Molecular Vibrational Polaritons Towards Quantum Technologies

Yang, Zimo; Xiang, Bo

doi:10.1002/qute.202100163

Cited by 7 publications

(8 citation statements)

References 70 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Indeed, intensity of radiation field enters Σ ≷ C via greater/lesser projections of Green function A, Eq. (11), which in turn is defined by Σ ≷ A , Eq. ( 6), whose Σ rad contribution, Eq.…”

Section: Numerical Resultsmentioning

confidence: 99%

See 1 more Smart Citation

Exceptional points treatment of cavity spectroscopies

Mukamel

Galperin

2023

The Journal of Chemical Physics

View full text Add to dashboard Cite

The infrared response of a system of two vibrational modes in a cavity is calculated by an effective non-Hermitian Hamiltonian derived by employing the nonequilibrium Green's functions (NEGF) formalism. Degeneracies of the Hamiltonian (exceptional points, EP) widely employed in theoretical analysis of optical cavity spectroscopies are used in an approximate treatment and compared with the full NEGF. Qualitative limitations of the EP treatment are explained by examining the approximations employed in the calculation.

show abstract

Section: Numerical Resultsmentioning

confidence: 99%

“…Developments in experimental techniques allow the spectroscopic measurements of molecular systems placed in cavities [1][2][3][4][5][6][7][8][9][10][11]. Cavity confinement promotes strong coupling between radiation field and molecular degrees of freedom.…”

Section: Introductionmentioning

confidence: 99%

Exceptional points treatment of cavity spectroscopies

Mukamel

Galperin

2023

The Journal of Chemical Physics

View full text Add to dashboard Cite

show abstract

“…We have made a few steps to prepare vibrational polaritons as a new quantum technology platform by showing that polaritons can nonlinearly interact with each other when sitting in different cavities. , We used photolithography and deposition techniques to create a checkerboard-pattern DBR, with adjacent squares having an ∼200 nm height difference. Thus, when the patterned DBR was paired with a flat DBR, they formed neighboring cavities with different longitudinal thicknesses and resonant frequencies (Figure B,C).…”

Section: Toward Vibrational-polariton-based Quantum Technologymentioning

confidence: 99%

Molecular Vibrational Polariton Dynamics: What Can Polaritons Do?

Xiong

2023

Acc. Chem. Res.

Self Cite

View full text Add to dashboard Cite

Metrics & MoreArticle Recommendations CONSPECTUS: When molecular vibrational modes strongly couple to virtual states of photonic modes, new molecular vibrational polariton states are formed, along with a large population of dark reservoir modes. The polaritons are much like the bonding and antibonding molecular orbitals when atomic orbitals form molecular bonds, while the dark modes are like nonbonding orbitals. Because the polariton states are half-matter and half-light, whose energy is shifted from the parental states, polaritons are predicted to modify chemistry under thermally activated conditions, leading to an exciting and emerging field known as polariton chemistry that could potentially shift paradigms in chemistry. Despite several published results supporting this concept, the chemical physics and mechanism of polariton chemistry remain elusive. One reason for this challenge is that previous works cannot differentiate polaritons from dark modes. This limitation makes delineating the contributions to chemistry from polaritons and dark states difficult. However, this level of insight is critical for developing a solid mechanism for polariton chemistry to design and predict the outcome of strong coupling with any given reaction. My group addressed the challenge of differentiating the dynamics of polaritons and dark modes by ultrafast two-dimensional infrared (2D IR) spectroscopy. Specifically, (1) we found that polaritons can facilitate intra-and intermolecular vibrational energy transfer, opening a pathway to control vibrational energy flow in liquid-phase molecular systems, and (2) by studying a single-step isomerization event, we verified that indeed polaritons can modify chemical dynamics under strong coupling conditions, but in contrast, the dark modes behave like uncoupled molecules and do not change the dynamics. This finding confirmed the central concept of polariton chemistry: polaritons modify the potential energy landscape of reactions. The result also clarified the role of dark modes, which lays a critical foundation for designing cavities for future polariton chemistry. Aside from using 2D IR spectroscopy to study polariton chemistry, we also used the same technique to develop molecular polaritons into a potential quantum simulation platform. We demonstrated that polaritons have Rabi oscillations, and using a checkerboard cavity design, we showed that polaritons could have large nonlinearity across space. We further used the checkerboard polaritons to simulate coherence transfer and visualize it. A unidirectional coherence transfer was observed, indicating non-Hermitian dynamics. The highlighted efforts in this Account provide a solid understanding of the capability of polaritons for chemistry and quantum information science. I conclude this Account by discussing a few challenges for moving polariton chemistry toward being predictable and making the polariton quantum platform a complement to existing systems.

show abstract

“…1 A ). Thus, UP and LP can be treated as one polariton qubit system at ambient conditions ( 28 , 29 , 34 ).…”

mentioning

confidence: 99%

“…The molecular vibrational polariton-based qubits is a potential platform for quantum simulation with several advantages, such as operating at ambient temperature, ease of tunability of cavities, intrinsic systems for quantum light molecular spectroscopy, and the customizable “designer” vibrational chromophores ( 35 – 37 ). Although similar efforts have been made on exciton polaritons, the single qubit property of the FP cavity has limited the scalability of molecular vibrational polaritons for advancing quantum simulation ( 34 ). One way to overcome the limitations is to form multi-qubit systems, also called qudits, using multi-cavity polariton systems.…”

mentioning

confidence: 99%

Enabling multiple intercavity polariton coherences by adding quantum confinement to cavity molecular polaritons

Yang

Bhakta

Xiong

2022

Proc. Natl. Acad. Sci. U.S.A.

View full text Add to dashboard Cite

In this study, the “particle in a box” idea, which was broadly developed in semiconductor quantum dot research, was extended into mid-infrared (IR) cavity modes by applying lateral confinement in an optical cavity. The discrete cavity modes hybridized with molecular vibrational modes, resulting in a quartet of polariton states that can support multiple coherence states in the IR regime. We applied tailored pump pulse sequences to selectively prepare these coherences and verified the multi-coherence existence. The simulation based on Lindblad equation showed that because the quartet of polariton states resided in the same cavity, they were specifically robust toward decoherence caused by fluctuations in space. The multiple robust coherences paved the way for entangled states and coherent interactions between cavity polaritons, which would be critical for advancing polariton-based quantum information technology.

show abstract

Molecular Vibrational Polaritons Towards Quantum Technologies

Cited by 7 publications

References 70 publications

Exceptional points treatment of cavity spectroscopies

Exceptional points treatment of cavity spectroscopies

Molecular Vibrational Polariton Dynamics: What Can Polaritons Do?

Enabling multiple intercavity polariton coherences by adding quantum confinement to cavity molecular polaritons

Contact Info

Product

Resources

About