Mode switching dynamics in organic polariton lasing

Funding: AJM and PT acknowledge support by the Academy of Finland under project numbers 303351, 307419, 327293, 318987 (QuantERA project RouTe), 318937 (PROFI), and 320167 (Flagship Programme, Photonics Research and Innovation (PREIN)), and by Centre for Quantum Engineering (CQE) at Aalto University. AJM acknowledges financial support by the Jenny and Antti Wihuri Foundation and ETH Zurich Postdoctoral Fellowship. KBA and JK acknowledge financial support from EPSRC program “Hybrid Polaritonics” (EP/M025330/1). KBA acknowledges support from The RSE Saltire Research Award.We study the dynamics of multimode polariton lasing in organic microcavities by using a second-order cumulant equation approach. By inspecting the time evolution of the photon mode occupations, we show that if multiple lasing peaks are observed in time-integrated mode occupations, the reason can be either bi-modal lasing or temporal switching between several modes. The former takes place within a narrow range of parameters while the latter occurs more widely. We find that the origin of the temporal switching is different in the weak- and strong-coupling regimes. At weak coupling slope efficiency is the determining factor, while for strong coupling it is changes in the eigenmodes and gain spectrum upon pumping. This difference is revealed by investigating the photoluminescence and momentum-resolved gain spectra. Our results underscore the importance of understanding the time evolution of the populations when characterizing the lasing behaviour of a multimode polariton system, and show how these features differ between weak and strong coupling.Publisher PDFPeer reviewe

Determining the validity of cumulant expansions for central spin models

For a model with many-to-one connectivity it is widely expected that mean-field theory captures the exact many-particle $N\to\infty$ limit, and that higher-order cumulant expansions of the Heisenberg equations converge to this same limit whilst providing improved approximations at finite $N$. Here we show that this is in fact not always the case. Instead, whether mean-field theory correctly describes the large-$N$ limit depends on how the model parameters scale with $N$, and we show that convergence of cumulant expansions may be non-uniform across even and odd orders. Further, even when a higher-order cumulant expansion does recover the correct limit, the error is not monotonic with $N$ and may exceed that of mean-field theory.Comment: 7 pages, 3 figures plus supplementary materia

Mode switching dynamics in organic polariton lasing

We study the dynamics of multimode polariton lasing in organic microcavities by using a second-order cumulant equation approach. By inspecting the time evolution of the photon mode occupations, we show that if multiple lasing peaks are observed in time-integrated mode occupations, the reason can be either bi-modal lasing or temporal switching between several modes. The former takes place within a narrow range of parameters while the latter occurs more widely. We find that the origin of the temporal switching is different in the weak- and strong-coupling regimes. At weak coupling slope efficiency is the determining factor, while for strong coupling it is changes in the eigenmodes and gain spectrum upon pumping. This difference is revealed by investigating the photoluminescence and momentum-resolved gain spectra. Our results underscore the importance of understanding the time evolution of the populations when characterizing the lasing behaviour of a multimode polariton system, and show how these features differ between weak and strong coupling

Mode switching dynamics in organic polariton lasing

We study the dynamics of multimode polariton lasing in organic microcavities by using a second-order cumulant equation approach. By inspecting the time evolution of the photon mode occupations, we show that if multiple lasing peaks are observed in time-integrated mode occupations, the reason can be either bi-modal lasing or temporal switching between several modes. The former takes place within a narrow range of parameters while the latter occurs more widely. We find that the origin of the temporal switching is different in the weak- and strong-coupling regimes. At weak coupling slope efficiency is the determining factor, while for strong coupling it is changes in the eigenmodes and gain spectrum upon pumping. This difference is revealed by investigating the photoluminescence and momentum-resolved gain spectra. Our results underscore the importance of understanding the time evolution of the populations when characterizing the lasing behaviour of a multimode polariton system, and show how these features differ between weak and strong coupling.Comment: 12 pages, 10 figure

Determining the validity of cumulant expansions for central spin models

For a model with many-to-one connectivity it is widely expected that mean-field theory captures the exact many-particle limit, and that higher-order cumulant expansions of the Heisenberg equations converge to this same limit whilst providing improved approximations at finite N. Here we show that this is in fact not always the case. Instead, whether mean-field theory correctly describes the large-N limit depends on how the model parameters scale with N, and the convergence of cumulant expansions may be non-uniform across even and odd orders. Further, even when a higher-order cumulant expansion does recover the correct limit, the error is not monotonic with N and may exceed that of mean-field theory

Determining the validity of cumulant expansions for central spin models

For a model with many-to-one connectivity it is widely expected that mean-field theory captures the exact many-particle N → ∞ limit, and that higher-order cumulant expansions of the Heisenberg equations converge to this same limit whilst providing improved approximations at finite N. Here we show that this is in fact not always the case. Instead, whether mean-field theory correctly describes the large-N limit depends on how the model parameters scale with N, and we show that convergence of cumulant expansions may be non-uniform across even and odd orders. Further, even when a higher-order cumulant expansion does recover the correct limit, the error is not monotonic with N and may exceed that of mean-field theory

Few-emitter lasing in single ultra-small nanocavities.

Peer reviewed: TrueAcknowledgements: We acknowledge support from EPSRC grants EP/G060649/1, EP/L027151/1, EP/G037221/1, EP/T014032/1, EPSRC NanoDTC and from the European Research Council (ERC) under Horizon 2020 research and innovation programme PICOFORCE (Grant Agreement No. 883703), THOR (Grant Agreement No. 829067) and POSEIDON (Grant Agreement No. 861950). O.S.O acknowledges the support of a Rubicon fellowship from the Netherlands Organisation for Scientific Research (NWO). We thank Rohit Chikkarddy and Rakesh Arul for valuable discussions and Jack Griffiths for making the cartoon in Figure 1.Publication status: PublishedFunder: EPSRC NanoDTCLasers are ubiquitous for information storage, processing, communications, sensing, biological research and medical applications. To decrease their energy and materials usage, a key quest is to miniaturise lasers down to nanocavities. Obtaining the smallest mode volumes demands plasmonic nanocavities, but for these, gain comes from only a single or few emitters. Until now, lasing in such devices was unobtainable due to low gain and high cavity losses. Here, we demonstrate a form of 'few emitter lasing' in a plasmonic nanocavity approaching the single-molecule emitter regime. The few-emitter lasing transition significantly broadens, and depends on the number of molecules and their individual locations. We show this non-standard few-emitter lasing can be understood by developing a theoretical approach extending previous weak-coupling theories. Our work paves the way for developing nanolaser applications as well as fundamental studies at the limit of few emitters

Few-emitter lasing in single ultra-small nanocavities

Peer reviewed: TrueAcknowledgements: We acknowledge support from EPSRC grants EP/G060649/1, EP/L027151/1, EP/G037221/1, EP/T014032/1, EPSRC NanoDTC and from the European Research Council (ERC) under Horizon 2020 research and innovation programme PICOFORCE (Grant Agreement No. 883703), THOR (Grant Agreement No. 829067) and POSEIDON (Grant Agreement No. 861950). O.S.O acknowledges the support of a Rubicon fellowship from the Netherlands Organisation for Scientific Research (NWO). We thank Rohit Chikkarddy and Rakesh Arul for valuable discussions and Jack Griffiths for making the cartoon in Figure 1.Publication status: PublishedFunder: EPSRC NanoDTCLasers are ubiquitous for information storage, processing, communications, sensing, biological research and medical applications. To decrease their energy and materials usage, a key quest is to miniaturise lasers down to nanocavities. Obtaining the smallest mode volumes demands plasmonic nanocavities, but for these, gain comes from only a single or few emitters. Until now, lasing in such devices was unobtainable due to low gain and high cavity losses. Here, we demonstrate a form of ‘few emitter lasing’ in a plasmonic nanocavity approaching the single-molecule emitter regime. The few-emitter lasing transition significantly broadens, and depends on the number of molecules and their individual locations. We show this non-standard few-emitter lasing can be understood by developing a theoretical approach extending previous weak-coupling theories. Our work paves the way for developing nanolaser applications as well as fundamental studies at the limit of few emitters

Few-emitter lasing in single ultra-small nanocavities

Peer reviewed: TrueAcknowledgements: We acknowledge support from EPSRC grants EP/G060649/1, EP/L027151/1, EP/G037221/1, EP/T014032/1, EPSRC NanoDTC and from the European Research Council (ERC) under Horizon 2020 research and innovation programme PICOFORCE (Grant Agreement No. 883703), THOR (Grant Agreement No. 829067) and POSEIDON (Grant Agreement No. 861950). O.S.O acknowledges the support of a Rubicon fellowship from the Netherlands Organisation for Scientific Research (NWO). We thank Rohit Chikkarddy and Rakesh Arul for valuable discussions and Jack Griffiths for making the cartoon in Figure 1.Publication status: PublishedFunder: EPSRC NanoDTCLasers are ubiquitous for information storage, processing, communications, sensing, biological research and medical applications. To decrease their energy and materials usage, a key quest is to miniaturise lasers down to nanocavities. Obtaining the smallest mode volumes demands plasmonic nanocavities, but for these, gain comes from only a single or few emitters. Until now, lasing in such devices was unobtainable due to low gain and high cavity losses. Here, we demonstrate a form of ‘few emitter lasing’ in a plasmonic nanocavity approaching the single-molecule emitter regime. The few-emitter lasing transition significantly broadens, and depends on the number of molecules and their individual locations. We show this non-standard few-emitter lasing can be understood by developing a theoretical approach extending previous weak-coupling theories. Our work paves the way for developing nanolaser applications as well as fundamental studies at the limit of few emitters

Few-emitter lasing in single ultra-small nanocavities.

Peer reviewed: TrueAcknowledgements: We acknowledge support from EPSRC grants EP/G060649/1, EP/L027151/1, EP/G037221/1, EP/T014032/1, EPSRC NanoDTC and from the European Research Council (ERC) under Horizon 2020 research and innovation programme PICOFORCE (Grant Agreement No. 883703), THOR (Grant Agreement No. 829067) and POSEIDON (Grant Agreement No. 861950). O.S.O acknowledges the support of a Rubicon fellowship from the Netherlands Organisation for Scientific Research (NWO). We thank Rohit Chikkarddy and Rakesh Arul for valuable discussions and Jack Griffiths for making the cartoon in Figure 1.Publication status: PublishedFunder: EPSRC NanoDTCLasers are ubiquitous for information storage, processing, communications, sensing, biological research and medical applications. To decrease their energy and materials usage, a key quest is to miniaturise lasers down to nanocavities. Obtaining the smallest mode volumes demands plasmonic nanocavities, but for these, gain comes from only a single or few emitters. Until now, lasing in such devices was unobtainable due to low gain and high cavity losses. Here, we demonstrate a form of 'few emitter lasing' in a plasmonic nanocavity approaching the single-molecule emitter regime. The few-emitter lasing transition significantly broadens, and depends on the number of molecules and their individual locations. We show this non-standard few-emitter lasing can be understood by developing a theoretical approach extending previous weak-coupling theories. Our work paves the way for developing nanolaser applications as well as fundamental studies at the limit of few emitters