Cooperative subwavelength molecular quantum emitter arrays

Holzinger, Raphael; Oh, Sue Ann; Reitz, Michael; Ritsch, Helmut; Genes, Claudiu

doi:10.1103/physrevresearch.4.033116

Cited by 8 publications

(12 citation statements)

References 42 publications

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“…Subwavelength atomic array as a promising light-matter platform provides an optimal playground for the observation and exploitation of quantum cooperative effects [2,3]. Our simulations can be of great interest as well for other researches such as excitation transfer [41-43, 45, 46, 78], or chiral quantum optics with atomic waveguide [60,[79][80][81].…”

Section: Conclusion and Discussionmentioning

confidence: 91%

“…The cooperative effects, such as superradiance [1], are some of the most intriguing phenomena in many-body physics, which cannot be interpreted solely by considering the individual constituents. Subwavelength quantum emitter arrays give rise to cooperative optical effects via dipole-dipole interactions [2,3]. For example, the quantum metasurface based on atomic arrays enables manipulation of macroscopic optical responses [4][5][6][7][8][9][10][11] or realization of atomic mirror [12][13][14][15][16].…”

Section: Introductionmentioning

confidence: 99%

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Optimal subradiant spin wave exchange in dipole-coupled atomic ring arrays

Han,

Chen,

Liu

et al. 2023

New J. Phys.

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The subwavelength array of quantum emitters provides an ideal platform for exploring rich many-body dynamics, such as super- and subradiance. In this paper, we explore the dynamics of spin wave exchange between two dipole-coupled atomic ring arrays. Subradiant spin waves lead to low-loss and high efficiency of ring-to-ring transfer. The optimal subradiant spin wave exchange occurs at appropriate separations between coplanar rings, despite the fact that the energy transfer efficiency is monotonically enhanced (in the regime ⩽ λ 0 / 2 ) as the rings’ separation decreases. However, the spin wave will scatter due to the dephasing mechanism of close-by atom pairs, as the separation of two rings is too small. With the increase in the number of atoms on the ring, the subradiant shielding effect also strengthens, leading to a shorter distance for the transfer of spin waves. We investigate the rotation of one of the rings and find that the optimal spin wave exchange corresponds to the scenario where the line connecting the two nearest atoms of the two rings aligns with the center of the circle. Moreover, we study the influence of transition dipole moment orientations on the effective interaction between two atomic rings. We observe that there is a critical point where the effective interaction strength changes dramatically owing to the cooperative effect of the subwavelength atomic array. We believe that our results could be important for quantum information processing based on atomic arrays.

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Section: Conclusion and Discussionmentioning

confidence: 91%

Section: Introductionmentioning

confidence: 99%

Optimal subradiant spin wave exchange in dipole-coupled atomic ring arrays

Han,

Chen,

Liu

et al. 2023

New J. Phys.

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“…With the definitions κ S total loss rate of the symmetric state, κ q loss rate for dark state q , κ q → scriptS incoherent repopulation rate from the dark to the bright state and κ q ′→ q incoherent rate for redistribution of energy within the dark state manifold, one can write ṗ S = prefix− ( γ scriptS + κ scriptS ) p S + prefix∑ q ≠ 0 κ q → scriptS p q , ṗ q = prefix− κ q p q + prefix∑ q ′ ≠ q κ q ′ → q p q ′ . The rate equations show that the symmetric state energy spills into the whole dark state manifold via rate κ S and, in addition, higher energy dark states spill into the lower energy ones via κ q . The quasi-unidirectionality of the process is ensured by the fact that, in this perturbative treatment, the coherent coupling between states is followed by quick vibrational relaxation, making the reverse process, governed by rates κ q → scriptS and κ q ′→ q from lower energy state to higher ones, very unlikely (as shown in ref for the two monomer case). Mathematically, the condition is s m ν m / N …”

Section: Resultsmentioning

confidence: 99%

“…The model can be better tackled on a collective basis resulting from the diagonalization of the first excitation subspace including dipole–dipole interactions. This can be done either in the discrete space where states are indexed from 1 to scriptN (see Figure a) or alternatively, with the quasi-momentum index q = 2 π k / ( N d ) obtained by a rescaling of the index of the mode k = prefix± 1 , ... , prefix± ( N − 1 ) / 2 (see Figure b).…”

Section: Methodsmentioning

confidence: 99%

“…The collective excitations are eigenstates of the dipole–dipole interaction Hamiltonian H d − d A q † false| g ⟩ ⊗ N = Ω q A q † false| g ⟩ ⊗ N where by definition we fix the symmetric shift Ω S ≡ Ω q = 0 . With periodic boundary conditions imposed, in the mesoscopic limit, one can derive the collective shifts as Ω q = 2∑ j Ω 1 j cos( q ( j – 1) d ). , Further simplifications occur by considering the nearest neighbor approximation and the collective eigenenergies become Ω q = 2Ω cos( qd ), where the nearest-neighbor coupling is simply denoted by Ω ≡Ω 12 . Closely following the procedure introduced in ref , one can analyze the coupling between states of different symmetries via electron–vibron couplings by an additional transformation to a collective basis for the vibrational degrees of freedom as well.…”

Section: Methodsmentioning

confidence: 99%

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Scaling Law for Kasha’s Rule in Photoexcited Molecular Aggregates

Holzinger,

Bassler,

Ritsch

et al. 2024

J. Phys. Chem. A

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We study the photophysics of molecular aggregates from a quantum optics perspective, with emphasis on deriving scaling laws for the fast nonradiative relaxation of collective electronic excitations, referred to as Kasha's rule. Aggregates exhibit an energetically broad manifold of collective states with delocalized electronic excitations originating from near-field dipole−dipole exchanges between neighboring monomers. Photoexcitation at optical wavelengths, much larger than the monomer− monomer average separation, addresses almost exclusively symmetric collective states, which for an arrangement known as H-aggregate show an upward hypsochromic shift. The extremely fast subsequent nonradiative relaxation via intramolecular vibrational modes populates lower energy, subradiant states, resulting in effective inhibition of fluorescence. Our analytical treatment allows for the derivation of an approximate scaling law of this relaxation process, linear in the number of available low-energy vibrational modes and directly proportional to the dipole−dipole interaction strength between neighboring monomers.

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Ultrafast Photoinduced Dynamics of Styryl-Substituted BODIPY Dyes and Their Aggregates

Ghosh,

Mula,

Biswas

et al. 2024

J. Phys. Chem. C

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We synthesized a series of boron dipyrromethene (BODIPY) dyes with varying p-methoxystyryl substituents to study their excited-state dynamics in both molecular and aggregated forms. Single-crystal X-ray diffraction revealed herringbone packing through π•••π stacking in the unsubstituted dye, which was disrupted upon styryl substitution. Unsubstituted BODIPY formed aqueous H-aggregates with considerable emission, whereas styryl-substituted variants exhibited unprecedented and unusual nonemissive, red-shifted H-aggregates. The HOMO−LUMO gap decreased with an increase in the number of styryl substituents, aligning with quantum chemical calculations. Femtosecond transient absorption spectroscopy and global analysis suggest slower solvation, vibrational cooling, and excited-state structural relaxation with increased substitution. The unsubstituted BODIPY Haggregates exhibited a distinct emissive state within the lower excitonic state manifold and ultrafast nonradiative relaxation from the dark state. On the other hand, styryl-substituted aggregates demonstrated vibration-assisted relaxation to the dark, singlet, lower excitonic state, which was long-lived. Our study highlights how structural modifications significantly influence the packing structure and photophysical properties of BODIPY dyes and aggregates, which are critical for biophotonics and optoelectronics applications.

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Cooperative subwavelength molecular quantum emitter arrays

Cited by 8 publications

References 42 publications

Optimal subradiant spin wave exchange in dipole-coupled atomic ring arrays

Optimal subradiant spin wave exchange in dipole-coupled atomic ring arrays

Scaling Law for Kasha’s Rule in Photoexcited Molecular Aggregates

Ultrafast Photoinduced Dynamics of Styryl-Substituted BODIPY Dyes and Their Aggregates

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