Spectral lines of single molecules in a fluctuating environment

G. Zumofen, J. Klafter

Mathias Pont, Anne-Laurence Phaneuf-L’Heureux, R. André +1 more

Motional narrowing is a phenomenon by which a quantum state can be entangled with a noisy environment and still retain its intrinsic coherence. Using two optically induced motional forces driving the environmental electrical field amplitude and fluctuations, we present a compelling illustration of the effects of motional narrowing on the energy, line shape, and line width of a single quantum emitter, a Te 2 molecule embedded in ZnSe, subject to spectral diffusion. Motional narrowing is achieved in several regimes, irrespectively of the inhomogeneous disorder initially present and the charge reservoir state sourcing the field. The optimal coherence limit set by the radiative rate can be approached by accelerating spectral diffusion into the THz regime. Motional narrowing applies to any quantum systems for which environmental fluctuations can be deliberately accelerated and alleviates the need for perfected materials and devices.

V. Palm, K. -S. K. Rebane

Th. Basché, Christoph Bräuchle

Abstract In recent years different microscopic and spectroscopic techniques were successfully employed to detect the fluorescence signals of single dye molecules in the condensed phase. In low temperature solids the fluorescence excitation line of a single dopant molecule is a high resolution optical probe of its local nanoenvironment. As inhomogeneous contributions and ensemble averaging are absent, many effects hidden when looking at large populations of molecules become observable. Two important research areas in single molecule spectroscopy deal with the investigation of quantum optical effects and the spectral jumping behaviour of single molecule excitation lines caused by fluctuations of two‐level systems inherent to disordered solids. Rather than delivering a complete presentation, we will focus on some selected examples which emphasize the unique features of spectroscopy with a single absorber.

Xiangji Cai, Yonggang Peng, Yujun Zheng

We theoretically investigate the statistical properties of photon emission of a driven two-level single-molecule system undergoing spectral diffusion induced by nonequilibrium environmental fluctuations. Within the framework of the generating function method and the stochastic Liouville equation, we analyze the influence of the nonequilibrium characteristics of environmental fluctuations respectively governed by nonstationary Ornstein-Uhlenbeck noise and random telegraph noise on the photon counting statistics of the driven single-molecule system. In the slow modulation limit of spectral diffusion, the intensity and statistical fluctuations of photon emission depend on the environmental nonequilibrium characteristics at short time scales, whereas they become independent of the nonequilibrium characteristics of environmental fluctuations in the steady state. In the fast modulation limit of spectral diffusion, neither the line shape nor the Mandel's parameter depends on the environmental nonequilibrium characteristics owing to the rapid relaxation of environmental fluctuations. These findings not only shed light on the role of nonequilibrium environmental fluctuations in shaping the photon emission properties of single-molecule systems but also provide a basis for distinguishing between equilibrium and nonequilibrium characteristics of environmental fluctuations in experimental measurements.

Evgenii B. Aleksandrov, V. N. Kulyasov