112 research outputs found

    Image Restoration: A General Wavelet Frame Based Model and Its Asymptotic Analysis

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    Image restoration is one of the most important areas in imaging science. Mathematical tools have been widely used in image restoration, where wavelet frame based approach is one of the successful examples. In this paper, we introduce a generic wavelet frame based image restoration model, called the "general model", which includes most of the existing wavelet frame based models as special cases. Moreover, the general model also includes examples that are new to the literature. Motivated by our earlier studies [1-3], We provide an asymptotic analysis of the general model as image resolution goes to infinity, which establishes a connection between the general model in discrete setting and a new variatonal model in continuum setting. The variational model also includes some of the existing variational models as special cases, such as the total generalized variational model proposed by [4]. In the end, we introduce an algorithm solving the general model and present one numerical simulation as an example

    On the Successiveness of the Two Extreme Cold Events in China during the 2020/21 Winter According to Cold Air Trajectories

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    Two extreme cold air events successively hit China during 28–31 December 2020 (the late 2020 event) and during 6–8 January 2021 (the early 2021 event), which caused great losses. These two events have received extensive attention in relation to synoptic weather systems and remote forcing. Although it has been noted that a near-surface cool condition can greatly impact tropospheric circulation, its role in the successiveness of two such extreme cold waves remains unclear. This study focused on cold air pathways from the Lagrangian perspective, and explored the potential influence of cold air over the key region in terms of connecting the two cold events using a piecewise potential vorticity inversion. With the obtained results, three cold air sources with three corresponding air routes were identified in the two cold events. The northern pathway dominated the late 2020 event, in which the cold air intruded from the eastern Laptev Sea and moved southward to China. In contrast, the early 2021 event was mainly associated with the northwestern pathway in which the cold air came from the Ural Mountains and moved clockwise. Notably, cold air traveling along the western route from western Lake Balkhash arrived at the north of the Tianshan Mountains earlier and amplified the positive height anomaly in situ. Moreover, such an enhanced positive height anomaly moved the direction of the cold air from the northern and northwestern routes southward and thus played a key role in the successiveness of the two extreme cold events

    On the Successiveness of the Two Extreme Cold Events in China during the 2020/21 Winter According to Cold Air Trajectories

    No full text
    Two extreme cold air events successively hit China during 28–31 December 2020 (the late 2020 event) and during 6–8 January 2021 (the early 2021 event), which caused great losses. These two events have received extensive attention in relation to synoptic weather systems and remote forcing. Although it has been noted that a near-surface cool condition can greatly impact tropospheric circulation, its role in the successiveness of two such extreme cold waves remains unclear. This study focused on cold air pathways from the Lagrangian perspective, and explored the potential influence of cold air over the key region in terms of connecting the two cold events using a piecewise potential vorticity inversion. With the obtained results, three cold air sources with three corresponding air routes were identified in the two cold events. The northern pathway dominated the late 2020 event, in which the cold air intruded from the eastern Laptev Sea and moved southward to China. In contrast, the early 2021 event was mainly associated with the northwestern pathway in which the cold air came from the Ural Mountains and moved clockwise. Notably, cold air traveling along the western route from western Lake Balkhash arrived at the north of the Tianshan Mountains earlier and amplified the positive height anomaly in situ. Moreover, such an enhanced positive height anomaly moved the direction of the cold air from the northern and northwestern routes southward and thus played a key role in the successiveness of the two extreme cold events

    Tantallacarborane Mediated Consecutive C–C and C–N Coupling Reactions of Alkyl Isonitriles: A Facile Route to N‑Heterocycles

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    Reactions of tantallacarborane methyl complexes ([η<sup>1</sup>:η<sup>5</sup>-(Me<sub>2</sub>NCH<sub>2</sub>CH<sub>2</sub>)­C<sub>2</sub>B<sub>9</sub>H<sub>10</sub>]­TaMe<sub>3</sub> (<b>1</b>) and [η<sup>1</sup>:η<sup>5</sup>-(MeOCH<sub>2</sub>CH<sub>2</sub>)­C<sub>2</sub>B<sub>9</sub>H<sub>10</sub>]­TaMe<sub>3</sub> (<b>8</b>)) with alkyl isonitriles have been studied. Complex <b>1</b> reacted with 1 equiv of RNC (R = TMSCH<sub>2</sub>, Cy, and <sup><i>i</i></sup>Pr) to afford double migratory insertion products [η<sup>1</sup>:η<sup>5</sup>-(Me<sub>2</sub>NCH<sub>2</sub>CH<sub>2</sub>)­C<sub>2</sub>B<sub>9</sub>H<sub>10</sub>]­Ta­[η<sup>2</sup>-<i>C</i>,<i>N</i>-C­(Me<sub>2</sub>)­NCH<sub>2</sub>TMS]­Me (<b>2</b>) and [σ:η<sup>1</sup>:η<sup>5</sup>-{MeN­(CH<sub>2</sub>)­CH<sub>2</sub>CH<sub>2</sub>}­C<sub>2</sub>B<sub>9</sub>H<sub>10</sub>]­Ta­[N­(<sup><i>i</i></sup>Pr)­R]­Me (R = Cy (<b>3</b>), <sup><i>i</i></sup>Pr (<b>4</b>)). However, treatment of <b>1</b> or <b>8</b> with 4 equiv of alkyl isonitriles gave two fused six-membered <i>N</i>-heterocycles <b>5</b>–<b>7</b> and <b>9</b> via consecutive C–C/C-N bond-forming reactions. All new complexes were characterized by <sup>1</sup>H, <sup>13</sup>C, and <sup>11</sup>B NMR spectra as well as elemental analyses. Their structures were further confirmed by single-crystal X-ray analyses. The results show that aryl and alkyl isonitriles exhibit significantly different reactivity patterns. This work also offers a very efficient method for the synthesis of N-heterocycles

    Reaction of 13-Vertex Carborane μ‑1,2-(CH<sub>2</sub>)<sub>3</sub>‑1,2‑C<sub>2</sub>B<sub>11</sub>H<sub>11</sub> with Nucleophiles: Scope and Mechanism

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    13-Vertex carborane, μ-1,2-(CH<sub>2</sub>)<sub>3</sub>-1,2-C<sub>2</sub>B<sub>11</sub>H<sub>11</sub> (<b>1</b>), reacted with a series of nucleophiles (Nu) to give the cage carbon extrusion products [μ-1,2-(CH<sub>2</sub>)<sub>3</sub>­CH­(Nu)-1-CB<sub>11</sub>H<sub>10</sub>]<sup>−</sup>, [μ-1,2-(CH<sub>2</sub>)<sub>2</sub>­CH­(Nu)­CH<sub>2</sub>-1-CB<sub>11</sub>H<sub>10</sub>]<sup>−</sup>, and/or [μ-1,2-(CH<sub>2</sub>)<sub>2</sub>­CHCH-1-CB<sub>11</sub>H<sub>10</sub>]<sup>−</sup>, depending on the nature of Nu and the reaction conditions. The key intermediates for the formation of CB<sub>11</sub><sup>–</sup> anions were isolated and structurally characterized as [μ–η:η:η-7,8,10-(CH<sub>2</sub>)<sub>3</sub>­CHB­(Nu)-7-CB<sub>10</sub>H<sub>10</sub>]<sup>−</sup> (Nu = OMe, NEt<sub>2</sub>). The reaction mechanism is thus proposed, which involves the attack of Nu at the most electron-deficient cage boron, followed by H-migration to one of the cage carbons, leading to the formation of the intermediate. Nu-migration gives the products

    Reactivity of Traditional Metal–Carbon (Alkyl) versus Nontraditional Metal–Carbon (Cage) Bonds in Organo-Rare-Earth Metal Complexes [η<sup>5</sup>:σ-(C<sub>9</sub>H<sub>6</sub>)(C<sub>2</sub>B<sub>10</sub>H<sub>10</sub>)]­Ln(CH<sub>2</sub>C<sub>6</sub>H<sub>4</sub>‑<i>o</i>‑NMe<sub>2</sub>)(THF)<sub>2</sub>

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    Equimolar reaction of 1-indenyl-1,2-carborane with Ln­(CH<sub>2</sub>C<sub>6</sub>H<sub>4</sub>-<i>o</i>-NMe<sub>2</sub>)<sub>3</sub> in THF gave highly constrained-geometry complexes [η<sup>5</sup>:σ-(C<sub>9</sub>H<sub>6</sub>)­C<sub>2</sub>B<sub>10</sub>H<sub>10</sub>]­Ln­(CH<sub>2</sub>C<sub>6</sub>H<sub>4</sub>-<i>o</i>-NMe<sub>2</sub>)­(THF)<sub>2</sub> (Ln = Y (<b>1a</b>), Gd (<b>1b</b>), Dy (<b>1c</b>)). They reacted with RNCNR or 2,6-Me<sub>2</sub>C<sub>6</sub>H<sub>3</sub>NCS to generate the Ln–C<sub>alkyl</sub> insertion products [η<sup>5</sup>:σ-(C<sub>9</sub>H<sub>6</sub>)­C<sub>2</sub>B<sub>10</sub>H<sub>10</sub>]­Ln­[η<sup>2</sup><i>-</i>(RN)<sub>2</sub>C­(CH<sub>2</sub>C<sub>6</sub>H<sub>4</sub>-<i>o</i>-NMe<sub>2</sub>)]­(THF) (R = TMS, Ln = Y (<b>2a</b>), Gd (<b>2b</b>); R = <sup><i>t</i></sup>Bu, Ln = Y (<b>3a</b>)) or [η<sup>5</sup>:σ-(C<sub>9</sub>H<sub>6</sub>)­C<sub>2</sub>B<sub>10</sub>H<sub>10</sub>]­Dy­[η<sup>2</sup><i>-</i>(2,6-Me<sub>2</sub>C<sub>6</sub>H<sub>3</sub>)­NC­(CH<sub>2</sub>C<sub>6</sub>H<sub>4</sub>-<i>o</i>-NMe<sub>2</sub>)­S]­(THF)<sub>2</sub> (<b>4c</b>). Treatment of <b>2a</b> with 1 equiv of R′NCNR′ to give the Y–C<sub>cage</sub> insertion complexes [η<sup>5</sup>:σ-(C<sub>9</sub>H<sub>6</sub>)­{N­(R′)­C­(NR′)}­C<sub>2</sub>B<sub>10</sub>H<sub>10</sub>]­Y­[η<sup>2</sup><i>-</i>{(TMS)­N}<sub>2</sub>­C­(CH<sub>2</sub>C<sub>6</sub>H<sub>4</sub>-<i>o</i>-NMe<sub>2</sub>)] (R′ = Cy (<b>5a</b>), <sup><i>i</i></sup>Pr (<b>6a</b>)). Similarly, unsaturated compounds Ph<sub>2</sub>CCO and Py<sub>2</sub>CO (Py = 2-pyridyl) also inserted into the Y–C<sub>cage</sub> bond in <b>2a</b> to yield [η<sup>5</sup>:σ-(C<sub>9</sub>H<sub>6</sub>)­{OC­(CPh<sub>2</sub>)}­C<sub>2</sub>B<sub>10</sub>H<sub>10</sub>]­Y­[η<sup>2</sup><i>-</i>{(TMS)­N}<sub>2</sub>C­(CH<sub>2</sub>C<sub>6</sub>H<sub>4</sub>-<i>o</i>-NMe<sub>2</sub>)] (<b>7a</b>) and [η<sup>5</sup>:σ-(C<sub>9</sub>H<sub>6</sub>)­{OC­(Py)<sub>2</sub>}­C<sub>2</sub>B<sub>10</sub>H<sub>10</sub>]­Y­[η<sup>2</sup><i>-</i>{(TMS)­N)}<sub>2</sub>­C­(CH<sub>2</sub>C<sub>6</sub>H<sub>4</sub>-<i>o</i>-NMe<sub>2</sub>)]­(THF) (<b>8a</b>), respectively. In sharp contrast to the earlier reports that the nontraditional metal–C<sub>cage</sub> σ bonds in metal–carboranyl complexes are generally inert toward electrophiles, the insertion of unsaturated molecules into the Y–C<sub>cage</sub> σ bond in <b>2a</b> represents the first example of this type of reactions. These results shed some light on how to activate the nontraditional metal–carbon (cage) bonds in metal–carboranyl complexes. All new complexes were characterized by spectroscopic techniques and elemental analyses. Some were further confirmed by single-crystal X-ray analyses

    Palladium-Catalyzed Regioselective Intramolecular Coupling of <i>o</i>‑Carborane with Aromatics via Direct Cage B–H Activation

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    Palladium-catalyzed intramolecular coupling of <i>o</i>-carborane with aromatics via direct cage B–H bond activation has been achieved, leading to the synthesis of a series of <i>o</i>-carborane-functionalized aromatics in high yields with excellent regioselectivity. In addition, the site selectivity can also be tuned by the substituents on cage carbon atom
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