MattSheldon.md rename to _speakers/MatthewSheldon.md diff --git a/_speakers/MichaelShatruk.md b/_speakers/MichaelShatruk.md new file mode 100644 index 0000000..511c2f1 --- /dev/null +++ b/_speakers/MichaelShatruk.md @@ -0,0 +1,6 @@ +--- +name: Michael Shatruk +first_name: Michael +last_name: Shatruk +asociation: Florida State University +--- diff --git a/_speakers/MichelineSoley.md b/_speakers/MichelineSoley.md new file mode 100644 index 0000000..485d669 --- /dev/null +++ b/_speakers/MichelineSoley.md @@ -0,0 +1,7 @@ +--- +name: Micheline Soley +first_name: Micheline +last_name: Soley +asociation: University of Wisconsin-Madison +#status: invited +--- diff --git a/_speakers/RuthTichauer.md b/_speakers/RuthTichauer.md new file mode 100644 index 0000000..373ca59 --- /dev/null +++ b/_speakers/RuthTichauer.md @@ -0,0 +1,7 @@ +--- +name: Ruth Tichauer +first_name: Ruth +last_name: Tichahuer +asociation: Universidad Autónoma de Madrid +#status: invited +--- \ No newline at end of file diff --git a/_speakers/josesanzvicario.md b/_speakers/josesanzvicario.md new file mode 100644 index 0000000..4ebf117 --- /dev/null +++ b/_speakers/josesanzvicario.md @@ -0,0 +1,7 @@ +--- +name: Jose Sanz-Vicario +first_name: José Luis +last_name: Sanz-Vicario +asociation: Universidad de Antioquia +# status: invited +--- \ No newline at end of file diff --git a/_talks/AnnetteCarroll.md b/_talks/AnnetteCarroll.md new file mode 100644 index 0000000..8e2d62d --- /dev/null +++ b/_talks/AnnetteCarroll.md @@ -0,0 +1,13 @@ +--- +name: Tunable Spin Dynamics with Ultracold Polar Molecules +speakers: + - Annette Carroll +categories: + - Talk +--- + +Ultracold molecules enable exploration of many-body physics due to their highly tunable dipolar interactions. Here, I will review our recent observations of out-of-equilibrium spin dynamics with polar molecules. With spin encoded in the lowest rotational states of the molecules, we realized a generalized t-J model with dipolar interactions [1]. We explored the role of Ising and spin-exchange couplings tuned with dc electric fields and the eLect of motion regulated by optical lattices on Ramsey contrast decay. Theoretical understanding of the experimental measurements will also be discussed. Further, we realized XXZ spin models with Floquet engineering [2] and verified that they produced similar dynamics as those controlled by dc electric fields. We additionally used Floquet engineering to realize a two-axis twisting Hamiltonian, inaccessible with static fields, and studied its mean-field dynamics. This work sets the stage for future explorations of exotic spin Hamiltonians with the tunability of molecular platforms. + +[1] A. N. Carroll et al., Observation of Generalized T-J Spin Dynamics with Tunable Dipolar Interactions, arXiv:2404.18916. + +[2] C. Miller, A. N. Carroll, J. Lin, H. Hirzler, H. Gao, H. Zhou, M. D. Lukin, and J. Ye, Two-Axis Twisting Using Floquet-Engineered XYZ Spin Models with Polar Molecules, Nature (2024). \ No newline at end of file diff --git a/_talks/constanzatoninelli.md b/_talks/constanzatoninelli.md new file mode 100644 index 0000000..f2d4380 --- /dev/null +++ b/_talks/constanzatoninelli.md @@ -0,0 +1,26 @@ +--- +name: Organic Molecules in Solids for Photonic Quantum Technologies +speakers: + - Constanza Toninelli +categories: + - Talk +--- + +In this contribution, the generation of quantum states of light from single molecules is discussed, tailored to multiple and diverse applications. We will focus on the use of polycyclic aromatic hydrocarbons (PAH), embedded in host matrices [1]. These molecules, due to their small size and well-defined properties, serve as nanoscopic sensors for pressure, strain, temperature, and various fields. The talk discusses recent advancements in coupling single PAH molecules to photonic structures to enhance and control their interaction with light [2]. Notably, two-photon interference experiments between photons emitted by diLerent molecules on the same chip are presented, addressing a fundamental challenge in solid-state platforms for photonic quantum technologies [3]. The experiment relies on multiple milestones, including addressing several molecules simultaneously as on-demand single-photon sources [4], independently tuning their frequencies optically [5,6], and conducting real-time measurements of two-photon interference [3,7]. Additionally, the presentation explores the use of organic molecules as nanoscopic thermal sensors, enabling semi- invasive local temperature measurements in a temperature range (3 K to 30 K) unattainable by most commercial technologies [8]. These results oLer insights into the local phononic environment in complex structures and an unexplored temperature regime. Finally, we will comment on the new prospects of using single molecules as interfaces between spin, optical and mechanical degrees of freedom. + + +[1] C. Toninelli et al., Nat. Mat. 20, (2021) + +[2] M. Colautti et al., Ad.Q.Tech. 3, (2020) + +[3] R. Duquennoy et al., Optica 9, 731-737, (2022) + +[4] P. Lombardi et al., Ad.Q.Tec. 3, (2020) + +[5] M. Colautti, et al., ACS Nano 14, 13584−13592 (2020) + +[6] R. Duquennoy et al., ACS Nano18, 32508−32516 (2024) + +[7] R. Duquennoy et al., Phys. Rev. Research 5, 023191 (2023) + +[8] V. Esteso et al., Phys. Rev. X Quantum 4, 040314 (2023). \ No newline at end of file diff --git a/_talks/davidleitner.md b/_talks/davidleitner.md new file mode 100644 index 0000000..85c95af --- /dev/null +++ b/_talks/davidleitner.md @@ -0,0 +1,18 @@ +--- +name: Quantum ergodicity and energy flow in molecules +speakers: + - David Leitner +categories: + - Talk +--- + +Under what conditions does a molecule thermalize under its own internal dynamics, and if it does how long does it take? I will discuss a theoretical framework, local random matrix theory, that establishes criteria for quantum ergodicity and energy flow in the vibrational state space of large molecules. I will also discuss some of the ways in which both limitations to and the rate of energy flow in the vibrational state space impact the kinetics of conformational isomerization in gas and condensed phase [1], reactions involving molecules attached to plasmonic nanoparticles [2], as well as thermal conductance of molecular junctions [3], which can now be measured for single molecules [4]. Comparison with results of a variety of experiments will be discussed. + + +[1.] Leitner, D. M. Quantum ergodicity and energy flow in molecules. Adv. Phys. 2015, 64, 445 - 517. + +[2.] Poudel, H.; Shaon, P. H.; Leitner, D. M. Vibrational Energy Flow in Molecules Attached to Plasmonic Nanoparticles. J. Phys. Chem. C 2024, 128, 8628 - 8636. + +[3.] Reid, K. M.; Pandey, H. D.; Leitner, D. M. Elastic and inelastic contributions to thermal transport between chemical groups and thermal rectification in molecules. J. Phys. Chem. C 2019, 6256 - 6264. + +[4.] Cui, L.; Hur, S.; Zkbar, Z. A.; Klöckner, J. C.; Jeong, W.; Pauly, F.; Jang, S.-Y.; Reddy, P.; Meyhofer, E. Thermal conductance of single-molecule junctions. Nature 2019, 572, 628 - 633. \ No newline at end of file diff --git a/_talks/dennisclougherty.md b/_talks/dennisclougherty.md new file mode 100644 index 0000000..b2f477e --- /dev/null +++ b/_talks/dennisclougherty.md @@ -0,0 +1,19 @@ +--- +name: Variational approach to atom-membrane dynamics +speakers: + - Dennis Clougherty +categories: + - Talk +--- +The adsorption of cold atoms to a surface differs in many ways from the adsorption of atoms at higher energies. It has been established both theoretically [1] and experimentally [2] that the adsorption rate of cold atoms can be dramatically suppressed in comparison to rates at higher energies by two quantum mechanical effects: (1) quantum reflection of the cold atoms away from the surface, and (2) a phonon orthogonality catastrophe [3] resulting from the surface displacement that accompanies adsorption. The first effect is a single particle phenomenon that depends on the wave mechanics of the cold atoms; the second effect is a many-body phenomenon that results from the behavior of the phonon matrix element between the initial and final states of the surface. In the most extreme case of adsorption on a 2D material, it has been proposed that this phonon reduction factor can completely suppress cold atom adsorption [4]. + +A time-dependent, nonperturbative description of phonon-assisted cold atom adsorption on a membrane will be presented. Using the Dirac-Frenkel variational principle, closed-form expressions for adsorption rates can be obtained. One strength of this method is that the case of intermediate atom-phonon coupling can be treated where the adsorption rate is found to change discontinuously with atom-phonon coupling strength at low membrane temperatures. The framework presented can be customized in a straightforward way to describe a variety of reactions in the quantum regime. Possible applications of these results to emerging quantum technologies will also be discussed. + + +[1] Dennis P. Clougherty and W. Kohn, Phys. Rev. B, 46, 4921 (1992). + +[2] I. A. Yu, J. M. Doyle, J. C. Sandberg, C. L. Cesar, D. Kleppner, and T. J. Greytak, Phys. Rev. Lett. 71, 1589 (1993). + +[3] Dennis P. Clougherty and Yanting Zhang, Phys. Rev. Lett. 109, 120401 (2012). + +[4] Dennis P. Clougherty, Phys. Rev. B, 96, 235404 (2017); Sanghita Sengupta and Dennis P. Clougherty, J. Phys.: Conf. Ser., 1148, 012007 (2018). diff --git a/_talks/feliperecabal.md b/_talks/feliperecabal.md index 3d4448b..dd7271f 100644 --- a/_talks/feliperecabal.md +++ b/_talks/feliperecabal.md @@ -1,28 +1,16 @@ --- -name: Driven-dissipative change transport in small networks; negative conductance and light-induced currents +name: Non-canonical steady state of two coupled oscillators in the strong coupling regime speakers: - Felipe Recabal categories: - Talk --- -Felipe Recabal (a) and Felipe Herrera (a,b) -(a) Department of Physics, Universidad de Santiago de Chile, Santiago, Chile +In a previous work, we describe the suppression of reaction rate inside a cavity where the electromagnetic vacuum is in strong coupling with an ensemble of molecule [1]. We model the system through a master equation where the local-Lindblad terms describe the relaxation processes of the cavity mode and the molecular vibrational modes. We show that local- Lindblad theory is necessary to obtain a non-canonical steady state for the system that describes the reaction rate suppression. Meanwhile, Redfield master equation in the system eigenbasis leads to canonical steady state that does not capture the resonant behavior. +Based on the previous discussion, in the work we microscopically derive a master equation for two coupled harmonic oscillators in the strong coupling regime (see Fig.1(a)). The derivation considers weak coupling and Born-Markov approximation for the system-bath interaction. The master equation obtained contains local terms, that describes relaxation, and non-local terms, due to include the oscillator coupling in the derivation [2,3]. Results shows that the non-local terms are associate to production of coherences induced by the baths, leading the system to a canonical steady state. When the non-local terms are neglected, the system have a non-canonical steady state, with results that agree with the resonant behavior observed using local Lindblad master equation (see Fig.1(b)). Possible ways to neglect the non-local terms are discussed, including tuning temperature and energy detuning, and the inclusion of non-linear system bath interactions. -(b) Millennium Institute for Research in Optics (MIRO), Chile +[1] W. Ahn, J. F. Triana, F. Recabal, F. Herrera & B. S. Simpkins, Science, 380(6650), 1165- 1168 (2023). -Nanojunction experiments with single molecules or quantum dots placed between macroscopic leads allow the exploration of quantum transport at the nanoscale [1]. We model these systems adopting a Markovian open-quantum system approach to compute the current-voltage response of small-size networks of interacting two-level conducting sites that are coupled to leads, and radiative and non-radiative reservoirs. We model the phenomenon of light-induced current, reported theoretically [2] and experimentally [3]. We validate our Markovian model by reproducing the experimental results on negative conductance [3] of single-molecule junctions with a two-site model in the absence of electromagnetic driving (Fig. 1). We show that Coulomb blocking of current can be neglected with an external electromagnetic driving source and non-radiative decay. At zero bias voltage, the photocurrent induced by the electromagnetic driving source has a direction that depends on the delocalized orbital. We finally extend these results by treating electron transport under vibrational strong coupling in an infrared cavity (Fig. 1c) and discuss possible verifications of our predictions in current experiments [5]. +[2] C. Joshi, et al., Phys. Rev. A, 90(6), 063815 (2014). -![alt text](../../assets/speakers_figures/felipeRecabal.png) - -**Figure 1.** (a) Dimer model. (b) Modelled (solid line) y experimental (dotted line) current-voltage curve of the molecule. (c) Splitting of vibrational levels by a cavity. Experimental data extracted from [5]. - -[1] M. Thoss, and F. Evers, J. Chem. Phys., 148, 030901 (2018). - -[2] M. Galperin, and A. Nitzan, Phys. Rev. Lett., 95, 206802 (2005). - -[3] J. Zhou, K. Wang, B. Xu, and Y. Dubi, J. Am. Chem. Soc., 140, 70-73 (2018). - -[4] M. Perrin, R. Frisenda, M. Koole, et al., Nat. Nanotechnol., 9, 830–834 (2014). - -[5] F. Herrera, and J. Owrutsky, J. Chem. Phys., 152, 100902 (2020). +[3] J. Sousa, et al., Phys. Rev. A, 106(3), 032401 (2022). \ No newline at end of file diff --git a/_talks/giacomovaltolina.md b/_talks/giacomovaltolina.md index a681aea..3df66e2 100644 --- a/_talks/giacomovaltolina.md +++ b/_talks/giacomovaltolina.md @@ -1,22 +1,10 @@ --- -name: Towards cavity-controlled ultracold chemistry +name: Towards quantum control of complex cold molecules inside a cavity speakers: - Giacomo Valtolina categories: - Talk --- -G. Valtolina, J. Seifert, M. Duerbeck, S. Schaller, G. Meijer +G. Valtolina -Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany - -Ultracold molecules hold great potential for future quantum technologies but chemical reactions have so far hampered their applications1. Recently, the development of several shielding methods has enabled the stabilization of molecular quantum gases against chemical reactions2,3,4. - -This approach allowed the attainment of quantum degeneracy in quantum gas of fermionic molecules by evaporative cooling2. Leveraging on these results, we are building a new experimental apparatus with ultracold bosonic molecules strongly coupled to an optical cavity. Cavity-control of ultracold reactions offers new opportunities for the creation of a stable, strongly dipolar gas of bosonic molecules at high density. - -[1] S. Ospelkaus et al. Science 327 (5967), 853-857 (2010) - -[2] G. Valtolina et al. Nature 588 (7837), 239-243 (2020) - -[3] K. Matsuda, et al. Science 370 (6522), 1324-1327 (2020) - -[4] J.R. Li et al. Nature Physics 17 (10), 1144-1148 (2021) +The ability to control chemistry with optical cavities is enticing, but theory and experiment have not yet fully agreed. Cold and ultracold molecules oLer near ideal state preparation which can help in identifying the parameter space where cavities can aLect chemical reactions. Here, we want to present two diLerent experimental strategies to study polariton chemistry in the gas phase with quantum-state resolution. The first experiment entails the creation of an ultracold molecular gas of dysprosium dimers strongly coupled to an optical cavity. The second focuses on the creation of internally cold molecular ions of dysprosium monoxide. With these platforms, we plan to develop techniques for cavity-control of bimolecular reactions and for photo-ionization and -dissociation of molecular species. diff --git a/_talks/herbertdiaz.md b/_talks/herbertdiaz.md new file mode 100644 index 0000000..d597cc9 --- /dev/null +++ b/_talks/herbertdiaz.md @@ -0,0 +1,9 @@ +--- +name: Variational Quantum Eigensolver for Estimating the Equilibrium Configuration of Molecules +speakers: + - Herbert Diaz +categories: + - Talk +--- + +With the emergence of new technologies, quantum computing opens up a new world of possibilities, capable of tackling computationally complex problems such as optimization, combinatorial challenges [1], and molecular simulations [2]. One of the current challenges is the noise and intermediate scale reached by quantum computers (NISQ era), where errors associated with quantum phenomena prevent several algorithms from demonstrating their full utility. A way to leverage current quantum computers is through the Variational Quantum Eigensolver (VQE) [3], a quantum-classical algorithm utilized to compute the expectation value of the minimum energy of the electronic structure for molecules. By mapping fermionic systems to qubits, we use this algorithm to obtain the equilibrium energy and geometric configuration of diatomic molecules such as H2, LiH, and HF, and for the triatomic molecules H2O and O3. \ No newline at end of file diff --git a/_talks/janetanders.md b/_talks/janetanders.md new file mode 100644 index 0000000..cc658e4 --- /dev/null +++ b/_talks/janetanders.md @@ -0,0 +1,21 @@ +--- +name: Impact of system-bath coupling on a quantum system's steady state +speakers: + - Janet Anders +categories: + - Talk +--- + +The dynamical convergence to the Gibbs state is a standard assumption across much of classical and quantum thermodynamics. However, for nanoscale and quantum systems the interaction with their environment becomes non-negligible, andso-called mean force (Gibbs) states are the equilibrium states [1]. Their properties can be important whenever energy is exchanged on the nanoscale, from quantum chemistry to magnetism. + +In this talk I will first provide analytical expressions for the mean force state [2] and then discuss the impacts of system-bath coupling for a few examples. These include the presence of steady state coherences [2] in the V-level system interacting with noisy electromagnetic fields [3], and the significant system-bath entanglement emerging when a spin couples to a more realistic 3D environment instead of the commonly studied 1D environment [4]. I will close with a full characterisation of the transition from ultraweak to ultrastrong coupling regime for the widely applicable spin-boson model [5]. + +[1] Trushechkin, Merkli, Cresser, Anders,AVS Quantum Sci. 4, 012301 (2022) + +[2] Cresser, Anders, PRL 127, 250601 (2021) + +[3] Tscherbul, Brumer, PRL 113, 113601 (2014) + +[4] Hogg, Cerisola, Cresser, Horsley, Anders, Quantum 8, 1357 (2024) + +[5] Cerisola, Berritta, Scali, Horsley, Cresser, Anders, NJP 26, 053032 (2024) diff --git a/_talks/josesanzvicario.md b/_talks/josesanzvicario.md new file mode 100644 index 0000000..3e98027 --- /dev/null +++ b/_talks/josesanzvicario.md @@ -0,0 +1,15 @@ +--- +name: Ultrafast photodynamics of molecular polaritons analyzed with nonlinear multidimensional spectroscopies +speakers: + - Jose Sanz-Vicario +categories: + - Talk +--- + +n recent experiments J-aggregates of organic dye molecules immersed in optical Fabry-Perot microcavities are subject to the strong coupling interaction between the matter and the quantized light field [1]. New entangled polariton states result from the hybridation between molecular states (electronic and vibrational) and cavity photon states. To model the electronic and nuclear molecular structure of an ensemble of molecules inside a cavity and its related photodynamics from first principles is by today’s computacional capability a formidable task. Parameterized models in quantum optics like the Jaynes-Cummings Hamiltonian for a single emitter, the Tavis- Cummings Hamiltonian for a collective of emitters and the Holstein-Tavis-Cummings (including vibrational states) have served well to understand the fundamental physics of atomic and molecular emitters in cavities. In addition, these dressed-by-light emitters are subject to dissipative processes due to cavity photon losses, intra- or inter-molecular vibrational relaxation, solvent or phonon effects if aggregates are in liquid solution or in solid matrices, respectively. It implies to deal with an open quantum system coupled to a complex thermal bath. + +In this work we present a scrutinized study of the ultrafast photodynamics of an ensemble of molecular polaritons by using nonlinear coherent two- dimensional spectroscopy, for which we have recently introduced a very efficient computational method of solution [2] and we show that the role of uncoupled dark states cannot be underestimated. + +[1] L. Mewes et al, Comunn. Phys. 3, 157 (2020). + +[2] D. Gallego-Valencia, L. Mewes, J. Feist and J. L. Sanz-Vicario, Phys Rev. A 109, 063704 (2024) \ No newline at end of file diff --git a/_talks/marissaweichman.md b/_talks/marissaweichman.md index 3e25f32..68e6b10 100644 --- a/_talks/marissaweichman.md +++ b/_talks/marissaweichman.md @@ -1,12 +1,25 @@ --- -name: New Platforms for Polariton Reaction Dynamics +name: New Experimental Platforms for Molecular Polaritonics speakers: - Marissa Weichman categories: - Talk --- -Polaritons are hybrid light-matter states with unusual properties that arise from strong interactions between a molecular ensemble and the confined electromagnetic field of an optical cavity. Cavity-coupled molecules appear to demonstrate energetics, reactivity, and photochemistry dramatically distinct from their free-space counterparts, but the mechanisms and scope of these phenomena remain open questions. Validating proposed mechanisms for cavity chemistry will require a new body of experimental work directly surveying strongly-coupled reaction trajectories on clean, easily-modeled reactive potentials, working in close partnership with theory. Here, we discuss two new platforms to investigate condensed-phase and gas-phase molecular reaction dynamics under vibrational strong coupling. -In the condensed phase, we have set out to survey cavity-altered reactivity in radical hydrogen-abstraction processes. These reactions have well-characterized potential energy surfaces; they can be initiated with photolysis and tracked directly on ultrafast timescales; they are exothermic and proceed rapidly so dynamical signatures are not washed out; and they are accessible to theory, enabling detailed interpretation of reaction pathways. We run our reactions in dichroic microcavities that permit vibrational strong coupling in the infrared in combination with broadband optical access in the visible and ultraviolet. We are using ultrafast transient absorption measurements to examine intracavity reaction rates with the goal of pinpointing precisely how these trajectories may be influenced by strong light-matter interactions. +Polaritons are hybrid light-matter states that arise from strong interactions between a molecular ensemble and the confined electromagnetic field of an optical cavity. Cavity-coupled molecules appear to demonstrate chemical behavior distinct from their free-space counterparts, but the mechanisms and scope of these phenomena remain open questions [1]. I will discuss new experimental platforms that the Weichman Lab is developing to investigate molecular reaction dynamics under vibrational strong coupling. -We will also discuss our recent demonstration of gas-phase molecular polaritons. While polaritons are now well-established in solution-phase and solid-state samples, they have not yet been reported in isolated gas-phase molecules, where attaining sufficiently strong light-matter interactions is a challenge. We show that the strong-coupling regime can be accessed in the gas phase at low temperatures where molecules are found in only a few lowest-energy quantum states and their absorption linewidths are narrow. We have built an apparatus that combines a cryogenic buffer gas cell with a feedback-stabilized optical cavity to reach this regime. This new infrastructure allows us to cavity-couple individual rotational-vibrational states, access a range of coupling strengths and detunings from resonance, and tune both molecular and cavity linewidths. We expect that this platform will enable surveys of cavity-altered molecular reactivity, dynamics, and photophysics with quantum-state-specificity and without the complications of solution-phase environment. +While polaritons are now well-established in solution-phase and solid-state systems, they had not been previously reported in gas-phase molecules, where attaining suLiciently strong light-matter interactions is a challenge. We access the strong coupling regime in an intracavity cryogenic buLer gas cell optimized for the preparation of cold, dense ensembles and report a demonstration of strongly coupled rovibrational transitoin in gas-phase methane [2,3]. In ongoing work, we will harness this infrastructure as a new testbed for fundamental studies of polariton physics and chemistry [4]. + +We are also searching for signatures of cavity-altered dynamics in benchmark solution-phase systems [5,6]. So far, we have focused on radical hydrogen-abstraction processes, which have well- characterized reactive surfaces and can be initiated with photolysis and tracked directly on ultrafast timescales. We use ultrafast transient absorption to examine intracavity reaction rates with the goal of better understanding exactly how and when reactive trajectories may be influenced by strong light-matter interactions. + +[1] K. Schwennicke, A. Koner, J. B. Pérez-Sánchez, W. Xiong, N. C. Giebink, M. L. Weichman, and J. Yuen-Zhou. When do molecular polaritons behave like optical filters? arXiv 2408.05036 (2024). + +[2] A. D. Wright, J. C. Nelson, and M. L. Weichman. Rovibrational polaritons in gas-phase methane. J. Am. Chem. Soc. 145, 5982 (2023). + +[3] A. D. Wright, J. C. Nelson, and M. L. Weichman. A versatile platform for gas-phase molecular polaritonics. J. Chem. Phys. 159, 164202 (2023). + +[4] J. C. Nelson and M. L. Weichman. More than just smoke and mirrors: Gas-phase polaritons for optical control of chemistry. J. Chem. Phys. 161, 074304 (2024). + +[5] A. P. Fidler, L. Chen, A. M. McKillop, and M. L. Weichman. Ultrafast dynamics of CN radical reactions with chloroform solvent under vibrational strong coupling. J. Chem. Phys. 159, 164302 (2023). + +[6] L. Chen, A. P. Fidler, A. M. McKillop, and M. L. Weichman. Exploring the impact of vibrational cavity coupling strength on ultrafast CN + c-C6H12 reaction dynamics. Nanophotonics 13, 2591 (2024). diff --git a/_talks/markusraschke.md b/_talks/markusraschke.md index 7f72414..9d38263 100644 --- a/_talks/markusraschke.md +++ b/_talks/markusraschke.md @@ -1,26 +1,19 @@ --- -name: Quantum vibrational microscopy and sensing +name: Quantum vibrational nano-imaging; a molecular ruler to image structure, coupling, and disorder in molecular materials speakers: - Markus Rashcke categories: - Talk --- -The quest from low-loss quantum materials, to efficient heat transport, high conductivity transistors, and chemical reactions all rely on understanding and engineering the local density of vibrational modes. In this talk, I will discuss the use of molecular vibrations and IR resonant nano-wire coupled molecular interactions as sensors and local probes for inter- to intra-molecular coupling, thermalization, and dissipation. This includes the development of new nano-imaging techniques that provide a qualitatively new window into the spatial, temporal, and low energy spectral vibrational landscape of molecular and other quantum materials. These new vibrational quantum scopes harness ideas developed in the context of quantum optomechanical control of motion to image the elementary processes of vibrational and polaron dynamics in ultrafast vibrational nano-movies with nanometer and femtosecond spatio-temporal resolution. +Properties and functions of molecular materials often emerge from intermolecular interactions and associated nanoscale structure and morphology. However, defects and disorder disturb from energy conversion to carrier transport. Conventional microscopy techniques lack spatial resolution and sensitivity to the low-energy scales of intermolecular interactions and intra-molecular energy relaxation. We address these problems in novel combinations of spatio-spectral and spatio-temporal infrared nano-imaging. Here, coupling between molecular vibrations leads to collective modes, with distinct spectral features sensitive to intermolecular distance and relative molecular orientation. Resolving this vibrational exciton formation as a molecular ruler in IR nano-spectroscopy, we image competing phases and local disorder in molecular solids – information inaccessible by conventional X-ray or electron-based crystallography. In the application to the growth of porphyrin model organic electronic nanocrystals we observe the evolution of defects in competing amorphous and crystalline phases with nanometer spatial resolution [1,5]. Similarly, imaging vibrational coupling in polymers [2] and molecular monolayer [3], we resolve domain formation from the molecular to nano-scale. Further, in another modality through mode selective coupling of vibrational resonances to IR nano-antennas and associated Purcell-enhanced modification of vibrational lifetimes, we resolve intramolecular vibrational interaction and vibrational energy redistribution (IVR) [4]. I will summarize with a perspective for nm-fs resolved precision vibrational nano-spectroscopy for functional imaging in the low-energy landscape of molecular matter. -![alt text](../../assets/speakers_figures/markusRaschke.png) +[1] Muller, et al., PNAS 117, 7030 (2020); -**Figure 1**. Infrared nano-imaging of spatial delocalization of the vibrational wavefunction, serving as quantum sensor and molecular ruler of molecular disorder, crystallinity, and intermolecular coupling that control the properties of functional molecular materials at their elementary level. +[2] Gray, et al., Nano Lett. 21, 5754 (2021); -[1] K.-D. Park et al., Science Adv. 5, eaav5931 (2019). +[3] Dönges et al. Nano Lett. 21, 6463 (2021); -[2] E. A. Muller, et al., ACS Photonics 5, 3594 (2018). +[4] Wilcken et al. PNAS 120, e2220852120 (2023); -[3] B. Metzger et al., Phys. Rev. Lett. 123, 153001 (2019). +[5] Puro, et al. 24, 1909 (2024). -[4] E. A. Muller, et al., PNAS 117, 7030 (2020). - -[5] M. A. May et al. Nano Lett. 21, 522 (2020). - -[6] D. Yoo, et al. Nature Photonics. 15, 125 (2021). - -[7] T. P. Gray, et al. Nano Lett. 21, 5754 (2021). diff --git a/_talks/matthewsheldon.md b/_talks/matthewsheldon.md new file mode 100644 index 0000000..93b9030 --- /dev/null +++ b/_talks/matthewsheldon.md @@ -0,0 +1,18 @@ +--- +name: Plasmonic Platforms for Polaritonic Chemistry +speakers: + - Matthew Sheldon +categories: + - Talk +--- + +We are developing experimental platforms to probe vibrational strong coupling (VSC) between molecules and resonant infrared (IR) nanophotonic architectures, in order to understand how this coupling can fundamentally control chemical reactivity, as well as enable new classes of light- matter interaction. This method of altering the potential energy surface of a chemical process via coherent, electromagnetic perturbation of vibrating bonds has also been termed “polaritonic chemistry”. We employ a combined experimental strategy leveraging expertise in (1) the design of IR “metasurfaces” composed of plasmonic metal substrates that provide tailorable VSC to molecules within their optical near-field; and (2) multiple continuous wave (CW) spectroscopic techniques that enable analysis of several non-equilibrium, dynamic electronic eLects in the metal substrate. Taken together, these tools allow studies into new regimes of spectral bandwidth (e.g. simultaneous multi-mode coupling), coupling strength, and time domains (e.g. studies of long lived and steady-state phenomena) that have been inaccessible using conventional optical cavities and time-resolved spectroscopies performed to date. + +Vibrational strong coupling is fundamentally interesting because it is a coherent interaction between radiation and molecular motion. The direct manipulation of a molecular process using externally controlled forcefields to obtain a desired outcome, i.e. “coherent control” or “quantum control”, has been a long-standing goal connected to the central aims of chemical science. Thus, this presentation will discuss the limits of chemical analysis and chemical control at interfaces leveraging a framework based on coherent interactions between controllable features of the engineered surface geometry and the molecular systems under study. + +[1] Z. Brawley*, S. Pannir-Sivajothi*, JE. Yim*, YR. Poh, J. Yuen-Zhou, M. Sheldon. "Vibrational weak and strong coupling modify a chemical reaction via cavity-mediated radiative energy +transfer." Nature Chemistry 2024, (accepted, in press) + +[2] JE. Yim, Z. Brawley, M. Sheldon. "Subradiant Plasmonic Cavities Make Bright Polariton States Dark." Nanophotonics 2024 + +[3] Z. T. Brawley, S. D. Storm, D. A. C. Mora, M. Pelton, M. Sheldon. "Angle-Independent Plasmonic Substrates for Multi-Mode Vibrational Strong Coupling with Molecular Thin Films." Journal of Chemical Physics 2021, 154, 104305 \ No newline at end of file diff --git a/_talks/michaelshatruk.md b/_talks/michaelshatruk.md new file mode 100644 index 0000000..298309e --- /dev/null +++ b/_talks/michaelshatruk.md @@ -0,0 +1,12 @@ +--- +name: High-Symmetry Lanthanide Complexes as Clock-Transition Qubits +speakers: + - Michael Shatruk +categories: + - Talk +--- +Qubit is an elementary unit of quantum computing, allowing coherent superposition of states that can be initialized, manipulated, and read-out for quantum information processing. Molecular spin qubits are appealing due to their synthetic tunability and a broad range of spin states that can be incorporated by using various transition and lanthanide metal ions. The generally short coherence time, however, remains the major obstacle for implementation of molecular qubits in quantum computing technology. In this contribution, we demonstrate how this challenge can be addressed by using high-symmetry lanthanide complexes to achieve clock transitions [1,2] characterized by a dramatically enhanced coherence time at specific values of resonant magnetic field. We use variable-frequency EPR spectroscopy to determine the clock-transition energy gaps for the ground- state doublets of crystal-field generated manifolds of ±mJ states and demonstrate the correlations of the gap magnitude to the geometry of the local coordination environment around the lanthanide ion. + +[1] M. Shiddiq, D. Komijani, Y. Duan, A. Gaita-Ariño, E. Coronado, S. Hill, Nature 2016, 531, 348-351. + +[2] A. Gaita-Ariño, F. Luis, S. Hill, E. Coronado, Nat. Chem. 2019, 11, 301-309. \ No newline at end of file diff --git a/_talks/michelinesoley.md b/_talks/michelinesoley.md new file mode 100644 index 0000000..13783ea --- /dev/null +++ b/_talks/michelinesoley.md @@ -0,0 +1,17 @@ +--- +name: From Ultracold Molecules to Quantum Computing; Collisions Under Quantum Control +speakers: + - Micheline Soley +categories: + - Talk +--- + +Molecules below one milliKelvin offer an unprecedented opportunity to examine chemical reactions at the level of individual quantum states and to prepare ultracold molecular qubits. A central problem in ultracold physics, which could provide new insight into the development of qubits, is how to simulate the dynamics of ultracold molecules. The long wavelengths associated with low temperatures, coupled with the exponential growth of computational cost as dimensionality increases, currently makes simulation of exact quantum dynamics of ultracold molecules cost-prohibitive for systems of more than three atoms. In addition, anomalous reflection of low-energy components of wavepackets from complex absorbing potentials (optical potentials or perfectly matching layers) has been a problem for decades in quantum scattering and time-dependent calculations, and is especially problematic in ultracold simulations given the systems’ low temperature. A solution to this problem could provide a new view into both the dynamics and control of ultracold molecular qubits. In this talk, I will present a novel method that addresses this problem based on the finding that, whereas low temperatures are typically associated with quantum mechanics, classical and semiclassical Wentzel-Kramers-Brillouin corrections can be added to complex absorbing potentials to reduce anomalous reflection by orders of magnitude. This technique offers a possible way to simulate the dynamics of ultracold molecular qubits and ultracold chemical reactions with higher accuracy and computational efficiency. + +Quantum control also offers an exciting possibility to create ultracold molecular qubits by directly controlling the outcome of ultracold molecular collisions. In this talk, I will introduce a method that applies reflectionless scattering mode (RSM) theory, recently developed in optics, to direct product formation in chemical reactions with zero reformation of reactants. Surprisingly, the method only requires two variable parameters, which offers an efficient and unique approach to the creation of ultracold molecules in desired quantum states. The talk will discuss how, by combining Wentzel- Kramers-Brillouin force analysis and reflectionless scattering mode theory, one can reveal theoretically the existence of a long-sought-after fundamental physical property - PT-symmetry- breaking phenomena in fundamental quantum scattering - via standard cold-atom experiments in programmable traps.1 The talk will conclude with a discussion of quantum computing algorithms, both on quantum computers and classical computers via tensor networks/matrix product states.2,3 + +[1] M. B. Soley, C. M. Bender, A. D. Stone, Physical Review Letters, 130 (2023) 250404. + +[2] T. H. Kyaw,* M. B. Soley,* B. Allen, P. Bergold, C. Sun, V. S. Batista, A. Aspuru-Guzik, Quantum Science and Technology, 9 (2024) 01LT01. + +[3] M. B. Soley,* P. E. Videla,* E. T. J. Nibbering, V. S. Batista, Journal of Physical Chemistry Letters, 13 (2022) 8254-8263. diff --git a/_talks/niclasmueller.md b/_talks/niclasmueller.md new file mode 100644 index 0000000..a28105d --- /dev/null +++ b/_talks/niclasmueller.md @@ -0,0 +1,18 @@ +--- +name: Detecting Collective Molecular Vibrations with Surface-Enhanced Raman Spectroscopy + +speakers: + - Niclas Mueller +categories: + - Talk +--- +In surface-enhanced Raman scattering (SERS), vibrations of molecules couple with optical modes of a plasmonic nanocavity via a molecular optomechanical interaction. This eLect is typically assumed to occur at individual molecules neglecting intermolecular vibrational coupling. Here, we show instead how collective vibrations are observed in SERS through two diLerent mechanisms: 1. Molecules can couple into collective vibrations through direct infrared (IR) dipole coupling, which is usually observed with IR spectroscopy. We show that cooperative frequency shifts from these collective IR vibrations can be also detected with SERS [1]. These collective states can be tuned with mixed self-assembled monolayers and allow us to monitor photochemical reactions. 2. Molecules can also form collective vibrations through the coupling of induced Raman dipoles when driven with intense laser pulses [2]. We show how such collective Raman vibrations enhance the optomechanical coupling with plasmonic nanocavities and reduce the onset of vibrational nonlinearities. + +Finally, I will show recent experiments where we probe the lifetime of molecular vibrations in plasmonic nanocavities with ultrafast Raman spectroscopy [3]. Using time-resolved coherent and incoherent anti-Stokes Raman spectroscopy we separate the contributions of vibrational dephasing and population decay, and isolate molecular signals from four-wave mixing. + + +[1] Mueller et al. Collective Mid-Infrared Vibrations in Surface-Enhanced Raman Scattering, Nano Lett. 22, 7254 (2022) + +[2] Jakob, Juan-Delgado, Mueller et al. Optomechanical Pumping of Collective Molecular Vibrations in Plasmonic Nanocavities, submitted (2024) + +[3] Jakob, Deacon et al. Accelerated molecular vibrational decay and suppressed electronic nonlinearities in plasmonic cavities through coherent Raman scattering, Phys. Rev. B 109, 195404 (2024) \ No newline at end of file diff --git a/_talks/ruthtichauer.md b/_talks/ruthtichauer.md index ea55537..936ea66 100644 --- a/_talks/ruthtichauer.md +++ b/_talks/ruthtichauer.md @@ -1,51 +1,33 @@ --- -name: Strongly Coupled Organic Molecules, Insights from Atomistic MD Simulations +name: Modelling Light-Matter Interactions with Atomic Resolution speakers: - Ruth Tichauer categories: - Talk --- -Ruth H. Tichauer (a,b), Ilia Sokolovskii (b), Johannes Feist (a), Gerrit Groenhof (b) -(a) Departamento de Física, Teórica de la Materia Condensada and Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid, Madrid, Spain +In addition to their advantageous size, cost-eLective and reproducible synthesis [1], the large binding energy of Frenkel excitons makes organic molecules promising candidates for future applications in energy harvesting [2], transport [3-5], and the design of novel quantum devices [6] relying on room temperature polariton formation [7,8]. However, the complex photo-physics taking place in such emitters, challenges conventional quantum optics approaches that consider idealised two-level systems characterised by a well-defined (broadened) resonance. -(b) Department of Chemistry and NanoScience Center, University of Jyväskylä, Finland +Employing an atomistic QM/MM description, we develop an approach [9,10] that captures the photo-chemistry within such molecules in the presence of intense and inhomogeneous electromagnetic fields emerging in plasmonic or hybrid metallo-dieletric nano-resonators of arbitrary shape [11,12]. I will introduce the model and share insights concerning the excitation dynamics of systems composed of organic molecules embedded in photonic resonators of various shapes. -While the complex internal dynamics as well as the immediate material environment of -organic chromophores limit their coherent emission and transport properties, coupling -these photoactive molecules to nanophotonic structures has the potential to open a new -era in energy harvesting [1], transport [2,3], and information processing [4,5]. In the -strong light-matter coupling regime, the large binding energy of Frenkel excitons makes -organic materials promising candidates for future applications as polariton formation -takes place at ambient conditions. -However, a model that describes accurately both the molecules and the electromagnetic -environment created by the light-confining structure is currently lacking which limits the -understanding of the effects of material properties in the dynamics of strongly coupled -systems. While we have achieved the first requirement of such a model by adopting an -atomistic QM/MM representation of the material part of the strongly coupled system -[6,7], the description of confined light was limited to modes of optical Fabry-Pérot -resonators [8]. To move beyond, we introduce an explicit description of the quantised -electromagnetic field for arbitrary nanophotonic structures such as plasmonic or hybrid -metallodieletric nanocavities [9]. In the talk, I will present the model and share ongoing -work aimed at investigating the properties of a few chromophores strongly coupled to a -plasmonic nanocavity [10]. +[1] C. Toninelli et al., Nat. Materials, 20 (2021) -1. J.Q. Quach et al., Sci. Adv., 8 (2022) +[2] J.Q. Quach et al., Sci. Adv., 8, eabk3160 (2022) -2. G.G. Rozenman et al., ACS Photonics, 5 (2018) +[3] A.M. Berghuis et al., ACS Photonics, (2022) -3. A.M. Berghuis et al., ACS Photonics, 9 (2022) +[4] Sokolovskii et al, Nat. Commun. 14 (2023) 6613 -4. C. Toninelli et al., Nat. Materials, 20 (2021) +[5] R.H. Tichauer et al, Adv. Sci., 10 (2023) 2302650 -5. D. Sanvitto and S. Kéna-Cohen, Nat. Materials, 15 (2016) +[6] D. Sanvitto and S. Kéna-Cohen, Nat. Materials, 15, 1061 (2016) [7] J. Fregoni et al., ACS Photonics. 9, 1096 (2022) -6. H.L. Luk et al., J. Chem. Theory Comput., 13 (2017) +[8] M.S. Rider and W.L. Barnes, Contemporary Physics, (2022) -7. G. Groenhof et al., J. Phys. Chem. Lett., 10 (2019) +[9] H.L. Luk et al., J. Chem. Theory Comput., 13, 4324 (2017) -8. R.H. Tichauer et al., J. Chem. Phys., 154 (2021) +[10] R.H. Tichauer et al., J. Chem. Phys., 154, 104112 (2021) -9. M. Sánchez-Barquilla et al., Nanophotonics, 11 (2022) +[11] I. Medina et al., Phys. Rev. Lett. 126, 093601 (2021) -10. J. Heintz et al., ACS Nano., 15 (2021) \ No newline at end of file +[12] M. Sánchez-Barquilla et al., Nanophotonics, 11 (2022) \ No newline at end of file diff --git a/_talks/taoli.md b/_talks/taoli.md new file mode 100644 index 0000000..598fa06 --- /dev/null +++ b/_talks/taoli.md @@ -0,0 +1,17 @@ +--- +name: A Tale of Two Methods for Simulating Molecular Polaritons +speakers: + - Tao Li +categories: + - Talk +--- + +Polariton formation between molecular transitions and cavity photon modes provides a novel strategy for modifying local molecular processes. However, our theoretical understanding of many polariton experiments remains elusive. For a realistic simulation of molecular polaritons in the collective regime, here, we introduce two numerical schemes developed in our group: the reduced semiclassical electrodynamics approach [1], and the mesoscale cavity molecular dynamics (CavMD) approach [2]. In the former scheme, only a few molecules, referred to as quantum impurities, are treated quantum mechanically, while the remaining macroscopic molecular layer and the cavity structure are modeled using dielectric functions with Maxwell's equations. In the latter method, a grid of realistic molecular ensembles coupled to many cavity modes are propagated within the framework of molecular dynamics. + +Using the reduced semiclassical electrodynamics approach, we study the polariton-induced Purcell eLect under electronic strong coupling: the radiative decay rate of the quantum impurity is significantly enhanced by the cavity when the impurity frequency matches the polariton frequency, while the rate can sometimes be greatly suppressed when the impurity is near resonance with the bulk molecules forming strong coupling [1]. Equipped with mesoscale CavMD, we simulate elementary polariton-polariton scattering events under vibrational strong coupling. This approach also facilitates the understanding of vibrational polaritons with broken in-plane translational symmetry [3]. + +[1] A. F. Bocanegra Vargas, T. E. Li. "Polariton-induced Purcell eWects via a reduced semiclassical electrodynamics approach". Submitted to J. Chem. Phys., 2024. + +[2] T. E. Li. " Mesoscale molecular simulations of Fabry–Pérot vibrational strong coupling". J. Chem. Theory Comput., 20, 7016-7031, 2024. + +[3] T. E. Li. "Vibrational polaritons with broken in-plane translational symmetry". J. Chem. Phys., 161, 064308, 2024. \ No newline at end of file