Coherent Optical Transient Studies of Dephasing and Relaxation in Electronic Transitions of Large Molecules in the Condensed Phase

Wiersma, Douwe A.

doi:10.1002/9780470142660.ch13

Cited by 19 publications

(2 citation statements)

References 115 publications

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“…Notably, the low-temperature linewidths are the same (~100 MHz) for different inequivalent divacancies in our 4H-SiC sample, where the nitrogen concentration is a few ppb, while divacancies in the 3C-SiC sample have about 20x larger linewidths (2 GHz), where the nitrogen concentration is about 0.5-1 ppm. The identical linewidths among inequivalent forms in the same 4H-SiC sample, similar broadening at high-temperatures, temperatureindependence below 20 K, and prior reports of poor linewidths in nitrogen-rich diamond, are all consistent with the idea that linewidths we observe are sample-dependent rather than intrinsic[60,[66][67][68][69]. These observations suggest that reducing impurities and annealing any residual crystal damage are promising routes towards achieving lifetime-limited linewidths in…”

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confidence: 89%

Isolated Spin Qubits in SiC with a High-Fidelity Infrared Spin-to-Photon Interface

et al. 2017

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The divacancies in SiC are a family of paramagnetic defects that show promise for quantum communication technologies due to their long-lived electron spin coherence and their optical addressability at near-telecom wavelengths. Nonetheless, a high-fidelity spin-photon interface, which is a crucial prerequisite for such technologies, has not yet been demonstrated. Here, we demonstrate that such an interface exists in isolated divacancies in epitaxial films of 3C-SiC and 4H-SiC. Our data show that divacancies in 4H-SiC have minimal undesirable spin mixing, and that the optical linewidths in our current sample are already similar to those of recent remote entanglement demonstrations in other systems. Moreover, we find that 3C-SiC divacancies have a millisecond Hahn-echo spin coherence time, which is among the longest measured in a naturally isotopic solid. The presence of defects with these properties in a commercial semiconductor that can be heteroepitaxially grown as a thin film on Si shows promise for future quantum networks based on SiC defects.

Funding Agencies|ARO [W911NF-15-2-0058]; AFOSR [FA9550-15-1-0029, FA9550-14-1-0231]; NSF MRSEC [DMR-1420709]; DOE LDRD Program; Swedish Research Council [621-2014-5825, 2016-04068]; AForsk foundation [16-576]; Carl-Trygger Stiftelse for Vetenskaplig Forskning [CTS 15:339]; Knut and Alice Wallenberg Foundation [KAW 2013.0300]; JSPS [26286047]; Swedish Energy Agency [43611-1]

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confidence: 89%

Isolated Spin Qubits in SiC with a High-Fidelity Infrared Spin-to-Photon Interface

et al. 2017

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“…One goal of high-resolution spectroscopy was to measure the true homogeneous width of the zero phonon, purely electronic transition of molecules in solids without the interference from inhomogeneous broadening. It is for this reason that much research in the 1970's and 1980's was devoted to methods like fluorescence line narrowing (FLN) (13,14) and transient spectroscopies such as free induction decay, optical nutation, and photon echoes (15)(16)(17). While these were all powerful methods with advantages and disadvantages, there was another method to assess the homogeneous width under certain circumstances, persistent spectral hole-burning, illustrated in Figure 4.…”

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Nobel Lecture: Single-molecule spectroscopy, imaging, and photocontrol: Foundations for super-resolution microscopy

Moerner

2015

Rev. Mod. Phys.

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The initial steps toward optical detection and spectroscopy of single molecules in condensed matter arose out of the study of inhomogeneously broadened optical absorption profiles of molecular impurities in solids at low temperatures. Spectral signatures relating to the fluctuations of the number of molecules in resonance led to the attainment of the single-molecule limit in 1989 using frequency-modulation laser spectroscopy. In the early 90's, many fascinating physical effects were observed for individual molecules, and the imaging of single molecules as well as observations of spectral diffusion, optical switching and the ability to select different single molecules in the same focal volume simply by tuning the pumping laser frequency provided important forerunners of the later superresolution microscopy with single molecules. In the room temperature regime, imaging of single copies of the green fluorescent protein also uncovered surprises, especially the blinking and photoinduced recovery of emitters, which stimulated further development of photoswitchable fluorescent protein labels. Because each single fluorophore acts a light source roughly 1 nm in size, microscopic observation and localization of individual fluorophores is a key ingredient to imaging beyond the optical diffraction limit. Combining this with active control of the number of emitting molecules in the pumped volume led to the super-resolution imaging of Eric Betzig and others, a new frontier for optical microscopy beyond the diffraction limit. The background leading up to these observations is described and current developments are summarized. The early days Introduction and early inspirationsI want to thank the Nobel Committee for Chemistry, the Royal Swedish Academy of Sciences, and the Nobel Foundation for selecting me for this prize recognizing the development of super-resolved fluorescence microscopy. I am truly honored to share the prize with my two esteemed colleagues, Stefan Hell and Eric Betzig. My primary contributions center on the first optical detection and spectroscopy of single molecules in the condensed phase(1), and on the observations of imaging, blinking and photocontrol not only for single molecules at low temperatures in solids, but also for useful variants of the green fluorescent protein at room temperature (2). This lecture describes the context of the events leading up to these advances as well as a portion of the subsequent developments both around the world and in my laboratory.In the mid-1980's, I derived much early inspiration from amazing advances that were occurring around the world where single nanoscale quantum systems were detected and explored for both scientific and technological reasons. Some of these were (i) the spectroscopy of single electrons or ions confined in vacuum electromagnetic traps (3-5), (ii) scanning tunneling microscopy (STM) (6) and atomic force microscopy (AFM) (7), and (iii) the study of ion currents in single membrane-embedded ion channels (8). But why not optical detection and ...

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The Redfield Equation in Condensed‐Phase Quantum Dynamics

Pollard

Felts

Friesner

1996

Advances in Chemical Physics

177

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Coherent Optical Transient Studies of Dephasing and Relaxation in Electronic Transitions of Large Molecules in the Condensed Phase

Cited by 19 publications

References 115 publications

Isolated Spin Qubits in SiC with a High-Fidelity Infrared Spin-to-Photon Interface

Isolated Spin Qubits in SiC with a High-Fidelity Infrared Spin-to-Photon Interface

Nobel Lecture: Single-molecule spectroscopy, imaging, and photocontrol: Foundations for super-resolution microscopy

The Redfield Equation in Condensed‐Phase Quantum Dynamics

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